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author:

Zhao, Jia (Zhao, Jia.) [1] | Lin, Sen (Lin, Sen.) [2]

Indexed by:

EI

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:

Catalyst selectivity Copper alloys Electrolytic reduction Energy barriers Hydrogenation Hydrogen bonds Molecular dynamics Reaction intermediates Reaction kinetics

Community:

  • [ 1 ] [Zhao, Jia]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350002, China
  • [ 2 ] [Lin, Sen]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350002, China

Reprint 's Address:

  • [lin, sen]state key laboratory of photocatalysis on energy and environment, college of chemistry, fuzhou university, fuzhou; 350002, china;;

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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: 2

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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