☆ 4.8 Review

Operando Scanning Electrochemical Probe Microscopy during Electrocatalysis

CHEMICAL REVIEWS (2023)

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Article Chemistry, Multidisciplinary

Localized Electrosynthesis and Subsequent Electrochemical Mapping of Catalytically Active Metal-Organic Frameworks

Itamar Liberman et al.

Summary: Metal-organic frameworks (MOFs) have great potential as catalytic materials in electrochemical energy conversion reactions. This study used scanning electrochemical microscopy (SECM) to perform localized electrosynthesis of MOFs and analyze their catalytic hydrogen evolution reaction activity. The results shed light on the operation principles of electroactive MOFs and their potential use in alternative fuel production schemes.

ADVANCED FUNCTIONAL MATERIALS (2022)

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Review Chemistry, Multidisciplinary

Electrocatalysis in Alkaline Media and Alkaline Membrane-Based Energy Technologies

Yao Yang et al.

Summary: This article provides a comprehensive review of the fundamentals of electrocatalysis in alkaline media and its applications in alkaline-based energy technologies. Nonprecious anion exchange membrane fuel cells offer a promising alternative to proton exchange membrane fuel cells for sluggish oxygen reduction reaction. The understanding of proton-coupled electron transfer and active sites has contributed to the development of high-performance and durable alkaline fuel cells.

CHEMICAL REVIEWS (2022)

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Article Chemistry, Physical

Electrochemically probing exciton transport in monolayers of two-dimensional semiconductors

Chloe L. Tolbert et al.

Summary: This study demonstrates the use of electrochemical microscopy techniques as powerful tools for visualizing processes in 2DSCs, even within individual monolayers. The CG-TC SECCM was applied to visualize carrier generation and transport within well-defined n-WSe2 samples prepared via mechanical exfoliation, revealing how carrier transport varies within complex 2DSC structures as layer thicknesses approach the monolayer limit. These results provide valuable new insights into carrier transport within monolayer TMD materials and highlight electrochemical imaging as a powerful yet underutilized approach for visualizing solid-state processes in semiconducting materials.

FARADAY DISCUSSIONS (2022)

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Article Chemistry, Physical

Hybrid scanning electrochemical cell microscopy-interference reflection microscopy (SECCM-IRM): tracking phase formation on surfaces in small volumes

Dimitrios Valavanis et al.

Summary: The combination of SECCM and IRM techniques allows for the study of interfacial processes with high spatial and temporal resolution. SECCM confines reactions to specific regions on a surface, while IRM detects processes close to the substrate. This technique enables real-time monitoring of SECCM meniscus and processes at the electrode/electrolyte interface, providing valuable insights into phase formation processes.

FARADAY DISCUSSIONS (2022)

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Article Chemistry, Physical

iR drop in scanning electrochemical cell microscopy

Brandon Blount et al.

Summary: Nanoscale electrochemical mapping techniques like SECCM are increasingly utilized to study local electrochemistry in electrocatalysis, allowing for a more accurate measurement of local electrode kinetics and revealing heterogeneity in mechanisms. Techniques for estimating and compensating for iR drop in SECCM experiments have been developed to improve the accuracy of measurements for determining local mechanisms in electrocatalysis.

FARADAY DISCUSSIONS (2022)

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Article Chemistry, Multidisciplinary

Tunable angle-dependent electrochemistry at twisted bilayer graphene with moire flat bands

Yun Yu et al.

Summary: This study reports a strong twist-angle dependence of heterogeneous charge transfer kinetics at twisted bilayer graphene electrodes, with the greatest enhancement observed near the 'magic angle'. The variation in electrochemical activity is controlled by the structural relaxation of the moire superlattice at twist angles of <2 degrees and the presence of 'topological defect' AA stacking regions.

NATURE CHEMISTRY (2022)

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Article Chemistry, Physical

Direct Electrochemical Visualization of the Orthogonal Charge Separation in Anatase Nanotube Photoanodes for Water Splitting

Marina Makarova et al.

Summary: The photoelectrochemical (PEC) catalytic effects of anatase TiO2-nanotube arrays grown on Ti felt are explored using scanning electrochemical cell microscopy (SECCM). The results support the transport of photoexcited electrons along the TiO2 nanotubes and the model of orthogonal electron-hole separation.

ACS CATALYSIS (2022)

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Review Chemistry, Physical

Operando Monitoring and Deciphering the Structural Evolution in Oxygen Evolution Electrocatalysis

Shouwei Zuo et al.

Summary: This review elaborates on recent advances in the study of OER electrocatalysts using several in situ/operando techniques, with an emphasis on tracking the structural evolution processes, recording reaction intermediates, and establishing the structure-activity/stability relationship.

ADVANCED ENERGY MATERIALS (2022)

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Article Electrochemistry

Probing Individual Cuprous Oxide Microcrystals towards Carbon Dioxide Reduction by using In Situ Raman-coupled Scanning Electrochemical Microscopy

Matthias Steimecke et al.

Summary: This study simultaneously investigated a single cuprous oxide microcrystal for CO2 electroreduction using Raman microscopy and scanning electrochemical microscopy. The structural changes of the Cu2O microcrystal converting into elemental Cu at low overpotentials were observed in situ. Formate ions were found to be the main product of CO2 reduction, which was detected electrochemically using a 10 μm Pt ultramicroelectrode.

CHEMELECTROCHEM (2022)

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Article Electrochemistry

Pd-Modified De-alloyed Au-Ni-Microelectrodes for In Situ and Operando Mapping of Hydrogen Evolution

Julian Kund et al.

Summary: This article presents the fabrication of Pd-modified microelectrodes for in situ electrochemical hydrogen measurements. Stability studies and pH-dependent investigations confirm the stability of these microsensors over a period of seven days and their applicability in a pH range of 3-10. The experiments using scanning electrochemical microscopy demonstrate the potential of these microsensors for operando studies in light-driven heterogeneous catalysis.

CHEMELECTROCHEM (2022)

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Article Materials Science, Multidisciplinary

Layer and material-type dependent photoresponse in WSe2/WS2 vertical heterostructures

ZhuangEn Fu et al.

Summary: This study demonstrates the layer-number dependence of photocurrents in TMD heterostructures and reveals anomalous layer and material-type dependent behaviors in WSe2/WS2 heterostructures.

2D MATERIALS (2022)

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Article Nanoscience & Nanotechnology

Revealing the Nature of Active Sites on Pt-Gd and Pt-Pr Alloys during the Oxygen Reduction Reaction

Regina M. Kluge et al.

Summary: This study uses EC-STM technique to investigate the ORR active areas of Pt5Gd and Pt5Pr in acidic media, and finds that compressed Pt-lanthanide (111) terraces contribute the most to the overall activity.

ACS APPLIED MATERIALS & INTERFACES (2022)

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Article Chemistry, Analytical

Topography Mapping with Scanning Electrochemical CellMicroscopy

Gen Liu et al.

Summary: This paper presents a high-resolution scanning electrochemical cell microscopy (SECCM) scheme that allows simultaneous observation of the topography and electrochemical activity of materials at the nanoscale. The use of homemade nanoprobes with an inner diameter of about 50 nm enables reliable measurements with a resolution of several tens of nanometers (≥65 nm). The scheme successfully records the topography and hydrogen evolution reaction (HER) activity of a self-assembled monolayer of gold nanoparticles with a diameter of about 45 nm. This approach has the potential to greatly expand the field of SECCM applications by routinely mapping the topographic and chemical properties of samples at the nanometer scale.

ANALYTICAL CHEMISTRY (2022)

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Article Chemistry, Analytical

Nanoscale Visualization of Electrochemical Activity at Indium Tin Oxide Electrodes

Oluwasegun J. Wahab et al.

Summary: This study investigates nanoscale electrochemistry at indium tin oxide (ITO) electrodes using high-resolution scanning electrochemical cell microscopy (SECCM). The research reveals the spatially heterogeneous charge transfer activity of ITO surfaces and measures a significantly higher charge transfer rate at the nanoscale compared to the macroscale.

ANALYTICAL CHEMISTRY (2022)

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Article Chemistry, Analytical

Decoupling Through-Tip Illumination from Scanning in Nanoscale Photo-SECM

Gaukhar Askarova et al.

Summary: The use of scanning electrochemical microscopy (SECM) for nanoscale imaging of photoelectrochemical processes at semiconductor surfaces has been demonstrated recently. An improved experimental setup was developed to decouple the tip from the optical fiber and deliver light to the back of the tip capillary using a complex lens system, resulting in improved quality of approach curves and photo-SECM images.

ANALYTICAL CHEMISTRY (2022)

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Article Chemistry, Multidisciplinary

Correlative Electrochemical Microscopy for the Elucidation of the Local Ionic and Electronic Properties of the Solid Electrolyte Interphase in Li-Ion Batteries

Carla S. Santos et al.

