文献类型：期刊文献

中文题名：碳二加氢失活Pd-Ag催化剂的表征

英文题名：The characterization of the deactivated C_2 hydrogenation Pd-Ag/Al_2O_3 catalyst

作者：张健[1];黄邦印[1];隋志军[1];周兴贵[1];袁渭康[1]

机构：[1]华东理工大学化学工程联合国家重点实验室,上海200237

年份：2017

卷号：46

期号：7

起止页码：839

中文期刊名：石油化工

外文期刊名：Petrochemical Technology

收录：CSTPCD;;Scopus;北大核心:【北大核心2014】；CSCD:【CSCD2017_2018】；

基金：国家自然科学基金项目(21376076)

语种：中文

中文关键词：碳二加氢;Pd—Ag催化剂;绿油;失活

外文关键词：C2 hydrogenation ; Pd-Ag catalyst ; green oil ; deactivation

摘要：以实验室部分失活和工厂永久失活的碳二加氢Pd-Ag催化剂为试样,采用GC-MS、N_2吸附-脱附、TEM、TG、ICP、CO化学吸附等手段对催化剂试样失活前后的结构和组成进行表征,并利用固定床等温反应器对催化剂催化乙炔选择性加氢的性能进行评价。实验结果表明,催化剂在反应中会发生由于绿油生成导致的暂时性失活现象,反应初期失活速率较快,10 h后反应失活速率减慢;快速失活阶段生成的绿油碳链长度短、烯烃含量高,易积累于催化剂的微小孔道中;慢速失活阶段绿油碳链长度和累积量逐渐增加,堵塞催化剂的孔道,并增加扩散阻力,使得催化剂暂时性失活。永久失活催化剂中有明显的Pd颗粒烧结和Ag流失,这可能是催化剂永久性失活的主要原因。
Selective of acetylene hydrogenation over a commercial Pd-Ag/Al2O3 catalyst was carried out on an isothermal fixed bed reactor. Both partially and permanently deactivated C2 hydrogenation catalysts were collected and characterized by the GC-MS,N2adsorption-desorption,TEM,TG,ICP and CO chemisorptions. The temporal deactivation of the catalysts was caused by the formation of green oil and could be divided into quickly and slowly stages. In the initial reaction stage,the deactivation rate was quick,and then decreased after 10 h reaction. In the quick deactivation stage,the green oil has shorter carbon chains and higher alkenes ratio,and preferentially resides in pore with smaller size due to the capillary condensation. During the slowly deactivation stage,with the increase of molar weight and productivity of green oil,it could gradually block the pore of the catalyst,which increases the diffusion resistance and causes the partially deactivation. The sintering of Pd and loss of Ag are observed on the permanently deactivation catalysts;this may be the reason of catalyst permanent deactivation.