Nature Catalysis最新文献_第2页

Cobaltosilicate zeolite beyond platinum catalysts for propane dehydrogenation 钴硅酸盐沸石超越铂催化剂用于丙烷脱氢

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-11 DOI: 10.1038/s41929-025-01320-x

Hang Zhou, Huan Li, Liang Wang, Shengqi Chu, Lujie Liu, Lu Liu, Jizhen Qi, Zhouhong Ren, Anyu Cai, Yu Hui, Yucai Qin, Lijuan Song, Xuedi Qin, Jiaqi Shi, Jue Hou, Yongqi Ding, Jiabi Ma, Shaodan Xu, Xin Tao, Lina Li, Qi Yang, Bingwen Hu, Xi Liu, Liwei Chen, Jianping Xiao, Feng-Shou Xiao

引用次数: 0

Identifying high-spin hydroxyl-coordinated Fe3+N4 as the active centre for acidic oxygen reduction using molecular model catalysts 用分子模型催化剂鉴定高自旋羟基配位Fe3+N4为酸性氧还原活性中心

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-07 DOI: 10.1038/s41929-025-01324-7

Kuang-Min Zhao, Dao-Xiong Wu, Wen-Kun Wu, Jia-Bao Nie, Fu-Shan Geng, Guang Li, Hai-Yan Shi, Sheng-Chao Huang, Huan Huang, Jing Zhang, Zhi-You Zhou, Yu-Cheng Wang, Shi-Gang Sun

{"title":"Identifying high-spin hydroxyl-coordinated Fe3+N4 as the active centre for acidic oxygen reduction using molecular model catalysts","authors":"Kuang-Min Zhao, Dao-Xiong Wu, Wen-Kun Wu, Jia-Bao Nie, Fu-Shan Geng, Guang Li, Hai-Yan Shi, Sheng-Chao Huang, Huan Huang, Jing Zhang, Zhi-You Zhou, Yu-Cheng Wang, Shi-Gang Sun","doi":"10.1038/s41929-025-01324-7","DOIUrl":"https://doi.org/10.1038/s41929-025-01324-7","url":null,"abstract":"Fe–N–C catalysts are the most promising alternative to Pt for the acidic oxygen reduction reaction (ORR), yet the electronic structure of their active centres remains elusive. Here we synthesize and characterize a conjugate-bridged iron phthalocyanine (FePc) dimer model catalyst with identical Fe sites and catalytic activity comparable to actual catalysts. A high-spin trivalent FeN4 with an axial hydroxyl ligand, denoted as OH–Fe3+N4 (S = 5/2), is identified as the active state. By contrast, monomer and non-conjugated dimer manifest the OH–Fe3+N4 (S = 3/2) state with an excessive adsorption energy of ORR intermediates. Polymerized FePc is composed of 35% of the S = 5/2 state and 65% of the Fe2+N4 (S = 0 or 1) state, showing a general weaker adsorption energy. Both overly strong and weak adsorption energy hinder the ORR. Theoretical calculations indicate that π–d interaction between Fe and the conjugated carbon plane dictates the spin state. This study will help to precisely design Fe-based ORR catalysts.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"59 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143790086","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

Enantioselective macrocyclization via catalytic metallic dipole relay 通过催化金属偶极中继实现对映体选择性大环化

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-04 DOI: 10.1038/s41929-025-01322-9

Bao-Le Qu, Meng Xiao, Lin He, Jun-Wei Shi, Zhihan Zhang, Wen-Jing Xiao, Liang-Qiu Lu

{"title":"Enantioselective macrocyclization via catalytic metallic dipole relay","authors":"Bao-Le Qu, Meng Xiao, Lin He, Jun-Wei Shi, Zhihan Zhang, Wen-Jing Xiao, Liang-Qiu Lu","doi":"10.1038/s41929-025-01322-9","DOIUrl":"https://doi.org/10.1038/s41929-025-01322-9","url":null,"abstract":"Chiral macrocycles play critical roles across medicinal chemistry and materials science, yet their catalytic asymmetric synthesis remains challenging. Existing methods predominantly rely on intramolecular cyclization of linear precursors and asymmetric resolution of racemic macrocycles, often requiring complex synthesis while offering limited structural diversity. Here, inspired by non-ribosomal cyclopeptide biosynthesis, we present a catalytic metallic dipole relay strategy for the construction of axially chiral macrolactones. This approach enables concise enantioselective synthesis through stepwise strain release in biaryl lactones and dynamic kinetic resolution mediated by π-allyl-Pd dipoles. The method demonstrates broad applicability to medium (up to 91% yield with 93% enantiomeric excess) and large (up to 93% yield with 99% enantiomeric excess and >19:1 diastereomeric ratio) ring systems under mild conditions. By establishing stereochemical control during both medium-ring formation and subsequent macrocyclization, this strategy overcomes traditional limitations in the generation of axial chirality while extending the methodology of transition-metal-catalysed asymmetric cyclization.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"77 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143775496","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 oxidation of nitric oxide to concentrated nitric acid with carbon-based catalysts at near-ambient conditions 近环境条件下用碳基催化剂将一氧化氮电化学氧化为浓硝酸