Summary: The solid-electrolyte interphase (SEI) provides a protective layer in lithium-ion batteries, preventing degradation of the electrolyte at the anode. This study used scanning electrochemical microscopy (SECM) to quantitatively assess the local electronic and ionic properties of SEI in Li-ion batteries, and found that the formation conditions and electrolyte type have a significant impact on its conductivity.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2022)

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Article Chemistry, Physical

High throughput screening driven discovery of Mn5Co10Fe30Ni55Ox as electrocatalyst for water oxidation and electrospinning synthesis

Teng Zhang et al.

Summary: A high-throughput experimental scheme is used to search for effective OER oxide electrocatalysts, and a material library of Mn-Co-Fe-Ni oxide is rapidly prepared and screened for OER activity. The composition of Mn5Co10Fe30Ni55Ox exhibits the highest catalytic activity, and a nanowire catalyst of the corresponding composition achieves low overpotential and a Tafel slope.

APPLIED SURFACE SCIENCE (2022)

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Article Chemistry, Physical

Calibrating SECCM measurements by means of a nanoelectrode ruler. The intrinsic oxygen reduction activity of PtNi catalyst nanoparticles

Emmanuel Batsa Tetteh et al.

Summary: SECCM is used to determine the intrinsic catalytic activity of single electrocatalyst particles, but may not be suitable for very small catalyst nanoparticles. A ruler method is introduced by researchers, using a carbon nanoelectrode decorated with a countable number of catalyst particles, to convert the activity measured by SECCM into the intrinsic catalytic activity of a certain number of catalyst nanoparticles.

NANO RESEARCH (2022)

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Article Chemistry, Physical

Photo-Responsive Doped 3D-Printed Copper Electrodes for Water Splitting: Refractory One-Pot Doping Dramatically Enhances the Performance

Christian Iffelsberger et al.

Summary: The researchers successfully doped FDM-printed copper electrodes with metal oxide crystals, resulting in significantly enhanced photoelectrochemical properties. They also used scanning photoelectrochemical microscopy to analyze the spatial activity of electrochemical and photoelectrochemical reactions.

JOURNAL OF PHYSICAL CHEMISTRY C (2022)

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Article Multidisciplinary Sciences

Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia

Wenhui He et al.

Summary: In this study, a design concept of tandem catalysts was proposed to achieve cascade conversion of waste nitrate to valuable ammonia using different transition metal phases. By transforming Cu-Co binary sulfides into Cu/CuOx and Co/CoO phases, efficient NH3 synthesis was achieved. The tandem catalyst system exhibited high Faradaic efficiency and NH3 yield rate in the presence of waste nitrate, and surpassed previous studies in terms of energy efficiency.

NATURE COMMUNICATIONS (2022)

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Review Nanoscience & Nanotechnology

Oxygen Evolution Reaction in Energy Conversion and Storage: Design Strategies Under and Beyond the Energy Scaling Relationship

Jiangtian Li

Summary: This paper comprehensively reviews the importance of the oxygen evolution reaction in energy conversion and storage devices, as well as the challenges and opportunities for OER catalysts. It focuses on the development and understanding of quantitative structure-activity relationships and summarizes the cutting-edge research frontiers for designing efficient catalysts and overcoming the scaling relationship.

NANO-MICRO LETTERS (2022)

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Review Chemistry, Multidisciplinary

Rational Design of Better Hydrogen Evolution Electrocatalysts for Water Splitting: A Review

Fan Liu et al.

Summary: This review introduces the design principles of hydrogen evolution reaction (HER) electrocatalysts, including thermodynamics, kinetics, and structural descriptors. It also discusses the reasonable design, preparation, mechanistic understanding, and performance enhancement of electrocatalysts. Furthermore, it briefly discusses recent advancements in the electrocatalytic water splitting technology and proposes the challenges and perspectives in developing highly efficient hydrogen evolution electrocatalysts.

ADVANCED SCIENCE (2022)

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Review Chemistry, Physical

Probing the reactive intermediate species generated during electrocatalysis by scanning electrochemical microscopy

Jean-Marc Noel et al.

Summary: This review presents recent strategies using local electrochemical probes to study the formation and reactivity of reactive intermediate species at the nanometer scale, with emphasis on the contributions of numerical simulation in obtaining quantitative information.

CURRENT OPINION IN ELECTROCHEMISTRY (2022)

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Article Materials Science, Multidisciplinary

Insight into the Effect of Metal Cations in the Electrolyte on Performance for Electrocatalytic CO2 Reduction Reaction

Junjun Li et al.

ENERGY & ENVIRONMENTAL MATERIALS (2022)

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Article Chemistry, Multidisciplinary

Interfaces Decrease the Alkaline Hydrogen-Evolution Kinetics Energy Barrier on NiCoP/Ti3C2TX MXene

Hua-Jie Niu et al.

Summary: Heterointerfaces can adjust the adsorption energy and decrease the kinetics energy barrier. The interface between NiCoP and MXene effectively reduces the energy barrier for alkaline hydrogen evolution reaction (HER) by 16.0-22.1%. In addition, the photothermal effect of MXenes can raise the catalyst temperature for energy savings.

ACS NANO (2022)

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Review Chemistry, Physical

Platinum-Rare Earth Alloy Electrocatalysts for the Oxygen Reduction Reaction: A Brief Overview

Carlos A. Campos-Roldan et al.

Summary: This review summarizes and discusses the latest advances on Pt-REM alloy electrocatalysts and their implementation in PEMFCs. It is of great significance for the synthesis, design, and performance goals of novel Pt-REM alloys.

CHEMCATCHEM (2022)

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Article Chemistry, Physical

Electrochemical Detection of Isolated Nanoscale Defects in 2D Transition Metal Dichalcogenides

Marc Brunet Cabre et al.

Summary: This study demonstrates that defects at nanometer and sub-nanometer scales in two-dimensional transition metal dichalcogenides can be detected electrochemically using scanning electrochemical cell microscopy (SECCM). By detecting anomalous electrochemical responses on mechanically exfoliated MoS2, the researchers found that these defects display faster electrochemical kinetics compared to the surrounding sample points. The analysis suggests that the defects are disk-shaped defects or one-dimensional defects with nanometer to sub-nanometer widths. This technique allows for the detection of features below the optical diffraction limit without the need for high-resolution electron microscopy or scanning tunneling microscopy.

JOURNAL OF PHYSICAL CHEMISTRY C (2022)

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Article Chemistry, Multidisciplinary

Unraveling the Structural Sensitivity of CO2 Electroreduction at Facet-Defined Nanocrystals via Correlative Single-Entity and Macroelectrode Measurements

Soojin Jeong et al.

Summary: The conversion of CO2 into value-added products is important for storing energy from intermittent renewable sources. This study investigates the electrocatalytic response of individual gold nanocrystals with different facet definitions for CO2 reduction reaction (CO2RR). It finds that {110}-terminated gold rhombohedra show superior activity and selectivity compared to {111}-terminated octahedra and high-index {310}-terminated truncated ditetragonal prisms.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

Electroprecipitation of Nanometer-Thick Films of Ln(OH)3 [Ln = La, Ce, and Lu] at Pt Microelectrodes and Their Effect on Electron-Transfer Reactions

Pavel Majumdar et al.

Summary: This study investigates the deposition of nanometer-thick Ln(OH)(3) films and their effect on electron-transfer reactions, both outer-sphere and inner-sphere. The results show that the film thickness influences the transport-limited current of outer-sphere reactions, and the degree of blockage depends on the redox species. The study also demonstrates the control of La(OH)(3) film thickness by anodic dissolution and the role of La3+ in reducing the supersaturation of dissolved H-2 needed for stable nanobubble nucleation.

LANGMUIR (2022)

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Article Chemistry, Multidisciplinary

Thousand-fold increase in O2 electroreduction rates with conductive MOFs

Ruperto G. Mariano et al.

Summary: Molecular materials have been found to have low electrocatalytic activity, possibly due to limitations in O2 transport. Through experiments, it was discovered that the actual electrocatalytic activity of a 2D conductive MOF material was underestimated by at least three orders of magnitude. When this material is supported on a gas diffusion electrode, it can achieve high ORR activity and electrosynthesis rates. Precise control over multiscale mass transport can enable high-current-density electrocatalysis in molecular materials.

ACS CENTRAL SCIENCE (2022)

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Article Engineering, Environmental

Photoelectrolysis of TiO2 is highly localized and the selectivity is affected by the light

Christian Iffelsberger et al.

Summary: Photoelectrochemistry, combining the advantages of electrochemical and photochemical processes, is a key area for sustainable prosperity. The study shows that the activity and selectivity of TiO2 photoelectrocatalyst are highly localized and illumination dramatically changes the selectivity in electrolysis reactions. This implies that light can be used to control the selectivity, greatly impacting the optimization of photoelectrocatalysts.

CHEMICAL ENGINEERING JOURNAL (2022)

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Article Chemistry, Analytical

Voltammetric Mapping of Hydrogen Evolution Reaction on Pt Locally via Scanning Electrochemical Cell Microscopy

Yufei Wang et al.

