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作 者:王保伟[1] 王婷婷 赵俊 李振花[1] 徐艳[1] 马新宾[1] WANG Bao-wei;WANG Ting-ting;ZHAO Jun;LI Zhen-hua;XU Yan;MA Xin-bin(Key Laboratory for Green Chemical Technology of the Ministry of Education,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China)
机构地区:[1]天津大学化工学院绿色合成与转化教育部重点实验室,天津300072
出 处:《燃料化学学报》2021年第7期952-959,共8页Journal of Fuel Chemistry and Technology
基 金:The project was supported by the National High Technology Research and Development Program of China(863 Project,2015AA050504).
摘 要:采用氢气程序升温还原方法制备了系列金属磷化物催化剂,研究了磷前驱体和H_(2)/CO比对其甲烷化催化性能的影响。结果表明,与磷酸氢二铵相比,由植酸制备的金属磷化物催化剂具有较高的甲烷化活性;植酸作为螯合剂可以有效地分散金属前驱体,降低还原温度,使催化剂具有较高的比表面积和较小的晶粒尺寸,并更好地还原为纯磷化物晶相。不同金属磷化物催化剂的活性顺序为MoP>WP>CoP>NiP。高H_(2)/CO比有利于甲烷化反应进行,随着反应物H_(2)/CO比的增加,所有磷化物催化剂的甲烷选择性都增加。A series of metal phosphides including MoP,WP,CoP and NiP was prepared by temperature-programmed reduction with hydrogen from different phosphorus precursors.The effect of phosphorus precursor and feed H_(2)/CO ratio on the catalytic performance of metal phosphides in the methanation was investigated.In comparison with diammonium hydrogen phosphate(DAP),phytic acid(PA)as a chelating agent can effectively disperse the metal precursor,reduce the reduction temperature,promote to form pure phosphide phase,and give the phosphide catalyst a higher surface area and a smaller particle size;as a result,the metal phosphides prepared with PA as a phosphorus precursor exhibit higher catalytic activity in methanation.In addition,the catalytic activity of various metal phosphides in methanation follows the sequence of MoP>WP>CoP>NiP.A high H_(2)/CO ratio in the feed is favorable for the methanation over the phosphide catalysts;the selectivity to methane increases with an increase in the H_(2)/CO ratio.
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