Determination of Fundamental Structure-Topology-Morphology-Properties for Naturally-derived Recyclable Polymer Materials Designed to Address Environmental and Societal Challenges

第1部分：非技术总结全球塑料污染问题正处于关键时刻。 聚合物材料（塑料）在日常产品中影响社会，促进安全，健康和福利，以及美观，愉悦和便利。 虽然一些塑料材料是耐用的，具有长期稳定性（例如轮胎，汽车塑料部件，头盔等），在初始设计阶段应考虑聚合物的整个寿命周期，以便在材料功能完成后纳入可回收机制。 塑料累积和持久性的负面环境影响正变得越来越重要。 这项工作的预期广泛影响将是天然来源的聚合物材料的进步，这些材料被设计为具有复杂性，使它们表现出独特的性能，并具有解聚和回收的内置机制。 重点将是构建材料，使其表现为超吸收性和坚韧的水凝胶，并将进行严格的研究，以确定聚合物材料的有效性，以满足与全球水资源挑战相关的需求，以及减少摩擦，生物污垢和冰形成的技术挑战。 这项工作的重要成果预计将是未来几代科学家的先进知识和认识，他们将考虑他们开发的技术的整个生命周期。 第二部分：技术概述总体目标是进行基础研究，从而深入了解双共价和非共价的组成-结构-拓扑-形态学效应。（超分子）交联的聚合物材料，其兴趣在于开发衍生自天然原料并被设计为表现出水凝胶、防污、防冰这些材料具有污染物螯合和其他行为，可用于解决社会挑战的各种应用，同时还可回收利用，以限制材料的长期不利环境影响。 葡萄糖将作为主要的结构单元，从该结构单元将构建拓扑复杂的滑动环聚合物网络，具有共价和超分子相互作用以产生动态的、机械稳健的水凝胶行为，进一步延伸到聚合物高内相乳液（polyHIPE）材料以获得超吸收性和高孔隙率。 将进行基础研究，以确定完整材料的性能，然后调查其故意解聚为基础的可回收性和长期水解降解性。 假设对结合共价键、超分子主-客体相互作用、滑动环拓扑结构和聚HIPE形态的联合收割机组分的网络的系统研究将增强对组成-结构-拓扑结构-形态结构-性质关系的基本理解，并导致能够具有超高吸水动力学和容量的先进材料，同时表现出动态，响应的物理化学和机械性能，适用于广泛的应用。 重要的是，将开发利用天然原料和内置解聚和拆卸路线来制造此类材料的技术，以促进可持续性和可回收性。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

PART 1: NON-TECHNICAL SUMMARYThe global plastics pollution problem is at a critical point. Polymer materials (plastics) impact society in everyday products that facilitate safety, health and welfare, and also beauty, pleasure and convenience. Although some plastic materials are meant to be durable and possess long-term stability (e.g. tires, plastic parts for automobiles, helmets, etc.), the full polymer life cycle should be considered during the initial design stages, to incorporate mechanisms for recyclability once the function of the material has been completed. The negative environmental effects of plastic accumulation and persistence are becoming of increasing importance. The expected broad impact of this work will be in the advancement of naturally-derived polymer materials that are designed to possess complexities that allow for them to exhibit unique properties, and have in-built mechanisms for their depolymerization and recycling. A focus will be upon constructing the materials to behave as super-absorbent and tough hydrogels, and rigorous studies will be conducted to determine the effectiveness of the polymer materials to meet needs associated with global water resource challenges, and technological challenges of reducing friction, biofouling, and ice formation. Significant outcomes of this work are expected to be an advanced knowledge and awareness by future generations of scientists who will consider the full life cycle of the technologies that they develop. PART 2: TECHNICAL SUMMARYThe overall objective is to conduct fundamental studies that lead to advanced understanding of the composition-structure-topology-morphology effects for dual covalently and non-covalently (supramolecularly) crosslinked polymer materials, with an interest in developing mechanically-robust functional polymers that are derived from natural feedstocks and designed to exhibit hydrogel, anti-fouling, anti-icing, pollutant sequestering and other behaviors for diverse applications that address societal challenges, while also being recyclable to limit adverse environmental impacts of the materials long-term. Glucose will serve as the primary building block from which topologically-complex slide-ring polymer networks will be constructed, having both covalent and supramolecular interactions to result in dynamic, mechanically-robust hydrogel behaviors, with further extension to polymeric high internal phase emulsion (polyHIPE) materials for superabsorbency and high porosity. Fundamental studies will be performed to determine the properties of the intact materials, followed by investigation of their intentional depolymerization-based recyclability and long-term hydrolytic degradability. It is hypothesized that systematic investigation of networks that combine components of covalent linkages, supramolecular host-guest interactions, slide-ring topology and polyHIPE morphology will enhance the fundamental understanding of composition-structure-topology-morphology-properties relationships and lead to advanced materials that are capable of ultra-high water uptake kinetics and capacity, while exhibiting dynamic, responsive physicochemical and mechanical behaviors for broad applications. Importantly, techniques to build such materials from naturally-sourced feedstocks and with in-built depolymerization and disassembly routes will be developed to advance sustainability and recyclability.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.