Thiourea-Assisted Atomic Dispersion of Co on MoS<sub>2</sub> for Promoting CO<sub>2</sub> Hydrogenation to Methanol
Zongyu Ma, Zhen Zhang, Yinye Chen, Jian Su, Jiachang Zuo, Mengqing Yang, Xiuyun Wang, Qingrong Qian, Qinghua Chen, Yongjin Luo
Abstract
In-plane sulfur vacancies in the MoS 2 catalyst exhibit great potential for low-temperature CO 2 hydrogenation to methanol. However, both CO 2 and H 2 adsorb and activate at sulfur vacancies, leading to competition between them. Anchoring atomically dispersed Co atoms over MoS 2 may facilitate H 2 adsorption and activation. Here, a thiourea-assisted strategy was employed to construct a Co–thiourea complex, which transformed into atomically dispersed Co species after heat treatment. Under reaction conditions of 5 MPa and 220 °C, the 0.5Co/MoS 2 catalyst achieved a methanol space-time yield of 323 mg MeOH g cat –1 h –1 after induction, with stability maintained for at least 500 h, compared to 177 mg MeOH g cat –1 h –1 for pristine MoS 2 . Mechanistic study revealed that the hydrogenation of CO 2 to methanol follows the COOH* pathway, where CO 2 is first hydrogenated to COOH* intermediate and then gradually hydrogenated CH 3 O* species. This work presents a viable strategy for developing atomically dispersed metal-MoS 2 catalysts for CO 2 hydrogenation to methanol.