Water Adsorption and Dissociation at Metal-Supported Ceria Thin Films: Thickness and Interface-Proximity Effects Studied with DFT+U Calculations
- Lucie SzabováLucie SzabováInternational Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, JapanDepartment of Surface and Plasma Science, Faculty of Mathematics and Physics, Charles University in Prague, V Holešovičkách 747/2, 180 00 Praha 8, Czech RepublicMore by Lucie Szabová
- ,
- Yoshitaka TateyamaYoshitaka TateyamaInternational Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, JapanPRESTO and CREST, Japan Science and Technology Agency (JST), 4-1-8 Honcho, Kawaguchi, Saitama 333-0012, JapanMore by Yoshitaka Tateyama
- ,
- Vladimír MatolínVladimír MatolínDepartment of Surface and Plasma Science, Faculty of Mathematics and Physics, Charles University in Prague, V Holešovičkách 747/2, 180 00 Praha 8, Czech RepublicMore by Vladimír Matolín
- , and
- Stefano Fabris*Stefano Fabris*E-mail: [email protected]CNR-IOM DEMOCRITOS, Istituto Officina dei Materiali, Consiglio Nazionale delle Ricerche, via Bonomea 265, I-34136 Trieste, ItalySISSA, Scuola Internazionale Superiore di Studi Avanzati, via Bonomea 265, I-34136 Trieste, ItalyMore by Stefano Fabris
Abstract
The chemistry of several catalytic processes can be controlled by tuning metal–oxide interfaces, as demonstrated by fundamental studies on inverse model catalysts. We investigate the effects of the metal–oxide interface on the surface reactivity of ceria (CeO2) thin films supported by a copper metal surface. Our density functional theory (DFT+U) calculations reveal that the interface has impact on the surface water adsorption and dissociation when the thickness of the ceria film is below ≈9 Å. On thinner films, the energetics of adsorption and dissociation display a significant variation, which arises from a combination of thickness and interface-proximity effects, and which we rationalize in terms of charge-density response at the adsorbate-oxide and oxide-metal interfaces. The adsorption energy is maximized for film thicknesses of 5.5 Å (corresponding to two O–Ce–O trilayers), while thinner films affect primarily the relative stability between molecular, semidissociated, and dissociated water adsorption. These results provide useful insights into the effect of low-dimensional ceria species in Cu/CeO2 catalysts.
Cited By
This article is cited by 16 publications.
- Luca Brugnoli, Maria Cristina Menziani, Shingo Urata, Alfonso Pedone. Development and Application of a ReaxFF Reactive Force Field for Cerium Oxide/Water Interfaces. The Journal of Physical Chemistry A 2021, 125 (25) , 5693-5708. https://doi.org/10.1021/acs.jpca.1c04078
- Lucie Szabová, Matteo Farnesi Camellone, Fabio Negreiros Ribeiro, Vladimír Matolín, Yoshitaka Tateyama, Stefano Fabris. Dynamical Solvent Effects on the Charge and Reactivity of Ceria-Supported Pt Nanoclusters. The Journal of Physical Chemistry C 2018, 122 (48) , 27507-27515. https://doi.org/10.1021/acs.jpcc.8b09154
- Filip Dvořák, Lucie Szabová, Viktor Johánek, Matteo Farnesi Camellone, Vitalii Stetsovych, Mykhailo Vorokhta, Andrii Tovt, Tomáš Skála, Iva Matolínová, Yoshitaka Tateyama, Josef Mysliveček, Stefano Fabris, Vladimír Matolín. Bulk Hydroxylation and Effective Water Splitting by Highly Reduced Cerium Oxide: The Role of O Vacancy Coordination. ACS Catalysis 2018, 8 (5) , 4354-4363. https://doi.org/10.1021/acscatal.7b04409
