{"title":"提高过氧酶催化C-H氧化羟基化效率的H2O2生成-检测-调控一体化平台","authors":"","doi":"10.1016/j.gresc.2023.11.006","DOIUrl":null,"url":null,"abstract":"<div><p>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<sub>2</sub>O<sub>2</sub>. Although the reported <em>in-situ</em> H<sub>2</sub>O<sub>2</sub> 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<sub>2</sub>O<sub>2</sub> generation-detection-regulation platform that integrated an effective organocatalyst-driven H<sub>2</sub>O<sub>2</sub> generation system, a precise electrochemical H<sub>2</sub>O<sub>2</sub> real-time detection device, and a convenient H<sub>2</sub>O<sub>2</sub> regulation strategy was first developed. The suitable range of H<sub>2</sub>O<sub>2</sub> 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.</p></div>","PeriodicalId":12794,"journal":{"name":"Green Synthesis and Catalysis","volume":"5 3","pages":"Pages 153-158"},"PeriodicalIF":0.0000,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S266655492300100X/pdfft?md5=1ac9958ba7a3d4adcfa9a5a865502f1e&pid=1-s2.0-S266655492300100X-main.pdf","citationCount":"0","resultStr":"{\"title\":\"A H2O2 generation-detection-regulation integrated platform for boosting the efficiency of peroxygenase-catalysed C–H oxidative hydroxylation\",\"authors\":\"\",\"doi\":\"10.1016/j.gresc.2023.11.006\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>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<sub>2</sub>O<sub>2</sub>. Although the reported <em>in-situ</em> H<sub>2</sub>O<sub>2</sub> 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<sub>2</sub>O<sub>2</sub> generation-detection-regulation platform that integrated an effective organocatalyst-driven H<sub>2</sub>O<sub>2</sub> generation system, a precise electrochemical H<sub>2</sub>O<sub>2</sub> real-time detection device, and a convenient H<sub>2</sub>O<sub>2</sub> regulation strategy was first developed. The suitable range of H<sub>2</sub>O<sub>2</sub> 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.</p></div>\",\"PeriodicalId\":12794,\"journal\":{\"name\":\"Green Synthesis and Catalysis\",\"volume\":\"5 3\",\"pages\":\"Pages 153-158\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-08-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S266655492300100X/pdfft?md5=1ac9958ba7a3d4adcfa9a5a865502f1e&pid=1-s2.0-S266655492300100X-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Green Synthesis and Catalysis\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S266655492300100X\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Green Synthesis and Catalysis","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S266655492300100X","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
A H2O2 generation-detection-regulation integrated platform for boosting the efficiency of peroxygenase-catalysed C–H oxidative hydroxylation
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 H2O2. Although the reported in-situ H2O2 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 H2O2 generation-detection-regulation platform that integrated an effective organocatalyst-driven H2O2 generation system, a precise electrochemical H2O2 real-time detection device, and a convenient H2O2 regulation strategy was first developed. The suitable range of H2O2 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.