首页 > 最新文献

JACS Au最新文献

英文 中文
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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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*, 
{"title":"Correction to “De Novo Engineering of Pd-Metalloproteins and Their Use as Intracellular Catalysts”","authors":"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*, ","doi":"10.1021/jacsau.4c0086310.1021/jacsau.4c00863","DOIUrl":"https://doi.org/10.1021/jacsau.4c00863https://doi.org/10.1021/jacsau.4c00863","url":null,"abstract":"","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.4c00863","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551631","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
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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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*, 

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.

共晶凝胶(Eutectogels)是一种新兴的软性材料,由于其在各个领域的巨大潜力,最近受到了广泛关注。这一类创新材料由固定在三维网络结构中的共晶溶剂组成。使用环保且成本效益高的共晶溶剂进一步凸显了这类材料在多种应用领域的吸引力。共晶凝胶具有大多数共晶溶剂的主要特点,包括环保、易于制备、低蒸汽压和良好的离子导电性。此外,共晶凝胶还可通过加入特定组合的共晶混合物成分,实现自愈合能力、粘附性和抗菌性等功能。本视角文章深入探讨了共晶凝胶的现状和相关挑战,尤其关注其在二氧化碳分离、药物输送系统、电池技术、生物催化和食品包装等领域的潜在应用。通过对这些不同领域的探索,我们旨在阐明共晶凝胶的变革能力,以及它们为解决紧迫的工业、学术和环境挑战所带来的机遇。
{"title":"Eutectogels: The Multifaceted Soft Ionic Materials of Tomorrow","authors":"Pablo A. Mercadal,&nbsp;Agustín González,&nbsp;Ana Beloqui,&nbsp;Liliana C. Tomé,&nbsp;David Mecerreyes,&nbsp;Marcelo Calderón and Matias L. Picchio*,&nbsp;","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":"<p >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 CO<sub>2</sub> 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.</p>","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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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*, 

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.

荧光成像引导光动力疗法(PDT)的精确治疗策略能有效减轻光敏剂对正常细胞和组织的不良影响。然而,光敏剂的低肿瘤富集度和高扩散性大大影响了成像的准确性和光动力疗法的效果。本研究开发了一种由硝基还原酶(NTR)激活的自固定光敏剂 CyNT-F,它在肿瘤组织中的富集能力更强,有利于缺氧肿瘤的精确、持续成像和局部放疗。CyNT-F 和 NTR 在原位发生酶促反应,生成高活性的甲酮醌,随后与邻近的蛋白质共价结合,产生荧光并激活 PDT。CyNT-F 在细胞内的保留时间较长(7 天),能有效抑制实体缺氧肿瘤的生长。我们相信,这种可激活和自固定的光导疗法是一种新型方法,可将不良反应降至最低,并实现对病变细胞和组织的时空精确消融。
{"title":"A Self-Immobilizing Photosensitizer with Long-Term Retention for Hypoxia Imaging and Enhanced Photodynamic Therapy","authors":"Zifan Zhu,&nbsp;Yun Feng,&nbsp;Qiufen Tian,&nbsp;Jiawen Li,&nbsp;Chencong Liu,&nbsp;Yuchi Cheng,&nbsp;Sanjun Zhang,&nbsp;Yijing Dang,&nbsp;Jing Gao,&nbsp;Yi Lai,&nbsp;Fan Zhang,&nbsp;Haijun Yu,&nbsp;Wen Zhang and Zhiai Xu*,&nbsp;","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":"<p >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-<i>b</i>-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.</p>","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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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

[This corrects the article DOI: 10.1021/jacsau.4c00379.].

[此处更正了文章 DOI:10.1021/jacsau.4c00379]。
{"title":"Correction to \"De Novo Engineering of Pd-Metalloproteins and Their Use as Intracellular Catalysts\".","authors":"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","doi":"10.1021/jacsau.4c00863","DOIUrl":"10.1021/jacsau.4c00863","url":null,"abstract":"<p><p>[This corrects the article DOI: 10.1021/jacsau.4c00379.].</p>","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://www.ncbi.nlm.nih.gov/pmc/articles/PMC11522897/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142559865","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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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*, 

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.

