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

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(3)

Published: Nov. 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.

Language: Английский

High-entropy nanoparticles: Synthesis-structure-property relationships and data-driven discovery DOI
Yonggang Yao, Qi Dong, Alexandra H. Brozena

et al.

Science, Journal Year: 2022, Volume and Issue: 376(6589)

Published: April 7, 2022

High-entropy nanoparticles have become a rapidly growing area of research in recent years. Because their multielemental compositions and unique high-entropy mixing states (i.e., solid-solution) that can lead to tunable activity enhanced stability, these received notable attention for catalyst design exploration. However, this strong potential is also accompanied by grand challenges originating from vast compositional space complex atomic structure, which hinder comprehensive exploration fundamental understanding. Through multidisciplinary view synthesis, characterization, catalytic applications, high-throughput screening, data-driven materials discovery, review dedicated discussing the important progress unveiling critical needs future development catalysis, energy, sustainability applications.

Language: Английский

Citations

551
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

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(12)

Published: Jan. 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.

Language: Английский

Citations

515
Understanding the structure-performance relationship of active sites at atomic scale DOI
Runze Li, Dingsheng Wang

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

Published: June 14, 2022

Language: Английский

Citations

480
Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis DOI Creative Commons
Hongyu Jing, Peng Zhu, Xiaobo Zheng

et al.

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

Citations

376
Regulations of active moiety in single atom catalysts for electrochemical hydrogen evolution reaction DOI Open Access
Peng Zhu, Xiang Xiong, Dingsheng Wang

et al.

Nano Research, Journal Year: 2022, Volume and Issue: 15(7), P. 5792 - 5815

Published: May 4, 2022

Language: Английский

Citations

314
Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis DOI Open Access
Xiaobo Zheng, Beibei Li, Qishun Wang

et al.

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

Published: June 2, 2022

Language: Английский

Citations

264
Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species DOI
Yu Xiong, Hongchao Li, Chuangwei Liu

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(17)

Published: March 8, 2022

Recognizing and controlling the structure-activity relationships of single-atom catalysts (SACs) is vital for manipulating their catalytic properties various practical applications. Herein, Fe SACs supported on nitrogen-doped carbon (SA-Fe/CN) are reported, which show high reactivity (97% degradation bisphenol A in only 5 min), stability (80% maintained after five runs), wide pH suitability (working range 3-11) toward Fenton-like reactions. The roles different N species these reactions further explored, both experimentally theoretically. It discovered that graphitic an adsorptive site target molecule, pyrrolic coordinates with Fe(III) plays a dominant role reaction, pyridinic N, coordinated Fe(II), minor contributor to SA-Fe/CN. Density functional theory (DFT) calculations reveal lower d-band center location pyrrolic-type sites leads easy generation Fe-oxo intermediates, thus, excellent properties.

Language: Английский

Citations

262
Ru–Co Pair Sites Catalyst Boosts the Energetics for the Oxygen Evolution Reaction DOI
Xiaobo Zheng, Jiarui Yang,

Zhongfei Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(32)

Published: May 31, 2022

Abstract Manipulating the coordination environment of active center via anion modulation to reveal tailored activity and selectivity has been widely achieved, especially for carbon‐based single‐atom site catalysts (SACs). However, tuning ligand fields by single‐site metal cation regulation identifying effects on resulting electronic configuration is seldom explored. Herein, we propose a Ru strategy engineer properties constructing Ru/LiCoO 2 SAC with atomically dispersed Ru−Co pair sites. Benefitting from strong coupling between Co sites, catalyst possesses an enhanced electrical conductivity achieves near‐optimal oxygen adsorption energies. Therefore, optimized delivers superior evolution reaction (OER) low overpotential, high mass 1000 A g oxide −1 at small overpotential 335 mV, excellent long‐term stability. It also exhibits rapid kinetics rate capability outstanding durability in zinc–air battery.

Language: Английский

Citations

247
MOF Encapsulating N‐Heterocyclic Carbene‐Ligated Copper Single‐Atom Site Catalyst towards Efficient Methane Electrosynthesis DOI
Shenghua Chen, Wenhao Li, Wenjun Jiang

et al.

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

Citations

240
P and Cu Dual Sites on Graphitic Carbon Nitride for Photocatalytic CO2Reduction to Hydrocarbon Fuels with High C2H6Evolution DOI
Gang Wang, Zhe Chen, Tao Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(40)

Published: Aug. 15, 2022

The light-driven CO2 reduction to multi-carbon products is especially meaningful, while the low efficiency of multi-electron transfer and sluggish C-C coupling greatly hinder its development. Herein, we report a photocatalyst comprising P Cu dual sites anchored on graphitic carbon nitride (P/Cu SAs@CN), which achieves high C2 H6 evolution rate 616.6 μmol g-1 h-1 in reducing hydrocarbons. detailed spectroscopic characterizations identify formation charge-enriched sites, where isolated atoms serve as hole capture during photocatalysis. Theoretical simulations combined with situ FTIR measurement reveal kinetically feasible process for intermediate (*OC-COH) confirm favorable production P/Cu SAs@CN photocatalyst. This work offers new insights into design atomic precision toward highly efficient photocatalytic conversion value-added products.

Language: Английский

Citations

225