Chen Lin, Han Hu*, Hanxu Zhu, Qingyang Luan, Zhenzhong Li*, Jinggang Wang* and Jin Zhu,
{"title":"二硫化物驱动的PBAT共聚物的按需降解：稳定的综合性能，长期储存，和氧化还原诱导的降解","authors":"Chen Lin, Han Hu*, Hanxu Zhu, Qingyang Luan, Zhenzhong Li*, Jinggang Wang* and Jin Zhu, ","doi":"10.1021/acs.macromol.4c0224410.1021/acs.macromol.4c02244","DOIUrl":null,"url":null,"abstract":"<p >Common biodegradable polyesters are degraded under favorable conditions, such as industrial compost. Poly(butylene adipate-<i>co</i>-terephthalate) (PBAT) is one of the most prospective and prevalent biodegradable polymer, while its degradation in natural environment is slow. Herein, we introduce a stimulus group with disulfide bonds to obtain a poly(butylene adipate-<i>co</i>-dithiodipropionate-<i>co</i>-terephthalate) (PBADiT) copolyester. Their melting temperature is higher than 120 °C and the thermal stability is sufficient for melt processing. They show high modulus (>110 MPa) and high toughness when ≤30% of disulfide bonds are introduced. BDi (butylene dithiodipropionate) units show slightly lower hydrolysis and enzymatic degradation ability, and PBADiT copolymers show acceptable storage stability in a damp environment. The redox response of PBADiT helps realize on-demand degradation after use. From 0.01 to 1 mol/L H<sub>2</sub>O<sub>2</sub> solutions, the hydrolysis of PBADiT can be regulated or accelerated by 15 days of fast hydrolysis with weight loss exceeding 40%. Reductive conditions, represented by 0.2 mol/L dithiothreitol (DTT) solutions, are also an efficient stimulus source for achieving rapid breakage of PBADiT. Hence, PBADiT copolymers provide a new approach for sustainable and degradable materials with required usage time and impart the polymer with accelerated degradation in redox environments.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"58 8","pages":"4170–4182 4170–4182"},"PeriodicalIF":5.2000,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Disulfide-Driven On-Demand Degradation of the PBAT Copolymer: Stable Comprehensive Performance, Long-Term Storage, and Redox-Induced Degradation\",\"authors\":\"Chen Lin, Han Hu*, Hanxu Zhu, Qingyang Luan, Zhenzhong Li*, Jinggang Wang* and Jin Zhu, \",\"doi\":\"10.1021/acs.macromol.4c0224410.1021/acs.macromol.4c02244\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Common biodegradable polyesters are degraded under favorable conditions, such as industrial compost. Poly(butylene adipate-<i>co</i>-terephthalate) (PBAT) is one of the most prospective and prevalent biodegradable polymer, while its degradation in natural environment is slow. Herein, we introduce a stimulus group with disulfide bonds to obtain a poly(butylene adipate-<i>co</i>-dithiodipropionate-<i>co</i>-terephthalate) (PBADiT) copolyester. Their melting temperature is higher than 120 °C and the thermal stability is sufficient for melt processing. They show high modulus (>110 MPa) and high toughness when ≤30% of disulfide bonds are introduced. BDi (butylene dithiodipropionate) units show slightly lower hydrolysis and enzymatic degradation ability, and PBADiT copolymers show acceptable storage stability in a damp environment. The redox response of PBADiT helps realize on-demand degradation after use. From 0.01 to 1 mol/L H<sub>2</sub>O<sub>2</sub> solutions, the hydrolysis of PBADiT can be regulated or accelerated by 15 days of fast hydrolysis with weight loss exceeding 40%. Reductive conditions, represented by 0.2 mol/L dithiothreitol (DTT) solutions, are also an efficient stimulus source for achieving rapid breakage of PBADiT. Hence, PBADiT copolymers provide a new approach for sustainable and degradable materials with required usage time and impart the polymer with accelerated degradation in redox environments.</p>\",\"PeriodicalId\":51,\"journal\":{\"name\":\"Macromolecules\",\"volume\":\"58 8\",\"pages\":\"4170–4182 4170–4182\"},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2025-04-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Macromolecules\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.macromol.4c02244\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"POLYMER SCIENCE\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Macromolecules","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.macromol.4c02244","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
Disulfide-Driven On-Demand Degradation of the PBAT Copolymer: Stable Comprehensive Performance, Long-Term Storage, and Redox-Induced Degradation
Common biodegradable polyesters are degraded under favorable conditions, such as industrial compost. Poly(butylene adipate-co-terephthalate) (PBAT) is one of the most prospective and prevalent biodegradable polymer, while its degradation in natural environment is slow. Herein, we introduce a stimulus group with disulfide bonds to obtain a poly(butylene adipate-co-dithiodipropionate-co-terephthalate) (PBADiT) copolyester. Their melting temperature is higher than 120 °C and the thermal stability is sufficient for melt processing. They show high modulus (>110 MPa) and high toughness when ≤30% of disulfide bonds are introduced. BDi (butylene dithiodipropionate) units show slightly lower hydrolysis and enzymatic degradation ability, and PBADiT copolymers show acceptable storage stability in a damp environment. The redox response of PBADiT helps realize on-demand degradation after use. From 0.01 to 1 mol/L H2O2 solutions, the hydrolysis of PBADiT can be regulated or accelerated by 15 days of fast hydrolysis with weight loss exceeding 40%. Reductive conditions, represented by 0.2 mol/L dithiothreitol (DTT) solutions, are also an efficient stimulus source for achieving rapid breakage of PBADiT. Hence, PBADiT copolymers provide a new approach for sustainable and degradable materials with required usage time and impart the polymer with accelerated degradation in redox environments.
期刊介绍：
Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.
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