Sodium-assisted MoS2 for boosting CO2 hydrogenation to methanol: The crucial role of sodium in defect evolution and modification

化学 Boosting(机器学习) 甲醇 催化作用 有机化学 计算机科学 机器学习
作者
Zhen Zhang,Jiachang Zuo,Luteng Luo,Xuhui Yang,Zongyu Ma,Hongjun Jin,Youzhu Yuan,Qingrong Qian,Qinghua Chen,Yongjin Luo
出处
期刊:Journal of Catalysis [Elsevier BV]
卷期号:436: 115621-115621
标识
DOI:10.1016/j.jcat.2024.115621
摘要

The effective conversion of CO2 to methanol utilizing green hydrogen under moderate conditions represents a promising approach for achieving carbon neutrality. MoS2 demonstrates exceptional catalytic performance at temperatures below 200 °C, however, generating in-plane sulfur defects is challenging due to the intact planar structure. Introducing heteroatoms to induce sulfur vacancy formation and modulate their chemical environment remains a significant obstacle. In this study, we developed a NaCl-assisted method for synthesizing MoS2 and discovered that a small quantity of sodium not only promotes the formation of sulfur vacancies during the induction period, but also encourages CO2 hydrogenation via the carboxylate route, as opposed to the CO2 dissociation to CO* route over non-modified sulfur vacancies. Furthermore, catalysts at various stages throughout the 60 h induction period were characterized, revealing that the increase in sulfur vacancies and enhanced H2 dissociation capability are primary factors contributing to improved methanol yield. The sodium-modified MoS2 achieves a methanol space–time yield of up to 571 mgMeOH gcat−1h−1 at 200 °C and 5 MPa with a 4.8 % CO2 conversion and 96 % methanol selectivity. The turnover frequency based on total sulfur vacancies reaches 170 h−1. This research is anticipated to offer a new strategy for enhancing the catalytic performance of CO2 hydrogenation to methanol using heteroatom-assisted defect engineering.
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