Summary: The advancement in nanoscale electrochemical tools has provided the opportunity to better understand heterogeneity at electrochemical interfaces, with SECCM increasingly used to reveal local kinetics and active site distribution in electrocatalysis. A scanning mode combining advantages of hopping and constant-contact scan has been revisited, resulting in faster voltammetric mapping.

ACS MEASUREMENT SCIENCE AU (2022)

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Article Chemistry, Physical

Tracking heterogeneous structural motifs and the redox behaviour of copper-zinc nanocatalysts for the electrocatalytic CO2 reduction using operando time resolved spectroscopy and machine learning

Martina Ruescher et al.

Summary: Copper-based catalysts are widely used for the electrocatalytic CO2 reduction reaction (CO2RR) to convert CO2 into valuable industrial chemicals. Bimetallic materials, such as ZnO/Cu2O nanocubes, show promising catalytic performance for CO2RR. In this study, operando spectroscopy and data analysis were used to investigate the chemical and structural changes of the catalysts under CO2RR conditions. It was found that the addition of Zn affects the kinetics of subsurface processes, while the Cu surface layer remains unchanged. The presence of Zn stabilizes cationic Cu(i) species and increases the selectivity towards C2+ products, while Zn-rich alloy phases promote the formation of CO and the parasitic hydrogen evolution reaction.

CATALYSIS SCIENCE & TECHNOLOGY (2022)

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Review Chemistry, Multidisciplinary

In situ/operando analysis of surface reconstruction of transition metal-based oxygen evolution electrocatalysts

Shengmei Chen et al.

Summary: This article reviews the progress in surface reconstruction and active species identification of transition metal-based electrocatalysts, and highlights the importance of in situ/operando techniques in revealing catalytic mechanisms and identifying new active species.

CELL REPORTS PHYSICAL SCIENCE (2022)

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Article Chemistry, Multidisciplinary

Visualization and Quantification of Electrochemical H2 Bubble Nucleation at Pt, Au, and MoS2 Substrates

Yulong Liu et al.

Summary: The study quantitatively investigated individual gas bubble nucleation on different electrode substrates using scanning electrochemical cell microscopy (SECCM) with a single channel pipet, revealing the nucleation and growth process of bubbles.

ACS SENSORS (2021)

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Article Chemistry, Multidisciplinary

Surface Interrogation of Electrodeposited MnOx and CaMnO3 Perovskites by Scanning Electrochemical Microscopy: Probing Active Sites and Kinetics for the Oxygen Evolution Reaction

Zhaoyu Jin et al.

Summary: Surface interrogation scanning electrochemical microscopy (SI-SECM) was used to investigate the manganese oxidation state in two electrodeposited manganese-based electrocatalysts, revealing differences in Mn-III and Mn-IV species quantities in MnOx and CaMnO3 under different potentials, as well as the presence of a Mn-V species during the oxygen evolution reaction (OER). Time-delay titration of Mn-V showed that MnOx exhibited two types of active sites with different OER reaction rates, while CaMnO3 only displayed one kinetic behavior with a faster reaction rate.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Review Chemistry, Multidisciplinary

In Situ/Operando Electrocatalyst Characterization by X-ray Absorption Spectroscopy

Janis Timoshenko et al.

Summary: X-ray absorption spectroscopy (XAS) is a crucial method for investigating the structure and composition of heterogeneous catalysts, revealing the nature of active sites and establishing links between structural motifs, local electronic structure, and catalytic properties. Recent advancements in instrumentation and data analysis approaches for deciphering X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectra have been discussed, with emphasis on applications in the field of heterogeneous catalysis, particularly in electrocatalysis.

CHEMICAL REVIEWS (2021)

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Review Chemistry, Multidisciplinary

Oxygen-Deficient Cobalt-Based Oxides for Electrocatalytic Water Splitting

Ahmed Badreldin et al.

Summary: Recent research interest has been focused on anionic point defect engineering of electrocatalytic surfaces, particularly in cobalt-based TMOs. Oxygen vacancy modulation shows promise in improving electrocatalytic activities and surface chemistry, offering potential for designing novel materials surpassing noble metal-based electrocatalysts.

CHEMSUSCHEM (2021)

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Article Microscopy

Release of insulin granules by simultaneous, high-speed correlative SICM-FCM

J. Bednarska et al.

Summary: The study applied SICM-FCM to investigate the exocytosis of insulin granules from the top surface of pancreatic beta-cells, providing insights into the topographical changes associated with physiologically induced release of insulin DCVs. This allowed for a direct observation of the kinetics of full fusion of insulin vesicles and subsequent solubilization of released insulin crystals.

JOURNAL OF MICROSCOPY (2021)

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Article Chemistry, Physical

In Situ Quantification of the Local Electrocatalytic Activity via Electrochemical Scanning Tunneling Microscopy

Richard W. Haid et al.

Summary: The EC-STM method combines surface reaction control and nanoscale imaging, allowing for the identification of active sites and quantitative information about their activity, which plays a crucial role in improving catalyst design and comparing local reactivity.

SMALL METHODS (2021)

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Article Chemistry, Analytical

Characterization of the Depth of Discharge-Dependent Charge Transfer Resistance of a Single LiFePO4 Particle

Takahiko Yamamoto et al.

Summary: The research focuses on the impact of depth of discharge (DOD) on the charge/discharge performance of lithium-ion secondary batteries, using scanning electrochemical cell microscopy (SECCM) to detect the charge transfer resistance at the solid-liquid interface.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Transparent Ultramicroelectrodes for Studying Interfacial Charge-Transfer Kinetics of Photoelectrochemical Water Oxidation at TiO2 Nanorods with Scanning Electrochemical Microscopy

Xiao Li et al.

Summary: The study introduces a new transparent UME-SECM method for investigating semiconductor PEC activities, capable of quantifying the interfacial charge-transfer rates and photocatalytic water oxidation reactions. This method provides insights into potential-dependent PEC water oxidation reaction mechanisms and quantitative analysis of photocurrent contributions.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Scanning Electrochemical Cell Microscopy Platform with Local Electrochemical Impedance Spectroscopy

Lei Cheng et al.

Summary: High-spatial-resolution local electrochemical impedance spectroscopy (LEIS) was achieved using scanning electrochemical cell microscopy (SECCM-LEIS), with a spatial resolution of approximately 180 nm. The stability and reliability of this platform were confirmed through long-term tests and Kramers-Kronig transformation. This technology revealed larger electric double-layer capacitance and smaller interfacial resistance at the edges of N-doped reduced graphene oxide compared to the planar surface, suggesting high electrochemical activity at the edges.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Multidisciplinary

Structural Dynamics of Ultrathin Cobalt Oxide Nanoislands under Potential Control

Corinna Stumm et al.

Summary: This study investigates the structural dynamics and stability of cobalt oxide on Au(111) under different potentials, revealing different properties and behaviors at various potential ranges.

ADVANCED FUNCTIONAL MATERIALS (2021)

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Review Chemistry, Multidisciplinary

Scanning Ion Conductance Microscopy

Cheng Zhu et al.

Summary: Scanning ion conductance microscopy (SICM) is a versatile tool for studying interfaces in biology and materials science, particularly in biophysical and electrochemical measurements. The heart of SICM is a nanometer-scale electrolyte filled glass pipette serving as a scanning probe, allowing for recording of surface topography at micro- and nanoscale levels. Hybridizing SICM with coincident characterization techniques like optical microscopy and faradaic electrodes has made it a powerful tool for nanoscale chemical measurement in various applications.

CHEMICAL REVIEWS (2021)

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Review Chemistry, Multidisciplinary

Research Progress of Oxygen Evolution Reaction Catalysts for Electrochemical Water Splitting

Yanying Liu et al.

Summary: This review summarizes the research progress of anode OER catalysts for hydrogen production by electrochemical water splitting in recent years, focusing on exploring new and efficient non-noble metal catalytic systems. The categories include transition metal-based compounds, carbonaceous materials, and transition metal-based metal-organic frameworks. The challenges and future development of the OER process of water splitting are also discussed.

CHEMSUSCHEM (2021)

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Article Energy & Fuels

Review of the Hydrogen Evolution Reaction-A Basic Approach

Thomas B. Ferriday et al.

Summary: This paper summarizes the latest efforts in alkaline HER electrocatalyst design, focusing on three main strategies inspired by theories describing the pH-dependence of HER activity. The authors predict that screening materials based on their hydrogen, hydroxide, and water binding energies, and utilizing different optimization parameters, could lead to the development of active and stable HER catalyst materials, advancing the current status of alkaline water electrolysis as an energy storage option.

ENERGIES (2021)

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Review Physics, Condensed Matter

In situ and operando electron microscopy in heterogeneous catalysis-insights into multi-scale chemical dynamics

See Wee Chee et al.

Summary: This article reviews the latest technology of in situ and operando electron microscopy (EM) studies of heterogeneous catalysts in gas and liquid environments during reactions. The importance of heterogeneous catalysts in efficient production of chemicals/fuels on an industrial scale and their role in ensuring a sustainable future for society is highlighted. The challenges and future directions in experimentally applying these techniques, as well as the critical discussion of spatially-resolved operando measurements and available experimental setups, are addressed.

