Pub Date : 2026-01-23DOI: 10.1016/j.progpolymsci.2026.102090
Sandra E. Smeltzer, Michael F. Cunningham
{"title":"Design and Use of Amphiphilic Polymers as Stabilizers in (Mini)emulsion Polymerization","authors":"Sandra E. Smeltzer, Michael F. Cunningham","doi":"10.1016/j.progpolymsci.2026.102090","DOIUrl":"https://doi.org/10.1016/j.progpolymsci.2026.102090","url":null,"abstract":"","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"66 1","pages":""},"PeriodicalIF":27.1,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146033791","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-13DOI: 10.1016/j.progpolymsci.2026.102089
Ji Feng , Fabrice Morlet-Savary , Michael Schmitt , Jing Zhang , Xiaotong Peng , Pu Xiao , Jacques Lalevée
In the pursuit of green polymer chemistry, natural sunlight represents the ideal energy source for photopolymerization due to its abundance and sustainability. While the transition from UV to LED light has improved energy efficiency, sunlight-driven photopolymerization offers a transformative path towards power-free and accessible material synthesis. The key challenge is the development of highly sensitive photoinitiating systems (PISs) capable of harnessing the broad solar spectrum. This review provides a comprehensive overview of the state-of-the-art in sunlight-induced photopolymerization. We explore the core photochemical mechanisms and survey the latest developed photoinitiators (PIs) and photocatalysts of versatile organic dyes. We highlight recent milestones where solar-driven systems have achieved polymerization rates comparable to their LED-activated counterparts, showcasing their practical viability. Furthermore, real-world applications in coatings, 3D printing, and biomaterials are discussed through specific case studies. By addressing current challenges and outlining future research directions, this review aims to promote further innovation in the rational design of solar-activated PISs, ultimately unlocking the full potential of sunlight as a cornerstone for sustainable manufacturing.
{"title":"Harnessing solar energy for polymer synthesis: Recent advances in photoinitiators and photocatalysts for natural light-induced photopolymerization","authors":"Ji Feng , Fabrice Morlet-Savary , Michael Schmitt , Jing Zhang , Xiaotong Peng , Pu Xiao , Jacques Lalevée","doi":"10.1016/j.progpolymsci.2026.102089","DOIUrl":"10.1016/j.progpolymsci.2026.102089","url":null,"abstract":"<div><div>In the pursuit of green polymer chemistry, natural sunlight represents the ideal energy source for photopolymerization due to its abundance and sustainability. While the transition from UV to LED light has improved energy efficiency, sunlight-driven photopolymerization offers a transformative path towards power-free and accessible material synthesis. The key challenge is the development of highly sensitive photoinitiating systems (PISs) capable of harnessing the broad solar spectrum. This review provides a comprehensive overview of the state-of-the-art in sunlight-induced photopolymerization. We explore the core photochemical mechanisms and survey the latest developed photoinitiators (PIs) and photocatalysts of versatile organic dyes. We highlight recent milestones where solar-driven systems have achieved polymerization rates comparable to their LED-activated counterparts, showcasing their practical viability. Furthermore, real-world applications in coatings, 3D printing, and biomaterials are discussed through specific case studies. By addressing current challenges and outlining future research directions, this review aims to promote further innovation in the rational design of solar-activated PISs, ultimately unlocking the full potential of sunlight as a cornerstone for sustainable manufacturing.</div></div>","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"175 ","pages":"Article 102089"},"PeriodicalIF":26.1,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145962195","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-09DOI: 10.1016/j.progpolymsci.2026.102087
Hojoon Choi , Yi Sak Noh , Du Yeol Ryu , Yusuke Yamauchi , Chang-Min Yoon , Seung Soo Oh , Jungmok You , Duk Man Yu , Jeonghun Kim
With the global transition towards carbon neutrality, a new hydrogen-centered economy is emerging. Membrane-based water electrolysis has attracted attention as a sustainable method for producing green hydrogen when integrated with renewable energy sources. In these systems, polymer membranes play a key role by selectively transferring ions (protons or hydroxide ions) and preventing gas crossover. Water electrolysis operates under diverse conditions—including high temperature, high pressure, and strongly acidic or alkaline environments—depending on the electrolyzer type. Ensuring long-term membrane durability under such conditions is critical. While commercial proton exchange membranes (PEMs) already demonstrate excellent performance and stability, their reliance on expensive fluorinated polymers motivates ongoing research into cost-effective alternatives. Similar challenges exist for other systems, where chemical stability and cost remain major concerns. This review presents recent developments in polymer-based membranes for a range of electrolysis technologies, including proton exchange, anion exchange, bipolar, and acid-alkaline systems. It highlights the relationship between polymer structures, physicochemical properties, and electrochemical performance. Through this comprehensive overview, we aim to provide practical guidance for future material design and selection in advanced water electrolysis applications.
