In:
Angewandte Chemie, Wiley, Vol. 132, No. 52 ( 2020-12-21), p. 23849-23856
Abstract:
It is still a great challenge to achieve high selectivity of CH 4 in CO 2 electroreduction reactions (CO 2 RR) because of the similar reduction potentials of possible products and the sluggish kinetics for CO 2 activation. Stabilizing key reaction intermediates by single type of active sites supported on porous conductive material is crucial to achieve high selectivity for single product such as CH 4 . Here, Cu 2 O(111) quantum dots with an average size of 3.5 nm are in situ synthesized on a porous conductive copper‐based metal–organic framework (CuHHTP), exhibiting high selectivity of 73 % towards CH 4 with partial current density of 10.8 mA cm −2 at −1.4 V vs. RHE (reversible hydrogen electrode) in CO 2 RR. Operando infrared spectroscopy and DFT calculations reveal that the key intermediates (such as *CH 2 O and *OCH 3 ) involved in the pathway of CH 4 formation are stabilized by the single active Cu 2 O(111) and hydrogen bonding, thus generating CH 4 instead of CO.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v132.52
DOI:
10.1002/ange.202010601
Language:
English
Publisher:
Wiley
Publication Date:
2020
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