JOURNAL OF PHYSICS-CONDENSED MATTER (2021)

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Review Energy & Fuels

M-N-C-based single-atom catalysts for H2, O2 & CO2 electrocatalysis: activity descriptors, active sites identification, challenges and prospects

Anuj Kumar et al.

Summary: This review highlights the application of single-atom catalysts in electrocatalytic activation of small molecules, focusing on activity descriptors, recent advancements, characterization techniques, design methods, challenges, and future prospects for metal-nitrogen-carbon based SACs.

FUEL (2021)

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Review Chemistry, Physical

Operando Methods in Electrocatalysis

Yao Yang et al.

Summary: Electrocatalysis is crucial for advancing renewable energy technologies, and understanding the structure and reaction mechanisms of electrocatalysts at electrode-electrolyte interfaces is fundamental. In situ and operando techniques, such as operando synchrotron-based X-ray techniques and in situ atomic-scale scanning transmission electron microscopy, provide valuable insights into the interfacial structural and compositional changes under reaction conditions, aiding in the study of charge transfer kinetics and reaction mechanisms. The continuous development of these techniques will contribute significantly to establishing structure/composition-reactivity correlations of electrocatalysts at unprecedented atomic-scale and molecular levels under realistic, real-time reaction conditions.

ACS CATALYSIS (2021)

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Article Chemistry, Analytical

Unveiling the contribution of the reproductive system of individual Caenorhabditis elegans on oxygen consumption by single-point scanning electrochemical microscopy measurements

Carla S. Santos et al.

Summary: By using scanning electrochemical microscopy (SECM) to measure the localized oxygen consumption rates (OCRs) in different regions of single adult Caenorhabditis elegans individuals, this study revealed marked heterogeneity of OCR along the worm, with high respiration rates at the reproductive system region. Through a self-referencing approach and genetic/pharmacological methods, SECM measurements indicate that viable eggs in the reproductive system are the main contributors to the total oxygen consumption of adult Caenorhabditis elegans, providing new insights into tissue-specific metabolic analyses and toxicity evaluation within single organisms.

ANALYTICA CHIMICA ACTA (2021)

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Article Chemistry, Multidisciplinary

Direct Probing of the Oxygen Evolution Reaction at Single NiFe2O4 Nanocrystal Superparticles with Tunable Structures

Xiaoxi Lu et al.

Summary: The study directly measures the oxygen evolution reaction in single self-assembled superparticles and shows that the NiFe2O4 superparticles' TOF depends on their diameter, while the incorporation of Au nanocrystals significantly increases the TOF, leveling off after a certain concentration. This research provides insights into the intrinsic structure-activity relationship of individual nanocrystal superlattices with tunable structures through direct electrochemical analysis.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Probing the Local Reaction Environment During High Turnover Carbon Dioxide Reduction with Ag-Based Gas Diffusion Electrodes

Stefan Dieckhoefer et al.

Summary: This study investigates the impact of electrochemical reactions on the electrode microenvironment, specifically focusing on the production of OH- and the consumption of water. Experimental results show that high turnover of HER/CO2RR at a gas diffusion electrode can modulate the alkalinity of the local electrolyte, affecting the reaction selectivity.

CHEMISTRY-A EUROPEAN JOURNAL (2021)

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Article Electrochemistry

Operando analysis of the electrosynthesis of Ag2O nanocubes by scanning electrochemical microscopy

Mathias Miranda Vieira et al.

Summary: The study utilizes scanning electrochemical microscopy to investigate the electrosynthesis mechanism of metal oxide nanoparticles, successfully synthesizing Ag2O nanocubes and revealing insights into their growth mechanism through dynamic analysis of reductive electrochemical impacts.

ELECTROCHEMISTRY COMMUNICATIONS (2021)

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Article Chemistry, Physical

The Potential of Zero Charge and the Electrochemical Interface Structure of Cu(111) in Alkaline Solutions

Andrea Auer et al.

Summary: Copper (Cu) exhibits structural dynamics and atomic density decrease at its potential of zero free charge (pzfc) in alkaline electrolyte, with a shift towards more positive potentials per decreasing pH unit. At higher potentials, full reconstruction and electric field dependent OH adsorption occurs, leading to a decrease in the atomic density of the first Cu layer.

JOURNAL OF PHYSICAL CHEMISTRY C (2021)

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Article Chemistry, Multidisciplinary

Emergence of Potential-Controlled Cu-Nanocuboids and Graphene-Covered Cu-Nanocuboids under Operando CO2 Electroreduction

Thanh Hai Phan et al.

Summary: Research has shown that Cu surfaces can reconstruct into Cu nanocuboids during the electroreduction of CO2, with the size of these structures being controllable by the applied potential and synthesis time. This finding presents a novel strategy for enhancing the long-term stability of Cu-based catalysts.

NANO LETTERS (2021)

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Article Chemistry, Physical

Fictitious phase separation in Li layered oxides driven by electro-autocatalysis

Jungjin Park et al.

Summary: Layered oxides electrodes in lithium-ion batteries are designed to be cycled under conditions avoiding phase transitions, but phase separation during delithiation has been observed, which is shown to be a dynamical artefact occurring in a many-particle system driven by autocatalytic electrochemical reactions.

NATURE MATERIALS (2021)

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Article Chemistry, Physical

Acceleration of Electrochemical CO2 Reduction to Formate at the Sn/Reduced Graphene Oxide Interface

Takuya Tsujiguchi et al.

Summary: Reduced graphene oxide (rGO) plays a crucial role in enhancing the CO2 adsorption ability of Sn/rGO composites, leading to a 4-fold increase compared to bare Sn catalysts. The oxidized functional groups of rGO provide adsorption sites for CO2 towards the adjacent Sn surface, promoting the production of formate while suppressing the formation of CO* near the surface. Experimental results show that CO2 reduction is accelerated at the interface of Sn/rGO, improving the Faradaic efficiency by 1.8 times compared to bare Sn catalysts.

ACS CATALYSIS (2021)

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Review Chemistry, Physical

Why nanoelectrochemistry is necessary in battery research?

Edgar Ventosa

Summary: The active materials are crucial for batteries and nanoelectrochemistry plays a significant role in battery research. Nanoelectrochemistry can be used for determining intrinsic kinetics and understanding the relationship between particle structure and electrochemical activity.

CURRENT OPINION IN ELECTROCHEMISTRY (2021)

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Article Chemistry, Analytical

Scanning Electrochemical and Photoelectrochemical Microscopy on Finder Grids: Toward Correlative Multitechnique Imaging of Surfaces

Sujoy Sarkar et al.

Summary: Scanning electrochemical microscopy (SECM) is a powerful technique for mapping surface reactivity and investigating heterogeneous processes on the nanoscale. By correlating SECM images with atomic scale structural information obtained by transmission electron microscopy (TEM), one can elucidate the nature of active sites and understand the origins of heterogeneous surface reactivity.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Nanoscale Reactivity Mapping of a Single-Crystal Boron-Doped Diamond Particle

Tomohiro Ando et al.

Summary: The study investigates the electrochemical properties of boron-doped diamond single crystal microparticles on different crystal faces, revealing faster electron transfer on the H-terminated (111) surface than on the H-terminated (100) surface, as well as significant differences between the O-terminated (100) face and the H-terminated (100) face. These differences are attributed to the removal of the H-surface conductivity layer and a potential-dependent density of states caused by boron doping.

ANALYTICAL CHEMISTRY (2021)

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Article Electrochemistry

Combining Nanoconfinement in Ag Core/Porous Cu Shell Nanoparticles with Gas Diffusion Electrodes for Improved Electrocatalytic Carbon Dioxide Reduction

Joao R. C. Junqueira et al.

Summary: Bimetallic silver-copper electrocatalysts combined with gas diffusion electrodes facilitate CO2RR under enhanced mass transport conditions, leading to increased formation of C2+ products and a variation in product distribution.

CHEMELECTROCHEM (2021)

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Article Electrochemistry

Scanning Electrochemical Cell Microscopy in a Glovebox: Structure-Activity Correlations in the Early Stages of Solid-Electrolyte Interphase Formation on Graphite

Daniel Martin-Yerga et al.

Summary: This study uses scanning electrochemical cell microscopy (SECCM) to investigate the formation of solid-electrolyte interphase (SEI) on graphite surfaces in Li-ion batteries. The presence of step edges on the surface promotes the formation of a more passivating SEI. The study also shows that an unstable SEI can be detected under fast formation conditions, while a slow formation rate leads to the growth of an increasingly passivating SEI.

CHEMELECTROCHEM (2021)

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Article Chemistry, Physical

Assessment of active areas for the oxygen evolution reaction on an amorphous iridium oxide surface

Regina M. Kluge et al.

Summary: Efficient production of hydrogen from water using electrocatalysis is hindered by slow kinetics of the oxygen evolution reaction (OER). Iridium (Ir) oxide catalysts in polymer electrolyte membrane electrolysers show promising activity and stability, but the structure-activity relations are not well understood. Noise in electrochemical scanning tunnelling microscopy (n-ECSTM) measurements on amorphous iridium oxide surfaces suggest little structure-sensitivity in OER, unlike in other catalytic reactions.

