Hydrostable Fluorinated Metal-Organic Frameworks for CO2 Capture from a Wet Flue Gas: Multiscale Computational Screening

被引：3

作者：

Palakkal, Athulya S. ^{[1
]}

Mohamed, Saad Aldin ^{[1
]}

Jiang, Jianwen ^{[1
]}

机构：

[1] Department of Chemical and Bimolecular Engineering, National University of Singapore

来源：

Chem and Bio Engineering | 2024年 / 1卷 / 11期

基金：

新加坡国家研究基金会;

关键词：

adsorption; CO[!sub]2[!/sub] capture; hydrostability; metal−organic frameworks; molecular dynamics simulation; Monte Carlo simulation;

D O I：

10.1021/cbe.4c00111

中图分类号：

学科分类号：

摘要：

Metal-organic frameworks (MOFs) are promising adsorbents for CO2 capture due to readily tunable porosity and diverse functionality; however, their performance is deteriorated by the presence of H2O in a flue gas. Fluorinated MOFs (FMOFs) may impede H2O interaction with frameworks and enhance CO2 adsorption under humid conditions. In this study, a multiscale computational screening study is reported to identify the top FMOFs for CO2 capture from a wet flue gas. Initially, geometric properties as well as heats of H2O adsorption are used to shortlist FMOFs with a suitable pore size and weak H2O affinity. Then, grand-canonical Monte Carlo simulations are conducted for adsorption of a CO2/N2/H2O mixture with 60% relative humidity in 5061 FMOFs. Based on the adsorption performance, 19 FMOFs are identified as top candidates. It is revealed that the position of F atom, rather than the amount, affects CO2 adsorption; moreover, N-decorated FMOFs are preferential for selective CO2 adsorption. Finally, the hydrostability of the top FMOFs is confirmed by first-principles molecular dynamics simulations. From a microscopic level, this study provides quantitative structure-performance relationships, discovers hydrostable FMOFs with high CO2 capture performance from a wet flue gas, and would facilitate the development of new MOFs toward efficient CO2 capture under humid conditions. © 2024 The Authors. Co-published by Zhejiang University and American Chemical Society.

引用

页码：970 / 978

页数：8

共 43 条

[1]

Monastersky R., Global Carbon Dioxide Levels Near Worrisome Milestone, Nature., 497, pp. 13-14, (2013)

[2]

Weaver A.J., Toward the Second Commitment Period of the Kyoto Protocol, Science., 332, pp. 795-796, (2011)

[3]

Figueroa J.D., Fout T., Plasynski S., McIlvried H., Srivastava R.D., Advances in CO2 Capture Technology-The U.S. Department of Energy’s Carbon Sequestration Program, Int. J. Greenh. Gas Control., 2, pp. 9-20, (2008)

[4]

Yang H., Xu Z., Fan M., Gupta R., Slimane R.B., Bland A.E., Wright I., Progress in Carbon Dioxide Separation and Capture: A Review, J. Environ. Sci., 20, pp. 14-27, (2008)

[5]

Kitagawa S., Porous Materials and the Age of Gas, Angew. Chem., Int. Ed., 127, pp. 10834-10835, (2015)

[6]

Sumida K., Rogow D.L., Mason J.A., McDonald T.M., Bloch E.D., Herm Z.R., Bae T.H., Long J.R., Carbon Dioxide Capture in Metal-Organic Frameworks, Chem. Rev., 112, pp. 724-781, (2012)

[7]

Liu J., Thallapally P.K., Mc Grail B.P., Brown D.R., Liu J., Progress in Adsorption-Based CO2 Capture by Metal-Organic Frameworks, Chem. Soc. Rev., 41, pp. 2308-2322, (2012)

[8]

Yu J., Xie L.H., Li J.R., Ma Y., Seminario J.M., Balbuena P.B., CO2 Capture and Separations Using MOFs: Computational and Experimental Studies, Chem. Rev., 117, pp. 9674-9754, (2017)

[9]

Mangano E., Kahr J., Wright P.A., Brandani S., Accelerated Degradation of MOFs under Flue Gas Conditions, Faraday Discuss., 192, pp. 181-195, (2016)

[10]

Liu J., Benin A.I., Furtado A.M.B., Jakubczak P., Willis R.R., Levan M.D., Stability Effects on CO2 Adsorption for the DOBDC Series of Metal-Organic Frameworks, Langmuir., 27, pp. 11451-11456, (2011)

← 1 2 3 4 5 →