Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture

While metal-organic frameworks (MOFs) are promising gas adsorbents, their tortuous microporous structures cause additional resistance for gas diffusion, thus hindering the accessibility of interior active sites. Here, we present a practical strategy to incorporate missing cluster defects into a repr...

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Main Authors: Niu, Jiabin, Li, Hao, Tao, Longgang, Fan, Qianwenhao, Liu, Wen, Tan, Mei Chee
Other Authors: School of Chemical and Biomedical Engineering
Format: Article
Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/171407
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1714072023-10-25T02:56:37Z Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture Niu, Jiabin Li, Hao Tao, Longgang Fan, Qianwenhao Liu, Wen Tan, Mei Chee School of Chemical and Biomedical Engineering Institute of Sustainability for Chemicals, Energy and Environment, A*STAR Engineering::Chemical engineering Graphene Oxide Defect Engineering While metal-organic frameworks (MOFs) are promising gas adsorbents, their tortuous microporous structures cause additional resistance for gas diffusion, thus hindering the accessibility of interior active sites. Here, we present a practical strategy to incorporate missing cluster defects into a representative low-coordinated MOFs structure, Mg-MOF-74, while maintaining the stability of a defect-rich structure. In this proposed method, graphene oxide (GO) is employed as modulator, and crystallization time is varied to promote defect formation by altering the nucleation and crystal growth processes. The best performing GO-modified Mg-MOF-74 sample (MOF@GO 40 h) achieved 18% and 15% improvement in surface area and total pore volume, respectively, over pristine Mg-MOF-74. The reduced diffusion resistance to gas flow translates to increased accessibility for gas molecules to active Mg adsorption sites inside the MOFs, leading to enhanced CO2 capture performance; the CO2 uptake quantity of MOF@GO 40 h arrives at 6.06 mmol/g at 0.1 bar and at 9.17 mmol/g at 1 bar and 25 °C, 19.29% and 16.37% higher, respectively, than that of the pristine Mg-MOF-74, with a CO2/N2 selectivity around 17.36% greater than that of pristine Mg-MOF-74. Our study demonstrates a facile approach for incorporating defects into MOFs systems with low coordination environments, thus expanding the library of defect-rich MOFs beyond the current highly coordinated MOF systems. This work is supported by SUTD GAP Funding. 2023-10-25T02:56:37Z 2023-10-25T02:56:37Z 2023 Journal Article Niu, J., Li, H., Tao, L., Fan, Q., Liu, W. & Tan, M. C. (2023). Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture. ACS Applied Materials & Interfaces, 15(26), 31664-31674. https://dx.doi.org/10.1021/acsami.3c06183 1944-8244 https://hdl.handle.net/10356/171407 10.1021/acsami.3c06183 37350311 2-s2.0-85164246266 26 15 31664 31674 en ACS Applied Materials & Interfaces © 2023 American Chemical Society. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Chemical engineering
Graphene Oxide
Defect Engineering
spellingShingle Engineering::Chemical engineering
Graphene Oxide
Defect Engineering
Niu, Jiabin
Li, Hao
Tao, Longgang
Fan, Qianwenhao
Liu, Wen
Tan, Mei Chee
Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture
description While metal-organic frameworks (MOFs) are promising gas adsorbents, their tortuous microporous structures cause additional resistance for gas diffusion, thus hindering the accessibility of interior active sites. Here, we present a practical strategy to incorporate missing cluster defects into a representative low-coordinated MOFs structure, Mg-MOF-74, while maintaining the stability of a defect-rich structure. In this proposed method, graphene oxide (GO) is employed as modulator, and crystallization time is varied to promote defect formation by altering the nucleation and crystal growth processes. The best performing GO-modified Mg-MOF-74 sample (MOF@GO 40 h) achieved 18% and 15% improvement in surface area and total pore volume, respectively, over pristine Mg-MOF-74. The reduced diffusion resistance to gas flow translates to increased accessibility for gas molecules to active Mg adsorption sites inside the MOFs, leading to enhanced CO2 capture performance; the CO2 uptake quantity of MOF@GO 40 h arrives at 6.06 mmol/g at 0.1 bar and at 9.17 mmol/g at 1 bar and 25 °C, 19.29% and 16.37% higher, respectively, than that of the pristine Mg-MOF-74, with a CO2/N2 selectivity around 17.36% greater than that of pristine Mg-MOF-74. Our study demonstrates a facile approach for incorporating defects into MOFs systems with low coordination environments, thus expanding the library of defect-rich MOFs beyond the current highly coordinated MOF systems.
author2 School of Chemical and Biomedical Engineering
author_facet School of Chemical and Biomedical Engineering
Niu, Jiabin
Li, Hao
Tao, Longgang
Fan, Qianwenhao
Liu, Wen
Tan, Mei Chee
format Article
author Niu, Jiabin
Li, Hao
Tao, Longgang
Fan, Qianwenhao
Liu, Wen
Tan, Mei Chee
author_sort Niu, Jiabin
title Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture
title_short Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture
title_full Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture
title_fullStr Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture
title_full_unstemmed Defect engineering of low-coordinated metal-organic frameworks (MOFs) for improved CO₂ access and capture
title_sort defect engineering of low-coordinated metal-organic frameworks (mofs) for improved co₂ access and capture
publishDate 2023
url https://hdl.handle.net/10356/171407
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