Nature Catalysis最新文献

Accessing carbon, boron and germanium spiro stereocentres in a unified catalytic enantioselective approach 在统一的催化对映选择方法中获得碳、硼和锗螺体中心

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-06-12 DOI: 10.1038/s41929-025-01352-3

Yi-Xuan Cao, Anne-Sophie Chauvin, Shuo Tong, Layth Alama, Nicolai Cramer

引用次数: 0

Ambient solar thermal catalysis for polyolefin upcycling using copper encapsulated in silicon nanosheets and chloroaluminate ionic liquid 利用硅纳米片封装铜和氯铝酸盐离子液体进行聚烯烃升级回收的环境太阳热催化

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-06-05 DOI: 10.1038/s41929-025-01349-y

Chuanwang Xing, Chengliang Mao, Shenghua Wang, Yuxuan Zhou, Lei Wu, Dake Zhang, Dingxuan Kang, Di Yang, Weiting Gong, Wendong Wei, Liang Wang, Chaoran Li, Geoffrey A. Ozin, Deren Yang, Wei Sun

{"title":"Ambient solar thermal catalysis for polyolefin upcycling using copper encapsulated in silicon nanosheets and chloroaluminate ionic liquid","authors":"Chuanwang Xing, Chengliang Mao, Shenghua Wang, Yuxuan Zhou, Lei Wu, Dake Zhang, Dingxuan Kang, Di Yang, Weiting Gong, Wendong Wei, Liang Wang, Chaoran Li, Geoffrey A. Ozin, Deren Yang, Wei Sun","doi":"10.1038/s41929-025-01349-y","DOIUrl":"https://doi.org/10.1038/s41929-025-01349-y","url":null,"abstract":"The accumulation of plastic waste has become a global issue. Socially and industrially viable, sustainable technical solutions are therefore required. Here we report a solar thermal catalytic system for polyolefins upcycling using copper nanoparticles encapsulated by stacked two-dimensional silicon. In a chloroaluminate ionic liquid solvent, unlike conventional thermal techniques, the upcycling can proceed under a mild temperature (55 °C) created photothermally under 4 sun irradiation. The polyethylene can be completely transformed into distinct and separable fractions of alkanes (C3–C7) and cyclic hydrocarbons (C8–C26) within hours, with a total yield of 91%. Mechanistic studies show a pathway involved two β-scissions of C–C bonds and a rapid cyclization. The approach offers versatility in the upcycling of various real-world polyolefin waste and features excellent feasibility in outdoor practices. The analyses of a conceptual upcycling facility using this technology showcase its appeal in both economic and eco-friendliness.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144218912","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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Understanding Mn-modulated restructuring of Fe-based catalysts for controlling selectivity in CO2 hydrogenation to olefins 了解锰调铁基催化剂在控制CO2加氢制烯烃选择性中的作用

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-06-02 DOI: 10.1038/s41929-025-01334-5

Qingxin Yang, Elizaveta A. Fedorova, Dong-Bo Cao, Erisa Saraçi, Vita A. Kondratenko, Carsten R. Kreyenschulte, Henrik Lund, Stephan Bartling, Jana Weiß, Dmitry E. Doronkin, Jan-Dierk Grunwaldt, Angelika Brückner, Haijun Jiao, Evgenii V. Kondratenko

{"title":"Understanding Mn-modulated restructuring of Fe-based catalysts for controlling selectivity in CO2 hydrogenation to olefins","authors":"Qingxin Yang, Elizaveta A. Fedorova, Dong-Bo Cao, Erisa Saraçi, Vita A. Kondratenko, Carsten R. Kreyenschulte, Henrik Lund, Stephan Bartling, Jana Weiß, Dmitry E. Doronkin, Jan-Dierk Grunwaldt, Angelika Brückner, Haijun Jiao, Evgenii V. Kondratenko","doi":"10.1038/s41929-025-01334-5","DOIUrl":"https://doi.org/10.1038/s41929-025-01334-5","url":null,"abstract":"For CO2 hydrogenation over iron-based catalysts, revealing the promoting effect of manganese and the nature of catalytically active sites remains a challenge that hinders targeted catalyst design. Here we elucidate the manganese-modulated restructuring of such catalysts during preconditioning and CO2 hydrogenation using in situ X-ray absorption spectroscopy. The reaction-induced decoration of the surface of iron carbide with a MnO-containing layer is essential to hinder methane formation in favour of C2–C4 olefins and C5+ hydrocarbons. The selectivity changes were rationalized via spatially resolved steady-state and time-resolved (micro)kinetic tests combined with density functional theory calculations. The promoter affects the ability of iron carbide to generate surface species from H2, CO2 and C2H4, thus controlling the surface C/H ratio, which is decisive for product selectivity. Consequently, the design of efficient multi-component heterogeneous catalysts requires a thorough understanding of the optimal catalyst architecture and, in particular, how to generate and stabilize it under reaction conditions.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-06-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144193084","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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Mobile co-catalysts at the solid–liquid interface in the oxygen evolution reaction 析氧反应中固液界面的移动助催化剂