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-03 DOI: 10.1038/s41929-025-01315-8

Rong Xia, Sydnee Dronsfield, Ahryeon Lee, Bradie S. Crandall, Jiashun Liang, Bjorn Hasa, Andy Redder, Gang Wu, Tiago J. Goncalves, Samira Siahrostami, Feng Jiao

{"title":"Electrochemical oxidation of nitric oxide to concentrated nitric acid with carbon-based catalysts at near-ambient conditions","authors":"Rong Xia, Sydnee Dronsfield, Ahryeon Lee, Bradie S. Crandall, Jiashun Liang, Bjorn Hasa, Andy Redder, Gang Wu, Tiago J. Goncalves, Samira Siahrostami, Feng Jiao","doi":"10.1038/s41929-025-01315-8","DOIUrl":"https://doi.org/10.1038/s41929-025-01315-8","url":null,"abstract":"Nitric oxide (NO) emissions pose significant environmental challenges that demand sustainable remediation strategies. Here we report an electrochemical approach to convert NO into salt-free, concentrated nitric acid (HNO3) using a carbon-based catalyst at near-ambient conditions. The system achieves >90% HNO3 Faradaic efficiency (FE) at 100 mA cm−2 with pure NO and retains >70% FE with dilute NO (0.5 vol%). Mechanistic studies identified nitrous acid as a critical intermediate, diverging from conventional thermocatalytic nitrogen dioxide pathways. By implementing a vapour-fed strategy in a membrane electrode assembly electrolyser, we directly synthesized 32 wt% HNO3 from NO and deionized water, achieving 86% FE at 800 mA cm−2 without electrolyte additives or downstream purification. This work establishes an electrochemical route to valorize NO emissions to high-purity HNO3, advancing sustainable pollution mitigation and chemical manufacturing.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"21 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766524","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

Breaking the linear scaling limit in multi-electron-transfer electrocatalysis through intermediate spillover 通过中间溢出打破多电子转移电催化的线性结垢极限

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-02 DOI: 10.1038/s41929-025-01323-8

Qilun Wang, Sung-Fu Hung, Kejie Lao, Xiang Huang, Fuhua Li, Hua Bing Tao, Hong Bin Yang, Wei Liu, Weijue Wang, Yaqi Cheng, Nozomu Hiraoka, Liping Zhang, Junming Zhang, Yuhang Liu, Jiazang Chen, Yinghua Xu, Chenliang Su, Jingguang G. Chen, Bin Liu

{"title":"Breaking the linear scaling limit in multi-electron-transfer electrocatalysis through intermediate spillover","authors":"Qilun Wang, Sung-Fu Hung, Kejie Lao, Xiang Huang, Fuhua Li, Hua Bing Tao, Hong Bin Yang, Wei Liu, Weijue Wang, Yaqi Cheng, Nozomu Hiraoka, Liping Zhang, Junming Zhang, Yuhang Liu, Jiazang Chen, Yinghua Xu, Chenliang Su, Jingguang G. Chen, Bin Liu","doi":"10.1038/s41929-025-01323-8","DOIUrl":"https://doi.org/10.1038/s41929-025-01323-8","url":null,"abstract":"The linear scaling relationships between the adsorption energies of multiple intermediates constrain the maximum reaction activity of heterogeneous catalysis. Here we propose an intermediate spillover strategy to decouple the elementary electron-transfer steps in an electrochemical reaction by building a bi-component interface, thereby independently tuning the corresponding intermediate adsorption at an individual catalytic surface. Taking the electrocatalytic oxygen reduction reaction as an example, oxophilic sites are preferable for activating oxygen molecules, then the adsorbed OH* intermediates spontaneously migrate to the adjacent sites with a weaker oxygen binding energy, where OH* intermediates are further reduced and desorbed to complete the overall catalytic cycle. Consequently, the designed Pd/Ni(OH)2 catalyst can remarkably elevate the half-wave potential of the oxygen reduction reaction to ~70 mV higher than that of the Pt/C catalyst, surmounting the theoretical overpotential limit of Pd. This design principle highlights an opportunity for utilizing intermediate spillover to break the ubiquitous scaling relationships in multi-step catalytic reactions.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"38 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758679","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

