Active and conductive layer stacked superlattices for highly selective CO2 electroreduction

Junyuan Duan, Tianyang Liu, Yinghe Zhao, Ruoou Yang, Yang Zhao, Wenbin Wang, Youwen Liu (), Huiqiao Li, Yafei Li () and Tianyou Zhai ()
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Junyuan Duan: Huazhong University of Science and Technology
Tianyang Liu: Nanjing Normal University
Yinghe Zhao: Huazhong University of Science and Technology
Ruoou Yang: Huazhong University of Science and Technology
Yang Zhao: Huazhong University of Science and Technology
Wenbin Wang: Huazhong University of Science and Technology
Youwen Liu: Huazhong University of Science and Technology
Huiqiao Li: Huazhong University of Science and Technology
Yafei Li: Nanjing Normal University
Tianyou Zhai: Huazhong University of Science and Technology

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Metal oxides are archetypal CO2 reduction reaction electrocatalysts, yet inevitable self-reduction will enhance competitive hydrogen evolution and lower the CO2 electroreduction selectivity. Herein, we propose a tangible superlattice model of alternating metal oxides and selenide sublayers in which electrons are rapidly exported through the conductive metal selenide layer to protect the active oxide layer from self-reduction. Taking BiCuSeO superlattices as a proof-of-concept, a comprehensive characterization reveals that the active [Bi2O2]2+ sublayers retain oxidation states rather than their self-reduced Bi metal during CO2 electroreduction because of the rapid electron transfer through the conductive [Cu2Se2]2- sublayer. Theoretical calculations uncover the high activity over [Bi2O2]2+ sublayers due to the overlaps between the Bi p orbitals and O p orbitals in the OCHO* intermediate, thus achieving over 90% formate selectivity in a wide potential range from −0.4 to −1.1 V. This work broadens the studying and improving of the CO2 electroreduction properties of metal oxide systems.

Date: 2022
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DOI: 10.1038/s41467-022-29699-2

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