当使用带有伯胺的微孔聚合物时,竞争性吸附可使气体分离膜的二氧化碳选择性得到增强。然而,这些聚合物中通过氢键产生的强大次生力导致其溶剂溶解度较低,因此无法采用标准溶液加工方法将这些聚合物制成膜。在此,我们通过合成八种具有代表性的微孔聚芳基醚(PAE)与叔胺,在保持有竞争力的吸附增强效果的同时,规避了这些生产限制。收集了这些样品的高压 H2S、CO2 和 CH4 吸附等温线,以证明相对于无功能对照聚合物,它们对酸性气体的亲和力有所增强。虽然在所有样品中都观察到了竞争性吸附,但与伯胺功能类似物相比,其吸附性的改善并不明显。对于基于 H2S 的分离,竞争吸附的优势抵消了塑化导致的选择性下降。这项详细研究有助于阐明叔胺在可溶液加工的微孔聚醚中分离酸性气体的作用。
{"title":"Tertiary-Amine-Functional Poly(arylene ether)s for Acid-Gas Separations","authors":"Pablo A. Dean,&nbsp;Yifan Wu,&nbsp;Sheng Guo,&nbsp;Timothy M. Swager* and Zachary P. Smith*,&nbsp;","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":"<p >Competitive sorption enables the emergent phenomenon of enhanced CO<sub>2</sub>-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 H<sub>2</sub>S, CO<sub>2</sub>, and CH<sub>4</sub> 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 H<sub>2</sub>S-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.</p>","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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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

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.

当使用带有伯胺的微孔聚合物时,竞争性吸附可使气体分离膜的二氧化碳选择性得到增强。然而,这些聚合物中通过氢键产生的强大次生力导致其溶剂溶解度较低,因此无法采用标准溶液加工方法将这些聚合物制成膜。在此,我们通过合成八种具有代表性的微孔聚芳基醚(PAE)与叔胺,在保持有竞争力的吸附增强效果的同时,规避了这些生产限制。收集了这些样品的高压 H2S、CO2 和 CH4 吸附等温线,以证明相对于无功能对照聚合物,它们对酸性气体的亲和力有所增强。虽然在所有样品中都观察到了竞争性吸附,但与伯胺功能类似物相比,其吸附性的改善并不明显。对于基于 H2S 的分离,竞争吸附的优势抵消了塑化导致的选择性下降。这项详细研究有助于阐明叔胺在可溶液加工的微孔聚醚中分离酸性气体的作用。
{"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":"<p><p>Competitive sorption enables the emergent phenomenon of enhanced CO<sub>2</sub>-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 H<sub>2</sub>S, CO<sub>2</sub>, and CH<sub>4</sub> 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 H<sub>2</sub>S-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.</p>","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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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*, 

DNA-encoded libraries connect the phenotypes of synthetic molecules to a DNA barcode; however, most libraries do not tap into the potential of Darwinian evolution. Herein, we report a DNA-templated synthesis (DTS) architecture to make peptides that are stabilized into α-helical conformations via head-to-tail supramolecular cyclization. Using a pilot library targeting MDM2, we show that repeated screening can amplify a binder from the lowest abundance in the library to a ranking that correlates to binding affinity. The study also highlights the need to design libraries such that the chemistry avoids biases from the heterogeneous yield in DTS.

