Nature chemistry最新文献_第5页

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-28 DOI: 10.1038/s41557-026-02236-0

Shira Joudan

引用次数: 0

Cyclopropanol can function as a caged dual-functional warhead for selective electrochemical bioconjugation. 环丙醇可作为笼型双功能战斗部用于选择性电化学生物偶联。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-28 DOI: 10.1038/s41557-026-02227-1

Shan Hu, Xiaoying Lian, Jinnawat Jongkhumkrong, Öznur Ölmez Nalcıoğlu, Akshani Anjula Wijesooriya, Diqi Yan, James D Sitter, Hao Liu, Michael Walla, William E Cotham, Aaron K Vannucci, Qian Wang

{"title":"Cyclopropanol can function as a caged dual-functional warhead for selective electrochemical bioconjugation.","authors":"Shan Hu, Xiaoying Lian, Jinnawat Jongkhumkrong, Öznur Ölmez Nalcıoğlu, Akshani Anjula Wijesooriya, Diqi Yan, James D Sitter, Hao Liu, Michael Walla, William E Cotham, Aaron K Vannucci, Qian Wang","doi":"10.1038/s41557-026-02227-1","DOIUrl":"https://doi.org/10.1038/s41557-026-02227-1","url":null,"abstract":"Bioorthogonal reactions enable the study and modulation of biological systems, but achieving precise control over when and where the reactions occur remains challenging. Here we show that cyclopropanol (CPol) can serve as a compact, energy-loaded chemical handle that is stable under physiological conditions, yet can be selectively activated using mild electrochemical stimuli. This strategy generates reactive β-haloketone moieties in situ, enabling efficient protein labelling for cellular imaging and proteomic analysis. Unexpectedly, CPol preferentially modifies acidic amino acids, such as glutamate and aspartate, within hydrophobic regions of proteins, rather than more commonly targeted residues. The electrochemical reaction is compatible with living cells, allowing real-time visualization using fluorogenic probes. We further demonstrate its utility by developing a choline-derived CPol probe that integrates into membrane lipid metabolism to label membrane-associated and cytoplasmic proteins. By combining bioorthogonality with electrochemical control, this approach offers a general and controllable platform for protein conjugation, with broader applications in chemical biology and live-cell studies.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148850518","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

Programmable regiodivergent light-driven cyclization of acyclic 1,5-dienes unlocks rigid bicyclic architectures. 非环1,5-二烯的可编程区域发散光驱动环化解锁刚性双环结构。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-27 DOI: 10.1038/s41557-026-02238-y

Ze-Xin Zhang, KaiChen Shu, Mihai V Popescu, Yiheng Guo, Jasper L Tyler, Robert S Paton, Varinder K Aggarwal

{"title":"Programmable regiodivergent light-driven cyclization of acyclic 1,5-dienes unlocks rigid bicyclic architectures.","authors":"Ze-Xin Zhang, KaiChen Shu, Mihai V Popescu, Yiheng Guo, Jasper L Tyler, Robert S Paton, Varinder K Aggarwal","doi":"10.1038/s41557-026-02238-y","DOIUrl":"10.1038/s41557-026-02238-y","url":null,"abstract":"Controlling regioselectivity in radical cyclizations remains a major challenge in synthetic chemistry, hindering the efficient assembly of strained, rigid bicyclic architectures from simple acyclic precursors. Here we show that a visible-light-mediated intramolecular [2 + 2] photocycloaddition of aza-1,5-dienes can successfully overcome the classical 'rule-of-five' selectivity governing radical cyclizations. By tuning the electronic properties of an easily removable amide N-substituent, we reprogram the initial energy-transfer-driven cyclization event, diverging from the usually kinetically favoured 5-exo-trig to the 6-endo-trig pathway. As a result, closely related substrates can be selectively directed to generate either bridged bicyclo[2.1.1] or vastly underexplored fused bicyclo[2.2.0] architectures, both of which offer rich downstream derivatization potential. Furthermore, an extensive computational study of this transformation revealed how the intricate interplay of electronic effects controls reaction regioselectivity. Overall, this work establishes a programmable, light-driven cyclization strategy that enables precise and selective construction of distinct bicyclic frameworks within a unified reaction manifold.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13590158/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148840867","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 general strategy towards multicolour fluorogenic peptides for wash-free bioassays. 用于免洗生物测定的多色荧光肽的一般策略。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-26 DOI: 10.1038/s41557-026-02228-0

Man Sing Wong, Lorena Mendive-Tapia, Utsa Karmakar, Lovelesh Vashist, Zandile Nare, Karolina Tokarczyk, Kohei Iijima, Kazuya Kikuchi, Syed Ali Abbas Abedi, Xiaogang Liu, Marc Vendrell

