Biofunctionalized “Kiwifruit-Assembly” of Oxidoreductases in Mesoporous ZnO/Carbon Nanoparticles for Efficient Asymmetric Catalysis

Abstract

A mesoporous ZnO/carbon composite is designed for coimmobilization of two oxidoreductases involving a novel "kiwifruit-assembly" pattern. The coimmobilization of (S)-carbonyl reductase II-glucose dehydrogenase on nanoparticles (SCRII–GDH_nano) exhibits 40–50% higher specific activity than the free enzyme and significantly improves stabilities of enzymes to heat, pH and solvents. It performs asymmetric catalysis of 75 × 10⁻³m substrate with a perfect yield of 100% and an excellent enantioselectivity of 99.9% within 1 h. SCRII–GDH_nano gives an over 72% yield and 99.9% enantioselectivity after it is reused for ten times. Even with a highly concentrated (400 × 10⁻³m) substrate, it shows about 60% yield and 99.9% enantioselectivity within 4 h. SCRII–GDH_nano presents 4.5–8.0-fold higher productivity in 2.0–8.0-fold shorter reaction time than the free enzyme. This work provides a general, facile, and unique approach for the immobilization of two oxidoreductases and gives high catalytic efficiency, long-term and good recycling stabilities by triggering radical proton-coupled electron transfer.

A mesoporous ZnO/carbon composite is designed for coimmobilization of two oxidoreductases. The biofunctionalized "kiwifruit-assembly" of oxidoreductases in nanoparticles performs asymmetric catalysis efficiently, even with high substrate concentrations by triggering radical proton-coupled electron transfer. The strategy provides a general, facile, and unique approach for the coimmobilization of two oxidoreductases with high catalysis efficiency, excellent long-term and recycling stability.

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