ACS Macro Letters最新文献_第9页

Inhibition of α-Synuclein Misfolding into β-Sheet Domains on Medium-Sized Gold Nanoclusters: Evidence from Enhanced Sampling MD Simulations 中等尺寸金纳米团簇抑制α-突触核蛋白错折叠成β片状结构域：来自增强采样 MD 模拟的证据

IF 5.8

ACS Macro Letters Pub Date : 2024-10-22 DOI: 10.1021/acsmacrolett.4c00533

Shuai Gong, Guanbin Gao, Taolei Sun, Lei Shen

{"title":"Inhibition of α-Synuclein Misfolding into β-Sheet Domains on Medium-Sized Gold Nanoclusters: Evidence from Enhanced Sampling MD Simulations","authors":"Shuai Gong, Guanbin Gao, Taolei Sun, Lei Shen","doi":"10.1021/acsmacrolett.4c00533","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00533","url":null,"abstract":"Targeting Parkinson’s disease (PD) related protein, α-synuclein (αS), via gold nanoclusters (AuNCs) has received considerable attention in PD treatments, but its molecular basis on the initial interactions between αS and AuNCs remains elusive due to the absence of a unique secondary structure of αS chains. Here, at the single-cluster level, we incorporate well-tempered metadynamics simulations to explore the structural and thermodynamic characteristics of the full length αS adsorbed on different-sized AuNCs (Aun, n = 25, 36, 44, 68, 102) with modeled thiolated ligands (Aun@Lig). The conformational landscapes of αS indicate that uncharged Aun@SCH2OH chaperones the native intrinsically disordered conformations of αS, while negatively and positively charged AuNCs greatly increase the likelihood of forming intramolecular β-sheet domains, which are necessary for αS fibrillation and are a hallmark of PD. The binding details further demonstrate the significant inhibitory effect of the medium-sized Au36@SCH2OH on αS misfolding into β-sheet domains. This provides a valuable guideline for customizing AuNCs to precisely manipulate protein folding and misfolding behaviors, with potential implications for disease treatments.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"66 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486763","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

Room-Temperature Synthesis of a Fluorine-Functionalized Nanoporous Organic Polymer for Highly Efficient SF6 Adsorption and Separation 用于高效吸附和分离 SF6 的氟官能化纳米多孔有机聚合物的室温合成

IF 5.8

ACS Macro Letters Pub Date : 2024-10-21 DOI: 10.1021/acsmacrolett.4c00559

Sihan Tong, Lu Yao, Qilin Wang, Jiangli Zhu, Zefeng Wang, Jun Yan

{"title":"Room-Temperature Synthesis of a Fluorine-Functionalized Nanoporous Organic Polymer for Highly Efficient SF6 Adsorption and Separation","authors":"Sihan Tong, Lu Yao, Qilin Wang, Jiangli Zhu, Zefeng Wang, Jun Yan","doi":"10.1021/acsmacrolett.4c00559","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00559","url":null,"abstract":"Sulfur hexafluoride (SF6) is widely used in the power industry and significantly contributes to the greenhouse effect, necessitating the development of efficient materials for SF6 capture, particularly fluorine-containing materials. However, existing fluorine-containing materials often require complex monomers and high synthesis temperatures. Herein, we report the synthesis of a fluorine-functionalized carbazole-based nanoporous organic polymer (CNOP-7) at room temperature, using commercially available 4,4′-bis(9H-carbazole-9-yl)-1,1′-biphenyl and 1,1,1-trifluoroacetone. CNOP-7 contains 14.7% fluorine atoms and exhibits a high specific surface area of 1270 m2·g–1, demonstrating excellent SF6 adsorption and separation performance. The SF6/N2 selectivity of CNOP-7 reaches 107 at 273 K and 73 at 298 K. Furthermore, dynamic breakthrough experiments confirm that CNOP-7 can efficiently and repeatedly separate SF6 from SF6/N2 mixtures. Molecular simulations reveal the mechanism behind its efficient separation. This work offers fresh perspectives on the development and fabrication of adsorbents for efficient SF6 sequestration.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"65 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452351","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

Room-Temperature Synthesis of a Fluorine-Functionalized Nanoporous Organic Polymer for Highly Efficient SF6 Adsorption and Separation 用于高效吸附和分离 SF6 的氟官能化纳米多孔有机聚合物的室温合成

IF 5.1

ACS Macro Letters Pub Date : 2024-10-21 DOI: 10.1021/acsmacrolett.4c0055910.1021/acsmacrolett.4c00559

