Ni/Al_(2)O_(3)催化十二氢-N-乙基咔唑分解的粒径效应及动力学分析  

Particle size effect and kinetic analysis of Ni/Al_(2)O_(3) catalyzed decomposition of dodecahydro-N-ethylarbazole

作　　者：张春颖 黄龙[1] 石沫男 马梦楠 张晨 ZHANG Chunying;HUANG Long;SHI Monan;MA Mengnan;ZHANG Chen(Enze Bimass Fine Chemicals Beijing Key Laboratory,College of New Materials and Chemical Engineering,Beijing Institute of Petrochemical Technology,Beijing 102617,China)

机构地区：[1]北京石油化工学院新材料与化工学院恩泽生物质精细化工北京市重点实验室,北京102617

出　　处：《石油化工》2024年第9期1245-1250,共6页Petrochemical Technology

基　　金：北京市属高等学校优秀青年人才培育计划项目(BPHR202203094);北京市科学技术协会青年人才托举工程(BYESS2023256)。

摘　　要：采用浸渍法制备了不同粒径的Ni/Al_(2)O_(3)催化剂,利用XRD、H2化学吸附、N2吸附-脱附等方法对催化剂进行了表征,考察了Ni粒径和反应条件对十二氢-N-乙基咔唑(12H-NEC)脱烷基及脱氢反应性能的影响。实验结果表明,随Ni负载量的增加,Ni平均粒径逐渐增大,Ni/Al_(2)O_(3)催化剂对12H-NEC的脱氢及脱烷基活性均呈先增大后下降趋势。Ni/Al_(2)O_(3)催化剂的Ni粒径在10~70 nm范围内,Ni粒径越小越有利于12H-NEC稳定性,适宜的脱氢温度为220℃。在10Ni/Al_(2)O_(3)催化剂作用下,12H-NEC脱烷基反应为一级动力学控制,指数前因子和表观活化能分别为1.27×10^(6) h^(-1)和79.30 kJ/mol。The impregnation method was used to prepare Ni/Al_(2)O_(3) catalysts of different particle sizes,and the catalysts were characterized by XRD,H2-chemisorption,and N2 adsorbtiondesorbtion,while the effect of nickel particle size and reaction conditions on dealkylation and dehydrogenation reaction performance of dodecahydro-N-ethylcarbazole(12H-NEC)was systematically investigated.The results show that for Ni/Al_(2)O_(3) catalysts,with the increase of Ni loading,the Ni average particle size gradually increases,dehydrogenation and dealkylation activity of 12H-NEC first increases and then decreases.The stability of 12H-NEC increases significantly with decreasing Ni particle size of Ni/Al_(2)O_(3) catalysts in the range of 10-70 nm,and the suitable dehydrogenation temperature is 220℃.The 12H-NEC dealkylation reaction with 10Ni/Al_(2)O_(3) catalysts shows the first-order kinetics control,and the pre-exponential factor and apparent activation energy are 1.27×10^(6) h^(-1) and 79.30 kJ/mol,respectively.

关 键 词：N-乙基咔唑 储氢 粒径 NI催化剂 宏观动力学 

分 类 号：TQ426.8[化学工程]