Photoenzymatic synthesis of 1-alkenes and hydroxyl fatty acids bycascading a COF photocatalyst and P450 peroxygenases  

光催化剂COF与P450过加氧酶级联催化合成1-烯烃和羟基脂肪酸

作　　者：Yuanyuan Jiang Peifeng Li Zhong Li Biaobiao Zhang Shengying Li 蒋媛媛;李培凤;李众;张彪彪;李盛英

机构地区：[1]State Key Laboratory of Microbial Technology,Shandong University,Qingdao 266237,China [2]Center of Artificial Photosynthesis for Solar Fuels,School of Science,Westlake University,Hangzhou 310024,China [3]Laboratory for Marine Biology and Biotechnology,Qingdao Marine Science and Technology Center,Qingdao 266237,China

出　　处：《Science Bulletin》2024年第21期3350-3354,共5页科学通报（英文版）

基　　金：supported by the National Key Research and Development Program of China(2022YFC3401802);the National Natural Science Foundation of China(32025001,32300021,22279105,and 32200017);the China Postdoctoral Science Foundation(2022M710080 and 2021M701989);the Postdoctoral Innovation Project of Shandong Province(SDCX-ZG-202201005);the China National Postdoctoral Program for Innovative Talents(BX20220191),the Shandong Provincial Natural Science Foundation(ZR2019ZD20,ZR2023QC021,and ZR2022QC070);Qingdao Natural Science Foundation(23-2-1-25-zyyd-jch)。

摘　　要：Fuels and oleochemicals have been chemically produced fromabundant biological oils or fatty acids for more than a century,and modern biotechnology is now accelerating the advances infatty acid chemistry [1,2]. A number of enzymes responsible forthe biosynthesis of hydrocarbons from fatty acids have been discovered, providing a promising strategy for enzymatic synthesisof fatty hydrocarbons [3]. CYP152 peroxygenases have attracted agreat deal of attention due to their ability to one-step oxidativelydecarboxylate or hydroxylate fatty acids using H2O2 as sole oxidant, generating valuable a-olefins or hydroxylated fatty acids[4,5] (Fig. 1a). In addition to a-olefins as biofuels and chemicalintermediates, hydroxylated fatty acids are also an important classof compounds with various applications in food, cosmetic, pharmaceutical, and biomaterial industries [6,7] (Fig. 1b). Among them,P450BSb is considered as the most promising CYP152 peroxygenasefor practical applications due to its high stability and activity tocatalyze both b-hydroxylation (the preferred reaction) and decarboxylation (the side reaction) of fatty acids that are both mechanistically initiated by Cb-H abstraction. Of note, directed evolutioncould remodel its catalytic preference on decarboxylation orb-hydroxylation (e.g., the P450BSb-DC mutant with 67% decarboxylation selectivity) [5].

关 键 词：HYDROXYL synthesis ENZYMATIC 

分 类 号：O623.12[理学—有机化学] O623.65[理学—化学] O643.36O644.1