ACS Macro LettersPub Date : 2024-12-09DOI: 10.1021/acsmacrolett.4c00775
Caitlin S. Sample, Brenden D. Hoehn, Marc A. Hillmyer
{"title":"Correction to “Cross-Linked Polyolefins through Tandem ROMP/Hydrogenation”","authors":"Caitlin S. Sample, Brenden D. Hoehn, Marc A. Hillmyer","doi":"10.1021/acsmacrolett.4c00775","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00775","url":null,"abstract":"In our original publication, we made an error in Figure 4 and the corresponding caption. The legend labels in Figure 4b are inverted, with the gray curves incorrectly labeled as “C90D10” and the black curves as “C10D90”. The caption has an additional typographical error. These errors do not affect the results or conclusions of the article, as the values in Figure 4a and the associated discussion reference the accurate data. The corrected versions of Figure 4 and the caption are presented here. Figure 4. (a) Mechanical properties of samples before and after hydrogenation. Values are average ± standard deviation for 5 (C90D10, C10D90, H–C10D90) or 3 (H–C90D10) replicates. (b) Representative tensile curves for C90D10, H–C90D10, C10D90, and H–C10D90. *Samples pulled out from grips. This article has not yet been cited by other publications.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"56 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797620","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}
ACS Macro LettersPub Date : 2024-12-09DOI: 10.1021/acsmacrolett.4c0077510.1021/acsmacrolett.4c00775
Caitlin S. Sample, Brenden D. Hoehn and Marc A. Hillmyer*,
{"title":"Correction to “Cross-Linked Polyolefins through Tandem ROMP/Hydrogenation”","authors":"Caitlin S. Sample, Brenden D. Hoehn and Marc A. Hillmyer*, ","doi":"10.1021/acsmacrolett.4c0077510.1021/acsmacrolett.4c00775","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00775https://doi.org/10.1021/acsmacrolett.4c00775","url":null,"abstract":"","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"14 1","pages":"1 1"},"PeriodicalIF":5.1,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143086899","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}
ACS Macro LettersPub Date : 2024-12-07DOI: 10.1021/acsmacrolett.4c0066510.1021/acsmacrolett.4c00665
Chihui Zheng, Gadi Slor, Youwei Ma* and Francesco Stellacci*,
{"title":"Direct Monomer Recovery from Ring-Closing Depolymerization of Thermosets","authors":"Chihui Zheng, Gadi Slor, Youwei Ma* and Francesco Stellacci*, ","doi":"10.1021/acsmacrolett.4c0066510.1021/acsmacrolett.4c00665","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00665https://doi.org/10.1021/acsmacrolett.4c00665","url":null,"abstract":"<p >Recovering monomers from the depolymerization of thermosets presents a significant challenge, which becomes even more daunting if one sets the goal of doing it directly, i.e., without complex chemical separation steps. To this end, we have synthesized a new type of polycarbonate thermoset by first copolymerizing alkyl cyclic carbonates (<b>ACC</b>s) with small amounts of allyloxy cyclic carbonates (<b>AoCC</b>s), followed by cross-linking the resulting allyloxy polycarbonate with excess tetrathiol compounds under UV irradiation. These cross-linked polycarbonates demonstrate enhanced thermal and mechanical properties compared to their linear analogues, while maintaining the linear polymers’ capacity for ring-closing depolymerization. The depolymerization process enables the direct recovery of <b>ACC</b> and its dimer, bypassing complex chemical separation steps that are commonly employed in the recycling of conventional chemically recyclable thermosets. The yields range from 74.7% to 91.7% depending on the ratios of <b>AoCC</b> to <b>ACC</b> in the thermosets. Furthermore, the recovered compounds can be repolymerized with <b>AoCC</b>s leading to polycarbonate of the same quality to the initially synthesized one.</p>","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 12","pages":"1704–1710 1704–1710"},"PeriodicalIF":5.1,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmacrolett.4c00665","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842273","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}
ACS Macro LettersPub Date : 2024-12-07DOI: 10.1021/acsmacrolett.4c00665
Chihui Zheng, Gadi Slor, Youwei Ma, Francesco Stellacci
{"title":"Direct Monomer Recovery from Ring-Closing Depolymerization of Thermosets","authors":"Chihui Zheng, Gadi Slor, Youwei Ma, Francesco Stellacci","doi":"10.1021/acsmacrolett.4c00665","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00665","url":null,"abstract":"Recovering monomers from the depolymerization of thermosets presents a significant challenge, which becomes even more daunting if one sets the goal of doing it directly, i.e., without complex chemical separation steps. To this end, we have synthesized a new type of polycarbonate thermoset by first copolymerizing alkyl cyclic carbonates (<b>ACC</b>s) with small amounts of allyloxy cyclic carbonates (<b>AoCC</b>s), followed by cross-linking the resulting allyloxy polycarbonate with excess tetrathiol compounds under UV irradiation. These cross-linked polycarbonates demonstrate enhanced thermal and mechanical properties compared to their linear analogues, while maintaining the linear polymers’ capacity for ring-closing depolymerization. The depolymerization process enables the direct recovery of <b>ACC</b> and its dimer, bypassing complex chemical separation steps that are commonly employed in the recycling of conventional chemically recyclable thermosets. The yields range from 74.7% to 91.7% depending on the ratios of <b>AoCC</b> to <b>ACC</b> in the thermosets. Furthermore, the recovered compounds can be repolymerized with <b>AoCC</b>s leading to polycarbonate of the same quality to the initially synthesized one.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"220 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142788623","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}
