Electrolytes can modify the thermodynamics and kinetics of water adsorption

Chia-Yi Lin^b, Austin Reese^b, Luka Mitrovic^a, Brady Bruno^a, Darrell Schlom^a, Jin Suntivich^a

^aCornell University, Department of Materials Science and Engineering, Ithaca, NY 14853, USA, Ithaca, United States

^bCornell University, Smith School of Chemical and Biomolecular Engineering, United States

Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)

#EEInt - Electrode-Electrolyte Interfaces in Electrocatalysis

Lausanne, Switzerland, 2024 November 12th - 15th

Organizers: Yu Katayama and Mariana Monteiro

Invited Speaker, Jin Suntivich, presentation 141
Publication date: 28th August 2024

This talk will discuss how electrolyte selection affects the thermodynamics and kinetics of water adsorption on metals and metal oxides. Water and ion adsorptions can modify the structure and activities of electrode-electrolyte interfaces; however, mapping their structure-property relationship has been challenging. To address this issue, we measure how bulk experimental variables such as solution pH and ions systematically affect water and ion adsorptions. In the first part, I will discuss the effects of solution pH and ions on the hydroxide and oxygen adsorption on well-defined metal-oxide surfaces [1]. The results will be compared to single-crystal platinum as a model for metals. In the second part, I will discuss the same effects but on kinetics to understand the adsorption mechanism [2]. If time permits, I will also show how pH and solution ions can modify the electrode-electrolyte interface using Second Harmonic Generation (SHG) spectroscopy, where we optically monitor the electrode potentials to infer information on the water orientation [3].

References:

[1] Kuo, D.Y., Paik, H., Kloppenburg, J., Faeth, B., Shen, K.M., Schlom, D.G., Hautier, G., Suntivich, J., Measurements of Oxygen Electroadsorption Energies and Oxygen Evolution Reaction on RuO2(110): A Discussion of the Sabatier Principle and its Role in Electrocatalysis, J. Am. Chem. Soc. 140 50 (2018), 17597-17605.

[2] Kuo, D.Y., Lu, X., Hu, B., Abruña, H.D., Suntivich, J., Rate and Mechanism of Electrochemical Formation of Surface-Bound Hydrogen on Pt(111) Single Crystals, J. Phys. Chem. Lett. 13 (2022) 6383-6390.

[3] Xu, P., Wang, R., Zhang, H., Carnevale, V., Borguet, E., Suntivich, J., Cation Modifies Interfacial Water Structures on Platinum during Alkaline Hydrogen Electrocatalysis, J. Am. Chem. Soc. 146 4 (2024), 2426-2434.

Acknowledgements:

We thank Dr. Ding-Yuan Kuo and Prof. Pengtao Xu for laying the groundwork for oxide electrochemistry and second harmonic generation experiments, Prof. Héctor D. Abruña, Prof. Juan Feliu, and Dr. Qihao Li for their help on single-crystal platinum growth, and Prof. Ismaila Dabo and Dr. Simon Gelin for their insights on interface thermodynamics. The work on single-crystal platinum is based upon work supported by the National Science Foundation under Grant No. CHE-2155157. The work on single-crystal oxides is based upon work supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under award DE-SC0023896.

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