Nature chemistry最新文献

Modular alkyl growth in amines via the selective insertion of alkynes into C–C bonds 通过选择性地在C-C键中插入炔在胺中的模烷基生长

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-06-12 DOI: 10.1038/s41557-025-01849-1

Xin-Yue Zhou, Lu Liu, Hairong Lyu, Xiao-Chen Wang

引用次数: 0

A designer minimalistic model parallels the phase-separation-mediated assembly and biophysical cues of extracellular matrix 设计师简约的模型平行于相分离介导的组装和细胞外基质的生物物理线索

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-06-09 DOI: 10.1038/s41557-025-01837-5

Xian Xie, Tianjie Li, Linjie Ma, Jiahao Wu, Yajing Qi, Boguang Yang, Zhuo Li, Zhinan Yang, Kunyu Zhang, Zhiqin Chu, To Ngai, Jiang Xia, Yi Wang, Pengchao Zhao, Liming Bian

{"title":"A designer minimalistic model parallels the phase-separation-mediated assembly and biophysical cues of extracellular matrix","authors":"Xian Xie, Tianjie Li, Linjie Ma, Jiahao Wu, Yajing Qi, Boguang Yang, Zhuo Li, Zhinan Yang, Kunyu Zhang, Zhiqin Chu, To Ngai, Jiang Xia, Yi Wang, Pengchao Zhao, Liming Bian","doi":"10.1038/s41557-025-01837-5","DOIUrl":"https://doi.org/10.1038/s41557-025-01837-5","url":null,"abstract":"The propensity for controlled liquid–liquid phase separation and subsequent directed phase transition are crucial for the coacervation-mediated assembly of extracellular matrix (ECM). This spatiotemporally controlled ECM assembly can be used to develop coacervate-based polymer assembly strategies to generate biomimetic materials that can emulate the complex structures and biophysical cues of the ECM. Inspired by the tropoelastin structure, here we develop a designer minimalistic model consisting of alternating hydrophobic moieties and covalent crosslinking domains. By increasing the valence and enhancing the interaction strength of the hydrophobic moieties, we can control the degree of the assembly to enhance the propensity for phase separation and thus emulate the extracellular coacervation process of tropoelastin, including droplet formation, coalescence and maturation. The subsequent covalent-bonding-triggered coacervate–hydrogel transition with enhanced assembly order stabilizes the phase-separated structure in the form of a heterogeneous hydrogel, thereby mimicking covalent crosslinking-derived elastin fibrillation. Furthermore, the heterogeneous hydrogel network establishes a biomimetic matrix that can effectively promote the mechanosensing of adherent stem cells.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"45 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144238003","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

Controlling our online professional persona 控制我们的在线职业形象

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-06-05 DOI: 10.1038/s41557-025-01839-3

Shira Joudan

引用次数: 0

Linked in with lignin 与木质素相连

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-06-05 DOI: 10.1038/s41557-025-01824-w

Moses Dike, Shudipto Konika Dishari

引用次数: 0

Information propagation through enzyme-free catalytic templating of DNA dimerization with weak product inhibition 无酶催化模板DNA二聚化的信息传播与弱产物抑制

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-06-05 DOI: 10.1038/s41557-025-01831-x

Javier Cabello-Garcia, Rakesh Mukherjee, Wooli Bae, Guy-Bart V. Stan, Thomas E. Ouldridge

{"title":"Information propagation through enzyme-free catalytic templating of DNA dimerization with weak product inhibition","authors":"Javier Cabello-Garcia, Rakesh Mukherjee, Wooli Bae, Guy-Bart V. Stan, Thomas E. Ouldridge","doi":"10.1038/s41557-025-01831-x","DOIUrl":"https://doi.org/10.1038/s41557-025-01831-x","url":null,"abstract":"Information propagation by sequence-specific, template-catalysed molecular assembly is a key process facilitating life’s biochemical complexity, yielding thousands of sequence-defined proteins from only 20 distinct building blocks. However, exploitation of catalytic templating is rare in non-biological contexts, particularly in enzyme-free environments, where even the template-catalysed formation of dimers is challenging. Typically, product inhibition—the tendency of products to bind to templates more strongly than individual monomers—prevents catalytic turnover. Here we present a rationally designed enzyme-free system in which a DNA template catalyses, with weak product inhibition, the production of sequence-specific DNA dimers. We demonstrate selective templating of nine different dimers with high specificity and catalytic turnover, then we show that the products can participate in downstream reactions, and finally that the dimerization can be coupled to covalent bond formation. Most importantly, our mechanism demonstrates a design principle for constructing synthetic molecular templating systems, a first step towards applying this powerful motif in non-biological contexts to construct many complex molecules and materials from a small number of building blocks.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"5 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144218785","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