DNA编码文库将合成分子的表型与DNA条形码连接起来;然而,大多数文库并没有挖掘达尔文进化论的潜力。在本文中,我们报告了一种DNA模板合成(DTS)结构,通过头尾超分子环化将多肽稳定为α螺旋构象。通过使用针对 MDM2 的试验文库,我们发现反复筛选可以将一个结合剂从文库中最低的丰度放大到与结合亲和力相关的等级。这项研究还强调了设计文库的必要性,这样才能避免 DTS 中异质产率造成的化学偏差。
{"title":"Translation of Deoxyribonucleic Acid into Synthetic Alpha Helical Peptides for Darwinian Evolution","authors":"Millicent Dockerill,&nbsp;Pramod M. Sabale,&nbsp;Francesco Russo,&nbsp;Sofia Barluenga and Nicolas Winssinger*,&nbsp;","doi":"10.1021/jacsau.4c0073810.1021/jacsau.4c00738","DOIUrl":"https://doi.org/10.1021/jacsau.4c00738https://doi.org/10.1021/jacsau.4c00738","url":null,"abstract":"<p >DNA-encoded libraries connect the phenotypes of synthetic molecules to a DNA barcode; however, most libraries do not tap into the potential of Darwinian evolution. Herein, we report a DNA-templated synthesis (DTS) architecture to make peptides that are stabilized into α-helical conformations via head-to-tail supramolecular cyclization. Using a pilot library targeting MDM2, we show that repeated screening can amplify a binder from the lowest abundance in the library to a ranking that correlates to binding affinity. The study also highlights the need to design libraries such that the chemistry avoids biases from the heterogeneous yield in DTS.</p>","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.4c00738","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550392","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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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

DNA-encoded libraries connect the phenotypes of synthetic molecules to a DNA barcode; however, most libraries do not tap into the potential of Darwinian evolution. Herein, we report a DNA-templated synthesis (DTS) architecture to make peptides that are stabilized into α-helical conformations via head-to-tail supramolecular cyclization. Using a pilot library targeting MDM2, we show that repeated screening can amplify a binder from the lowest abundance in the library to a ranking that correlates to binding affinity. The study also highlights the need to design libraries such that the chemistry avoids biases from the heterogeneous yield in DTS.

DNA编码文库将合成分子的表型与DNA条形码连接起来;然而,大多数文库并没有挖掘达尔文进化论的潜力。在本文中,我们报告了一种DNA模板合成(DTS)结构,通过头尾超分子环化将多肽稳定为α螺旋构象。通过使用针对 MDM2 的试验文库,我们发现反复筛选可以将一个结合剂从文库中最低的丰度放大到与结合亲和力相关的等级。这项研究还强调了设计文库的必要性,这样才能避免 DTS 中异质产率造成的化学偏差。
{"title":"Translation of Deoxyribonucleic Acid into Synthetic Alpha Helical Peptides for Darwinian Evolution.","authors":"Millicent Dockerill, Pramod M Sabale, Francesco Russo, Sofia Barluenga, Nicolas Winssinger","doi":"10.1021/jacsau.4c00738","DOIUrl":"10.1021/jacsau.4c00738","url":null,"abstract":"<p><p>DNA-encoded libraries connect the phenotypes of synthetic molecules to a DNA barcode; however, most libraries do not tap into the potential of Darwinian evolution. Herein, we report a DNA-templated synthesis (DTS) architecture to make peptides that are stabilized into α-helical conformations via head-to-tail supramolecular cyclization. Using a pilot library targeting MDM2, we show that repeated screening can amplify a binder from the lowest abundance in the library to a ranking that correlates to binding affinity. The study also highlights the need to design libraries such that the chemistry avoids biases from the heterogeneous yield in DTS.</p>","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/PMC11522901/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142559878","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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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

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.

