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Multiscale CO2 Electrocatalysis to C2+ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication

CHEMICAL REVIEWS (2023)

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Article Chemistry, Physical

Close to 90% Single-Pass Conversion Efficiency for CO2 Electroreduction in an Acid- Fed Membrane Electrode Assembly

Binbin Pan et al.

Summary: In this study, an acid-fed membrane electrode assembly (MEA) for CO2 electroreduction was demonstrated, achieving high CO Faradaic efficiencies and activities under acidic conditions. The balance between H+ and Cs+ concentrations was found to play a significant role in determining the selectivity and activity. Additionally, the acid-fed MEA exhibited a remarkable long-term stability.

ACS ENERGY LETTERS (2022)

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Article Chemistry, Physical

Enhancing acetate selectivity by coupling anodic oxidation to carbon monoxide electroreduction

Sean Overa et al.

Summary: This study presents an internally coupled purification strategy to improve the concentration and purity of acetate in CO electrolysis. By utilizing an alkaline-stable anion exchange membrane and a selective ethanol partial oxidation anode, the CO reduction product stream was controlled, resulting in stable operation of the CO electrolyzer and production of high concentration and high purity acetate product stream.

NATURE CATALYSIS (2022)

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Article Chemistry, Physical

High-throughput parallelized testing of membrane electrode assemblies for CO2 reduction

Talha Kose et al.

Summary: Characterization of electrochemical reactions with high throughput can speed up discovery and optimization cycles and provide data for machine-learning guided experiment planning. However, current development and testing of electrochemical systems rely on serial, labor-intensive lab processes. This study demonstrates a new MEA testing system that accelerates electrochemical system testing and improves repeatability and reliability.

CATALYSIS SCIENCE & TECHNOLOGY (2022)

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Article Chemistry, Multidisciplinary

Copper nanowire with enriched high-index facets for highly selective CO2 reduction

Lu Han et al.

Summary: By applying a square-wave potential treatment to copper nanowires, high-index crystalline surfaces of copper can be obtained, which enhances the selectivity of multicarbon products, particularly ethylene. This method has the potential to be applied in the design of other catalytic systems and provides insights for other electrochemical catalytic reactions.

SMARTMAT (2022)

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Review Chemistry, Multidisciplinary

Surface and interface chemistry in metal-free electrocatalysts for electrochemical CO2 reduction

Wei Zhang et al.

Summary: This article reviews the effect of surface and interface chemistry on metal-free electrocatalysts (MFEs) for the electrochemical reduction of CO2 (CO2RR). The surface and interface chemistry can regulate the electronic structure, increase active sites, and optimize adsorption strength of reaction intermediates, thus improving the reaction rate and overcoming reaction constraints. The article also discusses the research challenges and prospects for future designs of advanced MFEs in CO2RR.

SMARTMAT (2022)

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Review Chemistry, Multidisciplinary

Design strategies for markedly enhancing energy efficiency in the electrocatalytic CO2 reduction reaction

Wenchuan Lai et al.

Summary: This review provides a comprehensive understanding of the energy efficiency (EE) in electrocatalytic CO2 reduction reaction (CO2RR). The fundamental principles and recent strategies for achieving high EE are discussed, with a focus on electrocatalysts and system design. The emerging integrated electrolysis is highlighted as a promising approach to enhance the EE and economic benefits of the CO2RR. Future research opportunities in this field are also outlined.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

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Article Chemistry, Multidisciplinary

The effect of specific adsorption of halide ions on electrochemical CO2 reduction

Tenghui Yuan et al.

Summary: This study presents a facile method to immobilize the morphology of Cu-based catalysts during CO2RR, which reveals the specific adsorption mechanism of halide ions and provides a theoretical basis for the selectivity of multi-carbon products for Cu-based catalysts.

CHEMICAL SCIENCE (2022)

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Article Chemistry, Physical

Assessing the economic potential of large-scale carbonate-formation-free CO2 electrolysis

Xuechen Jing et al.

Summary: Electrochemical CO2 reduction is a potential approach for manufacturing carbon-neutral fuels and chemicals. However, the formation of carbonates increases energy consumption, resulting in costs exceeding the economic viability threshold for CO2 electroreduction. Techno-economic assessments show that addressing the carbonation issue can significantly reduce production costs.

CATALYSIS SCIENCE & TECHNOLOGY (2022)

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Review Chemistry, Applied

Recent advances in defect electrocatalysts: Preparation and characterization

Zhaohui Xiao et al.

Summary: This review summarizes recent progress in defect electrocatalysts, highlighting the importance of dynamic evolution of defect sites for designing and preparing high-performance electrocatalysts. Furthermore, it suggests future possibilities for the reasonable design of defect electrocatalysts to obtain desirable performance due to insufficient understanding of the defect-structure-property relationships.

JOURNAL OF ENERGY CHEMISTRY (2021)

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Article Green & Sustainable Science & Technology

Electrochemical CO2 Reduction: Tailoring Catalyst Layers in Gas Diffusion Electrodes

Kai Junge Puring et al.

Summary: Gas diffusion electrodes play a crucial role in the electrochemical conversion of CO2, where electrode composition and catalytic layer assembly have a significant impact on the performance. Optimized electrodes show high selectivity and efficiency in producing formate, CO, and H-2 at different current densities and electrolyte concentrations.

ADVANCED SUSTAINABLE SYSTEMS (2021)

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Review Engineering, Chemical

Bipolar membranes: A review on principles, latest developments, and applications

R. Parnamae et al.

Summary: Bipolar membranes (BPMs) are a special class of ion-exchange membranes that generate protons and hydroxide ions via water dissociation mechanism, finding applications in various sectors. Research and development in BPMs over the past two decades have led to a growing market and attention due to technical, environmental, and economic advancements. This review article provides an overview of BPM technology, discussing the current state of the art, properties, theoretical models, applications, optimization, fabrication advances, and potential novel applications.

JOURNAL OF MEMBRANE SCIENCE (2021)

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Article Chemistry, Multidisciplinary

Potential-Dependent Morphology of Copper Catalysts During CO2 Electroreduction Revealed by In Situ Atomic Force Microscopy

Georg H. Simon et al.

Summary: Electrochemical AFM is an effective tool for real-space characterization of catalysts under CO2RR conditions, revealing the complex interplay between morphology, structure, defect density, applied potential, and electrolyte in copper CO2RR catalysts. The study showed distinct nanoscale surface morphologies and their potential-dependent transformations during CO2RR on a Cu(100) model surface in 0.1 m KHCO3. In situ atomic-scale imaging identified specific adsorption at different cathodic potentials impacting the catalyst structure.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Nanoscience & Nanotechnology

Molecular-Scale Insights into Electrochemical Reduction of CO2 on Hydrophobically Modified Cu Surfaces

Shijia Mu et al.

Summary: This research reveals the mechanism of improvement in CO2 reduction reaction using hydrophobically molecule-modified catalysts, showing that these molecules reduce the dissociation of H2O, leading to a decreased H+ source for the HER and increased selectivity in CO2RR.

ACS APPLIED MATERIALS & INTERFACES (2021)

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Article Chemistry, Multidisciplinary

Hollow NiSe Nanocrystals Heterogenized with Carbon Nanotubes for Efficient Electrocatalytic Methanol Upgrading to Boost Hydrogen Co-Production

Bin Zhao et al.

Summary: In this study, a highly active electrocatalyst h-NiSe/CNTs was successfully fabricated to efficiently catalyze methanol to value-added formate at high and steady current density. The catalyst shows high selectivity and long-term stability, replacing sluggish OER performance and reducing energy consumption for H-2 generation by six times.