Interfacial assembly of biomimetic MOF-based porous membranes on coacervates to build complex protocells and prototissues. 基于mof的仿生多孔膜在凝聚体上的界面组装以构建复杂的原始细胞和原始组织。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-06-04 DOI: 10.1038/s41557-025-01827-7

Yanglimin Ji, Yiyang Lin, Yan Qiao

{"title":"Interfacial assembly of biomimetic MOF-based porous membranes on coacervates to build complex protocells and prototissues.","authors":"Yanglimin Ji, Yiyang Lin, Yan Qiao","doi":"10.1038/s41557-025-01827-7","DOIUrl":"https://doi.org/10.1038/s41557-025-01827-7","url":null,"abstract":"The bottom-up construction of cell-like entities or protocells is essential for emulating cytomimetic behaviours within artificial cell consortia. Complex coacervate microdroplets are promising candidates for primordial cells; however, replicating the complex cellular organization and cell-cell interactions using membraneless coacervates remains a major challenge. To address this, we developed membrane-bound coacervate protocells by interfacial assembly of metal-organic framework nanoparticles around coacervate microdroplets. By leveraging the inherently porous structure and surface chemistry of metal-organic frameworks, we demonstrated the ability to regulate biomolecular organization within the protocells and integrate proteins into the membrane, thereby imitating both integral and peripheral membrane proteins. These membranized coacervates were further engineered into artificial-organelle-incorporated protocells and tissue-like assemblies capable of signal processing and protocell-to-protocell communication. Our findings highlight the potential of designing artificial systems with spatially controlled biomolecular organization to mimic natural cellular functions, paving the way for the assembly of membranized coacervates into prototissues.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":""},"PeriodicalIF":19.2,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144226013","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

Building ultramicroporous zirconium metal‒organic frameworks with ligands of high coordination density through a reticular approach 用网状法构建具有高配位密度配体的超微孔金属锆有机骨架

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-06-04 DOI: 10.1038/s41557-025-01836-6

Liang Yu, Shenfang Li, Xin Zhou, Bochun Zhang, Kang Zhou, Qibin Xia, Sujing Wang, Jing Li, Hao Wang

{"title":"Building ultramicroporous zirconium metal‒organic frameworks with ligands of high coordination density through a reticular approach","authors":"Liang Yu, Shenfang Li, Xin Zhou, Bochun Zhang, Kang Zhou, Qibin Xia, Sujing Wang, Jing Li, Hao Wang","doi":"10.1038/s41557-025-01836-6","DOIUrl":"https://doi.org/10.1038/s41557-025-01836-6","url":null,"abstract":"The rational design and synthesis of ultramicroporous solids featuring uniform pore dimensions remains a notable challenge, yet these materials are critical for the selective discrimination of molecules with similar physicochemical properties. Here we report a family of ten ultramicroporous zirconium-based metal–organic frameworks assembled from isophthalate-based octatopic or hexatopic carboxylate linkers with high coordination density and Zr6 nodes with relatively low connectivity (4, 6 and 8). The diverse inorganic node geometry, ligand connectivity, structural topology, framework stability and ultramicroporosity of the resultant metal–organic frameworks underscore the pivotal role of linker geometry and functionality in tailoring the adsorptive properties of the material. These ultramicroporous solids hold promise for the separation of industrially relevant hydrocarbons. We show that HIAM-802 and HIAM-601 exhibit high-efficiency separation of hexane isomers based on branching by molecular exclusion. We validated their separation capabilities through breakthrough experiments and further clarified the underlying adsorption mechanisms by density functional theory calculations.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"4 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211619","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