JOURNAL OF CATALYSIS (2021)

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Article Chemistry, Physical

Operando visualization of the hydrogen evolution reaction with atomic-scale precision at different metal-graphene interfaces

Tomasz Kosmala et al.

Summary: The study found that thin iron films covered with monolayer graphene exhibit superior catalytic activity for the hydrogen evolution reaction compared to platinum. By evaluating noise in the tunnelling current of electrochemical scanning tunnelling microscopy, researchers discovered the exceptional activity of single iron atoms trapped within carbon vacancies and curved graphene areas on step edges. Density functional theory calculations further confirmed this sequence of activity.

NATURE CATALYSIS (2021)

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Article Chemistry, Physical

Microstructural origin of locally enhanced CO2 electroreduction activity on gold

Ruperto G. Mariano et al.

Summary: The study demonstrates that understanding the relationship between surface catalytic activity and bulk defects, such as dislocations, could lead to improvements in catalytic properties, particularly in CO2 electroreduction. Intentionally introducing dislocations into materials appears to be a promising strategy for enhancing catalytic activity.

NATURE MATERIALS (2021)

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Article Chemistry, Physical

High Spatial Resolution Electrochemical Microscopic Observation of Enhanced Charging under Bias at Active Sites of N-rGO

Rong Jin et al.

Summary: The recent breakthrough demonstrates that the activation free energy decreases with the oxidative charge stored at the catalyst, shedding light on the balance between chemistry and bias in electrocatalysis. By isolating non-faradic and faradic currents in SECCM imaging, researchers successfully mapped charge accumulation and electrochemical activity with high resolution. The observation of enhanced charging under bias at active sites of N-doped graphene oxide in the hydrogen evolution reaction provides direct evidence to support the proposed mechanism, presenting valuable insights for the design of efficient HER catalysts.

ACS APPLIED ENERGY MATERIALS (2021)

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Article Nanoscience & Nanotechnology

Conductive Polymer Intercalation Tunes Charge Transfer and Sorption-Desorption Properties of LDH Enabling Efficient Alkaline Water Oxidation

Min Ju et al.

Summary: This study presents a method to tune the charge transfer and sorption-desorption properties of a catalyst by intercalating a conductive polymer into a layered double hydroxide, resulting in improved catalytic performance for the oxygen evolution reaction. In situ scanning electrochemical microscopy revealed that the hybrid catalyst exhibited a higher catalytic current density at the subnanometer scale compared to the bare catalyst.

ACS APPLIED MATERIALS & INTERFACES (2021)

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Article Nanoscience & Nanotechnology

Catalyst Formation and In Operando Monitoring of the Electrocatalytic Activity in Flow Reactors

Christian Iffelsberger et al.

Summary: Flow reactors play a crucial role in chemical synthesis, electrochemical reactions, and wastewater treatment, with catalyst activity spatial analysis being important for optimization. The use of scanning electrochemical microscopy allows for localized tracking of catalytic activity with high resolution.

ACS APPLIED MATERIALS & INTERFACES (2021)

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Article Chemistry, Analytical

Scanning Ion Conductance Microscopy: Surface Charge Effects on Electroosmotic Flow Delivery from a Nanopipette

James Teahan et al.

Summary: Scanning ion conductance microscopy (SICM) is a powerful technique for studying interfacial properties and processes. This study investigates the potential-controlled delivery of uncharged electroactive molecules from an SICM tip to a working electrode substrate, revealing the strong dependence of species delivery on the charge of the substrate surface. The combination of experimental results and finite element method (FEM) simulations provides new insights into mass transport in SICM and its implications for local delivery using nanopipettes.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Ag+ Interference from Ag/AgCl Wire Quasi-Reference Counter Electrode Inducing Corrosion Potential Shift in an Oil-Immersed Scanning Micropipette Contact Method Measurement

Yuanjiao Li et al.

Summary: The commonly used Ag/AgCl wire quasi-reference counter electrode in the quantitative scanning micropipette contact method may leak Ag+ into the electrolyte solution, leading to interference in potential and generation of faradaic current. By using a leak-free Ag/AgCl electrode or increasing the distance between the electrode and micropipette tip droplet, the contamination of Ag+ can be eliminated, allowing accurate measurement of corrosion potentials during oil-immersed scanning micropipette contact method measurements.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

High-Content Label-Free Single-Cell Analysis with a Microfluidic Device Using Programmable Scanning Electrochemical Microscopy

Mi Shi et al.

Summary: A methodology combining P-SECM and an addressable microwell array dramatically shortened the time consumption for topography detection and ALP activity evaluation of single cells compared with traditional SECM imaging. By implementing the dual-mediator-based voltage-switching mode, the platform investigated ALP activity in hundreds of tumor and stromal cells, revealing higher ALP activity in cancer cells and heterogeneous distribution of ALP activity at the single-cell level. This platform holds potential as a high-content screening tool for label-free single-cell analysis with deterministic routing of addressed cells on a scalable microfluidic device.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Effect of a Cocatalyst on a Photoanode in Water Splitting: A Study of Scanning Electrochemical Microscopy

Zehui Yu et al.

Summary: Studies have shown that surface modification of BiVO4 with a cocatalyst like NiFe layered double hydroxide significantly enhances the PEC water splitting performance. Analysis using scanning electrochemical microscopy (SECM) reveals that NiFe-LDH suppresses electron back transfer, reducing surface recombination and improving water splitting efficiency.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Surface-Enhanced Raman Spectroscopy-Scanning Electrochemical Microscopy: Observation of Real-Time Surface pH Perturbations

Kendrich O. Hatfield et al.

Summary: SERS-SECM is a multimodal tool that can sensitively interrogate and trigger chemical/electrochemical dynamic surface phenomena in real time, providing insight on heterogeneous and homogeneous reactivity at electrochemical interfaces.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Numerical Correction of In Situ AFM-SECM Measurements

Alex Mirabal et al.

Summary: Research demonstrates that atomic force microscopy-based SECM technology can measure concentration profiles around active surfaces, but the presence of the tip can distort these profiles, affecting the chemical behavior at the catalytic surface. By inversely fitting data, kinetic and geometric parameters characterizing the tip effect can be derived, and the tip effects can be removed in the model.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Electrochemical Visualization of Gas Bubbles on Superaerophobic Electrodes Using Scanning Electrochemical Cell Microscopy

Yulong Liu et al.

Summary: In this study, the individual gas bubble nucleation and dynamics on nanoscale electrodes were investigated using scanning electrochemical cell microscopy (SECCM). The nanostructured catalyst surface showed significantly less supersaturation for gas bubble nucleation and a notable increase of bubble detachment compared to its flat counterpart. The results suggest that deliberate microstructure design on a catalyst surface is a promising strategy for improving electrocatalytic gas evolution in terms of both bubble nucleation and elimination.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Analytical

Simultaneous Intelligent Imaging of Nanoscale Reactivity and Topography by Scanning Electrochemical Microscopy

Dylan T. Jantz et al.

Summary: The study developed an intelligent nanoscale SECM mode that can simultaneously obtain separate reactivity and topography images of non-flat substrates with reactive and inert regions.

ANALYTICAL CHEMISTRY (2021)

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Article Chemistry, Multidisciplinary

A Metal-Organic Framework derived CuxOyCz Catalyst for Electrochemical CO2 Reduction and Impact of Local pH Change

Nivedita Sikdar et al.

Summary: Researchers have developed a series of CuxOyCz nanostructured electrocatalysts derived from a Cu-based MOF using porous self-sacrificial templates. By blending these catalysts with polytetrafluoroethylene (PTFE) on gas diffusion electrodes (GDEs), they were able to suppress competitive hydrogen evolution reactions and achieve a Faradaic efficiency of approximately 54% for C2+ products at -80 mA cm(-2). The increase in the OH-/H2O activity ratio due to locally generated OH- ions at higher current densities was observed regardless of the amount of PTFE.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Single Particle Nanoelectrochemistry Reveals the Catalytic Oxygen Evolution Reaction Activity of Co3O4 Nanocubes

Thomas Quast et al.

Summary: Co3O4 nanocubes were evaluated for their intrinsic electrocatalytic activity towards the oxygen evolution reaction using single-entity electrochemistry techniques. The study showed high efficiency and stability in OER, with combining multiple electrochemical methods allowing for in-depth analysis on the structure-activity relationship of individual nanoparticles.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Electrochemistry

In-situ detection of active sites for carbon-based bifunctional oxygen reduction and evolution catalysis

Richard W. Haid et al.

Summary: Carbon-based electrodes are increasingly popular as electrocatalysts for fuel cells and metal-air batteries due to their availability and versatility. This study investigated the surface behavior of highly oriented pyrolytic graphite under both ORR and OER conditions in 0.1 M KOH. By using noise analysis in electrochemical scanning tunneling microscopy, active sites were monitored and compared with nanoscale resolution. The results showed that step sites and defects are active for both ORR and OER, while terraces sites are largely inactive and only become involved in the OER at higher potentials. Surface degradation was evaluated during the operation, with no clear evidence of surface destruction observed in the experiments.

