Graphene-supported nanocomposite materials have become increasingly popular for their potential applications in areas such as catalysis. However, in graphene-based nanocomposite catalysts, the solid-solid interfaces between catalysts and graphene are often poorly defined. Understanding and optimizing such interfaces is particularly important for electrocatalytic applications such as CO2 reduction, in which electrons need to migrate from the graphene electrode to the catalyst. Molecular functionalization of graphene offers enormous opportunities to prepare new electrocatalysts with enhanced electron transfer kinetics. Using gold nanoclusters (AuNCs) as the model metal nanoclusters (MNCs), this project aims to develop a new strategy for constructing innovative electrocatalysts from MNCs and pristine graphene. Specifically, AuNCs will be covalently attached onto three-dimensional pristine graphene (3DG) electrodes through a series of rationally designed molecular linkers. A combination of synthesis, computational modeling, electrochemistry, and spectroscopy are employed to investigate how the linker structure affects the performance of the AuNC-3DG electrocatalytic CO2 reduction. The results obtained are anticipated to enhance our fundamental understanding of how control over solid-solid interfaces at the molecular level impacts the performance of nanocomposite materials in electrochemical devices. This work is supported by NSF Award # 2247574.

Collaborators: Jerome Delhommelle (UML), Mingdi Yan (UML), and Gonghu Li (UNH).