Nature Catalysis最新文献_第2页

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":null,"pages":null},"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 37.8 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":"https://doi.org/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.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"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 37.8 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":"https://doi.org/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.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","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":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Seed-assisted formation of NiFe anode catalysts for anion exchange membrane water electrolysis at industrial-scale current density 种子辅助形成用于工业规模电流密度阴离子交换膜电解水的镍铁合金阳极催化剂

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-13 DOI: 10.1038/s41929-024-01209-1

Zhiheng Li, Gaoxin Lin, Linqin Wang, Husileng Lee, Jian Du, Tang Tang, Guoheng Ding, Rong Ren, Wenlong Li, Xing Cao, Shiwen Ding, Wentao Ye, Wenxing Yang, Licheng Sun

{"title":"Seed-assisted formation of NiFe anode catalysts for anion exchange membrane water electrolysis at industrial-scale current density","authors":"Zhiheng Li, Gaoxin Lin, Linqin Wang, Husileng Lee, Jian Du, Tang Tang, Guoheng Ding, Rong Ren, Wenlong Li, Xing Cao, Shiwen Ding, Wentao Ye, Wenxing Yang, Licheng Sun","doi":"10.1038/s41929-024-01209-1","DOIUrl":"10.1038/s41929-024-01209-1","url":null,"abstract":"Alkaline oxygen evolution reaction is critical for green hydrogen production from water electrolysis but encounters great challenges when operated at industry-required ampere-scale current densities, such as insufficient mass transfer, reduced catalytic activity and limited lifetimes. Here we develop a one-step seed-assisted heterogeneous nucleation method (25 °C, 24 h) for producing a nickel–iron-based electrocatalyst (CAPist-L1, where CAP refers to the centre of artificial photosynthesis) for robust oxygen evolution reaction at ≥1,000 mA cm−2. Based on the insoluble nanoparticles in the heterogeneous nucleation system, a dense interlayer is formed that anchors the catalyst layer tightly on the substrate, ensuring stable long-term durability of 15,200 h (>21 months) in 1 M KOH at 1,000 mA cm−2. When applying CAPist-L1 as the anode catalyst in practical anion exchange membrane water electrolysis, it delivers a high activity of 7,350 mA cm−2 at 2.0 V and good stability at 1,000 mA cm−2 for 1,500 h at 80 °C. Anion exchange membrane water electrolysis is a promising technology for H2 production using precious metal-free catalysts, but certain hurdles persist for its broad deployment such as the operational stability of its anode catalyst. Now a seed-assisted heterogeneous nucleation method is put forward to prepare a NiFe catalyst with high activity and a stability of over 21 months at 1 A cm−2.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":42.8,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141974101","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

Iridium nitrenoid-enabled arene C−H functionalization 氮化铱使炔烃 C-H 功能化

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-08-12 DOI: 10.1038/s41929-024-01207-3

Liang-Wen Qi, Torben Rogge, K. N. Houk, Yixin Lu

{"title":"Iridium nitrenoid-enabled arene C−H functionalization","authors":"Liang-Wen Qi, Torben Rogge, K. N. Houk, Yixin Lu","doi":"10.1038/s41929-024-01207-3","DOIUrl":"10.1038/s41929-024-01207-3","url":null,"abstract":"Direct arene C−H functionalization via nucleophilic aromatic substitution remains a challenging task. Here we report an iridium nitrenoid-catalysed arene C−H functionalization strategy, making use of readily available aryl azides as electrophiles to react with different nucleophilic reaction partners. The practicality of this methodology is demonstrated by enantioselective synthesis of chiral 2-amino-2′-hydroxy-1,1′-binaphthyl, a class of building blocks, ligands and catalysts in asymmetric transformation, using β-naphthols and β-naphthyl azides as starting materials under the catalysis of a tailored oxazoline-chelated iridium complex. Mechanistic studies and density functional theory calculations show that the reaction proceeds through an iridium nitrenoid-mediated C−H functionalization pathway. The reported arene C−H functionalization strategy serves as a blueprint to expand the applicability of nucleophilic aromatic substitution reactions and is particularly valuable for the synthesis of aniline-containing molecules. Effective strategies for direct arene C−H functionalization are sought after. Here arene C−H functionalization via iridium nitrenoid-catalysed nucleophilic aromatic substitution allows the coupling of aryl azides with different carbon nucleophiles and is applied to the enantioselective synthesis of NOBINs","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":42.8,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141918856","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

