{"title":"Publisher Correction: Photoredox-catalysed amidyl radical insertion to bicyclo[1.1.0]butanes","authors":"Chetan C. Chintawar, Ranjini Laskar, Debanjan Rana, Felix Schäfer, Nele Van Wyngaerden, Subhabrata Dutta, Constantin G. Daniliuc, Frank Glorius","doi":"10.1038/s41929-024-01256-8","DOIUrl":"https://doi.org/10.1038/s41929-024-01256-8","url":null,"abstract":"<p>Correction to: <i>Nature Catalysis</i> https://doi.org/10.1038/s41929-024-01239-9, published online 22 October 2024.</p>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"2 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519378","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}
Pub Date : 2024-10-28DOI: 10.1038/s41929-024-01238-w
M. Klingenhof, H. Trzesniowski, S. Koch, J. Zhu, Z. Zeng, L. Metzler, A. Klinger, M. Elshamy, F. Lehmann, P. W. Buchheister, A. Weisser, G. Schmid, S. Vierrath, F. Dionigi, P. Strasser
Recent efforts in anion-exchange membrane water electrolysis (AEMWE) focus on developing superior catalysts and membrane electrode assemblies to narrow the performance gaps compared with proton-exchange membrane water electrolysis (PEMWE). Here we present and characterize Ir-free AEMWE cells with NiX (X = Fe, Co or Mn) layered double hydroxide (LDH) catalyst-coated membranes with polarization characteristics and hydrogen productivities approaching those of acidic PEMWE cells, achieving >5 A cm−2 at <2.2 V. Operando spectroscopy revealed a correlation between Ni4+ centres and redox-active O ligands with an O K-edge feature, attributed to µ3-O ligands in the γ-LDH catalytic phase via density functional theory calculations. This computational–experimental study challenges the previously assumed correlation between spectral O K-edge features and oxygen evolution reaction performance in Ni-based LDH catalysts and provides insights from the molecular to the technological level demonstrating how redox-active Ni–O species and innovative catalyst-coated membrane preparation boost AEMWE performance to values rivalling state-of-the-art PEMWE cell technology. Anion-exchange membrane water electrolysers have the potential to rival more costly acidic proton-exchange membrane electrolysers, but their performance and efficiency commonly still fall short. Now an anion-exchange membrane water electrolyser is prepared with a NiFe layered double hydroxide catalyst-coated membrane that achieves high current densities above 2 A cm−2 at 1.8 V and operando X-ray absorption spectroscopy is used to track the formation of the catalytically active γ-LDH phase.
最近,阴离子交换膜水电解法(AEMWE)的研究重点是开发优质催化剂和膜电极组件,以缩小与质子交换膜水电解法(PEMWE)的性能差距。在这里,我们介绍并表征了采用 NiX(X = 铁、钴或锰)层状双氢氧化物(LDH)催化剂涂层的无 Ir AEMWE 电池,其极化特性和氢气生产率接近酸性 PEMWE 电池,在 2.2 V 时达到 5 A cm-2。运算光谱显示了 Ni4+ 中心与氧化还原活性 O 配体之间的相关性,通过密度泛函理论计算,在 γ-LDH 催化阶段,O K 边特征归因于 µ3-O 配体。这项计算-实验研究挑战了之前假设的镍基 LDH 催化剂中 O K-edge 光谱特征与氧进化反应性能之间的相关性,并提供了从分子到技术层面的见解,展示了氧化还原活性 Ni-O 物种和创新的催化剂涂层膜制备如何将 AEMWE 性能提升到可与最先进的 PEMWE 电池技术相媲美的数值。
{"title":"High-performance anion-exchange membrane water electrolysers using NiX (X = Fe,Co,Mn) catalyst-coated membranes with redox-active Ni–O ligands","authors":"M. Klingenhof, H. Trzesniowski, S. Koch, J. Zhu, Z. Zeng, L. Metzler, A. Klinger, M. Elshamy, F. Lehmann, P. W. Buchheister, A. Weisser, G. Schmid, S. Vierrath, F. Dionigi, P. Strasser","doi":"10.1038/s41929-024-01238-w","DOIUrl":"10.1038/s41929-024-01238-w","url":null,"abstract":"Recent efforts in anion-exchange membrane water electrolysis (AEMWE) focus on developing superior catalysts and membrane electrode assemblies to narrow the performance gaps compared with proton-exchange membrane water electrolysis (PEMWE). Here we present and characterize Ir-free AEMWE cells with NiX (X = Fe, Co or Mn) layered double hydroxide (LDH) catalyst-coated membranes with polarization characteristics and hydrogen productivities approaching those of acidic PEMWE cells, achieving >5 A cm−2 at <2.2 V. Operando spectroscopy revealed a correlation between Ni4+ centres and redox-active O ligands with an O K-edge feature, attributed to µ3-O ligands in the γ-LDH catalytic phase via density functional theory calculations. This computational–experimental study challenges the previously assumed correlation between spectral O K-edge features and oxygen evolution reaction performance in Ni-based LDH catalysts and provides insights from the molecular to the technological level demonstrating how redox-active Ni–O species and innovative catalyst-coated membrane preparation boost AEMWE performance to values rivalling state-of-the-art PEMWE cell technology. Anion-exchange membrane water electrolysers have the potential to rival more costly acidic proton-exchange membrane electrolysers, but their performance and efficiency commonly still fall short. Now an anion-exchange membrane water electrolyser is prepared with a NiFe layered double hydroxide catalyst-coated membrane that achieves high current densities above 2 A cm−2 at 1.8 V and operando X-ray absorption spectroscopy is used to track the formation of the catalytically active γ-LDH phase.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 11","pages":"1213-1222"},"PeriodicalIF":42.8,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519246","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}
Pub Date : 2024-10-23DOI: 10.1038/s41929-024-01226-0
Estíbaliz Merino
Typically, active acyl intermediates are quenched with nucleophiles to complete carbonylation. Now, a visible-light-induced radical relay enables CO insertion and selective (hetero)aryl group migration without nucleophiles.
