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

Author

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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)

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%.

Suggested Citation

  • Zuyun He & Jinwoo Hwang & Zhiheng Gong & Mengzhen Zhou & Nian Zhang & Xiongwu Kang & Jeong Woo Han & Yan Chen, 2022. "Promoting biomass electrooxidation via modulating proton and oxygen anion deintercalation in hydroxide," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-31484-0
    DOI: 10.1038/s41467-022-31484-0
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    3. Yuyang Pan & Huiyan Zhang & Bowen Zhang & Feng Gong & Jianyong Feng & Huiting Huang & Srinivas Vanka & Ronglei Fan & Qi Cao & Mingrong Shen & Zhaosheng Li & Zhigang Zou & Rui Xiao & Sheng Chu, 2023. "Renewable formate from sunlight, biomass and carbon dioxide in a photoelectrochemical cell," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    4. Yuan Lu & Byoung Guan Lee & Cheng Lin & Tae-Kyung Liu & Zhipeng Wang & Jiaming Miao & Sang Ho Oh & Ki Chul Kim & Kan Zhang & Jong Hyeok Park, 2024. "Solar-driven highly selective conversion of glycerol to dihydroxyacetone using surface atom engineered BiVO4 photoanodes," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    5. Lin Chen & Chang Yu & Xuedan Song & Junting Dong & Jiawei Mu & Jieshan Qiu, 2024. "Integrated electrochemical and chemical system for ampere-level production of terephthalic acid alternatives and hydrogen," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    6. Hua Zhou & Yue Ren & Bingxin Yao & Zhenhua Li & Ming Xu & Lina Ma & Xianggui Kong & Lirong Zheng & Mingfei Shao & Haohong Duan, 2023. "Scalable electrosynthesis of commodity chemicals from biomass by suppressing non-Faradaic transformations," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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