金属-有机框架HKUST-1膜在气体分离中研究进展※

doi:10.6023/A21120545

化学学报 ›› 2022, Vol. 80 ›› Issue (3): 340-358.DOI: 10.6023/A21120545 上一篇下一篇

所属专题：中国科学院青年创新促进会合辑

综述

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)

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摘要/Abstract

发展高效、绿色且节能的物质分离与纯化技术具有重要意义, 气体分离更是在工业、能源、医疗及科技等领域有着广泛的应用. 传统的聚合物膜在实现高效气体分离方面还面临许多挑战, 新型分离膜材料的开发是当前研究热点和难点. 金属-有机框架(Metal-Organic Frameworks, MOFs)材料作为一种新兴多孔配位聚合物, 由于其具有独特可设计的拓扑结构以及可调节的功能而受到科学家们的广泛关注. 为了克服粉体或块体MOFs很难被高效用于气体分离的难题, 开发可用于分离的MOFs膜材料是一项具有重要意义且具有挑战性的任务. HKUST-1作为一种代表性的MOFs材料, 由于其结构稳定且原料经济并具有多级孔径的结构, 常被用作制备成膜材料用于气体分离的研究和实际应用. 总结了近十年HKUST-1膜的制备方法及其气体分离性能的研究进展, 并对这个方向的研究提出了自己的看法和展望.

关键词: 金属-有机框架, HKUST-1膜, 合成方法, 气体分离

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

引用此文

李崇, 李娜, 常立美, 谷志刚, 张健. 金属-有机框架HKUST-1膜在气体分离中研究进展^※[J]. 化学学报, 2022, 80(3): 340-358.

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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图/表 28

图1. (a) HKUST-1的四羧酸双铜(II)结构、(b)沿[100]方向观察[显示直径为0.9 nm(黄色球)的主通道和直径为0.5 nm(蓝色球)的侧孔]和(c)沿[011]方向观察[显示侧通道的直径为0.35 nm(红色球)的三角形窗口]的HKUST-1的晶体结构

Figure 1. (a) Dicopper(II) tetracarboxylate building block for HKUST-1, the crystal structure of HKUST-1 viewed along (b) the [100] direction [showing the main channels of 0.9 nm in diameter (yellow ball) and the tetrahedron side pockets of 0.5 nm in diameter (blue ball)] and (c) the [011] direction [showing the triangular windows of 0.35 nm in diameter (red ball) connecting the main channels and the side pockets]

图2. (a)纯HKUST-1膜制备过程示意图及(b)不锈钢网/PMMA-PMAA支撑的HKUST-1膜制备过程示意图[140]

Figure 2. (a) Schematic illustration of the preparation procedure for the free-standing HKUST-1 membrane and (b) illustration of the stainless steel net/PMMA-PMAA-supported HKUST-1 membrane preparation procedure[140]

图3. (a) CuBTC@PSF复合膜的原位结晶和逐层沉积晶体的合成方案示意图、CuBTC@PSF复合膜(b)正面和(c)截面的扫描电子显微镜(SEM)图、(d)气体H2、C3H6和CO2在室温和60 ℃下通过原始PSF膜、ZIF-8@PSF复合膜和CuBTC@PSF复合膜的气体渗透分析图以及(e)在室温和60 ℃下, ZIF-8@PSF和CuBTC@PSF对H2/C3H6和H2/CO2的选择性变化百分比[141]

Figure 3. (a) Synthesis scheme for the CuBTC@PSF composite membranes by in situ crystallization and layer by layer deposition of crystals, scanning electron microscope (SEM) images of the CuBTC@PSF composite membranes (b) top view and (c) cross section view, (d) gas permeation analysis at room temperature and 60 ℃ for gases H2, C3H6 and CO2 through the pristine PSF membrane, ZIF-8@PSF composite membranes and CuBTC@PSF composite membranes, and (e) selectivity change for H2/C3H6 and H2/CO2 through ZIF-8@PSF and CuBTC@PSF over the pristine PSF support[141]

