(389e) Understanding Electrochemistry from the Atomic to Macroscopic Scale

During this presentation, I will outline recent progress in the modeling of electrified interfaces based on my current research. The discussion will use examples from electrocatalysis and corrosion to highlight fundamental challenges in computational electrochemistry and how these challenges can be addressed. In particular, I will present methods that aim to bridge the gap between atomistic simulations and real systems by accounting for electrode potential effects, surfaces roughness and nanofeaturing, electrolyte concentration, and solvent dynamics at the electrode interface. Through these methods, I will demonstrate the mapping of physical behavior of the electrochemical system from the atomic to the macroscopic scale, as well as from the femtosecond to geological timescales.^[1-10]

My work finds motivation in the grand challenges in our society, including the development of sustainable energy solutions for the future. Electrochemical methods are expected to be instrumental in this transition offering unique possibilities to control selectivity and improve efficiency in chemical processes. Here, the identification of tailored electrocatalysts will play an important role in enabling the electrification of the chemical industry. In this endeavor, theoretical modeling will serve as a valuable guide towards rational design of active, selective, durable, and environmentally benign catalytic materials at the very nanoscale. Such predictions rely, however, on the development of accurate modeling tools able to capture the essential physics governing catalytic performance on multiple scales – including the methods discussed in this presentation.

To exemplify our methods, I will present results from a number of applications of broad general interest. This will include discussions on hydrogen and oxygen evolution reaction,^[1,10] important processes in the emerging hydrogen economy, as well as applications in the electroreduction of carbon dioxide and nitrate into value-added fuels and platform chemicals.^[6-9] The latter two are promising routes towards the simultaneous integration of renewable energy sources in the chemical industry and the closing of the anthropogenic carbon and nitrogen cycles. Finally, the issue of material stability will be addressed by studying the corrosion of copper – a versatile material with uses in the energy sector, as catalyst, in electronics, and in the construction of repositories for nuclear waste disposal.^[2-5] The close connections between the ability to make accurate predictions and the importance in moving from the modeling of ideal systems to the modeling of realistic surfaces and conditions will be emphasized throughout the presentation. One example is the role of active site distributions on rough copper catalysts for carbon dioxide in the product selectivity.^[6] Another example is the dynamic nature of the electrolyte at the electrocatalysts interface during coupled proton-electron transfer steps where off-equilibrium structures play and essential part in dictating the total reaction rate.^[1]

Putting my work in a wider perspective, it is clear that collaborations is essential in order to reach the ambitious goals of our society. The work that I and my coworkers have carried out merely adds a few pieces to the foundation that together with contributions from the whole community will aid in accelerating the progress in the important field of electrochemistry, paving the way towards increased understanding of the fundamentals in electrochemical systems and catalysis.

References:
[1] J Li, JH Stenlid, T Ludwig, PS Lamoureux, F Abild-Pedersen, J. Am. Chem. Soc., 143, 19341-19355 (2021)
[2] JH Stenlid, EC dos Santos, AJ Johansson, LGM Pettersson, Corros. Sci., 183, 109313 (2021)
[3] JH Stenlid, EC dos Santos, RM Arán-Ais, A Bagger, et al., Electrochim. Acta, 362, 137111 (2020)
[4] JH Stenlid, EC dos Santos, A Bagger, AJ Johansson, et al., J. Phys. Chem. C, 124, 469-481 (2019)
[5] JH Stenlid, EC dos Santos, AJ Johansson, LGM Pettersson, J. Electrochem. Soc., 166, C196-C20 (2019)
[6] JA Gauthier, JH Stenlid, F Abild-Pedersen, M Head-Gordon, AT Bell, ACS Energy Lett., 6, 3252-3260 (2021)
[7] HJ Peng, MT Tang, JH Stenlid, X Liu, F Abild-Pedersen, Nature Commun., 13, 1-11 (2022)
[8] MT Tang, HJ Peng, JH Stenlid, F Abild-Pedersen, J. Phys. Chem. C, 125, 26437-26447 (2021)
[9] MJ Liu, J Guo, AS Hoffman, JH Stenlid, et al., J. Am. Chem. Soc., 144, 5739-5744 (2022)
[10] M Görlin, JH Stenlid, S Koroidov, H-Y Wang, et al., Nat. Commun., 11, 1-11 (2020)