ACS Macro LettersPub Date : 2024-12-05DOI: 10.1021/acsmacrolett.4c00651
Yuta Miyamori, Youngwon Kong, Yuta Nabae, Kan Hatakeyama-Sato, Teruaki Hayakawa
{"title":"Highly Ordered Bimodal Mesoporous Carbon from ABC Triblock Terpolymers with Phenolic Resol","authors":"Yuta Miyamori, Youngwon Kong, Yuta Nabae, Kan Hatakeyama-Sato, Teruaki Hayakawa","doi":"10.1021/acsmacrolett.4c00651","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00651","url":null,"abstract":"Mesoporous carbons (MPCs) with a bimodal distribution of pore diameters are more advantageous than their monomodal counterparts for applications in adsorption, catalysis, and drug delivery systems; however, reports on their fabrication remain limited. In this study, we successfully fabricated bimodal MPCs using a soft template method with poly(2,2,2-trifluoroethyl methacrylate) (PTFEMA)-<i>b</i>-poly(4-vinylpyridine) (P4VP)-<i>b</i>-polystyrene (PS) and resol. The blend samples formed microphase-separated structures comprising PTFEMA spheres, PS cylinders, and matrix domains composed of P4VP and resol, leading to the separation of the PTFEMA and PS domains. The P4VP and resol matrix domains were carbonized at a high temperature of 900 °C, whereas the PTFEMA and PS domains were thermally decomposed. This process resulted in bimodal MPCs with both spherical and cylindrical mesopores. The pore diameters calculated using scanning electron microscopy were approximately 10 and 30 nm, while nitrogen adsorption measurements indicated a large specific surface area with a bimodal pore distribution.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"79 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782866","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}
ACS Macro LettersPub Date : 2024-12-05DOI: 10.1021/acsmacrolett.4c0065110.1021/acsmacrolett.4c00651
Yuta Miyamori, Youngwon Kong, Yuta Nabae, Kan Hatakeyama-Sato and Teruaki Hayakawa*,
{"title":"Highly Ordered Bimodal Mesoporous Carbon from ABC Triblock Terpolymers with Phenolic Resol","authors":"Yuta Miyamori, Youngwon Kong, Yuta Nabae, Kan Hatakeyama-Sato and Teruaki Hayakawa*, ","doi":"10.1021/acsmacrolett.4c0065110.1021/acsmacrolett.4c00651","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00651https://doi.org/10.1021/acsmacrolett.4c00651","url":null,"abstract":"<p >Mesoporous carbons (MPCs) with a bimodal distribution of pore diameters are more advantageous than their monomodal counterparts for applications in adsorption, catalysis, and drug delivery systems; however, reports on their fabrication remain limited. In this study, we successfully fabricated bimodal MPCs using a soft template method with poly(2,2,2-trifluoroethyl methacrylate) (PTFEMA)-<i>b</i>-poly(4-vinylpyridine) (P4VP)-<i>b</i>-polystyrene (PS) and resol. The blend samples formed microphase-separated structures comprising PTFEMA spheres, PS cylinders, and matrix domains composed of P4VP and resol, leading to the separation of the PTFEMA and PS domains. The P4VP and resol matrix domains were carbonized at a high temperature of 900 °C, whereas the PTFEMA and PS domains were thermally decomposed. This process resulted in bimodal MPCs with both spherical and cylindrical mesopores. The pore diameters calculated using scanning electron microscopy were approximately 10 and 30 nm, while nitrogen adsorption measurements indicated a large specific surface area with a bimodal pore distribution.</p>","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 12","pages":"1698–1703 1698–1703"},"PeriodicalIF":5.1,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmacrolett.4c00651","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849937","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}
{"title":"Rational Design of Self-Reporting Polymersomes for the Controlled Release of Sulfur Dioxide","authors":"Zhezhe Li, Yue Zhang, Suzhen Wang, Yihan Wu and Hailong Che*, ","doi":"10.1021/acsmacrolett.4c0068710.1021/acsmacrolett.4c00687","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00687https://doi.org/10.1021/acsmacrolett.4c00687","url":null,"abstract":"<p >As a new member of the gaseous regulators, sulfur dioxide (SO<sub>2</sub>) plays a crucial role in many biological activities. Recent studies have shown that SO<sub>2</sub> is capable of inducing cancer cell apoptosis by regulating intracellular reactive oxygen species (ROS), allowing SO<sub>2</sub> to serve as an efficient therapeutic agent. Although various polymer-based platforms have presented great potential for the controlled release of