ADVANCED FUNCTIONAL MATERIALS (2021)

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Article Chemistry, Multidisciplinary

3D-Printable Fluoropolymer Gas Diffusion Layers for CO2 Electroreduction

Joshua Wicks et al.

Summary: The rational design of gas diffusion electrode assemblies is crucial for selective and high-rate CO2 conversion to value-added multicarbon products. The study found that the microporosity and structure of gas diffusion layers can significantly affect the product distributions of catalysts operating at high current densities, with surface morphology design leading to a 100x increase in the C2H4:CO ratio and a pyramidal macrostructure causing a 1.8x increase in the C2H4 partial current density. These findings suggest new routes for improving CO2 reduction GDEs as a platform for 3D catalyst design.

ADVANCED MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Temperature-Dependent CO2 Electroreduction over Fe-N-C and Ni-N-C Single-Atom Catalysts

Long Lin et al.

Summary: In this study, the temperature-dependent CO2 reduction reactions over Fe-N-C and Ni-N-C single-atom catalysts were investigated, revealing variations in selectivity and activity. The differences in CO Faradaic efficiency and current density between Fe-N-C and Ni-N-C catalysts at different temperatures were found to be attributed to the varied adsorption strength of key reaction intermediates during CO2RR.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Boosting CO2 Electrochemical Reduction with Atomically Precise Surface Modification on Gold Nanoclusters

Site Li et al.

Summary: In this study, the surface modification of gold nanoclusters by Cd doping was found to significantly enhance the selectivity and activity for CO2 reduction reaction. The Cd-doped Au19Cd2 NC exhibited the highest CO2RR activity reported. Density-functional theory calculations revealed that Cd doping can boost the CO2RR performance by providing energetically feasible pathways and reducing the energy barrier for CO formation.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Coupling of Cu(100) and (110) Facets Promotes Carbon Dioxide Conversion to Hydrocarbons and Alcohols

Dazhong Zhong et al.

Summary: By utilizing the facet effect of copper crystals, this study achieves a high Faradaic efficiency and large partial current density towards C2+ products. When coupled with a Si solar cell, record-high solar conversion efficiencies for C2H4 and C2+ products are obtained.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Formic Acid Electro-Synthesis by Concurrent Cathodic CO2 Reduction and Anodic CH3OH Oxidation

Xinfa Wei et al.

Summary: This study presents a strategy for efficient formic acid synthesis by conducting concurrent cathodic CO2 reduction and anodic partial methanol oxidation reactions, resulting in significantly lowered potential and high Faraday efficiency in CO2 reduction.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

BiPO4-Derived 2D Nanosheets for Efficient Electrocatalytic Reduction of CO2 to Liquid Fuel

Yating Wang et al.

Summary: A 2D nanosheet-like electrocatalyst derived from bismuth phosphate (BiPO4) efficiently converts CO2 into liquid-phase formate with high Faradaic efficiency. The in situ generation of Bi-O active species on the catalyst surface and abundant insertion of oxygen atoms in the nanosheets contribute to the high activity for electrosynthesis of formate from CO2 and water.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Operando Investigation of Ag-Decorated Cu2O Nanocube Catalysts with Enhanced CO2 Electroreduction toward Liquid Products

Antonia Herzog et al.

Summary: Covering Cu2O nanocubes with Ag nanoparticles can enhance the Faradaic efficiency of CO2 electrochemical reduction reaction for C2+ liquid products. Partial reduction of Cu2O and reaction-driven redispersion of Ag on CuOx were observed during CO2RR, indicating the importance of Ag-Cu sites for C-C coupling and enhanced liquid product yield.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Physical

Regulating electrochemical CO2RR selectivity at industrial current densities by structuring copper@poly(ionic liquid) interface

Xiao-Qiang Li et al.

Summary: The study demonstrates a novel Cu@PIL hybrid material which achieves efficient electrocatalytic CO2 reduction to high value-added C2+ products.

APPLIED CATALYSIS B-ENVIRONMENTAL (2021)

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Article Engineering, Environmental

The anolyte matters: Towards highly efficient electrochemical CO2 reduction

Hao Jiang et al.

Summary: Utilizing OH- oxidation as a counter reaction to CO2 electroreduction can increase formate production rate and faradic efficiency. Alkaline anolyte helps stabilize catholyte pH, avoiding competitive hydrogen evolution reaction, and has the lowest power consumption compared to other anolytes.

CHEMICAL ENGINEERING JOURNAL (2021)

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Article Chemistry, Multidisciplinary

Suppression of Hydrogen Evolution in Acidic Electrolytes by Electrochemical CO2 Reduction

Christoph J. Bondue et al.

Summary: The study focuses on the electrochemical reduction of CO2 at gold electrodes under mildly acidic conditions. Increasing the CO2 partial pressure enhances the rate of CO2 reduction and suppresses hydrogen evolution, leading to high Faradaic efficiencies close to 100%. By suppressing hydrogen evolution and using protons for water formation, the study derived a general design principle for acid CO2 electrolyzers to match the mass transfer of protons to the electrode surface.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Oxidation State and Surface Reconstruction of Cu under CO2 Reduction Conditions from In Situ X-ray Characterization

Soo Hong Lee et al.

Summary: This study demonstrates the structural evolution of Cu catalyst surfaces during the CO2RR and reveals the surface reconstruction of Cu towards (100) facets in the presence of CO2. The findings highlight the dynamic nature of Cu electrocatalysts surface during CO2RR process and the importance of in situ characterization in understanding the role of surface structure in electrocatalysis.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Polymer Science

Influence of Ionomer Loading and Substrate Wettability on the Morphology of Ionomer Thin Films Using Coarse-Grained Solvent Evaporation Simulations

Takuya Mabuchi et al.

Summary: Coarse-grained molecular dynamics simulations were used to study the evolution of ionomer morphologies in solutions during solvent evaporation, revealing different film structures at low and high ionomer loadings. The effects of ionomer loading and substrate wettability on the morphologies of ionomer thin films after drying were investigated, showing different film structures on hydrophobic and hydrophilic substrates.

MACROMOLECULES (2021)

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Article Chemistry, Multidisciplinary

Improving the efficiency of CO2 electrolysis by using a bipolar membrane with a weak-acid cation exchange layer

Zhifei Yan et al.

Summary: This study investigates the effects of local environments on ionic flows in membrane electrolysers, and demonstrates the measurement and manipulation of local pH to improve CO₂ reduction efficiency.

NATURE CHEMISTRY (2021)

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Article Nanoscience & Nanotechnology

An industrial perspective on catalysts for low-temperature CO2 electrolysis

Richard I. Masel et al.

Summary: This Perspective discusses the key advances in nanocatalysts that have led to significant progress in the electrochemical conversion of CO2 to useful products, providing benchmarks for comparison and highlighting the need for further research.

NATURE NANOTECHNOLOGY (2021)

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Article Multidisciplinary Sciences

Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment

Zhuo Xing et al.

Summary: The study found that a hydrophobic microenvironment can significantly enhance CO2 gas-diffusion electrolysis efficiency. Furthermore, a balanced gas/liquid microenvironment can reduce the diffusion layer thickness, accelerate CO2 mass transport, and increase CO2 local concentration for electrolysis.

NATURE COMMUNICATIONS (2021)

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Article Chemistry, Physical

Potential Dependence of the Local pH in a CO2 Reduction Electrolyzer

Danielle A. Henckel et al.

Summary: The study found that the local pH of a gas diffusion electrode undergoing CO2 reduction is significantly lower than the bulk electrolyte pH, showing dependence on applied potential. The decrease in pH is attributed to the formation of malachite from soluble Cu(II) species on the initially oxidized electrode surface.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Hydrophobic Copper Interfaces Boost Electroreduction of Carbon Dioxide to Ethylene in Water

Hong-Qing Liang et al.

