Nature Catalysis最新文献_第4页

Single-turnover subparticle imaging reveals kinetic compensation in electrocatalytic surface water dissociation 单次翻转亚粒子成像揭示了电催化地表水解离的动力学补偿

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-08-13 DOI: 10.1038/s41929-026-01599-4

Lei Fan, Ebrahim Tayyebi, Ctirad Červinka, Hua Li, Jin Xie, Weidong Zhang, Shurui Chen, Jing Zhu, Xiaozhi Xu, Rob Atkin, Ju Li, Kai S. Exner, Xianwen Mao

{"title":"Single-turnover subparticle imaging reveals kinetic compensation in electrocatalytic surface water dissociation","authors":"Lei Fan, Ebrahim Tayyebi, Ctirad Červinka, Hua Li, Jin Xie, Weidong Zhang, Shurui Chen, Jing Zhu, Xiaozhi Xu, Rob Atkin, Ju Li, Kai S. Exner, Xianwen Mao","doi":"10.1038/s41929-026-01599-4","DOIUrl":"10.1038/s41929-026-01599-4","url":null,"abstract":"Bulk measurements obscure critical microscopic variations, limiting the mechanistic understanding of complex electrocatalyst interfaces central to sustainability technologies. Although emerging single-particle techniques address ensemble averaging, they focus on catalyst structure, reactant adsorption or special model reactions, and cannot quantify turnover rates of practical electrocatalytic reactions. Here we report domino-reaction-enabled label-free imaging for nanoscopic electrocatalysis (DELINE), enabling subparticle, single-turnover imaging of surface water dissociation under operando conditions. DELINE decouples size–structure effects in electrocatalysts, reveals unexpected heterogeneity in Volmer transition states and uncovers strong coupling between charge-transfer coefficient and exchange velocity. Using DELINE imaging, we provide evidence of a compensation rule in electrocatalysis, akin to Meyer–Neldel behaviour. Cost-effective and high-throughput, DELINE quantifies key activity descriptors at single-particle/subparticle levels under realistic conditions, bridging the theory–experiment gap and accelerating catalyst screening. Understanding nanoscale heterogeneity in electrocatalytic reactions is critical for advancing catalyst design and performance. Now, a single-turnover imaging technique with subparticle resolution, DELINE, is introduced, which enables the mapping of electrocatalytic reactions and is used to probe surface water dissociation.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 9","pages":"953-964"},"PeriodicalIF":48.3,"publicationDate":"2026-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148728990","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

Catalytic asymmetric intermolecular carbonyl–ene-type reactions of unactivated aldehydes and alkenes 催化非活化醛和烯烃分子间不对称羰基烯型反应

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-08-12 DOI: 10.1038/s41929-026-01589-6

Joyce A. A. Grimm, Lixia Shi, Nobuya Tsuji, Chendan Zhu, Markus Leutzsch, Jan Samsonowicz-Górski, Benjamin List

{"title":"Catalytic asymmetric intermolecular carbonyl–ene-type reactions of unactivated aldehydes and alkenes","authors":"Joyce A. A. Grimm, Lixia Shi, Nobuya Tsuji, Chendan Zhu, Markus Leutzsch, Jan Samsonowicz-Górski, Benjamin List","doi":"10.1038/s41929-026-01589-6","DOIUrl":"10.1038/s41929-026-01589-6","url":null,"abstract":"Carbonyl–ene-type reactions are recognized by chemists for their ability to form carbon–carbon bonds between aldehydes and alkenes, both abundantly available early-stage chemicals. However, despite remarkable progress with intramolecular variants, intermolecular carbonyl–ene-type reactions in which unactivated aldehydes react with unactivated alkenes are underexplored and, to the best of our knowledge, catalytic enantioselective versions have not yet been described. Here we report a solution to this problem that enables a variety of unactivated aromatic and aliphatic aldehydes to be united with alkenes, furnishing highly enantioenriched homoallylic alcohols. The method benefits from the high reactivity of confined silylium ion-based organic Lewis acid catalysts, which, according to computational studies, mediate a cationic Prins-type pathway. Intermolecular asymmetric carbonyl–ene-type reactions of unactivated aldehydes and alkenes remain largely unexplored. Now this transformation is achieved by combining confined imidodiphosphorimidate catalysts with an external silicon source to deliver enantioenriched homoallylic alcohols.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 8","pages":"893-900"},"PeriodicalIF":48.3,"publicationDate":"2026-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-026-01589-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148728991","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}

引用次数: 0

The important ingredient in your catalyst you never meant to add 你的催化剂中最重要的成分，你从没想过要加入

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-08-07 DOI: 10.1038/s41929-026-01596-7

Arun Devaraj

引用次数: 0

Chiral phosphorus by catalyst design 手性磷催化剂设计

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-08-05 DOI: 10.1038/s41929-026-01594-9

Kyle Knouse, David Butler

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Multifunctional chiral bis(amidine) organocatalysts enable stereoselective synthesis of phosphorothioate oligonucleotides 多功能手性双（氨基）有机催化剂可以立体选择性合成硫代寡核苷酸

