MoS2 monolayer catalyst doped with isolated Co atoms for the hydrodeoxygenation reaction

加氢脱氧 化学 催化作用 单层 加氢脱硫 硫黄 甲苯 除氧 密度泛函理论 碳氢化合物 共价键 选择性 光化学 无机化学 有机化学 计算化学 生物化学
作者
Guoliang Liu,Alex W. Robertson,Molly Meng‐Jung Li,Winson C. H. Kuo,Matthew T. Darby,Mohamad H. Muhieddine,Yung‐Chang Lin,Kazu Suenaga,Michail Stamatakis,Jamie H. Warner,Shik Chi Edman Tsang
出处
期刊:Nature Chemistry [Springer Nature]
卷期号:9 (8): 810-816 被引量:765
标识
DOI:10.1038/nchem.2740
摘要

The conversion of oxygen-rich biomass into hydrocarbon fuels requires efficient hydrodeoxygenation catalysts during the upgrading process. However, traditionally prepared CoMoS2 catalysts, although efficient for hydrodesulfurization, are not appropriate due to their poor activity, sulfur loss and rapid deactivation at elevated temperature. Here, we report the synthesis of MoS2 monolayer sheets decorated with isolated Co atoms that bond covalently to sulfur vacancies on the basal planes that, when compared with conventionally prepared samples, exhibit superior activity, selectivity and stability for the hydrodeoxygenation of 4-methylphenol to toluene. This higher activity allows the reaction temperature to be reduced from the typically used 300 °C to 180 °C and thus allows the catalysis to proceed without sulfur loss and deactivation. Experimental analysis and density functional theory calculations reveal a large number of sites at the interface between the Co and Mo atoms on the MoS2 basal surface and we ascribe the higher activity to the presence of sulfur vacancies that are created local to the observed Co–S–Mo interfacial sites. Converting oxygen-rich biomass into fuels requires the removal of oxygen groups through hydrodeoxygenation. MoS2 monolayer sheets decorated with isolated Co atoms bound to sulfur vacancies in the basal plane have now been synthesized that exhibit superior catalytic activity, selectivity and stability for the hydrodeoxygenation of 4-methylphenol to toluene when compared to conventionally prepared materials.
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