Stacking-Dependent Electrochemistry in Twisted-Bilayer Graphene Superlattices

Attaining more degrees of freedom in manipulating electron transfer kinetics across heterogeneous interfaces is crucial for achieving more efficient interconversion of electrical and chemical energy. Moiré superlattices of graphene layers provide a novel yet extensive platform for tailoring dynamics of electrochemical reactions. In this study, we describe angle- and stacking-dependent charge transfer rates that range more than two orders of magnitude in twisted trilayer graphene samples. In certain twist angle regimes, the electrochemical behavior of trilayer graphene approaches that of a bulk metal surface. This wide range of electrokinetic control originates from distinctive electronic density of states at moiré superlattices and variations in electronic structure at disparate stacking configurations (ABA, ABC, AAB, and ABB). This result, combined with our previous studies on twisted bilayer graphene, further establishes moiré superlattices as an emerging route for engineering electrochemical properties of two-dimensional materials.