Nature Catalysis最新文献_第7页

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 44.6 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

{"title":"Accessing carbon, boron and germanium spiro stereocentres in a unified catalytic enantioselective approach","authors":"Yi-Xuan Cao, Anne-Sophie Chauvin, Shuo Tong, Layth Alama, Nicolai Cramer","doi":"10.1038/s41929-025-01352-3","DOIUrl":"10.1038/s41929-025-01352-3","url":null,"abstract":"Achieving substrate generality in asymmetric catalysis remains a long-standing goal, particularly for the selective construction of chiral heteroatoms. Compared with carbon, sulfur, phosphorus and silicon stereogenic centres, methods for the construction of their boron and germanium congeners remain very scarce. Chiral (hetero) spirocycles are of relevance in several research domains. Methods effective for constructing carbon-centred chiral spirocycles do not translate to boron and germanium, leaving these chiral centres unexplored. We describe a unified strategy for constructing carbon, boron and germanium-centred chiral spirocyclic skeletons via enantioselective hetero [2+2+2] cycloaddition of a bis-alkyne with a nitrile. A chiral designer Ni(0) N-heterocyclic carbene complex enables the required long-range enantioinduction. The resulting enantio-enriched spirocycles feature a pyridine motif, making them exploitable for ligand design and functional materials featuring attractive photophysical and chiroptical properties. General methods to access stereogenic centres of different heteroatoms are limited. Now the nickel-catalysed enantioselective construction of carbon, boron and germanium-centred chiral spirocyclic frameworks via a hetero [2+2+2] cycloaddition of a bis-alkyne with a nitrile is presented.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"569-578"},"PeriodicalIF":44.6,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-025-01352-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144268590","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

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 44.6 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":"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. Solution-based methods exist to upcycle waste polyolefins, although these resort to the use of co-reactants and require non-negligible energy inputs. Here the authors show how a solar thermal catalytic system based on copper particles encapsulated within a 2D Si material can strongly alleviate such issues.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"556-568"},"PeriodicalIF":44.6,"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}

引用次数: 0

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 44.6 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":"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. Promoters are able to modulate the performance of catalysts for a given process, but this can be done through various mechanisms. Here the role of Mn as a promoter on Fe-based catalysts for CO2 hydrogenation to olefins is comprehensively investigated via spectroscopic and kinetic analyses. The promoter induces a restructuring of the catalyst surface, balancing the strength of the adsorption of reactants and intermediates.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 6","pages":"595-606"},"PeriodicalIF":44.6,"publicationDate":"2025-06-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-025-01334-5.pdf","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":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

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 44.6 1区化学

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

引用次数: 0

Shape matters too 形状也很重要

IF 44.6 1区化学

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

Davide Esposito

引用次数: 0

Capture to convert 捕获转换

IF 44.6 1区化学