Size-Dependent Nickel-Based Electrocatalysts for Selective CO2 Reduction

Zhida Li; Dong He; Xingxu Yan; Sheng Dai; Sabrina Younan; Zunjian Ke; Xiaoqing Pan; Xiangheng Xiao; Hongjun Wu; Jing Gu

doi:10.1002/anie.202000318

Size-Dependent Nickel-Based Electrocatalysts for Selective CO₂ Reduction

Angew Chem Int Ed Engl. 2020 Oct 12;59(42):18572-18577. doi: 10.1002/anie.202000318. Epub 2020 Aug 20.

Authors

Zhida Li^{1

2}, Dong He³, Xingxu Yan⁴, Sheng Dai⁴, Sabrina Younan², Zunjian Ke^{2

3}, Xiaoqing Pan^{4

5}, Xiangheng Xiao³, Hongjun Wu^{1

2}, Jing Gu²

Affiliations

¹ College of Chemistry & Chemical Engineering, Northeast Petroleum University, Daqing, 163318, China.
² Department of Chemistry and Biochemistry, San Diego State University, 5500 Campanile Drive, San Diego, CA, 92182-1030, USA.
³ Department of Physics and Key Laboratory of Artificial Micro- and Nano-structures of Ministry of Education, Institute of Technological Sciences, Wuhan University, Wuhan, 430072, China.
⁴ Department of Materials Science and Engineering, University of California, Irvine, Irvine, CA, 92697, USA.
⁵ Department of Physics and Astronomy, University of California, Irvine, Irvine, CA, 92697, USA.

PMID: 32686244
DOI: 10.1002/anie.202000318

Abstract

Closing the anthropogenic carbon cycle by converting CO₂ into reusable chemicals is an attractive solution to mitigate rising concentrations of CO₂ in the atmosphere. Herein, we prepared Ni metal catalysts ranging in size from single atoms to over 100 nm and distributed them across N-doped carbon substrates which were obtained from converted zeolitic imidazolate frameworks (ZIF). The results show variance in CO₂ reduction performance with variance in Ni metal size. Ni single atoms demonstrate a superior Faradaic efficiency (FE) for CO selectivity (ca. 97 % at -0.8 V vs. RHE), while results for 4.1 nm Ni nanoparticles are slightly lower (ca. 93 %). Further increase the Ni particle size to 37.2 nm allows the H₂ evolution reaction (HER) to compete with the CO₂ reduction reaction (CO₂ RR). The FE towards CO production decreases to under 30 % and HER efficiency increase to over 70 %. These results show a size-dependent CO₂ reduction for various sizes of Ni metal catalysts.

Keywords: CO selectivity; CO2 reduction; DFT calculations; nickel; size dependence.

Abstract

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