Nature chemistry最新文献

Bench-stable boracyclobutenes Bench-stable boracyclobutenes

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-28 DOI: 10.1038/s41557-025-01814-y

Leo Wessel, René Frank

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Transition-metal-free ammonia synthesis 无过渡金属氨合成

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-24 DOI: 10.1038/s41557-025-01806-y

Yeqin Guan, Ping Chen

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Porous metal–organic polyhedra with a gecko’s grip 多孔金属有机多面体和壁虎的抓地力

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-24 DOI: 10.1038/s41557-025-01811-1

Vincent Guillerm

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An enzymatic dual-oxa Diels–Alder reaction constructs the oxygen-bridged tricyclic acetal unit of (–)-anthrabenzoxocinone 酶促双氧Diels-Alder反应构建了(-)-蒽苯并恶辛酮的氧桥三环缩醛单元

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-22 DOI: 10.1038/s41557-025-01804-0

Xiaoli Yan, Xinying Jia, Zhenyao Luo, Shunjia Ji, Meng-Jie Zhang, Hui Zhang, Mingjia Yu, Julien Orts, Kai Jiang, Zhi Lin, Zixin Deng, Xu-Dong Kong, Bostjan Kobe, Yi-Lei Zhao, Mehdi Mobli, Xudong Qu

{"title":"An enzymatic dual-oxa Diels–Alder reaction constructs the oxygen-bridged tricyclic acetal unit of (–)-anthrabenzoxocinone","authors":"Xiaoli Yan, Xinying Jia, Zhenyao Luo, Shunjia Ji, Meng-Jie Zhang, Hui Zhang, Mingjia Yu, Julien Orts, Kai Jiang, Zhi Lin, Zixin Deng, Xu-Dong Kong, Bostjan Kobe, Yi-Lei Zhao, Mehdi Mobli, Xudong Qu","doi":"10.1038/s41557-025-01804-0","DOIUrl":"https://doi.org/10.1038/s41557-025-01804-0","url":null,"abstract":"The hetero-Diels–Alder (HDA) reaction is a key method for synthesizing six-membered heterocyclic rings in natural products and bioactive compounds. Despite its importance in synthetic chemistry, naturally occurring enzymatic HDA reactions are rare and limited to a single heteroatom. Here we report Abx(−)F, a bifunctional vicinal oxygen chelate (VOC)-like protein that catalyses dehydration and dual-oxa Diels–Alder reactions to stereoselectively form the oxygen-bridged tricyclic acetal of (–)-anthrabenzoxocinone ((−)-ABX). Isotope assays and density functional theory calculations reveal a dehydration-coordinated, concerted HDA mechanism. The crystal structure of Abx(−)F and NMR complex structures of Abx(−)F with its substrate analogue and (−)-ABX define the reaction’s structural basis. Mutational analysis identifies Asp17 as a general base that mediates dehydration, forming an o-quinone methide intermediate for stereoselective dual-oxa HDA. This work establishes the molecular and structural basis of a polyheteroatomic Diels–Alderase, paving the way for designing polyheteroatomic DA enzymatic tools.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"29 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143857619","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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Reactivity of syn-CH3CHOO with H2O enhanced through a roaming mechanism in the entrance channel 通过入口通道漫游机制增强了syn-CH3CHOO与H2O的反应性

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-16 DOI: 10.1038/s41557-025-01798-9

Yiqiang Liu, Lijie Liu, Yanlin Fu, Haotian Jiang, Hao Wu, Yue Liu, Xiaoxiao Lu, Xiaohu Zhou, Hongwei Li, Rex T. Skodje, Xingan Wang, Bina Fu, Wenrui Dong, Dong H. Zhang, Xueming Yang

{"title":"Reactivity of syn-CH3CHOO with H2O enhanced through a roaming mechanism in the entrance channel","authors":"Yiqiang Liu, Lijie Liu, Yanlin Fu, Haotian Jiang, Hao Wu, Yue Liu, Xiaoxiao Lu, Xiaohu Zhou, Hongwei Li, Rex T. Skodje, Xingan Wang, Bina Fu, Wenrui Dong, Dong H. Zhang, Xueming Yang","doi":"10.1038/s41557-025-01798-9","DOIUrl":"https://doi.org/10.1038/s41557-025-01798-9","url":null,"abstract":"Criegee intermediates are highly reactive species that play a pivotal role in the chemistry of the atmosphere, substantially impacting global climate and air quality. They are formed through the reaction of ozone with alkenes and considerably influence the formation of hydroxyl radicals and aerosols through their unimolecular decomposition and their reaction with key atmospheric components, respectively. However, their interaction with water vapour, a major atmospheric component, remains inadequately characterized. Here, using both time-dependent laser-induced fluorescence experiments and full-dimensional dynamics calculations, we investigate the reaction of syn-CH3CHOO, a prevalent Criegee intermediate, with water vapour. Our results reveal a much higher reaction rate than previously estimated, challenging the conventional notion that unimolecular decomposition dominates syn-CH3CHOO removal. Notably, we uncover a complex mechanism involving a roaming process that enhances reactivity. Our findings necessitate a revised assessment of reactions involving syn-mono- and di-substituted Criegee intermediates with water, which are crucial for accurately estimating the OH budget derived from these intermediates.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"2 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837177","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

