Superiority of Dual‐Atom Catalysts in Electrocatalysis: One Step Further Than Single‐Atom Catalysts

Advanced Energy Materials, Год журнала: 2022, Номер 12(9)

Опубликована: Янв. 18, 2022

Abstract In recent years, dual‐atom catalysts (DACs) have attracted extensive attention, as an extension of single‐atom (SACs). Compared with SACs, DACs higher metal loading and more complex flexible active sites, thus achieving better catalytic performance providing opportunities for electrocatalysis. This review introduces the research progress in years on how to design new enhance Firstly, advantages increasing are introduced. Then, role changing adsorption condition reactant molecules atoms is discussed. Moreover, ways which can reduce reaction energy barrier key steps change path explored. Catalytic applications different electrocatalytic reactions, including carbon dioxide reduction reaction, oxygen evolution hydrogen nitrogen followed. Finally, a brief summary made challenges prospects

Язык: Английский

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Год журнала: 2022, Номер 15(9), С. 7806 - 7839

Опубликована: Июнь 2, 2022

Язык: Английский

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Atomically Precise Dinuclear Site Active toward Electrocatalytic CO₂ Reduction

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(30), С. 11317 - 11324

Опубликована: Июль 22, 2021

The development of atomically precise dinuclear heterogeneous catalysts is promising to achieve efficient catalytic performance and also helpful the atomic-level understanding on synergy mechanism under reaction conditions. Here, we report a Ni2(dppm)2Cl3 dinuclear-cluster-derived strategy uniform Ni2 site, consisting two Ni1–N4 moieties shared with nitrogen atoms, anchored N-doped carbon. By using operando synchrotron X-ray absorption spectroscopy, identify dynamically structure electrochemical CO2 reduction reaction, revealing an oxygen-bridge adsorption Ni2–N6 site form O–Ni2–N6 enhanced Ni–Ni interaction. Theoretical simulations demonstrate that key can significantly lower energy barrier for activation. As result, catalyst exhibits >94% Faradaic efficiency carbon monoxide production. This work provides bottom-up target synthesis approaches evidences identity sites active toward reactions.

Язык: Английский

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“Capture-Backdonation-Recapture” Mechanism for Promoting N₂ Reduction by Heteronuclear Metal-Free Double-Atom Catalysts

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(21), С. 9344 - 9353

Опубликована: Май 20, 2022

Facing the increasingly serious energy and environmental crisis, development of heteronuclear metal-free double-atom catalysts is a potential strategy to realize efficient catalytic nitrogen reduction with low consumption no pollution because it could combine advantages flexible active sites in while also being pollution-free have high Faraday efficiency simultaneously. However, according existing mechanism, finite orbits other nonmetallic atoms, except boron atom, reduce possibility catalysis hinder catalysts. Herein, we propose new "capture-backdonation-recapture" which skillfully uses electron capture-backdonation-recapture between boron, substrate, elements solve above problems. Based on this by means first-principle calculations, material structure, adsorption energy, activity, selectivity 36 are systematically investigated evaluate their performance. B-Si@BP1 B-Si@BP3 selected for good performance limiting potentials -0.14 -0.10 V, respectively. Meanwhile, mechanism verified analyzing results transfer. Our work broadens ideas lays theoretical foundation future.

Язык: Английский

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Isolating Single and Few Atoms for Enhanced Catalysis

Advanced Materials, Год журнала: 2022, Номер 34(39)

Опубликована: Май 17, 2022

Abstract Atomically dispersed metal catalysts have triggered great interest in the field of catalysis owing to their unique features. Isolated single or few atoms can be anchored on substrates via chemical bonding space confinement maximize atom utilization efficiency. The key challenge lies precisely regulating geometric and electronic structure active centers, thus significantly influencing catalytic properties. Although several reviews been published preparation, characterization, application single‐atom (SACs), comprehensive understanding SACs, dual‐atom (DACs), atomic clusters has never systematically summarized. Here, recent advances engineering local environments state‐of‐the‐art DACs, for enhanced performance are highlighted. Firstly, various synthesis approaches presented. Then, special attention is focused elucidation terms state coordination structure. Furthermore, a summary isolated applications thermocatalysis, electrocatalysis, photocatalysis provided. Finally, potential challenges future opportunities this emerging This review will pave way regulate microenvironment site boosting processes.

