Nature chemistry最新文献_第10页

Singlet fission mediates carotenoid-to-bacteriochlorophyll energy transfer in purple photosynthetic bacteria 紫色光合细菌单线态裂变介导类胡萝卜素到细菌叶绿素的能量转移。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-23 DOI: 10.1038/s41557-026-02186-7

Shuangqing Wang, George A. Sutherland, James P. Pidgeon, Mateja Šmitran, David J. K. Swainsbury, Elizabeth C. Martin, Cvetelin Vasilev, Andrew Hitchcock, Daniel J. Gillard, Ravi Kumar Venkatraman, Dimitri Chekulaev, Alexander I. Tartakovskii, C. Neil Hunter, Jenny Clark

{"title":"Singlet fission mediates carotenoid-to-bacteriochlorophyll energy transfer in purple photosynthetic bacteria","authors":"Shuangqing Wang, George A. Sutherland, James P. Pidgeon, Mateja Šmitran, David J. K. Swainsbury, Elizabeth C. Martin, Cvetelin Vasilev, Andrew Hitchcock, Daniel J. Gillard, Ravi Kumar Venkatraman, Dimitri Chekulaev, Alexander I. Tartakovskii, C. Neil Hunter, Jenny Clark","doi":"10.1038/s41557-026-02186-7","DOIUrl":"10.1038/s41557-026-02186-7","url":null,"abstract":"Photosynthesis, the foundation of most life, begins when sunlight is captured by (bacterio)chlorophyll ((B)Chl) and carotenoid (Crt) pigments. These molecules are arranged so that captured energy migrates rapidly to reaction centres, where it is stored as a charge separation. The complementary absorption of Crt and (B)Chl pigments, and rapid energy transfer between them, underpins solar harvesting. Here we report a Crt-to-BChl energy transfer mechanism mediated by singlet fission, in which a high-energy singlet exciton (with spin quantum number S = 0) is converted into two low-energy triplet (S = 1) excitons. In purple photosynthetic bacteria, the Crt S2 singlet exciton splits into Crt and BChl triplet excitons on adjacent sites. Once formed, the triplets transfer cooperatively to BChl and onwards to reaction centres. Energy is transferred from a singlet Crt state, via the spin-protected long-lived triplet pair, to a singlet BChl state. Thus, this singlet fission-mediated mechanism augments solar energy harvesting for photosynthesis. The biological role of singlet fission—where two excitons are generated by one photon—is poorly understood. Now it has been shown that heterofission occurs in bacterial light-harvesting complexes, creating a triplet-pair reservoir that enhances carotenoid-to-bacteriochlorophyll energy transfer efficiency and temporarily staggers energy delivery to the reaction centre.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 9","pages":"1611-1619"},"PeriodicalIF":24.5,"publicationDate":"2026-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02186-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148304977","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

A tectonic shift in supramolecular proton highways 超分子质子高速公路的构造转变。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-22 DOI: 10.1038/s41557-026-02183-w

Graham N. Newton

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Discovering nickel enzymes within the aldo-keto reductase superfamily 在醛酮还原酶超家族中发现镍酶。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-19 DOI: 10.1038/s41557-026-02185-8

引用次数: 0

Author Correction: Modular diastereoselective synthesis of hindered cyclobutane amino nitriles through triplet nitrene-mediated ring expansion 作者更正：通过三态硝基烯介导的环扩张，阻碍环丁烷氨基腈的模块化非对映选择性合成。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-18 DOI: 10.1038/s41557-026-02202-w

Jun-Jie Yin, Su-Ge Xin, Hengyi Cao, Lumin Zhang

引用次数: 0

Programming stacking order in conducting van der Waals metal–organic frameworks through ligand aggregation 通过配体聚集进行范德华金属有机骨架的堆叠顺序规划。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-18 DOI: 10.1038/s41557-026-02180-z

Yunlong Fan, Jinkun Guo, Ze-Fan Yao, Zhenghan Zhang, Haoyang Zhang, Xing Huang, Zhichao Pan, Luming Yang, Chao Ma, Xinyan Wu, Khoa N. Le, Tianyang Chen, Zhichen Xu, Ling Zhang, Hao Chen, Tongyang Zhao, Shuo Qiao, Tingsong Zhang, Qingqing Ji, Yu-Qing Zheng, Lei Sun, Grigorii Skorupskii, Maxx Q. Arguilla, Yuanping Yi, Christopher H. Hendon, Mircea Dincă, Jian Li, Jin-Hu Dou

