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Metal–water interface formation : Thermodynamics from ab initio molecular dynamics simulations (2024)


Domínguez-Flores, F., Kiljunen, T., Groß, A., Sakong, S., & Melander, M. M. (2024). Metal–water interface formation : Thermodynamics from ab initio molecular dynamics simulations. Journal of Chemical Physics, 161(4), Article 044705. https://doi.org/10.1063/5.0220576


JYU-tekijät tai -toimittajat


Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajatDomínguez-Flores, Fabiola; Kiljunen, Toni; Groß, Axel; Sakong, Sung; Melander, Marko M.

Lehti tai sarjaJournal of Chemical Physics

ISSN0021-9606

eISSN1089-7690

Julkaisuvuosi2024

Ilmestymispäivä26.07.2024

Volyymi161

Lehden numero4

Artikkelinumero044705

KustantajaAIP Publishing

JulkaisumaaYhdysvallat (USA)

Julkaisun kielienglanti

DOIhttps://doi.org/10.1063/5.0220576

Julkaisun avoin saatavuusEi avoin

Julkaisukanavan avoin saatavuus

Julkaisu on rinnakkaistallennettu (JYX)https://jyx.jyu.fi/handle/123456789/97032


Tiivistelmä

Metal–water interfaces are central to many electrochemical, (electro)catalytic, and materials science processes and systems. However, our current understanding of their thermodynamic properties is limited by the scarcity of accurate experimental and computational data and procedures. In this work, thermodynamic quantities for metal–water interface formation are computed for a range of FCC(111) surfaces (Pd, Pt, Au, Ag, Rh, and PdAu) through extensive density functional theory based molecular dynamics and the two-phase entropy model. We show that metal–water interface formation is thermodynamically favorable and that most metal surfaces studied in this work are completely wettable, i.e., have contact angles of zero. Interfacial water has higher entropy than bulk water due to the increased population of low-frequency translational modes. The entropic contributions also correlate with the orientational water density, and the highest solvation entropies are observed for interfaces with a moderately ordered first water layer; the entropic contributions account for up to ∼25% of the formation free energy. Water adsorption energy correlates with the water orientation and structure and is found to be a good descriptor of the internal energy part of the interface formation free energy, but it alone cannot satisfactorily explain the interfacial thermodynamics; the interface formation is driven by the competition between energetic and entropic contributions. The obtained results and insight can be used to develop, parameterize, and benchmark theoretical and computational methods for studying metal–water interfaces. Overall, our study yields benchmark-quality data and fundamental insight into the thermodynamic forces driving metal–water interface formation.


YSO-asiasanatpintakemiarajapinnat (pinnat)rajapintailmiöttermodynamiikkasimulointimolekyylidynamiikkatiheysfunktionaaliteoria

Vapaat asiasanatdensity functional theory; molecular dynamics; quantum mechanical/molecular mechanical calculations; thermodynamics; computational methods; liquid solid interfaces; catalysts and catalysis; solvation


Liittyvät organisaatiot

JYU-yksiköt:


Hankkeet, joissa julkaisu on tehty


OKM-raportointiKyllä

VIRTA-lähetysvuosi2024

Alustava JUFO-taso1


Viimeisin päivitys 2024-14-10 klo 15:10