A selenoxide for single-atom protein modification of tyrosine residues enabled by water-resistant chalcogen and hydrogen bonding 一种用于酪氨酸残基单原子蛋白修饰的硒酸盐，通过耐水的硫和氢键来实现

IF 21.8 1区化学

Nature chemistry Pub Date : 2025-06-04 DOI: 10.1038/s41557-025-01842-8

Songyun Lin, Marina Hirao, Philipp Hartmann, Markus Leutzsch, Marie Sophie Sterling, Alessandro Vetere, Sandra Klimmek, Heike Hinrichs, Johanna Marie Mengeler, Johannes Lehmann, Jan Samsonowicz-Gόrski, Florian Berger, Tobias Ritter

{"title":"A selenoxide for single-atom protein modification of tyrosine residues enabled by water-resistant chalcogen and hydrogen bonding","authors":"Songyun Lin, Marina Hirao, Philipp Hartmann, Markus Leutzsch, Marie Sophie Sterling, Alessandro Vetere, Sandra Klimmek, Heike Hinrichs, Johanna Marie Mengeler, Johannes Lehmann, Jan Samsonowicz-Gόrski, Florian Berger, Tobias Ritter","doi":"10.1038/s41557-025-01842-8","DOIUrl":"https://doi.org/10.1038/s41557-025-01842-8","url":null,"abstract":"Post-translational modifications such as phosphorylation and acetylation are often minor structural modifications that can have profound effects on protein structure and thus broaden protein functions. Nevertheless, studying these effects directly is often out of reach because no general chemistry exists to introduce small modifications selectively; either a large, stable linker structure is selectively installed on protein residues, or a small substituent is introduced at the risk of low selectivity due to the use of reactive, indiscriminate molecules. Here we report a C–H functionalization reaction of tyrosine residues to access peptides and proteins modified by small structural changes including single-atom substitutions. A rationally designed selenoxide introduces a versatile selenonium linchpin featuring a Ctyr–Se bond that can be used for further transformations at specific tyrosine residues. Key to the advance is the interplay of water-resistant, intramolecular chalcogen and hydrogen bonding of the selenoxide reagent, which allows chemo- and site-selective electrophilic aromatic substitution of tyrosine residues in aqueous solutions.<figure></figure>","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"20 1","pages":""},"PeriodicalIF":21.8,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144211618","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

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 : 2025-06-01 Epub 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":"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":"941-951"},"PeriodicalIF":19.2,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12141034/pdf/","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":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Switchable skeletal editing of quinolines enabled by cyclizative sequential rearrangements. 通过循环顺序重排实现喹啉类的可切换骨架编辑。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-06-01 Epub Date: 2025-04-07 DOI: 10.1038/s41557-025-01793-0

Di Tian, Yu-Ping He, Lu-Sen Yang, Zhuo-Chen Li, Hua Wu

{"title":"Switchable skeletal editing of quinolines enabled by cyclizative sequential rearrangements.","authors":"Di Tian, Yu-Ping He, Lu-Sen Yang, Zhuo-Chen Li, Hua Wu","doi":"10.1038/s41557-025-01793-0","DOIUrl":"10.1038/s41557-025-01793-0","url":null,"abstract":"The rapid diversification of core ring structures in complex molecules through switchable skeletal editing is valuable in the drug discovery process. However, controllable methods for chemically divergent modifications of azaarene frameworks using common substrates are challenging, despite the potential to maximize structural diversity and complexity. Here we report the tunable skeletal editing of quinolines through Brønsted acid-catalysed multicomponent reactions of quinoline N-oxides, dialkyl acetylenedicarboxylates and water to generate nitrogen-containing heteroaromatic compounds together with linear compounds in a modular fashion. Specifically, in a one-pot procedure, after cyclization and sequential rearrangement processes, the quinoline N-oxides are easily converted into unique 2-substituted indolines. These then undergo acid-promoted fragmentation to give indoles, base-facilitated ring-opening to afford 2-alkenylanilines and oxidative cyclization to yield isoquinolinones. Catalytic asymmetric skeletal editing of quinolines is also realized, providing enantioenriched benzazepines bearing quaternary stereocentres, and late-stage skeletal modification of quinoline cores in several drugs is demonstrated.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":" ","pages":"952-960"},"PeriodicalIF":19.2,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143803894","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