Hierarchically Structured Nanocomposites via a “Systems Materials Science” Approach
Hierarchically Structured Nanocomposites via a “Systems Materials Science” Approach
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DOI：
10.1021/accountsmr.2c00153
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发表时间：
2022-11
影响因子：
14.6
通讯作者：
Rebecca L. Li;Carl J. Thrasher;T. Hueckel;R. Macfarlane
中科院分区：
文献类型：
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作者：
Rebecca L. Li;Carl J. Thrasher;T. Hueckel;R. Macfarlane
纳米复合材料可以实现所需的特性，否则无法单组分系统，使他们有吸引力的平台，以精确地调制材料的机械，电磁，热，和光学性能。由于这些属性通常依赖于组成材料的组织，就像它们的相对组成一样，有意编程复合属性需要跨越许多长度尺度的分层结构控制。然而，控制材料的原子、分子、纳米级、微米级和宏观级组成和结构的基本力都是相互关联的，因此必须同时进行操纵以适当地创建理想的设计材料。这种基本的相互依赖性表明，需要一个“系统材料科学”的方法来合理的纳米复合材料的设计。就像“系统生物学”和“系统化学”领域一样，“系统材料科学”的方法将强调从单个组件之间相互作用的复杂网络中产生的紧急连接。在材料合成方面，系统级方法需要考虑多个长度尺度上的结构变化（化学键合，纳米和微观结构的演变，宏观几何形状）在材料合成和加工的所有步骤中相互影响。在这个帐户中，我们强调了我们最近的工作，探索途径，“系统材料科学”的启发设计，通过开发多功能，可编程，和可扩展的纳米复合材料结构单元。我们的小组已经建立了一套聚合物接枝的纳米颗粒设计，这些设计是固有的复合结构，包含具有动态聚合物配体刷的刚性无机核。这些构建模块提供分子和纳米级手柄，通过利用生物分子识别、超分子化学、纳米颗粒合成和一系列不同的加工条件，将颗粒组装成更高级的结构。此外，它们还实现了材料设计的系统级方法，因为它们提供了一种使用纳米到宏观尺度修改材料结构的方法，作为改变分子到纳米级行为的方法。我们概述了指导我们思考复合材料合成的进展，强调了关键的设计图案，并详细说明了反馈和前馈机制如何在多个长度scale.This帐户的内容可以管理结构形成组织的长度scale.The的尺度，从能够指导组装的分子相互作用的检查开始。本节考虑精确性和可伸缩性之间的权衡，最终讨论提供可编程性、组合多功能性和可访问性之间平衡的策略。我们继续描述积木组装的热力学原理，显示如何通过组合物和组装环境来决定所得的纳米结构。此外，我们连接分子和纳米级的设计考虑到更高阶的介观结构（与主尺寸范围从数百纳米到数百微米）。我们讨论的动力学因素控制远程订购和额外的变量，他们叠加在设计和组装技术。在此之后，我们讨论宏观尺度的结构特征，我们强调在处理和操纵这些材料，同时保持或可编程地调制其纳米和微米级的顺序的困难。最后，我们对这些层次结构的相关应用领域进行了研究。
ConspectusNanocomposite materials can achieve desirable characteristics otherwise unavailable to single component systems, making them attractive platforms to precisely modulate a material’s mechanical, electromagnetic, thermal, and optical properties. Because these properties are often dependent on the organization of constituent materials just as much as their relative composition, intentionally programming composite properties requires hierarchical structural control across many length scales. However, the fundamental forces governing the atomic, molecular, nanoscale, microscale, and macroscale composition and structure of a material are all interlinked, and thus must be manipulated simultaneously to properly create ideal designer materials. This fundamental interdependency indicates the need for a “systems materials science” approach to rational nanocomposite design. Much like the fields of “systems biology” and “systems chemistry”, a “systems materials science” approach would emphasize emergent connections arising from complex networks of interactions between individual components. In the context of materials synthesis, a systems-level approach would need to consider how structural changes across multiple length scales (chemical bonding, nano- and microstructural evolution, macroscopic geometry) influence one another during all steps of material synthesis and processing.In this account, we highlight our recent work exploring pathways to “systems materials science” inspired design via the development of versatile, programmable, and scalable nanocomposite building blocks. Our group has established a suite of polymer-grafted nanoparticle designs that are inherently composite architectures, containing rigid inorganic cores with dynamic polymer ligand brushes. These building blocks provide molecular and nanoscale handles to dictate particle assembly into higher-order structures by exploiting biomolecular recognition, supramolecular chemistry, nanoparticle synthesis, and an array of different processing conditions. Moreover, they also enable systems-level approaches to material design, as they provide a means of using nano- to macroscale modifications to material structure as a means of altering molecular to nanoscale behaviors. We outline the advancements that have guided our thinking about composite synthesis, underscore key design motifs, and detail how feedback and feedforward mechanisms can govern structure formation at multiple length scales.The contents of this account are organized by length scale, starting with an examination of molecular interactions capable of guiding assembly. This section considers the trade-offs between precision and scalability, culminating in a discussion of strategies which provide a balance of programmability, compositional versatility, and accessibility. We proceed to describe the thermodynamic principles of building block assembly, showing how the resulting nanostructures can be dictated via both composition and assembly environment. Further, we connect molecular and nanoscale design considerations to higher order mesoscale structures (with principal dimensions ranging from hundreds of nanometers to hundreds of microns). We discuss the kinetic factors controlling long-range ordering and the additional variables they overlay on design and assembly techniques. Following this, we discuss macroscale structural features where we emphasize the difficulty in processing and manipulating these materials while maintaining or programmably modulating their nano- and microscale order. We end with an examination of relevant application areas for these hierarchical …