N2优先渗透ZIF-8复合膜的制备及其CO2捕集

doi:10.11949/j.issn.0438-1157.20190538

摘要/Abstract

摘要：

为了获得经济节能的烟道气CO₂回收方法，制备了一种新型的N₂优先渗透ZIF-8复合膜。以柔性聚砜(PSf)多孔膜为支撑层，采用Zn²⁺与壳聚糖的交联溶液对聚砜支撑层表面改性，使Zn²⁺固定在PSf膜表面；然后与2-甲基咪唑(Hmim)配位得到ZIF-8晶种层；最后通过界面聚合法二次生长制得ZIF-8复合膜。采用FTIR、XRD及SEM对ZIF-8复合膜的形貌结构进行表征，结果显示成功制备了致密的ZIF-8复合膜。在进料气为纯气条件下，探究了二次生长时间、Zn²⁺溶液的浓度、测试时间及测试压力对ZIF-8复合膜N₂/CO₂分离性能的影响，阐明其N₂优先渗透机理；并进一步考察了混合气分离性能。结果表明：在25℃和0.1 MPa下，最优ZIF-8复合膜的N₂渗透性为523 GPU，N₂/CO₂选择性为19；同条件下混合气的N₂渗透性和N₂/CO₂选择性分别为517 GPU和18。所制备的ZIF-8复合膜可以使N₂优先渗透，实现烟道气中高浓度N₂渗透，低浓度CO₂截留在膜的上游侧。原因主要是ZIF-8复合膜含有较多的CO₂强吸附位点，使CO₂被吸附在膜内不易从膜的下游侧脱附，渗透性小，而N₂优先渗透，这为N₂优先渗透膜的制备提供了一种新思路。

关键词: ZIF-8, 二次生长, 膜, 烟道气, CO₂捕集

Abstract:

To improve the economic benefits of CO₂ capture in flue gas, a novel N₂ selective zeolitic imidazolate framework-8 (ZIF-8) composite membrane has been designed in this work. The zinc ion (Zn²⁺) was tightly adhered to the polysulfone support by chelating crosslinked chitosan matrix. The ZIF-8 seeding layer was prepared by zinc ion coordinated with 2-methylimidazole (Hmim), and then the dense ZIF-8 composite membrane was prepared by the secondary growth method. The morphological structure of ZIF-8 composite membrane was characterized by FTIR, XRD and SEM. And the results showed that the dense ZIF-8 composite membrane has been prepared. The effects of the time of secondary growth, the concentration of Zn²⁺ solution, the continuous test time and feed gas pressure on gas separation performance of ZIF-8 composite membrane were systematically investigated by pure gas, and the gas transport mechanism was analyzed. In addition, the separation performance of membranes was investigated by CO₂/N₂ mixed gas. At testing temperature of 25℃ and feed gas pressure of 0.1 MPa, N₂ permeance and N₂/CO₂selectivity were 523 GPU and 19 for pure gas, respectively. While N₂ permeance and N₂/CO₂ selectivity were 517 GPU and 18 for mixed gas under the same condition, respectively. The results showed that the ZIF-8 composite membrane could preferentially permeate N₂in the flue gas. The ZIF-8 composite membrane contained many CO₂ active adsorption sites, so that CO₂ was adsorbed in the membrane and was not easily desorbed from the downstream side of the membrane, and N₂ could preferentially permeate, which provided a new idea for the preparation of N₂ selective membrane.

Key words: ZIF-8, secondary growth, membranes, flue gas, CO₂ capture

中图分类号:

TQ 028.8

廉玉姣, 王永洪, 张新儒, 李晋平. N₂优先渗透ZIF-8复合膜的制备及其CO₂捕集[J]. 化工学报, 2019, 70(9): 3573-3581.

Yujiao LIAN, Yonghong WANG, Xinru ZHANG, Jinping LI. Preparation of N₂ selective ZIF-8 composite membrane for CO₂ capture[J]. CIESC Journal, 2019, 70(9): 3573-3581.

图/表 8

图1 ZIF-8复合膜的制备图

Fig.1 Schematic diagram of ZIF-8 composite membrane fabrication

图2 ZIF-8复合膜表面ZIF-8晶粒的FTIR谱图(a)及XRD谱图(b)；ZIF-8晶种层(c)和ZIF-8复合膜的SEM图(d)

Fig.2 FTIR spectra (a) and XRD patterns (b) of ZIF-8 crystals collected from bottom of ZIF-8 composite membrane; SEM micrographs of surface of ZIF-8 seeding layer (c) and ZIF-8 composite membrane(d)

图3 二次生长时间对ZIF-8复合膜气体分离性能的影响(a)；不同方法(界面聚合法和溶液聚合法)制备的ZIF-8在298 K下的CO2吸附等温线(b)； ZIF-8复合膜的气体传递机理图(c)

Fig.3 Effect of secondary growth time on gas separation performance of ZIF-8 composite membranes(a); CO2 adsorption isotherms at 298 K of ZIF-8 prepared by interfacial polymerization and solution polymerization(b); schematic diagram of gas transport pathway for ZIF-8 composite membrane(c)

图4 Zn2+溶液的浓度对ZIF-8复合膜气体分离性能的影响

Fig.4 Effect of concentration of Zn2+ solution on gas separation performance of ZIF-8 composite membranes

图5 ZIF-8-48-7.5/15/30/60复合膜的气体分离性能随测试时间的变化

Fig.5 Effect of continuous test time on gas separation performance of ZIF-8-48-7.5/15/30/60 composite membranes

图6 进料压力对ZIF-8-48-15复合膜气体分离性能的影响

Fig.6 Effect of feed gas pressure on gas separation performance of ZIF-8-48-15 composite membrane

图7 ZIF-8复合膜纯气和混合气的气体渗透性和N2/CO2选择性对比

Fig.7 Gas permeance and N2/CO2 selectivity of ZIF-8 composite membranes as detemined by pure gas and mixed gas

图8 ZIF-8复合膜的N2渗透性和N2/CO2选择性与文献中的MOFs膜对比

Fig.8 Comparation of N2 permeance and N2/CO2 selectivity of ZIF-8 composite membrane in this work with other MOFs membrane from literatures

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N₂优先渗透ZIF-8复合膜的制备及其CO₂捕集

Preparation of N₂ selective ZIF-8 composite membrane for CO₂ capture

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