Liquid Fluxional Ga Single Atom Catalysts for Efficient Electrochemical CO2Reduction DOI
Zedong Zhang, Jiexin Zhu, Shenghua Chen

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(3)

Опубликована: Ноя. 18, 2022

Precise design and tuning of the micro-atomic structure single atom catalysts (SACs) can help efficiently adapt complex catalytic systems. Herein, we inventively found that when active center main group element gallium (Ga) is downsized to atomic level, whose characteristic has significant differences from conventional bulk rigid Ga catalysts. The SACs with a P, S coordination environment display specific flow properties, showing CO products FE ≈92 % at -0.3 V vs. RHE in electrochemical CO2 reduction (CO2 RR). Theoretical simulations demonstrate adaptive dynamic transition optimizes adsorption energy *COOH intermediate renews sites time, leading excellent RR selectivity stability. This liquid system interfaces lays foundation for future exploration synthesis catalysis.

Язык: Английский

Engineering Dual Single‐Atom Sites on 2D Ultrathin N‐doped Carbon Nanosheets Attaining Ultra‐Low‐Temperature Zinc‐Air Battery DOI
Tingting Cui,

Yun‐Peng Wang,

Tong Ye

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(12)

Опубликована: Янв. 7, 2022

Herein, a novel dual single-atom catalyst comprising adjacent Fe-N4 and Mn-N4 sites on 2D ultrathin N-doped carbon nanosheets with porous structure (FeMn-DSAC) was constructed as the cathode for flexible low-temperature Zn-air battery (ZAB). FeMn-DSAC exhibits remarkable bifunctional activities oxygen reduction reaction (ORR) evolution (OER). Control experiments density functional theory calculations reveal that catalytic activity arises from cooperative effect of Fe/Mn dual-sites aiding *OOH dissociation well nanosheet promoting active sits exposure mass transfer during process. The excellent enables ZAB to operate efficiently at ultra-low temperature -40 °C, delivering 30 mW cm-2 peak power retaining up 86 % specific capacity room counterpart.

Язык: Английский

Процитировано

526
Design concept for electrocatalysts DOI
Yao Wang, Xiaobo Zheng, Dingsheng Wang

и другие.

Nano Research, Год журнала: 2021, Номер 15(3), С. 1730 - 1752

Опубликована: Сен. 4, 2021

Язык: Английский

Процитировано

490
Understanding the structure-performance relationship of active sites at atomic scale DOI
Runze Li, Dingsheng Wang

Nano Research, Год журнала: 2022, Номер 15(8), С. 6888 - 6923

Опубликована: Июнь 14, 2022

Язык: Английский

Процитировано

485
The Progress and Outlook of Metal Single-Atom-Site Catalysis DOI
Liang Xiao, Ninghua Fu,

Shuangchao Yao

и другие.

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(40), С. 18155 - 18174

Опубликована: Сен. 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.

Язык: Английский

Процитировано

393
Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis DOI Creative Commons
Hongyu Jing, Peng Zhu, Xiaobo Zheng

и другие.

Advanced Powder Materials, Год журнала: 2021, Номер 1(1), С. 100013 - 100013

Опубликована: Ноя. 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.

Язык: Английский

Процитировано

378
Superiority of Dual‐Atom Catalysts in Electrocatalysis: One Step Further Than Single‐Atom Catalysts DOI
Runze Li, Dingsheng Wang

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

Процитировано

371
An Adjacent Atomic Platinum Site Enables Single‐Atom Iron with High Oxygen Reduction Reaction Performance DOI
Ali Han, Xijun Wang, Kun Tang

и другие.

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(35), С. 19262 - 19271

Опубликована: Июнь 22, 2021

Abstract The modulation effect has been widely investigated to tune the electronic state of single‐atomic M‐N‐C catalysts enhance activity oxygen reduction reaction (ORR). However, in‐depth study is rarely reported for isolated dual‐atomic metal sites. Now, catalytic activities Fe‐N 4 moiety can be enhanced by adjacent Pt‐N through effect, in which acts as modulator 3d orbitals active site and optimize ORR activity. Inspired this principle, we design synthesize electrocatalyst that comprises /Pt‐N moieties dispersed nitrogen‐doped carbon matrix (Fe‐N @NC) exhibits a half‐wave potential 0.93 V vs. RHE negligible degradation (ΔE 1/2 =8 mV) after 10000 cycles 0.1 M KOH. We also demonstrate not effective optimizing performances Co‐N Mn‐N systems.

Язык: Английский

Процитировано

363
Regulations of active moiety in single atom catalysts for electrochemical hydrogen evolution reaction DOI Open Access
Peng Zhu, Xiang Xiong, Dingsheng Wang

и другие.

Nano Research, Год журнала: 2022, Номер 15(7), С. 5792 - 5815

Опубликована: Май 4, 2022

Язык: Английский

Процитировано

317
Thermal Atomization of Platinum Nanoparticles into Single Atoms: An Effective Strategy for Engineering High-Performance Nanozymes DOI
Yuanjun Chen, Peixia Wang, Haigang Hao

и другие.

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(44), С. 18643 - 18651

Опубликована: Ноя. 2, 2021

Although great progress has been made in artificial enzyme engineering, their catalytic performance is far from satisfactory as alternatives of natural enzymes. Here, we report a novel and efficient strategy to access high-performance nanozymes via direct atomization platinum nanoparticles (Pt NPs) into single atoms by reversing the thermal sintering process. Atomization Pt NPs makes metal sites fully exposed results engineerable structural electronic properties, thereby leading dramatically enhanced enzymatic performance. As expected, as-prepared thermally stable single-atom nanozyme (PtTS-SAzyme) exhibited remarkable peroxidase-like activity kinetics, exceeding nanoparticle nanozyme. The following density functional theory calculations revealed that engineered P S not only promote process PtTS-SAzyme but also endow with unique structure owing electron donation atoms, well acceptance N which simultaneously contribute substantial enhancement enzyme-like PtTS-SAzyme. This work demonstrates nanoparticle-based an effective for engineering nanozymes, opens up new way rationally design optimize enzymes mimic

Язык: Английский

Процитировано

294
A Supported Pd2Dual‐Atom Site Catalyst for Efficient Electrochemical CO2Reduction DOI
Ningqiang Zhang, Xinxin Zhang, Yikun Kang

и другие.

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(24), С. 13388 - 13393

Опубликована: Апрель 5, 2021

Abstract Dual‐atom site catalysts (DACs) have emerged as a new frontier in heterogeneous catalysis because the synergistic effect between adjacent metal atoms can promote their catalytic activity while maintaining advantages of single‐atom (SACs), like 100 % atomic utilization efficiency and excellent selectivity. Herein, supported Pd 2 DAC was synthesized used for electrochemical CO reduction reaction (CO RR) first time. The as‐obtained exhibited superior RR performance with 98.2 faradic at −0.85 V vs. RHE, far exceeding that 1 SAC, coupled long‐term stability. density functional theory (DFT) calculations revealed intrinsic reason toward electron transfer dimeric sites. Thus, possessed moderate adsorption strength CO*, which beneficial production RR.

Язык: Английский

Процитировано

279