Engineering Photoswitching Dynamics in 3D Photochromic Metal–Organic Frameworks through a Metal–Organic Polyhedron Design
Metal–organic polyhedra (MOPs) are versatile supramolecular building blocks for the design of highly porous frameworks by reticular assembly because of their diverse geometries, multiple degrees of freedom regarding functionalization, and accessible metal sites. Lipophilic functionalization is demon...
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| Published in | Journal of the American Chemical Society Vol. 147; no. 10; pp. 8568 - 8577 |
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| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
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United States
American Chemical Society
12.03.2025
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| Abstract | Metal–organic polyhedra (MOPs) are versatile supramolecular building blocks for the design of highly porous frameworks by reticular assembly because of their diverse geometries, multiple degrees of freedom regarding functionalization, and accessible metal sites. Lipophilic functionalization is demonstrated to enable the rational assembly and crystallization with photoactive N-donor ligands in an aliphatic solvent to achieve multiaxially aligned photoresponsive diarylethene (DTE) moieties in 3D frameworks (DUT-210(M), M = Cu and Rh) featuring cooperative switchability. Combined experimental and theoretical investigations based on in situ PXRD, UV–vis spectroscopy, and density functional theory calculations demonstrate deliberate kinetic engineering of photoswitchability based on variations in metal–ligand bond strengths. The novel porous frameworks are an important step toward the knowledge-based development of photon-driven motors, actuators, and release systems. |
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| AbstractList | Metal–organic
polyhedra (MOPs) are versatile supramolecular
building blocks for the design of highly porous frameworks by reticular
assembly because of their diverse geometries, multiple degrees of
freedom regarding functionalization, and accessible metal sites. Lipophilic
functionalization is demonstrated to enable the rational assembly
and crystallization with photoactive N-donor ligands in an aliphatic
solvent to achieve multiaxially aligned photoresponsive diarylethene
(DTE) moieties in 3D frameworks (DUT-210(M), M = Cu and Rh) featuring
cooperative switchability. Combined experimental and theoretical investigations
based on in situ PXRD, UV–vis spectroscopy, and density functional
theory calculations demonstrate deliberate kinetic engineering of
photoswitchability based on variations in metal–ligand bond
strengths. The novel porous frameworks are an important step toward
the knowledge-based development of photon-driven motors, actuators,
and release systems. Metal-organic polyhedra (MOPs) are versatile supramolecular building blocks for the design of highly porous frameworks by reticular assembly because of their diverse geometries, multiple degrees of freedom regarding functionalization, and accessible metal sites. Lipophilic functionalization is demonstrated to enable the rational assembly and crystallization with photoactive N-donor ligands in an aliphatic solvent to achieve multiaxially aligned photoresponsive diarylethene (DTE) moieties in 3D frameworks (DUT-210(M), M = Cu and Rh) featuring cooperative switchability. Combined experimental and theoretical investigations based on in situ PXRD, UV-vis spectroscopy, and density functional theory calculations demonstrate deliberate kinetic engineering of photoswitchability based on variations in metal-ligand bond strengths. The novel porous frameworks are an important step toward the knowledge-based development of photon-driven motors, actuators, and release systems. Metal-organic polyhedra (MOPs) are versatile supramolecular building blocks for the design of highly porous frameworks by reticular assembly because of their diverse geometries, multiple degrees of freedom regarding functionalization, and accessible metal sites. Lipophilic functionalization is demonstrated to enable the rational assembly and crystallization with photoactive N-donor ligands in an aliphatic solvent to achieve multiaxially aligned photoresponsive diarylethene (DTE) moieties in 3D frameworks (DUT-210(M), M = Cu and Rh) featuring cooperative switchability. Combined experimental and theoretical investigations based on in situ PXRD, UV-vis spectroscopy, and density functional theory calculations demonstrate deliberate kinetic engineering of photoswitchability based on variations in metal-ligand bond strengths. The novel porous frameworks are an important step toward the knowledge-based development of photon-driven motors, actuators, and release systems.Metal-organic polyhedra (MOPs) are versatile supramolecular building blocks