Nature chemistry最新文献_第4页

Self-assembly of chiroptical ionic co-crystals from silver nanoclusters and organic macrocycles 银纳米团簇和有机大环的共取向离子晶体自组装。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-08 DOI: 10.1038/s41557-024-01696-6

Yingwei Li, Grant J. Stec, Hong Ki Kim, Surendra Thapa, Shao-Liang Zheng, Arthur McClelland, Jarad A. Mason

{"title":"Self-assembly of chiroptical ionic co-crystals from silver nanoclusters and organic macrocycles","authors":"Yingwei Li, Grant J. Stec, Hong Ki Kim, Surendra Thapa, Shao-Liang Zheng, Arthur McClelland, Jarad A. Mason","doi":"10.1038/s41557-024-01696-6","DOIUrl":"10.1038/s41557-024-01696-6","url":null,"abstract":"Atomically precise nanoclusters can be assembled into ordered superlattices with unique electronic, magnetic, optical and catalytic properties. The co-crystallization of nanoclusters with functional organic molecules provides opportunities to access an even wider range of structures and properties, but can be challenging to control synthetically. Here we introduce a supramolecular approach to direct the assembly of atomically precise silver nanoclusters into a series of nanocluster‒organic ionic co-crystals with tunable structures and properties. By leveraging non-covalent interactions between anionic silver nanoclusters and cationic organic macrocycles of varying sizes, the orientation of nanocluster surface ligands can be manipulated to achieve in situ resolution of enantiopure nanocluster‒organic ionic co-crystals that feature large chiroptical effects. Beyond chirality, this co-crystal assembly approach provides a promising platform for designing functional solid-state nanomaterials through a combination of supramolecular chemistry and atomically precise nanochemistry. The co-crystallization of nanoclusters with functional organic molecules can provide access to superlattices with unique properties, but this process remains synthetically challenging. Now it has been shown that silver nanoclusters and organic macrocycles can be assembled through a supramolecular approach into ionic co-crystals with tunable structures and large chiroptical effects.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"17 2","pages":"169-176"},"PeriodicalIF":19.2,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142951999","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 pseudo-cubic metal–organic cage with conformationally switchable faces for dynamically adaptive guest encapsulation 具有构象可切换面的伪立方金属有机笼，用于动态自适应客体封装。

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-08 DOI: 10.1038/s41557-024-01708-5

Houyang Xu, Tanya K. Ronson, Andrew W. Heard, Paula C. P. Teeuwen, Laura Schneider, Philipp Pracht, John D. Thoburn, David J. Wales, Jonathan R. Nitschke

{"title":"A pseudo-cubic metal–organic cage with conformationally switchable faces for dynamically adaptive guest encapsulation","authors":"Houyang Xu, Tanya K. Ronson, Andrew W. Heard, Paula C. P. Teeuwen, Laura Schneider, Philipp Pracht, John D. Thoburn, David J. Wales, Jonathan R. Nitschke","doi":"10.1038/s41557-024-01708-5","DOIUrl":"10.1038/s41557-024-01708-5","url":null,"abstract":"The creation of hosts capable of accommodating different guest molecules may enable these hosts to play useful roles in chemical purifications, among other applications. Metal–organic cages are excellent hosts for various guests, but they generally incorporate rigid structural units that hinder dynamic adaptation to specific guests. Here we report a conformationally adaptable pseudo-cubic cage that can dynamically increase its cavity volume to fit guests with differing sizes. This pseudo-cube incorporates a tetramine subcomponent with 2,6-naphthalene arms that cooperatively adopt a non-planar conformation, enabling the cage faces to switch between endo and exo states. A wide range of guest molecules were observed to bind within the cavity of this cage, spanning a range of sizes from 46% to 154% of the cavity volume of the empty cage. Experimental and computational evidence characterizes the flipping of cage faces from endo to exo, expanding the cavity upon binding of larger guests. Synthetic nanocages that can adapt the size and shape of their cavity in response to a given guest have potential applications in various areas, including chemical purification. Now a flexible, pseudo-cubic metal–organic cage has been developed that is able to dynamically expand its cavity from 46% to 154% of its initial volume by flipping its cage faces.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"17 2","pages":"289-296"},"PeriodicalIF":19.2,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41557-024-01708-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142951997","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

Remote control of chirality in hybrid perovskite materials 杂化钙钛矿材料手性的远程控制

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-07 DOI: 10.1038/s41557-024-01694-8

Ghewa AlSabeh, Mengqiong Zhu, Jovana V. Milić

引用次数: 0

Practical electronics and robotics for chemists 化学家的实用电子学和机器人技术

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-07 DOI: 10.1038/s41557-024-01703-w

Pawel L. Urban

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Porphyrins are nature’s workhorse 卟啉是自然界的主力

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-07 DOI: 10.1038/s41557-024-01701-y

Paulina Krzyszowska, Ewa Pacholska-Dudziak

引用次数: 0

Beyond grateful 除了感激

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-07 DOI: 10.1038/s41557-024-01704-9

