Nature chemistry最新文献

Protons undermine lithium-ion batteries with positively disastrous results

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-01-29 DOI: 10.1038/s41557-025-01733-y

Noah P. Holzapfel, Veronica Augustyn

引用次数: 0

Enantioselective synthesis of 2-substituted bicyclo[1.1.1]pentanes via sequential asymmetric imine addition of bicyclo[1.1.0]butanes and skeletal editing

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-01-28 DOI: 10.1038/s41557-024-01710-x

Jin-Teng Che, Wei-Yi Ding, Hong-Bo Zhang, Yong-Bin Wang, Shao-Hua Xiang, Bin Tan

{"title":"Enantioselective synthesis of 2-substituted bicyclo[1.1.1]pentanes via sequential asymmetric imine addition of bicyclo[1.1.0]butanes and skeletal editing","authors":"Jin-Teng Che, Wei-Yi Ding, Hong-Bo Zhang, Yong-Bin Wang, Shao-Hua Xiang, Bin Tan","doi":"10.1038/s41557-024-01710-x","DOIUrl":"https://doi.org/10.1038/s41557-024-01710-x","url":null,"abstract":"The substitution of an aromatic ring with a C(sp3)-rich bicyclic hydrocarbon, known as bioisosteric replacement, plays a crucial role in modern drug discovery. Substituted bicyclo[1.1.1]pentanes (BCPs) are particularly noteworthy owing to their uniquely three-dimensional stereochemical complexity. 1,3-Difunctionalized BCPs have been widely used as bioisosteres for para-substituted phenyl rings, and they have been incorporated into numerous lead pharmaceutical candidates. 2-Substituted BCPs (substituted at the bridge position) can function as alternatives to ortho- or meta-substituted arene rings; however, the general and efficient construction of these scaffolds remains challenging, particularly if performed in an enantioselective manner. Here we present an approach for synthesizing enantioenriched 2-substituted BCPs by a nitrogen-atom insertion-and-deletion strategy, involving a chiral Brønsted acid-catalytic enantioselective cycloaddition of bicyclo[1.1.0]butanes with imines and nitrogen deletion of resulting aza-bicyclo[2.1.1]hexanes (aza-BCHs) with generally good enantiopurity retention. Mechanistic experiments verify the radical pathway. Chiral BCPs have been readily incorporated into medicinally relevant molecules, and a drug analogue has been successfully prepared enantioselectively.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"32 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050300","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

Supramolecular dyads as photogenerated qubit candidates

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-01-27 DOI: 10.1038/s41557-024-01716-5

Ivan V. Khariushin, Philipp Thielert, Elisa Zöllner, Maximilian Mayländer, Theresia Quintes, Sabine Richert, Andreas Vargas Jentzsch

引用次数: 0

Coacervating proteins stick like a tick 聚集的蛋白质像虱子一样粘在一起

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-01-23 DOI: 10.1038/s41557-024-01720-9

Ali Miserez

引用次数: 0

A living library concept to capture the dynamics and reactivity of mixed-metal clusters for catalysis 一个活生生的图书馆概念，捕捉混合金属团簇催化的动力学和反应性

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-01-23 DOI: 10.1038/s41557-024-01726-3

Raphael Bühler, Max Schütz, Karla F. Andriani, Marcos G. Quiles, João Paulo A. de Mendonça, Vivianne K. Ocampo-Restrepo, Johannes Stephan, Sophia Ling, Samia Kahlal, Jean-Yves Saillard, Christian Gemel, Juarez L. F. Da Silva, Roland A. Fischer

