Journal
ACS CATALYSIS
Volume 10, Issue 17, Pages 9664-9673Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c01985
Keywords
chemoenzymatic catalysis; compartmentalization-channeling strategy; metal-organic frameworks; biocatalysis; heterogeneous catalysis
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Funding
- National Natural Science Foundation of China [21621004, 21776213]
- Tianjin Natural Science Foundation [19JCYBJC19700]
- Open foundation of State Key Laboratory of Chemical Engineering [SKL-ChE19B01]
- Open Funding Project of the State Key Laboratory of Biochemical Engineering [2020KF-06]
- Tianjin Synthetic Biotechnology Innovation Capacity Improvement Project [TSBICIP-KJGG-003]
- Program of Introducing Talents of Discipline to Universities [B06006]
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Chemoenzymatic catalysis inherits the attributes of enzymatic catalysis and chemical catalysis, where the efficiency is usually governed by the synergy of the two catalytic modules, particularly, the compatibility between two catalysts and the mass transfer between two catalytic processes. To achieve a high photosynthesis efficiency, green plants compartmentalize water oxidation and NADPH regeneration modules on two sides of the thylakoid membrane while conveying electron transfer and proton transport via the channeling of the electron transfer chain and ATP synthase, respectively. Herein, we demonstrate this principle in vitro by using UiO-66 to confine platinum nanoparticles (Pt NPs) inside and immobilize L-amino acid oxidase (LAAO) outside for the chemoenzymatic synthesis of a-keto acid. The framework structure of UiO-66 affords the compartmentalization of LAAO and Pt NPs to avoid the deactivation of LAAO by Pt NPs, while its angstrom-scale pore size ensures channeling of the byproduct, H2O2, from LAAO to Pt NPs for instant elimination. A 99.7% yield of alpha-keto acid is achieved, far surpassing that enabled by free LAAO (41.2%). The compartmentalization-channeling strategy offers a generic platform to coordinate reactions and mass transfer in complex catalytic processes beyond chemoenzymatic catalysis.
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