Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 56, Issue 33, Pages 9704-9709Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201703675
Keywords
biomimetic catalysis; metal-organic frameworks; metal-organic layers; oxidation; photocatalysis
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Funding
- National Natural Science Foundation
- Ministry of Science and Technology of the P.R. China [NSFC21671162, 2016YFA0200702, NSFC21471126]
- National Thousand Talents Program of the P.R. China
- Post-Doctoral Innovative Talents Project from China Postdoctoral Science Foundation [BX201600053]
- U.S. National Science Foundation [DMR-1308229]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1308229] Funding Source: National Science Foundation
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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.
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