{"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":"10.1016/j.gresc.2023.11.006","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":0.0,"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":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138512293","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ate complexes in organic synthesis: From ate reagents to ate catalysts","authors":"","doi":"10.1016/j.gresc.2024.04.010","DOIUrl":"10.1016/j.gresc.2024.04.010","url":null,"abstract":"<div><p>The realm of application of organometallic catalysis to organic synthesis has witnessed a transformative shift in recent years, owing much to the evolution of ate complexes from mere reagents to versatile catalysts. Ate complexes, formed through the coordination of a neutral Lewis acid with an organic anionic base, have emerged as pivotal intermediates that not only facilitate organic transformations but also serve as efficient catalysts in a wide range of chemical reactions. This review presents the fascinating journey of ate complexes, highlighting their development from stoichiometric reagents to active catalysts. Historically, ate complexes were primarily regarded as stoichiometric species essential for various metal-catalyzed transformations. However, constant research has unveiled their potential as catalysts in their own right, reshaping the landscape of modern organic synthesis. In this minireview, we discuss the pivotal role of ate complexes in the evolution of organic synthesis, from their early days as reactive intermediates to their current stature as catalytic pioneers offering a glimpse into the exciting future of this dynamic field.</p></div>","PeriodicalId":12794,"journal":{"name":"Green Synthesis and Catalysis","volume":"5 3","pages":"Pages 141-152"},"PeriodicalIF":0.0,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S266655492400053X/pdfft?md5=7a4de4c94a8dbec8c809e1e05e1cb03f&pid=1-s2.0-S266655492400053X-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141037151","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Synthesis of 1,4-oxathiins via [3+3] annulation of pyridinium 1,4‐zwitterionic thiolates with iodonium ylides","authors":"Zhibin Niu, C. Pi, Yangjie Wu, Xiuling Cui","doi":"10.1016/j.gresc.2024.07.002","DOIUrl":"https://doi.org/10.1016/j.gresc.2024.07.002","url":null,"abstract":"","PeriodicalId":12794,"journal":{"name":"Green Synthesis and Catalysis","volume":"12 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141848730","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Feiyu Qiu, Yi Chen, Peiqin Liao, Yuan Gao, Mian Guo, Heng Zhang, Aiwen Lei, Wu Li
{"title":"Electrochemical selective deuterium labelling of N-heteroarenes","authors":"Feiyu Qiu, Yi Chen, Peiqin Liao, Yuan Gao, Mian Guo, Heng Zhang, Aiwen Lei, Wu Li","doi":"10.1016/j.gresc.2024.06.003","DOIUrl":"https://doi.org/10.1016/j.gresc.2024.06.003","url":null,"abstract":"Hydrogen-deuterium exchange (HIE) reaction is the most direct way to achieve the deuterium labeling as there is no need for extra pre-functionalization. Herein, we report an electrochemical selective deuterium labelling of -heteroarenes using DO. The formation of aromatic radicals has been directly identified by using the time-resolved electron paramagnetic resonance (EPR) technique under electrochemical conditions. Mechanistic studies revealed that the hydrogen/deuterium (H/D) exchange involved continuous redox of -heteroarenes under paired electrolysis and the selectivity of deuteration was established by DFT calculations. This electrochemical synthesis method offers a promising avenue for deuterium incorporation at specific sites of aromatic compounds.","PeriodicalId":12794,"journal":{"name":"Green Synthesis and Catalysis","volume":"18 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142198860","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Li Yang, Priyanka Chakraborty, Pradip K. Das, Dongya Zhang, Kuo-Wei Huang
{"title":"Transformation of ambient CO2 in air into cyclic carbonates mediated by a phosphorus-nitrogen PN3-pincer iron complex","authors":"Li Yang, Priyanka Chakraborty, Pradip K. Das, Dongya Zhang, Kuo-Wei Huang","doi":"10.1016/j.gresc.2024.06.002","DOIUrl":"https://doi.org/10.1016/j.gresc.2024.06.002","url":null,"abstract":"The atom-economical reaction of carbon dioxide (CO) with epoxides possesses the potential to utilize captured CO₂ for synthesizing useful chemicals. Among a wide range of metal complexes employed for this transformation, iron (Fe) stands out because of its low cost, ready availability, and stability. In this work, a pyridine-based pincer PN³-Fe(II) complex was synthesized and used as an efficient catalyst for the CO₂ epoxide cycloaddition. More importantly, this complex enabled the direct capture of CO₂ in the atmosphere and conversion into cyclic carbonates in excellent yields.","PeriodicalId":12794,"journal":{"name":"Green Synthesis and Catalysis","volume":"99 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141885090","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}