{"title":"Advanced polymer design and synthesis for high-performance membranes in water electrolysis","authors":"Hojoon Choi , Yi Sak Noh , Du Yeol Ryu , Yusuke Yamauchi , Chang-Min Yoon , Seung Soo Oh , Jungmok You , Duk Man Yu , Jeonghun Kim","doi":"10.1016/j.progpolymsci.2026.102087","DOIUrl":"10.1016/j.progpolymsci.2026.102087","url":null,"abstract":"<div><div>With the global transition towards carbon neutrality, a new hydrogen-centered economy is emerging. Membrane-based water electrolysis has attracted attention as a sustainable method for producing green hydrogen when integrated with renewable energy sources. In these systems, polymer membranes play a key role by selectively transferring ions (protons or hydroxide ions) and preventing gas crossover. Water electrolysis operates under diverse conditions—including high temperature, high pressure, and strongly acidic or alkaline environments—depending on the electrolyzer type. Ensuring long-term membrane durability under such conditions is critical. While commercial proton exchange membranes (PEMs) already demonstrate excellent performance and stability, their reliance on expensive fluorinated polymers motivates ongoing research into cost-effective alternatives. Similar challenges exist for other systems, where chemical stability and cost remain major concerns. This review presents recent developments in polymer-based membranes for a range of electrolysis technologies, including proton exchange, anion exchange, bipolar, and acid-alkaline systems. It highlights the relationship between polymer structures, physicochemical properties, and electrochemical performance. Through this comprehensive overview, we aim to provide practical guidance for future material design and selection in advanced water electrolysis applications.</div></div>","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"174 ","pages":"Article 102087"},"PeriodicalIF":26.1,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-08DOI: 10.1016/j.progpolymsci.2026.102088
Jake Molineux , Kyung-Jo Kim , Arooj Gul , Sam W. Durfee , Robert A. Norwood , Jeffrey Pyun
Despite the ubiquity of commodity plastics for optical glass in modern society, there remains a need for scholarly delineation of key structure-property relationships to develop new robust, transparent glassy polymers for low-cost, high volume plastic optics. We review the most important synthetic commodity polymers applicable for plastic optical glass applications, herein, referred to as plastic glass, with an emphasis on defining the structure-property correlations required to retain high optical transparency. Furthermore, we discuss the critical need for methods to quantify optical transparency for bulk thick plastic glass materials beyond the current state-of-the-art thin film refractive index measurements, which often do not translate to optical properties in thick bulk glass. We discuss the requirements for measurement of optical transparency in high quality, bulk glass samples via quantification of optical absorption coefficients (α-values) across the visible-infrared (VIS-IR) spectrum (or the specific wavelengths of interest). Reported values for optical absorption coefficients using reproducible protocols remain difficult to find in the modern literature, even for established commodity plastic optics. Hence, we review the methods to determine optical absorption coefficients and properly correct for Fresnel reflection in transmission measurements to enable accurate comparison of different optical materials. The application of this measurement and analysis for determining optical transparency is anticipated to be an essential aspect for the development of next generation commodity plastic glass which remains challenging due to the need for a suite of features to converge, namely low cost, outstanding bulk material properties and manufacturability.
