The Catalysis (CAT) program creates, controls, integrates and interrogates complex catalytic microenvironments to increase the efficiency of chemical transformations that impact energy processing, utilization and storage. To do so, their teams pursue Multifunctional Catalysts and Catalytic Processes, Cooperative and Evolving Multi-Catalytic Systems, and Catalytic Systems in Confined Spaces. In all cases, CAT researchers monitor processes as they occur by novel spectroscopy at the ALS in specialized reactors and interpret these data and model catalytic intermediates with contemporary theoretical methods.