Protolife-inspired materials chemistry

制造具有小尺度结构和多组分的新材料预计在传感，存储和释放操作以及受控催化等广泛应用中具有重要意义。小规模结构可能取得重大突破的一个新领域是人工细胞样材料（原始细胞）的形成。这种方法的大部分灵感来自于模拟活细胞的关键方面，尽管有很大程度的简化。我们的方法来解决必要的简化是从富有想象力的场景中汲取灵感，这些场景被认为是早期地球上生命前组织的合理机制。因此，我们受到这些基于原生命的材料组织模型的启发，在实验室中开发新的策略，从而设计和构建具有新特性和功能的化学微室。从某种意义上说，我们的目标是抽象过去的想法，以便为未来开发新技术。我们的工作将推进新技术的制备新型的有组织的微尺度架构，自发地组装从多个组件，并结合在一起时，表现出特殊的功能。拟议的工作有三个主要主题，这将有助于我们制定合理的设计和建设的新类集成材料的基础上，使用生物和非生物成分的人工细胞样微区室的指导方针。这些主题集中在自组装原始细胞的合成，性质和利用，涉及（a）蛋白质聚合物构建块，（B）无机纳米颗粒膜，和（c）无膜微滴。在每一种情况下，我们都打算发现化学结构的新方法，包括在微区室内部和上构建超分子结构以产生类似于细胞骨架基质的软水凝胶，构建外部冠层以控制离子和分子通过膜的扩散，以及在原始细胞内掺入不同的组分以控制反应性。例如，我们打算用封装的纳米颗粒制备原始细胞，这些纳米颗粒可以用于光活化过程，如水分子的分裂。通过将这些过程限制在小规模架构内，我们希望实现新的控制和活动水平，这将为生物启发材料化学的新兴领域提供新的突破。

Making new materials that have small-scale structures and multiple components is expected to be of great importance in a wide range of applications such as sensing, storage and release operations, and controlled catalysis. One new area where small-scale structures could make a significant breakthrough is in the formation of artificial cell-like materials (protocells). Much of the inspiration for this approach comes from mimicking key aspects of the living cell, albeit with a large degree of simplification. Our approach to addressing the necessary simplification is to draw inspiration from imaginative scenarios that are being considered as plausible mechanisms for prebiotic organization on the early Earth. We are therefore inspired by these protolife-based models of materials organization to develop new strategies in the laboratory that will result in the design and construction of chemical micro-compartments with novel properties and functions. In a sense, we aim to abstract ideas about the past in order to develop new technologies for the future. Our work will advance new technologies for the preparation of novel types of organized microscale architectures that are spontaneously assembled from multiple components, and which when combined together exhibit special functions. The proposed work has three main themes that will help us develop guidelines for the rational design and construction of new classes of integrated materials based on artificial cell-like micro-compartments using biological and non-biological components. The themes are focused on the synthesis, properties and utilization of self-assembled protocells involving (a) protein-polymer building blocks, (b) inorganic nanoparticle membranes, and (c) membrane-free micro-droplets. In each case, we intend to discover new methods of chemical construction, including the building of supramolecular structures within and on the micro-compartments to produce soft hydrogels that are similar to the cytoskeletal matrix, building of external coronal layers to control the diffusion of ions and molecules through the membranes, and incorporation of diverse components inside the protocells for controlled reactivity. For example, we intend to prepare protocells with encapsulated nanoparticles that can be exploited in photo-activated processes such as the splitting of water molecules. By confining these processes within small-scale architectures, we expect to achieve new levels of control and activity, which will provide new breakthroughs in the emerging area of bioinspired materials chemistry.