Research Progresses of Metal-organic Framework HKUST-1-Based Membranes in Gas Separations※

doi:10.6023/A21120545

Acta Chimica Sinica ›› 2022, Vol. 80 ›› Issue (3): 340-358.DOI: 10.6023/A21120545 Previous Articles Next Articles

Special Issue: 中国科学院青年创新促进会合辑

Review

金属-有机框架HKUST-1膜在气体分离中研究进展^※

李崇^b, 李娜^b, 常立美^b, 谷志刚^a^,^b^,^*(), 张健^a^,^b

a 中国福建光电信息科学与技术创新实验室(闽都创新实验室) 福州 350108
b 中国科学院福建物质结构研究所福州 350002

投稿日期:2021-12-05 发布日期:2022-01-07
通讯作者: 谷志刚

作者简介:

李崇, 中国科学院福建物质结构研究所与福州大学联合培养2021级硕士研究生, 主要从事MOF薄膜的制备与应用研究.

李娜, 中国科学院福建物质结构研究所与福州大学联合培养2020级硕士研究生, 主要从事MOF薄膜的制备与应用研究.

谷志刚, 中国科学院福建物质结构研究所研究员, 中国科学院青年创新促进会会员, 博士生导师. 2014年获卡尔斯鲁厄理工大学(KIT)博士学位, 随后在KIT从事博后研究, 2015年在中科院福建物质结构研究所结构化学国家重点实验室任副研究员、2018晋升为研究员和博士生导师. 主要从事表面配位金属-有机框架薄膜(SURMOF)的组装及其在多个领域的功能与应用研究, 包括拓展其在非线性光学(光限幅)、光电薄膜器件、分子(手性)识别与分离等领域.

^† 共同第一作者

^※ 庆祝中国科学院青年创新促进会十年华诞.

基金资助:
国家自然科学基金(21872148); 中国科学院青年创新促进会(2018339); 中国福建光电信息科学与技术创新实验室(闽都创新实验室)基金(2021ZR131)

Research Progresses of Metal-organic Framework HKUST-1-Based Membranes in Gas Separations^※

Chong Li^b, Na Li^b, Limei Chang^b, Zhigang Gu^a^,^b(), Jian Zhang^a^,^b

a Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou 350108
b Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002

Received:2021-12-05 Published:2022-01-07
Contact: Zhigang Gu
About author:
^† These authors contributed equally to this work
^※ Dedicated to the 10th anniversary of the Youth Innovation Promotion Association, CAS.
Supported by:
National Natural Science Foundation of China(21872148); Youth Innovation Promotion Association, CAS(2018339); Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China(2021ZR131)

The development of high-efficiency, green and energy-saving material separation and purification technology is of great significance, and gas separation has a wide range of applications in the fields of industry, energy, medical treatment and technology. Since traditional polymer membranes still face many challenges in achieving high-efficient gas separation, the development of new separation membrane materials has become the current hotspot and difficult issue. As an emerging porous coordination polymer, metal-organic frameworks (MOFs) materials have attracted great attention due to their unique, designable topological structures and tunable functionalities. In order to overcome the problem that bulk or powder MOFs are difficult to be used for gas separation efficiently, it is of great significance and a challenging task to develop MOFs membranes for separation. As a representative MOF material, MOF HKUST-1 is widely used to prepare membranes for gas separation due to its advantages of high stability, economic raw material and hierarchical pore structure. The preparation methods and gas separation performances of the HKUST-1 membrane in the past ten years are summarized, and some viewpoints and the research prospect on this research area are described.

Key words: metal-organic framework, HKUST-1 membrane, synthesis method, gas separation

Cite this article

Chong Li, Na Li, Limei Chang, Zhigang Gu, Jian Zhang. Research Progresses of Metal-organic Framework HKUST-1-Based Membranes in Gas Separations^※[J]. Acta Chimica Sinica, 2022, 80(3): 340-358.