{"title":"Plastic optical glass as a critical material for optics and photonics","authors":"Jake Molineux , Kyung-Jo Kim , Arooj Gul , Sam W. Durfee , Robert A. Norwood , Jeffrey Pyun","doi":"10.1016/j.progpolymsci.2026.102088","DOIUrl":"10.1016/j.progpolymsci.2026.102088","url":null,"abstract":"<div><div>Despite the ubiquity of commodity plastics for optical glass in modern society, there remains a need for scholarly delineation of key structure-property relationships to develop new robust, transparent glassy polymers for low-cost, high volume plastic optics. We review the most important synthetic commodity polymers applicable for plastic optical glass applications, herein, referred to as plastic glass, with an emphasis on defining the structure-property correlations required to retain high optical transparency. Furthermore, we discuss the critical need for methods to quantify optical transparency for bulk thick plastic glass materials beyond the current state-of-the-art thin film refractive index measurements, which often do not translate to optical properties in thick bulk glass. We discuss the requirements for measurement of optical transparency in high quality, bulk glass samples via quantification of optical absorption coefficients (α-values) across the visible-infrared (VIS-IR) spectrum (or the specific wavelengths of interest). Reported values for optical absorption coefficients using reproducible protocols remain difficult to find in the modern literature, even for established commodity plastic optics. Hence, we review the methods to determine optical absorption coefficients and properly correct for Fresnel reflection in transmission measurements to enable accurate comparison of different optical materials. The application of this measurement and analysis for determining optical transparency is anticipated to be an essential aspect for the development of next generation commodity plastic glass which remains challenging due to the need for a suite of features to converge, namely low cost, outstanding bulk material properties and manufacturability.</div></div>","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"174 ","pages":"Article 102088"},"PeriodicalIF":26.1,"publicationDate":"2026-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145920472","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-06DOI: 10.1016/j.progpolymsci.2026.102079
Leiqing Hu , Yang Jiao , Gengyi Zhang , Jianyu Guan , Vinh T. Bui , Haiqing Lin
Carbon molecular sieves (CMSs), derived from the pyrolysis of polymeric precursors, have emerged as an attractive materials platform for molecular separations, as they exhibit polymodal pore structures featuring bottlenecks with strong size-sieving ability and microcavities with high molecular permeability. This review provides a comprehensive and critical examination of the microporous structures and molecular separation properties of CMSs derived from advanced polymers, including polyimides, polymers of intrinsic microporosity, and polybenzimidazoles, as well as hierarchical polymeric architectures, such as polymer blends, cross-linked polymers, and mixed-matrix materials containing nanofillers. The effects of carbonization protocols and post-modification with nanotechnologies on molecular separation properties are exhaustively described. We elucidate the relationships between their structures and separation properties and derive upper bounds using an activated diffusion model. The challenges and opportunities for practical membrane applications are outlined to inform the design of advanced carbon materials for a broad range of separations.
