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

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 Yang; Xiangjun Wei; Luozhen Jiang; Rui Si; Liang Yu; Ye Wang; Dehui Deng

doi:10.1038/s41467-023-42325-z

Nature Communications (Oct 2023)

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

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 Yang,
Xiangjun Wei,
Luozhen Jiang,
Rui Si,
Liang Yu,
Ye Wang,
Dehui Deng

Affiliations

Jingting Hu: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Zeyu Wei: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Yunlong Zhang: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Rui Huang: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Mingchao Zhang: State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University
Kang Cheng: State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University
Qinghong Zhang: State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University
Yutai Qi: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Yanan Li: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Jun Mao: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Junfa Zhu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Lihui Wu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wu Wen: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Shengsheng Yu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Yang Pan: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Jiuzhong Yang: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Xiangjun Wei: Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences
Luozhen Jiang: Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Rui Si: Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Liang Yu: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Ye Wang: State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University
Dehui Deng: State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences

DOI: https://doi.org/10.1038/s41467-023-42325-z
Journal volume & issue: Vol. 14, no. 1
pp. 1 – 11

Abstract

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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.

Published in Nature Communications

ISSN: 2041-1723 (Online)
Publisher: Nature Portfolio
Country of publisher: United Kingdom
LCC subjects: Science
Website: https://www.nature.com/ncomms/

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