Catalysis is the science and engineering of making chemical reactions go faster and more selectively toward the desired products. This project aims to design new catalysts for an important class of chemical reactions known as selective oxidation. Catalytically active metal nanoparticles will be encapsulated within metal-organic framework (MOF) crystals. Enshrouding metal nanoparticles within MOFs prevents their agglomeration and allows control over reactant access to their surfaces. However, there are an enormous number of metal nanoparticle and MOF types that could be chosen. Molecular-level modeling will, therefore, guide the selection and synthesis of appropriate metal surfaces and MOF channels so that the resulting materials have the desired properties. The objectives of this project are 1) to develop new ways of synthesizing heterogeneous catalyst materials with structural control ranging from the atomic level to the particle level and 2) to demonstrate how new levels of synthetic control, combined with predictive molecular-level modeling, can drastically decrease the development time of new catalytic materials.