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Atomic-Scale View on the H2O Formation Reaction from H2 on O-Rich RuO2(110)

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Interdisciplinary Nanoscience Center (iNANO) and Department of Physics and Astronomy, Aarhus University, DK-8000 Aarhus C, Denmark
*E-mail: [email protected]. Phone: ++45 8715 6731 (S.W.).
Cite this: J. Phys. Chem. C 2014, 118, 48, 27989–27997
Publication Date (Web):November 7, 2014
https://doi.org/10.1021/jp509510j
Copyright © 2014 American Chemical Society
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    Abstract

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    The H2O formation reaction from H2 on O-rich RuO2(110) was studied by temperature-programmed desorption and reaction (TPD/TPR) and scanning tunneling microscopy (STM) measurements and density functional theory (DFT) calculations. On the one hand, following H2 adsorption at 270 K, our TPD/TPR measurements reveal that the on-top O species (Oot) enhances the sticking probability of H2, thus facilitating the H2 adsorption and dissociation on O-rich RuO2(110). On the other hand, for low H2 adsorption temperature (170 K), the limited mobility of Had species hinders H2 adsorption at a high coverage of preadsorbed Oot. To better understand the strong influence of the adsorption temperature and the interplay between coadsorbed species, we conducted DFT calculations and high-resolution STM measurements. Two distinct adsorbate configurations, Had–Oot and Oot–Had–Oot, are identified by STM. Mechanisms and molecular models for H2 dissociation and Had diffusion on O-rich RuO2(110) are proposed.

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    Additional TPD/TPR and STM data, respectively, addressing the preparation of o-RuO2(110) surfaces with different Oot coverages (Figure S1), the calibration of the water coverages on s-RuO2(110) (Figure S2), the apparent STM heights of Had–Oot and Oot–Had–Oot species (Figure S3), the apparent STM heights of Oot species in the neighborhood of Oot–Had–Oot (Figure S4), and the diffusion of (Had)2–Oot and/or Had species on the surface at 150 K (Figure S5). This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cited By

    This article is cited by 10 publications.

    1. Zhu Liang, Minkyu Kim, Tao Li, Rahul Rai, Aravind Asthagiri, and Jason F. Weaver . Adsorption and Oxidation of Ethylene on the Stoichiometric and O-Rich RuO2(110) Surfaces. The Journal of Physical Chemistry C 2017, 121 (37) , 20375-20386. https://doi.org/10.1021/acs.jpcc.7b06865
    2. Manh-Thuong Nguyen, Rentao Mu, David C. Cantu, Igor Lyubinetsky, Vassiliki-Alexandra Glezakou, Zdenek Dohnálek, and Roger Rousseau . Dynamics, Stability, and Adsorption States of Water on Oxidized RuO2(110). The Journal of Physical Chemistry C 2017, 121 (34) , 18505-18515. https://doi.org/10.1021/acs.jpcc.7b03280
    3. Franziska Hess and Herbert Over . Rate-Determining Step or Rate-Determining Configuration? The Deacon Reaction over RuO2(110) Studied by DFT-Based KMC Simulations. ACS Catalysis 2017, 7 (1) , 128-138. https://doi.org/10.1021/acscatal.6b02575
    4. Michael A. Henderson, Arjun Dahal, Zdenek Dohnálek, and Igor Lyubinetsky . Strong Temperature Dependence in the Reactivity of H2 on RuO2(110). The Journal of Physical Chemistry Letters 2016, 7 (15) , 2967-2970. https://doi.org/10.1021/acs.jpclett.6b01307
    5. Michael A. Henderson, Rentao Mu, Arjun Dahal, Igor Lyubinetsky, Zdenek Dohnálek, Vassiliki-Alexandra Glezakou, and Roger Rousseau . Light Makes a Surface Banana-Bond Split: Photodesorption of Molecular Hydrogen from RuO2(110). Journal of the American Chemical Society 2016, 138 (28) , 8714-8717. https://doi.org/10.1021/jacs.6b05083
    6. Ankita Jadon, Carole Rossi, Mehdi Djafari-Rouhani, Alain Estève, David Pech. Interaction of hydrogen with the bulk, surface and subsurface of crystalline RuO2 from first principles. Physics Open 2021, 7 , 100059. https://doi.org/10.1016/j.physo.2021.100059
    7. Arjun Dahal, Rentao Mu, Igor Lyubinetsky, Zdenek Dohnálek. Hydrogen adsorption and reaction on RuO2(110). Surface Science 2018, 677 , 264-270. https://doi.org/10.1016/j.susc.2018.07.014
    8. Tao Li, Minkyu Kim, Zhu Liang, Aravind Asthagiri, Jason F. Weaver. Hydrogen oxidation on oxygen-rich IrO 2 (110). Catalysis, Structure & Reactivity 2018, 4 (4) , 1-13. https://doi.org/10.1080/2055074X.2018.1565002
    9. Hayk A. Zakaryan, Alexander G. Kvashnin, Artem R. Oganov. Stable reconstruction of the (110) surface and its role in pseudocapacitance of rutile-like RuO2. Scientific Reports 2017, 7 (1) https://doi.org/10.1038/s41598-017-10331-z
    10. Liming Liu, Honghan Wang, Xiaowen Zhang, Zhidong Lin. Synthesis of novel RuO2/NaBi(MoO4)2 nanosheets composite and its gas sensing performances towards ethanol. Sensors and Actuators B: Chemical 2016, 237 , 275-283. https://doi.org/10.1016/j.snb.2016.06.095
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