JACS Au最新文献_第10页

Palladium-Catalyzed Functionalization of Shortwave Infrared Heptamethine Fluorophores Expands Their In Vivo Utility 钯催化短波红外七甲基胺荧光团的功能化扩展了它们在体内的应用

IF 8.5

JACS Au Pub Date : 2025-04-04 DOI: 10.1021/jacsau.4c0127910.1021/jacsau.4c01279

Cesar A. Garcia, Emily B. Mobley, Eric Y. Lin, Kyle Bui and Ellen M. Sletten*,

{"title":"Palladium-Catalyzed Functionalization of Shortwave Infrared Heptamethine Fluorophores Expands Their In Vivo Utility","authors":"Cesar A. Garcia, Emily B. Mobley, Eric Y. Lin, Kyle Bui and Ellen M. Sletten*, ","doi":"10.1021/jacsau.4c0127910.1021/jacsau.4c01279","DOIUrl":"https://doi.org/10.1021/jacsau.4c01279https://doi.org/10.1021/jacsau.4c01279","url":null,"abstract":"Fluorescence imaging in the near-infrared (NIR, 700–1000 nm) and shortwave infrared (SWIR, 1000–2000 nm) regions is advantageous for studying mammals. This work applies palladium-catalyzed coupling methods to functionalize flavylium and chromenylium SWIR polymethine fluorophores, which are challenging substrates due to their small HOMO–LUMO gaps. These chemistries include Suzuki-Miyaura and Sonogashira couplings as well as an unprecedented coupling of alcohol substrates to ultimately achieve a panel of C–CAr, C–Csp, and C–O-alkyl functionalized SWIR fluorescent heptamethine dyes. The photophysical properties of the resulting fluorophores are analyzed against Hammett parameters to produce predictive metrics for absorption maxima. These metrics are strategically applied in the design of laser-matched, SWIR-emissive, chromenylium heptamethine dyes. Added functionalities advance the utility of SWIR fluorophores by increasing brightness in micelle formulations, modulating lipophilicity for alternative delivery vehicles, and enabling bioconjugation to targeting moieties. Ultimately, three functionalized fluorophores are employed in concert to achieve multicolor excitation-multiplexed imaging in murine cancer models.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 5","pages":"2089–2101 2089–2101"},"PeriodicalIF":8.5,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c01279","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133874","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

Effect of Pyridinecarboxaldehyde Functionalization on Reactivity and N-Terminal Protein Modification 吡啶甲酸功能化对反应性和n端蛋白修饰的影响

IF 8.5

JACS Au Pub Date : 2025-04-04 DOI: 10.1021/jacsau.5c0023810.1021/jacsau.5c00238

Lydia J. Barber, Ksenia S. Stankevich and Christopher D. Spicer*,

引用次数: 0

Electrode–Electrolyte Engineering and In Situ Spectroscopy for Urea Electrosynthesis from Carbon Dioxide and Nitrate Co-Reduction 二氧化碳和硝酸盐共还原电合成尿素的电极-电解质工程和原位光谱研究

IF 8.5

JACS Au Pub Date : 2025-04-03 DOI: 10.1021/jacsau.5c0006510.1021/jacsau.5c00065

Gabriel F. Costa, and , María Escudero-Escribano*,

{"title":"Electrode–Electrolyte Engineering and In Situ Spectroscopy for Urea Electrosynthesis from Carbon Dioxide and Nitrate Co-Reduction","authors":"Gabriel F. Costa,  and , María Escudero-Escribano*, ","doi":"10.1021/jacsau.5c0006510.1021/jacsau.5c00065","DOIUrl":"https://doi.org/10.1021/jacsau.5c00065https://doi.org/10.1021/jacsau.5c00065","url":null,"abstract":"The biogeochemical cycles of carbon and nitrogen are globally disturbed due to the intensive use of fossil fuels and fertilizers, which is reflected by the accumulation of carbon dioxide in the atmosphere and nitrate in water streams. The co-electroreduction of carbon dioxide and nitrate is a promising low-carbon alternative for urea synthesis that would help to reestablish both carbon and nitrogen cycles. This Perspective highlights the importance of rational catalyst and electrolyte engineering to enable electrochemical urea synthesis. Although the field has gained significant attention over the past few years, fundamental research under well-defined conditions remains underexplored. We highlight the importance of investigating structure-sensitivity and electrolyte effects on electrochemical C–N coupling through complementary in situ spectroscopy and online techniques. Model studies, including in situ surface-sensitive investigations, will be crucial to understand the molecular mechanisms and thus to rationally design more efficient systems for urea electrosynthesis, paving the way for their scalable and industrial applications.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 4","pages":"1538–1548 1538–1548"},"PeriodicalIF":8.5,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.5c00065","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878233","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

