Symmetry-Mismatched SBU Transformation in MOFs: Postsynthetic Metal Exchange from Zn to Fe and Its Effects on Gas Adsorption and Dye Selectivity
This research explores the alteration of metal–organic frameworks (MOFs) using a method called postsynthetic metal exchange. We focus on the shift from a Zn-based MOF containing a [Zn4O(COO)6] secondary building unit (SBU) of octahedral site symmetry (ANT-1(Zn)) to a Fe-based one with a [Fe3 IIIO...
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Published in | ACS applied materials & interfaces Vol. 15; no. 41; pp. 48406 - 48415 |
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Main Authors | , , , , , , , , , , , , , |
Format | Journal Article |
Language | English |
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American Chemical Society
18.10.2023
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Abstract | This research explores the alteration of metal–organic frameworks (MOFs) using a method called postsynthetic metal exchange. We focus on the shift from a Zn-based MOF containing a [Zn4O(COO)6] secondary building unit (SBU) of octahedral site symmetry (ANT-1(Zn)) to a Fe-based one with a [Fe3 IIIO(COO)6]+ SBU of trigonal prismatic site symmetry (ANT-1(Fe)). The symmetry-mismatched SBU transformation cleverly maintains the MOF’s overall structure by adjusting the conformation of the flexible 1,3,5-benzenetribenzoate linker to alleviate the framework strain. The process triggers a decrease in the framework volume and pore size alongside a change in the framework’s charge. These alterations influence the MOF’s ability to adsorb gas and dye. During the transformation, core–shell MOFs (ANT-1(Zn@Fe)) are formed as intermediate products, demonstrating unique gas sorption traits and adjusted dye adsorption preferences due to the structural modifications at the core–shell interface. Heteronuclear clusters, located at the framework interfaces, enhance the heat of CO2 adsorption. Furthermore, they also influence the selectivity of the dye size. This research provides valuable insights into fabricating novel MOFs with unique properties by modifying the SBU of a MOF with flexible organic linkers from one site symmetry to another. |
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AbstractList | This research explores the alteration of metal–organic frameworks (MOFs) using a method called postsynthetic metal exchange. We focus on the shift from a Zn-based MOF containing a [Zn4O(COO)6] secondary building unit (SBU) of octahedral site symmetry (ANT-1(Zn)) to a Fe-based one with a [Fe3 IIIO(COO)6]+ SBU of trigonal prismatic site symmetry (ANT-1(Fe)). The symmetry-mismatched SBU transformation cleverly maintains the MOF’s overall structure by adjusting the conformation of the flexible 1,3,5-benzenetribenzoate linker to alleviate the framework strain. The process triggers a decrease in the framework volume and pore size alongside a change in the framework’s charge. These alterations influence the MOF’s ability to adsorb gas and dye. During the transformation, core–shell MOFs (ANT-1(Zn@Fe)) are formed as intermediate products, demonstrating unique gas sorption traits and adjusted dye adsorption preferences due to the structural modifications at the core–shell interface. Heteronuclear clusters, located at the framework interfaces, enhance the heat of CO2 adsorption. Furthermore, they also influence the selectivity of the dye size. This research provides valuable insights into fabricating novel MOFs with unique properties by modifying the SBU of a MOF with flexible organic linkers from one site symmetry to another. |
Author | Lah, Myoung Soo Moon, Sung Wook Kim, Yung Sam Min, Seung Kyu Han, Seungwan Choi, Hyunkyung Jeong, Seok Sharma, Amitosh Kim, Dongwook Baek, Seung Bin Kim, Chul Sung Lim, Jaewoong Seong, Junmo Lee, Seonghwan |
AuthorAffiliation | Department of Chemistry Kookmin University Department of Physics |
AuthorAffiliation_xml | – name: Department of Physics – name: Kookmin University – name: Department of Chemistry |
Author_xml | – sequence: 1 givenname: Seungwan orcidid: 0000-0001-6154-3082 surname: Han fullname: Han, Seungwan organization: Department of Chemistry – sequence: 2 givenname: Dongwook orcidid: 0000-0003-4432-371X surname: Kim fullname: Kim, Dongwook organization: Department of Chemistry – sequence: 3 givenname: Seonghwan orcidid: 0000-0003-0131-8830 surname: Lee fullname: Lee, Seonghwan organization: Department of Chemistry – sequence: 4 givenname: Hyunkyung surname: Choi fullname: Choi, Hyunkyung organization: Kookmin University – sequence: 5 givenname: Sung Wook orcidid: 0000-0002-9487-7537 surname: Moon fullname: Moon, Sung Wook organization: Department of Chemistry – sequence: 6 givenname: Amitosh orcidid: 0000-0002-7819-2570 surname: Sharma fullname: Sharma, Amitosh organization: Department of Chemistry – sequence: 7 givenname: Junmo orcidid: 0000-0003-0520-6246 surname: Seong fullname: Seong, Junmo organization: Department of Chemistry – sequence: 8 givenname: Jaewoong orcidid: 0000-0002-4557-0870 surname: Lim fullname: Lim, Jaewoong organization: Department of Chemistry – sequence: 9 givenname: Seok surname: Jeong fullname: Jeong, Seok organization: Department of Chemistry – sequence: 10 givenname: Seung Bin surname: Baek fullname: Baek, Seung Bin organization: Department of Chemistry – sequence: 11 givenname: Yung Sam orcidid: 0000-0001-6306-7438 surname: Kim fullname: Kim, Yung Sam organization: Department of Chemistry – sequence: 12 givenname: Chul Sung surname: Kim fullname: Kim, Chul Sung email: cskim@kookmin.ac.kr organization: Kookmin University – sequence: 13 givenname: Seung Kyu orcidid: 0000-0001-5636-3407 surname: Min fullname: Min, Seung Kyu email: skmin@unist.ac.kr organization: Department of Chemistry – sequence: 14 givenname: Myoung Soo orcidid: 0000-0001-9517-7519 surname: Lah fullname: Lah, Myoung Soo email: mslah@unist.ac.kr organization: Department of Chemistry |
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Title | Symmetry-Mismatched SBU Transformation in MOFs: Postsynthetic Metal Exchange from Zn to Fe and Its Effects on Gas Adsorption and Dye Selectivity |
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