☆ 4.6 Review

Recent advances in regulating the performance of acid oxygen reduction reaction on carbon-supported non-precious metal single atom catalysts

JOURNAL OF ENERGY CHEMISTRY (2023)

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Article Chemistry, Multidisciplinary

A durable half-metallic diatomic catalyst for efficient oxygen reduction

Hongguan Li et al.

Summary: By designing the catalyst Fe/Zn-N-C based on theoretical screening, a unique half-metallic electronic structure is achieved, resulting in enhanced O-2 capture and bonding. The catalyst exhibits impressive ORR activities and durability in both acidic and alkaline media.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

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Article Chemistry, Multidisciplinary

Altering Ligand Fields in Single-Atom Sites through Second-Shell Anion Modulation Boosts the Oxygen Reduction Reaction

Jiayi Qin et al.

Summary: Researchers successfully manipulate the structure and oxygen reduction reaction (ORR) performance of single-atom Ru-N-C catalysts using an S-anion coordination strategy, resulting in outstanding long-term durability and high activity. Metal-air batteries using this catalyst also exhibit fast kinetics and excellent stability.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

Fast identification of the stability of atomically dispersed bi-atom catalysts using a structure descriptor-based model

Danyang Li et al.

Summary: In this study, density functional theory was used to investigate the stability of N-doped graphene-supported BACs, and prediction models were constructed for the quick identification of highly stable BACs for different electrocatalytic reactions.

JOURNAL OF MATERIALS CHEMISTRY A (2022)

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Article Chemistry, Multidisciplinary

Facilitating the acidic oxygen reduction of Fe-N-C catalysts by fluorine-doping

Xiafang Tao et al.

Summary: The study introduces a synthetic method for fluorine-doped FeNC catalysts with improved ORR performance, showcasing higher E-1/2 values and durability. The utilization of PFTA surfactants leads to significant changes in catalyst structure, enhancing key properties such as surface area and FeNx sites.

MATERIALS HORIZONS (2022)

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Article Chemistry, Multidisciplinary

Integration of Morphology and Electronic Structure Modulation on Atomic Iron-Nitrogen-Carbon Catalysts for Highly Efficient Oxygen Reduction

Cuncun Xin et al.

Summary: This study demonstrates the effective and facile strategy of molten-salts mediated pyrolysis for modulation of morphology and electronic structure of Fe-N-C materials to prepare efficient Fe-N/C single-atom catalysts for oxygen reduction reactions. The enhanced ORR activity is governed by axially bound Cl in FeN4Cl moieties as isolated active centers. Theoretical calculations rationalize the finding of accelerated pathway kinetics and tuning of potential determining step through coordination-engineered strategy.

ADVANCED FUNCTIONAL MATERIALS (2022)

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Article Chemistry, Multidisciplinary

Construction of N, P Co-Doped Carbon Frames Anchored with Fe Single Atoms and Fe2P Nanoparticles as a Robust Coupling Catalyst for Electrocatalytic Oxygen Reduction

Yuan Pan et al.

Summary: A coupling catalyst with highly dispersed N, P co-doped carbon frames anchored with Fe single atoms and Fe2P nanoparticles has been synthesized for the electrocatalytic oxygen reduction reaction. The optimized catalyst shows superior activity and stability in acidic and alkaline media, and theoretical calculations reveal a synergistic effect of Fe2P and doped P atoms. The study provides a novel idea for constructing high-efficiency ORR electrocatalysts with atomic-level precision.

ADVANCED MATERIALS (2022)

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Article Chemistry, Physical

Interface engineering of plasmonic induced Fe/N/C-F catalyst with enhanced oxygen catalysis performance for fuel cells application

Xue Yin et al.

Summary: In this study, the interface engineering of plasmonic induced Fe/N/C-F catalyst was demonstrated to enhance oxygen reduction performance for fuel cells applications. The strong interaction between F and Fe-N-4 active sites modified the catalyst interfacial properties, resulting in improved electronic structure and super-hydrophobicity. The hybrid contribution from active sites and carbon support efficiently optimized the three-phase microenvironment in the catalysis electrode, facilitating efficient oxygen reduction performance and practical application in fuel cells.

NANO RESEARCH (2022)

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Article Chemistry, Physical

Geometrically Deformed Iron-Based Single-Atom Catalysts for High-Performance Acidic Proton Exchange Membrane Fuel Cells

Lei Shi et al.

