Nature CatalysisPub Date : 2025-06-25DOI: 10.1038/s41929-025-01361-2
Debangshu Mukherjee
{"title":"Operando imaging reveals nanocatalyst reconstruction","authors":"Debangshu Mukherjee","doi":"10.1038/s41929-025-01361-2","DOIUrl":"10.1038/s41929-025-01361-2","url":null,"abstract":"Understanding the nature of structural evolution of Cu nanocatalysts during CO2 electroreduction is a long-standing question in catalysis science. Now, operando electron microscopy techniques correlated with X-ray spectroscopy and first-principles modelling demonstrate that the reaction products themselves drive the structural evolution in Cu nanocubes.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"518-520"},"PeriodicalIF":44.6,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478952","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature CatalysisPub Date : 2025-06-25DOI: 10.1038/s41929-025-01360-3
Magda H. Barecka
{"title":"Complex behaviour of isotopes in CO2 electroreduction","authors":"Magda H. Barecka","doi":"10.1038/s41929-025-01360-3","DOIUrl":"10.1038/s41929-025-01360-3","url":null,"abstract":"Isotope labelling with 13C-carbon has become a popular technique used to understand carbon dioxide electroreduction mechanisms. However, isotopes of carbon exhibit complex selectivity effects, which need to be carefully considered in the experimental design to avoid misinterpretations.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"513-517"},"PeriodicalIF":44.6,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature CatalysisPub Date : 2025-06-24DOI: 10.1038/s41929-025-01357-y
Tirtha Mandal, Mangish Ghosh, Hendrik Paps, Tanumoy Mandal, Oliver Reiser
{"title":"A general photocatalytic platform for the regio- and stereoselective β-chloroacylation of alkenes and alkynes using a heteroleptic copper(I) complex","authors":"Tirtha Mandal, Mangish Ghosh, Hendrik Paps, Tanumoy Mandal, Oliver Reiser","doi":"10.1038/s41929-025-01357-y","DOIUrl":"10.1038/s41929-025-01357-y","url":null,"abstract":"Atom transfer radical addition (ATRA) of aroyl chlorides to access β-chloroacyl derivatives via photoredox catalysis remains hamstrung by the need to use precious iridium photocatalysts and activated alkenes as acceptors. Here we report a unified platform for the regioselective chlorocarbonylation of alkenes via visible-light-mediated ATRA of aroyl chlorides catalysed by a heteroleptic Cu(I) complex featuring extensive substrate scope, scalability and functional group tolerance. In addition, alkynes are amenable substrates, allowing E-selective β-chlorovinyl ketone formation. The synthetic utility of the protocol is demonstrated through the functionalization of complex substrates, post-modifications of the products and the formal synthesis of pharmacologically relevant haloperidol, seratrodast and the naturally occurring piperidine alkaloid (−)-sedamine. This study undergirds the exclusive role of a heteroleptic copper(I) complex, which outperforms homoleptic copper(I) complexes—efficient for many ATRA processes—owing to its longer excited-state lifetime and adaptive ligand environment being tailored for the distinctive mechanistic steps catalysed by Cu(I) and Cu(II) in the title reaction. There are issues hampering the wider adoption of atom transfer radical addition (ATRA) of aroyl chlorides to access β-chloroacyl derivatives via photoredox catalysis. Now, Mandal et al. report the regioselective chlorocarbonylation of alkenes and alkynes via visible-light-mediated ATRA of aroyl chlorides catalysed by a heteroleptic Cu(I) complex.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"607-622"},"PeriodicalIF":44.6,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-025-01357-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144371205","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Photoenzymatic stereoablative enantioconvergence of γ-chiral oximes via hydrogen atom transfer","authors":"Zhengyi Zhang, Maolin Li, Wesley Harrison, Jingxia Lu, Zhenxiang Zhao, Yujie Yuan, Huimin Zhao","doi":"10.1038/s41929-025-01347-0","DOIUrl":"10.1038/s41929-025-01347-0","url":null,"abstract":"Producing enantioenriched molecules from racemic mixtures is essential for manufacturing. Traditional methods such as resolution, deracemization and enantioconvergent catalysis primarily involve separating or converting enantiomers without altering their structures, or functionalization of stereocentres at or proximal to functional groups. However, there are challenges in enantioselectively forging C–H bonds that are remote from functional groups via hydrogen atom transfer (HAT) with these methods. Here we introduce a strategy for the photoenzymatic stereoablative enantioconvergence of γ-chiral oximes using repurposed flavin-dependent ene-reductases. A photoinduced single-electron reduction of the γ-chiral oxime by an ene-reductase generates an iminyl radical, which then undergoes stereoablative 1,5-HAT at the γ-stereocentre. Subsequent chiral reconstruction through enzymatic HAT and spontaneous imine hydrolysis yields the γ-chiral ketone with high enantioselectivity. This work provides a robust method for remote stereoablative enantioconvergent HAT and broadens the synthetic utility of photobiocatalysis. Remote C–H bond formation via photoenzymatic hydrogen atom transfer has enabled the precise installation of remote stereocentres but is still in its infancy. Here, the authors report the photoenzymatic stereoablative enantioconvergence of γ-chiral oximes using repurposed flavin-dependent ene-reductases.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"548-555"},"PeriodicalIF":44.6,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144371206","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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