Electrode-Electrolyte Engineering and In Situ Spectroscopy for Urea Electrosynthesis from Carbon Dioxide and Nitrate Co-Reduction. 二氧化碳和硝酸盐共还原电合成尿素的电极-电解质工程和原位光谱研究。

IF 8.5

JACS Au Pub Date : 2025-04-03 eCollection Date: 2025-04-28 DOI: 10.1021/jacsau.5c00065

Gabriel F Costa, María Escudero-Escribano

{"title":"Electrode-Electrolyte Engineering and In Situ Spectroscopy for Urea Electrosynthesis from Carbon Dioxide and Nitrate Co-Reduction.","authors":"Gabriel F Costa, María Escudero-Escribano","doi":"10.1021/jacsau.5c00065","DOIUrl":"https://doi.org/10.1021/jacsau.5c00065","url":null,"abstract":"The biogeochemical cycles of carbon and nitrogen are globally disturbed due to the intensive use of fossil fuels and fertilizers, which is reflected by the accumulation of carbon dioxide in the atmosphere and nitrate in water streams. The co-electroreduction of carbon dioxide and nitrate is a promising low-carbon alternative for urea synthesis that would help to reestablish both carbon and nitrogen cycles. This Perspective highlights the importance of rational catalyst and electrolyte engineering to enable electrochemical urea synthesis. Although the field has gained significant attention over the past few years, fundamental research under well-defined conditions remains underexplored. We highlight the importance of investigating structure-sensitivity and electrolyte effects on electrochemical C-N coupling through complementary in situ spectroscopy and online techniques. Model studies, including in situ surface-sensitive investigations, will be crucial to understand the molecular mechanisms and thus to rationally design more efficient systems for urea electrosynthesis, paving the way for their scalable and industrial applications.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 4","pages":"1538-1548"},"PeriodicalIF":8.5,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12042039/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144060190","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

Organocatalyzed Enantioselective C–N Bond-Forming SNAr Reactions for Synthesizing Stereogenic-at-Boron BODIPYs 有机催化对映选择性C-N成键SNAr反应合成立体硼体

IF 8.5

JACS Au Pub Date : 2025-04-02 DOI: 10.1021/jacsau.5c0019610.1021/jacsau.5c00196

Yan-Dong Meng, Wei Fang, Zheng-Hao Pei, Wen-Hao Chen, Shu-Ying Ding, Meng-Lan Shen, Yingcui Bu*, Chuan-Zhi Yao, Qiankun Li, Jie Yu* and Hua-Jie Jiang*,

{"title":"Organocatalyzed Enantioselective C–N Bond-Forming SNAr Reactions for Synthesizing Stereogenic-at-Boron BODIPYs","authors":"Yan-Dong Meng, Wei Fang, Zheng-Hao Pei, Wen-Hao Chen, Shu-Ying Ding, Meng-Lan Shen, Yingcui Bu*, Chuan-Zhi Yao, Qiankun Li, Jie Yu* and Hua-Jie Jiang*, ","doi":"10.1021/jacsau.5c0019610.1021/jacsau.5c00196","DOIUrl":"https://doi.org/10.1021/jacsau.5c00196https://doi.org/10.1021/jacsau.5c00196","url":null,"abstract":"The precise construction of boron stereogenic centers represents a significant, yet challenging frontier in asymmetric catalysis, garnering growing attention in recent years. However, feasible catalysis has primarily been limited to transition-metal-catalyzed desymmetrization of pro-chiral BODIPY molecules, while enantioselective synthesis via organocatalysis remains unexplored. Herein, we achieve an organocatalyzed C–N bond-forming SNAr reaction of 3,5-dihalogen BODIPYs via phase-transfer catalysis, enabling the efficient synthesis of a broad range of boron-stereogenic BODIPYs with excellent enantioselectivities (>40 examples, up to 99% ee). The significance and potential of this catalytic approach are further underscored by the versatile applications of enantioenriched 3-amide BODIPYs in asymmetric synthesis, optical activity regulation, bioimaging, and sensing, promoting the development of boron-stereogenic fluorophores.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 4","pages":"1965–1973 1965–1973"},"PeriodicalIF":8.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.5c00196","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878196","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