Sihan Tong, Lu Yao, Qilin Wang, Jiangli Zhu, Zefeng Wang and Jun Yan*,

{"title":"Room-Temperature Synthesis of a Fluorine-Functionalized Nanoporous Organic Polymer for Highly Efficient SF6 Adsorption and Separation","authors":"Sihan Tong, Lu Yao, Qilin Wang, Jiangli Zhu, Zefeng Wang and Jun Yan*, ","doi":"10.1021/acsmacrolett.4c0055910.1021/acsmacrolett.4c00559","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00559https://doi.org/10.1021/acsmacrolett.4c00559","url":null,"abstract":"Sulfur hexafluoride (SF6) is widely used in the power industry and significantly contributes to the greenhouse effect, necessitating the development of efficient materials for SF6 capture, particularly fluorine-containing materials. However, existing fluorine-containing materials often require complex monomers and high synthesis temperatures. Herein, we report the synthesis of a fluorine-functionalized carbazole-based nanoporous organic polymer (CNOP-7) at room temperature, using commercially available 4,4′-bis(9H-carbazole-9-yl)-1,1′-biphenyl and 1,1,1-trifluoroacetone. CNOP-7 contains 14.7% fluorine atoms and exhibits a high specific surface area of 1270 m2·g–1, demonstrating excellent SF6 adsorption and separation performance. The SF6/N2 selectivity of CNOP-7 reaches 107 at 273 K and 73 at 298 K. Furthermore, dynamic breakthrough experiments confirm that CNOP-7 can efficiently and repeatedly separate SF6 from SF6/N2 mixtures. Molecular simulations reveal the mechanism behind its efficient separation. This work offers fresh perspectives on the development and fabrication of adsorbents for efficient SF6 sequestration.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 11","pages":"1469–1475 1469–1475"},"PeriodicalIF":5.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671796","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

Effects of a Mechanically Interlocked Structure on Ionic Conductivity in Polyrotaxane-Based Polymer Electrolytes 机械互锁结构对聚罗双环烷基聚合物电解质离子电导率的影响

IF 5.1

ACS Macro Letters Pub Date : 2024-10-16 DOI: 10.1021/acsmacrolett.4c0048010.1021/acsmacrolett.4c00480

Bitgaram Kim, Eunji Lee and Ji-Hun Seo*,

引用次数: 0

Effects of a Mechanically Interlocked Structure on Ionic Conductivity in Polyrotaxane-Based Polymer Electrolytes 机械互锁结构对聚罗双环烷基聚合物电解质离子电导率的影响

IF 5.8

ACS Macro Letters Pub Date : 2024-10-16 DOI: 10.1021/acsmacrolett.4c00480

Bitgaram Kim, Eunji Lee, Ji-Hun Seo

引用次数: 0

Crafting Nanostructured Hybrid Block Copolymer-Gold Nanoparticles by Confined Self-Assembly in Evaporative Droplets. 通过蒸发液滴中的受限自组装，制作纳米结构的嵌段共聚物-金纳米颗粒。

IF 5.1

ACS Macro Letters Pub Date : 2024-10-15 Epub Date: 2024-09-23 DOI: 10.1021/acsmacrolett.4c00519

Andrea Escher, Gianluca Bravetti, Simone Bertucci, Davide Comoretto, Christoph Weder, Ullrich Steiner, Paola Lova, Andrea Dodero

{"title":"Crafting Nanostructured Hybrid Block Copolymer-Gold Nanoparticles by Confined Self-Assembly in Evaporative Droplets.","authors":"Andrea Escher, Gianluca Bravetti, Simone Bertucci, Davide Comoretto, Christoph Weder, Ullrich Steiner, Paola Lova, Andrea Dodero","doi":"10.1021/acsmacrolett.4c00519","DOIUrl":"10.1021/acsmacrolett.4c00519","url":null,"abstract":"Hybrid organic-inorganic nanostructures offer significant potential for developing advanced functional materials with numerous technological applications. However, the fabrication process is often tedious and time-consuming. This study presents a facile method for fabricating block copolymer-based photonic microspheres incorporating plasmonic gold nanoparticles. Specifically, the confined self-assembly of poly(styrene)-b-poly(2-vinylpyridine) in emulsion droplets allows the formation of spherical, noniridescent, concentric lamellar structures, i.e., onion-like particles that are subsequently infiltrated with gold salt. Using ethanol as a preferential solvent allows the loading of metal ions exclusively into the poly(2-vinylpyridine) domains, which are subsequently reduced, leading to the in situ, spatially controlled formation of gold nanoparticles. The hybrid structures exhibit a well-defined photonic bandgap and plasmonic resonance at low gold concentrations. These results demonstrate the feasibility of fabricating optically active photonic structures comprising metal nanoparticles in a block copolymer array via a simple two-step fabrication process.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":" ","pages":"1338-1344"},"PeriodicalIF":5.1,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11483756/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306513","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

