IF 8.5

JACS Au Pub Date : 2024-10-03 DOI: 10.1021/jacsau.4c0086310.1021/jacsau.4c00863

Soraya Learte-Aymamí, Laura Martínez-Castro, Carmen González-González, Miriam Condeminas, Pau Martin-Malpartida, María Tomás-Gamasa, Sandra Baúlde, José R. Couceiro, Jean-Didier Maréchal*, Maria J. Macias*, José L. Mascareñas* and M. Eugenio Vázquez*,

引用次数: 0

Eutectogels: The Multifaceted Soft Ionic Materials of Tomorrow 共晶凝胶：未来的多元软离子材料

IF 8.5

JACS Au Pub Date : 2024-10-03 DOI: 10.1021/jacsau.4c0067710.1021/jacsau.4c00677

Pablo A. Mercadal, Agustín González, Ana Beloqui, Liliana C. Tomé, David Mecerreyes, Marcelo Calderón and Matias L. Picchio*,

{"title":"Eutectogels: The Multifaceted Soft Ionic Materials of Tomorrow","authors":"Pablo A. Mercadal, Agustín González, Ana Beloqui, Liliana C. Tomé, David Mecerreyes, Marcelo Calderón and Matias L. Picchio*, ","doi":"10.1021/jacsau.4c0067710.1021/jacsau.4c00677","DOIUrl":"https://doi.org/10.1021/jacsau.4c00677https://doi.org/10.1021/jacsau.4c00677","url":null,"abstract":"Eutectogels, a rising category of soft materials, have recently garnered significant attention owing to their remarkable potential in various domains. This innovative class of materials consists of a eutectic solvent immobilized in a three-dimensional network structure. The use of eco-friendly and cost-effective eutectic solvents further emphasizes the appeal of these materials in multiple applications. Eutectogels exhibit key characteristics of most eutectic solvents, including environmental friendliness, facile preparation, low vapor pressure, and good ionic conductivity. Moreover, they can be tailored to display functionalities such as self-healing capability, adhesiveness, and antibacterial properties, which are facilitated by incorporating specific combinations of the eutectic mixture constituents. This perspective article delves into the current landscape and challenges associated with eutectogels, particularly focusing on their potential applications in CO2 separation, drug delivery systems, battery technologies, biocatalysis, and food packaging. By exploring these diverse realms, we aim to shed light on the transformative capabilities of eutectogels and the opportunities they present to address pressing industrial, academic, and environmental challenges.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":null,"pages":null},"PeriodicalIF":8.5,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00677","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551592","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

A Self-Immobilizing Photosensitizer with Long-Term Retention for Hypoxia Imaging and Enhanced Photodynamic Therapy 用于缺氧成像和增强型光动力疗法的可长期保留的自固定光敏剂

IF 8.5

JACS Au Pub Date : 2024-10-03 DOI: 10.1021/jacsau.4c0078710.1021/jacsau.4c00787

Zifan Zhu, Yun Feng, Qiufen Tian, Jiawen Li, Chencong Liu, Yuchi Cheng, Sanjun Zhang, Yijing Dang, Jing Gao, Yi Lai, Fan Zhang, Haijun Yu, Wen Zhang and Zhiai Xu*,

{"title":"A Self-Immobilizing Photosensitizer with Long-Term Retention for Hypoxia Imaging and Enhanced Photodynamic Therapy","authors":"Zifan Zhu, Yun Feng, Qiufen Tian, Jiawen Li, Chencong Liu, Yuchi Cheng, Sanjun Zhang, Yijing Dang, Jing Gao, Yi Lai, Fan Zhang, Haijun Yu, Wen Zhang and Zhiai Xu*, ","doi":"10.1021/jacsau.4c0078710.1021/jacsau.4c00787","DOIUrl":"https://doi.org/10.1021/jacsau.4c00787https://doi.org/10.1021/jacsau.4c00787","url":null,"abstract":"The precise theranostic strategy of fluorescence imaging-guided photodynamic therapy (PDT) can effectively mitigate the adverse effect of photosensitizers in normal cells and tissues. However, low tumor enrichment and high diffusivity of photosensitizers significantly compromise the imaging accuracy and PDT effect. In this study, we have developed a nitroreductase (NTR)-activated and self-immobilizing photosensitizer CyNT-F, which showed enhanced enrichment in tumor tissues and facilitated precise and sustained imaging as well as PDT for hypoxia tumors. mPEG-b-PDPA nanomicelles encapsulating photosensitizers underwent dissociation and released CyNT-F in tumor cells. CyNT-F and NTR enzymatically reacted in situ to generate highly reactive quinone methide, subsequently covalently binding to adjacent proteins for fluorescence and PDT activation. CyNT-F exhibited longer intracellular retention (7 days) and effectively inhibited the tumor growth of solid hypoxia tumor. We believe the activatable and self-immobilizing strategy of PDT presents a novel methodology for minimizing the adverse effect and enabling spatiotemporally accurate ablation of diseased cells and tissues.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":null,"pages":null},"PeriodicalIF":8.5,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00787","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551630","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

