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Strategies for Substrate-Regulated P450 Catalysis: From Substrate Engineering to Co-catalysis

文献类型： 外文期刊

作者： Xu, Jiakun 3 ; Wang, Chunlan 3 ; Cong, Zhiqi 1 ;

作者机构： 1.Chinese Acad Sci, CAS Key Lab Biofuels, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Shandong, Peoples R China

2.Chinese Acad Sci, Shandong Prov Key Lab Synthet Biol, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Shandong, Peoples R China

3.Chinese Acad Fishery Sci, Key Lab Sustainable Dev Polar Fisheries, Minist Agr & Rural Affairs, Yellow Sea Fisheries Res Inst, Qingdao 266071, Shandong, Peoples R China

关键词： biocatalysis; enzymes; decoy molecules; oxidation; substrate engineering

期刊名称：CHEMISTRY-A EUROPEAN JOURNAL （ 影响因子：5.236； 五年影响因子：4.843 ）

ISSN： 0947-6539

年卷期： 2019 年 25 卷 28 期

页码：

收录情况： SCI

摘要： Cytochrome P450 enzymes (P450s) catalyze the monooxygenation of various organic substrates. These enzymes are fascinating and promising biocatalysts for synthetic applications. Despite the impressive abilities of P450s in the oxidation of C-H bonds, their practical applications are restricted by intrinsic drawbacks, such as poor stability, low turnover rates, the need for expensive cofactors (e.g., NAD(P)H), and the narrow scope of useful non-native substrates. These issues may be overcome through the general strategy of protein engineering, which focuses on the improvement of the catalysts themselves. Alternatively, several emerging strategies have been developed that regulate the P450 catalytic process from the viewpoint of the substrate. These strategies include substrate engineering, decoy molecule, and dual-functional small-molecule co-catalysis. Substrate engineering focuses on improving the substrate acceptance and reaction selectivity by means of an anchoring group. The latter two strategies utilize co-substrate-like small molecules that either are proposed to reform the active site, thereby switching the substrate specificity, or directly participate in the catalytic process, thereby creating new catalytic peroxygenation capabilities towards non-native substrates. For at least 10 years, these approaches have played unique roles in solving the problems highlighted above, either alone or in conjunction with protein engineering. Herein, we review three strategies for substrate regulation in the P450-catalyzed oxidation of non-native substrates. Furthermore, we address remaining challenges and potential solutions associated with these approaches.

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