The seed effort carried out by the groups of Rodríguez-López and Bhargava will address a new concept in electrocatalyst design that utilizes ultra-thin 2D electrodes as electronically-transparent substrates, Figure 1. The purpose is to enable unprecedented catalyst-catalyst interactions at atomic scales via the resulting heterostructure for exploring new strategies to control interfacial electrochemical reactivity. In the proposed scheme, high-quality large-area graphene electrodes act simultaneously as electrocatalytic supports, molecular templates, and ultra-thin separators that will enable electronic interactions between dissimilar metals, or metals and adsorbed molecular catalysts. We will target reactions of high interest to the community, such as the oxygen reduction reaction, which is involved in fuel cell, electrolyzer, battery, and sensor technologies. Our effort will also explore the fundamental aspects of electron transfer across this new type of interfaces. Synergizing scanning electrochemical microscopy and nano-IR and Raman spectroscopic imaging tools in the PI’s laboratories, we will gain a unique perspective of this new platform by exploring the electronic perturbations driving reactivity and mapping the formation of active reaction intermediates in situ. Collaboration with the Huang and van der Zande groups will enable us to access atomic-scale sample characterization and atomic-scale control of the sample morphology, and offering in exchange a new toolset, an interdisciplinary approach, and new concepts in catalysis to the I-MRSEC for future growth.