图4. (a)快速热沉积(RTD)技术的示意图、RTD合成的HKUST-1膜的扫描电镜图的(b)俯视图和(c)横截面图以及(d)通过RTD和二次生长法制备的HKUST-1膜的单一气体渗透率比较[116]

Figure 4. (a) Schematic illustration of rapid thermal deposition (RTD) technique, scanning electron micrographs of HKUST-1 membrane synthesized by RTD (b) top view and (c) cross-sectional view, and (d) comparison of single gas permeances of HKUST-1 membranes by RTD and secondary growth[116]

图5. 不同晶型[(a)立方、(b)立方八面体、(c)八面体]HKUST-1晶体膜的室温生长过程、分别使用(d)柠檬酸盐溶液与CHN薄膜和(e) CFAuNP/CHN复合薄膜制备HKUST-1立方体膜的过程[142]

Figure 5. Growth process of (a) cube, (b) cuboctahedron and (c) octahedron HKUST-1 crystal at room temperature, and preparation processes of HKUST-1 cube membranes using (d) citrate solution and CHN thin film and (e) CFAuNP (citrate-functionalized Au nanoparticle)/CHN composite thin film[142]

图6. (a) HKUST-1沿?100?投影的单元格、(b)包含6个方形窗口[001]面(c)和8个三角形窗口[111]面(d)的立方八面体生长单元、分别通过(e)立方体(f)立方八面体和(g)八面体HKUST-1膜的CO2/SF6的二元气体分离系数曲线[142]

Figure 6. (a) Unit cell of HKUST-1 projected along ?100?, (b) the cuboctahedron growth unit that contains (c) 6 square-window [001] facets and (d) 8 triangle-window [111] facets, and binary gas separation factor curves of CO2/SF6 through (e) cube, (f) cuboctahedron and (g) octahedron HKUST-1 membranes, respectively[142]

图7. (a) HKUST-1粉末和HKUST-1膜的制备过程示意图、(b)制备的HKUST-1膜在不同跨膜压降下的气体渗透率及气体渗透率与分子质量平方根倒数之间的关系以及(c) H2/CO2、H2/N2和H2/CH4二元气体通过所制备的HKUST-1膜的分离因子图[112]

Figure 7. (a) Preparation process of HKUST-1 powders and HKUST-1 membranes, (b) gas permeance through the activated HKUST-1 membrane at different trans-membrane pressure drops and the relationship between gas permeances and the reciprocal of the square root of the molecular masses, and (c) plot of H2/CO2, H2/N2 and H2/CH4 binary gases separation factors through the as-prepared HKUST-1 membrane[112]

图8. 在不锈钢网上制备HKUST-1膜的流程示意图[119]

Figure 8. Schematic diagram of the process of preparing HKUST-1 membrane on stainless steel mesh[119]

图9. (a) HKUST-1膜的制备过程示意图和(b, c)制备的HKUST-1膜的SEM图[110]

Figure 9. (a) The process of preparing MOF membranes and (b, c) SEM images of HKUST-1 films prepared[110]

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

表1. 298 K和0.1 MPa下单组分气体和混合组分气体通过改性多孔SiO2盘载HKUST-1膜渗透流动的分离系数[110]

Table 1. Permeable flow of the single component gas and mixed component gas through the modified porous SiO2 disk-supported HKUST-1 membrane and the separation factors in 298 K and 0.1 MPa[110]

图10. (a) HKUST-1膜的制备示意图、PIM-1-COOH/HKUST-1膜的(b)正面和(c)截面SEM图以及(d)常温常压下, 单组分气体透过PIM-1-COOH/HKUST-1膜的渗透通量与相应的动力学直径之间的关系图[131]

Figure 10. (a) Schematic illustration of the HKUST-1 membrane preparation, (b) top and (c) cross-section SEM view of PIM-1-COOH/HKUST-1, and (d) single gas permeance of various gases through the PIM-1-COOH/HKUST-1 membrane at room temperature and atmospheric pressure as a function of their kinetic diameter[131]

