Research Progress in Metal-Organic Framework and Its Composites for Separation of C2 Based on Sieving Multiple Effects

doi:10.6023/A20100494

Acta Chimica Sinica ›› 2021, Vol. 79 ›› Issue (4): 459-471.DOI: 10.6023/A20100494 Previous Articles Next Articles

Review

金属有机骨架及其复合材料基于筛分复合效应的C₂分离的研究进展

李旭飞^a^,^b, 闫保有^b, 黄维秋^a^,^b^,^*(), 浮历沛^b, 孙宪航^b, 吕爱华^b

a 常州大学材料科学与工程学院常州 213164
b 常州大学油气储运技术省重点实验室常州 213164

投稿日期:2020-10-27 发布日期:2020-12-11
通讯作者: 黄维秋

作者简介:

李旭飞, 男, 常州大学材料科学与工程学院在读博士研究生, 目前在常州大学油气回收工程技术研究中心参与重点研发项目, 主要从事MOF及其复合材料的设计、制备及吸附分离应用.

闫保有, 男, 常州大学石油工程学院在读硕士研究生, 目前在常州大学油气回收工程技术研究中心参与重点研发项目, 主要从事MOF材料的合成及其在有机废气治理中应用.

黄维秋, 男, 常州大学石油工程学院教授, 博士生导师, 江苏省“油气回收基础理论及其应用”科技创新团队带头人, 江苏省“333工程”中青年科技领军人才, 江苏省有机废气资源化工程技术中心主任. 30多年来, 组建省级团队在国内率先并长期开展以“油气回收”为代表的有机废气污染控制及资源化的基础研究及技术开发取得丰富工作积累及系列创新成果, 并成功实现产业化. 目前主要研究方向: 油气回收基础理论及应用、石油储存工艺和新型纳米功能材料及其在有机废气治理中应用.

浮历沛, 男, 博士, 江苏省高层次创新创业人才引进计划“科技副总”, 任教于常州大学石油工程学院. 近年来, 主持国家自然科学基金青年基金项目1项, 参与多项国家级项目研究, 发表论文多篇. 目前主要研究方向: 储运环保技术、新型功能材料开发及应用.

孙宪航, 男, 博士, 任教于常州大学石油工程学院. 参与多项国家级项目研究, 发表论文多篇. 目前主要研究方向: 油气回收技术, 活性炭脱附研究.

吕爱华, 女, 南京工业大学在读博士研究生, 任教于常州大学石油工程学院. 参与多项国家级项目研究, 发表论文多篇. 目前主要研究方向: 多孔介质传热传质及油气回收环保技术.

基金资助:
国家自然科学基金(51574044); 国家自然科学基金(51804045); 江苏省重点研发计划(产业前瞻与共性关键技术)(BE2018065)

Research Progress in Metal-Organic Framework and Its Composites for Separation of C₂ Based on Sieving Multiple Effects

Xufei Li^a^,^b, Baoyou Yan^b, Weiqiu Huang^a^,^b^,^*(), Lipei Fu^b, Xianhang Sun^b, Aihua Lv^b

a College of Materials Science & Engineering, Changzhou University, Changzhou 213164, China
b Jiangsu Provincial Key Laboratory of Oil & Gas Storage and Transportation Technology, Changzhou University, Changzhou 213164, China

Received:2020-10-27 Published:2020-12-11
Contact: Weiqiu Huang
About author:
* E-mail: hwq213@cczu.edu.cn
Supported by:
National Natural Science Foundation of China(51574044); National Natural Science Foundation of China(51804045); and the Key Research and Development Program of Jiangsu Province (Industry Foresight and Common Key Technology)(BE2018065)

