In Situ Topotactic Transformation of an Interstitial Alloy for CO Electroreduction

Changming Zhao; Gan Luo; Xiaokang Liu; Wei Zhang; Zhijun Li; Qian Xu; Qinghua Zhang; Huijuan Wang; Deming Li; Fangyao Zhou; Yunteng Qu; Xiao Han; Zezhou Zhu; Geng Wu; Jing Wang; Junfa Zhu; Tao Yao; Yafei Li; Henny J M Bouwmeester; Yuen Wu

doi:10.1002/adma.202002382

In Situ Topotactic Transformation of an Interstitial Alloy for CO Electroreduction

Adv Mater. 2020 Oct;32(39):e2002382. doi: 10.1002/adma.202002382. Epub 2020 Aug 23.

Authors

Changming Zhao¹, Gan Luo², Xiaokang Liu³, Wei Zhang³, Zhijun Li⁴, Qian Xu⁵, Qinghua Zhang⁶, Huijuan Wang⁷, Deming Li¹, Fangyao Zhou¹, Yunteng Qu¹, Xiao Han¹, Zezhou Zhu⁸, Geng Wu¹, Jing Wang¹, Junfa Zhu⁵, Tao Yao³, Yafei Li², Henny J M Bouwmeester^{9

10}, Yuen Wu¹

Affiliations

¹ Department of Chemistry, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei, 230026, China.
² Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, 210023, China.
³ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, P.R. China.
⁴ Provincial Key Laboratory of Oil and Gas Chemical Technology, College of Chemistry and Chemical Engineering, Northeast Petrolrum University, Daqing, 163318, P. R. China.
⁵ The Catalysis and Surface Science Endstation at the BL11U beamline in the National Synchrotron Radiation Laboratory (NSRL) in Hefei, China.
⁶ Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China.
⁷ USTC Center for Micro and Nanoscale Research and Fabrication, University of Science and Technology of China, P. R. China.
⁸ Division of Advanced Nanomaterials, Suzhou Institute of Nano-tech and Nano-bionics, Chinese Academy of Sciences, Suzhou, 215123, China.
⁹ Electrochemistry Research group, Membrane Science and Technology, MESA+ Institute for Nanotechnology, University of Twente, P.O. Box 217, Enschede, 7500 AE, The Netherlands.
¹⁰ CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, P. R. China.

PMID: 32830410
DOI: 10.1002/adma.202002382

Abstract

Electrochemical reduction of CO to value-added products holds promise for storage of energy from renewable sources. Copper can convert CO into multi-carbon (C₂₊ ) products during CO electroreduction. However, developing a Cu electrocatalyst with a high selectivity for CO reduction and desirable production rates for C₂₊ products remains challenging. Herein, highly lattice-disordered Cu₃ N with abundant twin structures as a precursor electrocatalyst is examined for CO reduction. Through in situ activation during the CO reduction reaction (CORR) and concomitant release of nitrogen, the obtained metallic Cu° catalyst particles inherit the lattice dislocations present in the parent Cu₃ N lattice. The de-nitrified catalyst delivers an unprecedented C₂₊ Faradaic efficiency of over 90% at a current density of 727 mA cm^-2 in a flow cell system. Using a membrane electrode assembly (MEA) electrolyzer with a solid-state electrolyte (SSE), a 17.4 vol% ethylene stream and liquid streams with concentration of 1.45 m and 230 × 10^-3 m C₂₊ products at the outlet of the cathode and SSE-containment layer are obtained.

Keywords: CO electroreduction; Cu 3N; high concentration products streams; lattice dislocations; multi-carbon products.

Abstract

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