Nature synthesis最新文献_第10页

Up–down approach for expanding the chemical space of metal–organic frameworks 拓展金属有机框架化学空间的 "上-下 "方法

Nature synthesis Pub Date : 2024-09-05 DOI: 10.1038/s44160-024-00638-x

Jiyeon Kim, Dongsik Nam, Hye Jin Cho, Eunchan Cho, Dharmalingam Sivanesan, Changhyeon Cho, Jaewoong Lee, Jihan Kim, Wonyoung Choe

{"title":"Up–down approach for expanding the chemical space of metal–organic frameworks","authors":"Jiyeon Kim, Dongsik Nam, Hye Jin Cho, Eunchan Cho, Dharmalingam Sivanesan, Changhyeon Cho, Jaewoong Lee, Jihan Kim, Wonyoung Choe","doi":"10.1038/s44160-024-00638-x","DOIUrl":"10.1038/s44160-024-00638-x","url":null,"abstract":"The vast structural diversity of metal–organic frameworks (MOFs) and the ability to tailor the structures makes the materials applicable for a broad range of uses. Traditional bottom-up and top-down design approaches have enabled a rapid increase in this structural diversity, yet the systematic screening for unknown synthesizable MOFs remains a challenge. Here we report a design strategy, the up–down approach, by merging the bottom-up and top-down approaches. This approach bridges the advantages of both methods, creating a synergistic strategy for discovering MOF structures. Targeting Zr-based MOFs, we search promising topology candidates and unveiled 26 future structural configurations by considering the possible orientations of Zr6 clusters. Through ribbon representation and sophisticated analysis of the ligand angles, we suggest structure models and synthesize Zr6-based MOFs with bct (1) and scu (1) configurations. The up–down approach will accelerate the discovery of previously unknown or inaccessible MOFs, providing exciting opportunities to expand the chemical space of MOFs. An up–down approach for discovering metal–organic frameworks (MOFs) identifies 26 unknown Zr-based MOF configurations and provides a valuable guide for synthetic chemists to expand the chemical space of MOFs.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1518-1528"},"PeriodicalIF":0.0,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195628","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Retraction Note: Synthesis of γ-graphyne using dynamic covalent chemistry 撤稿说明：利用动态共价化学合成γ-石墨烯

Nature synthesis Pub Date : 2024-09-02 DOI: 10.1038/s44160-024-00627-0

Yiming Hu, Chenyu Wu, Qingyan Pan, Yinghua Jin, Rui Lyu, Vikina Martinez, Shaofeng Huang, Jingyi Wu, Lacey J. Wayment, Noel A. Clark, Markus B. Raschke, Yingjie Zhao, Wei Zhang

引用次数: 0

On the characterization of γ-graphyne 论γ-石墨烯的特性

Nature synthesis Pub Date : 2024-09-02 DOI: 10.1038/s44160-024-00642-1

William B. Martin, Robert E. Warburton, Shane M. Parker, Valentin O. Rodionov

引用次数: 0

Retraction Note: Synthesizing γ-graphyne 撤稿说明：合成γ-石墨烯

Nature synthesis Pub Date : 2024-09-02 DOI: 10.1038/s44160-024-00625-2

Michael M. Haley

引用次数: 0

Spiro-buckybowl synthesis 螺-巴基波合成

Nature synthesis Pub Date : 2024-08-30 DOI: 10.1038/s44160-024-00650-1

Peter W. Seavill

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Methane to methanol 甲烷制甲醇

Nature synthesis Pub Date : 2024-08-30 DOI: 10.1038/s44160-024-00651-0

Alexandra R. Groves

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Integrating multiple interactions for the assembly of ordered organic frameworks 整合多种相互作用，组装有序有机框架

Nature synthesis Pub Date : 2024-08-30 DOI: 10.1038/s44160-024-00641-2

引用次数: 0

Upgrading carbon monoxide to bioplastics via integrated electrochemical reduction and biosynthesis 通过集成电化学还原和生物合成将一氧化碳升级为生物塑料

Nature synthesis Pub Date : 2024-08-28 DOI: 10.1038/s44160-024-00621-6

Tae-Ung Wi, Yongchao Xie, Zachary H. Levell, Danyi Feng, Jung Yoon ‘Timothy’ Kim, Peng Zhu, Ahmad Elgazzar, Tae Hwa Jeon, Mohsen Shakouri, Shaoyun Hao, Zhiwei Fang, Chang Qiu, Hyun-Wook Lee, Andrea Hicks, Yuanyue Liu, Chong Liu, Haotian Wang

