Kavli Affiliate: David T. Limmer
| First 5 Authors: Sonal Maroo, Leonardo Coello Escalante, Yizhe Wang, Matthew P. Erodici, Jonathon N. Nessralla
| Summary:
The activation free energy of electron transfer (ET) reactions is governed by
a crucial parameter: the reorganization energy. In heterogeneous ET at
electrified solid-liquid interfaces, it is presumed that only factors in the
electrolyte phase are responsible for determining the reorganization energy.
Here, we demonstrate the contribution of the electronic density of states (DOS)
of the electrode to the reorganization energy. Using van der Waals assembly of
two-dimensional crystals, we tune the DOS of graphene and measure its impact on
outer-sphere ET. We find the ensuing variation in ET rate arises from
modulation in a reorganization energy associated with image potential
localization in the electrode, which is dependent on the DOS. This work
establishes a fundamental role of the electrode electronic structure in
interfacial charge transfer.
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