Organocatalyzed Enantioselective C-N Bond-Forming S_NAr Reactions for Synthesizing Stereogenic-at-Boron BODIPYs. 有机催化对映选择性C-N成键SNAr反应合成立体硼体。

IF 8.5

JACS Au Pub Date : 2025-04-02 eCollection Date: 2025-04-28 DOI: 10.1021/jacsau.5c00196

Yan-Dong Meng, Wei Fang, Zheng-Hao Pei, Wen-Hao Chen, Shu-Ying Ding, Meng-Lan Shen, Yingcui Bu, Chuan-Zhi Yao, Qiankun Li, Jie Yu, Hua-Jie Jiang

引用次数: 0

Deciphering the Diffusion-Improved Selectivity of Ethylene Mediated by the Mesoscale Spatial Pattern of Aromatics in Zeolite-Catalyzed Methanol-to-Olefin Processes 沸石催化甲醇制烯烃过程中芳烃中尺度空间格局对乙烯扩散选择性的影响

IF 8.5

JACS Au Pub Date : 2025-04-01 DOI: 10.1021/jacsau.5c0004510.1021/jacsau.5c00045

Qingteng Chen, Jian Liu and Bo Yang*,

{"title":"Deciphering the Diffusion-Improved Selectivity of Ethylene Mediated by the Mesoscale Spatial Pattern of Aromatics in Zeolite-Catalyzed Methanol-to-Olefin Processes","authors":"Qingteng Chen, Jian Liu and Bo Yang*, ","doi":"10.1021/jacsau.5c0004510.1021/jacsau.5c00045","DOIUrl":"https://doi.org/10.1021/jacsau.5c00045https://doi.org/10.1021/jacsau.5c00045","url":null,"abstract":"Modeling the diffusion behavior of nonuniformly distributed systems at the mesoscopic scale presents significant challenges. In this study, we investigate how the nonuniform mesoscale spatial distribution of aromatic compounds, i.e., the hydrocarbon pool, affects olefin selectivity during the methanol-to-olefins (MTO) process. Ab initio molecular dynamics with enhanced sampling methods and kinetic Monte Carlo techniques were employed to analyze olefin diffusion in a “fully filled from the outside to the inside” distribution model. Our results reveal that while the coexistence of olefins with aromatic compounds hinders olefin diffusion, it simultaneously enhances ethylene selectivity. Further analysis of diffusion rate control and olefin residence time distributions within the zeolite model identifies key elementary diffusion processes and elucidates why aromatic compounds preferentially form at the rim of the SAPO-34 zeolite during the MTO process. This integrated approach enables the simulation of catalytic systems over larger spatial and temporal scales, providing a comprehensive understanding of the underlying mechanisms and facilitating the design of more efficient and ethylene-selective catalysts.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 4","pages":"1791–1802 1791–1802"},"PeriodicalIF":8.5,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.5c00045","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878176","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

Nanopore Environmental Analysis. 纳米孔环境分析。

IF 8.5

JACS Au Pub Date : 2025-04-01 eCollection Date: 2025-04-28 DOI: 10.1021/jacsau.5c00114

Xiaofeng Lu, Xiaoyu Du, Dong Zhong, Renjie Li, Junjie Cao, Shuo Huang, Yuqin Wang

{"title":"Nanopore Environmental Analysis.","authors":"Xiaofeng Lu, Xiaoyu Du, Dong Zhong, Renjie Li, Junjie Cao, Shuo Huang, Yuqin Wang","doi":"10.1021/jacsau.5c00114","DOIUrl":"https://doi.org/10.1021/jacsau.5c00114","url":null,"abstract":"As global pollution continues to escalate, timely and accurate monitoring is essential for guiding pollution governance and safeguarding public health. The increasing diversity of pollutants across environmental matrices poses a significant challenge for instrumental analysis methods, which often require labor-intensive and time-consuming sample pretreatment. Nanopore technology, an emerging single-molecule technique, presents a promising solution by enabling the rapid identification of multiple targets within complex mixtures with minimal sample preparation. A wide range of pollutants have been characterized using natural biological nanopores or artificial solid-state nanopores, and their distinct advantages include simple sample preparation, high sensitivity, and rapid onsite analysis. In particular, long-read nanopore sequencing has led to dramatic improvements in the analyses of environmental microbial communities, allows species-level taxonomic assignment using amplicon sequencing, and simplifies the assembly of metagenomes. In this Perspective, we review the latest advancements in analyzing chemical and biological pollutants through nanopore sensing and sequencing techniques. We also explore the challenges that remain in this rapidly evolving field and provide an outlook on the potential for nanopore environmental analysis to transform pollution monitoring, risk assessment, and public health protection.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 4","pages":"1570-1590"},"PeriodicalIF":8.5,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12042043/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144055670","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