Summary: This article proposes a simple but efficient method to synthesize a geometrically deformed single Fe site catalyst by trace NaCl-coating-assisted pyrolysis of Fe-containing zeolitic imidazolate frameworks. The newly developed catalysts exhibit improved oxygen reduction reaction (ORR) performance due to the significantly exposed active sites and enhanced mass transport. The enhanced intrinsic activity is attributed to the synergy of deformed Fe-N-4 moieties and the surrounding graphitic N dopant. Additionally, the locally increased graphitization can efficiently reduce carbon corrosion, thereby promoting catalyst stability.

ACS CATALYSIS (2022)

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Review Chemistry, Applied

MOFs fertilized transition-metallic single-atom electrocatalysts for highly-efficient oxygen reduction: Spreading the synthesis strategies and advanced identification

Kexin Song et al.

Summary: MOFs have been widely used for the preparation of transition-metallic single-atom electrocatalysts (TM-SACs), which have achieved great progress in terms of high activity, high loading, and high stability. Different strategies for preparing and modifying TM-SACs using MOFs have been summarized to guide the development of TM-SACs with optimal performance.

JOURNAL OF ENERGY CHEMISTRY (2022)

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Review Chemistry, Physical

Exploring Durable Single-Atom Catalysts for Proton Exchange Membrane Fuel Cells

Xin Wan et al.

Summary: This review explores the structure-stability relationship of Fe-N-C catalysts, providing valuable guidance for improved stability. Recent achievements include the discovery of several site-specific degradation mechanisms and identification of intrinsically stable active sites, and the discussion of Fe-free single-atom catalysts as an alternative solution.

ACS ENERGY LETTERS (2022)

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Article Chemistry, Physical

High loading of single atomic iron sites in Fe-NC oxygen reduction catalysts for proton exchange membrane fuel cells

Asad Mehmood et al.

Summary: This study demonstrates the achievement of high active site density in non-precious iron-based catalysts by exchanging iron into a preformed carbon-nitrogen matrix, coordinated solely as single-atom Fe-N-4 sites. The catalyst shows excellent performance in proton exchange membrane fuel cells, delivering high current densities and turnover frequency.

NATURE CATALYSIS (2022)

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Article Chemistry, Multidisciplinary

Facet Strain Strategy of Atomically Dispersed Fe-N-C Catalyst for Efficient Oxygen Electrocatalysis

Yang Yuan et al.

Summary: Increasing the portion of highly active metal centers in M-N-C catalysts is crucial for enhancing the overall performance of the oxygen reduction reaction (ORR). A facet strain strategy using a trans-layer compressive strain is proposed, which effectively activates the primitive FeN4 catalytic centers. The redesigned catalyst with compressed Fe-N bonds exhibits improved ORR activity compared to the conventional Fe-N-C and commercial Pt/C benchmarks.

ADVANCED FUNCTIONAL MATERIALS (2022)

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Article Chemistry, Multidisciplinary

Identification of the Highly Active Co-N4 Coordination Motif for Selective Oxygen Reduction to Hydrogen Peroxide

Shanyong Chen et al.

Summary: The research reveals that pyrrole-type CoN4 and pyridine-type CoN4 are responsible for 2e- ORR and 4e- ORR reactions, respectively. Pyrrole-type CoN4 catalyst exhibits excellent H2O2 selectivity and yield in acid media. This study is significant for understanding the structure-function relationship of Co-N4 single-atom catalysts and improving H2O2 production.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

Identification of a Robust and Durable FeN4Cx Catalyst for ORR in PEM Fuel Cells and the Role of the Fifth Ligand

Parisa Nematollahi et al.

Summary: In this study, the electronic structures of three FeN4 catalytic centers with different local topologies were investigated using first-principles calculations. The mechanism of their ORR activity in acidic electrolytes was unraveled, with a focus on a forgotten synthetic pyridinic Fe-N coordination. The study demonstrates that this catalyst can exhibit excellent activity for promoting direct four-electron ORR by adding a fifth ligand. Sites with good stability properties were also identified through the use of calculations and spectroscopy data.

ACS CATALYSIS (2022)

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Article Chemistry, Physical

Probing the Oxygen Reduction Reaction Intermediates and Dynamic Active Site Structures of Molecular and Pyrolyzed Fe-N-C Electrocatalysts by In Situ Raman Spectroscopy

Jie Wei et al.