for the design of highly porous frameworks by reticular assembly because of their diverse geometries, multiple degrees of freedom regarding functionalization, and accessible metal sites. Lipophilic functionalization is demonstrated to enable the rational assembly and crystallization with photoactive N-donor ligands in an aliphatic solvent to achieve multiaxially aligned photoresponsive diarylethene (DTE) moieties in 3D frameworks (DUT-210(M), M = Cu and Rh) featuring cooperative switchability. Combined experimental and theoretical investigations based on in situ PXRD, UV-vis spectroscopy, and density functional theory calculations demonstrate deliberate kinetic engineering of photoswitchability based on variations in metal-ligand bond strengths. The novel porous frameworks are an important step toward the knowledge-based development of photon-driven motors, actuators, and release systems. Metal–organic polyhedra (MOPs) are versatile supramolecular building blocks for the design of highly porous frameworks by reticular assembly because of their diverse geometries, multiple degrees of freedom regarding functionalization, and accessible metal sites. Lipophilic functionalization is demonstrated to enable the rational assembly and crystallization with photoactive N-donor ligands in an aliphatic solvent to achieve multiaxially aligned photoresponsive diarylethene (DTE) moieties in 3D frameworks (DUT-210(M), M = Cu and Rh) featuring cooperative switchability. Combined experimental and theoretical investigations based on in situ PXRD, UV–vis spectroscopy, and density functional theory calculations demonstrate deliberate kinetic engineering of photoswitchability based on variations in metal–ligand bond strengths. The novel porous frameworks are an important step toward the knowledge-based development of photon-driven motors, actuators, and release systems. |
| Author | Heine, Thomas Etter, Martin Kaskel, Stefan Bon, Volodymyr De, Ankita Jin, Eunji Wonanke, A. D. Dinga Bönisch, Nadine Karlsen, Martin A. Das, Shubhajit |
| AuthorAffiliation | Department of Chemistry Technische Universität Dresden Institute of Resource Ecology Chair of Theoretical Chemistry, Faculty of Chemistry and Food Chemistry Yonsei University Helmholtz Zentrum Dresden-Rossendorf Chair of Inorganic Chemistry I, Faculty of Chemistry and Food Chemistry P02.1 Beamline, PETRA III Deutsches Elektronen-Synchrotron DESY |
| AuthorAffiliation_xml | – name: Chair of Inorganic Chemistry I, Faculty of Chemistry and Food Chemistry – name: Department of Chemistry – name: Chair of Theoretical Chemistry, Faculty of Chemistry and Food Chemistry – name: Deutsches Elektronen-Synchrotron DESY – name: P02.1 Beamline, PETRA III – name: Technische Universität Dresden – name: Institute of Resource Ecology – name: Yonsei University – name: Helmholtz Zentrum Dresden-Rossendorf |
| Author_xml | – sequence: 1 givenname: Eunji orcidid: 0000-0002-2103-6526 surname: Jin fullname: Jin, Eunji email: eunji.jin@tu-dresden.de organization: Chair of Inorganic Chemistry I, Faculty of Chemistry and Food Chemistry – sequence: 2 givenname: Volodymyr orcidid: 0000-0002-9851-5031 surname: Bon fullname: Bon, Volodymyr organization: Chair of Inorganic Chemistry I, Faculty of Chemistry and Food Chemistry – sequence: 3 givenname: Shubhajit orcidid: 0000-0002-8027-6781 surname: Das fullname: Das, Shubhajit organization: Technische Universität Dresden – sequence: 4 givenname: A. D. Dinga surname: Wonanke fullname: Wonanke, A. D. Dinga organization: Technische Universität Dresden – sequence: 5 givenname: Martin surname: Etter fullname: Etter, Martin organization: Deutsches Elektronen-Synchrotron DESY – sequence: 6 givenname: Martin A. orcidid: 0000-0003-1262-8965 surname: Karlsen fullname: Karlsen, Martin A. organization: Deutsches Elektronen-Synchrotron DESY – sequence: 7 givenname: Ankita orcidid: 0000-0003-4962-0510 surname: De fullname: De, Ankita organization: Chair of Inorganic Chemistry I, Faculty of Chemistry and Food Chemistry – sequence: 8 givenname: Nadine surname: Bönisch fullname: Bönisch, Nadine organization: Chair of Inorganic Chemistry I, Faculty of Chemistry and Food Chemistry – sequence: 9 givenname: Thomas orcidid: 0000-0003-2379-6251 surname: Heine fullname: Heine, Thomas organization: Yonsei University – sequence: 10 givenname: Stefan orcidid: 0000-0003-4572-0303 surname: Kaskel fullname: Kaskel, Stefan email: stefan.kaskel@tu-dresden.de organization: Chair of Inorganic Chemistry I, Faculty of Chemistry and Food Chemistry |
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| SubjectTerms | crystallization density functional theory ligands lipophilicity solvents ultraviolet-visible spectroscopy |
| Title | Engineering Photoswitching Dynamics in 3D Photochromic Metal–Organic Frameworks through a Metal–Organic Polyhedron Design |
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