沸石咪唑酯骨架材料合成及其在气体吸附分离领域的研究进展

doi:10.16085/j.issn.1000-6613.2018-1090

化工进展 ›› 2019, Vol. 38 ›› Issue (05): 2243-2253.DOI: 10.16085/j.issn.1000-6613.2018-1090

沸石咪唑酯骨架材料合成及其在气体吸附分离领域的研究进展

薛雯丹,朱绪娅,周启星,李凤祥()

南开大学环境科学与工程学院，环境污染过程与基准教育部重点实验室，天津市城市生态环境修复与污染防治重点实验室，天津 300350

收稿日期:2018-05-28 修回日期:2018-09-13 出版日期:2019-05-05 发布日期:2019-05-05
通讯作者: 李凤祥
作者简介:<named-content content-type="corresp-name">薛雯丹</named-content>（1993—），女，博士研究生，研究方向为纳米结构功能材料与环境生物电化学。|李凤祥，博士，讲师，从事水污染控制工程、生物质能源化、废水生态毒理及修复研究。E-mail: <email>lifx@nankai.edu.cn</email>。
基金资助:
国家自然科学基金面上项目(31570504);天津市自然科学基金(16JCYBJC22900)

Synthesis of the zeolitic imidazole frameworks (ZIFs) and the research progress in gas adsorption and separation

Wendan XUE,Xuya ZHU,Qixing ZHOU,Fengxiang LI()

Tianjin Key Laboratory of Environmental Remediation and Pollution Control, Key Laboratory of Pollution Processes and Environmental Criteria at Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China

Received:2018-05-28 Revised:2018-09-13 Online:2019-05-05 Published:2019-05-05
Contact: Fengxiang LI

摘要/Abstract

摘要：

气体分离在石油化工和化工生产中有非常重要的作用。沸石咪唑酯骨架（ZIFs）作为一种新型的多孔材料，具有大比表面积、高孔隙率、多样的结构组成和超高的热稳定及化学稳定性，成为该领域的研究热点。本文围绕ZIFs材料的合成展开，详尽地总结了现阶段ZIFs在气体吸附分离领域的应用，重点介绍ZIFs在工业CO₂捕获及分离、轻质烃分离、气相色谱分离、用于气体分离的ZIFs基膜、惰性气体分离和有毒气体分离等行业的研究进展。同时指出，ZIFs材料在气体吸附分离领域的应用仍需要进一步研究，如新型低成本配体的开发、探索更多的合成方法来调整晶体结构、提升ZIFs材料的吸附效率，才能使ZIFs从实验室走向工业化。

关键词: 沸石咪唑酯骨架, 吸附, 分离, 合成, 金属有机骨架

Abstract:

Gas separation plays a crucial role in petrochemical engineering and chemical production. Zeolitic imidazole frameworks (ZIFs), as a new type of porous material, has become a research hotspot in gas separation because of its large surface area, high porosity, various structural compositions, and super high chemical and thermal stability. In this paper, the synthesis methods of ZIFs and its applications in adsorption and separation are reviewed. This article focuses on the progress in industrial CO₂ capture and separation, light hydrocarbon separation, gas chromatography, ZIFs based membrane, inert and toxic gas separation. It is also pointed out that the application of ZIFs in the gas adsorption and separation field still needs further study, such as developing novel low-cost ligands, exploring more synthesis methods to adjust the crystal structure, and enhancing the adsorption efficiency.

Key words: zeolitic imidazole frameworks (ZIFs), adsorption, separation, synthesis, metal organic frameworks (MOFs)

中图分类号:

薛雯丹, 朱绪娅, 周启星, 李凤祥. 沸石咪唑酯骨架材料合成及其在气体吸附分离领域的研究进展[J]. 化工进展, 2019, 38(05): 2243-2253.

Wendan XUE, Xuya ZHU, Qixing ZHOU, Fengxiang LI. Synthesis of the zeolitic imidazole frameworks (ZIFs) and the research progress in gas adsorption and separation[J]. Chemical Industry and Engineering Progress, 2019, 38(05): 2243-2253.

