水热稳定金属-有机骨架材料用于高效分离SF<sub>6</sub>/N<sub>2</sub>混合物的研究

常苗; 刘磊; 阳庆元; 刘大欢; 仲崇立

doi:10.11949/0438-1157.20191133

您当前的位置：

首页 >

文章列表页 >

水热稳定金属-有机骨架材料用于高效分离SF₆/N₂混合物的研究

分离工程 | 更新时间：2026-07-24

- 水热稳定金属-有机骨架材料用于高效分离SF₆/N₂混合物的研究
- Study on efficient separation of SF₆/N₂ mixture using a hydrothermally stable metal-organic framework
- 化工学报 2020年71卷第1期页码：320-328
- 作者机构：
  
  1. 北京化工大学有机无机复合材料国家重点实验室，北京 100029
  2. 天津工业大学分离膜与膜过程国家重点实验室，天津 300387
- 作者简介：
  
  常苗（1993—），男，硕士研究生，17810288674@163.com
  刘大欢（1980—），男，博士，教授，liudh@mail.buct.edu.cn
  仲崇立（1966—），男，博士，教授，zhongchongli@tjpu.edu.cn
- 基金信息：
  
  国家自然科学基金项目(21536001;21722602;21576009)
- DOI：10.11949/0438-1157.20191133
  中图分类号： TQ 028.8
- 收稿：2019-10-08，
  
  修回：2019-10-18，
  
  网络首发：2020-08-12，
  
  纸质出版：2020-01-05
- 稿件说明：
移动端阅览
常苗, 刘磊, 阳庆元, 刘大欢, 仲崇立. 水热稳定金属-有机骨架材料用于高效分离SF₆/N₂混合物的研究[J]. 化工学报, 2020, 71(1): 320-328 DOI: 10.11949/0438-1157.20191133.

CHANG Miao, LIU Lei, YANG Qingyuan, LIU Dahuan, ZHONG Chongli. Study on efficient separation of SF₆/N₂ mixture using a hydrothermally stable metal-organic framework[J]. CIESC Journal, 2020, 71(1): 320-328 DOI: 10.11949/0438-1157.20191133.
常苗, 刘磊, 阳庆元, 刘大欢, 仲崇立. 水热稳定金属-有机骨架材料用于高效分离SF₆/N₂混合物的研究[J]. 化工学报, 2020, 71(1): 320-328 DOI: 10.11949/0438-1157.20191133. DOI：

CHANG Miao, LIU Lei, YANG Qingyuan, LIU Dahuan, ZHONG Chongli. Study on efficient separation of SF₆/N₂ mixture using a hydrothermally stable metal-organic framework[J]. CIESC Journal, 2020, 71(1): 320-328 DOI: 10.11949/0438-1157.20191133. DOI：

摘要

混合物的高效分离，对SF

气体的回收与减弱其直接排放所导致的温室效应，具有重要的实际意义。合成了一种具有不同性质孔道结构的金属-有机骨架材料，Cu-MOF-OMe。该材料具有含不饱和配位金属位点和甲氧基双功能化的特征，且表现出良好的水热稳定性和再生性能。该材料表现出优异的综合分离性能，298 K和10

Pa下的分离选择性（361）和吸附剂选择性参数 (SSP) 值 (780)均远高于文献报道值。理论计算发现，亲水性孔道中的不饱和金属位和疏水性孔道中丰富的甲氧基的协同作用，为该MOF材料具有优异SF

分离性能的主要原因。研究结果可为SF

高效分离材料的设计与开发提供参考依据。

Abstract

The efficient separation of the SF

mixture has important practical significance for the recovery of SF

gas and the reduction of the greenhouse effect caused by its direct discharge. In this work

a metal–organic framework (Cu-MOF-OMe) was prepared with two different types and properties of pores. It possesses dually-functionalized characteristics of coordinatively unsaturated metal sites and methoxy groups

which exhibit good hydrothermal stability and adsorptive regenerability. This material also shows excellent separation performance for SF

mixture. At 298 K and 10

the observed adsorption selectivity (361) and sorbent selection parameter (SSP) value (780) are highest compared to various porous materials reported so far. Theoretical calculation results indicated that the underlying reason of such excellent separation properties is attributed to the cooperative effects of the open Cu sites in the hydrophilic pores and the abundant methoxy groups in the hydrophobic pores. The findings may pro

vide valuable foundation for developing highly efficient materials for practical of SF

separation.