ELECTROCHIMICA ACTA (2021)

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Article Electrochemistry

Bifunctional oxygen electrocatalysis at Co-B,N,S-graphene composite investigated by scanning electrochemical microscopy at variable temperatures and its application in Zn-air battery

Zhenjie Lu et al.

Summary: The study reported a cobalt compound oxygen electrocatalyst supported on doped graphene, showing excellent catalytic activity and long-term stability. Using an improved SECM technique, the local reactivity of the material can be studied at different temperatures. The Zn-air battery constructed based on this material exhibited a minimal charge/discharge voltage gap and high voltage efficiency.

ELECTROCHIMICA ACTA (2021)

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Article Electrochemistry

Differentiating electrochemically active regions of indium tin oxide electrodes for hydrogen evolution and reductive decomposition reactions. An in situ optical microscopy approach

Paolo Ciocci et al.

Summary: The electrochemical behavior of ITO during the hydrogen evolution reaction was investigated, revealing the formation of H-2 nanobubbles and In(0) nanoparticles, as well as the impact of intrinsic variation of ITO conductivity on the formation of these two species.

ELECTROCHIMICA ACTA (2021)

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Article Chemistry, Physical

Effect of Nonuniform Mass Transport on Nanobubble Nucleation at Individual Pt Nanoparticles

Nicholas S. Georgescu et al.

Summary: Understanding the nucleation and growth of nanoscopic H-2 bubbles on individual Pt nanoparticles through the hydrogen evolution reaction has been demonstrated using scanning electrochemical cell microscopy. The nonuniform distribution of electrogenerated H-2 at the NP/solution interface was observed, with a maximum concentration at the three-phase boundary. A correction factor was established to estimate the H-2 surface concentration required for nucleation, and a decrease in ionic current was measured between the two barrels of the SECCM nanopipette upon bubble formation.

JOURNAL OF PHYSICAL CHEMISTRY C (2021)

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Article Chemistry, Physical

Scanning Electrochemical Impedance Microscopy in Redox-Competition Mode for the Investigation of Antibodies Labelled with Horseradish Peroxidase

Antanas Zinovicius et al.

Summary: Scanning electrochemical microscopy enhanced by electrochemical impedance spectroscopy (SEIM) was employed to study immobilized antibodies labeled with horseradish peroxidase (Ab-HRP), showing that the charge-transfer resistance is a key parameter describing the behavior of HRP catalyzed reactions. The method is suitable for studying catalyzed reactions, evaluating antibody binding, and determining affinity properties.

MATERIALS (2021)

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Review Energy & Fuels

A brief review of electrocatalytic reduction of CO2-Materials, reaction conditions, and devices

Yuhou Pei et al.

Summary: Electrochemical CO2 reduction (ECR) is a promising strategy to address global warming by fixing CO2 in a clean and sustainable manner, but its performance is highly dependent on catalysis systems, reaction conditions, and device configurations. Further research is needed to address these factors for improved ECR efficiency.

ENERGY SCIENCE & ENGINEERING (2021)

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Article Chemistry, Physical

Absence of CO2 electroreduction on copper, gold and silver electrodes without metal cations in solution

Mariana C. O. Monteiro et al.

Summary: The study found that metal cations play a crucial role in stabilizing the CO2 intermediate during the reduction process on gold electrodes. Density functional theory simulations confirmed that partially desolvated metal cations enable the reduction by stabilizing the CO2- intermediate through short-range electrostatic interactions. In conclusion, the positively charged species from the electrolyte are key to stabilizing the crucial reaction intermediate.

NATURE CATALYSIS (2021)

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Review Chemistry, Physical

A comprehensive review on the recent developments in transition metal-based electrocatalysts for oxygen evolution reaction

Ashalatha Vazhayil et al.

Summary: This review summarizes the recent progress in non-noble-metal-based OER electrocatalysts, including the tuning approaches and key factors of various nanostructured materials, and discusses the applications and challenges in this field.

APPLIED SURFACE SCIENCE ADVANCES (2021)

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Article Chemistry, Multidisciplinary

Probing the local activity of CO2 reduction on gold gas diffusion electrodes: effect of the catalyst loading and CO2 pressure

Mariana C. O. Monteiro et al.

Summary: This research evaluates the CO2 reduction activity of GDEs using gold nanoelectrodes, demonstrating that the optimal local catalyst loading depends on the CO2 back pressure.

CHEMICAL SCIENCE (2021)

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Review Chemistry, Physical

Operando toolbox for heterogeneous interface in electrocatalysis

Chang Long et al.

Summary: This paper discusses the importance of interface chemistry in electrocatalysis and the application of the latest operando techniques, aiming to help researchers better choose systems, design experiments, and study mechanisms.

CHEM CATALYSIS (2021)

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Review Chemistry, Physical

Recent advances in electrocatalytic chloride oxidation for chlorine gas production

Yihan Wang et al.

Summary: This article summarizes the recent advances in electrocatalytic chlorine evolution reaction (CER), including history, catalytic mechanism, different types of electrocatalysts, and strategies for improving performance. Future research opportunities in materials design, structure-performance relationships, reactor technical improvements, and application scenarios extension are outlined.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

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Article Chemistry, Multidisciplinary

Directly visualizing carrier transport and recombination at individual defects within 2D semiconductors

Joshua W. Hill et al.

Summary: The novel Carrier Generation-Tip Collection Scanning Electrochemical Cell Microscopy (CG-TC SECCM) technique allows visualization of carrier transport within 2D semiconductors at the single-defect level. Studies on mechanically-exfoliated n-WSe2 nanosheets demonstrated anisotropic hole transport and significant surface charge influence on carrier transport at individual defect sites.

CHEMICAL SCIENCE (2021)

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Article Chemistry, Physical

Monitoring the active sites for the hydrogen evolution reaction at model carbon surfaces

Regina M. Kluge et al.

Summary: Carbon is commonly used as an electrode material in electrochemical energy conversion devices and has recently attracted interest as an environmentally friendly alternative to noble metal catalysts. Research has shown that electrochemical scanning tunnelling microscopy can be utilized to pinpoint the active sites for hydrogen evolution reaction on carbon-based electrode materials. This insight can guide the synthesis of enhanced electrocatalysts by locating the active sites on doped carbon-based materials.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2021)

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Article Chemistry, Multidisciplinary

Nanoscale electrochemistry in a copper/aqueous/oil three-phase system: surface structure-activity-corrosion potential relationships

Enrico Daviddi et al.

Summary: This study utilized SECCM and EBSD techniques to investigate the relationship between surface structure, electrochemical activity, and corrosion susceptibility of polycrystalline Cu. The findings highlight the significant role of high-index orientation grains and microsurface defects in modulating corrosion properties.

CHEMICAL SCIENCE (2021)

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Review Green & Sustainable Science & Technology

Covalent Organic Frameworks for Efficient Energy Electrocatalysis: Rational Design and Progress

Hua Zhang et al.

Summary: Efficient catalysts with precisely designed and predictable structures are highly desired for optimizing performance and understanding the mechanism behind catalytic activity. COFs, as a new class of framework materials, show significant potential as highly efficient electrocatalysts despite being in the early stage of research. Design principles for COFs as efficient electrocatalysts and an in-depth understanding of their catalytic mechanism provide guidance for further exploration of their vast potential.

ADVANCED ENERGY AND SUSTAINABILITY RESEARCH (2021)

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Article Chemistry, Multidisciplinary

Perovskite-Type Oxides La0.6M0.4Ni0.6Cu0.4O3 (M = Ag, Ba, Ce) towards the Oxygen Reduction Reaction (ORR) in Alkaline Medium: Structural Aspects and Electrocatalytic Activity

Alan R. F. Lima et al.

Summary: LANC electrocatalysts synthesized by the Pechini method show excellent catalytic activity towards ORR, with LANC/Carbon displaying the best performance through a pseudo four-electron transfer pathway. The enhanced electrocatalytic activity of LANC is likely due to the presence of Ag phase, improving the synergistic effect between perovskite and carbon.

JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

High-Resolution Electrochemical Mapping of the Hydrogen Evolution Reaction on Transition-Metal Dichalcogenide Nanosheets

Yasufumi Takahashi et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Review Chemistry, Multidisciplinary

Recent Advances in Electrocatalytic Hydrogen Evolution Using Nanoparticles

Jing Zhu et al.

CHEMICAL REVIEWS (2020)

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Article Electrochemistry

Nanoscale electrochemical visualization of grain-dependent anodic iron dissolution from low carbon steel

L. C. Yule et al.

ELECTROCHIMICA ACTA (2020)

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Review Chemistry, Physical

Developments and Perspectives in 3d Transition-Metal-Based Electrocatalysts for Neutral and Near-Neutral Water Electrolysis

Sengeni Anantharaj et al.