Summary: In this study, the effect of the electrode-electrolyte interface on CO2 reduction in water was investigated by coating CuO electrodes with polymers of varying hydrophilicities/phobicities. Results showed that hydrophobic polymers significantly enhanced the activity, selectivity, and stability of CuO-derived electrodes. This improvement in catalytic performance may be attributed to restricted water diffusion and a higher local pH near the electrode surface caused by hydrophobic polymers.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Role of the Carbon-Based Gas Diffusion Layer on Flooding in a Gas Diffusion Electrode Cell for Electrochemical CO2 Reduction

Kailun Yang et al.

Summary: The deployment of gas diffusion electrodes (GDEs) for the electrochemical CO2 reduction reaction (CO2RR) has significantly increased current densities, but stability challenges arise due to rapid flooding of GDEs. Research shows that applied potential plays a central role in causing instabilities in carbon gas diffusion layers (GDLs) during CO2RR, leading to independent flooding issues. The study findings can be applied to electrochemical reduction reactions using carbon-based GDEs with cathodic overpotentials less than -0.65 V versus a reversible hydrogen electrode.

ACS ENERGY LETTERS (2021)

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Article Chemistry, Physical

Electrochemical CO2-to-ethylene conversion on polyamine-incorporated Cu electrodes

Xinyi Chen et al.

Summary: A Cu-polyamine hybrid catalyst was developed to significantly enhance the selectivity for ethylene production in CO2 electrochemical conversion. Incorporating polyamine altered surface reactivity, leading to improved product selectivity at high current densities.

NATURE CATALYSIS (2021)

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Article Chemistry, Physical

In situ facile fabrication of Ni(OH)2 nanosheet arrays for electrocatalytic co-production of formate and hydrogen from methanol in alkaline solution

Jie Hao et al.

Summary: Ni(OH)2 nanosheet arrays were prepared on Ni foam through ultrasonication and exhibited high activity for selective oxidation of methanol to produce formate and hydrogen without CO2 emissions. The method reduces energy consumption for hydrogen evolution from water and simplifies the electrolysis system by allowing easy separation of anodic and cathodic products.

APPLIED CATALYSIS B-ENVIRONMENTAL (2021)

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Article Chemistry, Multidisciplinary

Surface Hydrides on Fe2P Electrocatalyst Reduce CO2 at Low Overpotential: Steering Selectivity to Ethylene Glycol

Karin U. D. Calvinho et al.

Summary: The development of efficient electrocatalysts for the CO2 reduction reaction to produce multicarbon products has been limited by high overpotentials and poor selectivity. By introducing iron phosphide as a catalyst, carbon product selectivity can be tuned by increasing negative bias.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Selective and High Current CO2 Electro-Reduction to Multicarbon Products in Near-Neutral KCl Electrolytes

Xiao Zhang et al.

Summary: A stable and selective electrocatalytic carbon dioxide reduction reaction (CO2RR) to C2+ products was achieved using a Cu electrocatalyst on a hydrophobic gas-diffusion layer (GDL) electrode in near-neutral KCl electrolytes. The instability of the catalyst in alkaline media under cathodic CO2RR conditions was largely suppressed by using a near-neutral electrolyte, showcasing the potential for long-term stability in CO2RR applications.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (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, Multidisciplinary

Hybrid Metal-Boron Diatomic Site Embedded in C2N Monolayer Promotes C-C Coupling in CO2 Electroreduction

Miaomiao He et al.

Summary: This study investigates the application of double-atom catalysts in CO2 reduction and demonstrates that hybrid M-B dual-atom centers can outperform single or double-M centers. Fe@B-C2N is predicted as a promising catalyst for the development of C2+ products.

SMALL (2021)

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Review Chemistry, Physical

The Fe Effect: A review unveiling the critical roles of Fe in enhancing OER activity of Ni and Co based catalysts

Sengeni Anantharaj et al.

Summary: This article discusses the critical role of Fe in Ni/Co-based OECs in the oxygen evolution reaction, highlighting several contradictory conclusions found in the research. It emphasizes the importance of understanding the Fe effect for efficient hydrogen generation in alkaline medium.

NANO ENERGY (2021)

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Article Multidisciplinary Sciences

Promoting ethylene production over a wide potential window on Cu crystallites induced and stabilized via current shock and charge delocalization

Hao Sun et al.

Summary: The substrate-catalyst interaction plays a critical role in steering the pathway of electrochemical CO2 reduction. Here the authors show the crystalline states of copper in reconstructed metal-organic frameworks were induced and stabilized by Ketjen Black conducting support, promoting C2H4 production.

NATURE COMMUNICATIONS (2021)

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Article Multidisciplinary Sciences

Dynamic transformation of cubic copper catalysts during CO2 electroreduction and its impact on catalytic selectivity

Philipp Grosse et al.

Summary: To design effective and stable catalysts for energy conversion applications, it is essential to understand how they transform under reaction conditions and reveal the structure-property relationships, especially for catalysts used in the electroreduction of carbon dioxide. Real-time electrochemical studies show the restructuring of copper(I) oxide cubes during reaction and its impact on catalyst selectivity. Understanding the changes in catalysts during reaction is crucial for rational design, with studies linking structural transformations of cubic copper oxide catalysts with their selectivity.

NATURE COMMUNICATIONS (2021)

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Article Multidisciplinary Sciences

Efficient CO2 electroreduction on facet-selective copper films with high conversion rate

Gong Zhang et al.

Summary: The authors developed a novel synthetic approach to prepare Cu(100)-rich thin film electrodes for CO2 electroreduction, achieving high Faradaic efficiency for ethylene and C2+ products. Scaling up the electrode led to increased total current and higher yield of desired C2+ products. Insights into Cu facets exposure effects on intermediates were provided through in situ spectroscopic methods and theoretical calculations, enabling precise design of CO2 reduction reactions for future industrial applications.

NATURE COMMUNICATIONS (2021)

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Article Chemistry, Physical

2.6% cm-2 Single-Pass CO2-to-CO Conversion Using Ni Single Atoms Supported on Ultra-Thin Carbon Nanosheets in a Flow Electrolyzer

Yang Zhang et al.

Summary: The study on CO2 reduction using SA Ni-NC revealed that optimized feed stream conditions can lead to high energy efficiency and conversion rates, demonstrating the potential for efficient CO2 conversion using flow electrolyzers.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Self-Cleaning CO2 Reduction Systems: Unsteady Electrochemical Forcing Enables Stability

Yi Xu et al.

Summary: The study introduces a self-cleaning CO2 reduction strategy to enhance the efficiency of electrochemical conversion of CO2 and prevent carbonate salt formation, demonstrating a significant extension of the cathode's lifespan.

ACS ENERGY LETTERS (2021)

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Review Energy & Fuels

Designing anion exchange membranes for CO2 electrolysers

Danielle A. Salvatore et al.

Summary: New technologies are needed to efficiently convert carbon dioxide into fuels and chemicals at near-ambient temperatures and pressures. Anion exchange membranes in zero-gap reactors show promise for mediating the electrochemical CO2 reduction reaction, but challenges remain in tailoring these membranes to meet the requirements of CO2RR systems.

NATURE ENERGY (2021)

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Review Chemistry, Physical

Coupling electrochemical carbon dioxide conversion with value-added anode processes: An emerging paradigm

A. Vass et al.

Summary: Water oxidation reaction, commonly used in mimicking natural photosynthesis for CO2 electroreduction, requires high energy input and generates low-value product oxygen. Finding suitable alternative anode processes is crucial, considering factors like product value, substrate abundance, cell voltage, catalysts, cell structure, and ease of product analysis. Future research needs to address these main questions.

