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Article
Chemistry, Physical
Rui Yuan et al.
Summary: We synthesized two asymmetric metalloporphyrin molecules, A-Cb-CoPor and A-TPA-CoPor, and coated them on carbon black as oxygen reduction reaction (ORR) electrocatalysts. We found that A-TPA-CoPor/C showed better ORR activity and selectivity compared to A-Cb-CoPor/C, mainly due to the structural advantages of the TPA unit. Additionally, both asymmetric porphyrin-based composites exhibited greater limiting current densities than CoPor1/C, which was attributed to the reduced charge transfer resistance.
MOLECULAR CATALYSIS
(2023)
Review
Chemistry, Physical
Li Zhang et al.
Summary: The development of cost-effective, robust, and durable electrocatalysts to replace expensive Pt-based catalysts in the oxygen reduction reaction (ORR) is a major research focus in renewable energy and electrocatalysis. Metal-nitrogen-carbon (M-N-C) single atom catalysts (SACs) have gained particular attention due to their high atom utilization efficiency, biomimetic active sites, and distinct electronic structure. This review provides a comprehensive summary of recent advancements in the microenvironment regulation of M-N-C SACs for improved ORR performance, including coordination environment manipulation, long-range substrate modulation, and the synergy between nanoparticles and single atom sites. The challenges and outlook in the development of M-N-C SACs are also discussed.
Article
Nanoscience & Nanotechnology
Lei Zhao et al.
Summary: In this study, small-sized PtZn alloy nanoparticles supported on a porous carbon nanofiber were prepared using an electrospinning strategy. The optimized catalyst exhibited excellent ORR activity and durability, attributed to the enhanced interaction between nanoparticles and the carbon support, inhibiting the migration and aggregation of nanoparticles during the ORR process.
NANO MATERIALS SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Shi-Yi Lin et al.
Summary: In this study, ZnCo dual-atomic sites were incorporated in hierarchical N-doped carbon via a one-step bio-inspired pyrolysis. The resulting ZnCo-N-x system exhibited excellent catalytic characteristics for the ORR. The assembled Zn-air battery showed a maximum power density of 123.7 mW cm(-2) and robust stability.
Review
Chemistry, Multidisciplinary
Chen Gao et al.
Summary: This review highlights the significance of exploring highly active and stable electrocatalysts with earth-abundant metal centers for the oxygen reduction reaction (ORR). The focus is on the synthetic strategies and design principles of metal-N-C (M-N-C) electrocatalysts derived from zeolite imidazolate framework (ZIF) for efficient ORR catalysis. The review discusses methods to improve intrinsic ORR activity, such as coordination structures, doping metal-free heteroatoms, and edge-hosted structures, as well as strategies to increase active site density, including formation of M-N complexes and porous structure design.
Article
Chemistry, Multidisciplinary
Lishan Peng et al.
Summary: This study reports the development of FeN4-O-NCR catalysts with excellent intrinsic activity for alkaline ORR by optimizing the intrinsic ORR activity of Fe single-atom sites. The catalyst demonstrates outstanding performance in electrochemical tests, outperforming existing catalysts, and exhibits high power density when used in a zinc-air battery.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Physical
Shuai Yang et al.
Summary: This study presents a novel strategy to fabricate 2D carbon nanorods from COFs and investigates their catalytic performance in the oxygen reduction reaction. The resulting catalyst exhibits high catalytic activity and provides new insights into the development of single atom catalysts.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Multidisciplinary
Chen Feng et al.
Summary: The study shows that by controlling the positions of single atoms, efficient electron transfer between Ir and Co tunes the adsorption strength of oxygenated intermediates, leading to improved efficiency in the oxygen evolution reaction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Jingjing Li et al.
