Nature Catalysis最新文献_第2页

Photobiocatalysis with non-haem iron enzymes for enantioselective radical transformations

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01263-9

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The STRENDA Biocatalysis Guidelines for cataloguing metadata

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01261-x

Stephan Malzacher, Dominik Meißner, Jan Range, Zvjezdana Findrik Blažević, Katrin Rosenthal, John M. Woodley, Roland Wohlgemuth, Peter Wied, Bernd Nidetzky, Robert T. Giessmann, Kridsadakorn Prakinee, Pimchai Chaiyen, Andreas S. Bommarius, Johann M. Rohwer, Rodrigo O. M. A. de Souza, Peter J. Halling, Jürgen Pleiss, Carsten Kettner, Dörte Rother

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1,3-Butadiene formation through selective acetylene electrolysis on partially oxidized copper

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01255-9

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Generating alkyl carbanions for organic synthesis

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01264-8

Sergio González-Granda, Corey R. J. Stephenson

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Alkali metal cations act as homogeneous cocatalysts for the oxygen reduction reaction in aqueous electrolytes

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01241-1

Sang Gu Ji, Minho M. Kim, Man Ho Han, Junsic Cho, Yoosang Son, Young Yong Kim, Jaeyoung Jeong, Zee Hwan Kim, Keun Hwa Chae, Hyung-Suk Oh, Hyungjun Kim, Chang Hyuck Choi

{"title":"Alkali metal cations act as homogeneous cocatalysts for the oxygen reduction reaction in aqueous electrolytes","authors":"Sang Gu Ji, Minho M. Kim, Man Ho Han, Junsic Cho, Yoosang Son, Young Yong Kim, Jaeyoung Jeong, Zee Hwan Kim, Keun Hwa Chae, Hyung-Suk Oh, Hyungjun Kim, Chang Hyuck Choi","doi":"10.1038/s41929-024-01241-1","DOIUrl":"10.1038/s41929-024-01241-1","url":null,"abstract":"Alkali metal cations (AM+) exhibit high solubility and ionic conductivity, making them optimal components in aqueous electrolytes. Despite the conventional belief that AM+ are chemically inert spectators, the strong dependence of electrocatalysis on AM+ has recently provoked debates about their unforeseen catalytic role. However, conclusive evidence is still lacking. Here we demonstrate that AM+ can couple with reaction intermediates and determine kinetics as homogeneous cocatalysts in aqueous conditions, for the alkaline oxygen reduction reaction on a carbon catalyst. In situ X-ray absorption spectroscopy reveals a change in the electronic structure of Na+ from its hydrated state on a charged electrode. In situ Raman spectroscopy further identifies that this change is due to the formation of water-unstable NaO2 as a key intermediate in OOH− production. Together with theoretical calculations, this finding enunciates the counterintuitive cocatalytic role of AM+ in aqueous environments, highlighting the exigency of refined interface design principles for better electrocatalysis. Alkali cations in electrolytes are commonly considered chemically inert species, but their role has recently been called into question. Now, using in situ spectroscopy and molecular dynamics simulations, it is shown that alkali cations couple with intermediates in the oxygen reduction reaction, acting as cocatalysts.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 12","pages":"1330-1338"},"PeriodicalIF":42.8,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858064","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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Polymer-decorated bacteria for cascade catalysis

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01273-7

Andrea Belluati, Nico Bruns

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An unsung hero in electrochemistry

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01265-7

Yang-Fan Xu, Xiangfeng Chen, Xiangdong Yao

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Merging photoredox with metalloenzymatic catalysis for enantioselective decarboxylative C(sp3)‒N3 and C(sp3)‒SCN bond formation

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01257-7

Jinyan Rui, Xinpeng Mu, Jordi Soler, Jared C. Paris, Yisong Guo, Marc Garcia-Borràs, Xiongyi Huang

