(Invited) Toward Rigorous Modeling of Metal-Metal, Metal-Oxide and Oxide-Oxide Interfaces for the Electrochemical Oxygen Cycle

Abstract

To achieve Net-Zero Emissions by 2050, hydrogen and hydrogen fuel cells will play a significant role in powering vehicles. In this presentation, I will show, through first-principles-based modeling, how to achieve rigorous modeling of solid-solid interface for the hydrogen and oxygen evolution reactions in electrolysis and the oxygen reduction reaction in fuel cells; and how the fundamental understanding paves the way toward developing both model electrocatalysts and industrial electrocatalysts with significantly improved performance. Specifically, I will introduce the following three topics.[1] metal-metal interfaces: strain evolution and strain tuning of epitaxial, stepped and free-standing platinum group metals for the oxygen reduction reaction in fuel cells.(1)[2] metal-oxide interfaces: stability and activity of monolayer oxide/Pt interface toward improving the hydrogen evolution reaction in alkaline conditions.(2)[3] oxide-oxide interfaces: self-consistent modeling of active phases, reaction centers, and catalytic mechanisms of Ni- and Co-based layered double hydroxides for the oxygen evolution reaction.(3, 4) L. Wang, Z. Zeng, W. Gao, T. Maxson, D. Raciti, M. Giroux, X. Pan, C. Wang, J. Greeley, Tunable intrinsic strain in two-dimensional transition metal electrocatalysts. Science 363, 870-874 (2019).Z. Zeng, K.-C. Chang, J. Kubal, N. M. Markovic, J. Greeley, Stabilization of ultrathin (hydroxy)oxide films on transition metal substrates for electrochemical energy conversion. Nature Energy 2, 17070 (2017).F. Dionigi, Z. Zeng, I. Sinev, T. Merzdorf, S. Deshpande, M. B. Lopez, S. Kunze, I. Zegkinoglou, H. Sarodnik, D. Fan, A. Bergmann, J. Drnec, J. F. d. Araujo, M. Gliech, D. Teschner, J. Zhu, W.-X. Li, J. Greeley, B. R. Cuenya, P. Strasser, In-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution. Nature Communications 11, 2522 (2020).F. Dionigi, J. Zhu, Z. Zeng, T. Merzdorf, H. Sarodnik, M. Gliech, L. Pan, W.-X. Li, J. Greeley, P. Strasser, Intrinsic Electrocatalytic Activity for Oxygen Evolution of Crystalline 3d-Transition Metal Layered Double Hydroxides. Angew. Chem., Int. Ed. 60, 14446-14457 (2021). Figure 1