Heterogeneous catalyst surfaces are known to dynamically reconfigure in response to a reaction with a substrate, owing to electronic changes that take place on substrate binding. Such dynamic behavior is thought to not only assist but be integral to the performance of solid catalysts. This behavior makes catalyst tuning challenging, however: if the active site is changing over the course of ca-talysis, then advanced in situ techniques must be used to probe structure and dynamics, and precisely configuring the catalyst's active site towards improved performance remains challenging. We are currently investigating the potential of multimetallic copper-sulfide nanoclusters to serve as dynamically flexible models for heterogeneous surfaces. We still study how these nanoclusters reconfigure in response to electron transfer and substrate binding in order to promote a function. Ultimately, study of these structures could lead to advanced strategies for promoting multielectron-driven reactions with high efficiency via previously unrecognized pathways of multimetallic cooperativity.