Interfacial electrochemistry, which deals with complex catalytic processes in the electrochemical double layer (EDL), is a plentiful source of challenging research as well as a highly dynamic field owing to the rapid development of surface-sensitive techniques and computational tools. We have been working on this subject by developing several methodologies for first-principles molecular dynamics (FPMD) simulations to model an electrochemical interface. First, we proposed a method to incorporate the electric field in the EDL with an appropriate boundary condition by solving the Poisson equation using Green’s function method, which is called effective screening medium (ESM) method [1]. Second, we have developed a simulation scheme to mimic a constant electrode potential in which we can control the Fermi energy of the electrode by connecting the system to a potentiostat [2]. Recently we have developed a novel calculation technique for the solvation structure of EDL by combining the FP simulation with the classical liquid theory [3].
In the seminar, I will introduce the simulation techniques developed by us and present recent simulation results for the cyclic voltammogram of oxygen evolution reaction (OER) and oxygen reduction reaction (ORR)[4]. I will present some possible applications of our latest developed simulation method [3] which can model not only an electrochemical interface but also an ion-exchange membrane.
References
[1] M. Otani and O. Sugino, Phys. Rev. B 73, 115407 (2006).
[2] N. Bonnet, T. Morishita, O. Sugino, and M. Otani, Phys. Rev. Lett. 109, 266101 (2012).
[3] S. Nishihara and M. Otani, submitted to Phy. Rev. B.
[4] T. Ikeshoji and M. Otani, Phys. Chem. Chem. Phys. 19, 4447 (2017)