CURRENT OPINION IN ELECTROCHEMISTRY (2021)

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Article Nanoscience & Nanotechnology

Investigation of Electrolyte-Dependent Carbonate Formation on Gas Diffusion Electrodes for CO2 Electrolysis

Emiliana R. Cofell et al.

Summary: This study investigates the degradation of gas diffusion electrodes (GDEs) in a flowing, alkaline CO2 electrolyzer via the formation of carbonate deposits on the GDE surface. The rate of carbonate deposit formation was found to increase with increasing electrolyte molarity and become more prevalent in K+-containing electrolytes. The formation of carbonate deposits was found to diminish electrode performance in ECO2R and reduce GDE hydrophobicity, leading to increased flooding and internal deposits within the GDE substrate.

ACS APPLIED MATERIALS & INTERFACES (2021)

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Article Nanoscience & Nanotechnology

Grain Boundary Engineering of Cu-Ag Thin-Film Catalysts for Selective (Photo)Electrochemical CO2 Reduction to CO and CH4

Wan Jae Dong et al.

Summary: The study investigated the relationship between grain boundary oxidation of Cu-Ag thin-film catalysts and the selectivity of the CO2 reduction reaction. A thicker Cu layer was found to prevent grain boundary oxidation and maintain catalytic properties similar to bulk Cu-Ag catalysts, while an optimized Cu-Ag thin film demonstrated bifunctional characteristics producing both CO and CH4 with high selectivity.

ACS APPLIED MATERIALS & INTERFACES (2021)

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Article Chemistry, Multidisciplinary

Divergent Paths, Same Goal: A Pair-Electrosynthesis Tactic for Cost-Efficient and Exclusive Formate Production by Metal-Organic-Framework-Derived 2D Electrocatalysts

Changsheng Cao et al.

Summary: The study introduces a novel approach to simultaneously produce formate on both electrodes through a selective electrocatalytic method, achieving high efficiency and reduced energy input. The coupled reaction system based on MOF-derived catalysts demonstrates excellent performance in formate electrosynthesis, providing high current densities and nearly 100% selectivity on both the anode and cathode.

ADVANCED MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Sub-Second Time-Resolved Surface-Enhanced Raman Spectroscopy Reveals Dynamic CO Intermediates during Electrochemical CO2 Reduction on Copper

Hongyu An et al.

Summary: The study successfully monitored the process of carbon dioxide reduction to hydrocarbons using time-resolved Raman spectroscopy, and found that anodic treatment and surface oxide reduction of the copper electrode can improve CO2RR efficiency and time resolution.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Chemical Identification of Catalytically Active Sites on Oxygen-doped Carbon Nanosheet to Decipher the High Activity for Electro-synthesis Hydrogen Peroxide

Shanyong Chen et al.

Summary: A chemical titration strategy was proposed to decipher the mechanism of oxygen-doped carbon nanosheet catalyst for 2 e(-) ORR, revealing that C=O species are the main active sites for electrocatalytic activity.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Physical

Strong interactions of metal-support for efficient reduction of carbon dioxide into ethylene

Dongxing Tan et al.

Summary: The Cu/CeO2 nanotubes catalyst shows high efficiency in electrochemical reduction of CO2 and solar-driven CO2 splitting reaction, attributed to the synergistic effects from the formation of inseparable interface structure between Cu and CeO2.

NANO ENERGY (2021)

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Article Engineering, Environmental

All roads lead to Rome: An energy-saving integrated electrocatalytic CO2 reduction system for concurrent value-added formate production

Dan Wu et al.

Summary: This study introduces a novel strategy of simultaneous formate generation at the cathode and anode to reduce electricity consumption and increase valuable fuel production. The integration system significantly lowers specific energy consumption for CO2R by 57.3% and for MOR by 71.2%, highlighting the economic benefits of coupling CO2R with alternative oxidation reactions.

CHEMICAL ENGINEERING JOURNAL (2021)

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Review Chemistry, Multidisciplinary

Tandem devices for simultaneous CO2 reduction at the cathode and added-value products formation at the anode

Umberto Savino et al.

Summary: The catalytic reduction of CO2 to obtain carbon-based molecules with high economic value faces challenges with the oxygen evolution reaction. Solutions to improve system performance through tandem reactions are explored, with a focus on catalysts and future sustainable power generation for electro-catalytic systems. This review aims to propose a more sustainable second generation of tandem catalytic reactions for high added-value products.

JOURNAL OF CO2 UTILIZATION (2021)

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Article Energy & Fuels

Tailored catalyst microenvironments for CO2 electroreduction to multicarbon products on copper using bilayer ionomer coatings

Chanyeon Kim et al.

Summary: The authors investigated and optimized the microenvironment near the copper catalyst surface using bilayer ionomer coatings to improve the efficiency of CO2 reduction. By tailoring the microenvironment and coupling it with pulsed electrolysis, higher local CO2/H2O ratio and pH values are achieved, leading to selective C2+ production.

NATURE ENERGY (2021)

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Article Chemistry, Physical

Effects of Uniaxial Lattice Strain and Explicit Water Solvation on CO2 Electroreduction over a Cu Electrode: A Density Functional Theory Perspective

Yuanyuan Du et al.

Summary: Strain engineering of metal-based catalysts has been shown to disrupt scaling relations of adsorbed species in catalytic reactions. By simulating applying lattice strain to evaluate CO2 electroreduction performance, it was found that the coupling between intrinsic lattice strain and adsorbate-induced strain determines the binding strength of key reaction intermediates. The solvation effect of water on CO2 electroreduction was also discussed.

JOURNAL OF PHYSICAL CHEMISTRY C (2021)

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Article Chemistry, Multidisciplinary

Hierarchical Copper with Inherent Hydrophobicity Mitigates Electrode Flooding for High-Rate CO2 Electroreduction to Multicarbon Products

Zhuang-Zhuang Niu et al.

Summary: The study focuses on designing a copper catalyst inspired by nature, with sufficient hydrophobicity and a unique hierarchical structure, to enhance the efficiency and stability of the CO2 reduction electrode.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Revisiting Understanding of Electrochemical CO2 Reduction on Cu(111): Competing Proton-Coupled Electron Transfer Reaction Mechanisms Revealed by Embedded Correlated Wavefunction Theory

Qing Zhao et al.

Summary: Copper electrodes are widely used in CO2 reduction reaction and play a key role in determining the reaction mechanisms using DFT. This study corrected the XC functional error using ECW theory and predicted the formation of different intermediates on Cu(111) under different mechanisms and applied potentials. Including explicitly modeled solvent molecules is important in predicting electron-transfer barriers and overreliance on simple surface models may lead to pitfalls in predicting reduction reactions.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Machine-Learning-Guided Discovery and Optimization of Additives in Preparing Cu Catalysts for CO2 Reduction

Ying Guo et al.

Summary: The study utilizes machine-learning to search for additives in the electrochemical deposition of Cu catalysts for CO2 reduction, showing that additives can cause subtle changes in catalyst morphology and surface structure, leading to significant shifts in CO2RR selectivity. Through ML cycles, catalysts selective for CO, HCOOH, and C2+ products were obtained.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Rational Surface and Interfacial Engineering of IrO2/TiO2 Nanosheet Arrays toward High-Performance Chlorine Evolution Electrocatalysis and Practical Environmental Remediation

Yunting Wang et al.

Summary: The study introduces hybrid IrO2/TiO2 nanosheet arrays (NSAs) with rational surface and interfacial tuning strategies for boosting chlorine evolution reaction (CER) electrocatalysis. The IrO2/TiO2 NSAs exhibit superb CER electrocatalytic activity and long-term durability, showing potential applications in industrial utilization and environmental remediation.

