化工进展 ›› 2022, Vol. 41 ›› Issue (1): 244-252.DOI: 10.16085/j.issn.1000-6613.2021-0302

• 工业催化 • 上一篇    下一篇

水热合成rGO负载的MoS2催化剂及其催化蒽加氢性能

郑安达1,2(), 杨成功1,2, 王冬娥1(), 田志坚1()   

  1. 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
  • 收稿日期:2021-02-08 修回日期:2021-03-16 出版日期:2022-01-05 发布日期:2022-01-24
  • 通讯作者: 王冬娥,田志坚
  • 作者简介:郑安达(1988—),男,博士研究生,研究方向为纳米金属催化剂。E-mail:zads@dicp.ac.cn
  • 基金资助:
    新疆维吾尔自治区重点研发计划(2017B02007-1)

Highly active MoS2/reduced graphene oxide catalyst for anthracene hydrogenation

ZHENG Anda1,2(), YANG Chenggong1,2, WANG Dong’e1(), TIAN Zhijian1()   

  1. 1.Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
    2.University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2021-02-08 Revised:2021-03-16 Online:2022-01-05 Published:2022-01-24
  • Contact: WANG Dong’e,TIAN Zhijian

摘要:

采用水热法制备了一系列还原氧化石墨烯(rGO)负载的MoS2催化剂(MoS2/rGO)。通过SEM、XRD、EDX、拉曼光谱、HRTEM等手段表征了不同钼源制备的MoS2/rGO催化剂中MoS2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MoS2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MoS2/rGO催化剂中MoS2催化加氢活性位。采用蒽作为重质油模型化合物评价了MoS2/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MoS2/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-MoS2/rGO催化剂的2.0倍和4.2倍。MoS2/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MoS2纳米片的堆积层数和片层长度。MoS2/rGO-ATTM催化剂的高催化加氢活性可以归结于其上MoS2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。

关键词: 二硫化钼, 还原氧化石墨烯, 水热, 催化剂, 催化加氢

Abstract:

MoS2 catalysts supported on reduced graphene oxide (MoS2/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 MoS2 over the surface of rGO support, and adjust the catalytic active sites of MoS2 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 MoS2/rGO catalysts. The MoS2/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-MoS2/rGO catalyst synthesized by impregnation method. The catalytic hydrogenation activities of MoS2/rGO catalysts were not related to their surface area, but depended on their stacking layers and slab lengths. The excellent catalytic activity of the MoS2/rGO-ATTM catalyst may be ascribed to the high exposure of hydrogenation active sites, the enhanced dispersion of MoS2 nanosheets in the catalyst, and the good suspension of the catalyst in the reaction mixture.

Key words: molybdenum disulfide(MoS2), reduced graphene oxide, hydrothermal, catalyst, catalytic hydrogenation

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