通常情况下,活性酰基中间体会被亲核物淬灭以完成羰基化。现在,一种由可见光诱导的自由基中继技术无需亲核剂即可实现 CO 插入和选择性(杂)芳基迁移。
{"title":"Synergistic role for CO","authors":"Estíbaliz Merino","doi":"10.1038/s41929-024-01226-0","DOIUrl":"10.1038/s41929-024-01226-0","url":null,"abstract":"Typically, active acyl intermediates are quenched with nucleophiles to complete carbonylation. Now, a visible-light-induced radical relay enables CO insertion and selective (hetero)aryl group migration without nucleophiles.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 10","pages":"1058-1059"},"PeriodicalIF":42.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487904","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}
Pub Date : 2024-10-23DOI: 10.1038/s41929-024-01246-w
Davide Esposito
{"title":"Blowing in the tube","authors":"Davide Esposito","doi":"10.1038/s41929-024-01246-w","DOIUrl":"10.1038/s41929-024-01246-w","url":null,"abstract":"","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 10","pages":"1053-1053"},"PeriodicalIF":42.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487870","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}
Pub Date : 2024-10-23DOI: 10.1038/s41929-024-01235-z
Sukriyo Chakraborty, Akkattu T. Biju
Thiamine, a common enzymatic cofactor, catalyses the benzoin condensation. From 1943, a panoply of mechanistic proposals were invoked to explain the intriguing transformation until two seminal papers by Ronald Breslow about 15 years after the discovery of this reaction helped resolve the mechanistic conundrum and heralded the birth of NHC-organocatalysis.
{"title":"Birth of organocatalysis by N-heterocyclic carbenes","authors":"Sukriyo Chakraborty, Akkattu T. Biju","doi":"10.1038/s41929-024-01235-z","DOIUrl":"10.1038/s41929-024-01235-z","url":null,"abstract":"Thiamine, a common enzymatic cofactor, catalyses the benzoin condensation. From 1943, a panoply of mechanistic proposals were invoked to explain the intriguing transformation until two seminal papers by Ronald Breslow about 15 years after the discovery of this reaction helped resolve the mechanistic conundrum and heralded the birth of NHC-organocatalysis.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 10","pages":"1060-1062"},"PeriodicalIF":42.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487875","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}
Pub Date : 2024-10-23DOI: 10.1038/s41929-024-01228-y
The performance of the electrochemical CO2 and CO reduction reactions is affected by the presence of alkali metal cations in the electrolyte, but the mechanism remains under debate. Now, experimental determination of the energetics and kinetic barriers of key elementary steps in the electrochemical CO reduction reaction on Cu enables deconvolution of the cation effect.
电化学二氧化碳和一氧化碳还原反应的性能受到电解液中碱金属阳离子存在的影响,但其机理仍存在争议。现在,通过实验确定了铜上电化学 CO 还原反应中关键基本步骤的能量和动力学障碍,从而得以解构阳离子效应。
{"title":"Deconvoluting the cation effect on carbon monoxide electroreduction","authors":"","doi":"10.1038/s41929-024-01228-y","DOIUrl":"10.1038/s41929-024-01228-y","url":null,"abstract":"The performance of the electrochemical CO2 and CO reduction reactions is affected by the presence of alkali metal cations in the electrolyte, but the mechanism remains under debate. Now, experimental determination of the energetics and kinetic barriers of key elementary steps in the electrochemical CO reduction reaction on Cu enables deconvolution of the cation effect.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 10","pages":"1063-1064"},"PeriodicalIF":42.8,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487874","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}