{"title":"Programming stacking order in conducting van der Waals metal–organic frameworks through ligand aggregation","authors":"Yunlong Fan, Jinkun Guo, Ze-Fan Yao, Zhenghan Zhang, Haoyang Zhang, Xing Huang, Zhichao Pan, Luming Yang, Chao Ma, Xinyan Wu, Khoa N. Le, Tianyang Chen, Zhichen Xu, Ling Zhang, Hao Chen, Tongyang Zhao, Shuo Qiao, Tingsong Zhang, Qingqing Ji, Yu-Qing Zheng, Lei Sun, Grigorii Skorupskii, Maxx Q. Arguilla, Yuanping Yi, Christopher H. Hendon, Mircea Dincă, Jian Li, Jin-Hu Dou","doi":"10.1038/s41557-026-02180-z","DOIUrl":"10.1038/s41557-026-02180-z","url":null,"abstract":"The physical properties of van der Waals materials are highly dependent on their stacking sequences. However, constructing layered materials with specific compositions and desired stackings is challenging. Here we show that a solvent-directed strategy enables targeted stacking in van der Waals metal–organic frameworks, an emerging class of van der Waals materials. By leveraging the tunable metastable states of conjugated ligands through various solvents, and stabilizing these states via metal–ligand coordination, we enable the inheritance of stacking patterns from ligands to van der Waals metal–organic frameworks. Notably, this strategy enables the controlled manipulation of stacking sequences and divergent charge transport regimes in two-dimensional and three-dimensional van der Waals metal–organic framework single crystals, yielding an electrical conductivity of 1,792 S cm−1. These results provide a versatile approach for designing layered materials with programmable stackings and tailored electronic properties. Controlling stacking sequences in van der Waals materials to tune their physical properties is challenging. Now a solvent-directed strategy enables programmable stacking control and divergent charge transport regimes in two-dimensional and three-dimensional conducting van der Waals metal–organic frameworks.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 9","pages":"1543-1552"},"PeriodicalIF":24.5,"publicationDate":"2026-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148278110","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

Discovery and characterization of a nickel enzyme family that catalyses intermolecular hydride shuttling 催化分子间氢化物穿梭的镍酶家族的发现和表征。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-17 DOI: 10.1038/s41557-026-02184-9

Zoë L. Semersky, Conor G. Raymond, John M. Rossi, Heike Hofstetter, Pranav Rao, Monica E. Neugebauer

{"title":"Discovery and characterization of a nickel enzyme family that catalyses intermolecular hydride shuttling","authors":"Zoë L. Semersky, Conor G. Raymond, John M. Rossi, Heike Hofstetter, Pranav Rao, Monica E. Neugebauer","doi":"10.1038/s41557-026-02184-9","DOIUrl":"10.1038/s41557-026-02184-9","url":null,"abstract":"Nickel-dependent enzymes catalyse incredible transformations. However, few have been discovered so far, limiting our understanding of the role of nickel in nature. Here we develop a bioinformatic pipeline to discover a family of nickel pincer mononucleotide (NPMN)-dependent enzymes with structures that are completely distinct from previously reported NPMN-dependent enzymes. We characterize one family member, NPMN-dependent hydride transferase (NphT), and find that it catalyses intermolecular hydride transfer, which we elucidate through its promiscuous disproportionation of sugars. We solve a 1.3-Å resolution crystal structure of NphT bound to NPMN and interrogate its mechanism through mutagenesis. We discover that NphT is one of many unexplored nickel enzymes within the large aldo-keto reductase superfamily, which catalyses reactions on a wide range of molecules, including secondary metabolites, sugars and drugs. This work reveals a unique enzymatic scaffold that can harness nickel, expands the known NPMN-catalysed transformations to intermolecular hydride transfer and establishes a pipeline for the discovery of distinct families of nickel-dependent enzymes. There is limited understanding of nickel-catalysed chemistry in nature. Now a bioinformatic pipeline reveals a structurally distinct family of nickel pincer nucleotide-dependent enzymes. Nickel pincer hydride transferase (NphT) was found to catalyse intermolecular hydride transfer by characterizing its crystal structure, conducting structure-guided mutagenesis and measuring its capacity to disproportionate sugars.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 9","pages":"1582-1592"},"PeriodicalIF":24.5,"publicationDate":"2026-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02184-9.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148272400","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

