Nature Catalysis最新文献_第7页

Understanding the interplay between electrocatalytic C(sp3)‒C(sp3) fragmentation and oxygenation reactions 了解电催化 C(sp3)-C(sp3)碎片化和加氧反应之间的相互作用

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-29 DOI: 10.1038/s41929-024-01218-0

Christine Lucky, Shengli Jiang, Chien-Rung Shih, Victor M. Zavala, Marcel Schreier

{"title":"Understanding the interplay between electrocatalytic C(sp3)‒C(sp3) fragmentation and oxygenation reactions","authors":"Christine Lucky, Shengli Jiang, Chien-Rung Shih, Victor M. Zavala, Marcel Schreier","doi":"10.1038/s41929-024-01218-0","DOIUrl":"10.1038/s41929-024-01218-0","url":null,"abstract":"Achieving the selective electrocatalytic activation of C(sp3)–C(sp3) and C(sp3)−H bonds is key to enabling the electricity-driven synthesis of chemicals, the sustainable upgrading of plastics and the development of fuel cells operating on energy-dense liquid fuels. When exposed to electrodes under oxidative bias, hydrocarbons undergo both C–C bond fragmentation and oxygenation. Currently, we lack control over the bifurcation of these pathways. Here we provide insights into the complex network of alkyl transformation reactions, showing that under oxidizing potentials, adsorbed butane transforms to adsorbed CHx fragments, which can be desorbed as methane before oxidation to adsorbed CO. Identifying the branchpoint between C‒C fragmentation and oxygenation allowed us to steer selectivity by applying pulsed potentials tailored to the desorption potential of specific adsorbates and the kinetics of intermediate oxidation. Our findings provide design criteria for improved fuel cell catalysts and open the door to selective C‒C cleavage in electrosynthetic pathways. The electrochemical activation of alkanes on metal catalysts is a complex process that is not fully understood. Now an electrochemical protocol is put forward to isolate the adsorption, fragmentation and oxygenation potential-dependent steps of butane activation on a platinum electrode and derive its intricate reaction network.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 9","pages":"1021-1031"},"PeriodicalIF":42.8,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142089960","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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Organocatalytic acylation of remote arene C–H bonds 远端芳烃 C-H 键的有机催化酰化反应

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-27 DOI: 10.1038/s41929-024-01195-4

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Radical control for enantioselective Csp3–Csp3 cross-coupling 对映选择性 Csp3-Csp3 交叉偶联的辐射控制

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-27 DOI: 10.1038/s41929-024-01208-2

Ju Byeong Chae, Annika R. Holm, Liviu M. Mirica

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Reshaping catalysis beyond the conventional 超越传统，重塑催化

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-27 DOI: 10.1038/s41929-024-01212-6

Amani M. Ebrahim

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A structured catalyst for anion exchange membrane water electrolysis 用于阴离子交换膜电解水的结构催化剂

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-27 DOI: 10.1038/s41929-024-01210-8

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Harnessing electron-rich arenes in nickel photoredox catalysis 在镍光氧化催化中利用富电子烯烃

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-27 DOI: 10.1038/s41929-024-01196-3

Sneha Nayak, Laura K. G. Ackerman-Biegasiewicz

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Identifying restructured motifs on iridium oxide catalyst surfaces for water electrolysis 识别电解水用氧化铱催化剂表面的重组图案

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-27 DOI: 10.1038/s41929-024-01201-9

引用次数: 0

Atomically dispersed ruthenium hydride on beta zeolite as catalysts for the isomerization of muconates 原子分散的氢化钌在β沸石上作为短碳酸盐异构化的催化剂

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-19 DOI: 10.1038/s41929-024-01205-5

Ibrahim Khalil, Marco Giulio Rigamonti, Kwinten Janssens, Aram Bugaev, Daniel Arenas Esteban, Sven Robijns, Thibaut Donckels, Mostafa Torka Beydokhti, Sara Bals, Dirk De Vos, Michiel Dusselier

{"title":"Atomically dispersed ruthenium hydride on beta zeolite as catalysts for the isomerization of muconates","authors":"Ibrahim Khalil, Marco Giulio Rigamonti, Kwinten Janssens, Aram Bugaev, Daniel Arenas Esteban, Sven Robijns, Thibaut Donckels, Mostafa Torka Beydokhti, Sara Bals, Dirk De Vos, Michiel Dusselier","doi":"10.1038/s41929-024-01205-5","DOIUrl":"10.1038/s41929-024-01205-5","url":null,"abstract":"Searching for sustainable polymers requires access to biomass-based monomers. In that sense, glucose-derived cis,cis-muconic acid stands as a high-potential intermediate. However, to unlock its potential, an isomerization to the value-added trans,trans-isomer, trans,trans-muconic acid, is required. Here we develop atomically dispersed low-loaded Ru on beta zeolite catalysts that produce trans,trans-muconate in ethanol with total conversion (to equilibrium) and a selectivity of >95%. We reach very high turnovers per Ru and productivity rates of 427 mM h−1 (~85 g l−1 h−1), surpassing the bio-based cis,cis-muconic acid production rates by an order of magnitude. By coupling isomerization to Diels–Alder cycloaddition, terephthalate intermediates are produced in around 90% yields, circumventing the isomer equilibrium. Isomerization is promoted by Ru hydride species where the hydrides are generated from the alcohol solvent, as evidenced by Fourier transform infrared spectroscopy. Beyond isomerization, the Ru–zeolite and its hydride-forming capacity could be of use as a heterogeneous catalyst for other hydride chemistries, demonstrated by a successful hydride transfer hydrogenation. Muconic acid is an important bio-based chemical; however its applications are limited by the lack of efficient methods to access its trans,trans-isomer. Here the authors address this problem with a catalyst based on single Ru atoms dispersed on zeolite BEA that is capable of unlocking hydride chemistries.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 8","pages":"921-933"},"PeriodicalIF":42.8,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007382","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

