Zi-Xuan Luo, Guo-Qiang Tian, Si-Chong Chen, Gang Wu, Yu-Zhong Wang
{"title":"将聚乳酸无溶剂一步法回收为可用聚合物及其闭环回收能力","authors":"Zi-Xuan Luo, Guo-Qiang Tian, Si-Chong Chen, Gang Wu, Yu-Zhong Wang","doi":"10.1021/acs.macromol.4c01104","DOIUrl":null,"url":null,"abstract":"Due to concerns of environmental pollution and resource shortage related to the fossil fuel-based nondegradable plastics, biomass/biobased degradable polymer materials, especially polylactide (PLA), have received increasing attention in recent years. Although PLA can be depolymerized back to the cyclic monomer lactide, achieving a closed-loop cycle of “polymer-monomer-polymer”, it is very attractive but still a great challenge for recycling PLA to a high-performance polymer through a simple and green strategy suitable for industrialization. Herein, a facile solvent-free one-pot recycling strategy is developed to efficiently convert PLA and end-of-life PLA disposable products into an upgraded PLA-based polymer with enhanced performance. The recycling strategy involves a controlled fast catalytic alcoholysis to prepare a dihydroxyl-terminated PLA oligomer, i.e., PLA-diol, and subsequently a chain extension reaction to obtain PLA-based polyurethane, i.e., PLA–PU. The resulted PLA-diol and PLA–PU with well-defined structures were clearly characterized by <sup>1</sup>H NMR, MALDI-TOF MS, etc. Significantly, the PLA–PU exhibits enhanced mechanical properties that are preferable to those of PLA and can be processed through injection molding, melt spinning, and 3D printing. Besides, PLA–PUs can be directly depolymerized into monomer <span>l</span>-lactide with a high yield under vacuum, revealing its excellent recyclability, which demonstrates a proof of concept for closed-loop recycling from PLA to PLA–PUs and back to PLA. This work opens a potentially new industrial avenue of recycling PLA and other aliphatic polyester plastics.","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":null,"pages":null},"PeriodicalIF":5.1000,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Solvent-Free One-Pot Recycling of Polylactide to Usable Polymers and Their Closed-Loop Recyclability\",\"authors\":\"Zi-Xuan Luo, Guo-Qiang Tian, Si-Chong Chen, Gang Wu, Yu-Zhong Wang\",\"doi\":\"10.1021/acs.macromol.4c01104\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Due to concerns of environmental pollution and resource shortage related to the fossil fuel-based nondegradable plastics, biomass/biobased degradable polymer materials, especially polylactide (PLA), have received increasing attention in recent years. Although PLA can be depolymerized back to the cyclic monomer lactide, achieving a closed-loop cycle of “polymer-monomer-polymer”, it is very attractive but still a great challenge for recycling PLA to a high-performance polymer through a simple and green strategy suitable for industrialization. Herein, a facile solvent-free one-pot recycling strategy is developed to efficiently convert PLA and end-of-life PLA disposable products into an upgraded PLA-based polymer with enhanced performance. The recycling strategy involves a controlled fast catalytic alcoholysis to prepare a dihydroxyl-terminated PLA oligomer, i.e., PLA-diol, and subsequently a chain extension reaction to obtain PLA-based polyurethane, i.e., PLA–PU. The resulted PLA-diol and PLA–PU with well-defined structures were clearly characterized by <sup>1</sup>H NMR, MALDI-TOF MS, etc. Significantly, the PLA–PU exhibits enhanced mechanical properties that are preferable to those of PLA and can be processed through injection molding, melt spinning, and 3D printing. Besides, PLA–PUs can be directly depolymerized into monomer <span>l</span>-lactide with a high yield under vacuum, revealing its excellent recyclability, which demonstrates a proof of concept for closed-loop recycling from PLA to PLA–PUs and back to PLA. This work opens a potentially new industrial avenue of recycling PLA and other aliphatic polyester plastics.\",\"PeriodicalId\":51,\"journal\":{\"name\":\"Macromolecules\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.1000,\"publicationDate\":\"2024-07-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Macromolecules\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.macromol.4c01104\",\"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://doi.org/10.1021/acs.macromol.4c01104","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
Solvent-Free One-Pot Recycling of Polylactide to Usable Polymers and Their Closed-Loop Recyclability
Due to concerns of environmental pollution and resource shortage related to the fossil fuel-based nondegradable plastics, biomass/biobased degradable polymer materials, especially polylactide (PLA), have received increasing attention in recent years. Although PLA can be depolymerized back to the cyclic monomer lactide, achieving a closed-loop cycle of “polymer-monomer-polymer”, it is very attractive but still a great challenge for recycling PLA to a high-performance polymer through a simple and green strategy suitable for industrialization. Herein, a facile solvent-free one-pot recycling strategy is developed to efficiently convert PLA and end-of-life PLA disposable products into an upgraded PLA-based polymer with enhanced performance. The recycling strategy involves a controlled fast catalytic alcoholysis to prepare a dihydroxyl-terminated PLA oligomer, i.e., PLA-diol, and subsequently a chain extension reaction to obtain PLA-based polyurethane, i.e., PLA–PU. The resulted PLA-diol and PLA–PU with well-defined structures were clearly characterized by 1H NMR, MALDI-TOF MS, etc. Significantly, the PLA–PU exhibits enhanced mechanical properties that are preferable to those of PLA and can be processed through injection molding, melt spinning, and 3D printing. Besides, PLA–PUs can be directly depolymerized into monomer l-lactide with a high yield under vacuum, revealing its excellent recyclability, which demonstrates a proof of concept for closed-loop recycling from PLA to PLA–PUs and back to PLA. This work opens a potentially new industrial avenue of recycling PLA and other aliphatic polyester plastics.
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.