关键词

Keywords

references

Tsai W T . The decomposition products of sulfur hexafluoride (SF 6 ): reviews of environmental and health risk analysis [J ] . Fluorine Chem ., 2007 , 128 : 1345 - 1352 .

Kim M B , Lee S J , Lee C Y , et al . High SF 6 selectivities and capacities in isostructural metal-organic frameworks with proper pore sizes and highly dense unsaturated metal sites [J ] . Micropor. Mesopor. Mat ., 2014 , 190 : 356 - 361 .

Christophorou L G , Vanbrunt R J . SF 6 /N 2 mixtures - basic and HV insulation properties [J ] . IEEE Trans . Dielectr. Electr. Insul ., 1995 , 2 : 952 - 1003 .

Yamamoto O , Takuma T , Kinouchi M . Recovery of SF 6 from N 2 /SF 6 gas mixtures by using a polymer membrane [J ] . IEEE Electr . Insul. Mag ., 2002 , 18 : 32 - 37 .

Imai T , Inohara T , Toyoda M . Use of zeolite filter in portable equipment for recovering SF 6 in SF 6 /N 2 mixtures [J ] . IEEE Trans . Dielectr. Electr. Insul ., 2004 , 11 : 166 - 173 .

Toyoda M , Murase H , Imai T , et al . SF 6 reclaimer from SF 6 /N 2 mixtures by gas separation with molecular sieving effect [J ] . IEEE Trans . Power Deliv ., 2003 , 18 : 442 - 448 .

Senkovska I , Barea E , Navarro J A R , et al . Adsorptive capturing and storing greenhouse gases such as sulfur hexafluoride and carbon tetrafluoride using metal-organic frameworks [J ] . Micropor. Mesopor. Mat ., 2012 , 156 : 115 - 120 .

Lee E K , Lee J D , Lee H J , et al . Pure SF 6 and SF 6 -N 2 mixture gas hydrates equilibrium and kinetic characteristics [J ] . Environ. Sci. Technol ., 2009 , 43 : 7723 - 7727 .

Cha I , Lee S , Lee J D , et al . Separation of SF 6 from gas mixtures using gas hydrate formation [J ] . Environ. Sci. Technol ., 2010 , 44 : 6117 - 6122 .

Skarmoutsos I , Eddaoudi M , Maurin G . Highly tunable sulfur hexafluoride separation by interpenetration control in metal organic frameworks [J ] . Micropor. Mesopor. Mat ., 2019 , 281 : 44 - 49 .

Chuah C Y , Goh K L , Bae T H . Hierarchically structured HKUST‑1 nanocrystals for enhanced SF 6 capture and recovery [J ] . J. Phys. Chem. C , 2017 , 121 ： 6748 - 6755 .

Skarmoutsos I , Tamiolakis G , Froudakis G E . Highly selective separation and adsorption-induced phase transition of SF 6 -N 2 fluid mixtures in three-dimensional carbon nanotube networks [J ] . J. Supercrit. Fluids , 2016 , 113 : 89 - 95 .

Takase A , Kanoh H , Ohba T . Wide carbon nanopores as efficient sites for the separation of SF 6 from N 2 [J ] . Sci . Rep ., 2015 , 5 : 11994 .

Kim P J , You Y W , Park H , et al . Separation of SF 6 from SF 6 /N 2 mixture using metal-organic framework MIL-100(Fe) granule [J ] . Chem. Eng. J ., 2015 , 262 : 683 - 690 .

Kim M B , Kim K M , Kim T H , et al . Highly selective adsorption of SF 6 over N 2 in a bromine-functionalized zirconium-based metal-organic framework [J ] . Chem. Eng. J ., 2018 , 339 : 223 - 229 .

Kim M B , Yoon T U , Hong D Y , et al . High SF 6 /N 2 selectivity in a hydrothermally stable zirconium-based metal-organic framework [J ] . Chem. Eng. J ., 2015 , 276 : 315 - 321 .

