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- Title
Edge-rich molybdenum disulfide tailors carbon-chain growth for selective hydrogenation of carbon monoxide to higher alcohols.
- Authors
Hu, Jingting; Wei, Zeyu; Zhang, Yunlong; Huang, Rui; Zhang, Mingchao; Cheng, Kang; Zhang, Qinghong; Qi, Yutai; Li, Yanan; Mao, Jun; Zhu, Junfa; Wu, Lihui; Wen, Wu; Yu, Shengsheng; Pan, Yang; Yang, Jiuzhong; Wei, Xiangjun; Jiang, Luozhen; Si, Rui; Yu, Liang
- 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. Controllable synthesis of higher alcohols from CO hydrogenation remains a great challenge. Here the authors show that potassium-decorated edge-rich MoS2 enables selective CO hydrogenation to higher alcohols by regulating the reaction kinetics of C-O cleavage, C-C coupling and desorption of alcohols.
- Subjects
CARBON monoxide; MOLYBDENUM disulfide; COUPLING reactions (Chemistry); HYDROGENATION; ALCOHOL
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-42325-z