Summary: This study demonstrates the use of a special ultrathin nitrogen-doped graphene nanomesh as a scaffold for highly exposed Fe-N-4 active sites. By adjusting the pore sizes of the nanomesh, highly loaded single-atom catalysts can be synthesized, which exhibit superior performance in oxygen reduction reactions and fuel cell tests. This work provides a novel strategy for constructing highly exposed transition metals and nitrogen co-doped carbon materials catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Hao Zhang et al.
Summary: A ball-milling method was used to synthesize Cu-based single-atom catalysts (SACs) embedded in S,N-codoped nanocarbon (M-NSDC, M = Cu, Fe, Co, Ni, Mn, Pt, and Pd) in this study. The Cu-NSDC SACs exhibited high electrochemical activity for the oxygen reduction reaction (ORR), excellent stability, and electrocatalytic selectivity. Density functional theory (DFT) calculations revealed that the desorption of OH* intermediates was the rate-determining step over Cu-NSDC.
Article
Chemistry, Multidisciplinary
Huizhu Cai et al.
Summary: This study investigates the strategy of enhancing the electrocatalytic oxygen reduction reaction (ORR) performance by modulating the local environment and density of FeN4 active sites. The results show that by integrating a second metal Mn with Fe to construct Fe&Mn/N-C catalysts, the density of FeN4 active sites can be enhanced and the electronic structure can be modulated, leading to a decrease in the energy barrier of ORR and improved ORR performance.
Article
Multidisciplinary Sciences
Zhirong Zhang et al.
Summary: This study investigates the influence of different anchoring sites on the oxygen-evolving electrocatalysis by selectively anchoring iridium single atoms onto different positions on a defective CoOOH surface. The results show that the electronic interaction between the single-atom iridium and the support modifies the electronic structure of the active center in Ir-1/T-O-CoOOH, while a hydrogen bonding stabilizes the intermediates and lowers the energy barrier in Ir-1/V-O-CoOOH. This indicates that the homogeneity of single-atom catalysts is not only determined by their structures, but also by the localized coordination environments.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Fei Xiao et al.
Summary: Researchers have designed a hybrid electrocatalyst consisting of atomically dispersed platinum and iron single atoms, as well as platinum-iron alloy nanoparticles. This electrocatalyst exhibits higher activity and durability in proton exchange membrane fuel cells.
Article
Chemistry, Physical
Rifael Z. Snitkoff-Sol et al.
Summary: Studying catalyst degradation during fuel cell operation is crucial for addressing durability issues. In this study, a new electrochemical method was reported to accurately quantify the electrochemically active site density of PGM-free catalysts and track their degradation in situ during fuel cell operation.
Article
Chemistry, Physical
Syed Shoaib Ahmad Shah et al.
Summary: The worldwide emission of greenhouse gases has sparked increased research interest in sustainable energy conversion and storage devices. Single-atom catalysts (SACs) as electrode materials have shown potential and play a role in solving the bottleneck problems of next-generation energy storage systems.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Wenjing Zhang et al.
Summary: This study presents an anchoring-carbonization strategy for immobilizing ultrafine high-entropy Pt alloy nanocrystals (HENs) in porous carbon, which enhances the anchor strength and inhibits the migration and size growth of HENs. The resulting material exhibits superior activity and durability in electrocatalytic oxygen reduction reaction (ORR), showing promising potential for various applications.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Bingqing Wang et al.
Summary: This study investigates the site distance effect on the catalytic reactivity of single-atom catalysts. The optimized distance between copper atoms matches with the molecular size of the reactant, resulting in the most efficient catalyst for the oxidation of organic contaminants.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Honghui Ou et al.
Summary: Single-atom active-site catalysts have attracted significant attention in the field of photocatalytic CO2 conversion. However, designing active sites for CO2 reduction and H2O oxidation simultaneously on a photocatalyst and combining the corresponding half-reaction in a photocatalytic system is still difficult. In this study, a bimetallic single-atom active-site photocatalyst with two compatible active centers of Mn and Co was synthesized. The active center of Mn promotes H2O oxidation by accumulating photogenerated holes, while the active center of Co enhances CO2 activation by modifying the bond length and bond angle of CO2 molecules. The synthesized Mn1Co1/CN catalyst exhibited a significantly higher CO production rate compared to the corresponding single-metal active-site photocatalyst due to the synergistic effect of the atomic active centers.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Hao Jiang et al.