Sun R , Tai C W , Strømme M , et al . Hierarchical porous carbon synthesized from novel porous amorphous calcium or magnesium citrate with enhanced SF 6 uptake and SF 6 /N 2 selectivity [J ] . ACS Appl . Nano Mater ., 2019 , 2 : 778 - 789 .

Hasell T , Miklitz M , Stephenson A , et al . Porous organic cages for sulfur hexafluoride separation [J ] . J. Am. Chem. Soc ., 2016 , 138 : 1653 - 1659 .

Fang X K , Hu X , Maenhout G J , et al . Sulfur hexafluoride (SF 6 ) emission estimates for china: an inventory for 1990—2010 and a projection to 2020 [J ] . Environ. Sci. Technol ., 2013 , 47 : 3848 - 3855 .

Chiang Y C , Wu P Y . Adsorption equilibrium of sulfur hexafluoride on multi-walled carbon nanotubes [J ] . J. Hazard. Mater ., 2010 , 178 : 729 - 738 .

Mohindra V , Chae H , Sawin H H , et al . Abatement of perfluorocompounds (PFC’s) in a microwave tubular reactor using O as an additive gas [J ] . IEEE Trans . Plasma Sci ., 1997 , 10 : 399 - 407 .

Ravishankara A R , Solomon S , Turnipseed A A , et al . Atmospheric lifetimes of long-lived halogenated species [J ] . Science , 1993 , 259 : 194 - 199 .

Builes S , Roussel T , Vega L F . Optimization of the separation of sulfur hexafluoride and nitrogen by selective adsorption using Monte Carlo simulations [J ] . AIChE J . 2011 , 57 : 962 - 974 .

Kim D H , Ko Y H , Kim T H , et al . Separation of N 2 /SF 6 binary mixtures using polyethersulfone (PESf) hollow fiber membrane [J ] . Korean J. Chem. Eng ., 2012 , 29 : 1081 - 1085 .

Cho W S , Lee K H , Chang H J , et al . Evaluation of pressure-temperature swing adsorption for sulfur hexafluoride (SF 6 ) recovery from SF 6 and N 2 gas mixture [J ] . Korean J. Chem. Eng ., 2011 , 28 : 2196 - 2201 .

Ho M T , Allinson G W , Wiley D E . Reducing the cost of CO 2 capture from flue gases using pressure swing adsorption [J ] . Ind. Eng. Chem. Res ., 2008 , 47 : 4883 - 4890 .

Wiersum A D , Chang J S , Serre C , et al . An adsorbent performance indicator as a first step evaluation of novel sorbents for gas separations: application to metal-organic frameworks [J ] . Langmuir , 2013 , 29 : 3301 - 3309 .

Tong M M , Lan Y S , Yang Q Y , et al . Exploring the structure-property relationships of covalent organic frameworks for noble gas separations [J ] . Chem. Eng. Sci ., 2017 , 168 : 456 - 464 .

Cui X L , Chen K J , Xing H B , et al . Pore chemistry and size control in hybrid porous materials for acetylene capture from ethylene [J ] . Science , 2016 , 353 : 141 - 144 .

Li B , Cui X L , O’Nolan D , et al . An ideal molecular sieve for acetylene removal from ethylene with record selectivity and productivity [J ] . Adv . Mater ., 2017 , 29 : 1704210 .

Yang L F , Cui X L , Yang Q W , et al . A single-molecule propyne trap: highly efficient removal of propyne from propylene with anion-pillared ultramicroporous materials [J ] . Adv . Mater ., 2018 , 30 : 1705374 .

Li L B , Wen H M , He C H , et al . A metal-organic framework with suitable pore size and specific functional sites for the removal of trace propyne from propylene [J ] . Angew. Chem. Int. Ed ., 2018 , 57 : 15183-15188 .

Furukawa H , Cordova K E , O’Keeffe M , et al . The chemistry and application of metal-organic frameworks [J ] . Science , 2013 , 341 : 974 - 986 .

Mueller U , Schubert M , Teich F , et al . Metal-organic frameworks-prospective industrial applications [J ] . J. Mater. Chem ., 2006 , 16 : 626 - 636 .

