Atomic‐Level Modulation of Electronic Density at Cobalt Single‐Atom Sites Derived from Metal–Organic Frameworks: Enhanced Oxygen Reduction Performance

Angewandte Chemie International Edition, Год журнала: 2020, Номер 60(6), С. 3212 - 3221

Опубликована: Окт. 30, 2020

Demonstrated here is the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance by combining density-functional theory (DFT) calculations electrochemical analysis. Guided DFT calculations, a MOF-derived catalyst with optimal Co1 -N3 PS moiety incorporated in hollow carbon polyhedron (Co1 PS/HC) was designed synthesized. PS/HC exhibits outstanding alkaline ORR activity half-wave potential 0.920 V superior kinetics record-level kinetic current an ultralow Tafel slope 31 mV dec-1 , exceeding that Pt/C almost all non-precious electrocatalysts. In acidic media still surpasses Pt/C. This work offers atomic-level insight into relationship site catalytic properties, promoting rational design efficient catalysts.

Язык: Английский

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Recent advances of noble-metal-free bifunctional oxygen reduction and evolution electrocatalysts

Chemical Society Reviews, Год журнала: 2021, Номер 50(13), С. 7745 - 7778

Опубликована: Янв. 1, 2021

Bifunctional oxygen reduction and evolution constitute the core processes for sustainable energy storage. The advances on noble-metal-free bifunctional electrocatalysts are reviewed.

Язык: Английский

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Oxygen Reduction Electrocatalysts toward Practical Fuel Cells: Progress and Perspectives

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(33), С. 17832 - 17852

Опубликована: Фев. 5, 2021

Fuel cells are an incredibly powerful renewable energy technology, but their broad applications remains lagging because of the high cost and poor reliability cathodic electrocatalysts for oxygen reduction reaction (ORR). This review focuses on recent progress ORR in fuel cells. More importantly, it highlights fundamental problems associated with insufficient activity translation from rotating disk electrode to membrane assembly Finally, atomic-level in-depth information catalysts cells, potential perspectives suggested, including large-scale preparation, unified assessment criteria, advanced interpretation techniques, simulation artificial intelligence. aims provide valuable insights into science technical engineering efficient

Язык: Английский

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Advances in the Development of Single‐Atom Catalysts for High‐Energy‐Density Lithium–Sulfur Batteries

Advanced Materials, Год журнала: 2022, Номер 34(30)

Опубликована: Март 3, 2022

Abstract Although lithium–sulfur (Li–S) batteries are promising next‐generation energy‐storage systems, their practical applications limited by the growth of Li dendrites and lithium polysulfide shuttling. These problems can be mitigated through use single‐atom catalysts (SACs), which exhibit advantages maximal atom utilization efficiency (≈100%) unique catalytic properties, thus effectively enhancing performance electrode materials in devices. This review systematically summarizes recent progress SACs intended for Li‐metal anodes, S cathodes, separators, briefly introducing operating principles Li–S batteries, action mechanisms corresponding SACs, fundamentals activity, then comprehensively describes main strategies synthesis. Subsequently, operation reinforced as well other metal–S individually illustrated, major challenges usage future development directions presented.

Язык: Английский

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Mesopore‐Rich Fe–N–C Catalyst with FeN₄–O–NC Single‐Atom Sites Delivers Remarkable Oxygen Reduction Reaction Performance in Alkaline Media

Advanced Materials, Год журнала: 2022, Номер 34(29)

Опубликована: Май 18, 2022

Fe-N-C catalysts offer excellent performance for the oxygen reduction reaction (ORR) in alkaline media. With a view toward boosting intrinsic ORR activity of Fe single-atom sites catalysts, fine-tuning local coordination to optimize binding energies intermediates is imperative. Herein, porous FeN4 -O-NCR electrocatalyst rich catalytically accessible -O (wherein single atoms are coordinated four in-plane nitrogen and one subsurface axial atom) supported on N-doped carbon nanorods (NCR) reported. K-edge X-ray absorption spectroscopy (XAS) verifies presence active -O-NCR, while density functional theory calculations reveal that offers lower energy more selective 4-electron/4-proton pathway compared traditional sites. Electrochemical tests validate outstanding ORR, outperforming Pt/C almost all other M-N-C reported date. A primary zinc-air battery constructed using delivers peak power 214.2 mW cm-2 at current 334.1 mA , highlighting benefits optimizing iron atoms.

Язык: Английский

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Noble-metal single-atoms in thermocatalysis, electrocatalysis, and photocatalysis

Energy & Environmental Science, Год журнала: 2021, Номер 14(5), С. 2954 - 3009

Опубликована: Янв. 1, 2021

This review summarizes the recent advances about noble-metal single-atom catalysts in thermocatalysis, electrocatalysis, and photocatalysis.

Язык: Английский

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Anion-exchange membrane water electrolyzers and fuel cells

Chemical Society Reviews, Год журнала: 2022, Номер 51(23), С. 9620 - 9693

Опубликована: Янв. 1, 2022

The key components, working management, and operating techniques of anion-exchange membrane water electrolyzers fuel cells are reviewed for the first time.

Язык: Английский

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Metal-metal interactions in correlated single-atom catalysts

Science Advances, Год журнала: 2022, Номер 8(17)

Опубликована: Апрель 29, 2022

Single-atom catalysts (SACs) include a promising family of electrocatalysts with unique geometric structures. Beyond conventional ones fully isolated metal sites, an emerging class the adjacent single atoms exhibiting intersite metal-metal interactions appear in recent years and can be denoted as correlated SACs (C-SACs). This type provides more opportunities to achieve substantial structural modification performance enhancement toward wider range electrocatalytic applications. On basis clear identification interactions, this review critically examines research progress C-SACs. It shows that control enables regulation atomic structure, local coordination, electronic properties atoms, which facilitate modulation behavior Last, we outline directions for future work design development C-SACs, is indispensable creating high-performing new SAC architectures.

Язык: Английский

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Regulating the coordination structure of metal single atoms for efficient electrocatalytic CO₂ reduction

Energy & Environmental Science, Год журнала: 2020, Номер 13(12), С. 4609 - 4624

Опубликована: Янв. 1, 2020

An in-depth summary about the regulation of coordination structure in single atom catalysts for CO₂RR is summarized.

Язык: Английский

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Intrinsic Activity of Metal Centers in Metal–Nitrogen–Carbon Single-Atom Catalysts for Hydrogen Peroxide Synthesis

Journal of the American Chemical Society, Год журнала: 2020, Номер 142(52), С. 21861 - 21871

Опубликована: Дек. 17, 2020

Metal–nitrogen–carbon (M–N–C) single-atom catalysts (SACs) show high catalytic activity for many important chemical reactions. However, an understanding of their intrinsic remains ambiguous because the lack well-defined atomic structure control in current M–N–C SACs. Here, we use covalent organic framework SACs with identical metal coordination environment as model to elucidate various centers A pH-universal trend is discovered among six 3d transition metals hydrogen peroxide (H2O2) synthesis, Co having highest activity. Using density functional calculations access a total 18 species, demonstrate that difference binding energy O2* and HOOH* intermediates (EO2* – EHOOH*) on single reliable thermodynamic descriptor predict centers. The predicted Ir from further validated experimentally. This work suggests class structurally defined clear mechanistic principles H2O2 which may be extendable other

Язык: Английский

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