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-08-05 DOI: 10.1038/s41929-026-01557-0

Shuai-Shuai Fang (, ), Guo-Dong Sun (, ), Jia-Wei Liu (, ), Ming-Hong Li (, ), Tian Xie (, ), Kang-Ning Yuan (, ), Hong-Qing Yao (, ), Yue-Ming Cai (, ), Chunhai Fan (, ), Ming Shang (, )

{"title":"Multifunctional chiral bis(amidine) organocatalysts enable stereoselective synthesis of phosphorothioate oligonucleotides","authors":"Shuai-Shuai Fang \u0000 (, ), Guo-Dong Sun \u0000 (, ), Jia-Wei Liu \u0000 (, ), Ming-Hong Li \u0000 (, ), Tian Xie \u0000 (, ), Kang-Ning Yuan \u0000 (, ), Hong-Qing Yao \u0000 (, ), Yue-Ming Cai \u0000 (, ), Chunhai Fan \u0000 (, ), Ming Shang \u0000 (, )","doi":"10.1038/s41929-026-01557-0","DOIUrl":"10.1038/s41929-026-01557-0","url":null,"abstract":"Phosphorothioate oligonucleotides (PS-ODNs) and cyclic dinucleotides are important therapeutic agents whose activity depends critically on phosphorus stereochemistry. However, existing strategies largely rely on chiral auxiliaries that require multistep installation and removal. Although chiral phosphoric acid catalysis enables diastereoselective synthesis of P-stereogenic dinucleotides via P(III)-phosphoramidite chemistry, this approach fails to access long-chain stereodefined PS-ODNs. Here we report a catalytic asymmetric P(V)-based strategy that enables stereocontrolled synthesis of PS-ODNs and cyclic dinucleotides using chiral organocatalysts. This platform integrates a catalyst-controlled nucleoside loading step with a stereospecific coupling process under mild, redox-neutral conditions. The method exhibits broad substrate scope, enabling efficient construction of diverse P–O, P–S, P–C and P–N linkages with high stereochemical fidelity. Notably, the method enables the stereocontrolled synthesis of PS-ODNs under both 5′ → 3′ and standard 3′ → 5′ solid-phase oligonucleotide synthesis workflows. Mechanistic studies support a cooperative activation mode involving hydrogen bonding, nucleophilic activation and general base catalysis. Existing methodologies for the stereocontrolled synthesis of phosphorothioate oligonucleotides and cyclic dinucleotides generally rely on chiral auxiliaries and are not catalytic. This study reports a catalytic asymmetric P(V)-based strategy, enabled by a C2-symmetric multifunctional chiral bis(amidine) organocatalyst, for the stereoselective synthesis of these classes of compounds.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 8","pages":"800-811"},"PeriodicalIF":48.3,"publicationDate":"2026-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148693495","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

The active site and its environment 活性部位及其环境

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-08-03 DOI: 10.1038/s41929-026-01575-y

Matteo Maestri

引用次数: 0

Uncovering the source of uncertainty 揭示不确定性的根源

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-07-31 DOI: 10.1038/s41929-026-01572-1

Lichen Liu

引用次数: 0

Quantifying uncertainty in catalyst activity and deactivation during CO2 hydrogenation via round-robin testing for data-driven modelling 通过数据驱动模型的循环测试，量化CO2加氢过程中催化剂活性和失活的不确定性

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-07-31 DOI: 10.1038/s41929-026-01559-y

Selin Bac, Dongjae Shin, Seunghwa Hong, Jake Heinlein, Anastassiya Khan, Greg Barber, Zhihengyu Chen, Michael M. Albrechtsen, Christopher Tassone, Robert M. Rioux, Matteo Cargnello, Simon R. Bare, Kirsten Winther, Phillip Christopher, Adam S. Hoffman

{"title":"Quantifying uncertainty in catalyst activity and deactivation during CO2 hydrogenation via round-robin testing for data-driven modelling","authors":"Selin Bac, Dongjae Shin, Seunghwa Hong, Jake Heinlein, Anastassiya Khan, Greg Barber, Zhihengyu Chen, Michael M. Albrechtsen, Christopher Tassone, Robert M. Rioux, Matteo Cargnello, Simon R. Bare, Kirsten Winther, Phillip Christopher, Adam S. Hoffman","doi":"10.1038/s41929-026-01559-y","DOIUrl":"10.1038/s41929-026-01559-y","url":null,"abstract":"Machine learning (ML) is rapidly emerging as a catalyst discovery method, whose success depends on curated experimental datasets with defined uncertainties. Despite this need, uncertainty in catalyst performance is rarely quantified across datasets generated using multiple reactors. Here we present a four-laboratory round-robin study of Rh/TiO2 catalysts for CO2 hydrogenation that demonstrates that accounting for both intra- and interlaboratory variability is essential for identifying features for experimentally derived ML models. Even with identical catalyst batches and testing protocols, relationships between inputs (reaction temperature, Rh loading and synthesis method) and outputs (conversion, selectivity and CO and CH4 production rates) that were clear in intralaboratory studies became statistically insignificant when interlaboratory variability was included. Heat management emerged as a key contributor to this variability. Our work demonstrates that uncertainty analysis must be included in the selection of performance metrics and input features for ML models while revealing sources of variability that limit rigour and reproducibility. This Analysis presents a round-robin study of Rh/TiO2 catalysts for CO2 hydrogenation across four laboratories, quantifying both intralaboratory and interlaboratory variability and discussing the implications of this uncertainty for machine learning predictions.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 8","pages":"912-923"},"PeriodicalIF":48.3,"publicationDate":"2026-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148693533","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

