Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Journal Year: 2022, Volume and Issue: 15(8), P. 6888 - 6923

Published: June 14, 2022

Language: Английский

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Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis

Advanced Powder Materials, Journal Year: 2021, Volume and Issue: 1(1), P. 100013 - 100013

Published: Nov. 15, 2021

Various metal-based electrocatalysts from nanocrystals, to clusters and single-atoms, have been well-discovered towards high-efficient power devices electrocatalytic conversion. To accelerate energy transformation materials discovery, developing high-throughput DFT calculations machine-learning techniques is of great necessity. This review comprehensively outlines the latest progress theory-guided design advanced materials. Especially, we focus on study single atoms in various devices, such as fuel cell (oxygen reduction reaction, ORR; acid oxidation reaction; alcohol reaction), other reactions for energy-related conversion small molecules, H2O2 evolution (2e− ORR), water splitting (H2 reaction/O2 HER/OER), N2 reaction (NRR), CO2 (CO2RR). Firstly, electronic structure, interaction mechanism, activation path are discussed provide an overall blueprint electrocatalysis batteries mentioned above. Thereafter, experimental synthesis strategies, structural recognition, performance figured out. Finally, some viewpoints into current issues future concept provided.

Language: Английский

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The Progress and Outlook of Metal Single-Atom-Site Catalysis

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(40), P. 18155 - 18174

Published: Sept. 29, 2022

Single-atom-site catalysts (SASCs) featuring maximized atom utilization and isolated active sites have progressed tremendously in recent years as a highly prosperous branch of catalysis research. Varieties SASCs been developed that show excellent performance many catalytic applications. The major goal SASC research is to establish feasible synthetic strategies for the preparation high-performance catalysts, achieve an in-depth understanding active-site structures mechanisms, develop practical with industrial value. This Perspective describes up-to-date development related such dual-atom-site (DASCs) nano-single-atom-site (NSASCs), analyzes current challenges encountered by these applications, proposes their possible future path.

Language: Английский

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

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(9)

Published: Jan. 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

Language: Английский

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

Nano Research, Journal Year: 2022, Volume and Issue: 15(9), P. 7806 - 7839

Published: June 2, 2022

Language: Английский

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MOF Encapsulating N‐Heterocyclic Carbene‐Ligated Copper Single‐Atom Site Catalyst towards Efficient Methane Electrosynthesis

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 61(4)

Published: Nov. 12, 2021

The exploitation of highly efficient carbon dioxide reduction (CO2 RR) electrocatalyst for methane (CH4 ) electrosynthesis has attracted great attention the intermittent renewable electricity storage but remains challenging. Here, N-heterocyclic carbene (NHC)-ligated copper single atom site (Cu SAS) embedded in metal-organic framework is reported (2Bn-Cu@UiO-67), which can achieve an outstanding Faradaic efficiency (FE) 81 % CO2 to CH4 at -1.5 V vs. RHE with a current density 420 mA cm-2 . FE our catalyst above 70 within wide potential range and achieves unprecedented turnover frequency (TOF) 16.3 s-1 σ donation NHC enriches surface electron Cu SAS promotes preferential adsorption CHO* intermediates. porosity facilitates diffusion 2Bn-Cu, significantly increasing availability each catalytic center.

Language: Английский

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Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(52)

Published: Oct. 6, 2022

Abstract The simultaneous presence of two active metal centres in diatomic catalysts (DACs) leads to the occurrence specific interactions between sites. Such interactions, referred as long‐range (LRIs), play an important role determining rate and selectivity a reaction. optimal combination must be determined achieve targeted efficiency. To date, various types DACs have been synthesised applied electrochemistry. However, LRIs not systematically summarised. Herein, regulation, mechanism, electrocatalytic applications are comprehensively summarised discussed. In addition basic information above, challenges, opportunities, future development proposed order present overall view reference for research.

Language: Английский

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A Site Distance Effect Induced by Reactant Molecule Matchup in Single‐Atom Catalysts for Fenton‐Like Reactions

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(33)

Published: June 20, 2022

Abstract Understanding the site interaction nature of single‐atom catalysts (SACs), especially densely populated SACs, is vital for their application to various catalytic reactions. Herein, we report a distance effect, which emphasizes how well adjacent copper atoms (denoted as d Cu1−Cu1 ) matches with reactant peroxydisulfate (PDS) molecular size determine Fenton‐like reaction reactivity on carbon‐supported SACs. The optimized in range 5–6 Å, PDS, endows catalyst nearly two times higher turnover frequency than that beyond this range, accordingly achieving record‐breaking kinetics oxidation emerging organic contaminants. Further studies suggest effect originates from alteration PDS adsorption dual‐site structure Cu 1 −Cu sites when falls within significantly enhancing interfacial charge transfer and consequently resulting most efficient activation so far.

Language: Английский

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Single‐atom catalysis for carbon neutrality

Carbon Energy, Journal Year: 2022, Volume and Issue: 4(6), P. 1021 - 1079

Published: July 14, 2022

Abstract Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission high amounts carbon dioxide (CO 2 ), resulting in a severe “Greenhouse effect.” Considering this situation, the concept “carbon neutrality” has been put forward by 125 countries one after another. To achieve goals neutrality,” two main strategies to reduce CO emissions develop sustainable clean can be adopted. Notably, these are crucial for synthesis advanced single‐atom catalysts (SACs) energy‐related applications. In review, we highlight unique SACs conversion into high‐efficiency energy, example, through photocatalytic, electrocatalytic, thermal catalytic hydrogenation technologies, convert hydrocarbon fuels (CO, CH 4 , HCOOH, 3 OH, multicarbon [C 2+ ] products). addition, introduce technologies devices replace polluting such as photocatalytic electrocatalytic water splitting produce hydrogen oxygen reduction reaction (ORR) fuel cells. Impressively, several representative examples (including d ‐, ds p f ‐blocks) conversion, H ORR discussed describe methods, characterization, corresponding activity. Finally, review concludes with description challenges outlooks future applications contributing toward neutrality.

Language: Английский

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The reformation of catalyst: From a trial-and-error synthesis to rational design

Nano Research, Journal Year: 2023, Volume and Issue: 17(4), P. 3261 - 3301

Published: Sept. 27, 2023

Language: Английский

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