掺杂MIL-53同源金属的氧化锆支撑体及膜的制备  

Preparation of Zirconia supports and membranes doped with MIL-53 homologous metals

作　　者：王欢 王彦博 王世龙 侯如静 王重庆 潘宜昌 WANG Huan;WANG Yanbo;WANG Shilong;HOU Rujing;WANG Chongqing;PAN Yichang(State Key Laboratory of Materials-Oriented Chemical Engineering,College of Chemical Engineering,Nanjing Tech University,Nanjing 211800,China)

机构地区：[1]南京工业大学化工学院材料化学工程国家重点实验室,江苏南京211800

出　　处：《南京工业大学学报（自然科学版）》2023年第6期621-630,共10页Journal of Nanjing Tech University(Natural Science Edition)

基　　金：国家自然科学基金(22022807);江苏省自然科学基金(BK20200033)。

摘　　要：采用平均粒径为12.4μm的ZrO_(2)粉体为原料,加入摩尔分数为2.6%的Y_(2)O_(3)作为稳定剂,掺杂摩尔分数为14.9%的同源(MIL-53)金属氧化物αAl_(2)O_(3),采用干压成型法制备多孔陶瓷支撑体。支撑体中的αAl_(2)O_(3)提供铝源与有机配体对苯二甲酸反应在该支撑体表面合成MIL-53种子层,通过晶种二次生长法制备了致密的MIL-53膜,并用于C6烷烃异构体的分离。采用扫描电子显微镜(SEM)、X线衍射仪(XRD)、压汞仪等对支撑体及MIL-53种子层和膜层的表面结构和性能进行表征。研究表明,在烧结温度为1300℃时,制得的支撑体性能良好,支撑体的孔隙率为30.1%,纯N_(2)通量达到1.17×10^(-7)m^(3)/(m^(2)·s·Pa)。此外,合成的MIL-53膜连续且致密,渗透汽化结果显示正己烷和3甲基戊烷的质量分数从原料侧的67.72%提浓到渗透侧的74.67%,而2,2二甲基丁烷从原来的32.28%下降到25.33%,且总通量高达1.56×10^(3)g/(m^(2)·h)。因此,制备的MIL 53膜具有一定的应用价值。The porous ceramic support was prepared by dry pressing method by using ZrO_(2)powder with an average particle size of 12.4μm,adding Y_(2)O_(3)with a molar fraction of 2.6%as a stabilizer and dopingα-Al_(2)O_(3)with a molar fraction of 14.9%as a homolog(MIL-53)metal oxide.Theα-Al_(2)O_(3)in the support provides aluminum source to react with the organic ligand terephthalic acid on the surface of the support to synthesize the MIL-53 seed layer,and the dense MIL 53 film was prepared by seed-secondary growth method,and was used for the separation of C6 alkane isomers.Scanning electron microscopy(SEM),X-ray diffraction(XRD)and mercury injection were used to characterize the surface structure and properties of the support,MIL-53 seed layer and film layer.The results showed that the prepared support had good performance at 1300℃,the porosity of the support was 30.1%,and the pure N_(2)flux reaches 1.17×10^(-7)m^(3)/(m^(2)·s·Pa).In addition,the synthesized MIL-53 membrane was continuous and dense,and the pervaporization results showed that the mass fraction of n-hexane and 3-methylpentane increased from 67.72%on the feedstock side to 74.67%on the permeable side,while the mass fraction of 2,2-dimethylbutane decreased from^(3)2.28%to 25.33%.The total flux was as high as 1.56×10^(3)g/(m^(2)·h).Therefore,the prepared MIL-53 membrane had certain application value.

关 键 词：ZrO_(2)支撑体 同源金属掺杂 MIL-53 渗透汽化 

分 类 号：TQ174.79[化学工程—陶瓷工业]