Fine separation of mixture is the primary importance technology and hot topic in the petrochemical industry. In particular, high-efficiency separation of C₂ (C₂H₂/C₂H₄ and C₂H₄/C₂H₆) is a difficult issue and challenge of the high-quality production in modern chemical process. Traditional heat-driven separation processes (e.g., fine distillation separation and selective catalytic hydrogenation separation) have the shortages of high energy consumption and low economic benefits. On the contrary, the processes with non-thermal driven separations (e.g., adsorptive and membrane-based separations) can greatly overcome these weaknesses. Among these adsorptive separation materials, metal-organic framework (MOF) materials own a huge various library of components/structure units. Their characters of controllable pore structures and adjustable compositions will bring about new opportunities for the high-efficiency refined separations. In this context, the crystals and pore parameters of MOF⁺ (MOF and its composites) materials in recent years were sorted out and summarized, the researches in the high-efficiency separation of MOF⁺ materials for C₂ were analyzed, and the key issues of the design, controllable preparation, and pore size control mechanism for MOF⁺ materials were focused on. In addition, the future research trend of MOF⁺ materials were also put forward.

Key words: metal-organic framework material, composite, pore size, C₂H₂/C₂H₄ separation, C₂H₄/C₂H₆ separation, selectivity

Cite this article

Xufei Li, Baoyou Yan, Weiqiu Huang, Lipei Fu, Xianhang Sun, Aihua Lv. Research Progress in Metal-Organic Framework and Its Composites for Separation of C₂ Based on Sieving Multiple Effects[J]. Acta Chimica Sinica, 2021, 79(4): 459-471.

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C₂的结构示意图

分子	动力学直径/nm	沸点/K	分子尺寸/nm
分子	动力学直径/nm	沸点/K	X	Y	Z
C₂H₂	0.330	189	0.332	0.334	0.570
C₂H₄	0.416	169	0.328	0.418	0.484
C₂H₆	0.444	185	0.381	0.408	0.482

C₂的结构示意图

分子	动力学直径/nm	沸点/K	分子尺寸/nm
分子	动力学直径/nm	沸点/K	X	Y	Z
C₂H₂	0.330	189	0.332	0.334	0.570
C₂H₄	0.416	169	0.328	0.418	0.484
C₂H₆	0.444	185	0.381	0.408	0.482

阴离子	键能△E/(kJ•mol^–1)		键能差/(kJ•mol^–1)
阴离子	C₂H₂	C₂H₄	键能差/(kJ•mol^–1)
B₁₂H₁₂^2–	–40.2	–25.6	14.6
Cl^–	–39.5	–27.8	11.7
Br^–	–37.4	–30.4	7.0
SiF₆^2–	–52.9	–39.8	13.1
BF₄^–	–31.5	–25.1	6.4
Tf₂N^–	–23.5	–17.1	6.4

阴离子	键能△E/(kJ•mol^–1)		键能差/(kJ•mol^–1)
阴离子	C₂H₂	C₂H₄	键能差/(kJ•mol^–1)
B₁₂H₁₂^2–	–40.2	–25.6	14.6
Cl^–	–39.5	–27.8	11.7
Br^–	–37.4	–30.4	7.0
SiF₆^2–	–52.9	–39.8	13.1
BF₄^–	–31.5	–25.1	6.4
Tf₂N^–	–23.5	–17.1	6.4

MOF	材料孔径/ (nm×nm)	BET/ (m²•g^–1)	C₂H₂吸附量/ (mmol•g^–1)	C₂H₄吸附量/ (mmol•g^–1)	温度/ K	IAST选择性 (1∶99)	C₂H₄纯度/ %	穿透时间^b/ (min•g^–1)	参考文献
M’MOF-3a	0.34×0.48	110	1.90	0.40	295	5	—	—	^[45]
Mn(Ⅱ)-Mn(Ⅲ)	0.55×0.40	362^a	3.20	0.24	283	16	—	18^c	^[46]
UTSA-100a	0.43×0.43	970	4.27	1.66	296	11	—	17	^[47]
SIFSIX-3-Zn	0.42×0.42	250	3.64	2.24	298	9	99.998	100	^[50]
SIFSIX-3-Ni	0.42×0.42	368	3.30	1.75	298	5	99.998	—	^[50]
SIFSIX-2-Cu-i	0.52×0.52	503	4.02	2.19	298	55	99.998	800	^[50]
SIFSIX-1-Cu	0.80×0.80	1178	8.50	4.11	298	11	99.998	600	^[50]
UTSA-220	0.30×0.32 0.40×0.65	577	3.40	2.53	298	10	99.9999	125	^[51]
UTSA-200a	0.34×0.34	612	3.65	0.63	298	6320	99.9999	1500	^[52]
ZU-32	0.35×0.35	467	3.97	2.19	298	67	99.999	800	^[53]
ZU-33	0.33×0.33	424	3.78	0.70	298	1100	99.9999	1600	^[53]

