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, Liang Wu, Wu Wen, Shengsheng Yu, Yang Pan, Jiuzhong Yang, Xiangjun Wei, Luozhen Jiang, Rui Si, Liang Yu, Ye Wang, Dehui Deng
Abstract
Abstract Selective hydrogenation of carbon monoxide (CO) to higher alcohols (C 2+ 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 C 2-4 OH is achieved over a potassium-modified edge-rich molybdenum disulfide (MoS 2 ) catalyst, which delivers a high CO conversion of 17% with a superior C 2-4 OH 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, C 2-4 OH to methanol selectivity ratio can be overturned from 0.4 to 2.2. Mechanistic studies reveal that sulfur vacancies at MoS 2 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 C 2-4 OH.