Nature Catalysis最新文献

In situ electrochemical production of solid peroxide from urine

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-01-20 DOI: 10.1038/s41929-024-01277-3

Xinjian Shi, Yue Jiang, Bailin Zeng, Zhuoyue Sun, Maojin Yun, Peng Lv, Yu Jia, Xiaolin Zheng

引用次数: 0

A hydrogenative oxidation strategy for the single-step synthesis of lactams from N-heteroarenes using water

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-01-20 DOI: 10.1038/s41929-024-01286-2

Yaoyu Liang, Jie Luo, Cai You, Yael Diskin-Posner, David Milstein

引用次数: 0

Coupled cation–electron transfer at the Pt(111)/perfluoro-sulfonic acid ionomer interface and its impact on the oxygen reduction reaction kinetics

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-01-13 DOI: 10.1038/s41929-024-01279-1

Kaiyue Zhao, Mingchuan Luo, Yongfan Zhang, Xiaoxia Chang, Bingjun Xu

引用次数: 0

Organic electrolyte cations promote non-aqueous CO2 reduction by mediating interfacial electric fields

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-01-10 DOI: 10.1038/s41929-024-01278-2

Jon-Marc McGregor, Jay T. Bender, Amanda S. Petersen, Louise Cañada, Jan Rossmeisl, Joan F. Brennecke, Joaquin Resasco

{"title":"Organic electrolyte cations promote non-aqueous CO2 reduction by mediating interfacial electric fields","authors":"Jon-Marc McGregor, Jay T. Bender, Amanda S. Petersen, Louise Cañada, Jan Rossmeisl, Joan F. Brennecke, Joaquin Resasco","doi":"10.1038/s41929-024-01278-2","DOIUrl":"https://doi.org/10.1038/s41929-024-01278-2","url":null,"abstract":"The electrochemical reduction of CO2 is sensitive to the microenvironment surrounding catalytic active sites. Although the impact of changing electrolyte composition on rates has been studied intensively in aqueous electrolytes, less is known about the influence of the electrochemical environment in non-aqueous solvents. Here we demonstrate that organic alkylammonium cations influence catalytic performance in non-aqueous media and describe a physical model that rationalizes these observations. Using results from kinetic, spectroscopic and computational techniques, we argue that the strength of the electric field at the catalyst surface is sensitive to the molecular identity of the organic cation in the electrolyte. This is true irrespective of solvent, electrolyte ionic strength or electrolyte anion. Our results suggest that changes in the interfacial electric field strength can be attributed to differences in the cation–electrode distance. Changes in the electric field strength affect CO formation rates as they modify the energetics of the kinetically relevant CO2 activation step.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"84 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142961389","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

Confined hot-pressurized water in Brønsted-acidic beta zeolite speeds up the O demethylation of guaiacol

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-01-09 DOI: 10.1038/s41929-024-01282-6

Massimo Bocus, Elias Van Den Broeck, Xian Wu, Mathias Bal, Jeroen Bomon, Louis Vanduyfhuys, Bert F. Sels, Bert U. W. Maes, Veronique Van Speybroeck

{"title":"Confined hot-pressurized water in Brønsted-acidic beta zeolite speeds up the O demethylation of guaiacol","authors":"Massimo Bocus, Elias Van Den Broeck, Xian Wu, Mathias Bal, Jeroen Bomon, Louis Vanduyfhuys, Bert F. Sels, Bert U. W. Maes, Veronique Van Speybroeck","doi":"10.1038/s41929-024-01282-6","DOIUrl":"https://doi.org/10.1038/s41929-024-01282-6","url":null,"abstract":"Biorefinery technologies that convert lignin into platform chemicals are essential to reduce our future dependence on fossil resources. In these technologies, a key process is the acid-catalysed O demethylation of guaiacol derivatives in hot-pressurized water using Brønsted mineral acids or microporous zeolites. The fundamental understanding of how hydronium ions behave in a confined environment versus bulk is still limited. Here we investigate the O demethylation of guaiacol in hot-pressurized water with HCl or H-BEA zeolite catalysts to elucidate the impact of zeolite microporosity on reaction mechanisms and rates. Operando molecular simulations combined with experimental kinetic studies reveal that, regardless of the catalyst type, O demethylation follows a concerted O-activated SN2 mechanism. The reaction rate is higher in the zeolite due to more active, under-coordinated hydronium ions. Additionally, the molecular organization of solvent and reactants around the confined active site plays a crucial role in modulating the association of the reacting species and the reaction kinetics.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"83 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937423","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

Site- and enantioselective allylic and propargylic C–H oxidation enabled by copper-based biomimetic catalysis

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-01-08 DOI: 10.1038/s41929-024-01276-4

Honggang Zhang, Yibo Zhou, Tilong Yang, Jingui Wu, Pinhong Chen, Zhenyang Lin, Guosheng Liu

{"title":"Site- and enantioselective allylic and propargylic C–H oxidation enabled by copper-based biomimetic catalysis","authors":"Honggang Zhang, Yibo Zhou, Tilong Yang, Jingui Wu, Pinhong Chen, Zhenyang Lin, Guosheng Liu","doi":"10.1038/s41929-024-01276-4","DOIUrl":"https://doi.org/10.1038/s41929-024-01276-4","url":null,"abstract":"Methods for direct enantioselective oxidation of C(sp3)–H bonds will revolutionize the preparation of chiral alcohols and their derivatives. Enzymatic catalysis, which uses key metal-oxo species to facilitate efficient hydrogen atom abstraction, has evolved as a highly selective approach for C–H oxidation in biological systems. Despite its effectiveness, reproducing this function and achieving high stereoselectivity in biomimetic catalysts has proven to be a daunting task. Here we present a copper-based biomimetic catalytic system that achieves highly efficient asymmetric sp3 C–H oxidation with C–H substrates as the limiting reagent. A Cu(II)-bound tert-butoxy radical is responsible for the site-selective C–H bond cleavage, which resembles the active site of copper-based enzymes for C–H oxidation. The developed method has been successfully accomplished with good functional group compatibility and exceptionally high site- and enantioselectivity, which is applicable for the late-stage oxidation of bioactive compounds.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"20 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142936391","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

Publisher Correction: Parahydrogen-enhanced magnetic resonance identification of intermediates in [Fe]-hydrogenase catalysis

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-12-23 DOI: 10.1038/s41929-024-01285-3

Lukas Kaltschnee, Andrey N. Pravdivtsev, Manuel Gehl, Gangfeng Huang, Georgi L. Stoychev, Christoph Riplinger, Maximilian Keitel, Frank Neese, Jan-Bernd Hövener, Alexander A. Auer, Christian Griesinger, Seigo Shima, Stefan Glöggler

引用次数: 0

Photoelectrochemical asymmetric catalysis

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01260-y

Chong Huang, Peng Xiong, Xiao-Li Lai, Hai-Chao Xu

引用次数: 0

[Fe]-hydrogenase intermediates revealed

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-12-20 DOI: 10.1038/s41929-024-01274-6

Sven T. Stripp

引用次数: 0

One zeolite for multiple Fe species