Nature chemistry最新文献_第6页

Regiospecific α-arylation of diverse carbonyl compounds using an organobismuth transporter. 不同羰基化合物的区域特异性α-芳基化使用有机铋转运体。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-18 DOI: 10.1038/s41557-026-02231-5

Li Li, Filippo Carpaneto, Pan-Pan Chen, K N Houk, Viresh H Rawal

{"title":"Regiospecific α-arylation of diverse carbonyl compounds using an organobismuth transporter.","authors":"Li Li, Filippo Carpaneto, Pan-Pan Chen, K N Houk, Viresh H Rawal","doi":"10.1038/s41557-026-02231-5","DOIUrl":"10.1038/s41557-026-02231-5","url":null,"abstract":"The α-arylation of carbonyl compounds is a cornerstone transformation in the synthesis of pharmaceuticals and natural products. Despite decades of efforts using transition metal, main-group and photoredox strategies, a general and practical α-arylation method with broad substrate scope has remained elusive. Here we show that 9-bismatriptycene (BisTrip), a rigid, shackled form of triphenylbismuth, functions as a universal aryl group transporter, enabling controlled and regiospecific α-arylation of diverse ketones, allowing the formation of sterically demanding quaternary centres and incorporation of iodoaryl units. BisTrip is readily loaded with aryl groups by a one-pot procedure using arylboronic acids to give Aryl-BisTrip and, after transferring the aryl to the enolate, is recovered quantitatively. Arylation of lithium enolates proceeds within seconds even at -78 °C and shows high fidelity in a memory-of-chirality experiment. Computations support a low barrier for C-C bond formation and account for the observed axial selectivity, establishing BisTrip as a practical platform for α-arylation.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13652010/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148795813","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}

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Signal-induced recruitment and dispatchment in reconfigurable phase-separated protocell networks 可重构相分离原始细胞网络中信号诱导的招募和调度。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-18 DOI: 10.1038/s41557-026-02225-3

Zhuping Yin, Rui Sun, Mei Li, Stephen Mann

{"title":"Signal-induced recruitment and dispatchment in reconfigurable phase-separated protocell networks","authors":"Zhuping Yin, Rui Sun, Mei Li, Stephen Mann","doi":"10.1038/s41557-026-02225-3","DOIUrl":"10.1038/s41557-026-02225-3","url":null,"abstract":"The construction of protocell networks with self-regulated spatial dynamics and functions is an important challenge in the emerging field of colloidal systems chemistry. Existing strategies predominantly produce protocell networks with fixed or randomly distributed spatial organization, relying on direct surface interactions or externally imposed conditions, while largely overlooking dynamic interactions with the surrounding environment, thereby limiting the emergence of reconfigurable network behaviours. Here we demonstrate chemical strategies for implementing the spontaneous segregation and selective translocation of binary/ternary populations of enzyme-containing proteinosomes in dextran droplet/polyethylene glycol aqueous phase-separated media. The segregated proteinosomes exhibit tunable membrane wettability, engage in cross-community chemical signalling and undergo signal-induced reversals in phase compatibility to produce reconfigurable networks capable of protocell-mediated recruitment and dispatchment. We exploit the protocell phase dynamics to spatiotemporally modulate DNase I activity in a subpopulation of translocating proteinosomes. Our methodology provides a platform for developing protocell communities with self-regulated spatiotemporal order and offers opportunities in cytomimetic modelling and colloidal systems chemistry. Constructing protocell networks with spatial dynamics remains a central challenge in colloidal systems chemistry. Now, binary populations of enzyme-containing protocells with different membrane wettability have been shown to spontaneously segregate in phase-separated media. Enzyme-mediated signals induce reversible phase compatibility, enabling selective protocell recruitment and dispatchment, and the construction of cytomimetic networks with self-regulated spatiotemporal order.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 10","pages":"1828-1837"},"PeriodicalIF":24.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02225-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148795804","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

Modulating endergonic triplet photosensitization for cycloadditions between bicyclo[1.1.0]butanes and alkenes. 调节双环[1.1.0]丁烷和烯烃之间的环加成的氧三重态光敏。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-18 DOI: 10.1038/s41557-026-02233-3

Wing Yi Tang, Jun Guo, Shaowei Nie, Jingyu Yang, Chong-Lei Ji, Xue-Zhi Wang, Hongzhi Zhou, Yuanhui Liu, Xu Sun, Meng-Ying Sun, Yao Zhang, Dongyi Liu, Zekun Li, Juan Du, Jun Yang, Jian He

