Generation and Self-Assembly of Novel Polymeric Materials Inspired by Nature

仿生材料领域是建立在这样一个前提上的，即人类可以从大自然中学习一些东西，通过可持续和经济的加工，创造出多种功能的多功能高性能材料。我们的研究项目主要集中在贻贝足丝纤维，由于技术和生物医学相关的材料特性（高韧性，自愈，湿粘合），它为生物启发聚合物提供了一个很好的榜样。我们之前的工作表明，这些特性源于蛋白质构建块的分层组织和蛋白质-金属配位交联。然而，目前对于足跖骨形成过程中如此高度的结构复杂性是如何实现的了解甚少。我们的研究项目的目标是阐明足丝的自组装过程，并利用提取的设计概念来开发仿生材料加工。贻贝足丝纤维是由10种不同的蛋白质自下而上自组装而成的，这些蛋白质在几分钟内经历了从流体前体到坚韧纤维的戏剧性转变。我们最近的工作表明，足丝蛋白储存在微米大小的分泌囊泡中，这些分泌囊泡在一个时空控制的过程中分泌。我们假设囊泡具有可控的微环境（pH值、离子强度和氧化还原电位），当刺激反应蛋白从分泌腺释放到海水中时，囊泡的自组装是通过改变环境条件和机械剪切触发的。我们认为，通过阐明在足丝组装中起作用的时空控制和物理化学原理，我们将获得新的见解，以启发通过超分子组装制造具有先进性能的聚合物材料的可持续实践。在过去7年的工作基础上，我们的主要目标是：1)通过对贻贝足形成的原位和体外研究，阐明贻贝足自组装的物理化学原理。II)通过新型微流体材料加工，将提取的原理应用于具有分层结构的新型聚合物材料的组装。这些目标将通过在化学，生物化学和材料科学的界面上进行多尺度，跨学科的研究，利用尖端的分析技术，包括共聚焦拉曼光谱，聚焦离子束扫描电子显微镜（FIB-SEM）和冷冻透射电子显微镜（TEM）来实现。我们项目的长期目标是生产高分子材料，将高性能与可持续制造实践和循环生命周期相结合。在新兴的绿色科技产业中，这将为加拿大带来切实的经济和环境效益。

The field of bio-inspired materials is founded on the premise that humans can learn something from nature about creating versatile high-performance materials for a wide variety of functions through sustainable and economical processing. Our research program focuses on mussel byssus fibers, which provide an excellent role model for bio-inspired polymers due to technologically and biomedically relevant materials properties (high toughness, self-healing, wet adhesion). Our previous work indicates these properties arise from hierarchical organization of protein building blocks and protein-metal coordination cross-linking. Presently, however, little is understood about how this high degree of structural complexity is achieved during byssus formation. The goals of our research program are to elucidate the byssus self-assembly process and utilize extracted design concepts towards the development of bio-inspired materials processing.Mussel byssus fibers are rapidly fabricated via bottom-up self-assembly of >10 different proteins, which undergo a dramatic transition from fluid precursor to tough fiber in just minutes. Our recent work indicates that byssus proteins are stored in micron-sized secretory vesicles, which are secreted in a spatiotemporally controlled process. We hypothesize that vesicles possess a controlled microenvironment (pH, ionic strength and redox potential) and that self-assembly is triggered via changing ambient conditions and mechanical shear as the stimuli responsive proteins are released from secretory glands into seawater. We posit that by elucidating the spatiotemporal control and physical chemical principles at play in byssus assembly, we will gain new insights for inspiring sustainable practices for fabricating polymeric materials with advanced properties via supramolecular assembly.Building off our group's work over the last 7 years, the primary aims are I) Elucidate physical chemical principles underlying mussel byssus self-assembly through in situ and in vitro investigation of byssus formation. II) Adapt extracted principles towards assembly of novel polymeric materials with hierarchical structure via novel microfluidics-based materials processing. These aims will be achieved through a multi-scale, cross-disciplinary investigation at the interface of chemistry, biochemistry and materials science, utilizing cutting edge analytical techniques including confocal Raman spectroscopy, focused ion beam scanning electron microscopy (FIB-SEM) and cryo-transmission electron microscopy (TEM). The long-term aim of our program is production of polymeric materials that combine high performance with sustainable fabrication practices and circular life cycles. This will have tangible benefits for Canada, both economically and environmentally, in the emerging green technologies industry.