图/表 7

参考文献 51

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名称	拓扑结构	沸石结构	金属原子密度(T/V) /nm^-3	孔径d _a /?	笼径d _p /?
ZIF-7	sod	SOD	2.49	2.9	4.31
ZIF-8	sod	SOD	2.45	3.4	11.6
ZIF-9	sod	SOD	2.51	3.9	4.31
ZIF-10	mer	MER	2.25	8.2	12.2
ZIF-11	rho	RHO	2.02	3.0	14.6
ZIF-12	rho	RHO	2.02	3.0	14.6
ZIF-20	lta	LTA	2.04	2.8	15.4
ZIF-22	lta	LTA	2.02	2.9	14.8
ZIF-60	mer	MER	2.24	7.2	9.4
ZIF-65	sod	SOD	2.33	3.4	10.4
ZIF-67	sod	SOD	2.46	3.4	11.6
ZIF-68	gme	GME	2.11	7.5	10.3
ZIF-69	gme	GME	2.10	4.4	7.8
ZIF-70	gme	GME	2.11	13.1	15.9
ZIF-76	lta	LTA	1.03	5.4	12.2
ZIF-78	gme	GME	2.08	3.8	7.1
ZIF-79	gme	GME	2.10	4.0	7.5
ZIF-80	gme	GME	2.07	9.8	13.2
ZIF-81	gme	GME	2.08	3.9	7.4
ZIF-82	gme	GME	2.09	8.1	12.3
ZIF-90	sod	SOD	2.33	3.5	11.2
ZIF-91	sod	SOD	2.33	3.2	11
ZIF-92	sod	SOD	2.33	0	5.2
ZIF-95	poz	—	1.51	3.7	24
ZIF-100	moz	—	1.29	3.4	35.6

名称	拓扑结构	沸石结构	金属原子密度(T/V) /nm^-3	孔径d _a /?	笼径d _p /?
ZIF-7	sod	SOD	2.49	2.9	4.31
ZIF-8	sod	SOD	2.45	3.4	11.6
ZIF-9	sod	SOD	2.51	3.9	4.31
ZIF-10	mer	MER	2.25	8.2	12.2
ZIF-11	rho	RHO	2.02	3.0	14.6
ZIF-12	rho	RHO	2.02	3.0	14.6
ZIF-20	lta	LTA	2.04	2.8	15.4
ZIF-22	lta	LTA	2.02	2.9	14.8
ZIF-60	mer	MER	2.24	7.2	9.4
ZIF-65	sod	SOD	2.33	3.4	10.4
ZIF-67	sod	SOD	2.46	3.4	11.6
ZIF-68	gme	GME	2.11	7.5	10.3
ZIF-69	gme	GME	2.10	4.4	7.8
ZIF-70	gme	GME	2.11	13.1	15.9
ZIF-76	lta	LTA	1.03	5.4	12.2
ZIF-78	gme	GME	2.08	3.8	7.1
ZIF-79	gme	GME	2.10	4.0	7.5
ZIF-80	gme	GME	2.07	9.8	13.2
ZIF-81	gme	GME	2.08	3.9	7.4
ZIF-82	gme	GME	2.09	8.1	12.3
ZIF-90	sod	SOD	2.33	3.5	11.2
ZIF-91	sod	SOD	2.33	3.2	11
ZIF-92	sod	SOD	2.33	0	5.2
ZIF-95	poz	—	1.51	3.7	24
ZIF-100	moz	—	1.29	3.4	35.6

应用	涉及气体成分
家庭医用富氧空气（N₂/O₂分离）	O₂、N₂、CO₂、H₂O及惰性气体
从甲烷气体中提取CO₂、CO和H₂	CO₂、CO、H₂、CH₄、N₂及H₂O
从炼油厂尾气生产H₂（分离H₂和H₂O，C1~C5烷烃和烯烃）	H₂和H₂O，C1～C5烷烃和烯烃
合成气中回收H₂（CO/H₂分离）	H₂和CO
溶剂蒸汽回收（H₂O、氯氟烃、醇、酮、BTX和N₂）	CH₄、CO₂、N₂、O₂和氯氟烃
垃圾填埋气中CH₄和CO₂的回收（CO₂/CH₄分离）	CH₄、CO₂、N₂、O₂和氯氟烃
天然气脱硫及燃料运输	H₂S、COS、N₂、H₂、CH₄、CO₂、H₂O、有机硫化物
挥发性有机化合物（VOCs）去除	BTX、乙苯、醇类、酮类、氯代烃类、N₂、H₂O等有机蒸汽
工业气体干燥、H₂O去除	H₂O、N₂、CH₄、CO₂、醇、氯代碳氟化合物
空气制动干燥、H₂O去除	H₂O、CO₂、N₂、O₂、Ar
电子气体净化	O₂、N₂、CO、CO₂、NF₃、N₂F₆、SF₆、CF₄、C₂F₆
石蜡分离（正构烷烃与异链烷烃、芳烃的分离）	各种石蜡，异链烷烃、芳烃
二甲苯分离	p-二甲苯、o-二甲苯、m-二甲苯、乙苯
从高炉煤气中除去CO₂	CO₂、N₂、O₂、CO、NO _x 、SO₂、C _x H _y 、HCl; CO₂、C _x H _y 、H₂S、N₂和He
烟道气捕获CO₂	CO₂、N₂、O₂、CO、NO _x 、SO₂、C _x H _y 、HCl
CO₂/CH₄和N₂/CH₄分离用于天然气提质	CH₄、N₂、CO₂、C₂H₆、C₃H₈、C₄H₁₀、H₂S和He
在核相关产业废气处理，NO _x 去除和Xe纯化	I₂、Kr、NO _x 、Xe
从天然气或空气中分离He	He、N₂、O₂、CO₂、H₂O；He、CH₄、CO₂、N₂
气体分离中Ne、Ar、Kr和Xe的分离或合成氨弛放气	Ne、Ar、Ke、Xe、N₂、O₂、CO₂、H₂O；Ne、Ar、Ke、Xe、H₂、N₂、CH₄、NH₃
从金属氢化物、碳氢化合物和酸性气体中去除硅烷	SiH₄和一些碳氢化合物或酸性气体（如CO₂、H₂S和COS）
烟气净化（去除烟气中的SO₂、NO _x 和HCl）	SO₂、NO _x 、HCl、N₂、CO₂、O₂、CO和C _x H _y
除去微量的NH₃	NH₃等气体
酒精脱水	H₂O和乙醇
从烯烃中去除二烯烃	二烯烃和烯烃
烯烃分离	各种烯烃
石蜡/烯烃分离	C₂H₄和C₂H₆；C₃H₆和C₃H₈
从天然气中分离CO₂和C₂H₄	CO₂、C₂H₄、CH₄、C₂H₆、C₃H₈、C₄H₁₀、H₂S、N₂、He
气体同位素分离	H₂、D₂和T_2；He和⁴He

