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Edge-rich molybdenum disulfide tailors carbon-chain growth for selective hydrogenation of carbon monoxide to higher alcohols

Author

Listed:
  • Jingting Hu

    (Chinese Academy of Sciences
    Xiamen University)

  • Zeyu Wei

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Yunlong Zhang

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Rui Huang

    (Chinese Academy of Sciences)

  • Mingchao Zhang

    (Xiamen University)

  • Kang Cheng

    (Xiamen University)

  • Qinghong Zhang

    (Xiamen University)

  • Yutai Qi

    (Chinese Academy of Sciences
    Xiamen University)

  • Yanan Li

    (Chinese Academy of Sciences
    Xiamen University)

  • Jun Mao

    (Chinese Academy of Sciences
    Xiamen University)

  • Junfa Zhu

    (University of Science and Technology of China)

  • Lihui Wu

    (University of Science and Technology of China)

  • Wu Wen

    (University of Science and Technology of China)

  • Shengsheng Yu

    (University of Science and Technology of China)

  • Yang Pan

    (University of Science and Technology of China)

  • Jiuzhong Yang

    (University of Science and Technology of China)

  • Xiangjun Wei

    (Chinese Academy of Sciences)

  • Luozhen Jiang

    (Chinese Academy of Sciences)

  • Rui Si

    (Chinese Academy of Sciences)

  • Liang Yu

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Ye Wang

    (Xiamen University)

  • Dehui Deng

    (Chinese Academy of Sciences
    Xiamen University
    University of Chinese Academy of Sciences)

Abstract

Selective hydrogenation of carbon monoxide (CO) to higher alcohols (C2+OH) is a promising non-petroleum route for producing high-value chemicals, in which precise regulations of both C-O cleavage and C-C coupling are highly essential but remain great challenges. Herein, we report that highly selective CO hydrogenation to C2-4OH is achieved over a potassium-modified edge-rich molybdenum disulfide (MoS2) catalyst, which delivers a high CO conversion of 17% with a superior C2-4OH selectivity of 45.2% in hydrogenated products at 240 °C and 50 bar, outperforming previously reported non-noble metal-based catalysts under similar conditions. By regulating the relative abundance of edge to basal plane, C2-4OH to methanol selectivity ratio can be overturned from 0.4 to 2.2. Mechanistic studies reveal that sulfur vacancies at MoS2 edges boost carbon-chain growth by facilitating not only C-O cleavage but also C-C coupling, while potassium promotes the desorption of alcohols via electrostatic interaction with hydroxyls, thereby enabling preferential formation of C2-4OH.

Suggested Citation

  • Jingting Hu & Zeyu Wei & Yunlong Zhang & Rui Huang & Mingchao Zhang & Kang Cheng & Qinghong Zhang & Yutai Qi & Yanan Li & Jun Mao & Junfa Zhu & Lihui Wu & Wu Wen & Shengsheng Yu & Yang Pan & Jiuzhong , 2023. "Edge-rich molybdenum disulfide tailors carbon-chain growth for selective hydrogenation of carbon monoxide to higher alcohols," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42325-z
    DOI: 10.1038/s41467-023-42325-z
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    References listed on IDEAS

    as
    1. Yuhao Wang & Shyam Kattel & Wengui Gao & Kongzhai Li & Ping Liu & Jingguang G. Chen & Hua Wang, 2019. "Exploring the ternary interactions in Cu–ZnO–ZrO2 catalysts for efficient CO2 hydrogenation to methanol," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    2. Jiao Deng & Haobo Li & Suheng Wang & Ding Ding & Mingshu Chen & Chuan Liu & Zhongqun Tian & K. S. Novoselov & Chao Ma & Dehui Deng & Xinhe Bao, 2017. "Multiscale structural and electronic control of molybdenum disulfide foam for highly efficient hydrogen production," Nature Communications, Nature, vol. 8(1), pages 1-8, April.
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