Author Correction: Synthesis of triple-decker sandwich compounds featuring a M–M bond through cyclo-Bi5 and cyclo-Sb5 rings 作者更正：通过环-Bi5 和环-Sb5 合成以 M-M 键为特征的三层夹层化合物

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-15 DOI: 10.1038/s41557-025-01825-9

Yu-He Xu, Xing Yang, Ya-Nan Yang, Lili Zhao, Gernot Frenking, Zhong-Ming Sun

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Valence-delocalized trithorium nanocluster superatoms with open-shell exalted diamagnetism 具有开壳高抗磁性的价离定域氚纳米团簇超原子

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-11 DOI: 10.1038/s41557-025-01790-3

John A. Seed, Xinglan Deng, Josef Tomeček, Adam Brookfield, David Collison, Floriana Tuna, Ashley J. Wooles, George F. S. Whitehead, Nikolas Kaltsoyannis, Stephen T. Liddle

{"title":"Valence-delocalized trithorium nanocluster superatoms with open-shell exalted diamagnetism","authors":"John A. Seed, Xinglan Deng, Josef Tomeček, Adam Brookfield, David Collison, Floriana Tuna, Ashley J. Wooles, George F. S. Whitehead, Nikolas Kaltsoyannis, Stephen T. Liddle","doi":"10.1038/s41557-025-01790-3","DOIUrl":"https://doi.org/10.1038/s41557-025-01790-3","url":null,"abstract":"Quantum-confined nanoclusters can be described by the jellium model, which emphasizes closed-shell electron configurations, but an open-shell variation with jellium aromaticity has been proposed. Such clusters are termed superatoms because they behave like an atom, and they exhibit unusual properties. Superatoms feature metal–metal bonding; hence, since their discovery 40 years ago, superatoms have exclusively involved main group or transition metals, with actinides only considered computationally as dopants owing to actinide–actinide bonding being exceedingly rare. Here we report trithorium nanoclusters exhibiting three-centre-one-electron actinide–actinide bonding. Experimental and computational analysis demonstrates Robin–Day Class III 6d-orbital valence delocalization in these clusters. These S = 1/2 clusters are paramagnetic, but in external applied magnetic fields they exhibit exalted diamagnetism, evidencing actinide open-shell jellium aromaticity superatom character. Exalted diamagnetism is not normally associated with a single unpaired electron, but with a 1S1 magic number, the valence delocalization enables exalted diamagnetism, which is aromaticity, via superatom ring currents.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"23 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819172","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

Universal membranization of synthetic coacervates and biomolecular condensates towards ultrastability and spontaneous emulsification 合成凝聚物和生物分子凝聚物向超稳定和自发乳化方向的普遍膜化

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-10 DOI: 10.1038/s41557-025-01800-4

Da Tang, Jun Zhu, Hao Wang, Nannan Chen, Hui Wang, Yongqi Huang, Lingxiang Jiang

{"title":"Universal membranization of synthetic coacervates and biomolecular condensates towards ultrastability and spontaneous emulsification","authors":"Da Tang, Jun Zhu, Hao Wang, Nannan Chen, Hui Wang, Yongqi Huang, Lingxiang Jiang","doi":"10.1038/s41557-025-01800-4","DOIUrl":"https://doi.org/10.1038/s41557-025-01800-4","url":null,"abstract":"Membranization of membraneless coacervates and condensates is emerging as a promising strategy to resolve their inherent susceptibility to fusion, ripening and environmental variations. Yet current membranization agents by design are largely limited to a subclass or a specific kind of coacervate or condensate systems. Here we develop a library of condensate-amphiphilic block polymers that can efficiently form a polymeric layer on the droplet interface for a wide spectrum of synthetic coacervates and biomolecular condensates. Condensate-amphiphilic block polymers are designed with a condenophilic block firmly anchored to the condensed phase, a condenophobic block extended to the dilute phase and a self-association block to promote membrane formation. Critical to our design is the condenophilic block of phenylboronic acid and amidoamine that target the disparate chemistry of condensed droplets via multivalent affinities. The condensate-amphiphilic block polymer membranes render the droplets mechanically robust against fusion, regulate interfacial properties such as permeability and stiffness, and substantially improve droplet tolerance to challenging conditions of temperature, salinity, pH and organic solvents.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"21 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813405","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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Nuclear spins are active in ultracold atom–molecule collisions 核自旋在超冷原子分子碰撞中是活跃的

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-08 DOI: 10.1038/s41557-025-01779-y

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A photoswitchable DNA G-quadruplex ligand enables optical control of transcription 光可切换的DNA g -四重体配体使转录的光学控制成为可能

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-04-08 DOI: 10.1038/s41557-025-01796-x

引用次数: 0