{"title":"Polymer-derived carbon molecular sieves with tailored polymodal pores for membrane separations","authors":"Leiqing Hu , Yang Jiao , Gengyi Zhang , Jianyu Guan , Vinh T. Bui , Haiqing Lin","doi":"10.1016/j.progpolymsci.2026.102079","DOIUrl":"10.1016/j.progpolymsci.2026.102079","url":null,"abstract":"<div><div>Carbon molecular sieves (CMSs), derived from the pyrolysis of polymeric precursors, have emerged as an attractive materials platform for molecular separations, as they exhibit polymodal pore structures featuring bottlenecks with strong size-sieving ability and microcavities with high molecular permeability. This review provides a comprehensive and critical examination of the microporous structures and molecular separation properties of CMSs derived from advanced polymers, including polyimides, polymers of intrinsic microporosity, and polybenzimidazoles, as well as hierarchical polymeric architectures, such as polymer blends, cross-linked polymers, and mixed-matrix materials containing nanofillers. The effects of carbonization protocols and post-modification with nanotechnologies on molecular separation properties are exhaustively described. We elucidate the relationships between their structures and separation properties and derive upper bounds using an activated diffusion model. The challenges and opportunities for practical membrane applications are outlined to inform the design of advanced carbon materials for a broad range of separations.</div></div>","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"174 ","pages":"Article 102079"},"PeriodicalIF":26.1,"publicationDate":"2026-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145975057","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-03DOI: 10.1016/j.progpolymsci.2026.102080
Zhangyong Si , Mary B. Chan-Park
Antimicrobial resistance has escalated into a critical global health threat, with multidrug-resistant bacteria and fungi undermining the effectiveness of conventional small-molecule antibiotics. Antimicrobial polymers have emerged as a versatile class of antimicrobials, offering structural modularity, tunable physicochemical properties and biological activity. This review summarizes recent advances in peptide-mimetic polymers, glycosylated polymers, main-chain cationic polymers, non-charged polymers, polymer-drug combinations, as well as their diverse uptake pathways and killing mechanisms, with a focus on translationally relevant design principles. Key strategies include backbone engineering and polymeric-drug combinations to maximize antimicrobial efficacy without compromising host compatibility; glycosylation and non-charged polymers to enhance stability and bioavailability; fully degradable designs to ensure safety and environmental sustainability; and engineering polymers with diverse uptake pathways and multi-target mechanisms that enable effective activity against multidrug-resistant pathogens and minimize the risk of resistance development. Advances in controlled polymerization and modular synthesis address the challenges of scalability, reproducibility, and regulatory compliance. Moreover, the integration of AI-guided rational molecular design, high-throughput library synthesis, and rapid platforms for biological activity evaluation is expected to accelerate the discovery and clinical translation of antimicrobial polymers.
{"title":"Recent advances in designing antimicrobial polymers with diverse uptake and killing mechanisms","authors":"Zhangyong Si , Mary B. Chan-Park","doi":"10.1016/j.progpolymsci.2026.102080","DOIUrl":"10.1016/j.progpolymsci.2026.102080","url":null,"abstract":"<div><div>Antimicrobial resistance has escalated into a critical global health threat, with multidrug-resistant bacteria and fungi undermining the effectiveness of conventional small-molecule antibiotics. Antimicrobial polymers have emerged as a versatile class of antimicrobials, offering structural modularity, tunable physicochemical properties and biological activity. This review summarizes recent advances in peptide-mimetic polymers, glycosylated polymers, main-chain cationic polymers, non-charged polymers, polymer-drug combinations, as well as their diverse uptake pathways and killing mechanisms, with a focus on translationally relevant design principles. Key strategies include backbone engineering and polymeric-drug combinations to maximize antimicrobial efficacy without compromising host compatibility; glycosylation and non-charged polymers to enhance stability and bioavailability; fully degradable designs to ensure safety and environmental sustainability; and engineering polymers with diverse uptake pathways and multi-target mechanisms that enable effective activity against multidrug-resistant pathogens and minimize the risk of resistance development. Advances in controlled polymerization and modular synthesis address the challenges of scalability, reproducibility, and regulatory compliance. Moreover, the integration of AI-guided rational molecular design, high-throughput library synthesis, and rapid platforms for biological activity evaluation is expected to accelerate the discovery and clinical translation of antimicrobial polymers.</div></div>","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"174 ","pages":"Article 102080"},"PeriodicalIF":26.1,"publicationDate":"2026-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145893804","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.progpolymsci.2026.102078
Biswajit Saha , Srutashini Das , Quentin Michaudel
To help guide future synthetic efforts toward advanced polymers with enhanced performance across uncharted chemical space, this review introduces the concept of “macroisostere” design, in which functional groups in high-commodity polymers are replaced with structurally analogous motifs. As a case study, we focus on the nascent family of sulfonyl (–SO2–)-containing polymers as “macroisosteres” of traditional carbonyl (–CO–)-based macromolecules. Historically, this class of polymers has remained largely underexplored due to limited synthetic accessibility compared to their carbonyl counterparts. The advent of Sulfur(VI) Fluoride Exchange (SuFEx) click chemistry has changed this landscape, enabling the efficient synthesis and systematic study of sulfonyl polymers and their physicochemical properties. In this review, we contrast classical synthetic routes with SuFEx-based strategies, showcasing how this powerful click chemistry provides access to materials with tunable properties including thermal, mechanical, and optoelectronic behaviors alongside sustainability. We also highlight the unique opportunities SuFEx offers for precision polymer synthesis, including the construction of macromolecules with chiral backbones arising from stereogenic S(VI) centers and the development of sequence-controlled architectures and post-polymerization modifications enabled by the orthogonality of SuFEx relative to other click reactions.