图11. (a)热播种法和二次生长法合成HKUST-1膜的工艺示意图、(b) HKUST-1膜的SEM图像及不同温度下各种气体的(c)渗透性和(d)理想选择性[115]

Figure 11. (a) Schematic illustration of the synthesis procedure of HKUST-1 membranes by the thermal seeding and the secondary growth methods, (b) SEM images of HKUST-1 membranes, and (c) permeance values and (d) ideal selectivity for various gas molecules as functions of temperature[115]

图12. (a)在氧化铝载体上逐步沉积BTC3–和Cu2+的示意图以及制备的HKUST-1膜的(b)表面和(c)横截面的SEM图[114]

Figure 12. (a) Schematic diagram of step-by-step deposition of BTC3– and Cu2+ on alumina support, and (b) surface and (c) the cross SEM of HKUST-1 membranes[114]

	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

表2. HKUST-1膜在25 ℃时的单组分气体和双组分混合气体渗透率、H2理想选择性和分离系数[114]

Table 2. Single and mixture component permeances and H2 ideal selectivity and binary separation factor of HKUST-1 membrane at 25 ℃[114]

图13. (a)热播种和(b)热喷播种方法示意图、Cu3(BTC)2膜的FE-SEM图像的(c)俯视图和(d)横截面图及(e)各种气体的渗透性与温度的关系图[111]

Figure 13. FE-SEM images of seeded supports: (a) thermal seeding, and (b) thermal spray seeding, (c) top view and (d) cross-sectional view of FE-SEM images of Cu3(BTC)2 membrane, and (e) permeance data of various gases as a function of temperature[111]

图14. (a)分布喷雾法示意图、(b)在镀金硅晶片(2 cm×2 cm)上喷涂HKUST-1薄膜时喷嘴的照片、(c) HKUST-1的晶体结构(显示了3D MOF 结构的1 nm孔)、(d)在室温下研究的膜的H2(黑色)和CO2(红色)的混合气体渗透率以及相应的分离因子(柱)及(e)喷涂的HKUST-1薄膜(100、125和150次循环)与目前的Robeson上限的关系[171]

Figure 14. (a) Schematic diagram of distributed spray method, (b) photograph of the nozzles during the spraying process of HKUST-1 films on a gold-coated Si-Wafer (2 cm×2 cm), (c) crystal structure of HKUST-1 (showing the 1 nm pores of the 3DMOF structure), (d) mixed gas permeances of H2 (black) and CO2 (red) as well as the corresponding separation factors (columns) for the membranes under study at room temperature, and (e) sprayed HKUST-1 thin films (100, 125 and 150 cycles) in relation to the present Robeson upper bound[171]

图15. HKUST-1薄膜在高真空室中生长的示意图[172]

Figure 15. Schematic diagram of HKUST-1 film growth in a high vacuum chamber[172]

图16. (a)在聚合物膜中形成纳米孔道和在其表面和孔道内制备HKUST-1 膜的示意图、(b) 使用LPE 方法在纳米孔聚合物中制造MOF的图示及(c) CO2相对于其他气体在HKUST-1/np-PET上的渗透性和理想选择性[173]

Figure 16. (a) Schematic illustration of the formation of nanochannels in the polymer membrane and subsequent confinement of the porous HKUST-1, (b) graphical presentation of MOF fabrication in nanopore polymer using LPE approach and (c) permeance and ideal selectivity of CO2 compared to other gases on HKUST-1/np-PET[173]

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

表3. 制备的 HKUST-1/聚合物MMMs的气体分离特性[184]

Table 3. Gas-separation properties of the prepared HKUST-1/polyimide MMMs[184]

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

表4. 混合基质膜和纯聚合物膜在35 ℃, CO2/N2 (V:V=20/80)混合物进料压力100 kPa下的气体分离性能a[185]

Table 4. Gas separation performance of the mixed-matrix membranes and pure polymer under the 100 kPa of CO2/N2 mixture (V:V=20/80) as the feed pressure at 35 ℃[185]