Summary: In this study, a bifunctional electrocatalyst composed of individually dispersed Ni single atoms on N-doped carbon nanosheets (Ni SAs-NC) was synthesized and demonstrated to exhibit outstanding performance for both oxygen reduction reaction (ORR) and urea oxidation reaction (UOR). By coupling ORR with UOR of low thermodynamic potential, a urea-assisted rechargeable Zn-air battery (ZAB) with significantly decreased charging voltage and high urea elimination rate was achieved. The high bifunctional electrocatalytic activities of Ni SAs-NC resulted in a dramatically increased energy conversion efficiency of 71.8%, improving conventional ZABs by 17.1%. This successful implementation of Ni SAs-based urea-assisted ZABs with improved energy conversion efficiency may advance practical applications of ZAB technology.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Multidisciplinary
Mengtian Zhang et al.
Summary: In this study, highly active single-atom catalysts (SACs) for oxygen reduction reaction (ORR) were explored using density functional theory (DFT) calculations and experimental synthesis. Co SACs showed the best ORR activity, comparable to platinum catalysts. X-ray absorption fine structure (XAFS) spectra confirmed that atomically dispersed Co-N-4 sites were the active sites. Additionally, the catalyst exhibited outstanding performance in a zinc-air battery.
Article
Chemistry, Physical
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.
Article
Energy & Fuels
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.
Article
Chemistry, Physical
Hanxu Yao et al.
Summary: Ru single atoms coupled with nanoclusters on hierarchical porous N-doped carbon exhibit high efficiency for hydrogen evolution reaction, with superior performance in alkaline and acidic conditions. These catalysts offer higher mass activity and lower cost for hydrogen production compared to commercial Pt/C, proving their industrial advantages.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Zhijun Li et al.
Summary: This study presents a straightforward high-temperature quenching method to construct isolated palladium atoms supported on cubic indium oxide catalyst. The palladium catalyst shows exceptional catalytic efficiency in the selective hydrogenation of nitrobenzene and exhibits excellent recyclability, anti-CO poisoning ability, storage stability, and substrate tolerance. DFT calculations reveal that the high catalytic activity of the catalyst arises from the optimized electronic structure and charge states of palladium atoms in the defect-containing indium oxide.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Review
Chemistry, Physical
Tao Shen et al.
Summary: Single-atom alloys (SAAs) are emerging materials that combine the advantages of alloys and single-atom catalysts, resulting in superior electrocatalytic performance. This review highlights the recent advances of SAAs in various electrochemical reactions, providing important insights for the design of highly effective electrocatalysts.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Bolong Yang et al.
Summary: In this study, a new synthetic method for preparing an oxygen reduction reaction (ORR) catalyst with Co-N5 active sites was successfully developed. Compared with the traditional Co-N-4 active sites, the obtained catalyst showed higher half-wave potential and maximum power density in alkaline polymer electrolyte fuel cells (APEFCs). The rate of ORR was significantly increased by modulating the electronic and geometric structure. Additionally, in-situ Raman spectroscopy demonstrated that Co-N-5 is the active site and axial Co-N coordination can enhance O-2 adsorption and activation, thereby boosting ORR performance. This research provides atomic-level insight into the relationship between the electronic structure of the active center and the ORR performance, as well as guidance for the rational design of high-efficiency electrocatalysts.
Article
Chemistry, Physical
Ruopeng Li et al.
