Nature synthesisPub Date : 2024-09-02DOI: 10.1038/s44160-024-00642-1
William B. Martin, Robert E. Warburton, Shane M. Parker, Valentin O. Rodionov
{"title":"On the characterization of γ-graphyne","authors":"William B. Martin, Robert E. Warburton, Shane M. Parker, Valentin O. Rodionov","doi":"10.1038/s44160-024-00642-1","DOIUrl":"10.1038/s44160-024-00642-1","url":null,"abstract":"","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 10","pages":"1208-1211"},"PeriodicalIF":0.0,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195625","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}
Nature synthesisPub Date : 2024-08-30DOI: 10.1038/s44160-024-00651-0
Alexandra R. Groves
{"title":"Methane to methanol","authors":"Alexandra R. Groves","doi":"10.1038/s44160-024-00651-0","DOIUrl":"10.1038/s44160-024-00651-0","url":null,"abstract":"","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 9","pages":"1065-1065"},"PeriodicalIF":0.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142170384","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}
Nature synthesisPub Date : 2024-08-30DOI: 10.1038/s44160-024-00641-2
{"title":"Integrating multiple interactions for the assembly of ordered organic frameworks","authors":"","doi":"10.1038/s44160-024-00641-2","DOIUrl":"10.1038/s44160-024-00641-2","url":null,"abstract":"A strategy is demonstrated for the hierarchical assembly of highly crystalline supramolecular nanotubes and tubular covalent organic frameworks (COFs), driven by cooperative dynamic covalent and coordination bonding. The pore size of the tubular COFs can be precisely controlled, and their reversible demetallation and remetallation could enable further tuning of the properties.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1453-1454"},"PeriodicalIF":0.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195627","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}
Nature synthesisPub Date : 2024-08-28DOI: 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}
Nature synthesisPub Date : 2024-08-26DOI: 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}
Nature synthesisPub Date : 2024-08-26DOI: 10.1038/s44160-024-00632-3
Hai-Sen Xu, Yi Luo, Runlai Li, Wen-Na Jiao, Si Huang, Wei-De Zhu, Hongfei Wang, Ting Chen, Mathias Nero, Fangzheng Chen, Qiang Gao, Xing Li, Mei Pan, Tom Willhammar, Kian Ping Loh, Cheng-Yong Su
{"title":"Hierarchical assembly of tubular frameworks driven by covalent and coordinate bonding","authors":"Hai-Sen Xu, Yi Luo, Runlai Li, Wen-Na Jiao, Si Huang, Wei-De Zhu, Hongfei Wang, Ting Chen, Mathias Nero, Fangzheng Chen, Qiang Gao, Xing Li, Mei Pan, Tom Willhammar, Kian Ping Loh, Cheng-Yong Su","doi":"10.1038/s44160-024-00632-3","DOIUrl":"10.1038/s44160-024-00632-3","url":null,"abstract":"Hierarchical assembly is used to construct complex materials using elementary building units, mainly depending on the non-covalent interactions involving dynamic bonds. Here we present a hierarchical assembly strategy to build highly crystalline tubular frameworks. A multi-level assembly process driven by dynamic covalent bonds and coordination bonds is shown to produce a supramolecular nanotubular framework and three tubular covalent organic frameworks (COFs). These materials consist of well-ordered triangular nanotubes assembled in an oriented manner. In tubular COFs, the spacing between adjacent nanotubes can be systematically adjusted by altering the connector lengths to create mesoporous structures with adjustable pore size. Moreover, reversible transformations between tubular COFs and layered COFs were achieved by the reversible addition and removal of Zn(NO3)2. The facile demetallation–remetallation process confers tuneable structural properties to the materials and enables the layered COFs to serve as efficient ‘sponges’ for metal ions. This study represents a notable advance in hierarchical assembly; incorporating covalent bonding into this process is expected to greatly accelerate the development of new materials. Driven by dynamic covalent and coordinate bonding, hierarchical components are formed in situ and assembled in an ordered manner, yielding highly crystalline supramolecular nanotubular frameworks and tubular covalent organic frameworks.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1498-1506"},"PeriodicalIF":0.0,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195632","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}
Nature synthesisPub Date : 2024-08-26DOI: 10.1038/s44160-024-00629-y
Louis-Charles Campeau
{"title":"Thianthrenium ions pair-up for Suzuki–Miyaura reactions","authors":"Louis-Charles Campeau","doi":"10.1038/s44160-024-00629-y","DOIUrl":"10.1038/s44160-024-00629-y","url":null,"abstract":"Aryl thianthrenium salts participate in Suzuki–Miyaura cross-coupling reactions with boronic acids. Notably, the reactions occur at low pH, facilitating the use of base-sensitive boronic acids or Lewis basic substrates.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1448-1450"},"PeriodicalIF":0.0,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195630","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}