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

表5. 纯ODPA-TMPDA和6FDA-TMPDA膜以及含有HKUST-1纳米晶体的MMMs的C2H4/C2H6分离性能a[186]

Table 5. C2H4/C2H6 separation performance of pure ODPA-TMPDA and 6FDA-TMPDA membranes together with nanocrystal HKUST-1- containing mixed-matrix membranes[186]

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

表6. 500 kPa和35 ℃下的纯气体渗透率和理想选择性[187]

Table 6. Pure gas permeability and ideal selectivity at 500 kPa and 35 ℃[187]

膜	渗透性^a/Barrer			混合气体选择性
膜	He	CH₄	N₂	He/CH₄	He/N₂
纯聚酰亚胺	22.7	0.19	0.23	119.4	98.7
10% Cu-BTC-R	35.8	0.19	0.25	188.4	143.2
20% Cu-BTC-R	50.2	0.21	0.26	239	193.1
30% Cu-BTC-R	55.2	0.2	0.29	276	190.3
40% Cu-BTC-R	64.3	0.19	0.26	338.4	247.3
45% Cu-BTC-R	70.4	0.38	0.35	185.2	201.1
5% Cu-BTC-N	25.7	0.21	0.25	122.3	102.8
10% Cu-BTC-N	30.5	0.32	0.35	95.3	87.1
15% Cu-BTC-N	37.5	0.56	0.51	66.7	73.5

表7. 500 kPa和35 ℃下的混合气体渗透率和选择性[187]

Table 7. Mixed gas measurements at 500 kPa and 35 ℃[187]

图17. 在500 kPa进料压力和35 ℃下含有(a)针状颗粒和(b)尺寸减小的颗粒的MMM的纯气体测量值[He渗透性(Barrer)、He/CH4和He/N2理想选择性]、包含质量分数为40%的Cu-BTC-R的MMM对二元气体混合物(c) He/N2 (V:V=1:1)和(d) He/CH4 (V:V=1:1)进行长达120 h的长期稳定性测试[187]

Figure 17. Pure gas measurements (He permeability in Barrer, He/CH4 and He/N2 ideal selectivity) of MMMs containing (a) needle particles and (b) size-reduced particles, and the long-term stability test of the MMM comprising 40% Cu-BTC-R up to 120 h for binary gas mixtures (c) He/N2 (V:V=1:1) and (d) He/CH4 (V:V=1:1) at 500 kPa feed pressure and 35 ℃[187]

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		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]

表8. 文献中报道的HKUST-1膜对氢气的分离性能总结

Table 8. Summary of the separation performance of HKUST-1 membrane for hydrogen reported in the literature

表8. 文献中报道的HKUST-1膜对氢气的分离性能总结

Table 8. Summary of the separation performance of HKUST-1 membrane for hydrogen reported in the literature

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]

表9. 文献中报道的HKUST-1膜对CH4的分离性能总结

Table 9. Summary of the separation performance of HKUST-1 membrane for CH4 reported in the literature

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]

表10. 文献中报道的HKUST-1膜对CO2的分离性能总结

Table 10. Summary of the separation performance of HKUST-1 membrane for CO2 reported in the literature

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)	He/N₂	He/CO₂	He/CH₄	年份	参考文献
多孔六钛酸钾圆盘	原位溶剂热生长	25~30	14	2.6	3.4	2.07	2012	[211]
α-Al₂O₃	反扩散法	—	0.746 (2 h)	3.67	3.66	2.99	2013	[192]
		—	0.169 (4 h)	23.64	3.16	20.33
		40	0.0767 (6 h)	109.8	3.29	136.6
聚酰亚胺	混合基质膜(MMMs)	30	2.224×10^–7	98.6	—	131.1	2020	[187]

表11. 文献中报道的HKUST-1膜对氦气的渗透性和分离性能总结

Table 11. Summary of the permeability and separation performance of HKUST-1 membrane for Helium reported in the literature

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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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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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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^※