Summary: This research reports novel NiTe-NiCoN and NiTe-NiFeN heterostructured electrocatalysts with outstanding performance in seawater electrolysis, demonstrating their excellent efficiency in hydrogen and oxygen reactions. Analysis reveals that the unique nanostructures of these materials play a key role in enhancing reaction activity and promoting kinetics.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Applied
Yaojia Cheng et al.
Summary: In this study, a novel oxygen reduction reaction (ORR) electrocatalyst containing Co single atoms and nanoparticles supported by carbon dots-derived carbon nanoflowers (Co SAs/NPs CNF) was designed. The catalyst exhibited high ORR activity, outstanding catalytic performance, and stability when used as the air-electrode catalyst in rechargeable Zn-air batteries (ZABs). The combination of supported single-atom sites and metal nanoparticles showed great benefits for ORR electrocatalysis.
CHINESE JOURNAL OF CATALYSIS
(2022)
Review
Chemistry, Physical
Sujuan Zha et al.
Summary: This article systematically summarizes the recent advances in heteroatom-doped M-N-C SACs, discusses the methods to enhance ORR activity by regulating coordination configurations, and proposes the future challenges and research directions of heteroatom-doped M-N-C SACs for the ORR.
SUSTAINABLE ENERGY & FUELS
(2022)
Article
Electrochemistry
Hui Yang et al.
Summary: The large-scale production of stable and active ORR electrocatalysts based on iron was achieved using a core-shell zeolitic imidazolate framework-tannic acid coordination polymer composite (ZIF-8@K-TA) as the catalyst precursor. The resulting H-Fe-Nx-C demonstrated efficient electrocatalytic activity and stability towards the ORR, surpassing the majority of recently reported Fe-N-C catalysts and the standard Pt/C catalyst, with outstanding tolerance to methanol.
Article
Chemistry, Multidisciplinary
Yuanjun Chen et al.
Summary: This study demonstrates the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance. The designed and synthesized Co-1-N3PS/HC catalyst shows outstanding ORR activity in alkaline and acidic media, surpassing Pt/C and most non-precious ORR electrocatalysts. Insights from this work promote rational design of efficient catalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Min Jie Wang et al.
Summary: This study presents a simple method for preparing single-atom catalysts and demonstrates their excellent performance in hydrogen evolution reactions, outperforming commercial Pt/C. Density functional theory calculations reveal that the strong coordination of Ru-N and Ru-S bonds plays a crucial role in their activity.
APPLIED SURFACE SCIENCE
(2021)
Review
Chemistry, Multidisciplinary
Baljeet Singh et al.
Summary: Supported single-metal atom catalysts consist of isolated active metal centers heterogenized on inert supports, offering control over their thermal stability, electronic properties, and catalytic activities through interactions with neighboring heteroatoms. The atomic dispersion of the catalytic centers reduces the required amount of metal and enables control over selectivity and catalyst turnover frequency.
Article
Chemistry, Physical
Xinxin Zhu et al.
Summary: A novel self-etched Pt-Co nanodendrite in nanoframe (Pt-Co ND-NF) was synthesized for the first time. It exhibited improved catalytic performance and stability, offering promising ways for highly strengthening catalytic activity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Review
Chemistry, Inorganic & Nuclear
Ashta C. Ghosh et al.
Summary: Transition metal-driven small molecule activation is essential for the production of fuels and chemicals or energy supply. The use of multimetallic catalysts, where two or more metal centers act in synergy to activate and transform the substrate(s), is widespread both in nature (metalloenzymes) and (bio)inorganic chemistry. Benefits of this strategy in terms of catalytic performances result from cooperation between different metals to bind and activate a single substrate, to activate different substrates reacting together, or with one assisting metal tuning the reactivity of the active metal center.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Physical
Feiteng Wang et al.
Summary: By systematically investigating the oxygen reduction reaction process on dual-metal-nitrogen-carbon catalysts through first-principle calculations, it is found that the high activity of dual-metal sites can be attributed to facilitating O-O bond cleavage and mitigating *OH removal issue. The introduction of a descriptor called antibonding center simplifies the evaluation of kinetics.
