• Complex
  • Title
  • Keyword
  • Abstract
  • Scholars
  • Journal
  • ISSN
  • Conference
成果搜索

author:

Zhao, J. (Zhao, J..) [1] | Lin, S. (Lin, S..) [2]

Indexed by:

Scopus

Abstract:

The electrocatalytic CO2 reduction reaction (CO2RR) is one of the most important electrocatalytic reactions. Starting from a well-defined *CO intermediate, the CO2RR can bifurcate into two pathways, either forming a hydrogenation product by *[sbnd]C[sbnd]O bond hydrogenation or leading to CO desorption by *[sbnd]C bond cleavage. However, it is perplexing why many dual-atom catalysts (DACs) exhibit high CO selectivity in experiments, despite previous theoretical studies arguing that the *[sbnd]C[sbnd]O bond hydrogenation is thermodynamically more favorable than the *[sbnd]C bond breaking. Furthermore, the selectivity is contingent upon the potential and is perturbed by the hydrogen evolution reaction (HER), which is far from clear. Using ab initio molecular dynamics and a “slow-growth” sampling method to evaluate the potential-dependent kinetics, we uncover the selectivity origin of CO2RR to CO on a typical NC-based DAC (CuFe-N6-C). Importantly, the results show that at higher CO* coverage, CO* desorption kinetics are accelerated, while the competing *[sbnd]C[sbnd]O bond hydrogenation reaction is inhibited at varying potentials. Furthermore, the selectivity of the HER is observed to increase as the potential decreases. However, at higher CO* coverage, the energy barrier for the *[sbnd]C bond cleavage is lower than that for HER, suggesting that HER is suppressed on CuFe-N6-C. Our work unlocks a long-standing puzzle about the selectivity of important DAC catalysts for CO2RR and provides insights for more effective catalyst design. © 2024 Elsevier Inc.

Keyword:

Ab initio molecular dynamics Dual-atom catalyst Electrocatalytic CO2 reduction Potential-dependent kinetics Selectivity

Community:

  • [ 1 ] [Zhao J.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, China
  • [ 2 ] [Lin S.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350002, China

Reprint 's Address:

Email:

Show more details

Related Keywords:

Source :

Journal of Colloid and Interface Science

ISSN: 0021-9797

Year: 2025

Volume: 680

Page: 257-264

9 . 4 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

Affiliated Colleges:

Online/Total:107/10048429
Address:FZU Library(No.2 Xuyuan Road, Fuzhou, Fujian, PRC Post Code:350116) Contact Us:0591-22865326
Copyright:FZU Library Technical Support:Beijing Aegean Software Co., Ltd. 闽ICP备05005463号-1