Angewandte Chemie International Edition· 2026Q1
Radical Negative‐Feedback in High Entropy UiO‐67 to Break the Activity–Stability Trade‐Off in Photocatalytic Oxygenation of CH 4
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- 2026year
Short summary
A high-entropy UiO-67 MOF (HE-UiO-67) with a radical negative-feedback mechanism achieves stable photocatalytic methane oxygenation for over 100 hours, yielding 9732 µmol g⁻¹ h⁻¹ of oxygenates with 93.5% selectivity.
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Key points
- HE-UiO-67 MOF utilizes a radical negative-feedback mechanism to prevent photocatalyst degradation.
- The mechanism involves reconstruction of Ce sites to block MOF damage when •OH concentration is high.
- The photocatalyst demonstrated stable operation for over 100 hours.
- Achieved an oxygenate yield of 9732 µmol g⁻¹ h⁻¹ with 93.5% selectivity in methane oxygenation.
AI-generated from the title and abstract; the full text is not read.
Abstract
ABSTRACT The activity–stability trade‐off has long been a Gordian knot for metal–organic frameworks (MOFs) photocatalyst. Here, a high‐entropy UiO‐67 MOF (HE‐UiO‐67) constructed with 2,2'‐bipyridine‐5,5'‐dicarboxylic acid as the linker and ZrCeHfSnFe metal nodes was designed to induce a hydroxyl radical (•OH) negative‐feedback mechanism to disentangle the trade‐off in methane oxygenation with H 2 O 2 . When the •OH concentration generated at Fe sites exceeds the tolerance threshold of adjacent Ce─O bonds, the Ce centers are reconstructed by ligand abstraction into the unsaturated Ce sites for driving the interfacial H 2 O 2 conversion into low oxidative O 2 or •OOH species in high‐entropy metal nodes, thereby blocking the MOFs damage. This unique radical negative feedback process in HE‐UiO‐67 can maximize the concentration of radicals while maintain the stable operation for over 100 h in an ambient pressure flow‐phase system, substantially exceeding most of the previous reports. Under visible light irradiation, HE‐UiO‐67 photocatalyst exhibits an outstanding liquid oxygenate yield of up to 9732 µmol g −1 h −1 with a selectivity of 93.5%. Overall, this study opens up a promising strategy for designing efficient and durable photocatalysts to break the activity–stability trade‐off in CH 4 oxygenation.
The authors' abstract, as published at the source. Angewandte Chemie International Edition, 2026 · DOI ↗
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Field: Inorganic Chemistry
Inorganic ChemistryChemistry