SMALL (2021)

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Article Multidisciplinary Sciences

Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis

Jun Li et al.

Summary: The oxide modulation strategy introduced silica on copper to create active Cu-SiOx interface sites, reducing the formation energies of key intermediates along the pathway to ethylene formation. The Cu-SiOx catalyst integrated in the MEA electrolyzer showed high ethylene Faradaic efficiencies and sustained operation, offering a sustainable route to produce valuable chemicals.

NATURE COMMUNICATIONS (2021)

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Article Chemistry, Physical

True Nature of the Transition-Metal Carbide/Liquid Interface Determines Its Reactivity

Christoph Griesser et al.

Summary: In aqueous electrolytes, surface oxide formation on hexagonal Mo2C completely suppresses CO2 activation, while in nonaqueous electrolytes, Mo2C shows CO2RR activity when protected from ambient air.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Elucidating the Facet-Dependent Selectivity for CO2 Electroreduction to Ethanol of Cu-Ag Tandem Catalysts

Pranit Iyengar et al.

Summary: This study elucidates the active sites for ethanol production on Cu-Ag CO2RR tandem catalysts using structural sensitivity effects, showing how ethanol and ethylene formation pathways exhibit selectivity differences in a CO-enriched environment. The findings highlight the potential of tandem catalysis and structure-sensitive effects to significantly alter the selectivity of electrochemical reactions.

ACS CATALYSIS (2021)

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Article Chemistry, Multidisciplinary

A novel strategy to achieve simultaneous efficient formate production and p-nitrophenol removal in a co-electrolysis system of CO2 and p-nitrophenol

Qinian Wang et al.

Summary: By controlling the anode potential and cathode surface area, simultaneous efficient CO2 conversion and organic pollutant removal can be achieved in the co-electrolysis system. This electrolysis mode demonstrated in the study can increase current efficiency and accelerate the use of the system in industrial applications.

JOURNAL OF CO2 UTILIZATION (2021)

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Article Chemistry, Physical

Tuning the Microenvironment in Gas-Diffusion Electrodes Enables High-Rate CO2 Electrolysis to Formate

Zhuo Xing et al.

Summary: Tuning the microenvironment of Bi-based catalyst in a gas-diffusion-electrode (GDE) by adding hydrophobic polytetrafluoroethylene (PTFE) nanoparticles substantially enhances CO2 electrolysis, achieving high formate production rates and CO2 conversion efficiencies.

ACS ENERGY LETTERS (2021)

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Article Chemistry, Physical

Formation of 1-Butanol from CO2 without *CO Dimerization on a Phosphorus-Rich Copper Cathode

Minjun Choi et al.

Summary: This study successfully achieved the conversion of carbon dioxide into 1-butanol on a phosphorus-rich copper cathode through a combination of faradaic and autonomous nonfaradaic reactions. The faradaic efficiency for 1-butanol formation reached 3.868%, indicating a promising new perspective for the C-C coupling reaction on Cu-based electrocatalysts.

ACS ENERGY LETTERS (2021)

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Article Chemistry, Multidisciplinary

In Situ Formed Sn1-XInX@In1-YSnYOZ Core@Shell Nanoparticles as Electrocatalysts for CO2 Reduction to Formate

Laura C. Pardo Perez et al.

Summary: Electrochemical reduction of CO2 (CO2RR) driven by renewable energy sources is gaining attention for sustainable production of chemicals and fuels. Metal/metal oxide composite nanoparticles formed by in situ reduction of bimetallic amorphous SnInOx thin films show high selectivity towards formate formation, with outstanding faradaic efficiency and formate mass activity. The core@shell structure of the nanoparticles remains stable under different electrolysis conditions, with high surface oxide contents favoring formate over hydrogen selectivity.

ADVANCED FUNCTIONAL MATERIALS (2021)

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Article Chemistry, Multidisciplinary

MnO2 Electrocatalysts Coordinating Alcohol Oxidation for Ultra-Durable Hydrogen and Chemical Productions in Acidic Solutions

Yan Li et al.

Summary: Manganese oxide demonstrates excellent electrocatalytic hydrogen production performance under acidic conditions, especially showing high stability and efficiency in glycerol solution.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Implanting Numerous Hydrogen-Bonding Networks in a Cu-Porphyrin-Based Nanosheet to Boost CH4 Selectivity in Neutral-Media CO2 Electroreduction

Yi-Rong Wang et al.

Summary: This study successfully utilized a Cu-porphyrin-based large-scale and ultrathin nanosheet as an electrocatalyst for CO2RR, achieving high CO2 conversion efficiency under neutral conditions. By constructing hydrogen-bonding networks, proton migration and intermediate stabilization were facilitated, providing a new pathway for efficient CO2RR catalyst development.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Highly Selective Tandem Electroreduction of CO2 to Ethylene over Atomically Isolated Nickel-Nitrogen Site/Copper Nanoparticle Catalysts

Dong-Li Meng et al.

Summary: An effective tandem catalysis strategy was developed to improve the selectivity of CO2RR towards C2H4, using multiple distinct catalytic sites in local vicinity. A tandem electrocatalyst PTF(Ni)/Cu was constructed, which significantly enhanced the Faradaic efficiency of C2H4 to 57.3% at -1.1 V versus RHE. Experimental and theoretical results showed that the local high concentration of CO generated by PTF(Ni) sites facilitated the C-C coupling on nearby Cu NP sites to form C2H4.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Physical

Amino Assisted Protonation for Carbon-Carbon Coupling during Electroreduction of Carbon Dioxide to Ethylene on Copper(I) Oxide

Hongwei Deng et al.

Summary: This study demonstrated the enhanced production of CO and C-2 products using an amino-modified Cu2O catalyst in electrocatalytic CO2RR. Experimental and computational analysis confirmed the promoting effect of amino modification on C2H4 production, offering a new perspective for the application of such catalysts in the field of CO2RR.

CHEMCATCHEM (2021)

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Article Electrochemistry

Electrochemical reduction of CO2 to CO in organic electrolyte with HCl oxidized to Cl2 on anode for phosgene synthesis

Chaojuan Li et al.

Summary: By electrolyzing CO2 and chloride solution, phosgene can be produced and the value of CO2 can be recovered.

ELECTROCHIMICA ACTA (2021)

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Article Chemistry, Inorganic & Nuclear

Br-Doped CuO Multilamellar Mesoporous Nanosheets with Oxygen Vacancies and Cetyltrimethyl Ammonium Cations Adsorption for Optimizing Intermediate Species and Their Adsorption Behaviors toward CO2 Electroreduction to Ethanol with a High Faradaic Efficiency

Wuzhengzhi Zhang et al.

Summary: In this study, Br-doped CuO multilamellar mesoporous nanosheets were successfully synthesized on Cu foam to serve as highly active and selective electrocatalysts for the CO2 electroreduction reaction (CO2ER) into ethanol. The introduction of Br- ions induced oxygen vacancies, while adsorbed CTA(+) cations modulated the O affinity of Cu sites, optimizing intermediate species and their adsorption behaviors. The optimized Br1.95%-CuO catalyst showed excellent catalytic stability and achieved a high faradaic efficiency of 53.3% for C2H5OH production.

INORGANIC CHEMISTRY (2021)

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Article Chemistry, Multidisciplinary

Oriented Electrostatic Effects on O2 and CO2 Reduction by a Polycationic Iron Porphyrin

Daniel J. Martin et al.

Summary: The study demonstrates that a metalloporphyrin catalyst with four cationic groups can stabilize charged intermediates and catalyze ORR and CO2RR reactions with fast rates and low overpotentials. Each of the four atropisomers of the metalloporphyrin show differences in maximum turnover frequencies and overpotentials for the two reactions, highlighting the complexity of charge positioning in affecting the thermodynamics and kinetics of multistep molecular electrochemical transformations.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Multidisciplinary Sciences

CO2 electrolysis to multicarbon products in strong acid

Jianan Erick Huang et al.