应用	涉及气体成分
家庭医用富氧空气（N₂/O₂分离）	O₂、N₂、CO₂、H₂O及惰性气体
从甲烷气体中提取CO₂、CO和H₂	CO₂、CO、H₂、CH₄、N₂及H₂O
从炼油厂尾气生产H₂（分离H₂和H₂O，C1~C5烷烃和烯烃）	H₂和H₂O，C1～C5烷烃和烯烃
合成气中回收H₂（CO/H₂分离）	H₂和CO
溶剂蒸汽回收（H₂O、氯氟烃、醇、酮、BTX和N₂）	CH₄、CO₂、N₂、O₂和氯氟烃
垃圾填埋气中CH₄和CO₂的回收（CO₂/CH₄分离）	CH₄、CO₂、N₂、O₂和氯氟烃
天然气脱硫及燃料运输	H₂S、COS、N₂、H₂、CH₄、CO₂、H₂O、有机硫化物
挥发性有机化合物（VOCs）去除	BTX、乙苯、醇类、酮类、氯代烃类、N₂、H₂O等有机蒸汽
工业气体干燥、H₂O去除	H₂O、N₂、CH₄、CO₂、醇、氯代碳氟化合物
空气制动干燥、H₂O去除	H₂O、CO₂、N₂、O₂、Ar
电子气体净化	O₂、N₂、CO、CO₂、NF₃、N₂F₆、SF₆、CF₄、C₂F₆
石蜡分离（正构烷烃与异链烷烃、芳烃的分离）	各种石蜡，异链烷烃、芳烃
二甲苯分离	p-二甲苯、o-二甲苯、m-二甲苯、乙苯
从高炉煤气中除去CO₂	CO₂、N₂、O₂、CO、NO _x 、SO₂、C _x H _y 、HCl; CO₂、C _x H _y 、H₂S、N₂和He
烟道气捕获CO₂	CO₂、N₂、O₂、CO、NO _x 、SO₂、C _x H _y 、HCl
CO₂/CH₄和N₂/CH₄分离用于天然气提质	CH₄、N₂、CO₂、C₂H₆、C₃H₈、C₄H₁₀、H₂S和He
在核相关产业废气处理，NO _x 去除和Xe纯化	I₂、Kr、NO _x 、Xe
从天然气或空气中分离He	He、N₂、O₂、CO₂、H₂O；He、CH₄、CO₂、N₂
气体分离中Ne、Ar、Kr和Xe的分离或合成氨弛放气	Ne、Ar、Ke、Xe、N₂、O₂、CO₂、H₂O；Ne、Ar、Ke、Xe、H₂、N₂、CH₄、NH₃
从金属氢化物、碳氢化合物和酸性气体中去除硅烷	SiH₄和一些碳氢化合物或酸性气体（如CO₂、H₂S和COS）
烟气净化（去除烟气中的SO₂、NO _x 和HCl）	SO₂、NO _x 、HCl、N₂、CO₂、O₂、CO和C _x H _y
除去微量的NH₃	NH₃等气体
酒精脱水	H₂O和乙醇
从烯烃中去除二烯烃	二烯烃和烯烃
烯烃分离	各种烯烃
石蜡/烯烃分离	C₂H₄和C₂H₆；C₃H₆和C₃H₈
从天然气中分离CO₂和C₂H₄	CO₂、C₂H₄、CH₄、C₂H₆、C₃H₈、C₄H₁₀、H₂S、N₂、He
气体同位素分离	H₂、D₂和T_2；He和⁴He

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沸石咪唑酯骨架材料合成及其在气体吸附分离领域的研究进展

Synthesis of the zeolitic imidazole frameworks (ZIFs) and the research progress in gas adsorption and separation

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