{"title":"锚定环氧化","authors":"Benjamin Martindale","doi":"10.1038/s41929-024-01247-9","DOIUrl":null,"url":null,"abstract":"<p>The team of researchers make use of the –NH<sub>2</sub> terminal groups present in native C<sub>3</sub>N<sub>4</sub> to covalently anchor an Fe(SalenCl<sub>2</sub>) molecular catalyst without the need for any additional linkers (pictured). This is performed by reacting the aryl chloride group of the molecule with C<sub>3</sub>N<sub>4</sub> in the presence of KO<sup><i>t</i></sup>Bu. With the Fe(Salen) attached to the surface, it is shown that styrene can be converted into styrene oxide under blue light-emitting diode irradiation in the presence of only O<sub>2</sub> and no other reagents. The reaction scope is expanded to cover a series of linear and cyclic alkenes including cyclohexene, α-pinene, 1-octene and <i>cis</i>-4-octene. The C<sub>3</sub>N<sub>4</sub>-FeCl(Salen) hybrid photocatalyst can be easily recovered by centrifugation and recycled.</p><p>The approach presented in this study offers a less-energy-intensive route than epoxidation by the Prilezhaev reaction using harsh stoichiometric peracids such as meta-chloroperoxybenzoic acid (<i>m</i>-CPBA), which are also hazardous to work with. Further optimization of conditions and different molecular catalyst combinations could be employed to enhance the efficiency and scope of reactivity.</p>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":42.8000,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Anchored epoxidation\",\"authors\":\"Benjamin Martindale\",\"doi\":\"10.1038/s41929-024-01247-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The team of researchers make use of the –NH<sub>2</sub> terminal groups present in native C<sub>3</sub>N<sub>4</sub> to covalently anchor an Fe(SalenCl<sub>2</sub>) molecular catalyst without the need for any additional linkers (pictured). This is performed by reacting the aryl chloride group of the molecule with C<sub>3</sub>N<sub>4</sub> in the presence of KO<sup><i>t</i></sup>Bu. With the Fe(Salen) attached to the surface, it is shown that styrene can be converted into styrene oxide under blue light-emitting diode irradiation in the presence of only O<sub>2</sub> and no other reagents. The reaction scope is expanded to cover a series of linear and cyclic alkenes including cyclohexene, α-pinene, 1-octene and <i>cis</i>-4-octene. The C<sub>3</sub>N<sub>4</sub>-FeCl(Salen) hybrid photocatalyst can be easily recovered by centrifugation and recycled.</p><p>The approach presented in this study offers a less-energy-intensive route than epoxidation by the Prilezhaev reaction using harsh stoichiometric peracids such as meta-chloroperoxybenzoic acid (<i>m</i>-CPBA), which are also hazardous to work with. Further optimization of conditions and different molecular catalyst combinations could be employed to enhance the efficiency and scope of reactivity.</p>\",\"PeriodicalId\":18845,\"journal\":{\"name\":\"Nature Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":42.8000,\"publicationDate\":\"2024-10-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1038/s41929-024-01247-9\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Catalysis","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1038/s41929-024-01247-9","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
The team of researchers make use of the –NH2 terminal groups present in native C3N4 to covalently anchor an Fe(SalenCl2) molecular catalyst without the need for any additional linkers (pictured). This is performed by reacting the aryl chloride group of the molecule with C3N4 in the presence of KOtBu. With the Fe(Salen) attached to the surface, it is shown that styrene can be converted into styrene oxide under blue light-emitting diode irradiation in the presence of only O2 and no other reagents. The reaction scope is expanded to cover a series of linear and cyclic alkenes including cyclohexene, α-pinene, 1-octene and cis-4-octene. The C3N4-FeCl(Salen) hybrid photocatalyst can be easily recovered by centrifugation and recycled.
The approach presented in this study offers a less-energy-intensive route than epoxidation by the Prilezhaev reaction using harsh stoichiometric peracids such as meta-chloroperoxybenzoic acid (m-CPBA), which are also hazardous to work with. Further optimization of conditions and different molecular catalyst combinations could be employed to enhance the efficiency and scope of reactivity.
期刊介绍：
Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry.
Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.
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