用于CO2捕获的金属有机框架材料改性研究进展

doi:10.16085/j.issn.1000-6613.2023-2143

摘要/Abstract

摘要：

金属有机框架材料（MOF）因其高比表面积、高选择性、结构可调性以及可再生性的优势而广泛应用于CO₂吸附与分离领域。首先对比了MOF与其他CO₂处理方式以及CO₂吸附材料的优缺点，得出MOF的独特优势。再根据MOF的结构以及化学特性，归纳了其对CO₂的物理和化学吸附机理，深入揭示了MOF作为CO₂吸附材料的基本原理。在此基础上，针对MOF在性能和结构上仍然存在且需要改进的缺陷，通过对比不同种类MOF的性能，对MOF的功能化改性（多金属掺杂、多材料复合、构建缺陷、胺功能化、极性基团功能化等），以及改性后MOF的CO₂吸附性能的研究进展进行了归纳。通过对这些改性方式的优缺点进行评估，并考虑其适用性和经济性，旨在找到更好的MOF改性方法。MOF改性未来的发展需要对多官能团负载、合成及负载方法绿色化、比表面积与结合位点比例等进行更深入的研究，此外改性表征方法的先进性也是未来MOF改性发展的关键要素。

关键词: 金属有机框架材料, 二氧化碳, 吸附, 选择性, 改性

Abstract:

Metal-organic frameworks (MOFs) are widely used in the field of CO₂ adsorption and separation due to their high specific surface area, high selectivity, structural tunability and renewability. Firstly, the advantages and disadvantages of MOFs and other CO₂ treatment methods and CO₂ adsorption materials were compared, and the unique advantages of MOFs were obtained. According to the structure and chemical characteristics of MOFs, the physical and chemical adsorption mechanism of CO₂ was summarized, and the basic principle of MOFs as CO₂ adsorption materials was deeply revealed. On this basis, in view of the defects that still existed in the performance and structure of MOFs and needed to be improved, the research progress of the functionalization modification of MOFs (multi-metal doping, multi-material composite, construction defects, amine functionalization, polar group functionalization, etc.) and the CO₂ adsorption performance of modified MOFs were summarized by comparing the performance of different types of MOFs. By evaluating the advantages and disadvantages of these modification methods and considering their applicability and economy, the aim was to find a better modification method for MOFs. The future development of MOFs modification required further in-depth research on the loading of multiple functional groups, greening of synthesis and loading methods and the ratio of surface area to binding sites. Additionally, the advancement of characterization methods for modifications was a key element in the future development of MOFs modification.

Key words: metal-organic framework, carbon dioxide, adsorption, selectivity, modification

中图分类号:

O647.3

肖翩翩, 卓超越, 钟瑾荣, 张跃飞. 用于CO₂捕获的金属有机框架材料改性研究进展[J]. 化工进展, 2024, 43(12): 6944-6956.

XIAO Pianpian, ZHUO Chaoyue, ZHONG Jinrong, ZHANG Yuefei. Recent advances on modification of metal-organic frameworks for CO₂ capture[J]. Chemical Industry and Engineering Progress, 2024, 43(12): 6944-6956.