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-06-02 DOI: 10.1038/s41929-025-01348-z

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An asymmetric transformation of carbenium ions 碳离子的不对称转变

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01330-9

引用次数: 0

Shape matters too 形状也很重要

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01354-1

Davide Esposito

{"title":"Shape matters too","authors":"Davide Esposito","doi":"10.1038/s41929-025-01354-1","DOIUrl":"https://doi.org/10.1038/s41929-025-01354-1","url":null,"abstract":"Previous attempts to account for particle shapes employed the Wulff methodology to estimate the impact of specific particle facets. However, this method only considers nanoparticles’ equilibrium shapes and does not reflect their evolution under reaction conditions. Therefore, using a combination of density functional theory and Boltzmann statistics, the team modelled a large ensemble of nanoparticles ranging between 0.5 and 10 nm, including all possible shapes that may effectively accommodate the active sites under reaction conditions. In this way, they were able to reproduce the common experimental trend of activity — expressed as turnover frequency (TOF) — as a function of particle size, featuring a maximum at around 2.3 nm (pictured, panel a). Eventually, particles in this range are associated with a high prevalence of fourfold sites, which are identified as the most reactive sites. However, for a specific particle size range, different shapes exist, characterized by a different fraction of fourfold sites (pictured in panels b–d for particles of size ~2 nm). As a result, different particle shapes contribute differently to the observed experimental TOF.This work offers a fresh perspective to rationalize the well-known structure sensitivity of CO2 methanation on nickel catalysts. More generally, the study suggests how modelling could inform catalyst synthesis for other structure-sensitive reactions to obtained shape-tuned catalysts with high activity.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"17 1","pages":"408-408"},"PeriodicalIF":37.8,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165390","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

Capture to convert 捕获转换

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01355-0

Benjamin Martindale

{"title":"Capture to convert","authors":"Benjamin Martindale","doi":"10.1038/s41929-025-01355-0","DOIUrl":"https://doi.org/10.1038/s41929-025-01355-0","url":null,"abstract":"An N-heterocyclic carbene (1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene; pictured) was selected for its high CO2 binding and activation ability together with its resistance to reduction under electrocatalytic conditions. This sorbent was found to react quantitatively with dilute sources of CO2 in the range 0.04–10%. The molecular electrocatalyst iron tetraphenylporphyrin (pictured) was able to directly reduce the carbene–CO2 complex under applied potential in tetrahydrofuran (THF) solution. Notably, even with water as the proton source, a high selectivity towards carbon products was observed. Furthermore, the dominant product was the eight-electron reduced CH4 (85% Faradaic efficiency), even though this Fe porphyrin catalyst typically favours the two-electron reduced CO when directly reducing CO2 in the absence of carbene.This report supports the idea that integrated electrochemical CO2 capture and conversion may be an effective strategy for direct utilization of dilute CO2 emissions. Unexpectedly, it also reveals the role that the sorbent can have as a catalytic auxiliary to alter the inherent selectivity of a given catalyst towards more unusual products.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"58 1","pages":"410-410"},"PeriodicalIF":37.8,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165391","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

A formaldehyde condensation pathway in CO2 electrolysis CO2电解中的甲醛缩合途径

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01344-3

Huali Wu, Damien Voiry

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Challenges and prospects in precision medicine with RNA-based biocatalysts 基于rna的生物催化剂在精准医学中的挑战与展望

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01337-2

Charles H. Jones, Mikael Dolsten

引用次数: 0

Clustering for methane 甲烷聚类

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-05-28 DOI: 10.1038/s41929-025-01358-x

Francesco Zamberlan

{"title":"Clustering for methane","authors":"Francesco Zamberlan","doi":"10.1038/s41929-025-01358-x","DOIUrl":"https://doi.org/10.1038/s41929-025-01358-x","url":null,"abstract":"The team of researchers found that ATP is necessary for the MCR methane production and that it also affects the binding of subunits among the MCR activation complex. Indeed, the high-resolution cryo-EM structures confirmed that the presence of ATP molecules stabilizes the A2 subunit within the MCR complex. The A2 component binds asymmetrically to only one of the MCR heterotrimers, while a latch-like structure within McrA regulates access to the F430 cavity. Interestingly, this feature comes into play and allows the exposure of the F430 complex in the proximal side of the complex, so that the contained Ni centre can be reduced to Ni(I), with a nascent coordination with the thiol in CoM–SH.Further structural and electronic investigations of the potential electron pathways towards F430 also allowed the identification of three electron densities coordinated by McrC, Mmp7 and Mmp17. Each of these is constituted by two [4Fe-3S] clusters bridged by belt sulfur atoms, in a fashion reminiscing of the L-cluster topology in the [8Fe-9S-C] precursor of the M-cluster involved in nitrogenase enzymes. This feature led the researchers to understand which enzyme family – MCR or nitrogenase – first developed this type of clusters: through phylogenetic studies, the team confirmed that these clusters were first used by MCR in methanogenesis and later incorporated into nitrogenase enzymatic scaffolds.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"71 1","pages":"412-412"},"PeriodicalIF":37.8,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165500","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