{"title":"A living library concept to capture the dynamics and reactivity of mixed-metal clusters for catalysis","authors":"Raphael Bühler, Max Schütz, Karla F. Andriani, Marcos G. Quiles, João Paulo A. de Mendonça, Vivianne K. Ocampo-Restrepo, Johannes Stephan, Sophia Ling, Samia Kahlal, Jean-Yves Saillard, Christian Gemel, Juarez L. F. Da Silva, Roland A. Fischer","doi":"10.1038/s41557-024-01726-3","DOIUrl":"https://doi.org/10.1038/s41557-024-01726-3","url":null,"abstract":"The exploration of ligated metal clusters’ chemical space is challenging, partly owing to an insufficiently targeted access to reactive clusters. Now, dynamic mixtures of clusters, defined as living libraries, are obtained through organometallic precursor chemistry. The libraries are populated with interrelated clusters, including transient and highly reactive ones, as well as more accessible but less reactive species. Their evolutions upon perturbation with substrate molecules are monitored and chemical information is gained without separation of the clusters. Here we prepared a library of all-hydrocarbon ligated Cu/Zn clusters and developed a bias-free computational framework suited to analyse the full compositional space that yields a reliable structural model for each cluster. This methodology enables efficient searches for structure–reactivity relationships relevant for catalysis with mixed-metal clusters: when treating the library with CO2 or 3-hexyne and H2, we discovered [Cu11Zn6](Cp*)8(CO2)2(HCO2) bearing a formate species related to CO2 reduction and [Cu9Zn7](Cp*)6(Hex)3(H)3 bearing C6 species related to alkyne semi-hydrogenation.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"62 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020818","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

Computational design of highly signalling-active membrane receptors through solvent-mediated allosteric networks 通过溶剂介导的变构网络的高信号活性膜受体的计算设计

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-01-23 DOI: 10.1038/s41557-024-01719-2

K.-Y. M. Chen, J. K. Lai, L. S. P. Rudden, J. Wang, A. M. Russell, K. Conners, M. E. Rutter, B. Condon, F. Tung, L. Kodandapani, B. Chau, X. Zhao, J. Benach, K. Baker, E. J. Hembre, P. Barth

{"title":"Computational design of highly signalling-active membrane receptors through solvent-mediated allosteric networks","authors":"K.-Y. M. Chen, J. K. Lai, L. S. P. Rudden, J. Wang, A. M. Russell, K. Conners, M. E. Rutter, B. Condon, F. Tung, L. Kodandapani, B. Chau, X. Zhao, J. Benach, K. Baker, E. J. Hembre, P. Barth","doi":"10.1038/s41557-024-01719-2","DOIUrl":"https://doi.org/10.1038/s41557-024-01719-2","url":null,"abstract":"Protein catalysis and allostery require the atomic-level orchestration and motion of residues and ligand, solvent and protein effector molecules. However, the ability to design protein activity through precise protein–solvent cooperative interactions has not yet been demonstrated. Here we report the design of 14 membrane receptors that catalyse G protein nucleotide exchange through diverse engineered allosteric pathways mediated by cooperative networks of intraprotein, protein–ligand and –solvent molecule interactions. Consistent with predictions, the designed protein activities correlated well with the level of plasticity of the networks at flexible transmembrane helical interfaces. Several designs displayed considerably enhanced thermostability and activity compared with related natural receptors. The most stable and active variant crystallized in an unforeseen signalling-active conformation, in excellent agreement with the design models. The allosteric network topologies of the best designs bear limited similarity to those of natural receptors and reveal an allosteric interaction space larger than previously inferred from natural proteins. The approach should prove useful for engineering proteins with novel complex protein binding, catalytic and signalling activities.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"12 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020817","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

Mesoporous single-crystal metal–organic frameworks 介孔单晶金属有机骨架

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-01-22 DOI: 10.1038/s41557-024-01727-2

Yingji Zhao, Yusuke Yamauchi

引用次数: 0

Author Correction: Cytoskeleton-functionalized synthetic cells with life-like mechanical features and regulated membrane dynamicity. 作者更正：细胞骨架功能化的合成细胞，具有类似生命的机械特征和可调节的膜动力学。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-21 DOI: 10.1038/s41557-025-01740-z

Sebastian Novosedlik, Felix Reichel, Thijs van Veldhuisen, Yudong Li, Hanglong Wu, Henk Janssen, Jochen Guck, Jan van Hest

引用次数: 0

Publisher Correction: Protocells by spontaneous reaction of cysteine with short-chain thioesters 出版者更正：由半胱氨酸与短链硫酯自发反应产生的原始细胞