文献类型：期刊文献

英文题名：Hydrolyzable Bio-Based Bisphenols Enabled by the Tishchenko Reaction for Polyurethane Vitrimers with Closed-Loop Recyclability

作者：Wang, Jiewen[1];Qiang, Hongru[1];Huang, Rong[1];Zhao, Dan[1];Tong, Zihan[1];Fan, Zhen[1];Du, Jianzhong[2,3,4];Zhu, Yunqing[1]

机构：[1]Tongji Univ, Sch Mat Sci & Engn, Dept Polymer Mat, Shanghai 201804, Peoples R China;[2]Tongji Univ, Shanghai Peoples Hosp 4, Translat Res Inst Brain & Brain Like Intelligence, Dept Gynaecol & Obstet,Shanghai Key Lab Anesthesio, Shanghai 200434, Peoples R China;[3]Tongji Univ, Sch Mat Sci & Engn, Key Lab Adv Civil Engn Mat, Minist Educ, 4800 Caoan Rd, Shanghai 201804, Peoples R China;[4]East China Univ Sci & Technol, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China

年份：2025

卷号：12

期号：26

外文期刊名：ADVANCED SCIENCE

收录：;EI(收录号：20251518229576);WOS:【SCI-EXPANDED(收录号:WOS:001463451700001)】；

基金：This work was supported by National Natural Science Foundation of China (22335005, 22175131, 22475154 and 21925505), the National Key R&D Program of China (2022YFC2402900), Innovation Program of Shanghai Municipal Education Commission (2023ZKZD28), and the Interdisciplinary Collaborative Research Project of Tongji University (2023-2-YB-03) and Tongcheng Youth Research and Development Fund (CPCIF-RA-0104). J.D. is a recipient of National Science Fund for Distinguished Young Scholars.

语种：英文

外文关键词：biobased bisphenols; closed-loop recyclability; green chemistry; renewable resources; vitrimer

摘要：Polyurethane (PU) is a cornerstone of modern materials science, yet its reliance on petroleum-based precursors and the limited recyclability of conventional formulations pose significant environmental challenges. In this study, a fully bio-based polyurethane vitrimer system is developed enabled by a dual-function SmI2-mediated strategy that integrates Tishchenko coupling and phenol deprotection in a single step, simplifying the synthesis of bio-based bisphenols with 100% atom utilization. These bisphenols introduce hydrolyzable ester bonds, allowing for complete degradation within approximate to 3 d (representative model), providing an efficient and eco-friendly end-of-life solution. This approach offers a sustainable alternative to conventional bisphenol A (BPA). Moreover, by leveraging the electronic effects of bio-based bisphenols, the dissociation temperature of phenol-carbamate bonds can be widely tuned (approximate to 70-120 degrees C), endowing the resulting Covalent Adaptable Network (CAN) PUs with excellent reprocessability, closed-loop recyclability, and reconfigurable shape memory capability. Furthermore, the aromatic and ester-rich structure enhances thermomechanical performance, yielding tensile strengths up to 33 MPa, elongations at break exceeding 400%, and toughness reaching 30 MJ m-3, surpassing most sustainable PUs. This work pioneers a scalable and fully bio-based PU vitrimer platform with tunable performance, recyclability, and sustainable degradability, offering a compelling alternative to traditional thermosets and thermoplastics for next-generation green materials.