ADVANCED ENERGY MATERIALS (2020)

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Article Nanoscience & Nanotechnology

Macroscale and Nanoscale Photoelectrochemical Behavior of p-Type Si(111) Covered by a Single Layer of Graphene or Hexagonal Boron Nitride

Annelise C. Thompson et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

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Article Chemistry, Analytical

Mapping the Potential of Zero Charge and Electrocatalytic Activity of Metal-Electrolyte Interface via a Grain-by-Grain Approach

Yufei Wang et al.

ANALYTICAL CHEMISTRY (2020)

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Article Chemistry, Physical

Nanoscale Variations in the Electrocatalytic Activity of Layered Transition-Metal Dichalcogenides

Binglin Tao et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2020)

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Article Chemistry, Multidisciplinary

Resistive-Pulse Sensing Inside Single Living Cells

Rongrong Pan et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

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Article Chemistry, Multidisciplinary

Probing Single-Particle Electrocatalytic Activity at Facet-Controlled Gold Nanocrystals

Myunghoon Choi et al.

NANO LETTERS (2020)

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Article Multidisciplinary Sciences

Atomically dispersed Pt-N4 sites as efficient and selective electrocatalysts for the chlorine evolution reaction

Taejung Lim et al.

NATURE COMMUNICATIONS (2020)

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Review Chemistry, Physical

Mechanistic Understanding of CO2 Reduction Reaction (CO2RR) Toward Multicarbon Products by Heterogeneous Copper-Based Catalysts

Tanya K. Todorova et al.

ACS CATALYSIS (2020)

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Review Biochemical Research Methods

Nanoelectrochemistry in the study of single-cell signaling

Ran Chen et al.

ANALYTICAL AND BIOANALYTICAL CHEMISTRY (2020)

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Article Chemistry, Analytical

Surface microstructural controls on electrochemical hydrogen absorption at polycrystalline palladium

Lewis C. Yule et al.

JOURNAL OF ELECTROANALYTICAL CHEMISTRY (2020)

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Article Chemistry, Analytical

A study of the electrochemical reactivity of titanium under cathodic polarization by means of combined feedback and redox competition modes of scanning electrochemical microscopy

Abdelilah Asserghine et al.

SENSORS AND ACTUATORS B-CHEMICAL (2020)

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Article Chemistry, Physical

Coulometric Titration of Active Sites at Mesostructured Cobalt Oxide Spinel by Surface Interrogation Mode of Scanning Electrochemical Microscopy

Julian Lorenz et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2020)

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Article Chemistry, Physical

Investigating the Redox Properties of Two-Dimensional MoS2 Using Photoluminescence Spectroelectrochemistry and Scanning Electrochemical Cell Microscopy

Lyndi E. Strange et al.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2020)

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Article Chemistry, Multidisciplinary

Visualization of Hydrogen Evolution at Individual Platinum Nanoparticles at a Buried Interface

Rui Gao et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

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Article Electrochemistry

Solid Electrolyte Interphase Evolution on Lithium Metal Electrodes Followed by Scanning Electrochemical Microscopy Under Realistic Battery Cycling Current Densities

Bastian Krueger et al.

CHEMELECTROCHEM (2020)

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Article Electrochemistry

Determining the Efficiency of Photoelectrode Materials by Coupling Cavity-Microelectrode Tips and Scanning Electrochemical Microscopy

Alberto Visibile et al.

CHEMELECTROCHEM (2020)

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Article Chemistry, Physical

In Situ/Operando Studies for Designing Next-Generation Electrocatalysts

Yanping Zhu et al.

ACS ENERGY LETTERS (2020)

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Review Biochemical Research Methods

Scanning electrochemical microscopy and its potential for studying biofilms and antimicrobial coatings

Giada Caniglia et al.

ANALYTICAL AND BIOANALYTICAL CHEMISTRY (2020)

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Article Chemistry, Analytical

Electrochemical Impedance Measurements in Scanning Ion Conductance Microscopy

Viacheslav Shkirskiy et al.

ANALYTICAL CHEMISTRY (2020)

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Article Chemistry, Analytical

Scanning Electrochemical Cell Microscopy (SECCM) in Aprotic Solvents: Practical Considerations and Applications

Cameron L. Bentley et al.

ANALYTICAL CHEMISTRY (2020)

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Review Chemistry, Multidisciplinary

Electrocatalysis as the Nexus for Sustainable Renewable Energy: The Gordian Knot of Activity, Stability, and Selectivity

Justus Masa et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

In Situ Scanning Tunneling Microscopy of Cobalt-Phthalocyanine-Catalyzed CO2Reduction Reaction

Xiang Wang et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

Probing the Activity of Iron Peroxo Porphyrin Intermediates in the Reaction Layer during the Electrochemical Reductive Activation of O2

Jean-Marc Noel et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

Direct Nanomachining on Semiconductor Wafer By Scanning Electrochemical Microscopy

Lianhuan Han et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Review Chemistry, Physical

Scanning electrochemical cell microscopy: A natural technique for single entity electrochemistry

Oluwasegun J. Wahab et al.

CURRENT OPINION IN ELECTROCHEMISTRY (2020)

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Article Nanoscience & Nanotechnology

Correlating the Local Electrocatalytic Activity of Amorphous Molybdenum Sulfide Thin Films with Microscopic Composition, Structure, and Porosity

Cameron L. Bentley et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

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Article Chemistry, Physical

Locally Engineering and Interrogating the Photoelectrochemical Behavior of Defects in Transition Metal Dichalcogenides

Joshua W. Hill et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2020)

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MODERN PHYSICS LETTERS B (2012)

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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2012)

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Visualization of Chlorine Evolution at Dimensionally Stable Anodes by Means of Scanning Electrochemical Microscopy

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Surface interrogation mode of scanning electrochemical microscopy for oxidation study of adsorbed CO generated from serine on platinum

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Screening of Electrocatalysts for Photoelectrochemical Water Oxidation on W-Doped BiVO4 Photocatalysts by Scanning Electrochemical Microscopy

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Factors in the Metal Doping of BiVO4 for Improved Photoelectrocatalytic Activity as Studied by Scanning Electrochemical Microscopy and First-Principles Density-Functional Calculation

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Imaging Biocatalytic Activity of Enzyme-Polymer Spots by Means of Combined Scanning Electrochemical Microscopy/Electrogenerated Chemiluminescence

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Electrocatalytic Activity of Spots of Electrodeposited Noble-Metal Catalysts on Carbon Nanotubes Modified Glassy Carbon

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Measurement of Ion Currents through Porous Membranes with Scanning Ion Conductance Microscopy

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Hydrogen Peroxide Production in the Oxygen Reduction Reaction at Different Electrocatalysts as Quantified by Scanning Electrochemical Microscopy

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Visualization of the Local Catalytic Activity of Electrodeposited Pt-Ag Catalysts for Oxygen Reduction by means of SECM

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Local Modulation of the Redox State of p-Nitrothiophenol Self-Assembled Monolayers Using the Direct Mode of Scanning Electrochemical Microscopy

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Electrocatalytic reduction of oxygen at electropolymerized films of metalloporphyrins deposited onto multi-walled carbon nanotubes

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Visualization of local electrocatalytic activity of metalloporphyrins towards oxygen reduction by means of redox competition scanning electrochemical microscopy (RC-SECM)

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Electrocatalytic Activity and Stability of Nitrogen-Containing Carbon Nanotubes in the Oxygen Reduction Reaction

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Reaction of Br2 with Adsorbed CO on Pt, Studied by the Surface Interrogation Mode of Scanning Electrochemical Microscopy

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Electrochemistry of Oxygen in Concentrated NaOH Solutions: Solubility, Diffusion Coefficients, and Superoxide Formation

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Article Multidisciplinary Sciences

Loss of T-tubules and other changes to surface topography in ventricular myocytes from failing human and rat heart

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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2009)

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Incorporation of functionalized palladium nanoparticles within ultrathin Nafion films: A nanostructured composite for electrolytic and redox-mediated hydrogen evolution

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CHEMISTRY-A EUROPEAN JOURNAL (2008)

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Scanning electrochemical microscopy for the direct patterning of a gold surface with organic moities derived from iodonium salt

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Topological and electron-transfer properties of glucose oxidase adsorbed on highly oriented pyrolytic graphite electrodes

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Scanning electrochemical microscopy of redox-mediated hydrogen evolution catalyzed by two-dimensional assemblies of palladium nanoparticles

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Supramolecular pattern of fullerene on 2D bimolecular chessboard consisting of bottom-up assembly of porphyrin and phthalocyanine molecules

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Interrogation of Surfaces for the Quantification of Adsorbed Species on Electrodes: Oxygen on Gold and Platinum in Neutral Media

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Electrolyte Gating in Redox-Active Tunneling Junctions-An Electrochemical STM Approach

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Electrodeposited noble metal particles in polyelectrolyte multilayer matrix as electrocatalyst for oxygen reduction studied using SECM

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Localised visualisation of O2 consumption and H2O2 formation by means of SECM for the characterisation of fuel cell catalyst activity

