In:
Angewandte Chemie, Wiley, Vol. 134, No. 23 ( 2022-06-07)
Abstract:
Regulating intermediates through elaborate catalyst design to control the reaction direction is crucial for promoting the selectivity of electrocatalytic CO 2 ‐to‐CH 4 . M−C (M=metal) bonds are particularly important for tuning the multi‐electron reaction; however, its construction in nanomaterials is challenging. Here, via rational design of in situ anchoring of Cu SAs (single atoms) on the unique platform graphdiyne, we firstly realize the construction of a chemical bond Cu−C (GDY). In situ Raman spectroelectrochemistry and DFT calculations confirm that due to the fabrication of the Cu−C bond, during CO 2 reduction, the formation of *OCHO intermediates is dominant rather than *COOH on Cu atoms, facilitating the formation of CH 4 . Therefore, we find that constructing the Cu−C bond in Cu SAs/GDY can supply an efficient charge transfer channel, but most importantly control the reaction intermediates and guide a more facile reaction pathway to CH 4 , thereby significantly boosting its catalytic performance. This work provides new insights on enhancing the selectivity for CO 2 RR at the atomic level.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v134.23
DOI:
10.1002/ange.202203569
Language:
English
Publisher:
Wiley
Publication Date:
2022
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