Promoting biomass electrooxidation via modulating proton and oxygen anion deintercalation in hydroxide

Zuyun He, Jinwoo Hwang, Zhiheng Gong, Mengzhen Zhou, Nian Zhang, Xiongwu Kang, Jeong Woo Han () and Yan Chen ()
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Zuyun He: South China University of Technology
Jinwoo Hwang: Pohang University Science and Technology
Zhiheng Gong: South China University of Technology
Mengzhen Zhou: South China University of Technology
Nian Zhang: Chinese Academy of Sciences
Xiongwu Kang: South China University of Technology
Jeong Woo Han: Pohang University Science and Technology
Yan Chen: South China University of Technology

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract The redox center of transition metal oxides and hydroxides is generally considered to be the metal site. Interestingly, proton and oxygen in the lattice recently are found to be actively involved in the catalytic reactions, and critically determine the reactivity. Herein, taking glycerol electrooxidation reaction as the model reaction, we reveal systematically the impact of proton and oxygen anion (de)intercalation processes on the elementary steps. Combining density functional theory calculations and advanced spectroscopy techniques, we find that doping Co into Ni-hydroxide promotes the deintercalation of proton and oxygen anion from the catalyst surface. The oxygen vacancies formed in NiCo hydroxide during glycerol electrooxidation reaction increase d-band filling on Co sites, facilitating the charge transfer from catalyst surface to cleaved molecules during the 2nd C-C bond cleavage. Consequently, NiCo hydroxide exhibits enhanced glycerol electrooxidation activity, with a current density of 100 mA/cm2 at 1.35 V and a formate selectivity of 94.3%.

Date: 2022
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DOI: 10.1038/s41467-022-31484-0

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