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Study on the anodic reaction of Ni in an alkaline solution by transient pH detection based on scanning electrochemical microscopy (SECM)

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Visualisation of the local bio-electrocatalytic activity in biofuel cell cathodes by means of redox competition scanning electrochemical microscopy (RC-SECM)

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Alternating current (AC) impedance imaging with combined atomic force scanning electrochemical microscopy (AFM-SECM)

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ELECTROCHEMISTRY COMMUNICATIONS (2007)

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Electrochemical reduction of oxygen on gold surfaces: A density functional theory study of intermediates and reaction paths

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Constant-distance mode scanning potentiometry. High resolution pH measurements in three-dimensions

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Feedback-independent Pt nanoelectrodes for shear force-based constant-distance mode scanning electrochemical microscopy

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SECM visualization of spatial variability of enzyme-polymer spots.: Part 2:: Complex interference elimination by means of selection of higbest sensitivity sensor substructures and artificial neural networks

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Scanning electrochemical microscopy combined with surface plasmon resonance: Studies of localized film thickness variations and molecular conformation changes

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Mechanism of oxygen electroreduction on gold surfaces in basic media

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Redox competition mode of scanning electrochemical microscopy (RC-SECM) for visualisation of local catalytic activity

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Unravelling single metalloprotein electron transfer by scanning probe techniques

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Development of a coupled SECM-EQCM technique for the study of pitting corrosion on iron

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Imaging of DNA hybridization on microscopic polypyrrole patterns using scanning electrochemical microscopy (SECM): the HRP bio-catalyzed oxidation of 4-chloro-1-naphthol

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Combined scanning electrochemical-atomic force microscopy (SECM-AFM): Simulation and experiment for flux-generation at un-insulated metal-coated probes

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Scanning electrochemical microscopy (SECM): localized glucose oxidase immobilization via the direct electrochemical microspotting of polypyrrole-biotin films

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Thermodynamic guidelines for the design of bimetallic catalysts for oxygen electroreduction and rapid screening by scanning electrochemical microscopy.: M-Co (M: Pd, Ag, Au)

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Trapping of proteins under physiological conditions in a nanopipette

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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2005)

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Letter Chemistry, Physical

In situ scanning tunneling microscopy study of the effect of iron octaethylporphyrin adlayer on the electrocatalytic reduction of O2 on Au(111)

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MOLECULAR AND CELLULAR ENDOCRINOLOGY (2004)

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Electrocatalysis under conditions of high mass transport rate: Oxygen reduction on single submicrometer-sized Pt particles supported on carbon

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Preparation of reliable probes for electrochemical tunneling spectroscopy

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Real-time pH microscopy down to the molecular level by combined scanning electrochemical microscopy/single-molecule fluorescence spectroscopy

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In situ STM study of the duplex passive films formed on Cu(111) and Cu(001) in 0.1 M NaOH

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CORROSION SCIENCE (2004)

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Constant-distance mode scanning potentiometry. 1. Visualization of calcium carbonate dissolution in aqueous solution

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An advanced biological scanning electrochemical microscope (Bio-SECM) for studying individual living cells

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Optimization of wired enzyme O-2-electroreduction catalyst compositions by scanning electrochemical microscopy

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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2004)

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Approach to writing and simultaneous reading of micropatterns: Combining surface plasmon resonance imaging with scanning electrochemical microscopy (SECM)

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Application of the boundary element method numerical simulations for characterization of heptode ultramicroelectrodes in SECM experiments

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Combination of an electrochemical tunneling microscope (ECSTM) and a scanning electrochemical microscope (SECM): application for tip-induced modification of self-assembled monolayers

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Electron tunnelling through azurin is mediated by the active site Cu ion

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CHEMICAL PHYSICS LETTERS (2003)

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Scanning electrochemical microscopy: Investigation of hydrogen oxidation at polycrystalline noble metal electrodes

CG Zoski

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Scanning electrochemical microscopy.: 47.: Imaging electrocatalytic activity for oxygen reduction in an acidic medium by the tip generation-substrate collection mode

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Direct evidence of the electronic conduction of the passive film on iron by EC-STM

I Díez-Pérez et al.

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Adlayer structures and electrocatalytic activity for O2 of metallophthalocyanines on Au(111):: In situ scanning tunneling microscopy study

S Yoshimoto et al.

JOURNAL OF PHYSICAL CHEMISTRY B (2003)

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Constant-distance mode scanning electrochemical microscopy (SECM) - Part I: Adaptation of a non-optical shear-force-based positioning mode for SECM tips

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CHEMISTRY-A EUROPEAN JOURNAL (2003)

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A novel light source for SICM-SNOM of living cells

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Integrated AFM-SECM in tapping mode: Simultaneous topographical and electrochemical imaging of enzyme activity

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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2003)

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Monitoring cell movements and volume changes with pulse-mode scanning ion conductance microscopy

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Scanning electrochemical microscopy. 45. Study of the kinetics of oxygen reduction on platinum with potential programming of the tip

B Liu et al.

JOURNAL OF PHYSICAL CHEMISTRY B (2002)

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Article Chemistry, Multidisciplinary

Electrogenerated chemiluminescence 69:: The tris(2,2′-bipyridine)ruthenium(II), (Ru(bpy)32+)/tri-n-propylamine (TPrA) system revisited -: A new route involving TPrA•+ cation radicals

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2002)

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Article Biophysics

Ion channels in small cells and subcellular structures can be studied with a smart patch-clamp system

J Gorelik et al.

BIOPHYSICAL JOURNAL (2002)

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Article Chemistry, Multidisciplinary

Detection of Tl(I) transport through a gramicidin-dioleoylphosphatidylcholine monolayer using the substrate generation-tip collection mode of scanning electrochemical microscopy

J Mauzeroll et al.

LANGMUIR (2002)

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Article Chemistry, Physical

Numerical simulations of complex nonsymmetrical 3D systems for scanning electrochemical microscopy using the boundary element method

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JOURNAL OF PHYSICAL CHEMISTRY B (2002)

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Article Biochemical Research Methods

Pulse-mode scanning ion conductance microscopy - a method to investigate cultured hippocampal cells

SA Mann et al.

JOURNAL OF NEUROSCIENCE METHODS (2002)

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Article Chemistry, Multidisciplinary

Micropatterning of HeLa cells on glass substrates and evaluation of respiratory activity using microelectrodes

M Nishizawa et al.

LANGMUIR (2002)

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Article Microscopy

Characterization of AC mode scanning ion-conductance microscopy

D Pastré et al.

ULTRAMICROSCOPY (2001)

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Article Chemistry, Multidisciplinary

Electron transfer reactions at gold nanoparticles

J Zhang et al.

CHEMICAL COMMUNICATIONS (2001)

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Article Chemistry, Physical

Scanning electrochemical microscopy. 43. Investigation of oxalate oxidation and electrogenerated chemiluminescence across the liquid-liquid interface

F Kanoufi et al.

JOURNAL OF PHYSICAL CHEMISTRY B (2001)

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Article Chemistry, Physical

Scanning electrochemical microscopy. 42. Studies of the kinetics and photoelectrochemistry of thin film CdS/electrolyte interfaces

SK Haram et al.

JOURNAL OF PHYSICAL CHEMISTRY B (2001)

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Article Chemistry, Analytical

Oxygen consumption of single bovine embryos probed by scanning electrochemical microscopy

H Shiku et al.

ANALYTICAL CHEMISTRY (2001)

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Article Chemistry, Analytical

Integrating an ultramicroelectrode in an AFM cantilever: Combined technology for enhanced information

C Kranz et al.

ANALYTICAL CHEMISTRY (2001)

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Article Chemistry, Physical

Mechanisms of in situ scanning tunnelling microscopy of organized redox molecular assemblies

AM Kuznetsov et al.

JOURNAL OF PHYSICAL CHEMISTRY A (2000)

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Article Electrochemistry

A scanning electrochemical microscopic observation of heterogeneous oxygen evolution on a polycrystalline titanium during anodic oxidation

K Fushimi et al.

ELECTROCHEMISTRY (2000)

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Article Chemistry, Analytical

Scanning electrochemical microscopy Part 39. The proton/hydrogen mediator system and its application to the study of the electrocatalysis of hydrogen oxidation

JF Zhou et al.

JOURNAL OF ELECTROANALYTICAL CHEMISTRY (2000)

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Article Chemistry, Analytical

Spatially addressed deposition and imaging of biochemically active bead microstructures by scanning electrochemical microscopy

CA Wijayawardhana et al.

ANALYTICAL CHEMISTRY (2000)

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Article Chemistry, Analytical

An instrument for simultaneous EQCM impedance and SECM measurements

B Gollas et al.

ANALYTICAL CHEMISTRY (2000)

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Article Electrochemistry

Integration of an electrochemical quartz crystal microbalance into a scanning electrochemical microscope for mechanistic studies of surface patterning reactions

C Hess et al.

ELECTROCHIMICA ACTA (2000)

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Article Biophysics

Cell volume measurement using scanning ion conductance microscopy

YE Korchev et al.

BIOPHYSICAL JOURNAL (2000)

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