Summary: This study reveals the identification of ORR intermediates and RDSs at different active sites through Raman spectroscopy of FeN4 active sites, and the dynamic structural changes of FeN4 during ORR catalysis. It also confirms the role of two types of C-N sites in pyrolyzed Fe-N-C catalysts, showing different ORR intermediates and RDSs.

ACS CATALYSIS (2022)

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Article Energy & Fuels

Atomically dispersed iron sites with a nitrogen-carbon coating as highly active and durable oxygen reduction catalysts for fuel cells

Shengwen Liu et al.

Summary: In this study, a highly durable and active Fe-N-C catalyst was synthesized by depositing a thin layer of nitrogen-doped carbon on the catalyst surface. The stability improvement of the catalyst can overcome the cost barriers of hydrogen fuel cells.

NATURE ENERGY (2022)

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Article Chemistry, Multidisciplinary

Identification of the Catalytically Dominant Iron Environment in Iron- and Nitrogen-Doped Carbon Catalysts for the Oxygen Reduction Reaction

Lingmei Ni et al.

Summary: By using Mossbauer spectroscopy and quantum chemistry, researchers have established an active site model for metal-and nitrogen-doped carbon catalysts obtained through pyrolysis. They found that pyrrolic nitrogen coordination is the active site, and identified a previously unknown intermediate.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

Multilevel Computational Studies Reveal the Importance of Axial Ligand for Oxygen Reduction Reaction on Fe-N-C Materials

Phillips Hutchison et al.

Summary: This study investigates the oxygen reduction reaction (ORR) mechanism of Fe-N-C materials in fuel cell applications using a multilevel computational approach. The research identifies the potential-limiting step of ORR and validates the active site model by experimental measurements. It also emphasizes the significance of solvent-substrate interactions and surface charge effects in understanding the PCET reaction mechanism.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

Molecular Degradation of Iron Phthalocyanine during the Oxygen Reduction Reaction in Acidic Media

Liyang Wan et al.

Summary: This study investigates the degradation mechanism of molecular iron phthalocyanine (FePc) during the acidic oxygen reduction reaction (ORR) and provides important insights for understanding the performance degradation of practical Fe/N/C catalysts.

ACS CATALYSIS (2022)

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Article Chemistry, Multidisciplinary

Tuning Fe Spin Moment in Fe-N-C Catalysts to Climb the Activity Volcano via a Local Geometric Distortion Strategy

Ruguang Wang et al.

Summary: In this work, the authors report for the first time the introduction of chalcogen oxygen groups as polar functional groups to break the symmetry of the FeN4 active center in Fe-N-C catalysts, thereby enhancing their oxygen reduction reaction activity. The study provides a new strategy for tuning the local coordination and electronic structure of single-atom catalysts.

ADVANCED SCIENCE (2022)

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Article Chemistry, Multidisciplinary

Seizing gaseous Fe2+ to densify O2-accessible Fe-N4 sites for high-performance proton exchange membrane fuel cells

Shu-Hu Yin et al.

Summary: Increasing the density of Fe-N-4 sites in Fe-N-C materials can enhance the kinetics of the oxygen reduction reaction in proton exchange membrane fuel cells. A surface-rich pyridinic-N carbon substrate has been shown to be more favorable for forming surface Fe-N2+2 sites with superior intrinsic activity. These structural advantages contribute to the high performance of Fe-g-NC/Phen in fuel cells.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

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Article Chemistry, Multidisciplinary

Highly accessible and dense surface single metal FeN4 active sites for promoting the oxygen reduction reaction

Guangbo Chen et al.

Summary: The study successfully constructed catalysts with densely exposed surface FeN4 moieties on hierarchically porous carbon, which exhibited excellent ORR activity in acidic media and promising performance in proton exchange membrane fuel cells.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

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Review Chemistry, Applied

Recent advances in spinel-type electrocatalysts for bifunctional oxygen reduction and oxygen evolution reactions

Xiao-Meng Liu et al.

Summary: The demand for efficient and environmentally-benign electrocatalysts is rapidly increasing, with a focus on high-performance bifunctional oxygen electrocatalysts. Spinel-type catalysts, with their versatility and advantages, have garnered attention in the field. This review provides insights into the design of spinel-type bifunctional oxygen electrocatalysts, emphasizing the relationship between structure and property.