图/表 8

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MOF	金属中心	比表面积/m²·g^-1	CO₂吸附容量/mmol·g^-1	压力/MPa	选择性CO₂/N₂	参考文献
MIL-53	Al	634	10.4	30	50	[18-19]
MIL-53	Mn_0.27Al_0.73	1748	11.8	30	83	[20]
MIL-53	Mn_0.5Al_0.5	1817	13.3	30	95	[20]
MIL-53	Mn_0.6Al_0.4	1576	12.8	30	45	[20]
HKUST-1	Cu	1440	3.4	1		[21]
HKUST-1	Li、Cu	1000	2.6	2		[22]
UiO-66	Zr	1455	4.3	20		[23]
MOF-74	Mg	1640	8.0	1	233	[24-26]
MOF-74	Zn_0.14Mg_0.86	1277	0.5	1		[27]
MOF-74	Zn_0.48Mg_0.52	794	2.1	1		[27]
MOF-74	Zn_0.75Mg_0.25	668	3.2	1		[27]
MOF-74	Ni	1274	5.2	1.1	11.3	[24,28]
MOF-74	Pd、Ni	1115	12.2	32	14.6	[28]
MOF-74	Co	1404	3.7	1.1	9.7	[28]
MOF-74	Pd、Co	1088	11.4	32	12.4	[28]
MOF-5	Zn	1858	0.5	1		[29]
MOF-11	Zn	2096	14.7	35		[30]
MOF-210	Zn	6240		50		[31]
Cu₃(BTC)₂	Cu	1781	10.7	35		[30]
MIL-100	Fe	1811	2.6	1	49.6	[32]
MIL-100	Al、Fe	1993	3.3	1	76.5	[32]
MIL-120	Al	3084	4.8	10		[33]
[Ni₆(OH)₄(COO)₈(H₂O)₆]	Ni	468	1.4	1		[34]
[Ni_4.1Co_1.9(OH)₄(BTB)_8/3(H₂O)₆]	Ni_4.1Co_1.9	491	1.7	1		[34]
[Ni_3.1Co_2.9(OH)₄(BTB)_8/3(H₂O)₆]	Ni_3.1Co_2.9	526	1.9	1		[34]
[Ni_2.8Co_3.2(OH)₄(BTB)_8/3(H₂O)₆]	Ni_2.8Co_3.2	819	2.3	1		[34]

MOF	金属中心	比表面积/m²·g^-1	CO₂吸附容量/mmol·g^-1	压力/MPa	选择性CO₂/N₂	参考文献
MIL-53	Al	634	10.4	30	50	[18-19]
MIL-53	Mn_0.27Al_0.73	1748	11.8	30	83	[20]
MIL-53	Mn_0.5Al_0.5	1817	13.3	30	95	[20]
MIL-53	Mn_0.6Al_0.4	1576	12.8	30	45	[20]
HKUST-1	Cu	1440	3.4	1		[21]
HKUST-1	Li、Cu	1000	2.6	2		[22]
UiO-66	Zr	1455	4.3	20		[23]
MOF-74	Mg	1640	8.0	1	233	[24-26]
MOF-74	Zn_0.14Mg_0.86	1277	0.5	1		[27]
MOF-74	Zn_0.48Mg_0.52	794	2.1	1		[27]
MOF-74	Zn_0.75Mg_0.25	668	3.2	1		[27]
MOF-74	Ni	1274	5.2	1.1	11.3	[24,28]
MOF-74	Pd、Ni	1115	12.2	32	14.6	[28]
MOF-74	Co	1404	3.7	1.1	9.7	[28]
MOF-74	Pd、Co	1088	11.4	32	12.4	[28]
MOF-5	Zn	1858	0.5	1		[29]
MOF-11	Zn	2096	14.7	35		[30]
MOF-210	Zn	6240		50		[31]
Cu₃(BTC)₂	Cu	1781	10.7	35		[30]
MIL-100	Fe	1811	2.6	1	49.6	[32]
MIL-100	Al、Fe	1993	3.3	1	76.5	[32]
MIL-120	Al	3084	4.8	10		[33]
[Ni₆(OH)₄(COO)₈(H₂O)₆]	Ni	468	1.4	1		[34]
[Ni_4.1Co_1.9(OH)₄(BTB)_8/3(H₂O)₆]	Ni_4.1Co_1.9	491	1.7	1		[34]
[Ni_3.1Co_2.9(OH)₄(BTB)_8/3(H₂O)₆]	Ni_3.1Co_2.9	526	1.9	1		[34]
[Ni_2.8Co_3.2(OH)₄(BTB)_8/3(H₂O)₆]	Ni_2.8Co_3.2	819	2.3	1		[34]