Correction to "De Novo Engineering of Pd-Metalloproteins and Their Use as Intracellular Catalysts". 对 "钯金属蛋白新工程及其作为细胞内催化剂的应用 "的更正。

IF 8.5

JACS Au Pub Date : 2024-10-03 eCollection Date: 2024-10-28 DOI: 10.1021/jacsau.4c00863

Soraya Learte-Aymamí, Laura Martínez-Castro, Carmen González-González, Miriam Condeminas, Pau Martin-Malpartida, María Tomás-Gamasa, Sandra Baúlde, José R Couceiro, Jean-Didier Maréchal, Maria J Macias, José L Mascareñas, M Eugenio Vázquez

引用次数: 0

Tertiary-Amine-Functional Poly(arylene ether)s for Acid-Gas Separations 用于酸气分离的叔胺官能团聚芳基醚

IF 8.5

JACS Au Pub Date : 2024-10-02 DOI: 10.1021/jacsau.4c0048910.1021/jacsau.4c00489

Pablo A. Dean, Yifan Wu, Sheng Guo, Timothy M. Swager* and Zachary P. Smith*,

{"title":"Tertiary-Amine-Functional Poly(arylene ether)s for Acid-Gas Separations","authors":"Pablo A. Dean, Yifan Wu, Sheng Guo, Timothy M. Swager* and Zachary P. Smith*, ","doi":"10.1021/jacsau.4c0048910.1021/jacsau.4c00489","DOIUrl":"https://doi.org/10.1021/jacsau.4c00489https://doi.org/10.1021/jacsau.4c00489","url":null,"abstract":"Competitive sorption enables the emergent phenomenon of enhanced CO2-based selectivities for gas separation membranes when using microporous polymers with primary amines. However, strong secondary forces in these polymers through hydrogen bonding results in low solvent solubility, precluding standard solution processing approaches to form these polymers into membrane films. Herein, we circumvent these manufacturing constraints while maintaining competitive-sorption enhancements by synthesizing eight representative microporous poly(arylene ether)s (PAEs) with tertiary amines. High-pressure H2S, CO2, and CH4 sorption isotherms were collected for these samples to demonstrate enhanced affinity for acid gases relative to the unfunctional control polymer. Although competitive sorption was observed for all samples, improvements were less pronounced than for primary-amine-functional analogs. For H2S-based separations, the benefits of competitive sorption offset decreases in selectivity due to plasticization. This detailed study helps to elucidate the role of tertiary amines for acid gas separations in solution-processable microporous PAEs.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":null,"pages":null},"PeriodicalIF":8.5,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00489","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551250","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

Tertiary-Amine-Functional Poly(arylene ether)s for Acid-Gas Separations. 用于酸气分离的叔胺官能团聚芳基醚。

IF 8.5

JACS Au Pub Date : 2024-10-02 eCollection Date: 2024-10-28 DOI: 10.1021/jacsau.4c00489

Pablo A Dean, Yifan Wu, Sheng Guo, Timothy M Swager, Zachary P Smith

{"title":"Tertiary-Amine-Functional Poly(arylene ether)s for Acid-Gas Separations.","authors":"Pablo A Dean, Yifan Wu, Sheng Guo, Timothy M Swager, Zachary P Smith","doi":"10.1021/jacsau.4c00489","DOIUrl":"10.1021/jacsau.4c00489","url":null,"abstract":"Competitive sorption enables the emergent phenomenon of enhanced CO2-based selectivities for gas separation membranes when using microporous polymers with primary amines. However, strong secondary forces in these polymers through hydrogen bonding results in low solvent solubility, precluding standard solution processing approaches to form these polymers into membrane films. Herein, we circumvent these manufacturing constraints while maintaining competitive-sorption enhancements by synthesizing eight representative microporous poly(arylene ether)s (PAEs) with tertiary amines. High-pressure H2S, CO2, and CH4 sorption isotherms were collected for these samples to demonstrate enhanced affinity for acid gases relative to the unfunctional control polymer. Although competitive sorption was observed for all samples, improvements were less pronounced than for primary-amine-functional analogs. For H2S-based separations, the benefits of competitive sorption offset decreases in selectivity due to plasticization. This detailed study helps to elucidate the role of tertiary amines for acid gas separations in solution-processable microporous PAEs.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":null,"pages":null},"PeriodicalIF":8.5,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11522933/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142560351","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

Translation of Deoxyribonucleic Acid into Synthetic Alpha Helical Peptides for Darwinian Evolution 将脱氧核糖核酸转化为合成阿尔法螺旋肽，实现达尔文进化论