{"title":"A general strategy towards multicolour fluorogenic peptides for wash-free bioassays.","authors":"Man Sing Wong, Lorena Mendive-Tapia, Utsa Karmakar, Lovelesh Vashist, Zandile Nare, Karolina Tokarczyk, Kohei Iijima, Kazuya Kikuchi, Syed Ali Abbas Abedi, Xiaogang Liu, Marc Vendrell","doi":"10.1038/s41557-026-02228-0","DOIUrl":"https://doi.org/10.1038/s41557-026-02228-0","url":null,"abstract":"Peptide-based fluorescent probes are valuable tools for live-cell imaging, but conventional labelling approaches often require washing or long incubation, limiting their signal-to-noise ratios. Fluorogenic amino acids (FgAAs) can overcome these limitations, yet their rational design remains challenging owing to the lack of generalizable quenching principles and synthetic routes compatible with diverse fluorophores. Here we developed a general strategy to convert constitutively bright fluorophores into turn-on FgAAs through intramolecular tryptophan-induced quenching. Computational analysis showed that quenching is governed by photoinduced electron transfer or twisted intramolecular charge transfer mechanisms, with adaptability across ultraviolet-to-near-infrared fluorophore scaffolds. We synthesized a large library of multicolour FgAAs and integrated them into solid-phase peptide synthesis to generate turn-on probes for real-time microscopy in live cells. We then designed fluorogenic peptides targeting programmed cell death protein 1 (PD-1), enabling T cell targeted drug screening and identifying avasimibe as a small-molecule modulator of PD-1 activity. This work establishes a rational strategy for designing multicolour FgAAs for peptide engineering, imaging and drug discovery.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":24.5,"publicationDate":"2026-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148830596","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

Artificial photosynthetic reduction of nitrogen to ammonia at room temperature using natural seawater 利用天然海水在室温下人工光合作用将氮还原为氨。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-25 DOI: 10.1038/s41557-026-02218-2

Doha Zidouhia, Thierry Tassaing, Nicolas Penin, Etienne Grau, Dario M. Bassani

{"title":"Artificial photosynthetic reduction of nitrogen to ammonia at room temperature using natural seawater","authors":"Doha Zidouhia, Thierry Tassaing, Nicolas Penin, Etienne Grau, Dario M. Bassani","doi":"10.1038/s41557-026-02218-2","DOIUrl":"10.1038/s41557-026-02218-2","url":null,"abstract":"Natural photosynthesis uses light and water to fuel cellular activity. While great strides have been made in reproducing elements of photosynthesis, efficiently coupling dinitrogen reduction to ammonia with water oxidation remains challenging. Here we report the light-driven production of ammonia from dinitrogen reduction with a quantum yield of 5.0% in water at normal temperature and pressure by leveraging inexpensive iron(II) salts, which produce solvated electrons upon ultraviolet C light irradiation, to reduce a Mo catalyst. The resulting Fe(III) ions also absorb ultraviolet light and undergo reduction back to Fe(II) while oxidizing water, thus coupling water oxidation with nitrogen reduction. Although the low solubility of nitrogen in water limits catalysis, we circumvented this limitation by using elevated dinitrogen pressures to reach photochemical quantum yields of 10.8%. We further demonstrate this reactivity to operate even in unpurified seawater or in ambient air. The process is calculated to be endoergonic by 329.2 kJ mol−1 in agreement with a photosynthetic process possessing a light-to-chemical energy conversion efficiency of 7.6%. Ammonia production is responsible for 1.8% of greenhouse gas emissions, inspiring research efforts into alternative, renewable-powered approaches. Now it has been shown that artificial photosynthesis, coupling nitrogen reduction to water oxidation, can proceed efficiently and with high selectivity in seawater or under ambient air.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 10","pages":"1737-1746"},"PeriodicalIF":24.5,"publicationDate":"2026-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148819100","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

Genetically targeted dyes light up cell-specific abiotic synthesis 基因靶向染料点亮细胞特异性非生物合成。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-21 DOI: 10.1038/s41557-026-02230-6

Ting Wu, Zhaowei Chen, Huanghao Yang

引用次数: 0

Understanding and suppressing gas evolution in lithium metal batteries with ether-based electrolytes 了解和抑制醚基电解质在锂金属电池中的气体释放。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-20 DOI: 10.1038/s41557-026-02219-1

