Abstract
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.
基金项目
National Natural Science Foundation of China(22273056)
Science and Technology Innovation Team of Shaanxi Province(2023-CX-TD-27)
Fundamental Research Funds for the Central Universities(GK202202001)
NETL
NSTL
万方数据