JOURNAL OF ENERGY CHEMISTRY (2021)

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Article Chemistry, Multidisciplinary

Turning on Zn 4s Electrons in a N2-Zn-B2 Configuration to Stimulate Remarkable ORR Performance

Jing Wang et al.

Summary: A newly explored zinc-based single-atom catalyst with a unique N-2-Zn-B-2 configuration demonstrates impressive ORR activity and remarkable long-term stability, achieved through manipulating the s-band by constructing a B,N co-coordinated Zn-B/N-C catalyst.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Tuning the p-Orbital Electron Structure of s-Block Metal Ca Enables a High-Performance Electrocatalyst for Oxygen Reduction

Zhiyu Lin et al.

Summary: This study reports a carbon catalyst with a single calcium atom coordinated with N and O, exhibiting exceptional ORR activities under both acidic and alkaline conditions, as well as outstanding performance in zinc-air battery. The high catalytic activity of main-group calcium is attributed to its electron structure being regulated by N and O coordination, facilitating the adsorption of ORR intermediates and electron transfer.

ADVANCED MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Dynamically Unveiling Metal-Nitrogen Coordination during Thermal Activation to Design High-Efficient Atomically Dispersed CoN4 Active Sites

Yanghua He et al.

Summary: The structural evolution of CoN4 sites during thermal activation was studied using a ZIF-8-derived carbon host. It was found that the critical transition occurs at 700 degrees C with optimal conversion at 900 degrees C, resulting in the highest intrinsic activity and four-electron selectivity for the ORR.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Review Chemistry, Inorganic & Nuclear

Molecular-MN4 vs atomically dispersed M-N4-C electrocatalysts for oxygen reduction reaction

Anuj Kumar et al.

Summary: This article highlights the motivation for developing efficient O-2 electrocatalysts and the application of molecular electrocatalysts, pointing out the challenges in activity and durability of M-N-4-C materials, and introduces ways to optimize their performance through chemical treatment.

COORDINATION CHEMISTRY REVIEWS (2021)

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Article Multidisciplinary Sciences

Anomalous collapses of Nares Strait ice arches leads to enhanced export of Arctic sea ice

G. W. K. Moore et al.

Summary: Ice arches at the northern and southern ends of Nares Strait, a key passage in the Arctic, are forming for shorter durations, leading to increased ice transport and accelerating the export of multi-year ice.

NATURE COMMUNICATIONS (2021)

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Article Chemistry, Physical

Atomic Fe Dispersed Hierarchical Mesoporous Fe-N-C Nanostructures for an Efficient Oxygen Reduction Reaction

Yu Zhou et al.

Summary: Due to the scarcity and high cost of precious metals, the hydrogen economy may rely on non-platinum-group-metal catalysts. A study found that a stabilized single-atom Fe and N co-doped ordered mesoporous carbon nanosphere catalyst exhibits excellent activity and durability, surpassing the current state-of-the-art Pt/C electrocatalysts.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Identification of durable and non-durable FeNx sites in Fe-N-C materials for proton exchange membrane fuel cells

Jingkun Li et al.

Summary: Fe-N-C materials show promise as an alternative to platinum in acidic polymer fuel cells, but limited understanding of their operando degradation hinders rational approaches to improved durability. Two distinct FeNx sites in the catalysts degrade differently during the oxygen reduction reaction, with one site substantially contributing after 50 hours of operation.

NATURE CATALYSIS (2021)

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Article Chemistry, Multidisciplinary

Electronic Spin Moment As a Catalytic Descriptor for Fe Single-Atom Catalysts Supported on C2N

Wenhui Zhong et al.

Summary: The study reveals that the catalytic activity of Fe single-atom supported on C2N for oxygen reduction reaction is influenced by the spin states. Manipulation of the spin states can effectively tune the catalytic activity, with the potential to design transition metal single-atom catalysts with improved performance.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Physical

Impact of Heterometallic Cooperativity of Iron and Copper Active Sites on Electrocatalytic Oxygen Reduction Kinetics

Masaru Kato et al.