Samantha T. Hung, Yuchun Wang, Ziman Cai, Chongzhen Wang, Zirui Shao, Juanjuan Sun, Haoran Li, Jinding Liang, Lu Bai, Erxiao Wu, Ulderico Ulissi, Xiaolin Yan, Fangyun Chen, Falin Zhu, Junhao He, Xiaonan Luo, Na Liu, Hansen Wang, Chuying Ouyang

{"title":"Understanding and suppressing gas evolution in lithium metal batteries with ether-based electrolytes","authors":"Samantha T. Hung, Yuchun Wang, Ziman Cai, Chongzhen Wang, Zirui Shao, Juanjuan Sun, Haoran Li, Jinding Liang, Lu Bai, Erxiao Wu, Ulderico Ulissi, Xiaolin Yan, Fangyun Chen, Falin Zhu, Junhao He, Xiaonan Luo, Na Liu, Hansen Wang, Chuying Ouyang","doi":"10.1038/s41557-026-02219-1","DOIUrl":"10.1038/s41557-026-02219-1","url":null,"abstract":"Understanding and suppressing gas evolution is critical to enabling high-energy-density lithium metal batteries (LMBs). Yet, comprehensive investigations in ether-based systems remain limited. Here we quantify gas generation in ether-based LMBs and elucidate the underlying mechanisms. We link CO and CO2 production to the cathode, and CH4 evolution to the anode. Notably, CO and CO2 are consumed at the Li anode to form Li-containing species such as Li2CO3. Although CH4 ultimately dominates the gaseous products, its evolution during cycling is delayed until a distinct onset point. We show that in a high-concentration ether electrolyte, anode activation improves Li deposition morphology and suppresses interfacial reactions, extending the number of cycles to gas onset and cell failure by an order of magnitude. Achieving these gains without altering the electrolyte enables the reconsideration of seemingly impractical electrolytes, highlighting a practical strategy to enhance the safety and performance of commercial LMBs. Gas evolution compromises the safety and commercial viability of high-energy lithium metal batteries. Now it has been shown that CH4 generated by ether-based electrolyte decomposition at the Li anode dominates gas evolution. A facile anode activation strategy suppresses CH4-forming interfacial reactions, dramatically reducing gas evolution and extending cycle life.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"18 10","pages":"1809-1818"},"PeriodicalIF":24.5,"publicationDate":"2026-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41557-026-02219-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148795785","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

When pathways trump orbitals in electrolyte design 在电解质设计中，当途径胜过轨道时。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-20 DOI: 10.1038/s41557-026-02239-x

Zheng Li, Chunsheng Wang

引用次数: 0

Publisher Correction: How webby is the wood-wide web? 出版者更正：整个森林的网络有多复杂？

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-20 DOI: 10.1038/s41557-026-02250-2

Bruce C. Gibb

引用次数: 0

Nitrene generation and transfer for unnatural biosynthesis in living cells. 活细胞中非自然生物合成的亚硝基烯的产生和转移。

IF 24.5 1区化学

Nature chemistry Pub Date : 2026-08-18 DOI: 10.1038/s41557-026-02224-4

Isaac Donnell, Andrew Quest, Jeremy Tang, Maodun Zhang, Brandon Bloomer, Douglas S Clark, Aindrila Mukhopadhyay, John Hartwig, Jay D Keasling

{"title":"Nitrene generation and transfer for unnatural biosynthesis in living cells.","authors":"Isaac Donnell, Andrew Quest, Jeremy Tang, Maodun Zhang, Brandon Bloomer, Douglas S Clark, Aindrila Mukhopadhyay, John Hartwig, Jay D Keasling","doi":"10.1038/s41557-026-02224-4","DOIUrl":"10.1038/s41557-026-02224-4","url":null,"abstract":"Synthetic biology has enabled the production of natural and unnatural products from inexpensive sustainable feedstocks. Yet, the scope of available products has been limited largely to compounds accessible from nature's chemical reactions. Evolved enzymes can catalyse reactions of unnatural substrates or reactions not found in nature but often require the addition of synthetic reagents to purified enzymes or to resting cells containing those enzymes. Here we show that chemical reactions of metabolic intermediates produced intracellularly in living cells can include intermolecular nitrene transfers. The biosynthesis of N-acetoxyanilines, in combination with the generation and transfer of N-aryl nitrene intermediates from them catalysed by a cytochrome P450, generates amino alcohols, diamines, diarylamines and aminoalkyl arenes from simple carbon feedstocks. These products-common substructures of pharmaceuticals and agrochemicals-are challenging to synthesize by standard organic chemistry and were produced from inexpensive, renewable feedstocks. Evolution of the enzymes in this pathway showed that titres can be increased by engineering and that the products can be synthesized with high enantioselectivity.","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":"148795828","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