Berlin 2018 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 61: Focus Session: Nanoscale Insights into Interfacial Electrochemistry I

O 61.6: Vortrag

Mittwoch, 14. März 2018, 12:30–12:45, HE 101

In-operando Vibrational Spectroscopies in Electrochemical Environment from First-principles — •Francesco Nattino¹, Oliviero Andreussi^1,2, and Nicola Marzari¹ — ¹Theory and Simulations of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, Station 12, CH-1015 Lausanne, Switzerland. — ²Institute of Computational Science, Università della Svizzera Italiana, Via Giuseppe Buffi 13, CH-6904 Lugano, Switzerland.

Electrocatalysis is expected to play a key role in the development of a clean energy cycle, from energy harvesting to transformation and storage. Spectroscopic techniques able to work under potential control can extremely contribute to design novel catalyst materials by providing insight on the mechanism of target electrochemical reactions. In this context, theory has the task to decipher the precious information that in-operando experimental techniques are able to provide.

We present here first-principles calculations on key reaction intermediates of two electrochemical processes: the oxidation of a gold single crystal surface and the carbon dioxide reduction on copper metal electrodes. Vibrational adsorbate frequencies are computed in a realistic electrochemical environment, exploiting an accurate implicit solvation model to mimic the electrolyte solutions. Our results complement very recent surface enhanced Raman spectroscopy (SERS) experiments and surface enhanced IR absorption (SEIRA) measurements, contributing to shed light on the reaction mechanism of the two electrocatalytical processes considered.