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Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen

Author

Listed:
  • Mingchuan Luo

    (University of Toronto)

  • Ziyun Wang

    (University of Toronto)

  • Yuguang C. Li

    (University of Toronto)

  • Jun Li

    (University of Toronto
    University of Toronto)

  • Fengwang Li

    (University of Toronto)

  • Yanwei Lum

    (University of Toronto)

  • Dae-Hyun Nam

    (University of Toronto)

  • Bin Chen

    (University of Toronto)

  • Joshua Wicks

    (University of Toronto)

  • Aoni Xu

    (University of Toronto)

  • Taotao Zhuang

    (University of Toronto)

  • Wan Ru Leow

    (University of Toronto)

  • Xue Wang

    (University of Toronto)

  • Cao-Thang Dinh

    (University of Toronto)

  • Ying Wang

    (University of Toronto)

  • Yuhang Wang

    (University of Toronto)

  • David Sinton

    (University of Toronto)

  • Edward H. Sargent

    (University of Toronto)

Abstract

Producing liquid fuels such as ethanol from CO2, H2O, and renewable electricity offers a route to store sustainable energy. The search for efficient electrocatalysts for the CO2 reduction reaction relies on tuning the adsorption strength of carbonaceous intermediates. Here, we report a complementary approach in which we utilize hydroxide and oxide doping of a catalyst surface to tune the adsorbed hydrogen on Cu. Density functional theory studies indicate that this doping accelerates water dissociation and changes the hydrogen adsorption energy on Cu. We synthesize and investigate a suite of metal-hydroxide-interface-doped-Cu catalysts, and find that the most efficient, Ce(OH)x-doped-Cu, exhibits an ethanol Faradaic efficiency of 43% and a partial current density of 128 mA cm−2. Mechanistic studies, wherein we combine investigation of hydrogen evolution performance with the results of operando Raman spectroscopy, show that adsorbed hydrogen hydrogenates surface *HCCOH, a key intermediate whose fate determines branching to ethanol versus ethylene.

Suggested Citation

  • Mingchuan Luo & Ziyun Wang & Yuguang C. Li & Jun Li & Fengwang Li & Yanwei Lum & Dae-Hyun Nam & Bin Chen & Joshua Wicks & Aoni Xu & Taotao Zhuang & Wan Ru Leow & Xue Wang & Cao-Thang Dinh & Ying Wang , 2019. "Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-13833-8
    DOI: 10.1038/s41467-019-13833-8
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    Cited by:

    1. Chen, Zhangsen & Zhang, Gaixia & Chen, Hangrong & Prakash, Jai & Zheng, Yi & Sun, Shuhui, 2022. "Multi-metallic catalysts for the electroreduction of carbon dioxide: Recent advances and perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 155(C).
    2. Wei Liu & Mengyang Xia & Chao Zhao & Ben Chong & Jiahe Chen & He Li & Honghui Ou & Guidong Yang, 2024. "Efficient ammonia synthesis from the air using tandem non-thermal plasma and electrocatalysis at ambient conditions," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Yan Lin & Tuo Wang & Lili Zhang & Gong Zhang & Lulu Li & Qingfeng Chang & Zifan Pang & Hui Gao & Kai Huang & Peng Zhang & Zhi-Jian Zhao & Chunlei Pei & Jinlong Gong, 2023. "Tunable CO2 electroreduction to ethanol and ethylene with controllable interfacial wettability," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Xiao Chen & Shuaiqiang Jia & Jianxin Zhai & Jiapeng Jiao & Mengke Dong & Cheng Xue & Ting Deng & Hailian Cheng & Zhanghui Xia & Chunjun Chen & Xueqing Xing & Jianrong Zeng & Haihong Wu & Mingyuan He &, 2024. "Multivalent Cu sites synergistically adjust carbonaceous intermediates adsorption for electrocatalytic ethanol production," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    5. Zhibo Yao & Hao Cheng & Yifei Xu & Xinyu Zhan & Song Hong & Xinyi Tan & Tai-Sing Wu & Pei Xiong & Yun-Liang Soo & Molly Meng-Jung Li & Leiduan Hao & Liang Xu & Alex W. Robertson & Bingjun Xu & Ming Ya, 2024. "Hydrogen radical-boosted electrocatalytic CO2 reduction using Ni-partnered heteroatomic pairs," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    6. Pengtang Wang & Hao Yang & Cheng Tang & Yu Wu & Yao Zheng & Tao Cheng & Kenneth Davey & Xiaoqing Huang & Shi-Zhang Qiao, 2022. "Boosting electrocatalytic CO2–to–ethanol production via asymmetric C–C coupling," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    7. Jiaqi Feng & Libing Zhang & Shoujie Liu & Liang Xu & Xiaodong Ma & Xingxing Tan & Limin Wu & Qingli Qian & Tianbin Wu & Jianling Zhang & Xiaofu Sun & Buxing Han, 2023. "Modulating adsorbed hydrogen drives electrochemical CO2-to-C2 products," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    8. Jiahui Bi & Pengsong Li & Jiyuan Liu & Shuaiqiang Jia & Yong Wang & Qinggong Zhu & Zhimin Liu & Buxing Han, 2023. "Construction of 3D copper-chitosan-gas diffusion layer electrode for highly efficient CO2 electrolysis to C2+ alcohols," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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