Efficient electroreduction of carbonyl compounds to alcohols over Fe/Fe2O3 interfaces 羰基化合物在Fe/Fe2O3界面上高效电还原为醇

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-02 DOI: 10.1038/s41929-025-01316-7

Jin Lin, Zhenpeng Liu, Haofei Wu, Zhiqi Wang, Guangqiu Wang, Ju Bu, Yanan Wang, Pan Liu, Junjie Wang, Jian Zhang

{"title":"Efficient electroreduction of carbonyl compounds to alcohols over Fe/Fe2O3 interfaces","authors":"Jin Lin, Zhenpeng Liu, Haofei Wu, Zhiqi Wang, Guangqiu Wang, Ju Bu, Yanan Wang, Pan Liu, Junjie Wang, Jian Zhang","doi":"10.1038/s41929-025-01316-7","DOIUrl":"https://doi.org/10.1038/s41929-025-01316-7","url":null,"abstract":"Catalytic hydrogenation of carbonyl compounds is widely used in chemical manufacturing and biomass refining, but current thermocatalytic processes require elevated temperatures, high-pressure H2 and expensive catalysts. Here we demonstrate an electroreduction of carbonyl compounds over Fe/Fe2O3 interfaces in Fe/Fe2O3 nanoarrays (Fe/Fe2O3 NAs), where Fe and Fe2O3 species synergistically accelerate the kinetics of acetone hydrogenation by promoting acetone adsorption and H* formation. With acetone as the probe molecule, an isopropanol partial current density of 1.6 A cm−2 and ~100% selectivity are achieved in 1 M KOH aqueous solution. Even in a large-scale, two-electrode electrolyser, Fe/Fe2O3 NAs stably deliver an acetone conversion of >99%, an isopropanol selectivity of 100%, and an isopropanol production rate of 21.6 g gcat−1 h−1 at 0.2 A cm−2 over a 1,000-h operation. Moreover, Fe/Fe2O3 NAs were applied in the electrochemical hydrogenation of various carbonyl compounds to corresponding alcohols with high conversion rates and selectivities.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"12 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758678","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

Wireless potentiometry of thermochemical heterogeneous catalysis 热化学非均相催化的无线电位测定

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-02 DOI: 10.1038/s41929-025-01308-7

Neil K. Razdan, Karl S. Westendorff, Yogesh Surendranath

{"title":"Wireless potentiometry of thermochemical heterogeneous catalysis","authors":"Neil K. Razdan, Karl S. Westendorff, Yogesh Surendranath","doi":"10.1038/s41929-025-01308-7","DOIUrl":"https://doi.org/10.1038/s41929-025-01308-7","url":null,"abstract":"The electrochemical potential of a catalyst defines the free-energy landscape of catalysis in liquid media and is readily measured for catalysts supported on conductive materials or wired to external circuits. However, the potential is difficult to quantify for thermochemical catalysts supported on electrical insulators, thereby impeding a unifying understanding of the role of electrochemical polarization during thermochemical catalysis. Here we develop a methodology to quantify the electrochemical potential of metal catalysts supported on insulators by introducing low concentrations of redox-active molecules that establish wireless electrical connections between the catalyst and a sensing electrode. Using this approach in tandem with simultaneous rate measurements, we demonstrate distinct rate-potential scalings for oxidative dehydrogenation of formic acid on SiO2-supported and Al2O3-supported versus TiO2-supported Pt and find deactivation modes specific to SiO2-supported Pt. These developments enable the comprehensive investigation of the role of electrochemical polarization in thermochemical catalysis and complement the existing toolkit for mechanistic investigation in catalysis.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"107 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758676","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

Precision installation of silyl synthetic handles within arenes by regiocontrolled ruthenium C(sp2)–H functionalization 区域控制钌C(sp2) -H功能化在芳烃内精确安装硅基合成手柄

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-02 DOI: 10.1038/s41929-025-01309-6

Jamie H. Docherty, Mishra Deepak Hareram, Luke M. Nichols, Ignacio Pérez-Ortega, Iñigo J. Vitorica-Yrezabal, Igor Larrosa

