MOF及其复合材料吸附去除VOCs应用研究进展

doi:10.16085/j.issn.1000-6613.2020-0387

摘要/Abstract

摘要：

金属有机骨架材料（MOF）是一种高比表面积、活性位点丰富、易化学修饰的新型多孔材料，但较差的水稳定性限制其在吸附挥发性有机化合物（VOCs）领域的应用，因此如何提高和巩固MOF的吸附性能已成为研究的热点。本文从单体MOF的合成、MOF复合材料的制备、吸附机理和吸附影响因素等方面综述了MOF及其复合材料吸附去除VOCs的研究进展。针对目前MOF材料在吸附VOCs方面的不足提出研究建议，展望其在VOCs吸附领域的发展方向为制备富含微-介孔结构和活性位点、水热稳定性强、抗水蒸气竞争吸附好和循环利用率高的新型高稳定性材料，以及开发新型MOF材料合成方法。

关键词: 金属有机骨架材料, 复合材料, 挥发性有机物, 吸附机理, 影响因素

Abstract:

Metal organic framework (MOF) is a new type of porous material with high specific surface area, abundant active sites and easy chemical modification. However, its poor water stability limits its application in adsorption of volatile organic compounds (VOCs). Therefore, one hot topic of MOF research is to improve its VOCs adsorption performance. This article reviews the research progress of MOF and its composites for the removal of VOCs from the aspects of synthesis of monomeric MOF, the preparation of MOF composites, the adsorption mechanism and the influence factors in adsorption. In view of the shortcomings of MOF materials in the adsorption of VOCs, research suggestions are put forward. The development directions of MOF materials in VOCs adsorption are to prepare new MOF materials with rich micro-mesoporous structure and active sites, strong hydrothermal stability, good resistance to water vapor’s competition adsorption and high recycling utilization, and to develop new synthesis methods.

Key words: metal organic framework (MOF), composites, volatile organic compounds (VOCs), adsorption mechanism, influence factors

中图分类号:

X511

李孟, 李炜, 张帅, 李雨薇, 刘芳, 赵朝成, 王永强. MOF及其复合材料吸附去除VOCs应用研究进展[J]. 化工进展, 2021, 40(1): 415-426.

Meng LI, Wei LI, Shuai ZHANG, Yuwei LI, Fang LIU, Chaocheng ZHAO, Yongqiang WANG. Research progress on adsorption of VOCs by MOF and its composite[J]. Chemical Industry and Engineering Progress, 2021, 40(1): 415-426.

图/表 10

参考文献 61

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制备方法	优点	缺点
水热法	工艺成熟、反应条件温和	耗时长、合成量少、二次污染
溶剂热法	材料结晶度高、反应条件温和	耗时长、需大量溶剂、成本高、二次污染
机械化学法	简单快捷、无溶剂、产量高、无污染	需高机械能、成本高
微波法	合成快、加热均匀、材料粒径小、产量高	需大量溶剂、成本高、不稳定
电化学合成法	合成时间短、易于控制、产量高	能耗大
溶胶-凝胶法	易操作控制、均匀性好	成本较高、耗时长

制备方法	优点	缺点
水热法	工艺成熟、反应条件温和	耗时长、合成量少、二次污染
溶剂热法	材料结晶度高、反应条件温和	耗时长、需大量溶剂、成本高、二次污染
机械化学法	简单快捷、无溶剂、产量高、无污染	需高机械能、成本高
微波法	合成快、加热均匀、材料粒径小、产量高	需大量溶剂、成本高、不稳定
电化学合成法	合成时间短、易于控制、产量高	能耗大
溶胶-凝胶法	易操作控制、均匀性好	成本较高、耗时长

典型 VOCs	吸附剂	比表面积 /m³?g^-1	孔径分布 /nm	孔容 /cm³?g^-1	吸附位点	亲、疏水性	吸附条件	吸附量 /m³?g^-1	吸附机理
甲苯	Cu-BTC^[33]	793.49	3.49	0.31	微、介孔	亲水性	T=298K，c₀=1300mg·m^-3， m=0.3g	62.7	孔道填充吸附
	Cu-BTC@GO-20%^[33]	512.6	3.86	0.35	微、介孔	亲水性	T=298K，c₀=1300mg·m^-3， m=0.3g	183.6
	Uio-66^[53]	1335	0.45～0.7	0.83	微孔	疏水性	T=298K	151	孔道填充吸附
	ZG-4^[54]	1112	—	—	微孔	亲水性	T=298K，55% RH	116	孔道填充吸附、π-π键作用
	Uio-66-NH₂^[41]	1250	1.98	0.62	微孔	疏水性	T=298K	147	孔道填充吸附、疏水性作用、氢键作用
	CZ-5%^[30]	1484.46	3.27	0.60	微、介孔	疏水性	T=298K，c₀=1300mg·m^-3， m=0.3g，30% RH	158.6	孔道填充吸附、π-π键作用、阳离子-π键作用、疏水性作用
	HK@CMC ^[55]	545		0.371	微、介孔	疏水性	T=298K,P=0.0379bar	285.6	孔道填充吸附
苯	Mg-MOF-74^[56]	—	1.6	0.88	微、介孔	—	T=300K、P=20Pa	640.5	范德华力、库仑作用、孔道填充吸附
苯	MC-500-6^[57]	2320	—	1.05	微、介孔	疏水性	T=298K	999.8	孔道填充吸附、π-π键作用
甲苯、二甲苯	H-MOZs^[52]	1570	—	0.90	微孔、介孔、大孔	—	T=298K	296.7（甲苯）、 148.2（二甲苯）	孔道填充吸附（介孔和大孔的存在促进吸附）
	Uio-66^[58]	—	—	—	微、介孔	—	T=298K，m=5mg，V=10mL，C=100μL·L^-1	22.94（甲苯） 38.31（二甲苯）	孔道填充吸附
	Uio-66-F4^[58]	—	—	—	微、介孔	疏水性		30.49（甲苯） 38.31（二甲苯）	孔道填充吸附、疏水性作用
二氯甲烷	ZG-15^[45]	559.3	2.2	0.32	微、介孔	亲水性	气流速率=20mL·min^-1，床层高度=10cm	240	孔道填充吸附、氢键作用、π-π键作用
苯酚	CNT@MOF-68(Al)^[49]	1290	1.6	—	微、介孔	疏水性	c₀=2000/μL·L^-1、CNT含量=0.75%	341.1	孔道填充吸附、氢键作用和π-π键作用
甲醛	ED-MIL-101-3^[15]	382	2.3	—	微、介孔	疏水性	T=298K、潮湿环境	164.86	疏水性作用、孔道填充吸附（微孔为主）
甲醇、乙醇、正己烷	RGO(2%wt)/ Cu-BTC^[59]	1549	1.54	—	微、介孔	亲水性	T=298K、潮湿环境	421（甲醇） 474.52（乙9醇） 406（正己烷）	静电排斥、亲水性作用、孔道填充吸附、π-π键作用
不同硝基酚	Uio-66-NH₂^[48]	1023	—	0.45	微、介孔	疏水性	pH=4，m=20mg，c₀=80mg·L^-1，T=288K，V=50mL	6.05（苯酚） 44.96（4-NP） 144.10（DNP） 141.09（TNP）	氢键作用、π-π键作用、静电相互作用、孔道填充吸附、配位反应

