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Angew Chem Int Ed Engl. 2017 Aug 7;56(33):9704-9709. doi: 10.1002/anie.201703675. Epub 2017 Jun 5.

Surface Modification of Two-Dimensional Metal-Organic Layers Creates Biomimetic Catalytic Microenvironments for Selective Oxidation.

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College of Chemistry and Chemical Engineering, iCHEM, PCOSS Xiamen University, Xiamen, 361005, China.
School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China.
Department of Chemistry, University of Chicago, Chicago, IL, 60637, USA.


Microenvironments in enzymes play crucial roles in controlling the activities and selectivities of reaction centers. Herein we report the tuning of the catalytic microenvironments of metal-organic layers (MOLs), a two-dimensional version of metal-organic frameworks (MOFs) with thickness down to a monolayer, to control product selectivities. By modifying the secondary building units (SBUs) of MOLs with monocarboxylic acids, such as gluconic acid, we changed the hydrophobicity/hydrophilicity around the active sites and fine-tuned the selectivity in photocatalytic oxidation of tetrahydrofuran (THF) to exclusively afford butyrolactone (BTL), likely a result of prolonging the residence time of reaction intermediates in the hydrophilic microenvironment of catalytic centers. Our work highlights new opportunities in using functional MOLs as highly tunable and selective two-dimensional catalytic materials.


biomimetic catalysis; metal-organic frameworks; metal-organic layers; oxidation; photocatalysis


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