Self-Assembly of Light Harvesting Films Using Functional Solvents

这个发现计划将探索一种新的方法，使用生物基溶剂，使有序的聚合物纳米结构适合使用气体膨胀液体（GXL）的光捕获。增材制造的复兴正在进行中，例如3D打印和快速成型。然而，目前的方法太慢，并且不能提供光/能量收集中的新兴应用所需的高性能材料特性。对于这些高性能光捕获涂层和设备，包括光伏发光剂和阳极、光催化涂层和温室薄膜;需要使用地球丰富和友好元素的新纳米颗粒（NP）以及控制其组装成有序结构的新方法。目前，需要多步复杂的化学反应来形成NP，稳定它们，然后将它们附着到表面以形成3D有序结构，控制表面拓扑结构的能力较差。在这些方法中，在各种反应/加工步骤中通常需要溶剂以促进NP分散和沉积。然而，目前的溶剂被认为是VOC，其对于工业用途越来越受管制，同时它们也不提供功能并且对NP自组装过程和沉积的控制非常差。 我们独特的研究计划将研究如何使用绿色生物基溶剂（包括乙酸烷基酯、碳酸酯和乳酸酯）来控制聚合物/NP反应化学和沉积步骤，以增强最终用途的结构和性能。对于NP生长，我们将探索如何使用溶胶-凝胶化学以定向方式生长各种金属醇盐构建块，无论是在溶液中还是从各种2D表面，如石墨烯片。这将需要研究功能溶剂如何协调和稳定这些生长的NP和聚合物-NP组件的物理化学，以及各种金属掺杂剂或量子点纳米晶体如何整合到生长的分子框架中。密度泛函理论（DFT）建模将被用来理解作为溶剂稳定性的函数的生长和组装过程，同时被用来预测掺杂剂/NP集成。将探索将这些构建模块制造成薄膜和涂层，其中材料性能和定向表面拓扑结构可以使用3D制造/打印来控制下一代光捕获涂层的阳光。通过控制制造过程中的UV固化和溶剂/溶质相互作用，我们可以使用这些下一代材料设计适当的结构和表面拓扑。由此产生的薄膜和器件将通过加拿大光源的各种物理化学技术和同步加速器研究来表征光转换和电子传输效应，而DFT将用于研究它们的能量传递过程。

This Discovery program will explore a new methodology using bio-based solvents to make ordered polymer nanostructures suitable for light harvesting using gas-expanded liquids (GXL). A renaissance is underway for additive manufacturing, such as 3D printing and rapid prototyping. However, current approaches are far too slow and do not provide the high performance material properties required for emerging applications in light/energy harvesting. For these high performance light harvesting coatings and devices, including photovoltaic encapsulants and anodes, photocatalytic coatings and greenhouse films; new nanoparticles (NPs) using earth abundant and friendly elements and a new way to control their assembly into ordered structures is required. Currently, multi-step complex chemistries are required to form NPs, stabilize them, then attach them to surfaces to form 3D ordered structures, with a poor ability to control surface topology. In these approaches, a solvent is normally required in the various reaction/processing steps to facilitate NP dispersion and deposition. However, current solvents are considered VOCs, which are becoming increasingly regulated for industrial use, while also they provide no functionality and give very poor control of the NP self-assembly process and deposition. Our unique research program will examine how green bio-based solvents including alkyl acetates, carbonates and lactates can be used to control both the polymer/NP reaction chemistry and deposition steps to enhance the end-use structure and performance. For NP growth, we will explore how sol-gel chemistry can be used to grow a variety of metal alkoxide building blocks in an oriented fashion, both in solution or from various 2D surfaces such as graphene sheets. This will entail examining the physical chemistry of how the functional solvents co-ordinate to and stabilize these growing NPs and polymer-NP assemblies, and how various metal dopants or quantum-dot nanocrystals can be integrated into the growing molecular framework. Density functional theory (DFT) modeling will be used to understand the growth and assembly process as a function of solvent stability, while being used to predict dopant/NP integration. Fabrication of these building blocks into films and coatings will be explored, where the materials performance and oriented surface topology's can control sunlight for next-generation light harvesting coatings using 3D fabrication/printing. By controlling the UV curing and solvent/solute interactions during fabrication, we can design appropriate structures and surface topologies using these next generation materials. The resulting films and devices will be characterized for light conversion and electron transport effects by various physico-chemical techniques and synchotron studies at the Canadian Light Source, while DFT will be used to examine their energy-transfer processes.