{"title":"Modulating endergonic triplet photosensitization for cycloadditions between bicyclo[1.1.0]butanes and alkenes.","authors":"Wing Yi Tang, Jun Guo, Shaowei Nie, Jingyu Yang, Chong-Lei Ji, Xue-Zhi Wang, Hongzhi Zhou, Yuanhui Liu, Xu Sun, Meng-Ying Sun, Yao Zhang, Dongyi Liu, Zekun Li, Juan Du, Jun Yang, Jian He","doi":"10.1038/s41557-026-02233-3","DOIUrl":"https://doi.org/10.1038/s41557-026-02233-3","url":null,"abstract":"While energy transfer photocatalysis has recently been used in the synthesis of multisubstituted polycyclic alkanes as benzene bioisosteres, the use of highly reactive noble-metal and organo-photocatalysts often leads to rapid generation of diradical intermediates, triggering polymerization side reactions and limiting functional-group tolerance. Here we show that heteroleptic copper(I)-BINAP complexes containing bidentate (pyrazolyl)pyridine ligands act as effective triplet photosensitizers for cycloadditions between bicyclo[1.1.0]butanes and alkenes. These copper catalysts, with their extended excited-state lifetimes, enable endergonic photosensitization for substrate activation, thereby moderating radical generation, suppressing alkene polymerization and broadening the substrate scope to include electron-deficient alkenes, enynes, dienes and even aliphatic alkenes. Bicyclo[2.1.1]hexanes with an aryl substituent at either the 3- or 2-position can be synthesized by activating either styrenes or bicyclo[1.1.0]butanes. These findings suggest that copper photocatalysis holds promise for enhancing the synthetic versatility of visible-light-driven energy transfer processes.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148795807","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 protein–foldamer supramolecular synthon for self-assembled hybrid architectures 用于自组装杂化结构的蛋白质-折叠体超分子合成。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-17 DOI: 10.1038/s41557-026-02222-6

Johannes Sigl, Vasily Morozov, Lingfei Wang, Janine Sachs, Eric Merlet, Eric Largy, Niklas Geue, Nicklas Österlund, Sunbum Kwon, Florian Sanchez, Léo Candela, Simon Huet, Kevin Pagel, Yann Ferrand, Céline Douat, Cameron D. Mackereth, Ivan Huc

{"title":"A protein–foldamer supramolecular synthon for self-assembled hybrid architectures","authors":"Johannes Sigl, Vasily Morozov, Lingfei Wang, Janine Sachs, Eric Merlet, Eric Largy, Niklas Geue, Nicklas Österlund, Sunbum Kwon, Florian Sanchez, Léo Candela, Simon Huet, Kevin Pagel, Yann Ferrand, Céline Douat, Cameron D. Mackereth, Ivan Huc","doi":"10.1038/s41557-026-02222-6","DOIUrl":"10.1038/s41557-026-02222-6","url":null,"abstract":"Constructing artificial assemblies that combine proteins and synthetic ligands has been hampered by the lack of protein–ligand interfaces that are sufficiently large and organized to enable precise structural control. Here ribosome display selection is used to identify a protein that binds a helical aromatic foldamer both tightly and selectively through a sizeable surface area. We used this complex as a supramolecular synthon to create well-defined hybrid foldamer–protein architectures. Examples include foldamers that bind two proteins and hold them at a precise distance, proteins that bind two foldamers and crystals in which proteins and foldamers are connected in cyclic or infinite arrays. The modularity of aromatic foldamers brings a further dimension to protein-based assemblies. A stable and modular artificial protein–foldamer helical supramolecular synthon enables the assembly of ordered architectures, in which the foldamer dictates protein orientation and spacing on the nanoscale.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 10","pages":"1819-1827"},"PeriodicalIF":24.5,"publicationDate":"2026-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02222-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148795770","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

Tailoring packing sequences in van der Waals metal–organic frameworks 在范德华金属有机框架裁剪包装序列。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-12 DOI: 10.1038/s41557-026-02223-5

Mingyu Yang, Zheng Meng

引用次数: 0

Oleic acid at the heart of olive oil 油酸是橄榄油的核心

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-31 DOI: 10.1038/s41557-026-02200-y

Patricia O’Hara

引用次数: 0

How webby is the wood-wide web? 整个森林的网有多网状？

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-31 DOI: 10.1038/s41557-026-02220-8

Bruce C. Gibb

引用次数: 0

Innovation without inventors 没有发明者的创新

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-30 DOI: 10.1038/s41557-026-02215-5

