| Title: | Microenvironmental tuning in isostructural conjugated metal–organic frameworks for superior photocatalytic ▫$H_2O_2$▫ generation |
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| Authors: | ID Ranjeesh, Kayaramkodath C. (Author)
ID Chakraborty, Avanti (Author)
ID Pena-Sánchez, Pilar (Author)
ID Martinez, Jose Ignacio (Author)
ID Khayum Mohammed, Abdul (Author)
ID Elmerhi, Nada (Author)
ID Canossa, Stefano (Author)
ID Finšgar, Matjaž (Author)
ID Gándara, Felipe (Author)
ID Pachfule, Pradip (Author)
ID Shetty, Dinesh (Author) |
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| Files: |  https://onlinelibrary.wiley.com/doi/epdf/10.1002/anie.6760851
 Angew_Chem_Int_Ed_-_2026_-_Ranjeesh_-_Microenvironmental_Tuning_in_Isostructural_Conjugated_Metal_Organic_Frameworks_for.pdf (3,38 MB)
MD5: 41B1F282E1AE99521715D8ED1AC7D90A
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| Language: | English |
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| Work type: | Article |
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| Typology: | 1.01 - Original Scientific Article |
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| Organization: | FKKT - Faculty of Chemistry and Chemical Engineering
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| Abstract: | Photocatalytic hydrogen peroxide (H2O2) generation via sunlight-driven water and oxygen reduction reactions presents a sustainable alternative to the energy-intensive anthraquinone process. Although metal–organic frameworks (MOFs) offer tunable platforms for photocatalysis, the influence of metal–ligand microenvironment modulation within isostructural systems remains largely unexplored. In this work, we report two chemically robust conjugated 3D MOFs, Mn-Tp and Fe-Tp, synthesized via a scalable, solvent-free mechanochemical route and their exploration as photocatalysts. Despite sharing identical topologies and morphologies, Mn-Tp exhibits markedly superior photocatalytic performance, achieving a remarkable H2O2 yield of 10,487 µmol g−1 h−1, an apparent quantum yield of 9.94% at 467 nm, and a solar-to-chemical conversion efficiency of 0.45%. Mechanistic investigations, supported by theoretical calculations, reveal that subtle differences in the metal-node microenvironment modulate the electronic structure, promote dual-channel H2O2 generation via oxygen reduction and water oxidation, and suppress decomposition pathways. This study highlights the crucial role of local redox tuning in enhancing photocatalytic functionality, providing a strategic blueprint for designing next-generation MOF-based catalysts for the sustainable production of oxidants. |
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| Keywords: | 3D-structures, density functional theory, hydrogen peroxide, isostructural materials, metal-organic framework, photocatalysis |
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| Publication status: | Published |
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| Publication version: | Version of Record |
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| Article acceptance date: | 14.07.2026 |
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| Publication date: | 13.08.2026 |
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| Publisher: | Wiley |
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| Year of publishing: | 2026 |
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| Number of pages: | 14 str. |
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| Numbering: | [article no.] e6760851 |
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| PID: | 20.500.12556/DKUM-100388  |
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| UDC: | 54 |
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| ISSN on article: | 1521-3773 |
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| COBISS.SI-ID: | 288990979 |
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| DOI: | 10.1002/anie.6760851 |
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| Publication date in DKUM: | 16.09.2026 |
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| Views: | 138 |
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| Downloads: | 5 |
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| Metadata: |    |
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| Categories: | Misc.
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