还原方法对Pd/有机硅杂化膜的结构及性能影响  

Effects of reduction methods on the structure and performance of Pd/organosilica hybrid membranes

作　　者：吴梓豪 任秀秀 姚政 徐荣[1] 郭猛[1] 钟璟[1] 沈敏 WU Zihao;REN Xiuxiu;YAO Zheng;XU Rong;GUO Meng;ZHONG Jing;SHEN Min(CNPC-CZU Innovation Alliance,Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology,School of Petrochemical Engineering,Changzhou University,Changzhou 213164,China;Jiangsu Maymuse Environmental Protection Technology Co.Ltd.,Changzhou 213164,China)

机构地区：[1]常州大学石油化工学院,中国石油-常州大学创新联合体,江苏省绿色催化材料与技术重点实验室,江苏常州213164 [2]江苏美淼环保科技有限公司,江苏常州213164

出　　处：《高校化学工程学报》2024年第6期916-923,共8页Journal of Chemical Engineering of Chinese Universities

基　　金：国家重点研发计划(2022YFB3805003);常州市科技计划(CZ20220033,CE20225007);江苏省研究生科研与实践创新计划(YPC23020217)。

摘　　要：为了提高有机硅膜对氢气的渗透选择性,将氯化钯(PdCl_(2))加入1,6-双(三乙氧基硅基)己烷(BTESH)形成的有机硅溶胶中,采用溶胶-凝胶法制备成膜,然后对Pd^(2+)进行还原,研究了乙醇、乙二醇和H_(2)/N_(2)氛围3种方法对Pd还原程度的影响,并将形成的Pd/BTESH膜用于氢气分离。结果表明:乙醇没有还原性,H_(2)/N_(2)氛围比乙二醇表现出更强的Pd还原能力,在氢气分离中展示出最好的分离性能,H_(2)/N_(2)选择性达到11.4。在H_(2)/N_(2)还原下,随着Pd掺杂量的增加,膜的H2渗透率先降低后升高,选择性则相反。经过Pd掺杂量的优化,在200℃下Pd/BTESH-0.2膜比BTESH有机硅膜的H_(2)/N_(2)选择性提高了72%,且表现出良好的水热稳定性。To improve hydrogen permeation selectivity of organosilica membranes,palladium chloride(PdCl_(2))was incorporated into 1,6-bis(triethoxysilicyl)hexane(BTESH)derived sols to prepare membranes via a sol-gel method.Pd^(2+)was then reduced and the effects of ethanol,ethylene glycol and H_(2)/N_(2) atmosphere on the reduction degree of Pd were studied.The obtained Pd/BTESH hybrid membranes were tested for hydrogen separation.The results show that ethanol has no reducing capacity,and H_(2)/N_(2) atmosphere displays a stronger reducing ability with a better hydrogen separation selectivity than that of ethylene glycol reduction,and the corresponding membrane shows H_(2)/N_(2) selectivity of 14.As the Pd contents increase in BTESH under H_(2)/N_(2) reduction,the H_(2) permeance decreases first and then increases,while selectivity is inverse.After optimization of Pd contents,the Pd/BTESH-0.2 membrane shows a H_(2)/N_(2) selectivity 72%higher than that of BTESH organosilica membranes at 200℃.In addition,the Pd/BTESH membrane has a good hydrothermal stability.

关 键 词：有机硅 还原方法 PD 膜 氢气分离 

分 类 号：TQ031.6[化学工程]