芳烃类氢载体催化转化制氢的研究  

Catalytic Conversion of Aromatic Hydrocarbon-based Hydrogen Carriers to Produce Hydrogen

作　　者：陈文轩 李学琴 刘鹏[1] 雷廷宙 李艳玲 吴幼青[2] CHEN Wenxuan;LI Xueqin;LIU Peng;LEI Tingzhou;LI Yanling;WU Youqing(School of Petrochemical Engineering,Changzhou University,Changzhou 213164,China;School of Resources and Environmental Engineering,East China University of Science and Technology,Shanghai 200237,China)

机构地区：[1]常州大学石油化工学院,江苏常州213164 [2]华东理工大学资源与环境工程学院,上海200237

出　　处：《林产化学与工业》2023年第2期63-72,共10页Chemistry and Industry of Forest Products

基　　金：国家自然科学基金资助项目(51906021);江苏省研究生科研与实践创新计划项目(SJCX22_1337)。

摘　　要：以分子筛为载体,采用不同辅助方法浸渍法制备镍基负载型分子筛催化剂,并在固定床反应器中研究了镍基分子筛催化剂对生物质焦油芳烃类氢载体——甲苯的催化热解制氢性能,考察了不同分子筛、辅助方法及工艺条件的影响,对催化剂的使用寿命进行了研究;并采用XRD、SEM、BET等方法对催化剂进行表征分析。研究结果表明:以HZSM-5(硅铝比25)分子筛为载体,采用超声波辅助浸渍法,且当超声波处理时间为20 min,超声波功率为80 W,Ni负载量(以分子筛质量计)为8%时制备出的Ni/HZSM-5分子筛催化剂的催化活性最强,在700℃下催化甲苯40 min的氢气产率可以达到76.6 mL/g,甲烷产率为27.6 mL/g,总气体产率为108.9 mL/g,甲苯转化率为76.8%,积炭量为238.2 mg/g,催化剂比表面积为241.8 m^(2)/g,总孔容为0.19 cm^(3)/g,平均孔径为3.16 nm;Ni的负载不会对HZSM-5的晶体结构造成明显影响,但Ni组分的加入起到了很好的催化效果,Ni/HZSM-5催化剂稳定性得到了提升,使用寿命得到了延长,对甲苯的催化制氢性能优于四氢萘、苯酚和乙酸。Nickel-based supported molecular sieve catalysts were prepared by excessive impregnation with different auxiliary methods using molecular sieve as the carrier.The catalytic pyrolysis performance of the nickel-based molecular sieve catalysts on the hydrogen carrier of biomass tar aromatic hydrocarbon-toluene to produce hydrogen was studied in a fixed-bed reactor.The effects of different molecular sieves,auxiliary methods and process conditions were investigated,and the service life of the catalyst was studied.The catalysts were characterized by XRD,SEM and BET.The results showed that the Ni/HZSM-5 molecular sieve catalyst using HZSM-5(the ratio of silicon to aluminum was 25)zeolite as the carrier had the highest catalytic activity,through the ultrasonic-assisted impregnation method,and the ultrasonic time was 20 min,the ultrasonic power was 80 W,and the Ni loading was 8%.At 700℃and 40 min,the yields of H 2 and CH 4 were 76.6 mL/g and 27.6 mL/g,respectirely,and the total gas yield reached 108.9 mL/g.The toluene conversion rate was 76.8%,and the carbon deposition was 238.2 mg/g.The specific surface area,the total pore volume and the average pore size of the catalyst were 241.8 m^(2)/g,0.19 cm^(3)/g and 3.16 nm,respectively.The Ni loading did not affect the crystal structure of HZSM-5 obviously,while it exhibited an excellent catalytic activity.The stability of Ni/HZSM-5 catalyst was improved,and the service life was also extended.The catalytic hydrogen production performance of toluene was better than that of tetralin,phenol and acetic acid.

关 键 词：镍基催化剂 催化热解 芳烃 制氢 

分 类 号：TQ35[化学工程] TK6[动力工程及工程热物理—生物能]