Nature chemistry最新文献_第8页

Aging-dependent evolving electrochemical potentials of biomolecular condensates regulate their physicochemical activities 生物分子凝聚物随年龄变化的电化学电位调控其物理化学活性

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-03-12 DOI: 10.1038/s41557-025-01762-7

Wen Yu, Xiao Guo, Yu Xia, Yuefeng Ma, Zhongli Tong, Leshan Yang, Xiaowei Song, Richard N. Zare, Guosong Hong, Yifan Dai

{"title":"Aging-dependent evolving electrochemical potentials of biomolecular condensates regulate their physicochemical activities","authors":"Wen Yu, Xiao Guo, Yu Xia, Yuefeng Ma, Zhongli Tong, Leshan Yang, Xiaowei Song, Richard N. Zare, Guosong Hong, Yifan Dai","doi":"10.1038/s41557-025-01762-7","DOIUrl":"https://doi.org/10.1038/s41557-025-01762-7","url":null,"abstract":"A passive consequence of macromolecular condensation is the establishment of an ion concentration gradient between the dilute and dense phases, which in turn governs distinct electrochemical properties of condensates. However, the mechanisms that regulate the electrochemical equilibrium of condensates and their impacts on emergent physicochemical functions remain unknown. Here we demonstrate that the electrochemical environments and the physical and chemical activities of biomolecular condensates, dependent on the electrochemical potential of condensates, are regulated by aging-associated intermolecular interactions and interfacial effects. Our findings reveal that enhanced dense-phase interactions during condensate maturation continuously modulate the ion distribution between the two phases. Moreover, modulating the interfacial regions of condensates can affect the apparent pH within the condensates. To directly probe the interphase and interfacial electric potentials of condensates, we have designed and implemented electrochemical potentiometry and second harmonic generation-based approaches. Our results suggest that the non-equilibrium nature of biomolecular condensates might play a crucial role in modulating the electrochemical activities of living systems.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"56 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599069","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

Designing single-polymer-chain nanoparticles to mimic biomolecular hydration frustration 设计单聚合物链纳米颗粒模拟生物分子水合挫折

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-03-12 DOI: 10.1038/s41557-025-01760-9

Tianyi Jin, Connor W. Coley, Alfredo Alexander-Katz

{"title":"Designing single-polymer-chain nanoparticles to mimic biomolecular hydration frustration","authors":"Tianyi Jin, Connor W. Coley, Alfredo Alexander-Katz","doi":"10.1038/s41557-025-01760-9","DOIUrl":"https://doi.org/10.1038/s41557-025-01760-9","url":null,"abstract":"Native folded proteins rely on sculpting the local chemical environment of their active or binding sites, as well as their shapes, to achieve functionality. In particular, proteins use hydration frustration—control over the dehydration of hydrophilic residues and the hydration of hydrophobic residues—to amplify their chemical or binding activity. Here we uncover that single-polymer-chain nanoparticles formed by random heteropolymers comprising four or more components can display similar levels of hydration frustration. We categorize these nanoparticles into three types based on whether either hydrophobic or hydrophilic residues, or both types, display frustrated states. We propose a series of physicochemical rules that determine the state of these nanoparticles. We demonstrate the generality of these rules in atomistic and simplified Monte Carlo models of single-polymer-chain nanoparticles with different backbones and residues. Our work provides insights into the design of single-chain nanoparticles, an emerging polymer modality that achieves the ease and cost of fabrication of polymeric material with the functionality of biological proteins.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"16 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599068","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

Publisher Correction: Amphoteric chalcogen-bonding and halogen-bonding rotaxanes for anion or cation recognition 出版者更正：阴离子或阳离子识别的两性硫键和卤键轮烷

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-03-12 DOI: 10.1038/s41557-025-01799-8

Yuen Cheong Tse, Andrew Docker, Igor Marques, Vítor Félix, Paul D. Beer

引用次数: 0

Aryl halide cross-coupling via formate-mediated transfer hydrogenation 甲酸介导的转移氢化芳基卤化物交叉偶联

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-03-11 DOI: 10.1038/s41557-024-01729-0