Summary: Carbon dioxide electroreduction (CO2R) is being actively studied as a promising route to convert carbon emissions to valuable chemicals and fuels. A study found that concentrating potassium cations in the vicinity of electrochemically active sites accelerates CO2 activation to enable efficient CO2R in acid. The research achieved a high CO2R efficiency on copper at pH <1 with a single-pass CO2 utilization of 77%.

SCIENCE (2021)

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Article Chemistry, Multidisciplinary

Electrochemical Reduction of CO2 Toward C2 Valuables on Cu@Ag Core-Shell Tandem Catalyst with Tunable Shell Thickness

Shuaishuai Zhang et al.

Summary: Cu@Ag core-shell nanoparticles with different silver layer thicknesses were fabricated for tandem catalysis in CO2 conversion, achieving high selectivity and stability for C-2 generation. The synergistic effect between Ag shell and Cu core enhances CO bonding strength, charge transfer, and electrochemical surface areas, leading to improved catalytic performance.

SMALL (2021)

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Article Multidisciplinary Sciences

Quasi-graphitic carbon shell-induced Cu confinement promotes electrocatalytic CO2 reduction toward C2+ products

Ji-Yong Kim et al.

Summary: Surface reconstruction of electrocatalysts is important for converting carbon dioxide to value-added chemical products. In this study, stable CO2 to C2H4 conversion is achieved by using copper nanoparticles protected by self-formed quasi-graphitic carbon shell.

NATURE COMMUNICATIONS (2021)

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Article Chemistry, Physical

Revealing the CO Coverage-Driven C-C Coupling Mechanism for Electrochemical CO2 Reduction on Cu2O Nanocubes via Operando Raman Spectroscopy

Chao Zhan et al.

Summary: This study used operando Raman spectroscopy to investigate the potential-dependent reduction process of Cu2O nanocubes, revealing a correlation between CO coverage and the selectivity for multicarbon products. The research provides a theoretical basis for the high selectivity generation of multicarbon products.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Comprehensive Mechanism of CO2 Electroreduction toward Ethylene and Ethanol: The Solvent Effect from Explicit WaterCu(100) Interface Models

Jirapat Santatiwongchai et al.

Summary: This study presents a comprehensive CO2 electro-reduction mechanism on a Cu(100) surface using density functional theory simulations, revealing various favorable alternative pathways and elucidating each step of the CO2 conversion to CO process. The results offer guidance on tuning the selectivity of ethylene and ethanol, and provide insights into the solvent effect on intermediates involved in CO2 electroreduction.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Toward an Understanding of the Enhanced CO2 Electroreduction in NaCl Electrolyte over CoPc Molecule-Implanted Graphitic Carbon Nitride Catalyst

Xinyi Tan et al.

Summary: This study achieved efficient CO2 electrolysis in seawater using CoPc/g-C3N4 electrocatalyst, with chlorine ions found to have positive effects on the CO2RR. In simulated seawater, a high faradaic efficiency of up to 98.1% towards CO was achieved.

ADVANCED ENERGY MATERIALS (2021)

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Article Electrochemistry

Understanding Structure-activity Relationship on Metal-Organic-Framework-Derived Catalyst for CO2 Electroreduction to C2 Products

Yunxi Han et al.

Summary: Research has shown that during the CO2 reduction reaction process, HKUST-1 will successively reconstruct into two different structures over time: 3D nanospheres composed of numerous small fragments and a 3D nano-network composed of cross-linked nanobelts. The former exhibits better catalytic activity due to more active sites, lower charge transfer resistance, and a higher Cu+/Cu-0 ratio. The optimum Faradaic efficiency (FE) of C-2 products (ethylene and ethanol) reaches 58.6% at -0.98 V versus reversible hydrogen electrode (RHE).

CHEMELECTROCHEM (2021)

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Article Chemistry, Physical

Single Pass CO2 Conversion Exceeding 85% in the Electrosynthesis of Multicarbon Products via Local CO2 Regeneration

Colin P. O'Brien et al.

Summary: The CO2 reduction reaction (CO2RR) provides an opportunity to consume CO2 and produce desirable products, but the alkaline conditions required often lead to loss of input CO2 to bicarbonate and carbonate, limiting the conversion of CO2 to multicarbon products. This study found that cation exchange membranes (CEMs) and bipolar membranes (BPMs) were not ideal for providing locally alkaline conditions, but the development of a permeable CO2 regeneration layer (PCRL) allowed for a more efficient CO2 conversion process with limited CO2 crossover.

ACS ENERGY LETTERS (2021)

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Article Chemistry, Physical

Integrated Capture and Electroreduction of Flue Gas CO2 to Formate Using Amine Functionalized SnOx Nanoparticles

Yingying Cheng et al.

Summary: By grafting alkanol-amines on a tin oxide surface, the study successfully integrated CO2 capture and electrochemical conversion of flue gas, achieving high Faradaic efficiency for formate production. Surface amino groups not only enrich CO2 and inhibit O2 reduction, but also accelerate CO2 reduction by promoting the formation of key intermediates.

ACS ENERGY LETTERS (2021)

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Article Chemistry, Physical

Interplay of electrochemical and electrical effects induces structural transformations in electrocatalysts

Feng Li et al.

Summary: The study investigates how electrochemical and complex current behaviors influence the structural stability of nanoscale objects during electrocatalysis.

NATURE CATALYSIS (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 Multidisciplinary Sciences

Process modeling, techno-economic assessment, and life cycle assessment of the electrochemical reduction of CO2: a review

Ana Somoza-Tornos et al.

Summary: The electrochemical reduction of CO2 is seen as a promising alternative to traditional fossil fuel technologies for chemical synthesis, but the low technology readiness levels make it difficult to predict performance at an industrial scale. Researchers have developed various techniques to assess these technologies, focusing on technical, environmental, and economic aspects, in order to evaluate the challenges and opportunities for industrial implementation of CO2 reduction through electrolysis.

ISCIENCE (2021)

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Review Chemistry, Multidisciplinary

Three-phase interface-assisted advanced electrochemistry-related applications

Yupeng Chen et al.

Summary: This article systematically summarizes the representative electrochemical reactions that occur at TPIs, including typical electrocatalytic reactions, common fuel cells, and enzymatic reactions for electrochemical detection. It also discusses the fabrication of materials with specific structures, synthesis of chiral pharmaceuticals, substrates for anti-corrosion, and general methods for constructing TPI-based electrodes.

CELL REPORTS PHYSICAL SCIENCE (2021)

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Article Chemistry, Multidisciplinary

Efficient electrochemical reduction of CO2 promoted by the electrospun Cu1.96S/Cu tandem catalyst

Shuo Liu et al.

Summary: The study presents a Cu1.96S/Cu tandem structure catalyst for CO2 reduction with high selectivity and production rate, outperforming most Cu-based catalysts. Theoretical simulations demonstrate that the improved performance is attributed to the Cu1.96S/Cu tandem structure, which enhances both CO generation and desorption steps, offering new possibilities for exploiting tandem catalysis mechanisms.

NANOSCALE (2021)

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Article Chemistry, Multidisciplinary

The product selectivity zones in gas diffusion electrodes during the electrocatalytic reduction of CO2

Tim Moller et al.

Summary: This study explores the factors influencing the performance of a Cu-based CO2 electrolyzer at high currents and emphasizes the importance of adjusting electrode structure, catalyst loading, and ionomer content to affect the selectivity of electrochemical CO2 reduction. Mass transport variations within the porous catalytic layer and local concentration gradients are crucial in determining overall selectivity. The research also shows how electrode structure can push the catalytic CO2 reduction selectivity towards specific products, highlighting the potential for optimization in the production of value-added products.

