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Published on: August 28, 2018
Thylakoid Membrane-Inspired Capsules with Fortified Cofactor Shuttling for Enzyme-Photocoupled Catalysis
Yiying Sun1,2, Jiafu Shi3,2,4, Zhuo Wang3,2
1Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, 92 Weijin Road, Nankai District, Tianjin 300072, P. R. China.
Abstract:
Enzyme-photocoupled catalytic systems (EPCSs), combining the natural enzyme with a library of semiconductor photocatalysts, may break the constraint of natural evolution, realizing sustainable solar-to-chemical conversion and non-natural reactivity of the enzyme. The overall efficiency of EPCSs strongly relies on the shuttling of energy-carrying molecules, e.g., NAD+/NADH cofactor, between active centers of enzyme and photocatalyst. However, few efforts have been devoted to NAD+/NADH shuttling. Herein, we propose a strategy of constructing a thylakoid membrane-inspired capsule (TMC) with fortified and tunable NAD+/NADH shuttling to boost the enzyme-photocoupled catalytic process. The apparent shuttling number (ASN) of NAD+/NADH for TMC could reach 17.1, ∼8 times as high as that of non-integrated EPCS. Accordingly, our TMC exhibits a turnover frequency (TOF) of 38 000 ± 365 h-1 with a solar-to-chemical efficiency (STC) of 0.69 ± 0.12%, ∼6 times higher than that of non-integrated EPCS.
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