活性半焦负载γ-MoN_xC_y的制备及其在甲烷化反应中的应用  

Preparation of Activated Semi-coke Supported γ-MoN_xC_y and Its Catalytic Performance for Methanation Effects

作　　者：张戎 范寒寒 王娟[1] 霍晓东 房倚天[4] ZHANG Rong;FAN Hanhan;WANG Juan;HUO Xiaodong;FANG Yitian(CNPC Research Institute o f Sa fety Environment Technology,B eijing,1Q22Q6,China;China University o f Geosciences B eijing j Beijing 100083,China;The Sci-Tech Academy of Shanxi Coal Imp.Exp.Group Co.Ltd.,Taiyuan 03001,China;Institute o f Coal Chemistry,Chinese Academy o f Sciences,Taiyuan 030001,China)

机构地区：[1]中国石油安全环保技术研究院,北京102206 [2]中国地质大学北京,北京100083 [3]山西煤炭进出口集团科学技术研究院有限公司,太原030006 [4]中国科学院山西煤炭化学研究所,太原030001

出　　处：《太原理工大学学报》2018年第2期196-203,共8页Journal of Taiyuan University of Technology

基　　金：中国科学院战略性先导科技专项0501课题资助项目(XDA07050100)

摘　　要：将六次甲基四胺(HMT)和钼酸铵(AHM)反应生成的络合物与霍林河(HLH)脱灰煤以不同方式混合后热解制备活性半焦负载的钼基碳化物催化剂,考察制备方式对催化剂甲烷化反应性能的影响。结果表明:制备方式对催化剂的晶相结构、形貌以及催化活性有很大影响。络合物沉积到煤表面制备的催化剂其活性及选择性最好,其次是络合物与煤机械混合后热解制备的催化剂,活性最差的是β-Mo_2C直接与半焦机械混合制备的催化剂。但无论哪种制备方式,活性半焦负载的钼基碳化物的催化活性都要高于非负载β-Mo_2C催化剂,这是由于活性半焦提高了金属活性组分Mo的分散度,且半焦与Mo的相互作用生成了催化活性较高的物相γ-MoN_xC_y.Activated semi-coke supported molybdenum carbides were prepared by pyrolyzing the mixture of HLH de-ashed lignite and the complex of hexamethylentetramine(HMT)and ammonium molybdate(AHM)with different preparation methods.The effects of preparation method on methanation were evaluated.The results show that preparation method heavily influenced the crystal structure,morphology and catalytic activity of the catalysts,the conversion of CO(XCO)and the selectivity of CH_4(SCH_4)were the best on the catalyst prepared by the depositionprecipitation method,the next was the catalyst prepared by mechanically mixing HLH de-ashed lignite with the complex of HMT and AHM and then thermally decomposing,while the catalytic activity of the catalyst prepared by mechanically mixing the semi-coke of HLH de-ashed lignite withβ-Mo_2C was the worst.The catalytic activity of all activated semi-coke supported molybdenum carbides are better than that of bulkβ-Mo_2C.This may be due to the dual action of the improved dispersion of Mo and the improved catalytic activity on account of the formation ofγ-MoNxCydue to the interaction between active metal component and the catalyst support.

关 键 词：碳化钼 活性半焦 制备方式 甲烷化 

分 类 号：O643.32[理学—物理化学]