Controlled Fabrication of Distinct Nanostructures from Discrete Oligourethanes via Thermal Annealing 通过热退火从离散低聚氨基甲酸酯中可控地制造出独特的纳米结构

IF 5.1

ACS Macro Letters Pub Date : 2024-10-15 DOI: 10.1021/acsmacrolett.4c0061510.1021/acsmacrolett.4c00615

Qiangqiang Shi, Yong Yu, Lingxiao Guo, Jialin Zhang, Jiajia Tan, Jin Zhang, Jinming Hu* and Shiyong Liu*,

{"title":"Controlled Fabrication of Distinct Nanostructures from Discrete Oligourethanes via Thermal Annealing","authors":"Qiangqiang Shi, Yong Yu, Lingxiao Guo, Jialin Zhang, Jiajia Tan, Jin Zhang, Jinming Hu* and Shiyong Liu*, ","doi":"10.1021/acsmacrolett.4c0061510.1021/acsmacrolett.4c00615","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00615https://doi.org/10.1021/acsmacrolett.4c00615","url":null,"abstract":"The self-assembly of sequence-defined polymers (SDPs) enables the formation of a diverse array of nanostructures; however, the construction of complex hierarchical structures via thermal annealing from SDPs remains relatively unexplored. In this study, two series of oligourethanes, 2Cit-pBn-OH and 2Cit-mBn-OH, were synthesized to investigate their thermal annealing behaviors. Nanorod clusters were generated from 2Cit-pB6-OH in a mixture of 1,4-dioxane and toluene, whereas 2Cit-pB8-OH formed nanosheets after thermal annealing. Upon modifying the structure of the repeating units, 2Cit-mB6-OH self-assembled into ultrathin nanosheets, transitioning from nanospheres after thermal annealing in a mixture of isopropanol and cyclohexane, while “flower” micelles were produced from 2Cit-mB8-OH. Interestingly, when isopropanol was replaced with a mixture of isopropanol and tetrahydrofuran (THF), uniform nanotubes were generated by 2Cit-mB6-OH under the same thermal annealing conditions. Additionally, a discrete amphiphile (2Cit-mB4-(S)DPEG) was synthesized, leading to the formation of uniform nanosheets in aqueous solution after thermal annealing. This work highlights the significant effects of sequence and repeating unit structure of SDPs on their self-assembly behaviors and presents a novel strategy for the controlled fabrication of unique nanostructures from SDPs.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 11","pages":"1456–1462 1456–1462"},"PeriodicalIF":5.1,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671845","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

A Total Internal Reflection Microscopy (TIRM)-Based Approach for Direct Characterization of Polymer Brush Conformational Change in Aqueous Solution. 基于全内反射显微镜 (TIRM) 的直接表征水溶液中聚合物刷构象变化的方法。

IF 5.1

ACS Macro Letters Pub Date : 2024-10-15 Epub Date: 2024-10-04 DOI: 10.1021/acsmacrolett.4c00476

Jiahao Wu, Feng Cao, Pui Wo Felix Yeung, Manjia Li, Kohji Ohno, To Ngai

{"title":"A Total Internal Reflection Microscopy (TIRM)-Based Approach for Direct Characterization of Polymer Brush Conformational Change in Aqueous Solution.","authors":"Jiahao Wu, Feng Cao, Pui Wo Felix Yeung, Manjia Li, Kohji Ohno, To Ngai","doi":"10.1021/acsmacrolett.4c00476","DOIUrl":"10.1021/acsmacrolett.4c00476","url":null,"abstract":"This study presents a novel approach utilizing total internal reflection microscopy (TIRM) to effectively characterize the swelling and collapse of polymer brushes in aqueous solutions. Zwitterionic poly(carboxybetaine methacrylate) (PCBMA) and nonionic poly[oligo(ethylene glycol) methyl ether methacrylate] (POEGMA) brushes are chosen as model systems. By investigation of an intriguing theory-experiment discrepancy observed during the measurement of near-wall hindered diffusion, valuable insights into the compressibility of polymer brushes are obtained, revealing their conformational information in aqueous solution. The results demonstrate that zwitterionic PCBMA brushes exhibit minimal antipolyelectrolyte effects in 0.1-10 mM NaCl solution but undergo significant swelling with increasing pH. On the other hand, nonionic POEGMA brushes exhibit similar responses to ionic strength as weak polyelectrolyte brushes. These unexpected findings enhance our understanding of polymer brushes beyond classical theories. The TIRM-based approach proves to be effective for characterizing polymer brushes and other soft nanomaterials.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":" ","pages":"1376-1382"},"PeriodicalIF":5.1,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11483946/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370167","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