Yoon Cho, Yu-Hsiang Chang, Kevin P. Quirion, Zachary H. Strong, Zachary J. Dubey, Nam Nguyen, Seoyoung Lee, Natalie S. Taylor, Jessica M. Hoover, Nicholas A. White, Peng Liu, Michael J. Krische

{"title":"Aryl halide cross-coupling via formate-mediated transfer hydrogenation","authors":"Yoon Cho, Yu-Hsiang Chang, Kevin P. Quirion, Zachary H. Strong, Zachary J. Dubey, Nam Nguyen, Seoyoung Lee, Natalie S. Taylor, Jessica M. Hoover, Nicholas A. White, Peng Liu, Michael J. Krische","doi":"10.1038/s41557-024-01729-0","DOIUrl":"https://doi.org/10.1038/s41557-024-01729-0","url":null,"abstract":"Transfer hydrogenation is widely practised across all segments of chemical industry, yet its application to aryl halide reductive cross-coupling is undeveloped because of competing hydrogenolysis. Here, exploiting the distinct reactivity of PdI species, an efficient catalytic system for the reductive cross-coupling of activated aryl bromides with aryl iodides via formate-mediated hydrogen transfer is described. These processes display orthogonality with respect to Suzuki and Buchwald–Hartwig couplings, as pinacol boronates and anilines are tolerated and, owing to the intervention of chelated intermediates, are effective for challenging 2-pyridyl systems. Experimental and computational studies corroborate a unique catalytic cycle for reductive cross-coupling where the PdI precatalyst, [Pd(I)(PtBu3)]2, is converted to the dianionic species, [Pd2I4][NBu4]2, from which aryl halide oxidative addition is more facile. Rapid, reversible Pd-to-Pd transmetallation delivers mixtures of iodide-bridged homo- and hetero-diarylpalladium dimers. The hetero-diarylpalladium dimers are more stable and have lower barriers to reductive elimination, promoting high levels of cross-selectivity.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"4 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143589657","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

General strategy for the synthesis of N-monofluoromethyl amides n -单氟甲基酰胺合成的一般策略

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-03-11 DOI: 10.1038/s41557-025-01769-0

引用次数: 0

Biomimetic 1,2-amino migration via photoredox catalysis. 光氧化还原催化的仿生1,2-氨基迁移。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-03-07 DOI: 10.1038/s41557-025-01775-2

Weitai Fan, Yuang Cui, Beibei Zhan, Yizhou Chen, Lei Bao, Yufan Liang, Xiaheng Zhang

{"title":"Biomimetic 1,2-amino migration via photoredox catalysis.","authors":"Weitai Fan, Yuang Cui, Beibei Zhan, Yizhou Chen, Lei Bao, Yufan Liang, Xiaheng Zhang","doi":"10.1038/s41557-025-01775-2","DOIUrl":"https://doi.org/10.1038/s41557-025-01775-2","url":null,"abstract":"Synthetic organic chemists continually draw inspiration from biocatalytic processes to innovate synthetic methodologies beyond existing catalytic platforms. Within this context, although 1,2-amino migration represents a viable biochemical process, it remains underutilized within the synthetic organic chemistry community. Here we present a biomimetic 1,2-amino migration accomplished through the synergistic combination of biocatalytic mechanism and photoredox catalysis. This platform enables the modular synthesis of γ-substituted β-amino acids by utilizing abundant α-amino-acid derivatives and readily available organic molecules as coupling partners. This mild method features excellent substrate and functionality compatibility, affording a diverse range of γ-substituted β-amino acids (more than 80 examples) without the need for laborious multistep synthesis. Mechanistic studies, supported by both experimental observations and theoretical analysis, indicate that the 1,2-amino migration mechanism involves radical addition to α-vinyl-aldimine ester, 3-exo-trig cyclization and a subsequent rearrangement process. We anticipate that this transformation will serve as a versatile platform for the highly efficient construction of unnatural γ-substituted β-amino acids.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":19.2,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143586323","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 of a fluorinated macrobicyclic antibiotic through chemical synthesis 通过化学合成发现一种氟化大双环抗生素。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-03-07 DOI: 10.1038/s41557-025-01738-7