典型 VOCs	吸附剂	比表面积 /m³?g^-1	孔径分布 /nm	孔容 /cm³?g^-1	吸附位点	亲、疏水性	吸附条件	吸附量 /m³?g^-1	吸附机理
甲苯	Cu-BTC^[33]	793.49	3.49	0.31	微、介孔	亲水性	T=298K，c₀=1300mg·m^-3， m=0.3g	62.7	孔道填充吸附
	Cu-BTC@GO-20%^[33]	512.6	3.86	0.35	微、介孔	亲水性	T=298K，c₀=1300mg·m^-3， m=0.3g	183.6
	Uio-66^[53]	1335	0.45～0.7	0.83	微孔	疏水性	T=298K	151	孔道填充吸附
	ZG-4^[54]	1112	—	—	微孔	亲水性	T=298K，55% RH	116	孔道填充吸附、π-π键作用
	Uio-66-NH₂^[41]	1250	1.98	0.62	微孔	疏水性	T=298K	147	孔道填充吸附、疏水性作用、氢键作用
	CZ-5%^[30]	1484.46	3.27	0.60	微、介孔	疏水性	T=298K，c₀=1300mg·m^-3， m=0.3g，30% RH	158.6	孔道填充吸附、π-π键作用、阳离子-π键作用、疏水性作用
	HK@CMC ^[55]	545		0.371	微、介孔	疏水性	T=298K,P=0.0379bar	285.6	孔道填充吸附
苯	Mg-MOF-74^[56]	—	1.6	0.88	微、介孔	—	T=300K、P=20Pa	640.5	范德华力、库仑作用、孔道填充吸附
苯	MC-500-6^[57]	2320	—	1.05	微、介孔	疏水性	T=298K	999.8	孔道填充吸附、π-π键作用
甲苯、二甲苯	H-MOZs^[52]	1570	—	0.90	微孔、介孔、大孔	—	T=298K	296.7（甲苯）、 148.2（二甲苯）	孔道填充吸附（介孔和大孔的存在促进吸附）
	Uio-66^[58]	—	—	—	微、介孔	—	T=298K，m=5mg，V=10mL，C=100μL·L^-1	22.94（甲苯） 38.31（二甲苯）	孔道填充吸附
	Uio-66-F4^[58]	—	—	—	微、介孔	疏水性		30.49（甲苯） 38.31（二甲苯）	孔道填充吸附、疏水性作用
二氯甲烷	ZG-15^[45]	559.3	2.2	0.32	微、介孔	亲水性	气流速率=20mL·min^-1，床层高度=10cm	240	孔道填充吸附、氢键作用、π-π键作用
苯酚	CNT@MOF-68(Al)^[49]	1290	1.6	—	微、介孔	疏水性	c₀=2000/μL·L^-1、CNT含量=0.75%	341.1	孔道填充吸附、氢键作用和π-π键作用
甲醛	ED-MIL-101-3^[15]	382	2.3	—	微、介孔	疏水性	T=298K、潮湿环境	164.86	疏水性作用、孔道填充吸附（微孔为主）
甲醇、乙醇、正己烷	RGO(2%wt)/ Cu-BTC^[59]	1549	1.54	—	微、介孔	亲水性	T=298K、潮湿环境	421（甲醇） 474.52（乙9醇） 406（正己烷）	静电排斥、亲水性作用、孔道填充吸附、π-π键作用
不同硝基酚	Uio-66-NH₂^[48]	1023	—	0.45	微、介孔	疏水性	pH=4，m=20mg，c₀=80mg·L^-1，T=288K，V=50mL	6.05（苯酚） 44.96（4-NP） 144.10（DNP） 141.09（TNP）	氢键作用、π-π键作用、静电相互作用、孔道填充吸附、配位反应

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