以MCM-41作载体的Ni2P催化剂对喹啉的加氢脱氮性能.docVIP

以MCM-41作载体的Ni2P催化剂对喹啉的加氢脱氮性能 鲁墨弘1 王安杰1* 李翔1 任靖1 胡永康2 ( 1大连理工大学精细化工国家重点实验室，辽宁 大连 116012；2抚顺石油化工研究院，辽宁 抚顺113001) 摘要：通过原位还原方法制备了以MCM-41作载体的Ni-P催化剂并考察了其对喹啉的加氢脱氮（HDN）反应性能。结果表明，催化剂活性在Ni/P摩尔比为1和1.25时最高，并随着担载量的增加逐渐增加。Ni-P催化剂的HDN活性远高于硫化态Ni-W催化剂，可能与Ni-P催化剂加氢活性较强有关。XRD结果表明不同Ni/P摩尔比催化剂中都有Ni2P活性相。 关键词：Ni2P; 加氢脱氮；喹啉；原子比；担载量 Hydrodenitrogenation of Quinoline Catalyzed by MCM-41-Supported Nickel Phosphides LU Mohong1,WANG Anjie1*,LI Xiang1, REN Jing1, HU Yongkang2 (1State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116012, Liaoning,China； 2Fushun Research Institute of Petroleum and Petrochemicals,Fushun 113001 Liaoning,China) Abstract: MCM-41-supported nickel phosphides were prepared by an in-situ reduction method. Their hydrodenitrogen（HDN）activities were evaluated by HDN of 1 % quinoline in decalin. It is indicated that the HDN activity of Ni-P/MCM-41 increased with the increase in the loading of Ni2O and P2O5.The supported nickel phosphides with initial Ni/P ratios of 1 and 1.25 exhibited much higher HDN activity than the supported Ni-W sulfide. XRD patterns of both high-performance phosphide catalysts revealed that the active phase was Ni2P. It seems that HDN of quinoline on the MCM-41-supported nickel phosphides exclusively proceeds via the pathway which involves the fully saturated intermediates. Key words: nickel phosphide; hydrodenitrogenation; quinoline; atomic ratio; loading 联系人：王安杰,第一作者：鲁墨弘（1977-），男，博士生。 基金项目：国家自然科学基金资助项目20333030）；教育部博士点基金；辽宁省中青年学科带头人资助项目。 Corresponding author: Prof. WANG Anjie. E-mail: anjwang@chem..dlut.edu.cn Foundation item: supported by the Natural Science Foundation of China , the Education Ministry of China (20030141026) and CNPC Innovation Foundation.  引 言 加氢脱硫（HDS）（HDN）HDS反应有强烈的抑制HDN越来越受到重视，而传统的硫化态的加氢精制催化剂已难以满足要求。近年来，以Ni2P为代表的过渡金属磷化物以其优异的HDN和HDS性能以及较高的稳定性引起了人们的重视[1-4]。我们在前期工作中，用原位还原的方法制备了以MCM-41作载体的具有较高HDS活性的Ni2P催化剂[5]。本文在此基础上以原油中具有代表性的含N化合物——喹啉（Q）作为模型化合物，进一步考察其HDN性能。 1 试验部分 1.1催