CO2/carbonate-mediated electrochemical water oxidation to hydrogen peroxide

Lei Fan, Xiaowan Bai, Chuan Xia, Xiao Zhang, Xunhua Zhao, Yang Xia, Zhen-Yu Wu, Yingying Lu (), Yuanyue Liu () and Haotian Wang ()
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Lei Fan: Rice University
Xiaowan Bai: The University of Texas at Austin
Chuan Xia: Rice University
Xiao Zhang: Rice University
Xunhua Zhao: The University of Texas at Austin
Yang Xia: Rice University
Zhen-Yu Wu: Rice University
Yingying Lu: College of Chemical and Biological Engineering, Zhejiang University
Yuanyue Liu: The University of Texas at Austin
Haotian Wang: Rice University

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Electrochemical water oxidation reaction (WOR) to hydrogen peroxide (H2O2) via a 2e− pathway provides a sustainable H2O2 synthetic route, but is challenged by the traditional 4e− counterpart of oxygen evolution. Here we report a CO2/carbonate mediation approach to steering the WOR pathway from 4e− to 2e−. Using fluorine-doped tin oxide electrode in carbonate solutions, we achieved high H2O2 selectivity of up to 87%, and delivered unprecedented H2O2 partial currents of up to 1.3 A cm−2, which represents orders of magnitude improvement compared to literature. Molecular dynamics simulations, coupled with electron paramagnetic resonance and isotope labeling experiments, suggested that carbonate mediates the WOR pathway to H2O2 through the formation of carbonate radical and percarbonate intermediates. The high selectivity, industrial-relevant activity, and good durability open up practical opportunities for delocalized H2O2 production.

Date: 2022
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DOI: 10.1038/s41467-022-30251-5

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