Jennifer M. Rampling

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Deciphering the infrared spectrum of the hydrated proton using full-dimensional quantum dynamics 利用全维量子动力学破译水合质子的红外光谱。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-27 DOI: 10.1038/s41557-026-02209-3

David Mendive-Tapia, Christoph Schran, Banshi Das, Fabien Gatti, Markus Schröder, Dominik Marx, Oriol Vendrell

{"title":"Deciphering the infrared spectrum of the hydrated proton using full-dimensional quantum dynamics","authors":"David Mendive-Tapia, Christoph Schran, Banshi Das, Fabien Gatti, Markus Schröder, Dominik Marx, Oriol Vendrell","doi":"10.1038/s41557-026-02209-3","DOIUrl":"10.1038/s41557-026-02209-3","url":null,"abstract":"The nature of the aqueous proton has been traditionally interpreted through two limiting structural motifs: the Zundel and Eigen cations. However, experimental infrared (IR) spectra of the solvated proton reveal a far more dynamic character, as evidenced by distinct intensity modulations within the characteristic continuum absorption band. In fact, recent ultrafast two-dimensional IR spectroscopy suggests that solvation-induced structural distortions around H2O⋯H+⋯OH2 motifs critically shape the IR response. Here we investigate the role of such asymmetry through full-dimensional quantum dynamics simulations of the extended Zundel complex H+(H2O)6, which structurally encompasses both Zundel and Eigen motifs. Systematic removal of one water molecule from the second solvation shell gradually introduces deviations from the perfectly symmetric Zundel-like complex towards Eigen-like spectral features. These results provide a direct map between the asymmetric solvation environment and the structural response of the first and second solvation shells of the aqueous proton, offering a structural and dynamical basis for understanding how this asymmetry governs proton mobility in aqueous environments. The infrared spectra of the aqueous proton show dynamic character beyond the classical Zundel H+(H2O)2 and Eigen H+(H2O)3 structural motifs. Fully quantum modelling the larger H+(H2O)6 complex provides a direct link between asymmetric solvation environments and the spectroscopic response of the solvated proton.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 10","pages":"1773-1780"},"PeriodicalIF":24.5,"publicationDate":"2026-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02209-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148605415","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

Solvent-bridged electrolytes for high-energy Li-ion batteries under extreme conditions. 用于极端条件下高能锂离子电池的溶剂桥式电解质。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-27 DOI: 10.1038/s41557-026-02221-7

Yawei Chen, Fanyang Huang, Qiu Zhang, Lei Zheng, Ai-Min Li, Dejian Dong, Kangxuan Xia, Taeyong Lee, Weiran Zhang, Zheng Li, Xin Zhang, Chang-Xin Zhao, Fu Chen, Jiancun Rao, Karen Gaskell, Enyuan Hu, Chunsheng Wang

{"title":"Solvent-bridged electrolytes for high-energy Li-ion batteries under extreme conditions.","authors":"Yawei Chen, Fanyang Huang, Qiu Zhang, Lei Zheng, Ai-Min Li, Dejian Dong, Kangxuan Xia, Taeyong Lee, Weiran Zhang, Zheng Li, Xin Zhang, Chang-Xin Zhao, Fu Chen, Jiancun Rao, Karen Gaskell, Enyuan Hu, Chunsheng Wang","doi":"10.1038/s41557-026-02221-7","DOIUrl":"10.1038/s41557-026-02221-7","url":null,"abstract":"High-capacity anodes are desirable for high-energy lithium-ion batteries but suffer from limited cycle life due to large volume changes during cycling. The LiF-based solid-electrolyte interphase (SEI) has led to prolonged cycling stability. However, current LiF-forming electrolyte designs require anions to enter the Li+ solvation sheath, which inherently reduces the electrolyte's ionic conductivity, limiting both fast-charging and low-temperature performance. Here we develop solvent-bridged electrolytes composed of LiPF6 dissolved in a cosolvent system comprising a bridging cyclic ether that solvates both PF6- and Li+ to form a LiF-rich SEI, and a structural linear ether that governs the electrolyte liquid range. By mitigating direct Li+-anion interactions, the electrolytes maintain high ionic conductivity, enabling stable cycling of micrometre-sized silicon anodes under extreme conditions involving high rates (>4 C), low temperatures (down to -55 °C) and Li plating. Solvent-bridged electrolytes address the intrinsic trade-offs between LiF-rich SEI formation and electrolyte ionic conductivity, offering a promising approach for high-capacity anodes operating under demanding conditions.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148605487","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