一步水热合成MoS_(2)/C催化剂及其催化浆态床菲加氢反应性能  

One-step hydrothermal synthesis of MoS_(2)/C catalysts for the slurry-phase hydrogenation of phenanthrene

作　　者：黄蓉 杨成功 王冬娥[1] 田志坚[1] Huang Rong;Yang Chenggong;Wang Donge;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：《工业催化》2023年第9期25-33,共9页Industrial Catalysis

基　　金：国家自然科学基金面上基金项目(22272168);中国科学院大连化学物理研究所创新基金青年基金项目(DICP I202235)。

摘　　要：随着原油储量的急剧下降,急需将重质原料转化为轻质油品以缓解原油的供应压力。浆态床加氢是一种可以将重质原料高效转化的先进技术,其核心难题在于开发高活性的加氢催化剂。采用葡萄糖和麦芽糖为碳源一步水热法合成MoS_(2)/C纳米催化剂,并采用XRD、Raman、元素分析、SEM和HRTEM等方法表征催化剂的组成和结构。表征结果表明,MoS_(2)/C催化剂由MoS_(2)-C-MoS_(2)碳插层结构的纳米片组成,纳米片具有层间距大、侧边尺寸小且堆积层数少的结构特点。以菲为重油模型化合物评价MoS_(2)/C催化剂的加氢性能。结果表明,以葡萄糖为碳源且原料C/Mo原子比为5时制备的MoS_(2)/C-G-5催化剂具有优异的催化加氢活性。该催化剂的菲加氢转化率高达85.6%,加氢率37.4%,深度加氢产物八氢菲选择性56.4%,分别是不加碳源制备的MoS_(2)催化剂的1.6、2.4和2.3倍。MoS_(2)/C催化剂的MoS_(2)-C-MoS_(2)碳插层纳米结构可充分暴露MoS_(2)的加氢活性位,显著提高催化剂的催化加氢活性。As the crude oil reserves decreased dramatically,it’s urgent to upgrade heavy feedstocks into light oils to relieve the supply pressure of crude oil.The slurry-phase hydrogenation is an advanced technology to efficiently upgrade heavy feedstocks.The challenge of slurry-phase hydrogenation lies in developing high active hydrogenation catalysts.In this work,MoS_(2)/C catalysts were synthesized by a facile one-step hydrothermal method with glucose and maltose as the soluble carbon sources.The compositions and structures of MoS_(2)/C catalysts were characterized by X-ray diffraction,Raman spectroscopy,elemental analysis,scanning electron microscopy and high-resolution transmission electron microscopy.The characterization results indicated that the MoS_(2)/C catalysts are composed of nanosheets with MoS_(2)-C-MoS_(2)carbon intercalated structure.The nanosheets display enlarged interlayer distance,short slabs and few stacking layers.The catalytic hydrogenation activities of MoS_(2)/C catalysts were evaluated with phenanthrene as the model compound of heavy oils in the slurry-bed reactor.MoS_(2)/C catalyst with glucose as carbon precursor and the C to Mo atomic ratio of 5 in the raw materials exhibits the highest catalytic hydrogenation activity.For MoS_(2)/C-G-5 catalyst,the phenanthrene conversion,hydrogenation percent of phenanthrene and the selectivity to the deep hydrogenation product octahydrophenanthrene can respectively reach 85.6%,37.4%and 56.4%,which are 1.6,2.4 and 2.3 times as high as those of MoS_(2)catalyst synthesized without carbon source.The MoS_(2)-C-MoS_(2)carbon intercalated nanostructures of MoS_(2)/C catalyst could expose more hydrogenation active sites to improve its hydrogenation activity significantly.

关 键 词：催化化学 MoS_(2)/C催化剂 碳插层结构 一步水热法 菲加氢 浆态床 

分 类 号：TQ426.95[化学工程] TQ643.36