水热合成rGO负载的MoS_(2)催化剂及其催化蒽加氢性能  

Highly active MoS_(2)/reduced graphene oxide catalyst for anthracene hydrogenation

作　　者：郑安达 杨成功 王冬娥[1] 田志坚[1] ZHENG Anda;YANG Chenggong;WANG Dong’e;TIAN Zhijian(Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院大连化学物理研究所,辽宁大连116023 [2]中国科学院大学,北京100049

出　　处：《化工进展》2022年第1期244-252,共9页Chemical Industry and Engineering Progress

基　　金：新疆维吾尔自治区重点研发计划(2017B02007-1,2017B02007-2)。

摘　　要：采用水热法制备了一系列还原氧化石墨烯(rGO)负载的MoS_(2)催化剂(MoS_(2)/rGO)。通过SEM、XRD、EDX、拉曼光谱、HRTEM等手段表征了不同钼源制备的MoS_(2)/rGO催化剂中MoS_(2)的堆积层数、片层尺寸、分散性等纳米结构。表征结果显示水热法可以成功地将MoS_(2)高分散、均匀地负载在rGO表面,且可以通过调控钼源种类调变MoS_(2)/rGO催化剂中MoS_(2)催化加氢活性位。采用蒽作为重质油模型化合物评价了MoS_(2)/rGO催化剂的催化加氢性能,结果表明以四硫代钼酸铵为钼源水热法制备的MoS_(2)/rGO-ATTM催化剂蒽加氢率和八氢蒽选择性分别是浸渍法制备IM-MoS_(2)/rGO催化剂的2.0倍和4.2倍。MoS_(2)/rGO催化剂的催化加氢活性与比表面积无关,主要取决于其上MoS_(2)纳米片的堆积层数和片层长度。MoS_(2)/rGO-ATTM催化剂的高催化加氢活性可以归结于其上MoS_(2)纳米片的高催化加氢活性位暴露量、催化剂的高分散性和高悬浮性。MoS_(2) catalysts supported on reduced graphene oxide(MoS_(2)/rGO)were synthesized through hydrothermal process.The nanostructure parameters including stacking layers,slab length,and dispersion were characterized by scanning electron microscopy with energy dispersive X-ray spectroscopy,X-ray diffraction,Raman spectroscopy and high-resolution transmission electron microscopy.The results indicated that the hydrothermal synthesis method could successfully load MoS_(2) over the surface of rGO support,and adjust the catalytic active sites of MoS_(2) by tuning the Mo precursors.Polycyclic aromatic hydrocarbon anthracene was used as the model compound of heavy oils to evaluate the catalytic hydrogenation performance of the MoS_(2)/rGO catalysts.The MoS_(2)/rGO-ATTM catalyst,synthesized with ammonium tetrathiomolybdate as Mo precursor by the hydrothermal method,demonstrated an extremely high anthracene hydrogenation conversion of 55.1% and a high selectivity to octahydroanthracene of 86.6%,which were respectively 2.0 times and 4.2 times as high as those of the IM-MoS_(2)/rGO catalyst synthesized by impregnation method.The catalytic hydrogenation activities of MoS_(2)/rGO catalysts were not related to their surface area,but depended on their stacking layers and slab lengths.The excellent catalytic activity of the MoS_(2)/rGO-ATTM catalyst may be ascribed to the high exposure of hydrogenation active sites,the enhanced dispersion of MoS_(2) nanosheets in the catalyst,and the good suspension of the catalyst in the reaction mixture.

关 键 词：二硫化钼 还原氧化石墨烯 水热 催化剂 催化加氢 

分 类 号：TE624[石油与天然气工程—油气加工工程]