Ben I. C. Tresco, Kelvin J. Y. Wu, Antonio Ramkissoon, Elena V. Aleksandrova, Michael Purdy, Dominic N. Y. See, Richard Y. Liu, Yury S. Polikanov, Andrew G. Myers

{"title":"Discovery of a fluorinated macrobicyclic antibiotic through chemical synthesis","authors":"Ben I. C. Tresco, Kelvin J. Y. Wu, Antonio Ramkissoon, Elena V. Aleksandrova, Michael Purdy, Dominic N. Y. See, Richard Y. Liu, Yury S. Polikanov, Andrew G. Myers","doi":"10.1038/s41557-025-01738-7","DOIUrl":"10.1038/s41557-025-01738-7","url":null,"abstract":"The emergence of bacterial antimicrobial resistance threatens to undermine the utility of antibiotic therapy in medicine. This threat can be addressed, in part, by reinventing existing antibiotic classes using chemical synthesis. Here we present the discovery of BT-33, a fluorinated macrobicyclic oxepanoprolinamide antibiotic with broad-spectrum activity against multidrug-resistant bacterial pathogens. Structure–activity relationships within the macrobicyclic substructure reveal structural features that are essential to the enhanced potency of BT-33 as well as its increased metabolic stability relative to its predecessors clindamycin, iboxamycin and cresomycin. Using X-ray crystallography, we determine the structure of BT-33 in complex with the bacterial ribosome revealing that its fluorine atom makes an additional van der Waals contact with nucleobase G2505. Through variable-temperature 1H NMR experiments, density functional theory calculations and vibrational circular dichroism spectroscopy, we compare macrobicyclic homologues of BT-33 and a C7 desmethyl analogue and find that the C7 methyl group of BT-33 rigidifies the macrocyclic ring in a conformation that is highly preorganized for ribosomal binding. Antibiotic resistance can be addressed by reinventing classes of antibiotics through chemical synthesis. Here BT-33—a fully synthetic antibiotic—affords broad-spectrum activity against the bacterial ribosome. X-ray crystallography, theoretical calculations and structure–activity relationship studies reveal the structural features that contribute to the enhanced antibacterial activity and metabolic stability of BT-33.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"17 4","pages":"582-589"},"PeriodicalIF":19.2,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143586325","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

Non-enzymatic methylcyclization of alkenes. 烯烃的非酶甲基环化。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-03-07 DOI: 10.1038/s41557-025-01774-3

Immanuel Plangger, Elias Schmidhammer, Sebastian Schaar, Klaus Wurst, Maren Podewitz, Thomas Magauer

{"title":"Non-enzymatic methylcyclization of alkenes.","authors":"Immanuel Plangger, Elias Schmidhammer, Sebastian Schaar, Klaus Wurst, Maren Podewitz, Thomas Magauer","doi":"10.1038/s41557-025-01774-3","DOIUrl":"10.1038/s41557-025-01774-3","url":null,"abstract":"Methyltransferases are a broad class of enzymes that catalyse the transfer of methyl groups onto a wide variety of substrates and functionalities. In their most striking variant, bifunctional methyltransferase-cyclases both transfer a methyl group onto alkenes and induce cyclization (methylcyclization). Although recent years have seen substantial advances in the methylation of alkenes, especially hydromethylation, the reactivity demonstrated by bifunctional methyltransferase-cyclases in nature has yet to be developed into a synthetically viable method. Here we report a silver(I)-mediated electrophilic methylcyclization that rivals selectivities found in enzymes while not being limited by their inherent substrate specificity. Our method benefits from the use of commercial reagents, is applicable to a wide range of substrates, including heterocycles, and affords unique structures that are difficult to access via conventional synthetic methods. Furthermore, computational studies have been utilized to unravel the underlying mechanism and ultimately support a stepwise cationic reaction pathway with a rate-limiting methyltransfer.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":19.2,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7617478/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143586327","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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Preparing and publishing a paper 准备和发表论文

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-03-06 DOI: 10.1038/s41557-025-01759-2

Shira Joudan

引用次数: 0

The phosphate of life 生命的磷酸盐

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-03-06 DOI: 10.1038/s41557-025-01758-3

Elena De Vita, Rebecca Page

引用次数: 0