SO<sub>2</sub>, most of the systems are incapable of monitoring the intracellular generation of SO<sub>2</sub>. In this work we present the rational design of SO<sub>2</sub>-releasing biodegradable polymersomes, accompanied by a self-reporting property. The polymersome consists of a hydrophilic block of poly(ethylene glycol) (PEG) and a hydrophobic segment of poly(trimethylene carbonate) (PTMC)-based SO<sub>2</sub> donors. The polymersomes not only exhibit good SO<sub>2</sub>-releasing performance upon treatment with glutathione (GSH), but can also regulate the fluorescence change of the system, offering a good platform for real-time monitoring of the intracellular production of SO<sub>2</sub>. Significantly, the <i>in vitro</i> and <i>in vivo</i> studies indicate the potential for exploitation of these polymersomes as antitumor agents. We expect that incorporating both the SO<sub>2</sub>-releasing capacity and self-reporting feature within a polymersome system will provide a unique opportunity for the development of intelligent gas nanovehicles.</p>","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 12","pages":"1691–1697 1691–1697"},"PeriodicalIF":5.1,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850626","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}
ACS Macro LettersPub Date : 2024-11-27DOI: 10.1021/acsmacrolett.4c00687
Zhezhe Li, Yue Zhang, Suzhen Wang, Yihan Wu, Hailong Che
{"title":"Rational Design of Self-Reporting Polymersomes for the Controlled Release of Sulfur Dioxide","authors":"Zhezhe Li, Yue Zhang, Suzhen Wang, Yihan Wu, Hailong Che","doi":"10.1021/acsmacrolett.4c00687","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00687","url":null,"abstract":"As a new member of the gaseous regulators, sulfur dioxide (SO<sub>2</sub>) plays a crucial role in many biological activities. Recent studies have shown that SO<sub>2</sub> is capable of inducing cancer cell apoptosis by regulating intracellular reactive oxygen species (ROS), allowing SO<sub>2</sub> to serve as an efficient therapeutic agent. Although various polymer-based platforms have presented great potential for the controlled release of SO<sub>2</sub>, most of the systems are incapable of monitoring the intracellular generation of SO<sub>2</sub>. In this work we present the rational design of SO<sub>2</sub>-releasing biodegradable polymersomes, accompanied by a self-reporting property. The polymersome consists of a hydrophilic block of poly(ethylene glycol) (PEG) and a hydrophobic segment of poly(trimethylene carbonate) (PTMC)-based SO<sub>2</sub> donors. The polymersomes not only exhibit good SO<sub>2</sub>-releasing performance upon treatment with glutathione (GSH), but can also regulate the fluorescence change of the system, offering a good platform for real-time monitoring of the intracellular production of SO<sub>2</sub>. Significantly, the <i>in vitro</i> and <i>in vivo</i> studies indicate the potential for exploitation of these polymersomes as antitumor agents. We expect that incorporating both the SO<sub>2</sub>-releasing capacity and self-reporting feature within a polymersome system will provide a unique opportunity for the development of intelligent gas nanovehicles.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"258 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142718897","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}
ACS Macro LettersPub Date : 2024-11-26DOI: 10.1021/acsmacrolett.4c0065610.1021/acsmacrolett.4c00656
Ronan J. Flood, Aurélien Thureau and Peter B. Crowley*,
{"title":"A Macrocycle-Mediated Protein Cage","authors":"Ronan J. Flood, Aurélien Thureau and Peter B. Crowley*, ","doi":"10.1021/acsmacrolett.4c0065610.1021/acsmacrolett.4c00656","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00656https://doi.org/10.1021/acsmacrolett.4c00656","url":null,"abstract":"<p >Engineered protein cages are of great interest considering their diverse applications in delivery and catalysis. Here, we describe macrocycle-triggered icosahedral cage assembly of a designed β-propeller. Cage assembly was evidenced by small-angle X-ray scattering and X-ray crystallography.</p>","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 12","pages":"1686–1690 1686–1690"},"PeriodicalIF":5.1,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmacrolett.4c00656","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850828","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}
ACS Macro LettersPub Date : 2024-11-26DOI: 10.1021/acsmacrolett.4c00656
Ronan J. Flood, Aurélien Thureau, Peter B. Crowley
{"title":"A Macrocycle-Mediated Protein Cage","authors":"Ronan J. Flood, Aurélien Thureau, Peter B. Crowley","doi":"10.1021/acsmacrolett.4c00656","DOIUrl":"https://doi.org/10.1021/acsmacrolett.4c00656","url":null,"abstract":"Engineered protein cages are of great interest considering their diverse applications in delivery and catalysis. Here, we describe macrocycle-triggered icosahedral cage assembly of a designed β-propeller. Cage assembly was evidenced by small-angle X-ray scattering and X-ray crystallography.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"20 1","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142718888","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}