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Surface Modification of Two‐Dimensional Metal–Organic Layers Creates Biomimetic Catalytic Microenvironments for Selective Oxidation
Author(s) -
Shi Wenjie,
Cao Lingyun,
Zhang Hua,
Zhou Xin,
An Bing,
Lin Zekai,
Dai Ruihan,
Li Jianfeng,
Wang Cheng,
Lin Wenbin
Publication year - 2017
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201703675
Subject(s) - catalysis , chemistry , sbus , selectivity , gluconic acid , synergistic catalysis , metal , metal organic framework , tetrahydrofuran , combinatorial chemistry , monolayer , organic chemistry , chemical engineering , photochemistry , adsorption , engineering , biochemistry , solvent
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.