Protolife-inspired materials chemistry

制造具有小规模结构和多组分的新材料有望在传感、储存和释放操作以及可控催化等广泛应用中发挥重要作用。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(原细胞)的形成。这种方法的大部分灵感来自于模仿活细胞的关键方面，尽管有很大程度的简化。我们解决必要简化的方法是从想象中的情景中获得灵感，这些情景被认为是早期地球上的益生菌组织的合理机制。因此，我们受到这些基于原始生命的材料组织模型的启发，在实验室开发新的策略，从而设计和建造具有新特性和功能的化学微隔室。在某种意义上，我们的目标是抽象过去的想法，以便为未来开发新技术。我们的工作将推动新技术的发展，以制备由多个组件自发组装而成的新型有组织的微型建筑，当它们组合在一起时，会显示出特殊的功能。拟议的工作有三个主要主题，将帮助我们制定指导方针，合理设计和建造基于使用生物和非生物成分的人造细胞状微隔室的新型集成材料。主题集中于自组装原细胞的合成、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，我们都打算发现新的化学结构方法，包括在微格内和微格上建立超分子结构以产生类似于细胞骨架基质的软水凝胶，建立外部冠层来控制离子和分子在膜中的扩散，以及在原细胞内加入不同的成分以控制反应。例如，我们打算用包裹的纳米颗粒制备原始细胞，这种纳米颗粒可以用于光激活过程，如分解水分子。通过将这些过程限制在小规模的建筑中，我们预计将实现新的控制和活动水平，这将在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.