Systematic Design of Porous Heterogeneous Hierarchical Materials and Structures to Optimize Reactive Transport Processes

当今的许多高性能材料都需要具有多种功能，才能最有效地用于各种反应性传输应用，例如燃料升级的催化剂、二氧化碳捕获的吸附剂、电池的电极、水处理的膜或生物医学应用的抗菌剂。所需的材料系统通常是不同材料（异质）的组合，放置在整个系统的特定位置（分层），具有受控的孔隙、通道和活性颗粒。传统上，这种材料是为主要功能而设计的，例如运输效率，而只考虑密度或强度等其他特性。通过将严格的计算和实验方法相结合，将开发一种新的设计方法，该方法将考虑材料性能以及制造和结构方面，从而为特定应用的材料系统提供全面的性能定制。在这个项目中开发的设计框架不是特定于一种材料，因此将在生物医学应用到能源系统的许多复杂材料系统中具有深远的应用。为了实现反应输运过程中多孔非均质分层材料设计的范式转变，pi开发了一种集成的计算和实验方法。这些材料包括一个有机和/或无机支架，其设计具有孔隙度、弯曲度和颗粒大小的多层次和分布，并以活性位点（通常是纳米级无机化合物）装饰，这些活性位点可以在支架“构建”期间或之后加入。pi将使用材料信息学来开发和分析属性-结构关系，以确定合适的支架和活性位点材料。作为典型设计过程的根本转变，他们还将考虑材料系统结构的设计。一种新的基于实验设计（DOE）的方法将被用于优化多孔材料的结构和活性位点分布，该方法结合了通过预测材料系统的多孔反应传输的计算流体动力学研究。作为该设计方法的一个组成部分，pi将开发一种DOE方法来制造多孔非均质分层材料，该方法在设计方面计算最佳，同时仍可物理制造。该计算设计框架将以可再生燃料升级为样本应用进行实验验证，首先是甲烷重整，然后是异质生物质热解生物燃料。

Many of today's high performance materials are required to perform multiple functions to be most effective for a variety of reactive transport applications such as catalysts for fuel upgrading, adsorbents for carbon dioxide capture, electrodes for batteries, membranes for water treatment or anti-bacterial agents for biomedical applications. The required material systems are often combinations of different materials (heterogeneous) placed at specific locations throughout the system (hierarchical) with controlled pores, channels and active particles. Traditionally such a material is designed for a primary function, such as transport efficiency, with only secondary consideration of other properties such as density or strength. By coupling rigorous computational and experimental methods, a new design approach will be developed that considers both the material properties along with fabrication and structural aspects allowing for the comprehensive tailoring of properties for the materials system for a specific application. The design framework developed in this project is not specific for one material so will have far reaching applications for many complex materials systems for use in biomedical applications to energy systems.To enable a paradigm shift in the design of porous heterogeneous hierarchical materials for reactive transport processes, the PIs have developed an integrated computational and experimental approach. The materials comprise an organic and/or inorganic scaffold designed with multiple levels and distributions of porosities, tortuosities and particle sizes, which are decorated with active sites, often nanoscale inorganic compounds, that can be incorporated during or after "construction" of the scaffold. The PIs will employ materials informatics for the development and analysis of property-structure relationships for materials identification of appropriate scaffold and active site materials. As a fundamental shift from the typical design process, they will also consider the design of the structure of the materials system. A novel design of experiments (DOE) based methodology will be used to optimize the porous materials architecture and active site distribution by integrating computational fluid dynamics studies on the porous reactive transport through the projected material systems. As an integral part of this design methodology, the PIs will develop a DOE approach to the fabrication of porous heterogeneous hierarchical materials that is computationally optimal in terms of design while still being physically manufacturable. This computational design framework will be experimentally validated using renewable fuel upgrading as a sample application, beginning with methane reforming, then with heterogeneous biomass pyrolysis biofuels.