JOURNAL OF CATALYSIS
(2021)
Review
Chemistry, Multidisciplinary
Yongxia Wang et al.
Summary: Significant progress has been made in the study of M-N-C materials, utilizing advanced synthetic and characterization techniques to improve electrocatalytic performance and deepen understanding of fundamental principles. Recent research has focused on synthetic strategies, characterization techniques, and applications of specifically coordinated M-N-C catalysts in typical electrocatalytic reactions.
ADVANCED MATERIALS
(2021)
Review
Chemistry, Inorganic & Nuclear
Yuliang Li et al.
Summary: Metal macrocyclic complexes with square-planar M-N-4 coordination sites, such as metal porphyrins, have been extensively studied as catalysts for electrocatalytic ORR. The immobilization of these catalysts on appropriate supporting materials is crucial for practical applications. N-4-metallomacrocycles show promising potential for use in metal-air batteries.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Energy & Fuels
Horie Adabi et al.
Summary: This study presents a high-performing commercial oxygen reduction catalyst that can replace platinum group metal catalysts, resulting in improved performance and reduced cost for anion-exchange membrane fuel cells.
Article
Chemistry, Physical
Zhaoyu Jin et al.
Summary: Regulating the site density of single-atom catalysts can significantly improve electrocatalysis performance, such as the oxygen reduction reaction. Strong interactions between adjacent Fe-N-4 moieties can enhance intrinsic ORR activity, with a marked improvement continuing until neighbouring Fe atoms approach as close as about 0.7 nm. Identifying the fundamental mechanism of the inter-site distance effect in Fe-N-4 catalysts may maximize the potential of densely populated SACs.
Review
Chemistry, Multidisciplinary
Qingyun Qu et al.
Summary: This review discusses the latest progress of single-atomic-site catalysts (SACs) in acidic oxygen reduction reactions (ORR), focusing on the relationship between the structure of SACs and their performance, as well as the challenges and prospects in the acidic ORR field.
TRENDS IN CHEMISTRY
(2021)
Review
Chemistry, Multidisciplinary
Jiheon Kim et al.
Summary: This review highlights recent advances in M-N-C catalysts in terms of atomic-level understanding and design of mononuclear active sites, the effect of the porous carbon structure on the electrocatalytic performance, and improving catalytic stability, and suggests future directions to enhance M-N-C catalysts for highly active and stable PEMFC performance.
TRENDS IN CHEMISTRY
(2021)
Review
Chemistry, Multidisciplinary
Christopher J. Reed et al.
Summary: This review summarizes progress in understanding the structures and reactions of heme-copper oxidases, nitric oxide reductases, and sulfite reductases at the molecular level, providing important insights into the key features of these catalytic sites through studies of native enzymes and biomimetic models. Discussion on the reaction selectivity of these enzymes is facilitated through comparisons of their similar heteronuclear active sites, offering outlook for further investigations.
CHEMICAL SOCIETY REVIEWS
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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
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NATURE COMMUNICATIONS
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APPLIED CATALYSIS B-ENVIRONMENTAL
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Review
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Jung Hyun Park et al.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2020)
Article
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JOURNAL OF CATALYSIS
(2020)
Review
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ADVANCED ENERGY MATERIALS
(2020)
Review
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Tingting Sun et al.
Article
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Dewen Wang et al.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2019)
Review
Chemistry, Inorganic & Nuclear
Ming Zhong et al.
COORDINATION CHEMISTRY REVIEWS
(2019)
Review
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Article
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APPLIED SURFACE SCIENCE
(2019)
Article
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Article
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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2019)
Article
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Jinqiang Zhang et al.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2019)
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(2019)
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Review
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NATURE COMMUNICATIONS
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XM Yang et al.
MACROMOLECULAR RAPID COMMUNICATIONS
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