Summary: A Cu-, Fe-, and N-doped carbon nanotubes ORR electrocatalyst, (Cu,Fe)-N-CNT, was synthesized in this study, which showed a selective 4e(-) reduction efficiency of O-2 to H2O2 of about 99%, demonstrating higher catalytic activity and selectivity compared to other non-PGM catalysts. The research findings suggest that heterometallic cooperation has a significant impact on the ORR kinetics.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Acid-Stable and Active M-N-C Catalysts for the Oxygen Reduction Reaction: The Role of Local Structure

Tipaporn Patniboon et al.

Summary: This study systematically investigated the catalytic activity and stability of metal-nitrogen carbon catalysts in acidic conditions using density functional theory, identifying acid-stable and active MNx structures for oxygen reduction reaction. The findings provide helpful guidance for the rational modification of carbon matrices hosting MNx moieties and the selection of metal atoms to optimize activity and stability in the ORR.

ACS CATALYSIS (2021)

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Article Chemistry, Physical

Phosphorus-Driven Electron Delocalization on Edge-Type FeN4 Active Sites for Oxygen Reduction in Acid Medium

Hengbo Yin et al.

Summary: This study demonstrates that incorporating long-range P into FeN4 sites can enhance electron delocalization and significantly improve the catalytic activity for oxygen reduction reaction. The presence of P results in a lower free energy barrier, leading to superior performance in both acidic and alkaline media, showcasing a potential alternative to Pt/C catalysts in fuel cells and batteries.

ACS CATALYSIS (2021)

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Article Energy & Fuels

New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan Gao et al.

Summary: Fe-N-C catalyst, known for its high ORR activity and low cost, faces durability challenges due to the formation of H2O2 during the 2e(-) pathway in the ORR process. This study provides insights into the effect of potential on catalyst degradation, revealing that the combination of electrochemical and chemical oxidation triggers the highest H2O2 release rate at 0.6 V.

FRONTIERS IN ENERGY (2021)

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Article Chemistry, Multidisciplinary

Promoting Atomically Dispersed MnN4 Sites via Sulfur Doping for Oxygen Reduction: Unveiling Intrinsic Activity and Degradation in Fuel Cells

Lin Guo et al.

Summary: A sulfur-doped Mn-N-C catalyst was synthesized through an effective adsorption-pyrolysis process, exhibiting favorable oxygen reduction reaction (ORR) activity in acidic media. The catalyst showed enhanced performance and stability in comparison to the S-free catalyst, with insights provided into catalyst degradation associated with Mn oxidation and agglomeration. The promoted ORR activity was mainly attributed to the spatial effect from the repulsive interaction between the ORR intermediates and adjacent S dopants.

ACS NANO (2021)

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Article Chemistry, Multidisciplinary

Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres

Cheng Tang et al.

Summary: This study demonstrates that the molecular-level local structure, including first and second coordination spheres, plays a critical role in determining the selectivity of catalytic reactions. By modifying the first and second coordination spheres of Co-SACs, it is possible to tailor the oxygen reduction reaction selectivity. The unique selectivity change originates from the structure-dependent shift of active sites, leading to improved activity and selectivity for acidic H2O2 electrosynthesis.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Physical

Single Atomic Cerium Sites with a High Coordination Number for Efficient Oxygen Reduction in Proton-Exchange Membrane Fuel Cells

Mengzhao Zhu et al.

Summary: The study introduces a hard-template method to synthesize rare-earth single cerium-atom-doped metal-organic frameworks with a hierarchically macro-meso-microporous structure, demonstrated by spherical aberration correction electron microscopy. The Ce sites embedded in the hierarchically macromeso-microporous N-doped carbon catalyst show high half-wave potential and power density in the oxygen reduction reaction.

ACS CATALYSIS (2021)

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Article Chemistry, Applied

Insights into efficient transition metal-nitrogen/carbon oxygen reduction electrocatalysts

Hao-Yu Wang et al.

Summary: The importance of accelerating the sluggish oxygen reduction reaction (ORR) process at the cathode with earth-abundant metal-based catalysts for the commercialization of low-temperature polymer electrolyte membrane fuel cells is discussed. Transition metal-nitrogen-carbon (M-N/C) catalysts are considered as the most promising non-precious metal catalysts for ORR, due to their high catalytic activity, long-term stability, and low cost. Different M-N/C catalysts classified by precursors and strategies for design and optimization are highlighted, along with the challenges and possible opportunities for future development of high-performance ORR catalysts.

