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Alcohols electrooxidation coupled with H2 production at high current densities promoted by a cooperative catalyst

Author

Listed:
  • Zhenhua Li

    (Beijing University of Chemical Technology)

  • Yifan Yan

    (Beijing University of Chemical Technology)

  • Si-Min Xu

    (Beijing University of Chemical Technology)

  • Hua Zhou

    (Tsinghua University)

  • Ming Xu

    (Beijing University of Chemical Technology)

  • Lina Ma

    (Beijing University of Chemical Technology)

  • Mingfei Shao

    (Beijing University of Chemical Technology)

  • Xianggui Kong

    (Beijing University of Chemical Technology)

  • Bin Wang

    (Sinopec Group)

  • Lirong Zheng

    (the Chinese Academy of Sciences)

  • Haohong Duan

    (Tsinghua University)

Abstract

Electrochemical alcohols oxidation offers a promising approach to produce valuable chemicals and facilitate coupled H2 production. However, the corresponding current density is very low at moderate cell potential that substantially limits the overall productivity. Here we report the electrooxidation of benzyl alcohol coupled with H2 production at high current density (540 mA cm−2 at 1.5 V vs. RHE) over a cooperative catalyst of Au nanoparticles supported on cobalt oxyhydroxide nanosheets (Au/CoOOH). The absolute current can further reach 4.8 A at 2.0 V in a more realistic two-electrode membrane-free flow electrolyzer. Experimental combined with theoretical results indicate that the benzyl alcohol can be enriched at Au/CoOOH interface and oxidized by the electrophilic oxygen species (OH*) generated on CoOOH, leading to higher activity than pure Au. Based on the finding that the catalyst can be reversibly oxidized/reduced at anodic potential/open circuit, we design an intermittent potential (IP) strategy for long-term alcohol electrooxidation that achieves high current density (>250 mA cm−2) over 24 h with promoted productivity and decreased energy consumption.

Suggested Citation

  • Zhenhua Li & Yifan Yan & Si-Min Xu & Hua Zhou & Ming Xu & Lina Ma & Mingfei Shao & Xianggui Kong & Bin Wang & Lirong Zheng & Haohong Duan, 2022. "Alcohols electrooxidation coupled with H2 production at high current densities promoted by a cooperative catalyst," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-021-27806-3
    DOI: 10.1038/s41467-021-27806-3
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    3. Zheng-Jie Chen & Jiuyi Dong & Jiajing Wu & Qiting Shao & Na Luo & Minwei Xu & Yuanmiao Sun & Yongbing Tang & Jing Peng & Hui-Ming Cheng, 2023. "Acidic enol electrooxidation-coupled hydrogen production with ampere-level current density," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Jiachen Li & Yuqiang Ma & Cong Zhang & Chi Zhang & Huijun Ma & Zhaoqi Guo & Ning Liu & Ming Xu & Haixia Ma & Jieshan Qiu, 2023. "Green electrosynthesis of 3,3’-diamino-4,4’-azofurazan energetic materials coupled with energy-efficient hydrogen production over Pt-based catalysts," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    5. Wei Chen & Liang Zhang & Leitao Xu & Yuanqing He & Huan Pang & Shuangyin Wang & Yuqin Zou, 2024. "Pulse potential mediated selectivity for the electrocatalytic oxidation of glycerol to glyceric acid," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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