- Matteo Farnesi Camellone, Fabio Negreiros Ribeiro, Lucie Szabová, Yoshitaka Tateyama, and Stefano Fabris . Catalytic Proton Dynamics at the Water/Solid Interface of Ceria-Supported Pt Clusters. Journal of the American Chemical Society 2016, 138 (36) , 11560-11567. https://doi.org/10.1021/jacs.6b03446
- Klára Ševčíková, Lucie Szabová, Miroslav Kettner, Petr Homola, Nataliya Tsud, Stefano Fabris, Vladimír Matolín, and Václav Nehasil . Experimental and Theoretical Study on the Electronic Interaction between Rh Adatoms and CeOx Substrate in Dependence on a Degree of Cerium Oxide Reduction. The Journal of Physical Chemistry C 2016, 120 (10) , 5468-5476. https://doi.org/10.1021/acs.jpcc.5b11431
- Qin Zhou, Humaira Akber, Aidi Zhao, Fan Yang, Zhi Liu. Interaction of Water with Ceria Thin Film. ChemCatChem 2023, 15 (15) https://doi.org/10.1002/cctc.202300318
- Luca Brugnoli, Shingo Urata, Alfonso Pedone. H 2 O 2 adsorption and dissociation on various CeO 2 (111) surface models: a first-principles study. Journal of Physics: Condensed Matter 2022, 34 (16) , 164006. https://doi.org/10.1088/1361-648X/ac5278
- Ruiyu Wang, Michael L. Klein, Vincenzo Carnevale, Eric Borguet. Investigations of water/oxide interfaces by molecular dynamics simulations. WIREs Computational Molecular Science 2021, 11 (6) https://doi.org/10.1002/wcms.1537
- Zhong-Kang Han, Xinyi Duan, Xiaoyan Li, Dawei Zhang, Yi Gao. The dynamic interplay between water and oxygen vacancy at the near-surface of ceria. Journal of Physics: Condensed Matter 2021, 33 (42) , 424001. https://doi.org/10.1088/1361-648X/ac13fc
- Saleh E. Rawadieh, Mohammednoor Altarawneh, Ibrahem S. Altarawneh, Mohammad A. Batiha, Leema A. Al-Makhadmeh. A kinetic model for evolution of H2 and CO over Zr-doped ceria. Molecular Catalysis 2020, 498 , 111256. https://doi.org/10.1016/j.mcat.2020.111256
- Andreas Röckert, Jolla Kullgren, Peter Broqvist, Seif Alwan, Kersti Hermansson. The water/ceria(111) interface: Computational overview and new structures. The Journal of Chemical Physics 2020, 152 (10) https://doi.org/10.1063/1.5142724
- Bingling He, Jiansheng Shen, Dongwei Ma, Jinlong Wang, Sujun Cheng, Zhixue Tian. H2O adsorption on the Au and Pd single atom catalysts supported on ceria: A first-principles study. Applied Surface Science 2018, 462 , 399-408. https://doi.org/10.1016/j.apsusc.2018.08.149
- Leydi del R. Silva-Calpa, Priscila C. Zonetti, Daniela C. de Oliveira, Roberto R. de Avillez, Lucia G. Appel. Acetone from ethanol employing Zn x Zr 1−x O 2−y. Catalysis Today 2017, 289 , 264-272. https://doi.org/10.1016/j.cattod.2016.09.011
- Yaroslava Lykhach, Albert Bruix, Stefano Fabris, Valérie Potin, Iva Matolínová, Vladimír Matolín, Jörg Libuda, Konstantin M. Neyman. Oxide-based nanomaterials for fuel cell catalysis: the interplay between supported single Pt atoms and particles. Catalysis Science & Technology 2017, 7 (19) , 4315-4345. https://doi.org/10.1039/C7CY00710H
- Michalis Konsolakis. The role of Copper–Ceria interactions in catalysis science: Recent theoretical and experimental advances. Applied Catalysis B: Environmental 2016, 198 , 49-66. https://doi.org/10.1016/j.apcatb.2016.05.037
- Zhong‐Kang Han, Yi Gao. Water Adsorption and Dissociation on Ceria‐Supported Single‐Atom Catalysts: A First‐Principles DFT+U Investigation. Chemistry – A European Journal 2016, 22 (6) , 2092-2099. https://doi.org/10.1002/chem.201504588