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Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates

Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates

Authors :
Guihua Li
Yonghui Zhao
Jerry Pui Ho Li
Wei Chen
Shoujie Li
Xiao Dong
Yanfang Song
Yong Yang
Wei Wei
Yuhan Sun
Source :
Catalysts, Vol 11, Iss 1502, p 1502 (2021)
Publication Year :
2021
Publisher :
MDPI AG, 2021.

Abstract

Conversion of CO2 to valuable chemicals driven by renewable electricity via electrocatalytic reduction processes is of great significance for achieving carbon neutrality. Copper-based materials distinguish themselves from other electrocatalysts for their unique capability to produce multicarbon compounds in CO2 electroreduction. However, the intrinsic active composition and C–C coupling mechanism of copper-based catalysts are still ambiguous. This is largely due to the absence of appropriate in situ approaches to monitor the complicated processes of CO2 electroreduction. Here, we adopted operando spectroscopy techniques, including Raman and infrared, to investigate the evolution of compositions and intermediates during gas-phase CO2 electroreduction on Cu foam, Cu2O nanowire and CuO nanowire catalysts. Although all the three copper-based catalysts possessed the activity of electroreducing gas-phase CO2 to multicarbon oxygenates, Cu2O nanowires showed the much superior performance with a 71.9% Faradaic efficiency of acetaldehyde. Operando Raman spectra manifested that the cuprous oxide remained stable during the whole gas-phase CO2 electroreduction, and operando diffuse reflectance infrared Fourier transform spectroscopy (DRFITS) results provide direct evidences of key intermediates and their evolutions for producing multicarbon oxygenates, in consistence with the density functional theory calculations.

Details

ISSN :
20734344
Volume :
11
Database :
OpenAIRE
Journal :
Catalysts
Accession number :
edsair.doi.dedup.....c7d3b502391f4e1d04106a7f438c09fa
Full Text :
https://doi.org/10.3390/catal11121502