Michelle Francl

引用次数: 0

Bottleable triplet nitrenes 瓶装三态亚胺

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-07 DOI: 10.1038/s41557-024-01700-z

Dominik Munz

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Accelerating stereoselective radical cross-couplings 加速立体选择性自由基交叉偶联

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-07 DOI: 10.1038/s41557-024-01702-x

Gregory R. Alvey, David L. Avetian, Markus D. Kärkäs

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De novo design of ribosomally synthesized and post-translationally modified peptides 核糖体合成和翻译后修饰肽的从头设计

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-07 DOI: 10.1038/s41557-024-01685-9

Emerson Glassey, Zhengan Zhang, Andrew M. King, David L. Niquille, Christopher A. Voigt

{"title":"De novo design of ribosomally synthesized and post-translationally modified peptides","authors":"Emerson Glassey, Zhengan Zhang, Andrew M. King, David L. Niquille, Christopher A. Voigt","doi":"10.1038/s41557-024-01685-9","DOIUrl":"10.1038/s41557-024-01685-9","url":null,"abstract":"In nature, peptides are enzymatically modified to constrain their structure and introduce functional moieties. De novo peptide structures could be built by combining enzymes from different pathways, but determining the rules of their use is difficult. We present a biophysical model to combine enzymes sourced from bacterial ribosomally synthesized and post-translationally modified peptide (RiPP) gene clusters. Using a pipeline to evaluate more than 1,000 peptides, the model was parameterized under uniform conditions in Escherichia coli for enzymes from different classes (graspetide, spliceotide, pantocin, cyanobactin, glycocin, lasso peptide and lanthipeptide). Synthetic leader peptides with recognition sequences for up to three enzymes were designed to modify core sequences sharing no identity to natural RiPPs. Empirically, RiPPs with the desired modifications constituted 7–67% of the total peptides produced, and 6 of our 8 peptide designs were successfully modified. This work is an example of the design of enzyme-modified peptides and libraries, using a framework that can be expanded to include new enzymes and chemical moieties. Combining enzymes from different pathways in nature could enable de novo peptide design, but determining enzyme-specificity rules is non-trivial. Here a biophysical model combining enzymes sourced from bacterial ribosomally synthesized and post-translationally modified peptide (RiPP) gene clusters was generated to formalize enzyme-specificity rules and create peptide scaffolds with defined post-translational modifications.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"17 2","pages":"233-245"},"PeriodicalIF":19.2,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142934720","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

Synthesis of single-crystalline sp2-carbon-linked covalent organic frameworks through imine-to-olefin transformation 通过亚胺-烯烃转化合成sp2-碳键单晶共价有机骨架

IF 19.2 1区化学

Nature chemistry Pub Date : 2025-01-06 DOI: 10.1038/s41557-024-01690-y

Shengxu Li, Shunqi Xu, En Lin, Tonghai Wang, Haoyong Yang, Junyi Han, Yuxiang Zhao, Qunji Xue, Paolo Samorì, Zhenjie Zhang, Tao Zhang

{"title":"Synthesis of single-crystalline sp2-carbon-linked covalent organic frameworks through imine-to-olefin transformation","authors":"Shengxu Li, Shunqi Xu, En Lin, Tonghai Wang, Haoyong Yang, Junyi Han, Yuxiang Zhao, Qunji Xue, Paolo Samorì, Zhenjie Zhang, Tao Zhang","doi":"10.1038/s41557-024-01690-y","DOIUrl":"10.1038/s41557-024-01690-y","url":null,"abstract":"sp2-carbon-linked covalent organic frameworks (sp2c-COFs) are crystalline porous polymers with repeat organic units linked by sp2 carbons, and have attracted increasing interest due to their robust skeleton and tunable semiconducting properties. Single-crystalline sp2c-COFs with well-defined structures can represent an ideal platform for investigating fundamental physics properties and device performance. However, the robust olefin bonds inhibit the reversible-reaction-based crystal self-correction, thus yielding polycrystalline or amorphous polymers. Here we report an imine-to-olefin transformation strategy to form single-crystal sp2c-COFs. The isolated single crystals display rectangular nanotube-like domains with sizes up to approximately 24 μm × 0.8 μm × 0.8 μm, and permanent pore distribution around 1.1 nm. The highly conjugated olefin linkage endows the crystals with enhanced electronic connectivity which determines a remarkable room-temperature metal-free ferromagnetism (8.6 × 10−3 emu g−1). Our protocol is robust and generally applicable for the synthesis of single-crystalline sp2c-COFs for future spin-electron devices. Olefin-linked covalent organic frameworks are materials with potential application as organic semiconductors, but their synthesis remains challenging. Now, single-crystal sp2-carbon-linked covalent organic frameworks have been prepared through an imine-to-olefin transformation strategy; the resulting materials feature enhanced room-temperature metal-free ferromagnetism.","PeriodicalId":18909,"journal":{"name":"Nature chemistry","volume":"17 2","pages":"226-232"},"PeriodicalIF":19.2,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929695","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