Potent and biased agonists of class B1 GPCRs from a heterochiral design strategy 来自异手性设计策略的B1类gpcr的有效和偏倚激动剂。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-16 DOI: 10.1038/s41557-026-02182-x

Ruslan Gibadullin, Lauren My-Linh Tran, Jiani Niu, Rylie K. Morris, Ariel J. Kuhn, John A. Mannone, Tae Wook Kim, Giuseppe Deganutti, Samuel H. Gellman

{"title":"Potent and biased agonists of class B1 GPCRs from a heterochiral design strategy","authors":"Ruslan Gibadullin, Lauren My-Linh Tran, Jiani Niu, Rylie K. Morris, Ariel J. Kuhn, John A. Mannone, Tae Wook Kim, Giuseppe Deganutti, Samuel H. Gellman","doi":"10.1038/s41557-026-02182-x","DOIUrl":"10.1038/s41557-026-02182-x","url":null,"abstract":"Glucagon is used to treat severe hypoglycaemia in patients with diabetes, and PTH(1–34), an N-terminal fragment of parathyroid hormone, is used to treat osteoporosis. Each peptide activates a cognate G-protein-coupled receptor (GPCR). High-resolution structures of peptide–receptor complexes show that glucagon and PTH(1–34) are fully α-helical in the bound state. Here we describe a design strategy that destabilizes the helical conformation of glucagon or PTH(1–34) but nevertheless delivers potent agonists of each receptor. Replacement of multiple l-α-amino-acid residues with d-α-amino-acid residues, at selected positions, generates heterochiral analogues of both glucagon and PTH(1–34) that approach the all-l peptide in receptor activation potency (cAMP production). The heterochiral agonists are biased away from β-arrestin recruitment relative to the all-l peptide. The glucagon analogues are also biased away from receptor internalization relative to glucagon itself. These unanticipated findings for two dissimilar class B1 GPCRs raise the prospect that heterochiral design will be impactful for other members of this receptor family, which includes multiple therapeutic targets. Many peptides that activate class B1 GPCRs, such as the glucagon receptor (GCGR) or the parathyroid hormone receptor-1 (PTH1R4), are α-helical in the active receptor-bound form. Now, despite destabilizing the helical conformation of parent glucagon and PTH agonists, the presented design strategy generates potent and biased heterochiral analogues by replacing select l-α-amino-acid residues with d-α-amino acids.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 9","pages":"1639-1649"},"PeriodicalIF":24.5,"publicationDate":"2026-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02182-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148265410","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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Isotropic zero thermal expansion in sodalite crystals from 11 to 893 K 钠石晶在11 ~ 893 K范围内的各向同性零热膨胀。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-16 DOI: 10.1038/s41557-026-02174-x

Youquan Liu (, ), Xingxing Jiang (, ), Maxim S. Molokeev, Mikhail Plyaskin, Zhenhuang Su (, ), Qianru Lin (, ), Jie Sheng (, ), Wen Wen (, ), Xingyu Gao (, ), M. T. Dove, Zheshuai Lin (, )

{"title":"Isotropic zero thermal expansion in sodalite crystals from 11 to 893 K","authors":"Youquan Liu \u0000 (, ), Xingxing Jiang \u0000 (, ), Maxim S. Molokeev, Mikhail Plyaskin, Zhenhuang Su \u0000 (, ), Qianru Lin \u0000 (, ), Jie Sheng \u0000 (, ), Wen Wen \u0000 (, ), Xingyu Gao \u0000 (, ), M. T. Dove, Zheshuai Lin \u0000 (, )","doi":"10.1038/s41557-026-02174-x","DOIUrl":"10.1038/s41557-026-02174-x","url":null,"abstract":"Isotropic zero thermal expansion (ZTE) materials are essential for applications requiring extreme dimensional stability, yet their operation is typically limited to narrow temperature windows below 400 K. Here we report the incorporation of flexible interstitial groups via fractionally occupied atoms into a closed-framework sodalite structure (Cd4Al6O12SO4, CASO). This material exhibits isotropic ZTE, with a thermal expansion coefficient of 0.21(23) × 10−6 K−1 from 11 K to 893 K. The high-temperature ZTE behaviour originates from the preserved transverse vibrations that drive negative thermal expansion—arising from the enhanced vibrations of positionally disordered ligand atoms—which effectively counterbalance the intrinsic positive thermal expansion. Moreover, CASO maintains structural integrity up to 1,100 K, features a solar-blind ultraviolet transparency window down to 275 nm and exhibits thermally induced optical fluctuations at least twice as low as those of conventional optical materials. This work provides both a high-performance crystal for extreme thermal environments and a strategy for designing wide-temperature-range ZTE materials. Phonon engineering of zero thermal expansion materials faces a trade-off between open frameworks, which can enable negative thermal expansion through transverse vibrations but can suffer from thermal instability, and closed frameworks, which are more robust yet exhibit weaker negative thermal expansion. Now, fractional atomic occupancy in sodalite-type closed frameworks is shown to exhibit isotropic zero thermal expansion over a wide temperature range.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 9","pages":"1620-1627"},"PeriodicalIF":24.5,"publicationDate":"2026-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148265334","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