JOURNAL OF ENERGY CHEMISTRY (2021)

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Article Chemistry, Multidisciplinary

Hydrogen Passivation of M-N-C (M = Fe, Co) Catalysts for Storage Stability and ORR Activity Improvements

Jieyuan Liu et al.

Summary: Long-term exposure of M-N-C catalysts in air causes surface oxidation and hydroxylation, leading to decreased ORR activity and fuel-cell performances. Hydrogen passivation protects active sites and improves storage stability of the catalysts.

ADVANCED MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Improving the Stability of Non-Noble-Metal M-N-C Catalysts for Proton-Exchange-Membrane Fuel Cells through M-N Bond Length and Coordination Regulation

Zhengpei Miao et al.

Summary: An effective strategy is developed to enhance the stability of non-noble-metal catalysts in fuel cells by improving the bonding strength between metal ions and chelating polymers. The optimized catalyst exhibits outstanding activity and stability in both half-cell and fuel cell cathodes, with near 100% retention of current density for an extended period. The study suggests that the Fe-N-4/C site can strongly stabilize Fe centers against demetalation, providing insights for further catalyst design.

ADVANCED MATERIALS (2021)

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Review Chemistry, Multidisciplinary

Emerging Dual-Atomic-Site Catalysts for Efficient Energy Catalysis

Weiyu Zhang et al.

Summary: Atomically dispersed metal catalysts with well-defined structures have been a research hotspot in heterogeneous catalysis. Dual-atomic-site catalysts, as an extension of single-atom catalysts, possess higher metal loading and more flexible active sites, offering the potential for better catalytic performance.

ADVANCED MATERIALS (2021)

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Article Chemistry, Multidisciplinary

An Adjacent Atomic Platinum Site Enables Single-Atom Iron with High Oxygen Reduction Reaction Performance

Ali Han et al.

Summary: The modulation effect can enhance the catalytic activity of Fe-N-4 moiety through adjacent Pt-N-4 moiety, but it is less effective for optimizing the ORR performances of Co-N-4/Pt-N-4 and Mn-N-4/Pt-N-4 systems.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Pyrolysis-Free Synthesized Catalyst towards Acidic Oxygen Reduction by Deprotonation

Ying Zang et al.

Summary: The research team successfully synthesized a catalyst for oxygen reduction in acidic conditions using a pyrolysis-free route, achieving outstanding performance and stability. This finding provides new insights into optimizing catalysts for practical applications and mechanistic studies.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Origin of Selective Production of Hydrogen Peroxide by Electrochemical Oxygen Reduction

Xunhua Zhao et al.

Summary: This study identified factors affecting the selectivity of the oxygen reduction reaction and developed a new model to simulate the electrochemical reaction kinetics at the solid-water interface.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Physical

Chemical vapour deposition of Fe-N-C oxygen reduction catalysts with full utilization of dense Fe-N4 sites

Li Jiao et al.

Summary: Replacing scarce and expensive platinum with metal-nitrogen-carbon (M-N-C) catalysts for the oxygen reduction reaction in proton exchange membrane fuel cells has been impeded by the low active site density and site utilization of M-N-C. These limitations have now been overcome by implementing trans-metalation of Zn-N-4 sites into Fe-N-4 sites.

NATURE MATERIALS (2021)

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Article Chemistry, Physical

Spin-State-Dependent Peroxymonosulfate Activation of Single-Atom M-N Moieties via a Radical-Free Pathway

Jie Miao et al.

Summary: Transition metal catalysts anchored on carbon nanotubes were developed to efficiently activate peroxymonosulfate for nonradical oxidation. The study found that the spin state of the catalyst strongly influenced its catalytic activity, with higher spin states promoting electron transfer and enhancing the oxidation capacity of reactive species. These findings advance the mechanistic understanding of transition metal-mediated persulfate activation and contribute to the development of efficient spintronic catalysts for environmental applications.

ACS CATALYSIS (2021)

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Review Chemistry, Physical

Molecular Control of Carbon-Based Oxygen Reduction Electrocatalysts through Metal Macrocyclic Complexes Functionalization

Yaoshuai Hong et al.

Summary: Fuel cells and metal-air batteries have great potential for sustainable energy technologies due to their zero pollution and high efficiency. However, the high cost and scarcity of Pt-based materials as cathode catalysts limit their scalability. Recent progress in nonprecious-metal catalysts has addressed some of these challenges.