Electrochemical nitrate reduction to ammonia with cation shuttling in a solid electrolyte reactor 在固体电解质反应器中通过阳离子穿梭进行硝酸盐还原成氨的电化学反应

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-08-12 DOI: 10.1038/s41929-024-01200-w

Feng-Yang Chen, Ahmad Elgazzar, Stephanie Pecaut, Chang Qiu, Yuge Feng, Sushanth Ashokkumar, Zhou Yu, Chase Sellers, Shaoyun Hao, Peng Zhu, Haotian Wang

{"title":"Electrochemical nitrate reduction to ammonia with cation shuttling in a solid electrolyte reactor","authors":"Feng-Yang Chen, Ahmad Elgazzar, Stephanie Pecaut, Chang Qiu, Yuge Feng, Sushanth Ashokkumar, Zhou Yu, Chase Sellers, Shaoyun Hao, Peng Zhu, Haotian Wang","doi":"10.1038/s41929-024-01200-w","DOIUrl":"https://doi.org/10.1038/s41929-024-01200-w","url":null,"abstract":"While electrochemical nitrate reduction to ammonia represents a promising route for water treatment and ammonia generation, one critical challenge in the field is the need for high-concentration supporting electrolytes in this electrochemical system. Here we report a three-chamber porous solid electrolyte reactor design coupled with cation shielding effects for efficient nitrate reduction reaction without supporting electrolytes. By feeding treated water from the cathode chamber to the middle porous solid electrolyte layer, we can realize an alkali metal cation shuttling loop from the middle layer back into the cathode chamber to boost the nitrate reduction selectivity and suppress the hydrogen evolution side reaction. This reactor system can deliver high ammonia Faradaic efficiencies (>90%) at practical current densities (>100 mA cm−2) under a typical wastewater nitrate concentration of 2,000 ppm, enabling a high-purity water effluent and NH3(g) as products with no need for electrolyte recovery processes.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141974103","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

Carbon monoxide enabling synergistic carbonylation and (hetero)aryl migration 一氧化碳促成协同羰基化和（杂）芳基迁移

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-08-06 DOI: 10.1038/s41929-024-01204-6

Yuanrui Wang, Hefei Yang, Yan Zheng, Mingxia Hu, Jintao Zhu, Zhi-Peng Bao, Yanying Zhao, Xiao-Feng Wu

引用次数: 0

A red-light-powered silicon nanowire biophotochemical diode for simultaneous CO2 reduction and glycerol valorization 红光供电的硅纳米线生物光化学二极管，可同时实现二氧化碳还原和甘油增值

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-07-30 DOI: 10.1038/s41929-024-01198-1

Jimin Kim, Jia-An Lin, Jinhyun Kim, Inwhan Roh, Soohyung Lee, Peidong Yang

{"title":"A red-light-powered silicon nanowire biophotochemical diode for simultaneous CO2 reduction and glycerol valorization","authors":"Jimin Kim, Jia-An Lin, Jinhyun Kim, Inwhan Roh, Soohyung Lee, Peidong Yang","doi":"10.1038/s41929-024-01198-1","DOIUrl":"https://doi.org/10.1038/s41929-024-01198-1","url":null,"abstract":"A bias-free photochemical diode, in which a p-type photocathode is connected to an n-type photoanode to harness light for driving photoelectrochemical reduction and oxidation pairs, serves as a platform for realizing light-driven fuel generation from CO2. However, the conventional design, in which cathodic CO2 reduction is coupled with the anodic oxygen evolution reaction (OER), requires substantial energy input. Here we present a photochemical diode device that harnesses red light (740 nm) to simultaneously drive biophotocathodic CO2-to-multicarbon conversion and photoanodic glycerol oxidation as an alternative to the OER to overcome the above thermodynamic limitation. The device consists of an efficient CO2-fixing microorganism, Sporomusa ovata, interfaced with a silicon nanowire photocathode and a Pt–Au-loaded silicon nanowire photoanode. This photochemical diode operates bias-free under low-intensity (20 mW cm−2) red light irradiation with ~80% Faradaic efficiency for both the cathodic and anodic products. This work provides an alternative photosynthetic route to mitigate excessive CO2 emissions and efficiently generate value-added chemicals from CO2 and glycerol.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141794571","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

Catalysing rate and capacity 催化率和催化能力

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-26 DOI: 10.1038/s41929-024-01184-7

Soumyadip Mondal, Stefan A. Freunberger

引用次数: 0