Alkyl-Substituted Polycaprolactone Poly(urethane-urea)s as Mechanically Competitive and Chemically Recyclable Materials 作为具有机械竞争力和化学可回收材料的烷基取代聚己内酯聚脲

IF 5.8

ACS Macro Letters Pub Date : 2024-10-15 DOI: 10.1021/acsmacrolett.4c00474

Derek C. Batiste, Michaela R. Pfau-Cloud, Hee Joong Kim, Christopher J. Ellison, Marc A. Hillmyer

{"title":"Alkyl-Substituted Polycaprolactone Poly(urethane-urea)s as Mechanically Competitive and Chemically Recyclable Materials","authors":"Derek C. Batiste, Michaela R. Pfau-Cloud, Hee Joong Kim, Christopher J. Ellison, Marc A. Hillmyer","doi":"10.1021/acsmacrolett.4c00474","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00474","url":null,"abstract":"We report the mechanical performance and chemical recycling advantages of implementing alkyl-substituted poly(ε-caprolactones) (PCLs) as soft segments in thermoplastic poly(urethane-urea) (TPUU) materials. Poly(4-methylcaprolactone) (P4MCL) and poly(4-propylcaprolactone) (P4PrCL) were prepared, reacted with isophorone diisocyanate, and chain-extended with water to form TPUUs. The resulting materials’ tensile properties were similar or superior to a commercially available polyester thermoplastic poly(urethane) and had superior elastic recovery properties compared to a PCL analogue due to the noncrystalline nature of P4MCL and P4PrCL. Additionally, monomers were recovered from the TPUU materials in high yields via ring-closing depolymerization using a reactive distillation approach at an elevated temperature and a reduced pressure (240–260 °C, 25–140 mTorr) with zinc chloride (ZnCl2) as the catalyst. The thermodynamics of polymerization were estimated using Van’t Hoff analyses for 4MCL and 4PrCL; these results indicated that the propyl group in 4PrCL results in a lower practical ceiling temperature (Tc) for P4PrCL.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"124 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436333","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

Alkyl-Substituted Polycaprolactone Poly(urethane-urea)s as Mechanically Competitive and Chemically Recyclable Materials 作为具有机械竞争力和化学可回收材料的烷基取代聚己内酯聚脲

IF 5.1

ACS Macro Letters Pub Date : 2024-10-15 DOI: 10.1021/acsmacrolett.4c0047410.1021/acsmacrolett.4c00474

Derek C. Batiste, Michaela R. Pfau-Cloud, Hee Joong Kim, Christopher J. Ellison* and Marc A. Hillmyer*,

{"title":"Alkyl-Substituted Polycaprolactone Poly(urethane-urea)s as Mechanically Competitive and Chemically Recyclable Materials","authors":"Derek C. Batiste, Michaela R. Pfau-Cloud, Hee Joong Kim, Christopher J. Ellison* and Marc A. Hillmyer*, ","doi":"10.1021/acsmacrolett.4c0047410.1021/acsmacrolett.4c00474","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00474https://doi.org/10.1021/acsmacrolett.4c00474","url":null,"abstract":"We report the mechanical performance and chemical recycling advantages of implementing alkyl-substituted poly(ε-caprolactones) (PCLs) as soft segments in thermoplastic poly(urethane-urea) (TPUU) materials. Poly(4-methylcaprolactone) (P4MCL) and poly(4-propylcaprolactone) (P4PrCL) were prepared, reacted with isophorone diisocyanate, and chain-extended with water to form TPUUs. The resulting materials’ tensile properties were similar or superior to a commercially available polyester thermoplastic poly(urethane) and had superior elastic recovery properties compared to a PCL analogue due to the noncrystalline nature of P4MCL and P4PrCL. Additionally, monomers were recovered from the TPUU materials in high yields via ring-closing depolymerization using a reactive distillation approach at an elevated temperature and a reduced pressure (240–260 °C, 25–140 mTorr) with zinc chloride (ZnCl2) as the catalyst. The thermodynamics of polymerization were estimated using Van’t Hoff analyses for 4MCL and 4PrCL; these results indicated that the propyl group in 4PrCL results in a lower practical ceiling temperature (Tc) for P4PrCL.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 11","pages":"1449–1455 1449–1455"},"PeriodicalIF":5.1,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671844","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