IF 8.5

JACS Au Pub Date : 2024-10-02 DOI: 10.1021/jacsau.4c0073810.1021/jacsau.4c00738

Millicent Dockerill, Pramod M. Sabale, Francesco Russo, Sofia Barluenga and Nicolas Winssinger*,

引用次数: 0

Translation of Deoxyribonucleic Acid into Synthetic Alpha Helical Peptides for Darwinian Evolution. 将脱氧核糖核酸转化为合成阿尔法螺旋肽，实现达尔文进化论。

IF 8.5

JACS Au Pub Date : 2024-10-02 eCollection Date: 2024-10-28 DOI: 10.1021/jacsau.4c00738

Millicent Dockerill, Pramod M Sabale, Francesco Russo, Sofia Barluenga, Nicolas Winssinger

引用次数: 0

Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH₃. 由双核-铜基团构建的二维 MOF，用于高性能电催化 NO 还原成 NH3。

IF 8.5

JACS Au Pub Date : 2024-10-01 eCollection Date: 2024-10-28 DOI: 10.1021/jacsau.4c00475

Rong Luo, Bao-Jing Li, Zhan-Peng Wang, Ming-Guang Chen, Gui-Lin Zhuang, Quan Li, Jia-Ping Tong, Wen-Tai Wang, Yu-Hua Fan, Feng Shao

{"title":"Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH3.","authors":"Rong Luo, Bao-Jing Li, Zhan-Peng Wang, Ming-Guang Chen, Gui-Lin Zhuang, Quan Li, Jia-Ping Tong, Wen-Tai Wang, Yu-Hua Fan, Feng Shao","doi":"10.1021/jacsau.4c00475","DOIUrl":"10.1021/jacsau.4c00475","url":null,"abstract":"Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH3 synthesis. However, their complex kinetics and energy demands necessitate high-performance electrocatalysts to ensure effective and selective process outcomes. Herein, we report that a two-dimensional Cu-based metal-organic framework (MOF), {[Cu(HL)]·H2O} n , (Cu-OUC, H3L = 5-(2'-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH3 conversion. Electrochemical experimental studies showed that in 0.1 M K2SO4 solution, the as-prepared Cu-OUC achieved a peak Faradaic efficiency of 96.91% and a notable NH3 yield as high as 3415.82 μg h-1 mg-1. The Zn-NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm-2 while simultaneously achieving an NH3 yield of 616.92 μg h-1 mg-1. Theoretical calculations revealed that the surface of Cu-OUC effectively facilitates NO activation through a two-way charge transfer mechanism of \"electron acceptance and donation\", with the *NO formation step being the potential-determining stage. The study pioneers the use of a MOF as an electrocatalyst for ambient NO-to-NH3 conversion.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":null,"pages":null},"PeriodicalIF":8.5,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11522898/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142559879","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

Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH3 由双核-铜基团构建的二维 MOF 用于高性能电催化 NO 还原成 NH3

IF 8.5

JACS Au Pub Date : 2024-10-01 DOI: 10.1021/jacsau.4c0047510.1021/jacsau.4c00475

Rong Luo, Bao-Jing Li, Zhan-Peng Wang, Ming-Guang Chen, Gui-Lin Zhuang*, Quan Li, Jia-Ping Tong, Wen-Tai Wang*, Yu-Hua Fan and Feng Shao*,

{"title":"Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH3","authors":"Rong Luo, Bao-Jing Li, Zhan-Peng Wang, Ming-Guang Chen, Gui-Lin Zhuang*, Quan Li, Jia-Ping Tong, Wen-Tai Wang*, Yu-Hua Fan and Feng Shao*, ","doi":"10.1021/jacsau.4c0047510.1021/jacsau.4c00475","DOIUrl":"https://doi.org/10.1021/jacsau.4c00475https://doi.org/10.1021/jacsau.4c00475","url":null,"abstract":"Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH3 synthesis. However, their complex kinetics and energy demands necessitate high-performance electrocatalysts to ensure effective and selective process outcomes. Herein, we report that a two-dimensional Cu-based metal–organic framework (MOF), {[Cu(HL)]·H2O}n, (Cu-OUC, H3L = 5-(2′-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH3 conversion. Electrochemical experimental studies showed that in 0.1 M K2SO4 solution, the as-prepared Cu-OUC achieved a peak Faradaic efficiency of 96.91% and a notable NH3 yield as high as 3415.82 μg h–1 mg–1. The Zn–NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm–2 while simultaneously achieving an NH3 yield of 616.92 μg h–1 mg–1. Theoretical calculations revealed that the surface of Cu-OUC effectively facilitates NO activation through a two-way charge transfer mechanism of “electron acceptance and donation”, with the *NO formation step being the potential-determining stage. The study pioneers the use of a MOF as an electrocatalyst for ambient NO-to-NH3 conversion.","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":null,"pages":null},"PeriodicalIF":8.5,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00475","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142517036","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

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