环境电化学还原氮氧化物是一种可持续还原氮氧化物和合成 NH3 的双重解决方案。然而,它们复杂的动力学和能量需求要求高性能的电催化剂,以确保有效和选择性的工艺结果。在此,我们报告了一种二维铜基金属有机框架(MOF){[Cu(HL)]-H2O} n(Cu-OUC,H3L = 5-(2'-羧基苯氧基)间苯二甲酸)可作为一种稳定的电催化剂,高效地实现 NO 到 NH3 的转化。电化学实验研究表明,在 0.1 M K2SO4 溶液中,制备的 Cu-OUC 的峰值法拉第效率达到 96.91%,显著的 NH3 产率高达 3415.82 μg h-1 mg-1。水溶液中的 Zn-NO 电池可产生功率密度为 2.04 mW cm-2 的电能,同时实现 616.92 μg h-1 mg-1 的 NH3 产量。理论计算显示,Cu-OUC 表面通过 "电子接受和捐赠 "的双向电荷转移机制有效促进了 NO 的活化,而 *NO 的形成步骤是电位决定阶段。该研究开创性地将 MOF 用作常温 NO-NH3 转化的电催化剂。
{"title":"Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH<sub>3</sub>.","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":"<p><p>Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH<sub>3</sub> 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)]·H<sub>2</sub>O} <sub><i>n</i></sub> , (<b>Cu-OUC</b>, H<sub>3</sub>L = 5-(2'-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH<sub>3</sub> conversion. Electrochemical experimental studies showed that in 0.1 M K<sub>2</sub>SO<sub>4</sub> solution, the as-prepared <b>Cu-OUC</b> achieved a peak Faradaic efficiency of 96.91% and a notable NH<sub>3</sub> yield as high as 3415.82 μg h<sup>-1</sup> mg<sup>-1</sup>. The Zn-NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm<sup>-2</sup> while simultaneously achieving an NH<sub>3</sub> yield of 616.92 μg h<sup>-1</sup> mg<sup>-1</sup>. Theoretical calculations revealed that the surface of <b>Cu-OUC</b> 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-NH<sub>3</sub> conversion.</p>","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 Q1 CHEMISTRY, MULTIDISCIPLINARY 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*, 

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.

环境电化学还原氮氧化物是一种可持续还原氮氧化物和合成 NH3 的双重解决方案。然而,它们复杂的动力学和能量需求要求高性能的电催化剂,以确保有效和选择性的工艺结果。在此,我们报告了一种二维铜基金属有机框架(MOF){[Cu(HL)]-H2O}n(Cu-OUC,H3L = 5-(2′-羧基苯氧基)间苯二甲酸)可作为一种稳定的电催化剂,高效实现 NO 到 NH3 的转化。电化学实验研究表明,在 0.1 M K2SO4 溶液中,制备的 Cu-OUC 的峰值法拉第效率达到 96.91%,显著的 NH3 产率高达 3415.82 μg h-1 mg-1。水溶液中的 Zn-NO 电池可产生功率密度为 2.04 mW cm-2 的电能,同时实现 616.92 μg h-1 mg-1 的 NH3 产量。理论计算显示,Cu-OUC 表面通过 "电子接受和捐赠 "的双向电荷转移机制有效促进了 NO 的活化,而 *NO 的形成步骤是电位决定阶段。该研究开创性地将 MOF 用作常温 NO-NH3 转化的电催化剂。
{"title":"Two-Dimensional MOF Constructed by a Binuclear-Copper Motif for High-Performance Electrocatalytic NO Reduction to NH3","authors":"Rong Luo,&nbsp;Bao-Jing Li,&nbsp;Zhan-Peng Wang,&nbsp;Ming-Guang Chen,&nbsp;Gui-Lin Zhuang*,&nbsp;Quan Li,&nbsp;Jia-Ping Tong,&nbsp;Wen-Tai Wang*,&nbsp;Yu-Hua Fan and Feng Shao*,&nbsp;","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":"<p >Ambient electrochemical NO reduction presents a dual solution for sustainable NO reduction and NH<sub>3</sub> 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)]·H<sub>2</sub>O}<sub><i>n</i></sub>, (<b>Cu-OUC</b>, H<sub>3</sub>L = 5-(2′-carboxylphenoxy)isophthalic acid) acts as a stable electrocatalyst with high efficiency for NO-to-NH<sub>3</sub> conversion. Electrochemical experimental studies showed that in 0.1 M K<sub>2</sub>SO<sub>4</sub> solution, the as-prepared <b>Cu-OUC</b> achieved a peak Faradaic efficiency of 96.91% and a notable NH<sub>3</sub> yield as high as 3415.82 μg h<sup>–1</sup> mg<sup>–1</sup>. The Zn–NO battery in aqueous solution can produce electricity possessing a power density of 2.04 mW cm<sup>–2</sup> while simultaneously achieving an NH<sub>3</sub> yield of 616.92 μg h<sup>–1</sup> mg<sup>–1</sup>. Theoretical calculations revealed that the surface of <b>Cu-OUC</b> 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-NH<sub>3</sub> conversion.</p>","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
期刊
JACS Au
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1