高效分离乙烷/乙烯的烷烃选择性吸附剂研究进展

doi:10.11949/0438-1157.20220599

摘要/Abstract

摘要：

乙烯是石油化学工业的基础原材料，聚合级乙烯工业纯化的关键挑战是去除其中的乙烷杂质，这一步骤难度大、能耗高。近年来，以乙烷选择性吸附剂为核心的吸附分离纯化技术快速发展，并得到学术界和工业界的关注。该技术可在温和工况下高选择性分离出乙烯中的乙烷杂质，显现出巨大潜力。本文总结了近年来乙烷选择性吸附剂（特别是乙烷选择性MOFs）的研究进展，并归纳阐释其选择性吸附机理。同时，在前人研究成果的基础上，总结可行的乙烷选择性吸附剂的设计策略，指出当前开发高效乙烷选择性吸附剂面临的挑战和未来的研究方向。

关键词: 吸附, 分离, 选择性, 乙烷, 乙烯

Abstract:

Ethylene, the essential raw material in petroleum chemistry industry, is usually produced with ethane impurity. It is of industrial significance to separate ethane from ethylene for the production of polymerization grade ethylene. Conventional distillation operated at high pressure and low temperature suffers from intensive energy cost and crucial technical challenges. Adsorptive separation separates ethane from ethylene at mild condition, hence holds tremendous potential in industrial application. This paper reviews the most recent research progress of ethane-selective adsorbents, including metal-organic frameworks (MOFs), hydrogen-bonded organic frameworks (HOFs) and porous carbon. Moreover, the ethane-selective adsorption mechanisms are generalized and clarified in detail. In addition, the feasible design strategy of ethane-selective adsorbents is summarized, and the current challenges and future research direction are discussed.

Key words: adsorption, separation, selectivity, ethane, ethylene

中图分类号:

TQ 028.1

张博, 陈晓霏, 赵思尧, 周欣. 高效分离乙烷/乙烯的烷烃选择性吸附剂研究进展[J]. 化工学报, 2022, 73(10): 4255-4267.

Bo ZHANG, Xiaofei CHEN, Siyao ZHAO, Xin ZHOU. Progress of ethane-selective adsorbents for efficient purification of ethylene[J]. CIESC Journal, 2022, 73(10): 4255-4267.

图/表 8

参考文献 93

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乙烷选择性吸附剂	条件	乙烷吸附量/(mmol/g)	乙烯吸附量/(mmol/g)	IAST选择性	文献
UiO-67-(NH₂)₂	296 K，1 bar	5.32	4.32	1.7	[71]
CAU-3-NDCA	298 K，1 bar	2.42	1.61	1.56	[7]
MOF-841	298 K，1 bar	4.70	3.40	1.6	[72]
Ni(BODC)(TED)	298 K，1 bar	3.36	2.61	1.83^①	[73]
LIFM-63	298 K，1 bar	3.0	2.1	1.6	[8]
MIL-53-BDC	298 K，1 bar	2.93	2.78	1.70	[74]
MIL-53-NDCA	298 K，1 bar	4.24	3.12	1.53	[74]
MIL-53-BPDC	298 K，1 bar	2.97	2.07	1.47	[74]
ZJNU-115	298 K，1 atm	4.20	3.75	1.56	[75]
BUT-10	298 K，1 bar	4.76	3.56	1.72	[76]
ScBPDC	298 K，1 bar	3.42	2.41	1.7^②	[77]
ZJNU-7	298 K，1 bar	4.13	3.80	1.56	[78]
Co(AIN)₂	298 K，1 bar	3.16	3.14	2.96	[79]
FMOF-2	303 K，5 kPa	0.90	0.60	3.3^③	[47]
CPM-80-Zn	298 K，1 bar	4.77	4.24	1.8	[80]
CPM-81-Co	298 K，1 bar	5.51	5.07	1.8	[80]
SNNU-40	298 K，1 bar	7.54	4.91	1.57	[52]
MIL-125	298 K，1 bar	4.83	3.98	1.43	[81]
MUV-11	298 K，1 bar	1.83	1.72	1.53	[81]
ZSTU-2	298 K，1 bar	2.73	2.35	1.62	[81]
DMOF	298 K，1 bar	2.79^④	2.08^④	1.51	[50]
DMOF-DM	298 K，1 bar	4.03^④	3.11^④	1.70	[50]
DMOF-TM	298 K，1 bar	5.31^④	4.99^④	1.88	[50]
MOF-525	298 K，1 bar	2.77	2.10	1.24	[82]
MOF-525(Co)	298 K，1 bar	2.24^⑤	1.91^⑤	1.11	[82]
UPC-612	298 K，1 bar	3.57	2.69	1.4	[82]
UPC-613	298 K，1 bar	2.56	2.25	1.47	[82]
JXNU-9	298 K，1 atm	3.61	2.45	1.53	[83]
PCN-250(Fe₂Zn)	298 K，1 bar	5.95	5.42	1.7^①	[66]
PCN-250(Fe)	298 K，1 bar	6.00	5.00	1.6^①	[66]
NUM-9	298 K，1 bar	2.48	2.30	1.61	[5]
MOF-545	298 K，1 bar	3.12	2.57	1.31	[48]
ZJU-HOF-10(sc)	296 K，1 bar	2.19	1.88	1.9	[40]
ZJU-HOF-10(v)	296 K，1 bar	0.64	0.58	1.54	[40]
ZJU-HOF-1	298 K，1 bar	4.87	3.87	2.25	[38]
CAC-900-3	298 K，1 bar	6.02	4.86	2.6	[70]
AAC-800-3	298 K，1 bar	5.98	4.68	2.2	[70]
WAC-800-3	298 K，1 bar	6.09	4.96	1.8	[70]
SIFSIX-CAC-800-3	298 K，1 bar	5.02	4.14	1.4	[70]
DUT-8(Ni)	303 K，1 bar	3.96	2.27	1.65	[84]
RT-Cu(Qc)₂	298 K，1 bar	2.04	0.56	4.1	[85]
Ca(H₂tcpb)	298 K，1 bar	2.78	2.67	1.75	[86]
NIIC-20-Bu	298 K，1 bar	2.50	1.40	15.4	[56]
ZJU-120a	298 K，1 bar	4.91	3.93	2.74	[58]
NUM-7a	298 K，1 bar	3.04	2.68	1.76	[65]