An alkyl-swap platform for late-stage modification of secondary N-methylamines 二级n -甲胺后期修饰的烷基交换平台。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-15 DOI: 10.1038/s41557-026-02178-7

Uroš Vezonik, Giulia Iannelli, Daniel Kaiser, Nuno Maulide

{"title":"An alkyl-swap platform for late-stage modification of secondary N-methylamines","authors":"Uroš Vezonik, Giulia Iannelli, Daniel Kaiser, Nuno Maulide","doi":"10.1038/s41557-026-02178-7","DOIUrl":"10.1038/s41557-026-02178-7","url":null,"abstract":"The selective functionalization of unprotected amines with simple, unactivated alkenes and alkynes remains a challenge in contemporary synthesis. Here we present a strategy for the peripheral modification of secondary N-methylamines that complements state-of-the-art approaches and tolerates a wide range of functional groups and native amine substrates. This method is primed for application in late-stage functionalization contexts, including the direct bioconjugation of fully functionalized, unprotected building blocks and complex peptides. The retrosynthetic flexibility unlocked by this method also enables the preparation of several commercial, high-grossing pharmaceuticals in a single synthetic step. The selective functionalization of unprotected amines with alkenes remains a challenge in contemporary synthesis. Now a strategy has been developed for an alkyl swap of N-methylamines, enabling late-stage bioconjugation and peptide modification. The resulting retrosynthetic disconnection also streamlines the preparation of several pharmaceuticals and medicinally relevant compounds.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 9","pages":"1650-1657"},"PeriodicalIF":24.5,"publicationDate":"2026-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02178-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148258802","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

Copper-catalysed site-selective arylation of pyrazoles 铜催化吡唑的位点选择性芳基化。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-06-12 DOI: 10.1038/s41557-026-02148-z

Minghao Wang, Xintong Hou, Stephanie A. Corio, Lori Digal, Jennifer S. Hirschi, Vy M. Dong

{"title":"Copper-catalysed site-selective arylation of pyrazoles","authors":"Minghao Wang, Xintong Hou, Stephanie A. Corio, Lori Digal, Jennifer S. Hirschi, Vy M. Dong","doi":"10.1038/s41557-026-02148-z","DOIUrl":"10.1038/s41557-026-02148-z","url":null,"abstract":"A major challenge in late-stage functionalization is the selective N-arylation of unsymmetric pyrazoles, five-membered heterocycles with two adjacent nitrogen atoms, which are prevalent in blockbuster medicines and bioactive molecules. Traditional cross-coupling methods usually favour one type of regioisomer, limiting access to complementary structures that could accelerate drug discovery and streamline structure–activity relationship studies. Here we show that copper catalysis harnesses arynes to achieve switchable arylation of pyrazoles under mild conditions. By tuning Cu–pyrazole coordination, we direct arylation to either nitrogen atom, unlocking selectivity between two similar sites. Mechanistic studies reveal how steric and electronic effects govern regioselectivity, transforming an inherently unpredictable process into a blueprint for selective recognition of N–N linkages. This approach establishes a general strategy for controlling site selectivity in nitrogen-rich heterocycles and highlights the use of strained intermediates in late-stage diversification. N-aryl pyrazole is a prevalent motif among pharmaceuticals across various therapeutic areas but can be challenging to synthesize due to the high similarity of the two nitrogen atoms. Now it has been shown that the use of copper catalysis and arynes provides a switchable protocol to access both regioisomers.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 8","pages":"1487-1495"},"PeriodicalIF":24.5,"publicationDate":"2026-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02148-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148239711","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