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气体	混合组分气体通量/ (10^–6 mol•m^-2•s^-1•Pa^-1)	单组分气体通量/ (10^–6 mol•m^-2•s^-1•Pa^-1)	分离因子	理想分离因子	Knudsen扩散系数
H₂	0.148	0.161	10.20	8.75	3.74
N₂	0.0145	0.0184	10.20	8.75	3.74
H₂	0.152	0.161	11.34	8.13	2.83
CH₄	0.0134	0.0198	11.34	8.13	2.83
H₂	0.143	0.161	10.07	9.53	4.69
CO₂	0.0142	0.0169	10.07	9.53	4.69

气体	混合组分气体通量/ (10^–6 mol•m^-2•s^-1•Pa^-1)	单组分气体通量/ (10^–6 mol•m^-2•s^-1•Pa^-1)	分离因子	理想分离因子	Knudsen扩散系数
H₂	0.148	0.161	10.20	8.75	3.74
N₂	0.0145	0.0184	10.20	8.75	3.74
H₂	0.152	0.161	11.34	8.13	2.83
CH₄	0.0134	0.0198	11.34	8.13	2.83
H₂	0.143	0.161	10.07	9.53	4.69
CO₂	0.0142	0.0169	10.07	9.53	4.69

	气体	渗透率/ (10^-7 mol•m^-2•s^-1•Pa^-1)	H₂的理想选择性	H₂的分离因子
单组分气体	H₂	7.48	—	—
	CH₄	2.57	2.9	—
	N₂	2.00	3.7	—
	CO₂	1.48	5.1	—
混合气体	H₂	5.16	—	3
	CH₄	1.68	—	3
	H₂	4.79	—	3.7
	N₂	1.25	—	3.7
	H₂	6.74	—	4.6
	CO₂	1.40	—	4.6

	气体	渗透率/ (10^-7 mol•m^-2•s^-1•Pa^-1)	H₂的理想选择性	H₂的分离因子
单组分气体	H₂	7.48	—	—
	CH₄	2.57	2.9	—
	N₂	2.00	3.7	—
	CO₂	1.48	5.1	—
混合气体	H₂	5.16	—	3
	CH₄	1.68	—	3
	H₂	4.79	—	3.7
	N₂	1.25	—	3.7
	H₂	6.74	—	4.6
	CO₂	1.40	—	4.6

聚合物	负载量(φ/%)	渗透性^a/Barrer		选择性
聚合物	负载量(φ/%)	O₂	CO₂	O₂/N₂	CO₂/CH₄
Ultem 1000	21.32	1.15	4.34	7.62	42.16
Matrimide 5218	19.67	5.20	24.8	6.66	37.8
RODPA/TMPDA	21.30	29.50	155.0	4.91	27.5
6FDA/TMPDA	22.53	318.0	1560	3.40	18.76

金属-有机框架HKUST-1膜在气体分离中研究进展^※

Research Progresses of Metal-organic Framework HKUST-1-Based Membranes in Gas Separations^※

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膜	CO₂渗透性^b/ Barrer	CO₂/N₂选择性
Matrimid	10.4±0.1	31.0±3.0
Matrimid+HKUST-1-0NH₂ (w=10%)	15.5±1.7	32.3±0.2
Matrimid+HKUST-1-0NH₂ (w=20%)	22.2±3.4	33.8±3.4
Matrimid+HKUST-1-25NH₂ (w=10%)	12.3±0.5	39.4±0.8
Matrimid+HKUST-1-25NH₂ (w=20%)	13.0±0.2	42.7±0.9

膜	C₂H₄渗透性^b/ Barrer	C₂H₄/C₂H₆ 选择性
ODPA-TMPDA	6.3±0.4	3.9±0.4
ODPA-TMPDA+HKUST-1 (w=10%)	13.6±1.7	3.6±0.3
ODPA-TMPDA+HKUST-1 (w=20%)	16.0±0.2	3.4±0.2
6FDA-TMPDA	108±7.2	2.5±0.1
6FDA-TMPDA+HKUST-1 (w=10%)	148±11.8	2.5±0.5
6FDA-TMPDA+HKUST-1 (w=20%)	183±3.8	2.4±0.1

