ACS Macro Letters最新文献_第10页

Bulk Depolymerization of Polystyrene with Comonomer Radical Triggers 共聚单体自由基引发聚苯乙烯本体解聚的研究

IF 5.1

ACS Macro Letters Pub Date : 2025-04-23 DOI: 10.1021/acsmacrolett.5c0015910.1021/acsmacrolett.5c00159

James B. Young, Jared I. Bowman, Megan E. Lott, Lily A. Diodati, Kaden C. Stevens, Rhys W. Hughes, Lauren E. Mann, Alex H. Balzer, LaShanda T. J. Korley* and Brent S. Sumerlin*,

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引用次数: 0

Rapid Gelation of Dicyclopentadiene Resins for Additive Manufacturing of Thermoset Polymers 用于热固性聚合物增材制造的双环戊二烯树脂的快速凝胶化

IF 5.1

ACS Macro Letters Pub Date : 2025-04-23 DOI: 10.1021/acsmacrolett.5c0013210.1021/acsmacrolett.5c00132

Pranav Krishnan, Jacob J. Lessard, Jeffrey S. Moore and Nancy R. Sottos*,

引用次数: 0

Bulk Depolymerization of Polystyrene with Comonomer Radical Triggers 共聚单体自由基引发聚苯乙烯本体解聚的研究

IF 5.8

ACS Macro Letters Pub Date : 2025-04-23 DOI: 10.1021/acsmacrolett.5c00159

James B. Young, Jared I. Bowman, Megan E. Lott, Lily A. Diodati, Kaden C. Stevens, Rhys W. Hughes, Lauren E. Mann, Alex H. Balzer, LaShanda T. J. Korley, Brent S. Sumerlin

{"title":"Bulk Depolymerization of Polystyrene with Comonomer Radical Triggers","authors":"James B. Young, Jared I. Bowman, Megan E. Lott, Lily A. Diodati, Kaden C. Stevens, Rhys W. Hughes, Lauren E. Mann, Alex H. Balzer, LaShanda T. J. Korley, Brent S. Sumerlin","doi":"10.1021/acsmacrolett.5c00159","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00159","url":null,"abstract":"This study introduces a novel approach to depolymerize polystyrene in the absence of solvent at significantly reduced temperatures through the incorporation of a thermally labile comonomer. Specifically, we employ N-(methacryloxy)phthalimide (PhthMA) as a comonomer with an activated ester capable of thermally triggered decarboxylation. Thermal treatment enables the generation of backbone radicals that promote β-scission and subsequent unzipping. These polystyrene analogs depolymerize with up to 91% reversion to monomer in under 2 h at temperatures significantly lower than those required for conventional polystyrene. As compared to depolymerization triggered by decarboxylation at the ω-chain end, this pendent-group approach was considerably more efficient. The recovered styrene monomer from the bulk depolymerization of poly(styrene-co-PhthMA) copolymers can undergo direct repolymerization, yielding new styrenic materials. This comonomer strategy extends across various styrenic copolymers, highlighting its potential as a broadly applicable method for initiating depolymerization among vinyl polymer classes.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"48 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866154","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

Functionalization of Water-Soluble Metallopolymer Electrocatalysts for Water-Splitting Using Atom Transfer Radical Polymerization and Click Chemistry 基于原子转移自由基聚合和Click化学的水溶性金属聚合物电催化剂的功能化研究

IF 5.1

ACS Macro Letters Pub Date : 2025-04-23 DOI: 10.1021/acsmacrolett.5c0013810.1021/acsmacrolett.5c00138

