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Converting copper sulfide to copper with surface sulfur for electrocatalytic alkyne semi-hydrogenation with water

Author

Listed:
  • Yongmeng Wu

    (Tianjin University)

  • Cuibo Liu

    (Tianjin University)

  • Changhong Wang

    (Tianjin University)

  • Yifu Yu

    (Tianjin University)

  • Yanmei Shi

    (Tianjin University)

  • Bin Zhang

    (Tianjin University
    Collaborative Innovation Center of Chemical Science and Engineering)

Abstract

Electrocatalytic alkyne semi-hydrogenation to alkenes with water as the hydrogen source using a low-cost noble-metal-free catalyst is highly desirable but challenging because of their over-hydrogenation to undesired alkanes. Here, we propose that an ideal catalyst should have the appropriate binding energy with active atomic hydrogen (H*) from water electrolysis and a weaker adsorption with an alkene, thus promoting alkyne semi-hydrogenation and avoiding over-hydrogenation. So, surface sulfur-doped and -adsorbed low-coordinated copper nanowire sponges are designedly synthesized via in situ electroreduction of copper sulfide and enable electrocatalytic alkyne semi-hydrogenation with over 99% selectivity using water as the hydrogen source, outperforming a copper counterpart without surface sulfur. Sulfur anion-hydrated cation (S2−-K+(H2O)n) networks between the surface adsorbed S2− and K+ in the KOH electrolyte boost the production of active H* from water electrolysis. And the trace doping of sulfur weakens the alkene adsorption, avoiding over-hydrogenation. Our catalyst also shows wide substrate scopes, up to 99% alkenes selectivity, good reducible groups compatibility, and easily synthesized deuterated alkenes, highlighting the promising potential of this method.

Suggested Citation

  • Yongmeng Wu & Cuibo Liu & Changhong Wang & Yifu Yu & Yanmei Shi & Bin Zhang, 2021. "Converting copper sulfide to copper with surface sulfur for electrocatalytic alkyne semi-hydrogenation with water," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-24059-y
    DOI: 10.1038/s41467-021-24059-y
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    Cited by:

    1. Juwen Gu & Wanbing Gong & Qian Zhang & Ran Long & Jun Ma & Xinyu Wang & Jiawei Li & Jiayi Li & Yujian Fan & Xinqi Zheng & Songbai Qiu & Tiejun Wang & Yujie Xiong, 2023. "Enabling direct-growth route for highly efficient ethanol upgrading to long-chain alcohols in aqueous phase," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    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. Nannan Meng & Jiang Shao & Hongjiao Li & Yuting Wang & Xiaoli Fu & Cuibo Liu & Yifu Yu & Bin Zhang, 2022. "Electrosynthesis of formamide from methanol and ammonia under ambient conditions," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    4. Meng He & Yongmeng Wu & Rui Li & Yuting Wang & Cuibo Liu & Bin Zhang, 2023. "Aqueous pulsed electrochemistry promotes C−N bond formation via a one-pot cascade approach," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    5. Yongmeng Wu & Jinghui Zhao & Changhong Wang & Tieliang Li & Bo-Hang Zhao & Ziyang Song & Cuibo Liu & Bin Zhang, 2023. "Electrosynthesis of a nylon-6 precursor from cyclohexanone and nitrite under ambient conditions," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    6. Suheng Wang & Kelechi Uwakwe & Liang Yu & Jinyu Ye & Yuezhou Zhu & Jingting Hu & Ruixue Chen & Zheng Zhang & Zhiyou Zhou & Jianfeng Li & Zhaoxiong Xie & Dehui Deng, 2021. "Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions," Nature Communications, Nature, vol. 12(1), pages 1-9, December.

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