{"title":"Upgrading carbon monoxide to bioplastics via integrated electrochemical reduction and biosynthesis","authors":"Tae-Ung Wi, Yongchao Xie, Zachary H. Levell, Danyi Feng, Jung Yoon ‘Timothy’ Kim, Peng Zhu, Ahmad Elgazzar, Tae Hwa Jeon, Mohsen Shakouri, Shaoyun Hao, Zhiwei Fang, Chang Qiu, Hyun-Wook Lee, Andrea Hicks, Yuanyue Liu, Chong Liu, Haotian Wang","doi":"10.1038/s44160-024-00621-6","DOIUrl":"10.1038/s44160-024-00621-6","url":null,"abstract":"It is challenging to obtain high-value hydrocarbons that are longer than C3 via electrochemical CO2/CO reduction. Integrating electrochemical CO2/CO electrolysers with a downstream bioreactor is one solution for obtaining high-value long-chain products, but the electrolytes in these two systems are mismatched, preventing smooth integration. Here we demonstrate a porous solid electrolyte reactor that produces highly selective and electrolyte-free acetate and couple it with a biosynthesis system for generating C4+ polyhydroxybutyrate bioplastic. A finely tuned electrolyte containing biocompatible salt medium with acetate can be directly injected into the downstream bioreactor without any separation or salt-mixing processes. In the optimized coupled platform, Ralstonia eutropha bacteria can grow with acetate generated from the CO electrocatalytic reduction reactor, and produce bioplastic as the final value-added product. Integrating electrochemical CO electrolysers with a bioreactor can yield high-value long-chain carbon products, but the electrolytes for the two systems are mismatched. Now, a porous solid electrolyte reactor, which can produce acetate directly in bioelectrolyte, is demonstrated. Direct integration with a bioreactor produces bioplastic from CO via the acetate intermediate.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 11","pages":"1392-1403"},"PeriodicalIF":0.0,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195629","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","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: Aza-annulation reactions extend π-conjugated systems 出版商更正：氮杂环氧化反应扩展了π-共轭体系

Nature synthesis Pub Date : 2024-08-27 DOI: 10.1038/s44160-024-00652-z

Marcell M. Bogner, Gábor London

引用次数: 0

Suzuki–Miyaura coupling of arylthianthrenium tetrafluoroborate salts under acidic conditions 芳基噻吩四氟硼酸盐在酸性条件下的 Suzukii-Miyaura 偶联反应

Nature synthesis Pub Date : 2024-08-26 DOI: 10.1038/s44160-024-00631-4

Li Zhang, Yuanhao Xie, Zibo Bai, Tobias Ritter

{"title":"Suzuki–Miyaura coupling of arylthianthrenium tetrafluoroborate salts under acidic conditions","authors":"Li Zhang, Yuanhao Xie, Zibo Bai, Tobias Ritter","doi":"10.1038/s44160-024-00631-4","DOIUrl":"10.1038/s44160-024-00631-4","url":null,"abstract":"The palladium-catalysed Suzuki–Miyaura cross-coupling (SMC) is currently the most commonly used reaction to construct carbon–carbon bonds in the pharmaceutical industry. Typical methods require the use of a base, which limits the substrate scope. To mitigate this shortcoming, substantial effort has been made to develop base-tolerant organoboron reagents, efficient catalysts and reaction conditions that do not require external bases. Still, many boronic acids cannot be used or must be independently protected, and many Lewis-basic functional groups poison the catalyst. Here we report a conceptually different SMC reaction that can proceed even under acidic conditions, with a broad substrate scope. Key to this advance is the formation of an acid-stable, palladium-based ion pair between the reaction partners that does not require base for subsequent productive transmetallation. Boronic acids that cannot be used directly in other SMC reactions, such as 2-pyridylboronic acid and boronic acids with strong Lewis bases, can now be used successfully. Suzuki–Miyaura cross-coupling between (hetero)aryl (pseudo)halides and base-sensitive and Lewis-basic (hetero)arylboronic acids is challenging, owing to potential side reactions and catalyst poisoning. Now, the Suzuki–Miyaura cross-coupling of arylthianthrenium salts with (hetero)arylboronic acids, under acidic conditions, is reported, enabling the efficient coupling of base-sensitive and Lewis-basic (hetero)arylboronic acids.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1490-1497"},"PeriodicalIF":0.0,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44160-024-00631-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195633","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0