Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons

Nature Chemistry
Yansong ZhouEdward H Sargent

Abstract

The electrochemical reduction of CO2 to multi-carbon products has attracted much attention because it provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the efficiency of CO2 conversion to C2 products remains below that necessary for its implementation at scale. Modifying the local electronic structure of copper with positive valence sites has been predicted to boost conversion to C2 products. Here, we use boron to tune the ratio of Cuδ+ to Cu0 active sites and improve both stability and C2-product generation. Simulations show that the ability to tune the average oxidation state of copper enables control over CO adsorption and dimerization, and makes it possible to implement a preference for the electrosynthesis of C2 products. We report experimentally a C2 Faradaic efficiency of 79 ± 2% on boron-doped copper catalysts and further show that boron doping leads to catalysts that are stable for in excess of ~40 hours while electrochemically reducing CO2 to multi-carbon hydrocarbons.

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Citations

Mar 29, 2019·Advanced Materials·Wei WangTierui Zhang
Nov 21, 2019·Nature·Fengwang LiEdward H Sargent
Dec 12, 2019·Proceedings of the National Academy of Sciences of the United States of America·Yanming LiuThomas J Meyer
Aug 7, 2019·Nature Materials·David WakerleyVictor Mougel
Dec 12, 2019·Chemistry, an Asian Journal·Ji Yong ChoiHyunjoon Song
Jun 17, 2020·Nature Communications·Run ShiTierui Zhang
Nov 30, 2019·Nature Communications·Xue WangEdward H Sargent
Feb 3, 2021·Chemical Communications : Chem Comm·Linfeng XieQing Li
Feb 12, 2021·Journal of the American Chemical Society·Jianchun WangRobert H Grubbs
Oct 20, 2020·Chemical Society Reviews·Wanlin GaoSang-Eon Park

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Methods Mentioned

BETA
X-ray
electron tomography
NMR

Software Mentioned

Vienna Ab initio Simulation Package code
ASTRA

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