Nanopore Environmental Analysis 纳米孔环境分析

IF 8.5

JACS Au Pub Date : 2025-04-01 DOI: 10.1021/jacsau.5c0011410.1021/jacsau.5c00114

Xiaofeng Lu, Xiaoyu Du, Dong Zhong, Renjie Li, Junjie Cao, Shuo Huang* and Yuqin Wang*,

{"title":"Nanopore Environmental Analysis","authors":"Xiaofeng Lu, Xiaoyu Du, Dong Zhong, Renjie Li, Junjie Cao, Shuo Huang* and Yuqin Wang*, ","doi":"10.1021/jacsau.5c0011410.1021/jacsau.5c00114","DOIUrl":"https://doi.org/10.1021/jacsau.5c00114https://doi.org/10.1021/jacsau.5c00114","url":null,"abstract":"As global pollution continues to escalate, timely and accurate monitoring is essential for guiding pollution governance and safeguarding public health. The increasing diversity of pollutants across environmental matrices poses a significant challenge for instrumental analysis methods, which often require labor-intensive and time-consuming sample pretreatment. Nanopore technology, an emerging single-molecule technique, presents a promising solution by enabling the rapid identification of multiple targets within complex mixtures with minimal sample preparation. A wide range of pollutants have been characterized using natural biological nanopores or artificial solid-state nanopores, and their distinct advantages include simple sample preparation, high sensitivity, and rapid onsite analysis. In particular, long-read nanopore sequencing has led to dramatic improvements in the analyses of environmental microbial communities, allows species-level taxonomic assignment using amplicon sequencing, and simplifies the assembly of metagenomes. In this Perspective, we review the latest advancements in analyzing chemical and biological pollutants through nanopore sensing and sequencing techniques. We also explore the challenges that remain in this rapidly evolving field and provide an outlook on the potential for nanopore environmental analysis to transform pollution monitoring, risk assessment, and public health protection.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 4","pages":"1570–1590 1570–1590"},"PeriodicalIF":8.5,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.5c00114","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878185","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

Deciphering the Diffusion-Improved Selectivity of Ethylene Mediated by the Mesoscale Spatial Pattern of Aromatics in Zeolite-Catalyzed Methanol-to-Olefin Processes. 沸石催化甲醇制烯烃过程中芳烃中尺度空间格局对乙烯扩散选择性的影响

IF 8.5

JACS Au Pub Date : 2025-04-01 eCollection Date: 2025-04-28 DOI: 10.1021/jacsau.5c00045

Qingteng Chen, Jian Liu, Bo Yang

{"title":"Deciphering the Diffusion-Improved Selectivity of Ethylene Mediated by the Mesoscale Spatial Pattern of Aromatics in Zeolite-Catalyzed Methanol-to-Olefin Processes.","authors":"Qingteng Chen, Jian Liu, Bo Yang","doi":"10.1021/jacsau.5c00045","DOIUrl":"https://doi.org/10.1021/jacsau.5c00045","url":null,"abstract":"Modeling the diffusion behavior of nonuniformly distributed systems at the mesoscopic scale presents significant challenges. In this study, we investigate how the nonuniform mesoscale spatial distribution of aromatic compounds, i.e., the hydrocarbon pool, affects olefin selectivity during the methanol-to-olefins (MTO) process. Ab initio molecular dynamics with enhanced sampling methods and kinetic Monte Carlo techniques were employed to analyze olefin diffusion in a \"fully filled from the outside to the inside\" distribution model. Our results reveal that while the coexistence of olefins with aromatic compounds hinders olefin diffusion, it simultaneously enhances ethylene selectivity. Further analysis of diffusion rate control and olefin residence time distributions within the zeolite model identifies key elementary diffusion processes and elucidates why aromatic compounds preferentially form at the rim of the SAPO-34 zeolite during the MTO process. This integrated approach enables the simulation of catalytic systems over larger spatial and temporal scales, providing a comprehensive understanding of the underlying mechanisms and facilitating the design of more efficient and ethylene-selective catalysts.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"5 4","pages":"1791-1802"},"PeriodicalIF":8.5,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12041954/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144056129","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