Catalytic processes are relied upon globally for trillions of dollars per year of industry. The conversion of oil to gasoline, transformation of natural gas and nitrogen into fertilizer, and conversion of un-burnt fuels into less harmful gasses in the tail pipes of cars all rely on solid state catalysts. Increasing demands for efficient, environmentally friendly chemical processes, in concert with the push to utilize emerging natural resources, rely on the development novel catalytic materials and processes. We use principles from chemical engineering, materials science, physical chemistry and solid-state physics to engineer catalytic reactions towards these goals. We develop molecular level insights into governing phenomena of catalytic reactions by coupling quantum chemical calculations with an array of experimental and characterization techniques. Mechanistic insights are utilized to guide the synthesis of catalysts with targeted geometries, compositions and architectures.