Arthur C. Gibson, Richard S. Glass, Dennis L. Lichtenberger* and Jeffrey Pyun*,

{"title":"Functionalization of Water-Soluble Metallopolymer Electrocatalysts for Water-Splitting Using Atom Transfer Radical Polymerization and Click Chemistry","authors":"Arthur C. Gibson, Richard S. Glass, Dennis L. Lichtenberger* and Jeffrey Pyun*, ","doi":"10.1021/acsmacrolett.5c0013810.1021/acsmacrolett.5c00138","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00138https://doi.org/10.1021/acsmacrolett.5c00138","url":null,"abstract":"The diverse functionalization of the polymeric support phase of diiron disulfide [2Fe-2S] metallopolymer electrocatalysts offers a route to the enhanced generation of molecular hydrogen via water-splitting. Click chemistry has been shown to be a useful tool in post-polymerization functionalization for a wide range of polymeric materials under mild conditions, which is a requirement for [2Fe-2S] metallopolymers due to the presence of iron carbonyl (Fe–CO) bonds in the active site. In this study, we developed a new synthetic methodology to functionalize [2Fe-2S] metallopolymers using atom transfer radical polymerization (ATRP) and post-polymerization functionalization using azide–alkyne “click” cycloaddition. Azide functional [2Fe-2S] metallopolymers were prepared by the ATRP of 3-azidopropyl methacrylate (AzPMA) with either methyl methacrylate (MMA) or 2-(dimethylamino)ethyl methacrylate (DMAEMA), followed by copper-catalyzed “click” cycloaddition with functional terminal alkynes. Both families of PMMA and PDMAEMA functional [2Fe-2S] metallo-copolymers were found to retain Fe–CO bonds from the catalyst active site after the click chemistry reactions and, more importantly, exhibited high electrocatalytic activity for electrochemical water-splitting under pH-neutral aqueous conditions.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 5","pages":"582–588 582–588"},"PeriodicalIF":5.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088385","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

Functionalization of Water-Soluble Metallopolymer Electrocatalysts for Water-Splitting Using Atom Transfer Radical Polymerization and Click Chemistry 基于原子转移自由基聚合和Click化学的水溶性金属聚合物电催化剂的功能化研究

IF 5.8

ACS Macro Letters Pub Date : 2025-04-23 DOI: 10.1021/acsmacrolett.5c00138

Arthur C. Gibson, Richard S. Glass, Dennis L. Lichtenberger, Jeffrey Pyun

{"title":"Functionalization of Water-Soluble Metallopolymer Electrocatalysts for Water-Splitting Using Atom Transfer Radical Polymerization and Click Chemistry","authors":"Arthur C. Gibson, Richard S. Glass, Dennis L. Lichtenberger, Jeffrey Pyun","doi":"10.1021/acsmacrolett.5c00138","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00138","url":null,"abstract":"The diverse functionalization of the polymeric support phase of diiron disulfide [2Fe-2S] metallopolymer electrocatalysts offers a route to the enhanced generation of molecular hydrogen via water-splitting. Click chemistry has been shown to be a useful tool in post-polymerization functionalization for a wide range of polymeric materials under mild conditions, which is a requirement for [2Fe-2S] metallopolymers due to the presence of iron carbonyl (Fe–CO) bonds in the active site. In this study, we developed a new synthetic methodology to functionalize [2Fe-2S] metallopolymers using atom transfer radical polymerization (ATRP) and post-polymerization functionalization using azide–alkyne “click” cycloaddition. Azide functional [2Fe-2S] metallopolymers were prepared by the ATRP of 3-azidopropyl methacrylate (AzPMA) with either methyl methacrylate (MMA) or 2-(dimethylamino)ethyl methacrylate (DMAEMA), followed by copper-catalyzed “click” cycloaddition with functional terminal alkynes. Both families of PMMA and PDMAEMA functional [2Fe-2S] metallo-copolymers were found to retain Fe–CO bonds from the catalyst active site after the click chemistry reactions and, more importantly, exhibited high electrocatalytic activity for electrochemical water-splitting under pH-neutral aqueous conditions.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"53 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866152","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

Intermacromolecular Interaction Determines the Long-Ranged Force and Self-Assembly of Microgels at the Air/Water Interface 大分子间的相互作用决定了微凝胶在空气/水界面上的远程力和自组装

