新型非常规天然气直接催化转化制芳烃催化剂的研究  

Study on novel catalysts for direct catalytic conversion of unconventional natural gas to aromatics

作　　者：刘志开 曹辉 王天云[1] 韩国栋 刘意[1] 张燚[1] Liu Zhikai;Cao Hui;Wang Tianyun;Han Guodong;Liu Yi;Zhang Yi(State Key Laboratory of Organic-Inorganic Composites,Beijing University of Chemical Technology,Beijing 100029,China;CNOOC Refining and Chemical Research Institute(Beijing)Co.,Ltd.)

机构地区：[1]北京化工大学有机无机复合材料国家重点实验室,北京100029 [2]中海油炼油化工科学研究院(北京)有限公司

出　　处：《无机盐工业》2019年第12期83-88,共6页Inorganic Chemicals Industry

基　　金：中海油炼油化工科学研究院(北京)有限公司外委项目(项目号：LHYJY/KJ/SA2017-0017)

摘　　要：近年来,常规天然气供应紧张,因此非常规天然气的开发利用显得尤为重要。甲烷无氧芳构化作为非常规天然气的直接转化方式之一,由于其工艺流程简单、芳烃选择性集中、产物附加值高等特点,一直受到广大科研工作者的关注。为提高甲烷转化率及甲苯和二甲苯等产物的选择性,通过一步浸渍法制备了0.189%Mg/8%Mo/HZSM-5(以质量分数计)催化剂,在700℃、101 kPa条件下通过将甲烷无氧芳构化反应与芳烃烷基化反应耦合,其中甲醇作为烷基化试剂与甲烷以共进料的方式进入反应体系,将甲烷的转化率提升至27.45%、甲苯和二甲苯的选择性分别达到28.29%和24.65%,并且8 h内催化剂未出现活性减弱,实现了反应的高效稳定运行。Recently,it is important to develop unconventional natural gas,because the supply of conventional natural gas is tight.Methane dehydroaromatization(MDA)is one of the direct conversion pathways of unconventional natural gas.Due to its simple process,high selectivity of aromatics and high value-added products,it has been the focus of researchers.In order to improve methane conversion rate and the selectivity of products such as toluene and xylene,0.189% Mg/8% Mo/HZSM-5(mass fraction)catalyst prepared by one-step impregnation method,and the MDA reaction and aromatic alkylation reaction were coupled at 700℃ under 101 kPa.Methanol as an alkylating agent and methane were introduced into the reaction system by co-feeding to increase the methane conversion rate to 27.45%,and the selectivity of toluene and xylene reached 28.29% and 24.65%,respectively.The activity of the catalyst was not weakened within 8 h,which achieves efficient and stable operation of MDA.

关 键 词：甲烷无氧脱氢芳构化反应 Mg/Mo/HZSM-5催化剂 耦合 甲醇 

分 类 号：TQ136.12[化学工程—无机化工]