119. (Mater. Horiz.) Green circular design for unmodified lignin: solvent-free valorization into high-performance covalent adaptable networks
作者：Shanshan Dai, Shuaiqi Yang, Shuai Du, Haoyang Jin, Xin Wang, Fengyuan Zhang and Songqi Ma*
關鍵字：熱固性樹脂，木質素，高值利用
論文來源：期刊
具體來源：Materials Horizons
發表時間：2025年
This study presents a solvent- and purification-free solubilisation-cross-linking strategy to valorize industrial lignin waste into covalent adaptable networks (CANs). Unmodified lignin from pulping wastewater undergoes hydrogen bond-driven solubilisation in bio-based 1,3-propanediol (PDO), forming homogeneous solubilised lignin without chemical modification. Subsequent catalyst-free copolymerization with itaconic anhydride (ITA) yields CANs with exceptional mechanical strength (63 MPa), exceeding those of the reported lignin-based CANs and rivaling bisphenol-A epoxies. Ortho-carboxyl groups enable internal catalysis of ester exchange, allowing >74% strength retention after thermal reshaping and selective degradation by PDO for closed-loop oligomer repolymerization. Pre-cross-linked films exhibit strong interfacial bonding to tinplate (7.9 MPa) and wood (4.6 MPa) with heat-triggered debonding. The process avoids volatile organics, metal catalysts, petrochemicals, and purification, achieving 100% atom economy and >98% bio-based content. This work establishes a paradigm for transforming lignin into circular materials that addresses plastic sustainability and biomass valorization.
原文鏈接：http://dx.doi.org/10.1039/D5MH01488C