MOF	改性基团	比表面积/m²·g^-1	CO₂吸附容量/mmol·g^-1	压力/MPa	CO₂/N₂选择性	参考文献
Mg-MOF-74	TEPA		10.0			[62]
MOF-177		2000~4500	1.2	1	20	[63]
MOF-177-PEI	PEI	1145	2.8	1		[64]
MOF-177-DETA	DETA	1225	2.8	1		[64]
MOF-177-TEPA	TEPA	1380	3.8	1		[64]
MOF-808		1706	14	1	35.9	[65]
MOF-808-TEPA	TEPA	814	1.1	1	84.4	[65]
MOF-808-ED	ED	1289	1.2	1	48.4	[65]
MOF-808-DETA	DETA	20	0.7	1	52.7	[65]
CuBTTri		1770	3.7	1		[66]
Mmen-CuBTTri	Mmen	870	4.2	1	327	[66]
MIL-100		1170	1.1	0.8	12.6	[67]
MIL-100@PPD	PPD	820	4.6	10		[68]
EN@MIL-100	EN	657	0.9	0.8		[67]
MIL-101		3125	1.0	1	2.3	[69]
MIL-101@PPD	PPD	1007	7.3	10		[68]
MIL-101@PEI(50%)	PEI	1802	3.1	1	22	[69]
MIL-101@PEI(70%)	PEI	1112	4.0	1	84	[69]
MIL-101@PEI(100%)	PEI	608	4.1	1	120	[69]
NH₂-MIL-101	—NH₂	1569	3.3	1	16	[70]
MIL-53		1269	9.7	30		[71]
MIL-53@NH₃	NH₃	989	10.8	30		[71]
Mg₂(dobpdc)		3178	1.5	1		[72]
een-Mn₂(dobpdc)	een		4.25	0.15		[73]
En-Mg₂(dobpdc)	En	1253	3.6	0.15		[74]
Den-Mg₂(dobpdc)	Den	840	4.8	1		[75]
Men-Mg₂(dobpdc)	Men	1036	4.5	1		[75]
Dmen-Mg₂(dobpdc)	Dmen	675	3.8	0.15	554	[76]

MOF	改性基团	比表面积/m²·g^-1	CO₂吸附容量/mmol·g^-1	压力/MPa	CO₂/N₂选择性	参考文献
Mg-MOF-74	TEPA		10.0			[62]
MOF-177		2000~4500	1.2	1	20	[63]
MOF-177-PEI	PEI	1145	2.8	1		[64]
MOF-177-DETA	DETA	1225	2.8	1		[64]
MOF-177-TEPA	TEPA	1380	3.8	1		[64]
MOF-808		1706	14	1	35.9	[65]
MOF-808-TEPA	TEPA	814	1.1	1	84.4	[65]
MOF-808-ED	ED	1289	1.2	1	48.4	[65]
MOF-808-DETA	DETA	20	0.7	1	52.7	[65]
CuBTTri		1770	3.7	1		[66]
Mmen-CuBTTri	Mmen	870	4.2	1	327	[66]
MIL-100		1170	1.1	0.8	12.6	[67]
MIL-100@PPD	PPD	820	4.6	10		[68]
EN@MIL-100	EN	657	0.9	0.8		[67]
MIL-101		3125	1.0	1	2.3	[69]
MIL-101@PPD	PPD	1007	7.3	10		[68]
MIL-101@PEI(50%)	PEI	1802	3.1	1	22	[69]
MIL-101@PEI(70%)	PEI	1112	4.0	1	84	[69]
MIL-101@PEI(100%)	PEI	608	4.1	1	120	[69]
NH₂-MIL-101	—NH₂	1569	3.3	1	16	[70]
MIL-53		1269	9.7	30		[71]
MIL-53@NH₃	NH₃	989	10.8	30		[71]
Mg₂(dobpdc)		3178	1.5	1		[72]
een-Mn₂(dobpdc)	een		4.25	0.15		[73]
En-Mg₂(dobpdc)	En	1253	3.6	0.15		[74]
Den-Mg₂(dobpdc)	Den	840	4.8	1		[75]
Men-Mg₂(dobpdc)	Men	1036	4.5	1		[75]
Dmen-Mg₂(dobpdc)	Dmen	675	3.8	0.15	554	[76]

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用于CO₂捕获的金属有机框架材料改性研究进展

Recent advances on modification of metal-organic frameworks for CO₂ capture

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