摘要
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).H_(2)O_(2)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 electroactivity for the ORR to produce H_(2)O_(2)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 H_(2)O_(2),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.
作者
朱雪芳
丁钰
李淑妮
蒋育澄
陈煜
Xuefang Zhu;Yu Ding;Shuni Li;Yucheng Jiang;Yu Chen(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)
基金
supported by the National Natural Science Foundation of China(22273056)
the Science and Technology Innovation Team of Shaanxi Province(2023-CX-TD-27)
the Fundamental Research Funds for the Central Universities(GK202202001).