Язык: Английский

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Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

Interdisciplinary materials, Год журнала: 2022, Номер 1(1), С. 51 - 87

Опубликована: Янв. 1, 2022

Single-atom catalysts, featuring some of the most unique activities, selectivity, and high metal utilization, have been extensively studied over past decade. Given their activity, especially towards small molecules or key intermediate conversions, they can be synergized together with other active species (typically single atoms, atomic clusters, nanoparticles) in either tandem parallel both, leading to much better performance complex catalytic processes. Although there reports on effectively combining multiple components into one entity, combination synergy between atoms not reviewed examined a systematic manner. Herein, this overview, synergistic interactions, binary complementary effects, bifunctional functions are defined discussed detail. The integration marriages investigated particular emphasis homogeneous heterogeneous combinations, spatial distribution, synthetic strategies, thus-derived outstanding performance, new light shined mechanisms by zooming several case studies. dynamic nature each interactions such entities electrocatalytic processes visited, basis situ/operando evidence. Last, we feature current challenges future perspectives these integrated that offer guidance for advanced catalyst design rational species.

Язык: Английский

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Review of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS)

Advanced Materials, Год журнала: 2023, Номер 36(1)

Опубликована: Апрель 20, 2023

This topical review focuses on the distinct role of carbon support coordination environment single-atom catalysts (SACs) for electrocatalysis. The article begins with an overview atomic configurations in SACs, including a discussion advanced characterization techniques and simulation used understanding active sites. A summary key electrocatalysis applications is then provided. These processes are oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), nitrogen (NRR), dioxide (CO

Язык: Английский

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Coadsorption of NRR and HER Intermediates Determines the Performance of Ru-N₄ toward Electrocatalytic N₂ Reduction

ACS Catalysis, Год журнала: 2022, Номер 12(4), С. 2505 - 2512

Опубликована: Фев. 3, 2022

Electrochemical N2 reduction (NRR) to ammonia is seriously limited by the competing hydrogen evolution reaction (HER), but atomic-scale factors controlling HER/NRR competition are unknown. Herein we unveil mechanism, thermodynamics, and kinetics determining efficiency on state-of-the-art NRR electrocatalyst, Ru-N4, using grand canonical ensemble density functional theory (GCE-DFT). We show that NRR/HER intermediates coadsorb catalyst where suppress HER selectivity determined initial step forming *NNH or *H. Our results provide crucial insight into complex competition, necessity of GCE-DFT calculations, suggest ways improve selectivity.

Язык: Английский

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Atomically Dispersed Heteronuclear Dual‐Atom Catalysts: A New Rising Star in Atomic Catalysis

Small, Год журнала: 2021, Номер 18(12)

Опубликована: Дек. 12, 2021

Abstract Atomic catalysts (AC) are gaining extensive research interest as the most active new frontier in heterogeneous catalysis due to their unique electronic structures and maximum atom‐utilization efficiencies. Among all atom catalysts, atomically dispersed heteronuclear dual‐atom (HDACs), which featured with asymmetric sites, have recently opened pathways field of advancing atomic catalysis. In this review, up‐to‐date investigations on together last advances theoretical predictions experimental constructions summarized. Furthermore, current synthetic strategies accessible characterization techniques for these kinds also discussed. Finally, crucial challenges both aspects, well future prospects HDACs energy‐related applications provided. It is believed that review will inspire rational design synthesis generation highly effective HDACs.

Язык: Английский

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Emerging two-dimensional nanomaterials for electrochemical nitrogen reduction

Chemical Society Reviews, Год журнала: 2021, Номер 50(22), С. 12744 - 12787

Опубликована: Янв. 1, 2021

This review focuses on high-performance 2D electrocatalysts for nitrogen-reduction, highlighting massive-potential strong activity, high NH 3 yield and faradaic efficiency.

Язык: Английский

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