SIFSIX-3-Ni膜的制备及氢气分离性质

doi:10.7503/cjcu20190085

高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (9): 1818.doi: 10.7503/cjcu20190085

SIFSIX-3-Ni膜的制备及氢气分离性质

穆鑫,姜双双,张舒皓,任浩,孙福兴()

吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012

收稿日期:2019-01-29 出版日期:2019-09-10 发布日期:2019-07-12
通讯作者: 孙福兴 E-mail:fxsun@jlu.edu.cn
基金资助:
国家自然科学基金(批准号: )资助(21871105, 21531003);国家自然科学基金(21871105, 21531003)

Growth and Gas Permeation Properties of SIFSIX-3-Ni Membrane ^†

MU Xin,JIANG Shuangshuang,ZHANG Shuhao,REN Hao,SUN Fuxing()

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry,Jilin University, Changchun 130012, China

Received:2019-01-29 Online:2019-09-10 Published:2019-07-12
Contact: SUN Fuxing E-mail:fxsun@jlu.edu.cn
Supported by:
? Supported by the National Natural Science Foundation of China(21871105, 21531003);Supported by the National Natural Science Foundation of China(21871105, 21531003)

摘要/Abstract

摘要：

利用(NH₄)₂SiF₆修饰大孔玻璃基底后, 在溶剂热条件下制备了SIFSIX-3-Ni膜, 并研究了温度和浓度对制备SIFSIX-3-Ni膜的影响. 能谱分析(XPS)结果表明大孔玻璃表面引入了氟元素. SIFSIX-3-Ni膜的粉末X射线衍射(PXRD)峰位置和模拟结果一致, 表明成功制备出SIFSIX-3-Ni膜. 从扫描电子显微镜(SEM)照片中观察到膜连续均匀, 厚度约为20 μm. 热重分析(TGA)结果表明, 活化前的膜没有客体分子. 单组分测试结果表明, 膜的H₂, CO₂和N₂渗透量分别为6.83×10 ^-6, 7.42×10 ^-7和8.89×10 ^-7 mol·m ^-2·s ^-1·Pa ^-1, H₂/CO₂和H₂/N₂的理想分离比分别为9.20和7.68. 在连续测试5 h后, H₂, CO₂和N₂渗透量基本保持不变, 表明SIFSIX-3-Ni膜具有很好的稳定性.

关键词: SIFSIX-3-Ni多晶膜, 原位生长法, 氢气分离

Abstract:

Using the macroporous glass-frit disk modified by (NH₄)₂SiF₆ as the substrate, we prepared the SIFSIX-3-Ni membrane by the in situ growth method under solvothermal conditions. The effect of temperature and concentration on the preparation of SIFSIX-3-Ni membrane were investigated in detail. X-Ray photoelectron spectroscopy(XPS) demonstrates that F atom was integrated into the substrate surface. The powder X-ray diffraction(PXRD) patterns were in accordance with the simulated one, indicating that we obtained SIFSIX-3-Ni membranes successfully. Scanning electron microscopy(SEM) showed that the SIFSIX-3-Ni-3 membrane was continuous and uniform with a thickness of about 20 μm. Thermogravimetric analysis(TGA) showed that there was no guest molecules in the membrane before activation. Single gas permeation measurement on SIFSIX-3-Ni-3 membrane demonstrated that the permeability of H₂, CO₂ and N₂ were 6.83×10 ^-6, 7.42×10 ^-7 and 8.89×10 ^-7 mol·m ^-2·s ^-1·Pa ^-1 respectively, and the ideal selectivities of H₂/CO₂ and H₂/N₂ were 9.20 and 7.68 respectively. The membrane can retain almost the same permeance of H₂, CO₂ and N₂ after 5 h of continuous testing, indicating that SIFSIX-3-Ni membrane have good stability.

Key words: SIFSIX-3-Ni membrane, In situ growth method, H₂ separation

中图分类号:

O614
O657

TrendMD:

穆鑫, 姜双双, 张舒皓, 任浩, 孙福兴. SIFSIX-3-Ni膜的制备及氢气分离性质. 高等学校化学学报, 2019, 40(9): 1818.

MU Xin, JIANG Shuangshuang, ZHANG Shuhao, REN Hao, SUN Fuxing. Growth and Gas Permeation Properties of SIFSIX-3-Ni Membrane ^†. Chem. J. Chinese Universities, 2019, 40(9): 1818.

图/表 8

Fig.1 PXRD patterns of the activated(a), as-synthesized(b) and simulated(c) SIFSIX-3-Ni(A) and adsorption isotherm of CO2 at 298 K for SIFSIX-3-Ni(B)

Scheme 1 Schematic diagram of in situ growth method of SIFSIX-3-Ni membrane

Fig.2 F1s XPS spectra of (NH4)2SiF6 powder(a), SIFSIX-3-Ni membrane(b), glass frit disk treated in(NH4)2SiF6 solution(c), glass frit disk treated in a solution of H2SO4 and H2O2(d) and raw glass-frit disk surface(e)(A) and enlarged pattern of glass frit disk treated in (NH4)2SiF6 solution(B)

Fig.3 PXRD patterns of SIFSIX-3-Ni membrane(A) and TG analysis of SIFSIX-3-Ni-3 membrane(B) (A) a. activated SIFSIX-3-Ni-3, b. SIFSIX-3-Ni-3, c. SIFSIX-3-Ni-2, d. SIFSIX-3-Ni-1, e. simulated; (B) a. activated, b. as-synthesized.

Fig.4 SEM images of SIFSIX-3-Ni-1(A), SIFSIX-3-Ni-2(B) and SIFSIX-3-Ni-3(C) membrane

Fig.5 Optical images of SIFSIX-3-Ni-2 membrane(A), SEM images of macroporous glass-frit disk(B), SIFSIX-3-Ni-2 membrane(C, D) and cross-section of the SIFSIX-3-Ni-2 membrane(E, F)

Fig.6 Optical image of SIFSIX-3-Ni-3 membrane(A), SEM images of macroporous glass-frit disk(B), SIFSIX-3-Ni-3 membrane(C, D) and cross-section of the SIFSIX-3-Ni-3 membrane(E, F)

Fig.7 H2, N2 and CO2 permeance as a function of molecular weight(A) and H2(c), N2(b) and CO2(a) permeance with time(B) on SIFSIX-3-Ni-3 membrane

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SIFSIX-3-Ni膜的制备及氢气分离性质

Growth and Gas Permeation Properties of SIFSIX-3-Ni Membrane ^†

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Growth and Gas Permeation Properties of SIFSIX-3-Ni Membrane ^†