ENERGY & ENVIRONMENTAL SCIENCE (2021)

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Article Chemistry, Multidisciplinary

Elucidating the structure-dependent selectivity of CuZn towards methane and ethanol in CO2 electroreduction using tailored Cu/ZnO precatalysts

Seyedeh Behnaz Varandili et al.

Summary: Understanding the compositional and structural features of catalysts controlling selectivity is crucial in chemical reactions. This study leveraged tailored Cu/ZnO precatalysts to identify intrinsic features of CuZn catalysts for CO2 reduction, revealing Cu@CuZn core@shell structures selective for methane and ethanol. Surface alloying and metallic Zn concentration were found to improve ethanol selectivity, with density functional theory explaining the selectivity based on electronic and tandem effects. These findings contribute to the rational tuning of bimetallic catalysts for CO2 reduction towards increased selectivity, especially for alcohols.

CHEMICAL SCIENCE (2021)

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Review Chemistry, Multidisciplinary

Electrocatalytic reduction of CO2 and CO to multi-carbon compounds over Cu-based catalysts

Wenchao Ma et al.

Summary: This tutorial review explores the electrocatalytic reduction of CO2 with H2O to multi-carbon (C2+) compounds, focusing on the similarities and differences in the electrocatalytic CO2 and CO reduction reactions (CO2RR and CORR) into C2+ compounds over Cu-based catalysts. It discusses fundamental aspects, reaction mechanisms, efficient catalysts, and key factors determining selectivity, activity, and stability. Opportunities, challenges, and future trends in the electrocatalytic CO2RR and CORR are also highlighted for the synthesis of C2+ olefins and oxygenates.

CHEMICAL SOCIETY REVIEWS (2021)

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Article Chemistry, Multidisciplinary

Engineering Covalent Organic Framework Membranes

Guangwei He et al.

Summary: Membrane technology is increasingly important for sustainable development, with COFs emerging as potent membrane materials due to their unique structure and properties compared to polymers, zeolites, and MOFs. COFs have highly tunable pore structure, high porosity, and excellent stability, making them ideal for advanced membrane applications. Various engineering approaches towards COF membranes, such as reticular engineering, crystal engineering, and nanochannel engineering, are actively being explored to enhance their separation efficiency and stability.

ACCOUNTS OF MATERIALS RESEARCH (2021)

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Review Chemistry, Physical

The role of electrode wettability in electrochemical reduction of carbon dioxide

Mengran Li et al.

Summary: The wettability of the electrode plays a crucial role in CO2RR by affecting the reactivity, selectivity, and stability of the electrode. Improving cathode performance by altering the wettability of the catalyst layer in gas-diffusion electrodes can lead to more efficient CO2RR. Current challenges and opportunities lie in developing efficient and selective cathodes for CO2RR at industrially relevant rates.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

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Article Materials Science, Multidisciplinary

Dynamic structure change of Cu nanoparticles on carbon supports for CO2 electro-reduction toward multicarbon products

Qiang Li et al.

Summary: Cu nanoparticles with different sizes, morphology, and surface structures exhibit distinct activity and selectivity in CO2 reduction reaction. The study demonstrates that the dynamic structure change of Cu clusters on graphite-like carbon supports plays an important role in the production of multicarbon products. The study also reveals that the roughened surface morphologies resulting from the dynamic structure change of the catalysts play an essential role in the selectivity of CO2 electro-reduction.

INFOMAT (2021)

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Review Chemistry, Multidisciplinary

Layered double hydroxide-based electrocatalysts for the oxygen evolution reaction: identification and tailoring of active sites, and superaerophobic nanoarray electrode assembly

Daojin Zhou et al.

Summary: Understanding the structure and active sites of LDHs is crucial for designing and regulating high-performance electrocatalysts. Recent advancements and strategies for enhancing OER activity in LDHs, such as doping, intercalation, and defect-making, are discussed in this review. The concept of superaerophobicity and certain operating standards for OER measurements are also highlighted to improve the performance of LDHs in large scale water splitting applications.

CHEMICAL SOCIETY REVIEWS (2021)

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Article Chemistry, Multidisciplinary

Selective electrocatalytic CO2 reduction to acetate on polymeric Cu-L (L = pyridinic N and carbonyl group) complex core-shell microspheres

Fei Guo et al.

Summary: This study presents a novel polymeric Cu-ligand core-shell microsphere for highly selective acetate production in CO2RR, with the suppression of H-2 evolution. The unique co-coordination mechanism and porous core structure facilitate the efficient conversion of CO2 to acetate product.

GREEN CHEMISTRY (2021)

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Review Energy & Fuels

Bridging the gap between highly active oxygen reduction reaction catalysts and effective catalyst layers for proton exchange membrane fuel cells

Jiantao Fan et al.

Summary: The impressive performance of low-platinum-loading oxygen reduction reaction catalysts in initial electrochemical tests is often not reflected in real fuel cells, leading researchers to explore strategies to address this issue.

NATURE ENERGY (2021)

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Article Chemistry, Physical

Core-shell-structured CNT@hydrous RuO2 as a H2/CO2 fuel cell cathode catalyst to promote CO2 methanation and generate electricity

Jixiang Hu et al.

Summary: In this study, a core-shell structure of CNT@hydrous RuO2 was fabricated to accelerate the CO2 methanation reaction and enhance methane production rate. CNT@hydrous RuO2, as a proton-electron mixed conductive material, effectively promotes catalytic reactions involving multiple proton-electron transfers.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

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Article Chemistry, Physical

Highly efficient CO2 electrolysis within a wide operation window using octahedral tin oxide single crystals

Hai Liu et al.

Summary: The study demonstrates that tuning octahedral tin oxide single crystals can improve formate selectivity and increase formate partial current density, while breaking the limitations of the scaling relationship on the surface of conventional SnO2 nanoparticles. On the surface of SnO2 (111), the catalytic activity is highest in seawater, achieving a maximum formate selectivity of 95%. Combining these catalysts with chlor-alkali electrolyzers can effectively convert CO2 into formate and produce Cl-2 simultaneously.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

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Review Chemistry, Multidisciplinary

High temperature proton exchange membrane fuel cells: progress in advanced materials and key technologies

Rizwan Haider et al.

Summary: High temperature proton exchange membrane fuel cells (HT-PEMFCs) have advantages such as fast reaction kinetics and high tolerance to impurities, but challenges like high cost and low durability hinder their practical applications. Researchers worldwide are focusing on exploring new materials and technologies to develop high-performance HT-PEMFCs. To facilitate further research and development of HT-PEMFCs, existing challenges are discussed and future research directions are proposed.

CHEMICAL SOCIETY REVIEWS (2021)

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Article Chemistry, Physical

Orientation of a bipolar membrane determines the dominant ion and carbonic species transport in membrane electrode assemblies for CO2 reduction

Marijn A. Blommaert et al.

Summary: A bipolar membrane can be used in reverse bias and forward bias in an electrochemical cell. The orientation of the BPM affects the environment of the CO2 reduction catalyst and ion transport mechanism. Reverse bias reduces CO2 crossover and cathodic potential, while forward bias shows lower CO selectivity and higher salt concentration.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

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Article Chemistry, Multidisciplinary

Promoting CO2 electroreduction on CuO nanowires with a hydrophobic Nafion overlayer

Mang Wang et al.

Summary: By modifying CuO nanowire electrodes with a thick Nafion overlayer, a hydrophobic electrode surface was constructed, which enhanced the selectivity of CO2 RR and suppressed HER activity. This work emphasizes the importance of hydrophobicity in the selectivity of CO2 reduction.

