首页|Electroenzymatic cascade reaction on a biohybrid boosts the chiral epoxidation reaction

Electroenzymatic cascade reaction on a biohybrid boosts the chiral epoxidation reaction

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The chiral epoxidation of styrene and its derivatives is an important transformation that has attracted considerable scientific interest in the chemical industry.Herein,we integrate enzymatic catalysis and electrocatalysis to propose a new route for the chiral epoxidation of styrene and its derivatives.Chloroperoxidase(CPO)functionalized with 1-ethyl-3-methylimidazolium bromide(ILEMB)was loaded onto cobalt nitrogen-doped carbon nanotubes(CoN@CNT)to form a biohybrid(CPO-ILEMB/CoN@CNT).H2O2 species were generated in situ through a two-electron oxygen reduction reaction(2e-ORR)at CoN@CNT to initiate the following enzymatic epoxidation of styrene by CPO.CoN@CNT had high elec-troactivity for the ORR to produce H2O2 at a more positive potential,prohibiting the conversion of FeⅢ to FeⅡ in the heme of CPO to maintain enzymatic activity.Meanwhile,CoN@CNT could serve as an ideal carrier for the immobilization of CPO-ILEMB.Hence,the coimmobilization of CPO-ILEMB and CoN@CNT could facilitate the diffusion of intermediate H2O2,which achieved 17 times higher efficiency than the equivalent amounts of free CPO-ILEMB in bulk solution for styrene epoxidation.Notably,an enhancement(～45％)of chiral selectivity for the epoxidation of styrene was achieved.

Electroenzymatic cascade reactionChloroperoxidaseHydrogen peroxide electrogenerationEpoxidation reactionChiral catalysis

Xuefang Zhu、Yu Ding、Shuni Li、Yucheng Jiang、Yu Chen

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School of Chemistry & Chemical Engineering,Key Laboratory of Macromolecular Science of Shaanxi Province,Shaanxi Normal University,Xi'an 710119,China

School of Materials Science and Engineering,Shaanxi Normal University,Xi'an 710119,China

National Natural Science Foundation of ChinaScience and Technology Innovation Team of Shaanxi ProvinceFundamental Research Funds for the Central Universities

222730562023-CX-TD-27GK202202001

2024

10.1016/j.scib.2023.12.025

科学通报(英文版)
中国科学院

科学通报(英文版)

CSTPCD
ISSN：1001-6538
年,卷(期)：2024.69(4)
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