{"title":"From carbonyl to sulfonyl: Unlocking advanced polymers with SuFEx-enabled “macroisosteres”","authors":"Biswajit Saha , Srutashini Das , Quentin Michaudel","doi":"10.1016/j.progpolymsci.2026.102078","DOIUrl":"10.1016/j.progpolymsci.2026.102078","url":null,"abstract":"<div><div>To help guide future synthetic efforts toward advanced polymers with enhanced performance across uncharted chemical space, this review introduces the concept of “macroisostere” design, in which functional groups in high-commodity polymers are replaced with structurally analogous motifs. As a case study, we focus on the nascent family of sulfonyl (–SO<sub>2</sub>–)-containing polymers as “macroisosteres” of traditional carbonyl (–CO–)-based macromolecules. Historically, this class of polymers has remained largely underexplored due to limited synthetic accessibility compared to their carbonyl counterparts. The advent of Sulfur(VI) Fluoride Exchange (SuFEx) click chemistry has changed this landscape, enabling the efficient synthesis and systematic study of sulfonyl polymers and their physicochemical properties. In this review, we contrast classical synthetic routes with SuFEx-based strategies, showcasing how this powerful click chemistry provides access to materials with tunable properties including thermal, mechanical, and optoelectronic behaviors alongside sustainability. We also highlight the unique opportunities SuFEx offers for precision polymer synthesis, including the construction of macromolecules with chiral backbones arising from stereogenic S(VI) centers and the development of sequence-controlled architectures and post-polymerization modifications enabled by the orthogonality of SuFEx relative to other click reactions.</div></div>","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"174 ","pages":"Article 102078"},"PeriodicalIF":26.1,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145893809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Amid growing concerns about dwindling fossil fuel reserves, the development and utilization of sustainable resources have emerged as urgent global priorities. Lignocellulosic biomass, primarily composed of lignin and carbohydrates, holds great promise as a renewable feedstock for the production of bio-based chemicals, fuels, and materials, thereby reducing our reliance on fossil fuels. However, extensive lignin-carbohydrate interactions (LCIs) significantly contribute to the recalcitrance of lignocellulosic biomass, obstructing its efficient fractionation and conversion. Understanding these interactions is critical to comprehensively grasping the mechanisms of intrinsic recalcitrance and formulating strategies to overcome it. In this review, we present an in-depth overview of LCIs, emphasizing the importance of elucidating these interactions to enhance lignocellulose utilization. Unlike previous reviews, we explore both lignin-carbohydrate covalent interactions (LCCIs)—including benzyl ether (BE), γ-ester (GE), and phenyl glycoside (PG) linkages—and lignin-carbohydrate non-covalent interactions (LCNCIs), such as those between lignin and cellulose, as well as lignin and hemicellulose. In addition, we discuss methods for modulating both LCNCIs and LCCIs to improve lignocellulose utilization. Lastly, this review identifies existing challenges and future opportunities in uncovering LCIs, aiming to guide research towards a more comprehensive understanding of the LCI network. The goal is to assist in unleashing the full potential of lignocellulosic biomass across diverse fields, while promoting efficient, environmentally sustainable, and economically viable applications. This review will catalyze deeper scientific engagement with LCIs and inspire innovative strategies for the optimal utilization of lignocellulosic biomass.
