Electroreduction of CO2to Formate on a Copper-Based Electrocatalyst at High Pressures with High Energy Conversion Efficiency

Jiachen Li, Yun Kuang, Yongtao Meng, Xin Tian, Wei Hsuan Hung, Xiao Zhang, Aowen Li, Mingquan Xu, Wu Zhou, Ching Shun Ku, Ching Yu Chiang, Guanzhou Zhu, Jinyu Guo, Xiaoming Sun, Hongjie Dai

Research output: Contribution to journalArticlepeer-review

68 Scopus citations

Abstract

Electrocatalytic CO2 reduction (CO2RR) to valuable fuels is a promising approach to mitigate energy and environmental problems, but controlling the reaction pathways and products remains challenging. Here a novel Cu2O nanoparticle film was synthesized by square-wave (SW) electrochemical redox cycling of high-purity Cu foils. The cathode afforded up to 98% Faradaic efficiency for electroreduction of CO2 to nearly pure formate under ≥45 atm CO2 in bicarbonate catholytes. When this cathode was paired with a newly developed NiFe hydroxide carbonate anode in KOH/borate anolyte, the resulting two-electrode high-pressure electrolysis cell achieved high energy conversion efficiencies of up to 55.8% stably for long-term formate production. While the high-pressure conditions drastically increased the solubility of CO2 to enhance CO2 reduction and suppress hydrogen evolution, the (111)-oriented Cu2O film was found to be important to afford nearly 100% CO2 reduction to formate. The results have implications for CO2 reduction to a single liquid product with high energy conversion efficiency.

Original languageEnglish
Pages (from-to)7276-7282
Number of pages7
JournalJournal of the American Chemical Society
Volume142
Issue number16
DOIs
StatePublished - 22 Apr 2020

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