Advanced Materials, volume 34, issue 29, pages 2202854

Synergistic Cr 2 O 3 @Ag Heterostructure Enhanced Electrocatalytic CO 2 Reduction to CO

Huai Qin Fu 1
Liu Junxian 1
Nicholas M. Bedford 2
Yun Wang 1
Ji-Wei Sun 3
Yu Zou 1
Mengyang Dong 1
Joshua Wright 4
Hui Diao 5
Porun Liu 1
Hua Gui Yang 3
Huijun Zhao 1
Show full list: 12 authors
Publication typeJournal Article
Publication date2022-06-10
scimago Q1
SJR9.191
CiteScore43.0
Impact factor27.4
ISSN09359648, 15214095
General Materials Science
Mechanical Engineering
Mechanics of Materials
Abstract
The electrocatalytic CO2RR to produce value-added chemicals and fuels has been recognized as a promising means to reduce the reliance on fossil resources; it is, however, hindered due to the lack of high-performance electrocatalysts. The effectiveness of sculpturing metal/metal oxides (MMO) heterostructures to enhance electrocatalytic performance toward CO2RR has been well documented, nonetheless, the precise synergistic mechanism of MMO remains elusive. Herein, an in operando electrochemically synthesized Cr2O3–Ag heterostructure electrocatalyst (Cr2O3@Ag) is reported for efficient electrocatalytic reduction of CO2 to CO. The obtained Cr2O3@Ag can readily achieve a superb FECO of 99.6% at −0.8 V (vs RHE) with a high JCO of 19.0 mA cm−2. These studies also confirm that the operando synthesized Cr2O3@Ag possesses high operational stability. Notably, operando Raman spectroscopy studies reveal that the markedly enhanced performance is attributable to the synergistic Cr2O3–Ag heterostructure induced stabilization of CO2•−/*COOH intermediates. DFT calculations unveil that the metallic-Ag-catalyzed CO2 reduction to CO requires a 1.45 eV energy input to proceed, which is 0.93 eV higher than that of the MMO-structured Cr2O3@Ag. The exemplified approaches in this work would be adoptable for design and development of high-performance electrocatalysts for other important reactions.
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