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  4. Efficient Cu2O Photocathodes for Aqueous Photoelectrochemical CO2 Reduction to Formate and Syngas
 
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research article

Efficient Cu2O Photocathodes for Aqueous Photoelectrochemical CO2 Reduction to Formate and Syngas

Xia, Meng  
•
Pan, Linfeng  
•
Liu, Yongpeng  
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December 13, 2023
Journal Of The American Chemical Society

Photoelectrochemical carbon dioxide reduction (PEC-CO2R) represents a promising approach for producing renewable fuels and chemicals using solar energy. However, attaining even modest solar-to-fuel (STF) conversion efficiency often necessitates the use of costly semiconductors and noble-metal catalysts. Herein, we present a Cu2O/Ga2O3/TiO2 photocathode modified with Sn/SnOx catalysts through a simple photoelectrodeposition method. It achieves a remarkable half-cell STF efficiency of similar to 0.31% for the CO2R in aqueous KHCO3 electrolyte, under AM 1.5 G illumination. The system enables efficient production of syngas (FE: similar to 62%, CO/H-2 approximate to 1:2) and formate (FE: similar to 38%) with a consistent selectivity over a wide potential range, from +0.34 to -0.16 V vs the reversible hydrogen electrode. We ascribe the observed performance to the favorable optoelectronic characteristics of our Cu2O heterostructure and the efficient Sn/SnOx catalysts incorporated in the PEC-CO2R reactions. Through comprehensive experimental investigations, we elucidate the indispensable role of Cu2O buried p-n junctions in generating a high photovoltage (similar to 1 V) and enabling efficient bulk charge separation (up to similar to 70% efficiency). Meanwhile, we discover that the deposited Sn/SnOx catalysts have critical dual effects on the overall performance of the PEC devices, serving as active CO2R catalysts as well as the semiconductor front contact. It could facilitate interfacial electron transfer between the catalysts and the semiconductor device for CO2R by establishing a barrier-free ohmic contact.

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Type
research article
DOI
10.1021/jacs.3c06146
Web of Science ID

WOS:001133460100001

Author(s)
Xia, Meng  
•
Pan, Linfeng  
•
Liu, Yongpeng  
•
Gao, Jing  
•
Li, Jun  
•
Mensi, Mounir  
•
Sivula, Kevin  
•
Zakeeruddin, Shaik M.  
•
Ren, Dan  
•
Gratzel, Michael  
Date Issued

2023-12-13

Publisher

Amer Chemical Soc

Published in
Journal Of The American Chemical Society
Volume

145

Issue

51

Start page

27939

End page

27949

Subjects

Physical Sciences

•

Atomic Layer

•

Carbon-Dioxide

•

Artificial Photosynthesis

•

Enhanced Activity

•

Water Oxidation

•

Tin Electrodes

•

Conversion

•

Films

•

Photocatalyst

•

Catalyst

Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LSPM  
LIMNO  
LPI  
FunderGrant Number

Xi'an Jiaotong University

514259

Strategic Japanese-Swiss Science and Technology grant

GRS-080/19

Swiss National Science Foundation (SNSF)

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Available on Infoscience
February 20, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/204861
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