膜	渗透性^a/Barrer			理想选择性
膜	He	CH₄	N₂	He/CH₄	He/N₂
纯聚酰亚胺	23.1	0.18	0.23	131.1	98.6
10% Cu-BTC-R	36.09	0.18	0.24	200.5	150.3
20% Cu-BTC-R	51.9	0.19	0.26	273.5	199.9
30% Cu-BTC-R	57.03	0.19	0.27	300.1	211.2
40% Cu-BTC-R	66.4	0.18	0.25	369.1	265.8
45% Cu-BTC-R	74.5	0.35	0.34	212.9	219.2
5% Cu-BTC-N	27.2	0.2	0.25	136.2	109
10% Cu-BTC-N	34.8	0.29	0.33	120.03	105.4
15% Cu-BTC-N	40.1	0.52	0.49	77.1	81.8
努森选择性	—	—	—	1.99	2.64

基底		合成方法	膜厚度/μm	渗透率/ (10^–7 mol•m^–2•s^–1•Pa^–1)	理想选择性			年份	参考文献
基底		合成方法	膜厚度/μm	渗透率/ (10^–7 mol•m^–2•s^–1•Pa^–1)	H₂/N₂	H₂/CO₂	H₂/CH₄	年份	参考文献
多孔氧化铝		原位生长	20	0.02 (190 ℃)	23 (190 ℃)	4.03 (190 ℃)	—	2009	[117]
铜网		种子二次生长	60	12.7	4.6	4.52	7.8	2009	[120]
α-Al₂O₃		种子二次生长	25	18.5	3.7	3.5	2.4	2010	[115]
α-Al₂O₃		SBS二次生长	25	7.48	3.7	5.1	2.9	2011	[114]
不锈钢网		原位生长	—	13.9	5.08	8.68	7.93	2012	[140]
α-Al₂O₃中空陶瓷纤维(HCFs)		种子二次生长	13	0.725	8.66	13.56	6.19	2012	[123]
氢氧化铜纳米链(CHNs)		种子生长法	5	15.8	3.7	4.7	2.8	2013	[128]
阳极氧化铝(AAO)		种子二次生长	50	1.8	4.2	4.8	3	2013	[113]
α-Al₂O₃	反扩散法		—	0.998 (2 h)	4.92	4.9	4.01	2013	[192]
			—	0.21 (4 h)	28.6	3.82	24.6
			40	0.09 (6 h)	123	3.69	153
α-Al₂O₃		二次生长法	12.5	0.175	7.5	5.3	4.4	2013	[111]
聚偏氟乙烯(PVDF)中空纤维		压力辅助室温生长	6.5	20.1	3.3	4.2	2.5	2014	[124]
不锈钢		电沉积	—	8.5	3.9	4.6	—	2015	[118]
聚偏氟乙烯(PVDF)中空纤维		原位生长	43	84.6	5.87	7.3	—	2015	[125]
阳极氧化铝(AAO)		种子二次生长	8	16.7	6.77	5.63	7.71	2016	[112]
多孔泡沫镍	纳米微结构辅助定向可控制备法		20	27.41	5.2	6	3.7	2016	[107]
			50	19.00	4.4	6.2	3.1
			70	10.96	5	6.9	3.6
			100	7.81	5.1	7.5	3.8
不锈钢网		原位生长	—	7.61	5.6	9.74	6.7	2017	[119]
纳米多孔聚合物(np-PET)		液相外延生长(LPE)	—	2.4	11.14	1.2	10.66	2018	[173]
SiO₂		原位生长	—	1.61	10.2	10.07	11.34	2018	[110]
氧化石墨烯(GO)		原位生长	0.1~0.3	5.77	—	73.2	—	2018	[121]
Al₂O₃		原位生长	72	11.9	9.69	12.04	7.77	2020	[131]

