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

doi:10.6023/A20100494

化学学报 ›› 2021, Vol. 79 ›› Issue (4): 459-471.DOI: 10.6023/A20100494 上一篇下一篇

综述

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)

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摘要/Abstract

精细化分离是石油化工生产的关键技术及研究热点之一, 其中C₂ (C₂H₂/C₂H₄和C₂H₄/C₂H₆)的高效精细分离更是现代化工过程中高质量生产的难点和新挑战. 传统的热驱动分离过程(如精馏分离和选择性催化加氢分离)存在能耗高、经济效益低的缺陷, 而采用非热驱动分离过程(如吸附分离和膜分离)可大幅度节能降耗. 在众多吸附分离材料中, 金属有机骨架(MOF)材料拥有庞大的组分/结构单元库, 其组成和孔结构的可控、可调特性为C₂的精细化高效分离带来了新的机遇. 以此为导向, 整理并归纳了近年来MOF⁺材料(MOF及其复合材料)的晶体和孔道参数, 分析其在高效分离C₂方面的科学研究成果, 针对MOF⁺材料的设计、可控制备、孔径调控机制等关键科学问题, 提出了未来MOF⁺材料的研究趋势.

关键词: 金属有机骨架材料, 复合材料, 孔径, C₂H₂/C₂H₄分离, C₂H₄/C₂H₆分离, 选择性

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

引用此文

李旭飞, 闫保有, 黄维秋, 浮历沛, 孙宪航, 吕爱华. 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[J]. 化学学报, 2021, 79(4): 459-471.

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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图/表 21

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

表1. C2分子的物理性质

Table 1. The physical properties of C2 molecules

图1. 三种吸附分离方式示意图[20]

Figure 1. Schematic diagrams of three adsorptive separation strategies[20]

图2. 吸附质分子与吸附剂孔径间关系模型图

Figure 2. Relationship model between adsorbate molecular and adsorbent pore size

图3. 代表性MOF材料的三维结构[45⇓-47,50-51]

Figure 3. Three-dimensional (3D) structures of representative MOFs[45⇓-47,50-51]

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

表2. 不同阴离子与C2H2和C2H4的键能及键能差[48-49]

Table 2. Bond energies and their differences of different anions with C2H2 and C2H4[48-49]

图4. (a) UTSA-200a分离C2H2和C2H4的示意图, (b) SIFSIX材料的穿透曲线和配体对比[52]

Figure 4. (a) Schematic diagrams of UTSA-200a for separating C2H2 and C2H4, (b) comparisons of breakthrough curves and linkers for SIFSIXs[52]

图5. (a) ZU-32和ZU-33的孔径和三维结构, (b)不同MOF材料对C2H2的吸附量和选择性对比[53]

Figure 5. (a) Pore sizes and 3D structures of ZU-32 and ZU-33, (b) comparisons of adsorption capacities and selectivities on different MOFs for C2H2[53]

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]

表3. 用于C2H2/C2H4分离的代表性刚性MOF材料的结构参数

Table 3. Structure parameters of representative rigid MOFs for the separation of C2H2/C2H4

图6. ELM-11 (a和b)和ELM-13 (c和d)在273和298 K时的C2H2和C2H4吸附等温线对比[60]

Figure 6. Comparisons of adsorption isotherms for C2H2 and C2H4 on ELM-11 (a and b) and ELM-13 (c and d) at 273 and 298 K[60]

图7. NTU-65在不同温度时的CO2、C2H2和C2H4吸附等温线对比[61]

Figure 7. Comparisons of adsorption isotherms for CO2, C2H2 and C2H4 on NTU-65 at different temperatures[61]

图8. (a) UTSA-300a和NCU-100a的三维结构及其(b)对C2H2和C2H4的吸附等温线对比[62-63]

Figure 8. (a) 3D structures of UTSA-300a and NCU-100a and (b) their comparisons of adsorption isotherms for C2H2 and C2H4[62-63]

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]

表4. 用于C2H2/C2H4分离的代表性柔性MOF材料的结构参数

Table 4. Structure parameters of representative flexible MOFs for the separation of C2H2/C2H4

图9. M-gallate的(a)三维结构和(b)分离示意图, (c)成型的Mg-gallate, (d) Co-gallate在298 K时的C2H2和C2H4吸附等温线[68]

Figure 9. (a) 3D structures and (b) separation schematic diagram of M-gallate, (c) shaped Mg-gallate, (d) adsorption isotherms for C2H2 and C2H4 on Co-gallate at 298 K[68]

图10. (a) UTSA-280材料的三维结构, (b)刚性C4O42–的示意图, (c) UTSA-280吸附C2H4的侧视图, (d)基于C2H4和C2H6分子最小横截面积的尺寸/形状筛分示意图, (e) UTSA-280在298 K时C2H4和C2H6的吸附等温线, (f)不同MOF材料对C2H4/C2H6的选择性对比[69]

Figure 10. (a) 3D structure of UTSA-280, (b) schematic diagram of rigid C4O42–, (c) side view of the packing diagram of UTSA-280 adsorbed C2H4, (d) schematic diagram of the size/shape sieving based on the minimum cross-sectional areas of C2H4 and C2H6 molecules, (e) adsorption isotherms for C2H4 and C2H6 on USTA-280 at 298 K, (f) comparisons of adsorption selectivities for C2H4/C2H6 on different MOFs[69]

图11. (a) UTSA-280材料的脱水及氨吸附改性后的结构变化示意图, (b) UTSA-280、UTSA-280-M1、UTSA-280-M2材料在298 K的C2H4(实心点)和C2H6(空心点)吸附等温线[70]

Figure 11. (a) Schematic diagrams of structure changes on UTSA-280 caused by H2O removal and NH3 modified, (b) adsorption isotherms for C2H4 (solid points) and C2H6 (hollow points) on UTSA-280, UTSA-280-M1 and UTSA-280-M2 at 298 K[70]

图12. 代表性MOF材料的三维结构: (a) Fe2(O2)(dobdc), (b) MUF-15, (c) MAF-49和(d) JNU-2[2,7,71-72]

Figure 12. 3D structures of representative MOFs: (a) Fe2(O2)(dobdc), (b) MUF-15, (c) MAF-49 and (d) JNU-2[2,7,71-72]

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]

表5. 用于C2H4/C2H6分离的代表性MOF材料的结构参数

Table 5. Structure parameters of representative MOFs for the separation of C2H4/C2H6

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]

表6. 部分ZIF材料的组成和结构参数

Table 6. Compositions and structure parameters of partial ZIFs

图13. (a) ZIF-8混合基质膜的断面及其(b)对C2H4和C2H6的渗透性和选择性[78]

Figure 13. (a) Cross section of ZIF-8 MMM and (b) its permeances and selectivities for C2H4 and C2H6[78]

图14. (a) SIFSIX-2-Cu-i/PIL混合基质膜示意图及其(b)对C2H2的渗透性和选择性[81]

Figure 14. (a) Schematic diagram of SIFSIX-2 Cu-i/PIL MMMs and (b) their permeances and selectivities for C2H2[81]

图15. 协同吸附分离技术[82]

Figure 15. Synergistic sorbent separation technology (SSST)[82]

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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

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

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