{"title":"Revealing the molecular interactions between lignin and carbohydrates towards improved lignocellulose utilization","authors":"Shixu Yu , Yucheng Hu , Tingting Cao, Yutong Zhu, Haichao Li, Tingting You, Feng Xu","doi":"10.1016/j.progpolymsci.2025.102070","DOIUrl":"10.1016/j.progpolymsci.2025.102070","url":null,"abstract":"<div><div>Amid growing concerns about dwindling fossil fuel reserves, the development and utilization of sustainable resources have emerged as urgent global priorities. Lignocellulosic biomass, primarily composed of lignin and carbohydrates, holds great promise as a renewable feedstock for the production of bio-based chemicals, fuels, and materials, thereby reducing our reliance on fossil fuels. However, extensive lignin-carbohydrate interactions (LCIs) significantly contribute to the recalcitrance of lignocellulosic biomass, obstructing its efficient fractionation and conversion. Understanding these interactions is critical to comprehensively grasping the mechanisms of intrinsic recalcitrance and formulating strategies to overcome it. In this review, we present an in-depth overview of LCIs, emphasizing the importance of elucidating these interactions to enhance lignocellulose utilization. Unlike previous reviews, we explore both lignin-carbohydrate covalent interactions (LCCIs)—including benzyl ether (BE), <em>γ</em>-ester (GE), and phenyl glycoside (PG) linkages—and lignin-carbohydrate non-covalent interactions (LCNCIs), such as those between lignin and cellulose, as well as lignin and hemicellulose. In addition, we discuss methods for modulating both LCNCIs and LCCIs to improve lignocellulose utilization. Lastly, this review identifies existing challenges and future opportunities in uncovering LCIs, aiming to guide research towards a more comprehensive understanding of the LCI network. The goal is to assist in unleashing the full potential of lignocellulosic biomass across diverse fields, while promoting efficient, environmentally sustainable, and economically viable applications. This review will catalyze deeper scientific engagement with LCIs and inspire innovative strategies for the optimal utilization of lignocellulosic biomass.</div></div>","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"173 ","pages":"Article 102070"},"PeriodicalIF":26.1,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145771226","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-13DOI: 10.1016/j.progpolymsci.2025.102069
Song Gu , Baoming Zhao , Gustavo de Figueiredo Brito , Li Chen , Jinwen Zhang
Thermosetting polymers and their fiber-reinforced composites are widely used in engineering structures due to their superior thermal and mechanical properties, chemical resistance, and high specific strength and stiffness. However, their densely covalent crosslinked networks present trade-offs between degradation efficiency, selectivity, and scalability for end-of-life recycling, which hinder the retention and reuse of material value. As production and in-service stock continue to grow, end-of-life waste streams are rapidly expanding, exacerbating environmental burdens and the loss of high-value resources. Recycling of thermosets and their composites has therefore become a pressing challenge. This review focuses on the concept of selective bond cleavage strategies and examines two complementary pathways: end-based recycling, which targets the selective deconstruction of existing thermosets and composites, and source-based recycling, which involves designing new resin systems with built-in recyclability. It discusses hydrolysis, alcoholysis, aminolysis, ammonolysis, hydrazinolysis and acidolysis of ester, urea and imide linkages, as well as degradation mediated by strong bases, Lewis and Brønsted acids, and transition metals that cleave CO, CN and CC bonds. The design principles of cleavable or dynamic motifs, together with reversible polymerization and on-demand depolymerization in recyclable thermosets are also summarized. Through a comparative literature analysis, we highlight the trade-off between degradation efficiency and selectivity in end-based recycling and the balance among service performance, processability and deconstruction efficiency in source-based recycling. An application-oriented framework centered on selective deconstruction and efficient reconstruction is proposed, emphasizing the critical roles of mass/heat transfer, solvent and phase behavior, separation and reutilization, process intensification and scale-up, and system-level techno-economic analysis and life cycle assessment. Finally, we outline the key challenges and future directions for bridging laboratory-scale research with engineering practice and industrial implementation.
