基于天然植物资源的绿色高分子复合材料：紧密界面结合力的构筑与增强机制研究

The production route of biodegradable green materials utilizing naturally renewable resources is very helpful to solve problems that we are facing with energy resources and living environment. The idea of using oilseed protein after oil extraction and natural plant fibers, as renewable raw materials, to produce green polymer composites meets the need of sustainable development and recycling economy. Protein derived bio-plastics have been long known for their inferior mechanical performance, and reinforcing fibers can be easily detached from protein matrix, thus failing to act as a load-bearing component in the composite. In this project, in order to improve interface bonding force between protein matrix and reinforcing natural fiber, we design the following new structures: structure of elementary plant fiber/crystalline polymer/protein macromolecules, showing multi-phase synergistic reinforcing effect; structure of surface-modified fiber/plant protein, displaying in situ cross-linking reinforcing effect. Ideally, the resulting composites with either structure would have desirable mechanical properties due to the enhanced bonding force at fiber/protein interfaces. Studies of chemical modification, thermal behavior of polymer chains and composite processing are fundamental issues in this work. The goals after completion of this project, in a timely manner, include: successful synthesis of the green composites in a controllable way, unfolding the reinforcing mechanism to understand the intrinsic relationships between mechanical properties of the material and its hierarchical structure. In addition, this project could pave the road to expanding value-added applications for oilseed protein in non-feed industry, and to green materialization for natural plant fibers in non-textile field.

采用天然可再生资源制备可降解绿色材料的产业化路线有利于解决日益严峻的资源和环境问题。本项目利用榨油后的废弃油籽蛋白资源和天然植物纤维为可再生原料，制备可降解绿色高分子复合材料符合可持续和可循环经济的发展理念。迄今已知的蛋白质基可降解塑料普遍力学强度较差，增强性纤维易从蛋白质基体中脱落。本项目通过构建纤维原纤丝/高分子界面晶体/植物蛋白大分子多相协同增强结构、表面改性纤维/植物蛋白原位交联增强结构，利用结构协同效应和原位增强效应，提高纤维增强相和蛋白质基体之间的结合力，以期获得具有紧密界面结合力的高强度植物纤维/蛋白绿色复合材料。通过化学改性、高分子热响应、复合材料加工等基础研究，实现目标材料的可控合成，并揭示其多层级结构和力学性能之间的调控增强机制。此外，本项目为拓展废弃植物油籽蛋白在非饲料行业的高附加值应用、天然植物纤维在非纺织领域的绿色材料化应用提供理论指导和技术借鉴。

本项目对天然植物资源进行高效转化利用，获得了具有紧密界面结合力、高强度、较好韧性、耐水和耐热稳定性的环境和生态友好型可生物降解类高分子及全绿色聚合物基复合材料。以废弃棉籽蛋白粉为原料，在蛋白质纯化、尿素变性、甘油增塑、改性淀粉交联的基础上，将其与取向排列的天然长纤维或与可降解结晶型高分子（如聚乳酸和聚己内酯）共混复合，采用热压硫化或溶液浇注等加工方法制备得到了一系列生物质基全绿色复合材料。通过设计构建高效原位交联、径向纤维增强、界面晶体桥接、界面增容等增强性结构，创建了蛋白/天然纤维、结晶型高分子/纳米纤维强结合界面和共混增容界面。系统测试评价了复合材料的力学性能、耐水和耐热稳定性能，通过原位扫描电镜-拉伸断裂结构演化实验、界面晶体在纳米纤维表面的等温结晶动力学、改性淀粉对棉籽蛋白的交联效率等实验研究，揭示了纤维多级结构、界面横晶、蛋白/纤维紧密界面等结构与复合材料高强化性能间的构效关系，阐明了纤维断裂机理和复合材料相关增强机制。项目执行期间，共发表学术论著13篇，申请发明专利3项，培养青年教师1名、硕博研究生5名。

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