基底	方法	膜厚度/μm	渗透率/ (10^–7 mol•m^–2•s^–1•Pa^–1)	理想选择性		年份	参考文献
基底	方法	膜厚度/μm	渗透率/ (10^–7 mol•m^–2•s^–1•Pa^–1)	CH₄/N₂	CH₄/CO₂	年份	参考文献
α-Al₂O₃	种子二次生长	25	8	1.57	1.57	2010	[115]
α-Al₂O₃	SBS二次生长	25	2.57	1.28	1.76	2011	[114]
α-Al₂O₃中空陶瓷纤维(HCFs)	种子二次生长	13	0.125	1.24	2.27	2012	[123]
不锈钢网	原位生长	—	1.75	0.64	1.09	2012	[140]
阳极氧化铝(AAO)	种子二次生长	50	0.6	1.4	1.6	2013	[113]
氢氧化铜纳米链(CHNs)	种子二次生长法	30	11.2	1.32	1.71	2013	[198]
氢氧化铜纳米链 (CHNs)	种子生长法	5	6.32	1.32	1.68	2013	[128]
α-Al₂O₃	二次生长法	12.5	0.04	1.7	1.2	2013	[111]
α-Al₂O₃	反扩散法	—	0.249 (2 h)	1.23	1.22	2013	[192]
		—	0.00831 (4 h)	1.16	0.155
		40	0.00059 (6 h)	0.804	0.024
氢氧化铜纳米链(CHNs)	种子生长法	2.5	7.4(立方体)	—	1.67(立方体)	2014	[142]
		5	6.4(立方八面体)	—	1.67(立方八面体)
		5	5.6(八面体)	—	1.64(八面体)
多孔泡沫镍	纳米微结构辅助定向可控制备法	20	7.32	1.39	1.61	2016	[107]
		50	6.10	1.42	1.99
		70	3.00	1.38	1.9
		100	2.08	1.35	2
SiO₂	原位生长	—	0.198	1.08	1.17	2018	[110]
Al₂O₃	原位生长	72	7.42	1.27	1.92	2020	[131]

基底	方法	膜厚度/μm	渗透率/ (10^–7 mol•m^–2•s^–1•Pa^–1)	CO₂/N₂理想选择性	年份	参考文献
铜网	水热法	—	2.81	1	2009	[120]
α-Al₂O₃	种子二次生长	25	5	0.64	2010	[115]
α-Al₂O₃	SBS二次生长	25	1.48	0.73	2011	[114]
α-Al₂O₃中空陶瓷纤维(HCFs)	种子二次生长	13	0.055	0.54	2012	[123]
多孔六钛酸钾圆盘	原位溶剂热生长	25~30	4.118	0.76	2012	[211]
不锈钢网	原位生长	—	1.6	0.59	2012	[140]
氢氧化铜纳米链(CHNs)	种子二次生长法	30	6.54	0.77	2013	[198]
氢氧化铜纳米链(CHNs)	种子二次生长法	5	3.76	0.79	2013	[128]
α-Al₂O₃	二次生长法	12.5	0.033	1.42	2013	[111]
α-Al₂O₃	反扩散法	—	0.204 (2 h)	1	2013	[192]
		—	0.0536 (4 h)	7.49
		40	0.0245 (6 h)	33.33
聚偏氟乙烯(PVDF)中空纤维	压力辅助室温生长	6.5	4.79	0.79	2014	[124]
PVDF中空纤维	原位生长	43	11.58	0.8	2015	[125]
多孔泡沫镍	纳米微结构辅助定向可控制备法	≈20	4.54	0.86	2016	[107]
		≈50	3.07	0.712
		70	1.58	0.728
		100	1.04	0.675
不锈钢网	原位生长	—	0.765	0.57	2017	[119]
SiO₂	原位生长	—	0.169	0.92	2018	]110]
Al₂O₃	原位生长	72	3.87	0.66	2020	[131]
纳米多孔聚合物(np-PET)	液相外延(LPE)生长	—	0.285	13.2	2020	[173]

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金属-有机框架HKUST-1膜在气体分离中研究进展※

Research Progresses of Metal-organic Framework HKUST-1-Based Membranes in Gas Separations※

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Fig. & Tab. 28

References 221

Related Articles 15

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金属-有机框架HKUST-1膜在气体分离中研究进展^※

Research Progresses of Metal-organic Framework HKUST-1-Based Membranes in Gas Separations^※