界面聚合法制备用于脱氮提纯CH_(4)的N_(2)优先渗透ZIF-90/聚酰胺混合基质膜  

Preparation of ZIF-90/polyamide mixed matrix membrane with N_(2)preferential permeation for CH_(4)purification based on interfacial polymerization

作　　者：于喆淼 王志[1] 生梦龙 邢广宇 王纪孝[1] YU Zhemiao;WANG Zhi;SHENG Menglong;XING Guangyu;WANG Jixiao(Chemical Engineering Research Center,School of Chemical Engineering and Technology,Tianjin University,Tianjin Key Laboratory of Membrane Science and Desalination Technology,State Key Laboratory of Chemical Engineering,Tianjin Collaborative Innovation Center of Chemical Science and Engineering,Tianjin 300350,China)

机构地区：[1]天津大学化工学院化学工程研究所,天津市膜科学与海水淡化技术重点实验室,化学工程联合国家重点实验室,天津化学化工协同创新中心,天津300350

出　　处：《化工学报》2022年第7期3273-3286,F0002,共15页CIESC Journal

基　　金：国家自然科学基金重点项目(21938007);河北省自然科学基金重点项目(E2020402036)。

摘　　要：作为一种高效的分离方法,膜法分离非常规天然气具有较理想的应用前景。相较CH_(4)优先渗透膜,N_(2)优先渗透膜优势在于分离N_(2)/CH_(4)混合气后CH_(4)处于高压侧,利于后续处理。以均苯三甲酰氯为油相单体,间苯二胺为水相单体,采用界面聚合法在聚砜基膜上制备致密超薄聚酰胺分离层,并通过向其中引入孔径可允许N_(2)分子通过而不允许CH_(4)分子通过的纳米颗粒ZIF-90,在膜内形成固定的N_(2)传递通道,成功制备了用于脱氮提纯CH_(4)的N_(2)优先渗透混合基质膜。膜渗透选择性能测试结果显示当混合基质膜中纳米颗粒掺杂量为0.30 g·L^(-1)时,2 bar(1 bar=0.1 MPa)进料压力下,N_(2)渗透速率达1.16×10^(-9) mol·m^(-2)·s^(-1)·Pa^(-1),N_(2)/CH_(4)分离因子达16.6,分离因子比未掺杂ZIF-90的聚酰胺膜提高46.5%,具有一定的处理非常规天然气脱氮提纯甲烷的应用潜力。Unconventional natural gas after pretreatment still contains high concentration of N_(2),which can not meet the requirements of pipeline transportation.As an efficient separation method,membrane separation of unconventional natural gas has an ideal application prospect,and the membranes used for separation of unconventional natural gas can be divided into CH_(4)preferential permeation membrane and N_(2)preferential permeation membrane.Compared with the CH_(4)preferential permeation membrane,the advantage of N_(2)preferential permeation membrane is that the CH_(4)product is at the high pressure side after separating N_(2)/CH_(4)mixture,which is conducive to the subsequent treatment.In this work,trimesoyl chloride was used as the oil phase monomer,m-phenylenediamine was used as the water phase monomer,and a dense ultra-thin polyamide separation layer was prepared on polysulfone by interfacial polymerization.By introducing ZIF-90 nanoparticles with pore size that can allow N_(2)molecules to pass through but not CH_(4)molecules,a fixed N_(2)transfer channel was formed in the membrane and the mixed matrix membrane with N_(2)preferential permeation was successfully prepared for N_(2)removal and CH_(4)purification.The permselectivity test results show that the permeation rate of N_(2)is 1.16×10^(-9) mol·m^(-2)·s^(-1)·Pa^(-1) and the separation factor of N_(2)/CH_(4)is 16.6 when the content of nanoparticles in the composite membrane is 0.30 g·L^(-1) and the feed pressure is 2 bar.The separation factor is 46.5%higher than that of the non doping ZIF-90,which shows the potential of the mixed matrix membrane to remove N_(2)andpurify CH_(4)for unconventional natural gas.

关 键 词：气体 分离 N_(2)/CH_(4)分离 界面聚合 膜 混合基质膜 

分 类 号：TQ028.8[化学工程]