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Layer-structure adjustable MoS_(2) catalysts for the slurry-phase hydrogenation of polycyclic aromatic hydrocarbons

查看全文 作　　者：Donge [1]Wang;Jiahe [1]Li;Huaijun [1]Ma;Chenggong [1,2]Yang;Zhendong [1]Pan;Wei [1]Qu;Zhijian [1,3]Tian 高影响力作者 机构地区：[1]Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China;[2]University of Chinese Academy of Sciences,Beijing 100049,China;[3]State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China高影响力机构 出　　处：《Journal of Energy Chemistry》索引2021年第30卷第12期,共12页高影响力期刊 基　　金：financially supported by the Autonomous Region Key R&D Program of Xin Jiang (2017B02007-1, 2017B02007-2);the High Level Talent Innovation and Entrepreneurship Project of Dalian (2019CT04)。 摘　　要：Slurry-phase hydrogenation technology is the frontier topic in the efficient conversion of heavy oils into light fractions around the world.Developing highly active dispersed MoS_(2) catalysts is the major obstacle to realize the industrial application of upgrading heavy oils.In this work,both top-down ball-milling method and bottom-up hydrothermal method were designed to synthesize MoS_(2) catalysts with controllable layer structures.The stacking layers and lateral sizes for micro-scaled MoS_(2) catalysts by ball-milling method can be reduced to their limits and stabilize at 6~8 layers and lateral size of ca.30 nm.The more flexible bottom-up hydrothermal method can construct MoS_(2) catalysts with much smaller lateral sizes and fewer stacking layers,especially,MoS_(2) catalyst fabricated with ammonium tetrathiomolybdate as Mo and S precursor possesses average stacking layers of 2 and lateral size of 5 ~ 10 nm.Polycyclic aromatic hydrocarbons anthracene,phenanthrene and naphthalene were used as model compounds of heavy oils to investigate the catalytic hydrogenation performance of designed MoS_(2) catalysts.The catalytic activities of MoS_(2) catalysts can be well correlated with their stacking layers and lateral size.The edges of top and bottom S-Mo-S atomic layers for MoS_(2) sheets,named rim sites,are positively correlated with the exposure of active sites for catalytic hydrogenation of PAHs.The highest catalytic activity of MoS_(2) catalyst results from its layer structures of 100% rim sites and the smallest lateral size of5 ~ 10 nm,which is beneficial to expose maximum active sites for catalytic hydrogenation reactions.This work can guide us to design the highly active hydrogenation catalysts,and promote the industrial application of upgrading heavy oils. 关 键 词：MoS_(2) Active sites Catalytic hydrogenation Slurry-phase Polycyclic aromatic hydrocarbons
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