Strong p‐d Orbital Hybridization on Bismuth Nanosheets for High Performing CO2 Electroreduction DOI

Xueying Cao,

Yadong Tian,

Jizhen Ma

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(6)

Published: Nov. 27, 2023

Abstract Single‐atom alloys (SAAs) show great potential for a variety of electrocatalytic reactions. However, the atomic orbital hybridization effect SAAs on electrochemical reactions is unclear yet. Herein, in situ confinement vanadium/molybdenum/tungsten atoms bismuth nanosheet shown to create with rich grain boundaries, respectively. With detailed analysis microstructure and composition, strong p‐d between vanadium enables exceptional performance carbon dioxide (CO 2 ) reduction Faradaic efficiency nearly 100% C1 products wide range from −0.6 −1.4 V, long‐term electrolysis stability 90 h. In‐depth investigations theoretical computations reveal that electron delocalization toward via evokes active centers efficient CO activation σ‐donation O‐to‐Bi, thus reduces protonation energy barriers formate production. such fundamental understanding, SAA electrocatalyst employed fabricated solar‐driven electrolytic cell 5‐hydroxymethylfurfural oxidation, achieving an outstanding 2,5‐furandicarboxylic acid yield 90.5%. This study demonstrates feasible strategy rationally design advanced electrocatalysts basic principles hybridization.

Language: Английский

Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading DOI Creative Commons

Qiqi Mao,

Mu Xu,

Wenxin Wang

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Sept. 14, 2023

Organic electrocatalytic conversion is an essential pathway for the green of low-cost organic compounds to high-value chemicals, which urgently demands development efficient electrocatalysts. Here, we report a Cu single-atom dispersed Rh metallene arrays on foam cathodic nitrobenzene electroreduction reaction and anodic methanol oxidation reaction. In coupled system, Cusingle-atom-Rh requires only low voltages 1.18 V reach current densities 100 mA cm-2 generating aniline formate, with up ~100% conversion/ selectivity over ~90% formate Faraday efficiency, achieving synthesis chemicals. Density functional theory calculations reveal electron effect between host catalytic mechanism. The synergistic H*-spillover can improve process reduce energy barrier process, thus enhancing activity target product selectivity.

Language: Английский

Citations

59

Main-group indium single-atom catalysts for electrocatalytic NO reduction to NH3 DOI
Kai Chen, Nana Zhang, Fuzhou Wang

et al.

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(13), P. 6814 - 6819

Published: Jan. 1, 2023

In single atoms confined in amorphous MoO 3 (In 1 /a-MoO ) are reported to be an efficient catalyst for NO electroreduction NH , attributed the ability of single-site inhibit hydrogen evolution and optimize NO-to-NH hydrogenation energetics.

Language: Английский

Citations

57

Single Atom Environmental Catalysis: Influence of Supports and Coordination Environments DOI

Lian‐Hua Xu,

Weiping Liu, Kai Liu

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(50)

Published: Aug. 27, 2023

Abstract Single‐atom catalysts (SACs) are desirable in environmental catalysis due to friendliness, structural stability, and maximum utilization of active metal sites. Extensive research has compared the catalytic performance between SACs with different single‐atom metals. However, their is also highly dependent on supports, which play an important role modulating local coordination environment SACs. Unfortunately, a comprehensive review that systematically discusses relationship supports environment, as well combined effects scare. In this review, three widely investigated applications including advanced oxidation processes (AOPs), mainly Fenton Fenton‐like reactions, nitrate reduction reaction (NO 3 RR) focused. By correlating characterization results, performances, computational environments reactivity examined detail, from origin pathways AOPs NO RR attempted reveal. Finally look forward for potential opportunities challenges on‐demand applications, provided.

Language: Английский

Citations

57

Ce-doped MoS2−xnanoflower arrays for electrocatalytic nitrate reduction to ammonia DOI
Yaojing Luo, Kai Chen, Guohui Wang

et al.

Inorganic Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 10(5), P. 1543 - 1551

Published: Jan. 1, 2023

Ce-doped and MoS 2−x nanoflower arrays exhibit a high activity for electrocatalytic nitrate-to-ammonia conversion (NO 3 RR), attributed to the synergy of S-vacancy Ce-dopant enhance NO − activation reduce reaction energy barriers.

Language: Английский

Citations

52

Strong p‐d Orbital Hybridization on Bismuth Nanosheets for High Performing CO2 Electroreduction DOI

Xueying Cao,

Yadong Tian,

Jizhen Ma

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(6)

Published: Nov. 27, 2023

Abstract Single‐atom alloys (SAAs) show great potential for a variety of electrocatalytic reactions. However, the atomic orbital hybridization effect SAAs on electrochemical reactions is unclear yet. Herein, in situ confinement vanadium/molybdenum/tungsten atoms bismuth nanosheet shown to create with rich grain boundaries, respectively. With detailed analysis microstructure and composition, strong p‐d between vanadium enables exceptional performance carbon dioxide (CO 2 ) reduction Faradaic efficiency nearly 100% C1 products wide range from −0.6 −1.4 V, long‐term electrolysis stability 90 h. In‐depth investigations theoretical computations reveal that electron delocalization toward via evokes active centers efficient CO activation σ‐donation O‐to‐Bi, thus reduces protonation energy barriers formate production. such fundamental understanding, SAA electrocatalyst employed fabricated solar‐driven electrolytic cell 5‐hydroxymethylfurfural oxidation, achieving an outstanding 2,5‐furandicarboxylic acid yield 90.5%. This study demonstrates feasible strategy rationally design advanced electrocatalysts basic principles hybridization.

Language: Английский

Citations

50