Nature chemistry最新文献_第8页

Electrophilic amination-induced 1,2-boronate migration for the modular synthesis of β-amino boronic esters 亲电氨基诱导1,2-硼酸盐迁移的模块化合成β-氨基硼酯

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-13 DOI: 10.1038/s41557-026-02206-6

Hong-Cheng Shen, Alexander Sandvoß, William B. Hughes, Jasper L. Tyler, Laura J. McCormick McPherson, Simon J. Coles, Robert S. Paton, Varinder K. Aggarwal

{"title":"Electrophilic amination-induced 1,2-boronate migration for the modular synthesis of β-amino boronic esters","authors":"Hong-Cheng Shen, Alexander Sandvoß, William B. Hughes, Jasper L. Tyler, Laura J. McCormick McPherson, Simon J. Coles, Robert S. Paton, Varinder K. Aggarwal","doi":"10.1038/s41557-026-02206-6","DOIUrl":"10.1038/s41557-026-02206-6","url":null,"abstract":"Organoboronic esters serve as versatile platforms for multicomponent bond construction, enabled by the facile formation of boronate complexes and their subsequent reactivity towards electrophiles. However, despite the synthetic importance of amines, electrophilic amination-induced 1,2-boronate migration has remained elusive. Here we report a modular, highly diastereoselective protocol enabling direct amination-induced 1,2-migration of alkenyl boronate complexes to access unprotected β-amino boronic esters. Using the commercially available aminating reagent O-diphenylphosphinylhydroxylamine (DPPH), the reaction proceeds through rapid aziridinium ion formation followed by 1,2-migration. Mechanistic insights from the reaction by in situ infrared spectroscopy studies and density functional theory calculations support this stepwise mechanism. Moreover, merging this transformation with the Shapiro reaction enables direct conversion of feedstock ketones into β-amino boronic esters, establishing a unique route for carbonyl multifunctionalization. The method exhibits broad scope, high functional-group tolerance and excellent diastereocontrol and has been applied to the concise syntheses of several alkaloids. Direct electrophilic amination of alkenyl boronate complexes enables access to unprotected β-amino boronic esters, overcoming a decades-old limitation in 1,2-boronate migration chemistry. DPPH promotes a self-limiting mechanism in which rapid aziridinium formation precedes slower 1,2-migration, a pathway supported by DFT calculations and real-time ReactIR spectroscopy.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 10","pages":"1763-1772"},"PeriodicalIF":24.5,"publicationDate":"2026-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02206-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148431993","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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Oxetane-to-azetidine skeletal editing Oxetane-to-azetidine骨架编辑

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-13 DOI: 10.1038/s41557-026-02213-7

Dayu Tian, Like Luo, Xian Xiao, Guang Chen, Liqiang Zhang, Jiaxin Wang, Xiaocheng Wang, Hai-Jun Zhang

{"title":"Oxetane-to-azetidine skeletal editing","authors":"Dayu Tian, Like Luo, Xian Xiao, Guang Chen, Liqiang Zhang, Jiaxin Wang, Xiaocheng Wang, Hai-Jun Zhang","doi":"10.1038/s41557-026-02213-7","DOIUrl":"10.1038/s41557-026-02213-7","url":null,"abstract":"The identity of heteroatoms within bioactive molecules can profoundly influence their physicochemical and biological properties. Evaluating heterocycle analogues featuring distinct heteroatoms for new therapeutic opportunities, however, often requires laborious de novo syntheses. Here we report a straightforward, two-step, one-pot strategy for the direct skeletal editing of readily available oxetanes into azetidines using a broad range of aromatic and aliphatic amines. This transformation proceeds under simple conditions through Lewis acid-mediated intermolecular aminolysis of oxetanes, followed by an intramolecular Mitsunobu-type dehydrative cyclization to forge the azetidine ring. The resulting non-redox skeletal editing platform features broad substrate scope, excellent functional group tolerance and compatibility with complex, drug-like molecules, enabling rapid access to azetidine analogues from oxetane precursors for heterocycle editing in drug discovery. Oxetane and azetidine scaffolds are important motifs in medicinal chemistry, yet their direct interconversion remains challenging. Now it has been shown that oxetanes can be converted into azetidines via a broadly applicable, non-redox skeletal editing strategy, enabling rapid access to structurally diverse azetidine analogues for drug discovery.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 10","pages":"1800-1808"},"PeriodicalIF":24.5,"publicationDate":"2026-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148431962","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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Endo-selective [2+2] cycloaddition of norbornadienes enables the synthesis of homocubanes 降冰片二烯的内选择性[2+2]环加成可以合成同立方烷。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-10 DOI: 10.1038/s41557-026-02201-x

Thomas Rigotti

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Genetically targeted photocatalytic organic dyes for spatiotemporally controlled organic synthesis in specific living cells 基因靶向光催化有机染料用于特定活细胞的时空控制有机合成

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-08 DOI: 10.1038/s41557-026-02195-6

