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

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

278
Non-carbon-supported single-atom site catalysts for electrocatalysis DOI
Xiaobo Zheng, Peng Li, Shi Xue Dou

et al.

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(5), P. 2809 - 2858

Published: Jan. 1, 2021

Non-carbon supported SACs were classified into eight categories based on the nature of their substrates for first time, and corresponding anchoring stabilization mechanisms have been systematically summarized discussed.

Language: Английский

Citations

277
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

267
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

252
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

228
Atomically dispersed materials: Ideal catalysts in atomic era DOI
Tao Gan, Dingsheng Wang

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

Citations

221
Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis DOI
Wenhao Li, Jiarui Yang, Dingsheng Wang

et al.

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

Citations

215
A Site Distance Effect Induced by Reactant Molecule Matchup in Single‐Atom Catalysts for Fenton‐Like Reactions DOI
Bingqing Wang, Cheng Cheng, Mengmeng Jin

et al.

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

Citations

212
Single‐atom catalysis for carbon neutrality DOI Creative Commons
Ligang Wang, Dingsheng Wang, Yadong Li

et al.

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

Citations

209
Lewis Acid Site-Promoted Single-Atomic Cu Catalyzes Electrochemical CO2 Methanation DOI
Shenghua Chen, Bingqing Wang, Jiexin Zhu

et al.

Nano Letters, Journal Year: 2021, Volume and Issue: 21(17), P. 7325 - 7331

Published: Aug. 17, 2021

Developing an efficient catalyst for the electrocatalytic CO2 reduction reaction (CO2RR) is highly desired because of environmental and energy issues. Herein, we report a single-atomic-site Cu supported by Lewis acid to CH4. Theoretical calculations suggested that sites in metal oxides (e.g., Al2O3, Cr2O3) can regulate electronic structure atoms optimizing intermediate absorption promote methanation. Based on these theoretical results, ultrathin porous Al2O3 with enriched was explored as anchor single atoms; this modification achieved faradaic efficiency (FE) 62% at −1.2 V (vs RHE) corresponding current density 153.0 mA cm–2 CH4 formation. This work demonstrates effective strategy tailoring into

Language: Английский

Citations

190