Protein-confined imidazolium intermediates enable diverse biocatalytic C–C and C–N bond formations 蛋白质限制的咪唑中间体使多种生物催化C-C和C-N键形成

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-07-31 DOI: 10.1038/s41929-026-01587-8

Zachary Birch-Price, Amy E. Hutton, Fei Zhao, Mary Ortmayer, Veronika Stoianova, Christian Merten, Colin Levy, Richard Obexer, Anthony P. Green

{"title":"Protein-confined imidazolium intermediates enable diverse biocatalytic C–C and C–N bond formations","authors":"Zachary Birch-Price, Amy E. Hutton, Fei Zhao, Mary Ortmayer, Veronika Stoianova, Christian Merten, Colin Levy, Richard Obexer, Anthony P. Green","doi":"10.1038/s41929-026-01587-8","DOIUrl":"10.1038/s41929-026-01587-8","url":null,"abstract":"Developing enzymatic strategies to selectively construct C–C and C–heteroatom bonds is a major objective in modern biocatalysis. Here we combine genetic code reprogramming and laboratory evolution to establish a family of allylic transferase enzymes that can achieve a remarkable breadth of chemistry, enabling the generation of valuable motifs including γ‑butenolides, chiral amines and all-carbon quaternary centres. Our enzymes operate through the formation of electrophilic imidazolium intermediates that can be generated from reagents equipped with a para-nitrophenol leaving group to facilitate high-throughput evolution. These intermediates can be intercepted with diverse carbon and nitrogen nucleophiles to generate densely functionalized products featuring Cβ or Cγ stereocentres. Interestingly, structural analysis suggests that catalysis proceeds through an unanticipated ternary complex involving para-nitrophenol and the incoming substrate nucleophile. This study adds a family of C–C and C–N bond-forming enzymes to the biocatalytic repertoire and illustrates how artificial enzymes can achieve precise control over challenging chemical conversions. Small catalytic nucleophiles can promote allylic transfer processes, but achieving regio- and stereocontrol is challenging. Here the authors develop a family of allylic transferase enzymes to mediate diverse C–C and C–N bond formations through the confinement of key intermediates within proteins.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 8","pages":"882-892"},"PeriodicalIF":48.3,"publicationDate":"2026-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-026-01587-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148693542","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}

引用次数: 0

Evidence of Eley–Rideal mechanism in Cu-catalysed CO2 electroreduction in flow cells with a protective layer 具有保护层的液流电池中cu催化CO2电还原的eley - ideal机制的证据

IF 48.3 1区化学

Nature Catalysis Pub Date : 2026-07-30 DOI: 10.1038/s41929-026-01584-x

Qiwen Sun, Yao Ye, Zebang Yin, Gong Zhang, Xiaoxia Chang, Jinlong Gong, Bingjun Xu

{"title":"Evidence of Eley–Rideal mechanism in Cu-catalysed CO2 electroreduction in flow cells with a protective layer","authors":"Qiwen Sun, Yao Ye, Zebang Yin, Gong Zhang, Xiaoxia Chang, Jinlong Gong, Bingjun Xu","doi":"10.1038/s41929-026-01584-x","DOIUrl":"10.1038/s41929-026-01584-x","url":null,"abstract":"Understanding the impact of cell architectures on product selectivity and the carbon–carbon coupling mechanism of the CO2 electrochemical reduction reaction remains a central challenge due to the complex mass transport conditions of reactants and intermediates. Here we demonstrate that introducing a porous protective layer on copper-based gas diffusion electrodes in flow cells can modulate the mass transport of both the reactant and an intermediate, and can bridge the activity gap between flow cell and membrane electrode assembly configurations. Electrokinetic investigations in flow cells with and without a protective layer provide direct evidence of the Eley–Rideal mechanism in the copper-catalysed carbon–carbon coupling step. Coelectrolysis of 12CO2/13CO in different reactor configurations reveals that the interfacial microenvironment depends sensitively on the interplay between surface reactions and mass transport from and to the catalyst layer. The roles of cell architecture and mass transport on the selectivity of electrocatalytic CO2 reduction have been challenging to decipher. Here a porous protective layer is used to study the copper-catalysed carbon–carbon coupling step in flow cells, supporting an Eley–Rideal mechanism.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 8","pages":"858-868"},"PeriodicalIF":48.3,"publicationDate":"2026-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148612728","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