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 () and Dehui Deng ()
Additional contact information
Jingting Hu: Chinese Academy of Sciences
Zeyu Wei: Chinese Academy of Sciences
Yunlong Zhang: 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
Yanan Li: Chinese Academy of Sciences
Jun Mao: Chinese Academy of Sciences
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
Ye Wang: Xiamen University
Dehui Deng: Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-42325-z

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