NANOSCALE (2021)

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Article Engineering, Chemical

An overview of the Department of Energy's CarbonSAFE Initiative: Moving CCUS toward commercialization

Mary Sullivan et al.

AICHE JOURNAL (2020)

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Article Multidisciplinary Sciences

Molecular tuning of CO2-to-ethylene conversion

Fengwang Li et al.

NATURE (2020)

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Review Chemistry, Multidisciplinary

CO2 Reduction: From Homogeneous to Heterogeneous Electrocatalysis

Sheng Zhang et al.

ACCOUNTS OF CHEMICAL RESEARCH (2020)

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Article Chemistry, Multidisciplinary

Electronic Redistribution: Construction and Modulation of Interface Engineering on CoP for Enhancing Overall Water Splitting

Lei Yang et al.

ADVANCED FUNCTIONAL MATERIALS (2020)

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Article Chemistry, Multidisciplinary

Boosting H2 Generation Coupled with Selective Oxidation of Methanol into Value-Added Chemical over Cobalt Hydroxide@Hydroxysulfide Nanosheets Electrocatalysts

Kun Xiang et al.

ADVANCED FUNCTIONAL MATERIALS (2020)

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Article Chemistry, Multidisciplinary

In Situ Reconstruction of a Hierarchical Sn-Cu/SnOx Core/Shell Catalyst for High-Performance CO2 Electroreduction

Ke Ye et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

Direct Evidence of Local pH Change and the Role of Alkali Cation during CO2 Electroreduction in Aqueous Media

Fen Zhang et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

Elucidating the Electrocatalytic CO2 Reduction Reaction over a Model Single-Atom Nickel Catalyst

Song Liu et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

Mechanistic Insights into Electroreductive C-C Coupling between CO and Acetaldehyde into Multicarbon Products

Xiaoxia Chang et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

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Article Chemistry, Multidisciplinary

Investigating the Origin of Enhanced C2+ Selectivity in Oxide-/Hydroxide-Derived Copper Electrodes during CO2 Electroreduction

Qiong Lei et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

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Article Nanoscience & Nanotechnology

Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface

Hongxia Wang et al.

NATURE NANOTECHNOLOGY (2020)

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Article Multidisciplinary Sciences

CO2 electrolysis to multicarbon products at activities greater than 1 A cm-2

F. Pelayo Garcia de Arquer et al.

SCIENCE (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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Article Chemistry, Physical

Controlling Speciation during CO2 Reduction on Cu-Alloy Electrodes

Xinyi Chen et al.

ACS CATALYSIS (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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Article Chemistry, Physical

Boosting CO2 Electroreduction to CH4 via Tuning Neighboring Single-Copper Sites

Anxiang Guan et al.

ACS ENERGY LETTERS (2020)

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Review Multidisciplinary Sciences

Strategies in catalysts and electrolyzer design for electrochemical CO2 reduction toward C2+ products

Lei Fan et al.

SCIENCE ADVANCES (2020)

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Article Chemistry, Physical

Catalyst synthesis under CO2 electroreduction favours faceting and promotes renewable fuels electrosynthesis

Yuhang Wang et al.

NATURE CATALYSIS (2020)

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Review Chemistry, Multidisciplinary

Stability and Degradation Mechanisms of Copper-Based Catalysts for Electrochemical CO2 Reduction

Stefan Popovic et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

Acid-Base Interaction Enhancing Oxygen Tolerance in Electrocatalytic Carbon Dioxide Reduction

Pengsong Li et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

Electrocatalytic Reduction of CO2 to Acetic Acid by a Molecular Manganese Corrole Complex

Ratnadip De et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

A Precious-Metal-Free Hybrid Electrolyzer for Alcohol Oxidation Coupled to CO2-to-Syngas Conversion

Mark A. Bajada et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Multidisciplinary

Electrochemical Reduction of CO2 to Ethane through Stabilization of an Ethoxy Intermediate

Anthony Vasileff et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020)

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Article Chemistry, Physical

Self-growing Cu/Sn bimetallic electrocatalysts on nitrogen-doped porous carbon cloth with 3D-hierarchical honeycomb structure for highly active carbon dioxide reduction

Luwei Peng et al.

APPLIED CATALYSIS B-ENVIRONMENTAL (2020)

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Article Chemistry, Physical

Crossover of liquid products from electrochemical CO2 reduction through gas diffusion electrode and anion exchange membrane

Jie Zhang et al.

JOURNAL OF CATALYSIS (2020)

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Article Multidisciplinary Sciences

Electrochemically scrambled nanocrystals are catalytically active for CO2-to-multicarbons

Yifan Li et al.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2020)

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Article Chemistry, Multidisciplinary

Electrocatalytic Reduction of CO2 to Ethylene by Molecular Cu-Complex Immobilized on Graphitized Mesoporous Carbon

Mani Balamurugan et al.

SMALL (2020)

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Article Chemistry, Physical

Mechanistic Investigation of Biomass Oxidation Using Nickel Oxide Nanoparticles in a CO2-Saturated Electrolyte for Paired Electrolysis

Seungwoo Choi et al.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2020)

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Article Multidisciplinary Sciences

Selective electroreduction of CO2 to acetone by single copper atoms anchored on N-doped porous carbon

Kun Zhao et al.

NATURE COMMUNICATIONS (2020)

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Article Chemistry, Physical

Facet-Dependent Selectivity of Cu Catalysts in Electrochemical CO2 Reduction at Commercially Viable Current Densities

Gian Luca De Gregorio et al.

ACS CATALYSIS (2020)

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Article Chemistry, Physical

Covalent Triazine Framework Confined Copper Catalysts for Selective Electrochemical CO2 Reduction: Operando Diagnosis of Active Sites

Lushan Ma et al.

ACS CATALYSIS (2020)

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Article Chemistry, Multidisciplinary

pH-Dependent Hydrogen and Water Binding Energies on Platinum Surfaces as Directly Probed through Surface-Enhanced Infrared Absorption Spectroscopy

Shangqian Zhu et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

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Article Chemistry, Multidisciplinary

Progress and Perspective for In Situ Studies of CO2 Reduction

Xiaodong Li et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

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Article Electrochemistry

Role of H2O for CO2 Reduction Reactions at Platinum/Electrolyte Interfaces in Imidazolium Room-Temperature Ionic Liquids

Bjoern Ratschmeier et al.

CHEMELECTROCHEM (2020)

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Article Chemistry, Physical

Managing Hydration at the Cathode Enables Efficient CO2 Electrolysis at Commercially Relevant Current Densities

Angelica Reyes et al.

ACS ENERGY LETTERS (2020)

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Article Chemistry, Physical

A Robust, Scalable Platform for the Electrochemical Conversion of CO2 to Formate: Identifying Pathways to Higher Energy Efficiencies

Yingying Chen et al.

ACS ENERGY LETTERS (2020)

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Article Energy & Fuels

Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation

Xue Wang et al.

NATURE ENERGY (2020)

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Article Multidisciplinary Sciences

Accelerated discovery of CO2 electrocatalysts using active machine learning

Miao Zhong et al.

NATURE (2020)

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Carbon dioxide (CO2) levels this century will alter the protein, micronutrients, and vitamin content of rice grains with potential health consequences for the poorest rice-dependent countries

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Activity and Selectivity Control in CO2 Electroreduction to Multicarbon Products over CuOx Catalysts via Electrolyte Design

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Steering post-C-C coupling selectivity enables high efficiency electroreduction of carbon dioxide to multi-carbon alcohols

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Selective formation of C2 compounds from electrochemical reduction of CO2 at a series of copper single crystal electrodes

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