Overcoming limitations in non-activated alkene cross-coupling with nickel catalysis and anionic ligands 利用镍催化和阴离子配体克服非活化烯烃交叉偶联的局限性

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-15 DOI: 10.1038/s41929-024-01211-7

Dong Wu, Weiyu Kong, Yang Bao, Chengmi Huang, Wei Liu, Yuqiang Li, Guoyin Yin

{"title":"Overcoming limitations in non-activated alkene cross-coupling with nickel catalysis and anionic ligands","authors":"Dong Wu, Weiyu Kong, Yang Bao, Chengmi Huang, Wei Liu, Yuqiang Li, Guoyin Yin","doi":"10.1038/s41929-024-01211-7","DOIUrl":"10.1038/s41929-024-01211-7","url":null,"abstract":"Multicomponent cross-coupling reactions involving alkenes represent a compelling strategy for accessing three-dimensional molecules, a key pursuit in contemporary medicinal chemistry. Transition metal-catalysed processes predominantly necessitate the use of conjugated alkenes or non-activated alkenes equipped with specific auxiliary functional groups, for example, 8-aminoquinoline. However, it remains a huge challenge to directly use unmodified native functional groups, such as alcohols and ethers, as directing groups. Here, by utilizing an anionic bidentate ligand such as acac, we have successfully addressed the challenge of employing weakly coordinating native functional groups as directing groups in a nickel-catalysed cross-coupling of non-activated alkenes. This reaction enables the simultaneous introduction of an sp2 fragment and an sp3 fragment to two carbons of the alkenes with high chemo- and regioselectivity. This work demonstrates the advantages and potential of anionic bidentate ligands in the cross-coupling of non-activated alkenes. The transition metal-catalysed multicomponent cross-coupling of alkenes currently relies on strongly coordinating groups to direct the reactivity. Now Wu et al. present a nickel catalyst that enables the installation of sp2 and sp3 fragments on alkenes using alcohols and ethers as directing groups.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 11","pages":"1154-1164"},"PeriodicalIF":42.8,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141986498","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

Radical strain-release photocatalysis for the synthesis of azetidines 用于合成氮杂环丁烷的自由基应变释放光催化技术

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-14 DOI: 10.1038/s41929-024-01206-4

Ricardo I. Rodríguez, Vasco Corti, Lorenzo Rizzo, Stefano Visentini, Marco Bortolus, Agnese Amati, Mirco Natali, Giorgio Pelosi, Paolo Costa, Luca Dell’Amico

{"title":"Radical strain-release photocatalysis for the synthesis of azetidines","authors":"Ricardo I. Rodríguez, Vasco Corti, Lorenzo Rizzo, Stefano Visentini, Marco Bortolus, Agnese Amati, Mirco Natali, Giorgio Pelosi, Paolo Costa, Luca Dell’Amico","doi":"10.1038/s41929-024-01206-4","DOIUrl":"10.1038/s41929-024-01206-4","url":null,"abstract":"The increasing popularity of four-member rings in drug discovery has prompted the synthetic chemistry community to advance and reinvent old strategies to craft these structures. Recently, the strain-release concept has been used to build complex architectures. However, although there are many strategies for accessing small carbocyclic derivatives, the synthesis of azetidines remains underdeveloped. Here we report a photocatalytic radical strategy for accessing densely functionalized azetidines from azabicyclo[1.1.0]butanes. The protocol operates with an organic photosensitizer, which finely controls the key energy-transfer process with distinct types of sulfonyl imines. The radical intermediates are intercepted by the azabicyclo[1.1.0]butanes via a radical strain-release process, providing access to difunctionalized azetidines in a single step. This radical process is revealed by a combination of spectroscopic and optical techniques and density functional theory calculations. The power and generality of this method is illustrated with the synthesis of various azetidine targets, including derivatives of celecoxib and naproxen. Four-membered rings have become popular motifs in drug discovery, prompting the synthetic organic chemistry community to develop more expedite approaches to access these scaffolds. Here, the authors report a photocatalytic radical strategy for accessing densely functionalized azetidines from azabicyclo[1.1.0]butanes.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 11","pages":"1223-1231"},"PeriodicalIF":42.8,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01206-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141980821","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