金属有机骨架及其复合材料基于筛分复合效应的C₂分离的研究进展

Research Progress in Metal-Organic Framework and Its Composites for Separation of C₂ Based on Sieving Multiple Effects

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References 89

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MOF	材料孔径/ (nm×nm)	BET/ (m²•g^–1)	C₂H₂吸附量/ (mmol•g^–1)	C₂H₄吸附量/ (mmol•g^–1)	温度/ K	IAST选择性 (1∶99)	C₂H₄纯度/%	穿透时间/ (min•g^–1)	参考文献
ELM-11	—	—	3.5	0.06	298	60^a	—	9^a	[60]
ELM-13	—	—	3.0	0.18	298	10000^a	—	6	[60]
NTU-65	0.26×0.34 0.52×0.63	680	3.36	0.05	298	—	99.95	85	[61]
UTSA-300a	0.35×0.39	311	3.08	0.04	298	75^b	99.9	12^b	[62]
NCU-100a	0.36×0.43	358	4.57	0.32	298	7291	99.9995	167	[63]

分离方式	MOF	材料孔径/ (nm×nm)	BET/ (m²•g^–1)	C₂H₄吸附量/ (mmol•g^–1)	C₂H₆吸附量/ (mmol•g^–1)	温度/ K	IAST选择性 (50∶50)	C₂H₄纯度/%	穿透时间/ (min•g^–1)	参考文献
C₂H₄选择性吸附筛分	Ni-gallate	0.347×0.485	424	2.00	0.28	298	16.8	—	83	[68]
	Mg-gallate	0.356×0.484	559	3.00	0.26	298	37.3	—	162	[68]
	Co-gallate	0.369×0.495	475	3.37	0.31	298	52.0	—	138	[68]
	UTSA-280	0.380×0.380 0.320×0.450	331	2.50	0.10	298	>10⁴	—	30	[69]
	UTSA-280-M1	—	—	2.20	0.05	298	1100	—	35	[70]
	UTSA-280-M2	—	—	2.83	0.05	298	1200	—	50	[70]
C₂H₆选择性吸附筛分	Fe₂(O₂)(dobdc)	—	1073	2.63	3.32	298	4.4	99.99	15	[2]
	MUF-15	0.850×0.350 0.700×0.380 0.320×0.120	1130	4.15	4.69	293	2.0	99.95	20	[71]
	MAF-49	0.330×0.300	—	1.65	1.70	316	2.7	99.986	170	[7]
	NJU-2	0.420×0.420 0.720×0.720 0.920×0.920 0.370×0.370	1219	3.62	4.19	298	1.6	99.99	100	[72]

ZIF	组成	BET/(m²•g^–1)	孔径/nm	笼径/nm	参考文献
ZIF-65	Co(nIm)₂	760	3.4	10.4	[77]
ZIF-67	Co(mIm)₂	1280	3.4	11.6	[77]
ZIF-71	Zn(dcIm)₂	827	4.2	16.5	[77]
ZIF-8	Zn(mIm)₂	1947	3.4	11.6	[31]
ZIF-90	Zn(Ica)₂	1270	3.5	11.2	[79]
ZIF-95	Zn(cbIm)₂	1050	3.7	24	[80]
ZIF-100	Zn₂₀(cbIm)₃₉(OH)	595	3.4	35.6	[80]

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金属有机骨架及其复合材料基于筛分复合效应的C2分离的研究进展