{"title":"Merging photoredox with metalloenzymatic catalysis for enantioselective decarboxylative C(sp3)‒N3 and C(sp3)‒SCN bond formation","authors":"Jinyan Rui, Xinpeng Mu, Jordi Soler, Jared C. Paris, Yisong Guo, Marc Garcia-Borràs, Xiongyi Huang","doi":"10.1038/s41929-024-01257-7","DOIUrl":"10.1038/s41929-024-01257-7","url":null,"abstract":"The scope of nature’s catalytic abilities has been expanded by recent advancements in biocatalysis to include synthetic transformations with no biological equivalent. However, these newly introduced catalytic functions represent only a small fraction of reactions utilized in synthetic catalysis. Here we present a biocatalytic platform that combines photoredox and metalloenzymatic catalysis for enantioselective radical transformations. Under green light irradiation, the eosin Y photocatalyst enables 4-hydroxyphenylpyruvate dioxygenases to catalyse enantioselective decarboxylative azidation and thiocyanation of N-hydroxyphthalimide esters. The final optimized variant obtained through directed evolution can afford diverse chiral organic azide and thiocyanate compounds with up to 77% yield, 385 total turnovers and 94% enantiomeric excess. Mechanistic studies show that the eosin Y catalyst mediates the generation of both C(sp3) radical and Fe(III)‒N3/Fe(III)‒NCS intermediate, leading to efficient enantioselective C‒N3 and C‒SCN bond formation in the enzyme active site. These findings establish an adaptable biocatalytic platform for introducing abiological metallophotoredox catalysis into biology. Decarboxylative azidation is a valuable transformation in organic chemistry, but a biocatalytic equivalent remained elusive. Now merging photoredox with metalloenzymatic catalysis enables the enantioselective decarboxylative radical azidation and thiocyanation of N-hydroxyphthalimide esters.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 12","pages":"1394-1403"},"PeriodicalIF":42.8,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858194","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}

引用次数: 0

Methanotrophic catalysis for methane oxidation to formaldehyde

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01252-y

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Earth-abundant electrocatalysts for acidic oxygen evolution 用于酸性氧进化的地球富集电催化剂

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-17 DOI: 10.1038/s41929-024-01266-6

Rendian Wan, Tenghui Yuan, Liuchen Wang, Bing Li, Meilin Liu, Bote Zhao

{"title":"Earth-abundant electrocatalysts for acidic oxygen evolution","authors":"Rendian Wan, Tenghui Yuan, Liuchen Wang, Bing Li, Meilin Liu, Bote Zhao","doi":"10.1038/s41929-024-01266-6","DOIUrl":"10.1038/s41929-024-01266-6","url":null,"abstract":"Proton-exchange membrane water electrolysis is a promising technology for green hydrogen production, but its widespread commercialization is hindered by the high cost and scarcity of precious-metal-based catalysts for the oxygen evolution reaction (OER). Recent progress has been made in developing low-cost, earth-abundant electrocatalysts for the acidic OER, but little is known about degradation pathways. This makes the design of active and robust catalysts challenging. Here we review recent advances in the design of earth-abundant catalysts for the acidic OER, examining the degradation mechanisms from the device level to the catalyst electronic structure level, and highlighting the relevant characterization techniques. We discuss the thermodynamic and kinetic stability of the catalysts and present a quantitative comparative analysis of electrochemical data to evaluate different materials and design strategies for catalysts. We also examine the performance of the catalysts in proton-exchange membrane water electrolysers and conclude with a discussion of the key scientific challenges and future perspectives in the field. Proton-exchange membrane water electrolysers often rely on scarce iridium or ruthenium catalysts at the anode, as many low-cost, earth-abundant catalysts cannot withstand the harsh operational conditions. This Review discusses the state of the art in earth-abundant water oxidation catalysts and examines their degradation mechanisms at multiple levels.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 12","pages":"1288-1304"},"PeriodicalIF":42.8,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832610","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}

引用次数: 0