A H_(2)O_(2) generation-detection-regulation integrated platform for boosting the efficiency of peroxygenase-catalysed C-H oxidative hydroxylation  

作　　者：Xiaowang Zhang Zhuotao Tan Mengjiao Xu Wei Zhuang Hanjie Ying Zhenyu Chu Chenjie Zhu 

机构地区：[1]College of Biotechnology and Pharmaceutical Engineering,Nanjing Tech University,Nanjing 211816,China [2]College of Chemical Engineering,Nanjing Tech University,Nanjing 211816,China

出　　处：《Green Synthesis and Catalysis》2024年第3期153-158,共6页绿色合成与催化（英文）

基　　金：supported by the Program of the National Natural Science Foundation of China(Nos.22178170,22378195 and 22208156);the Six Talent Peaks Project in Jiangsu Province(No.SWYY-045);the Jiangsu Province Natural Science Foundation for Youth(No.BK20200685).

摘　　要：The peroxygenases are ideal biocatalysts for the selective oxyfunctionalisation of stable C-H bonds.However,the catalytic efficiency of this approach is limited due to enzyme lability toward oxidant H_(2)O_(2).Although the reported in-situ H_(2)O_(2) generation system enables the stable biocatalytic process without deactivating the enzyme,the greatest catalytic potential of peroxygenases still cannot be fulfilled effectively.To address the above issue,a H_(2)O_(2) generation-detection-regulation platform that integrated an effective organocatalyst-driven H_(2)O_(2) generation system,a precise electrochemical H_(2)O_(2) real-time detection device,and a convenient H_(2)O_(2) regulation strategy was first developed.The suitable range of H_(2)O_(2) generation rate for maximizing the catalytic efficiency of peroxygenases while minimizing inactivation of the enzyme was firstly obtained by simply adjusting the amount of organocatalyst.According to the determined suitable range,the C-H oxyfunctionalisation efficiency of peroxygenases for each substrate was significantly boosted,achieving~3-fold of the reported highest turnover frequency.

关 键 词：C-H activation Enzyme catalysis Hydrogen peroxide ORGANOCATALYSIS Oxyfunctionalisation 

分 类 号：O64[理学—物理化学]