乙烷选择性吸附剂	条件	乙烷吸附量/(mmol/g)	乙烯吸附量/(mmol/g)	IAST选择性	文献
UiO-67-(NH₂)₂	296 K，1 bar	5.32	4.32	1.7	[71]
CAU-3-NDCA	298 K，1 bar	2.42	1.61	1.56	[7]
MOF-841	298 K，1 bar	4.70	3.40	1.6	[72]
Ni(BODC)(TED)	298 K，1 bar	3.36	2.61	1.83^①	[73]
LIFM-63	298 K，1 bar	3.0	2.1	1.6	[8]
MIL-53-BDC	298 K，1 bar	2.93	2.78	1.70	[74]
MIL-53-NDCA	298 K，1 bar	4.24	3.12	1.53	[74]
MIL-53-BPDC	298 K，1 bar	2.97	2.07	1.47	[74]
ZJNU-115	298 K，1 atm	4.20	3.75	1.56	[75]
BUT-10	298 K，1 bar	4.76	3.56	1.72	[76]
ScBPDC	298 K，1 bar	3.42	2.41	1.7^②	[77]
ZJNU-7	298 K，1 bar	4.13	3.80	1.56	[78]
Co(AIN)₂	298 K，1 bar	3.16	3.14	2.96	[79]
FMOF-2	303 K，5 kPa	0.90	0.60	3.3^③	[47]
CPM-80-Zn	298 K，1 bar	4.77	4.24	1.8	[80]
CPM-81-Co	298 K，1 bar	5.51	5.07	1.8	[80]
SNNU-40	298 K，1 bar	7.54	4.91	1.57	[52]
MIL-125	298 K，1 bar	4.83	3.98	1.43	[81]
MUV-11	298 K，1 bar	1.83	1.72	1.53	[81]
ZSTU-2	298 K，1 bar	2.73	2.35	1.62	[81]
DMOF	298 K，1 bar	2.79^④	2.08^④	1.51	[50]
DMOF-DM	298 K，1 bar	4.03^④	3.11^④	1.70	[50]
DMOF-TM	298 K，1 bar	5.31^④	4.99^④	1.88	[50]
MOF-525	298 K，1 bar	2.77	2.10	1.24	[82]
MOF-525(Co)	298 K，1 bar	2.24^⑤	1.91^⑤	1.11	[82]
UPC-612	298 K，1 bar	3.57	2.69	1.4	[82]
UPC-613	298 K，1 bar	2.56	2.25	1.47	[82]
JXNU-9	298 K，1 atm	3.61	2.45	1.53	[83]
PCN-250(Fe₂Zn)	298 K，1 bar	5.95	5.42	1.7^①	[66]
PCN-250(Fe)	298 K，1 bar	6.00	5.00	1.6^①	[66]
NUM-9	298 K，1 bar	2.48	2.30	1.61	[5]
MOF-545	298 K，1 bar	3.12	2.57	1.31	[48]
ZJU-HOF-10(sc)	296 K，1 bar	2.19	1.88	1.9	[40]
ZJU-HOF-10(v)	296 K，1 bar	0.64	0.58	1.54	[40]
ZJU-HOF-1	298 K，1 bar	4.87	3.87	2.25	[38]
CAC-900-3	298 K，1 bar	6.02	4.86	2.6	[70]
AAC-800-3	298 K，1 bar	5.98	4.68	2.2	[70]
WAC-800-3	298 K，1 bar	6.09	4.96	1.8	[70]
SIFSIX-CAC-800-3	298 K，1 bar	5.02	4.14	1.4	[70]
DUT-8(Ni)	303 K，1 bar	3.96	2.27	1.65	[84]
RT-Cu(Qc)₂	298 K，1 bar	2.04	0.56	4.1	[85]
Ca(H₂tcpb)	298 K，1 bar	2.78	2.67	1.75	[86]
NIIC-20-Bu	298 K，1 bar	2.50	1.40	15.4	[56]
ZJU-120a	298 K，1 bar	4.91	3.93	2.74	[58]
NUM-7a	298 K，1 bar	3.04	2.68	1.76	[65]

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