Bae Y S , Snurr R Q . Development and evaluation of porous materials for carbon dioxide separation and capture [J ] . Angew. Chem. Int. Ed ., 2011 , 50 : 11586-11596 .

Biswas S , Vanpoucke D E P , Verstraelen T , et al . New functionalized metal-organic frameworks MIL-47-X (X = —Cl, —Br, —CH 3 , —CF 3 , —OH, —OCH 3 ): synthesis, characterization, and CO 2 adsorption properties [J ] . J. Phys. Chem. C , 2013 , 117 : 22784-22796 .

Au V K M , Nakayashiki K , Huang H B , et al . Stepwise expansion of layered metal-organic frameworks for nonstochastic exfoliation into porous nanosheets [J ] . J. Am. Chem. Soc ., 2019 , 141 : 53 - 57 .

Bachman J E , Reed D A , Kapelewski M T , et al . Enabling alternative ethylene production through its selective adsorption in the metal-organic framework Mn 2 ( m -dobdc) [J ] . Energy Environ . Sci ., 2018 , 11 : 2423 - 2431 .

Wang K K , Huang H L , Liu D H , et al . Covalent triazine-based frameworks with ultramicropores and high nitrogen contents for hi ghly selective CO 2 capture [J ] . Environ . Sci . Technol ., 2016 , 50 ; 4869 - 4876 .

Breneman C M , Wiberg K B . Determining atom-centered monopoles from molecular electrostatic potentials: the need for high sampling density in formamide conformational analysis [J ] . J. Comput. Chem ., 1990 , 11 : 361 - 373 .

Dellis D , Samios J . Molecular force field investigation for sulfur hexafluoride: a computer simulation study [J ] . Fluid Phase Equilibria , 2010 , 291 : 81 - 89 .

Potoff J J , Siepmann J I . Vapor-liquid equilibria of mixtures containing alkanes, carbon dioxide, and nitrogen [J ] . AIChE J ., 2001 , 47 : 1676 - 1682 .

Rappé A K , Casewit C J , Colwell K S , et al . UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations [J ] . J. Am. Chem. Soc ., 1992 , 114 : 10024-10035 .

Vlugt T J H , García P E , Dubbeldam D , et al . Computing the heat of adsorption using molecular simulations: the effect of strong coulombic interactions [J ] . J. Chem. Theory Comput ., 2008 , 4 : 1107 - 1118 .

Chen Y J , Li P , Modica J A , et al . Acid-resistant mesoporous metal-organic framework toward oral insulin delivery: protein encapsulation, protection, and release [J ] . J. Am. Chem. Soc ., 2018 , 140 : 5678 - 5681

Li L Y , Yang L F , Wang J W , et al . Highly efficient separation of methane from nitrogen on a squarate-based metal-organic framework [J ] . AIChE J ., 2018 , 64 : 3681 - 3689 .

Hu J L , Sun T J , Liu X W , et al . Separation of CH 4 /N 2 mixtures in metal-organic frameworks with 1D micro-channels [J ] . RSC Adv ., 2016 , 6 : 64039-64046 .

Lin R B , Wu H , Li L B , et al . Boosting ethane/ethylene separation within isoreticular ultramicroporous metal-organic frameworks [J ] . J. Am. Chem. Soc ., 2018 , 140 : 12940-12946 .

浏览量

下载量

CSCD

文章被引用时，请邮件提醒。

提交

工具集

关联资源

含开放金属位点MIL-101(Cr)掺杂的混合基质膜制备及其CO2分离性能

用于甲烷-氮气体系分离的膜技术研究进展

CH4-N2在MOFs结构材料中的吸附分离性能

炭分子筛CH4/N2吸附分离

面向氧氮氩分离的MOFs材料研究进展

水热稳定金属-有机骨架材料用于高效分离SF6/N2混合物的研究

Study on efficient separation of SF6/N2 mixture using a hydrothermally stable metal-organic framework

DOI：10.11949/0438-1157.20191133

摘要

Abstract

关键词

Keywords

references

水热稳定金属-有机骨架材料用于高效分离SF₆/N₂混合物的研究

Study on efficient separation of SF₆/N₂ mixture using a hydrothermally stable metal-organic framework