IF 5.1

ACS Macro Letters Pub Date : 2025-04-22 DOI: 10.1021/acsmacrolett.5c0011110.1021/acsmacrolett.5c00111

Wei Liu*, Zuwei Zhao, Li Zhang, Kangle Zhou, Pui Wo Felix Yeung, Hang Jiang, Cheng Yang, Yuwei Zhu and To Ngai*,

引用次数: 0

Metathesis Depolymerization of a Fluorogenic Self-Immolative Polymer 一种荧光自焚聚合物的复分解解聚

IF 5.1

ACS Macro Letters Pub Date : 2025-04-21 DOI: 10.1021/acsmacrolett.5c0019210.1021/acsmacrolett.5c00192

Gavin J. Giardino, and , Jia Niu*,

引用次数: 0

Metathesis Depolymerization of a Fluorogenic Self-Immolative Polymer 一种荧光自焚聚合物的复分解解聚

IF 5.8

ACS Macro Letters Pub Date : 2025-04-21 DOI: 10.1021/acsmacrolett.5c00192

Gavin J. Giardino, Jia Niu

引用次数: 0

Intermacromolecular Interaction Determines the Long-Ranged Force and Self-Assembly of Microgels at the Air/Water Interface 大分子间的相互作用决定了微凝胶在空气/水界面上的远程力和自组装

IF 5.8

ACS Macro Letters Pub Date : 2025-04-21 DOI: 10.1021/acsmacrolett.5c00111

Wei Liu, Zuwei Zhao, Li Zhang, Kangle Zhou, Pui Wo Felix Yeung, Hang Jiang, Cheng Yang, Yuwei Zhu, To Ngai

引用次数: 0

Organobase-Catalyzed Carboxyl-yne Click Polymerization 有机碱催化的羧基炔咔嗒聚合

IF 5.1

ACS Macro Letters Pub Date : 2025-04-19 DOI: 10.1021/acsmacrolett.5c0012310.1021/acsmacrolett.5c00123

Han Si, Jie Zhang, Anjun Qin* and Ben Zhong Tang,

{"title":"Organobase-Catalyzed Carboxyl-yne Click Polymerization","authors":"Han Si, Jie Zhang, Anjun Qin* and Ben Zhong Tang, ","doi":"10.1021/acsmacrolett.5c0012310.1021/acsmacrolett.5c00123","DOIUrl":"https://doi.org/10.1021/acsmacrolett.5c00123https://doi.org/10.1021/acsmacrolett.5c00123","url":null,"abstract":"Polyesters have been widely used in the biological and engineering fields. However, the polycondensations used require high reaction temperatures and long reaction times, and the ring-opening polymerizations are generally intolerant to functional groups. Therefore, the development of a new polymerization toward polyesters under mild reaction conditions will further promote their development. In this work, we established a new organobase-catalyzed click polymerization of ester-activated alkynes and bis(carboxylic acid)s under mild reaction conditions, and regio- and stereoregular poly(β-acyloxyacrylate)s with weight-average molecular weights up to 24200 were obtained in yields up to 96%. The resultant polymers show versatile properties. The aliphatic poly(β-acyloxyacrylate)s exhibit crystalline behavior, whereas the aromatic polymers demonstrate high thermal stability. The polymer containing tetraphenylethene units exhibits the trade-off of high refractive index and Abbé Number. Thanks to the dynamic nature of β-acyloxyacrylate units, the resultant polymers could be quickly degraded upon addition of phenol derivatives and organobase, which could be applied in the fabrication of fluorescent photopatterns. Thus, this work not only provides a powerful polymerization toward polyesters and a facile reaction for postmodification of the materials containing carbonyl groups, but also enriches the family of X-yne click polymerization.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 5","pages":"551–557 551–557"},"PeriodicalIF":5.1,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088436","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