Key Lab of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China.
Department of Applied Chemistry, School of Chemistry and Molecular Engineering, Nanjing Tech University, Nanjing, China.
Nat Commun. 2023 Jan 31;14(1):513. doi: 10.1038/s41467-023-36259-9.
The hydrogenation of CO or CO to single organic product has received widespread attentions. Here we show a highly efficient and selective catalyst, MoS@ions-ZSM-5, with molybdenum sulfide clusters ([MoS]) confined in zeolitic cages of ZSM-5 molecular sieve for the reactions. Using continuous fixed bed reactor, for CO hydrogenation to methanol, the catalyst MoS@NaZSM-5 shows methanol selectivity larger than 98% at 10.2% of carbon dioxide conversion at 180 °C and maintains the catalytic performance without any degeneration during continuous reaction of 1000 h. For CO hydrogenation, the catalyst MoS@HZSM-5 exhibits a selectivity to C and C hydrocarbons stably larger than 98% in organics at 260 °C. The structure of the catalysts and the mechanism of CO hydrogenation over the catalysts are fully characterized experimentally and theorectically. Based on the results, we envision that the MoS@ions-ZSM-5 catalysts display the importance of active clusters surrounded by permeable materials as mesocatalysts for discovery of new reactions.
CO 或 CO 加氢转化为单一有机产物受到广泛关注。在此，我们展示了一种高效、选择性的催化剂 MoS@ions-ZSM-5，其中钼硫化物簇([MoS])限域在 ZSM-5 分子筛的沸石笼中。使用连续固定床反应器，在 CO 加氢制甲醇反应中，催化剂 MoS@NaZSM-5 在 180°C、二氧化碳转化率为 10.2%时甲醇选择性大于 98%，在 1000 小时的连续反应过程中保持催化性能无任何退化。对于 CO 加氢反应，催化剂 MoS@HZSM-5 在 260°C 时在有机相中稳定地表现出对 C 和 C 烃类的选择性大于 98%。通过实验和理论全面表征了催化剂的结构和 CO 加氢反应的机理。基于这些结果，我们设想 MoS@ions-ZSM-5 催化剂作为介孔催化剂，其活性簇被可渗透材料包围，对于发现新反应具有重要意义。