{"title":"Selective bond cleavage strategies for chemical recycling of thermosets and their composites","authors":"Song Gu , Baoming Zhao , Gustavo de Figueiredo Brito , Li Chen , Jinwen Zhang","doi":"10.1016/j.progpolymsci.2025.102069","DOIUrl":"10.1016/j.progpolymsci.2025.102069","url":null,"abstract":"<div><div>Thermosetting polymers and their fiber-reinforced composites are widely used in engineering structures due to their superior thermal and mechanical properties, chemical resistance, and high specific strength and stiffness. However, their densely covalent crosslinked networks present trade-offs between degradation efficiency, selectivity, and scalability for end-of-life recycling, which hinder the retention and reuse of material value. As production and in-service stock continue to grow, end-of-life waste streams are rapidly expanding, exacerbating environmental burdens and the loss of high-value resources. Recycling of thermosets and their composites has therefore become a pressing challenge. This review focuses on the concept of selective bond cleavage strategies and examines two complementary pathways: end-based recycling, which targets the selective deconstruction of existing thermosets and composites, and source-based recycling, which involves designing new resin systems with built-in recyclability. It discusses hydrolysis, alcoholysis, aminolysis, ammonolysis, hydrazinolysis and acidolysis of ester, urea and imide linkages, as well as degradation mediated by strong bases, Lewis and Brønsted acids, and transition metals that cleave C<img>O, C<img>N and C<img>C bonds. The design principles of cleavable or dynamic motifs, together with reversible polymerization and on-demand depolymerization in recyclable thermosets are also summarized. Through a comparative literature analysis, we highlight the trade-off between degradation efficiency and selectivity in end-based recycling and the balance among service performance, processability and deconstruction efficiency in source-based recycling. An application-oriented framework centered on selective deconstruction and efficient reconstruction is proposed, emphasizing the critical roles of mass/heat transfer, solvent and phase behavior, separation and reutilization, process intensification and scale-up, and system-level techno-economic analysis and life cycle assessment. Finally, we outline the key challenges and future directions for bridging laboratory-scale research with engineering practice and industrial implementation.</div></div>","PeriodicalId":413,"journal":{"name":"Progress in Polymer Science","volume":"173 ","pages":"Article 102069"},"PeriodicalIF":26.1,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145753338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-11DOI: 10.1016/j.progpolymsci.2025.102068
Haocong Shi, Mengtao Wang, Chaoying Wan
Polymers are viscoelastic materials, associated with hierarchical dynamics of chain motion, which is time- and temperature-dependent. The viscoelastic properties are influenced by a number of structural parameters, such as chemical composition, molecular weight, entanglement, molecular topology, phase morphology, the degree of crystallinity, network structures and/or polymer-filler interactions. With the increasing complexities of polymer systems, and the demands for new functions, such as self-healing and stimuli-responsiveness, understanding and quantifying the polymer dynamic behavior is a prerequisite for effective polymer design. Rheology is an efficient and powerful technique in quantifying the viscoelastic behavior of polymer systems across a wide range of time and length scales. Generally, rheology is subdivided into (1) shear and elongation rheology (2) time-dependent, e.g. oscillatory or stationary deformation, and (3) deformation in the linear or non-linear regime. Small amplitude oscillatory shear (SAOS) is perhaps the most commonly used experimental technique to reveal relationships among dynamic moduli (G’, G’’), tan(δ) = G’’/G’, and relaxation (relaxation time τ and related activation energy Ea). Among these properties, the frequency-dependent phase angle δ (ω), which quantifies the phase lag between input strain and output stress, is of high information content. We highlight δ (ω) and δ (|G*|) (the latter is commonly known as van Gurp-Palmen plot), a key rheological signature in differentiation of multiscale polymer architectures. The δ versus |G*| relationship is also explored to validate time–temperature superposition (TTS), offering insights into polymer topology and phase morphology, as well as providing the foundation for nonlinear rheology and transient network design. We reviewed the application of phase angle (δ) in linear shear rheology analysis, through examples of different polymer chain topology (e.g. long-chain branching), phase morphology, entanglements, crystalline, crosslinks and polymer nanocomposites, to provide new insights and help understand the multiscale structure-dynamics relationships in polymer systems.
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