ADVANCED ENERGY MATERIALS (2021)

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Article Chemistry, Applied

Single-atom catalysts with anionic metal centers: Promising electrocatalysts for the oxygen reduction reaction and beyond

Jinxing Gu et al.

Summary: Ongoing efforts focus on developing single-atom catalysts (SACs) for oxygen reduction reaction (ORR) with anionic metal centers, which shows promising performance. Anionic Au and Co metal centers exhibit comparable or better limiting potentials towards ORR than conventional Pt-based catalysts. Additionally, anionic Os and Re metal centers can electrochemically catalyze the nitrogen reduction reaction (NRR) with potential close to that of Ru(0001).

JOURNAL OF ENERGY CHEMISTRY (2021)

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Article Chemistry, Multidisciplinary

Nano-geometric deformation and synergistic Co nanoparticles-Co-N4 composite sites for proton exchange membrane fuel cells

Xiaoyang Cheng et al.

Summary: A novel strategy was developed to enhance the ORR activity of Co single-atom catalysts by introducing a deformed CoN4 site and Co nanoparticle-CoN4 composite sites, which effectively replenished the total density of CoN4. The resulting concave nanocube-like catalyst exhibited excellent ORR performance and high power density in acidic media, with theoretical studies confirming the enhanced O-2 activation and reduced carbon layer erosion. This research not only provides a new approach to develop ORR catalysts, but also contributes to a deeper understanding of ORR fundamentals.

ENERGY & ENVIRONMENTAL SCIENCE (2021)

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Review Chemistry, Physical

Advanced Atomically Dispersed Metal-Nitrogen-Carbon Catalysts Toward Cathodic Oxygen Reduction in PEM Fuel Cells

Yijie Deng et al.

Summary: Research shows that atomically dispersed metal-nitrogen-carbon catalysts have significant potential in improving the oxygen reduction reaction and membrane electrode assembly performance of proton exchange membrane fuel cells, indicating promising avenues for addressing current bottlenecks in hydrogen energy conversion.

ADVANCED ENERGY MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Theoretically probing the possible degradation mechanisms of an FeNC catalyst during the oxygen reduction reaction

Na Yang et al.

Summary: The stability issue of the FeNC catalyst in fuel cells has hindered its practical application, with research revealing that Fe site oxidation during the oxygen reduction reaction can lead to irreversible damage to the FeN4 moiety. A trade-off potential was proposed to describe the anti-oxidation abilities of the TM site in the TMNX moiety during the ORR, highlighting the competitive relationship between catalyzing the ORR and Fe site oxidation.

CHEMICAL SCIENCE (2021)

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Review Chemistry, Multidisciplinary

Pyrolyzed M-Nx catalysts for oxygen reduction reaction: progress and prospects

Ergui Luo et al.

Summary: Recent research efforts on cost-effective catalysts in fuel cells, especially on the cathode, have shown promising advancements in the development of M-N-x/C materials. The focus has been on clarifying the nature of catalytic sites and utilizing advanced characterization tools to optimize synthesis methodologies. Future directions aim to achieve rational and controllable synthesis of catalysts with sufficient active sites and strategies to mitigate catalyst degradation.

ENERGY & ENVIRONMENTAL SCIENCE (2021)

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Article Chemistry, Physical

Atomic Fe-Zn dual-metal sites for high-efficiency pH-universal oxygen reduction catalysis

Jie Xu et al.

Summary: The study demonstrated the preparation of Fe-Zn-SA/NC catalyst for efficient ORR reaction in all pH range, showing high half-wave potentials and stability, comparable to Pt/C. The Fe-Zn-SA/NC catalyst also exhibited high power density and durability when assembled into a Zn-air battery, indicating its potential for real energy-related devices. The theoretical calculations attribute the superior catalytic activity of Fe-Zn-SA/NC to the lower energy barriers of ORR at the Fe-Zn-N-6 centers, offering new insights for dual-atom catalysts in energy conversion related catalytic reactions.

NANO RESEARCH (2021)

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Hierarchically Ordered Porous Carbon with Atomically Dispersed FeN4 for Ultraefficient Oxygen Reduction Reaction in Proton-Exchange Membrane Fuel Cells

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