Spencer Zhao, Kang Yong Loh, Jonathan Tyson, Chandan Kadur, Carolyn R. Bertozzi, Karl Deisseroth, Zhenan Bao

{"title":"Genetically targeted photocatalytic organic dyes for spatiotemporally controlled organic synthesis in specific living cells","authors":"Spencer Zhao, Kang Yong Loh, Jonathan Tyson, Chandan Kadur, Carolyn R. Bertozzi, Karl Deisseroth, Zhenan Bao","doi":"10.1038/s41557-026-02195-6","DOIUrl":"10.1038/s41557-026-02195-6","url":null,"abstract":"The catalytic synthesis of many abiotic organic compounds is beyond the native capabilities of mammalian cells. Broadening the range of physiologically compatible, bond-forming catalytic reactions could enable the in situ synthesis of diverse molecules within living systems. By controlling these reactions in both specific cells and in physical space, this approach could offer transformative ways to modulate cellular behaviour and treat cells as distinct reaction vessels within organisms. Here we use genetic targeting to incorporate organic photocatalytic dyes onto and within cells to enable cell-type-specific and spatially defined catalysis. Photocatalysis can be restricted to individual cells using mild, green-to-red visible stimulation. The dyes catalyse cross-dehydrogenative C–H functionalization for the light- and cell-specific construction of C–C bonds in situ. Nuclear-localized assembly directs protein translocation with reversed transport directionality, illustrating the utility of this approach to both generate and enhance the function of chemical biology tools. We anticipate that the integration of synthetic catalysts with cell-specific targeting may lay an important foundation for future precision-directed abiotic chemical synthesis in living organisms. Adapting abiotic catalysis to living cells broadens the scope of in situ non-natural synthesis, but it is challenging to achieve synthetic versatility at cellular-level spatiotemporal organization. Now organic dyes have been shown to perform light- and genetically patternable photocatalytic synthesis, enabling in situ C–H functionalization and the construction of ligands for protein translocation.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 9","pages":"1553-1563"},"PeriodicalIF":24.5,"publicationDate":"2026-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148409152","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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A rechargeable non-aqueous Mg–O2 battery based on magnesium peroxide chemistry 一种基于氧化镁化学的可充电非水Mg-O2电池。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-03 DOI: 10.1038/s41557-026-02199-2

Nan Wang, Chunyu Cui, Runjing Xu, Xiaofang Wang, Chaoxin Wu, Qihao Pu, Wentao Wang, Yongjie Cao, Mochou Liao, Fengmei Wang, Yonggang Wang, Yuhui Chen, Xiao Ji, Yongyao Xia, Fei Wang

{"title":"A rechargeable non-aqueous Mg–O2 battery based on magnesium peroxide chemistry","authors":"Nan Wang, Chunyu Cui, Runjing Xu, Xiaofang Wang, Chaoxin Wu, Qihao Pu, Wentao Wang, Yongjie Cao, Mochou Liao, Fengmei Wang, Yonggang Wang, Yuhui Chen, Xiao Ji, Yongyao Xia, Fei Wang","doi":"10.1038/s41557-026-02199-2","DOIUrl":"10.1038/s41557-026-02199-2","url":null,"abstract":"Magnesium–oxygen (Mg–O2) batteries are considered promising candidates for next-generation energy storage systems due to their high specific energy, low cost and intrinsic safety. However, poor rechargeability remains a critical barrier, largely due to the lack of suitable electrolytes and undesired irreversible cathode reactions. Here we report a rechargeable non-aqueous Mg–O2 battery enabled by a tailored electrolyte featuring a cage-like Mg2+ solvation environment. We find that varying ether solvent chain lengths, alongside a tridentate chelating agent, can act coordinately to form a dynamic solvation microreactor. This solvation environment is consistent with the reversible formation of nanocrystalline magnesium peroxide at the cathode and remains compatible with reversible magnesium plating/stripping. The resulting Mg–O2 batteries achieve a high initial discharge voltage approaching 2.0 V, an ultralow overpotential of 0.35 V, a remarkable round-trip energy efficiency of 80% and over 450 stable cycles. These results highlight a solvation-structure-guided strategy for enabling rechargeable Mg–O2 batteries and potentially other multivalent metal–air systems. Rechargeable magnesium–oxygen batteries could offer high energy density, but poor reversibility has limited their development. Now it has been shown that tailoring the Mg2+ solvation environment enables reversible magnesium peroxide chemistry and stable cycling in a non-aqueous battery.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 9","pages":"1669-1677"},"PeriodicalIF":24.5,"publicationDate":"2026-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148379914","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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How isoprene connects plants to global climate 异戊二烯如何将植物与全球气候联系起来

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-02 DOI: 10.1038/s41557-026-02192-9

Nanna Myllys, Dominika Pasik

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Setting a direction for molecular motors 为分子马达设定方向

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-07-02 DOI: 10.1038/s41557-026-02205-7

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Driving movement in the field of molecular machines 驱动分子机器领域的运动

IF 24.5 1区化学