{"title":"Precision installation of silyl synthetic handles within arenes by regiocontrolled ruthenium C(sp2)–H functionalization","authors":"Jamie H. Docherty, Mishra Deepak Hareram, Luke M. Nichols, Ignacio Pérez-Ortega, Iñigo J. Vitorica-Yrezabal, Igor Larrosa","doi":"10.1038/s41929-025-01309-6","DOIUrl":"https://doi.org/10.1038/s41929-025-01309-6","url":null,"abstract":"The site-selective functionalization of C(sp2)–H bonds represents a powerful strategy for the synthesis of structurally diverse compounds with broad applicability. Here we report efficient regioselective catalytic methods for the formation of benzyltrimethylsilanes through ruthenium-catalysed C(sp2)–H silylmethylation. The developed protocols enable selective functionalization at both ortho and meta positions within arenes bearing N-based directing groups. The resulting silylmethyl compounds can undergo diverse transformations, including nucleophilic aromatic substitution, carbonyl addition, olefination and desilylation. Significantly, the regiodivergent installation of silylmethyl synthetic handles allows for the synthesis of the pharmaceutical losmapimod and could further be applied in direct late-stage functionalizations. Mechanistically, an essential role for biscyclometallated ruthenium(II) species has been found, with the formation of intermediate ruthenium(III) species indicated by paramagnetic NMR experiments. These synthetic inventions and mechanistic elucidations signify a transformative step within ruthenium-catalysed C(sp2)–H functionalization, enabling diverse syntheses and providing a framework for future development.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"18 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758677","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

Photoinduced nickel-catalysed enantioconvergent sp3–sp3 coupling of unactivated olefins and aziridines 光诱导镍催化的非活化烯烃和叠氮醚的对映收敛sp3-sp3偶联

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-03-28 DOI: 10.1038/s41929-025-01319-4

Liangliang Zhang, Hao Wang, Tomás G. Santiago, Wen-Jun Yue, Ruben Martin

{"title":"Photoinduced nickel-catalysed enantioconvergent sp3–sp3 coupling of unactivated olefins and aziridines","authors":"Liangliang Zhang, Hao Wang, Tomás G. Santiago, Wen-Jun Yue, Ruben Martin","doi":"10.1038/s41929-025-01319-4","DOIUrl":"https://doi.org/10.1038/s41929-025-01319-4","url":null,"abstract":"Catalytic sp3–sp3 bond-forming reactions have been the subject of considerable interest in both academic and pharmaceutical laboratories. This is largely due to the observation that a higher content of sp3-hybridized carbons has recently been shown to improve several molecular attributes that contribute to clinical success. Although the ready availability of unactivated olefins and aziridines makes them ideal precursors to forge enantioenriched sp3–sp3 architectures with added-value amine functions, an enantioconvergent catalytic scenario of these counterparts has not yet been realized. Here we describe a nickel-catalysed blueprint that enables the enantioselective construction of amine-containing sp3–sp3 architectures via photoinduced enantioconvergent coupling of racemic aziridines with alkylzirconium reagents generated in situ from unactivated terminal and even internal olefins. The broad applicability of this protocol is illustrated in a series of late-stage diversification of advanced synthetic intermediates.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"35 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723138","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

Critical insights into the steam electrolysis electrode in protonic ceramic cells for hydrogen production 质子陶瓷电池中用于制氢的蒸汽电解电极的关键见解

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-03-28 DOI: 10.1038/s41929-025-01313-w

Meng Li, Fan Liu, Dong Ding

{"title":"Critical insights into the steam electrolysis electrode in protonic ceramic cells for hydrogen production","authors":"Meng Li, Fan Liu, Dong Ding","doi":"10.1038/s41929-025-01313-w","DOIUrl":"https://doi.org/10.1038/s41929-025-01313-w","url":null,"abstract":"Intermediate-temperature protonic ceramic electrolysis cells (PCECs), which combine the benefits of both lower- and higher-temperature electrolysis, are among the most efficient technologies for the production of green hydrogen. To ensure economic competitiveness and broad adoption, ongoing innovations in cell materials are essential to improve durability and reduce costs. The water oxidation half-reaction at the anode is a key area for improvement as it is a major contributor to performance degradation and efficiency loss in PCECs. Current anode designs, which are largely derived from solid oxide electrolysis cells, fail to address the specific requirements for PCECs under realistic operating conditions. This Perspective highlights the unique challenges faced by PCEC anodes, focusing on the impact of high steam concentrations and the critical role of proton-coupled electron-transfer mechanisms—factors that are absent in solid oxide electrolysis cells. Furthermore, we explore design principles for advancing anodes tailored for PCECs, offering guidance for future research and development in this promising field.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"72 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723139","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