Abstract
Despite the importance of RuO2 in photocatalytic water splitting and catalysis in general, the interactions of water with even its most stable (110) surface are not well understood. In this study we employ a combination of high-resolution scanning tunneling microscopy imaging with density functional theory based ab initio molecular dynamics, and we follow the formation and binding of linear water clusters on coordinatively unsaturated ruthenium rows. We find that clusters of all sizes (dimers, trimers, tetramers, extended chains) are stabilized by donating one proton per every two water molecules to the surface bridge bonded oxygen sites, in contrast with water monomers that do not show a significant propensity for dissociation. The clusters with odd number of water molecules are less stable than the clusters with even number and are generally not observed under thermal equilibrium. For all clusters with even numbers, the dissociated dimers represent the fundamental building blocks with strong intradimer hydrogen bonds and only very weak interdimer interactions resulting in segmented water chains.
| Original language | English |
|---|---|
| Pages (from-to) | 23552-23558 |
| Number of pages | 7 |
| Journal | Journal of Physical Chemistry C |
| Volume | 119 |
| Issue number | 41 |
| DOIs | |
| Publication status | Published - Oct 15 2015 |
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ASJC Scopus subject areas
- Physical and Theoretical Chemistry
- Electronic, Optical and Magnetic Materials
- Surfaces, Coatings and Films
- Energy(all)
Cite this
Deprotonated Water Dimers : The Building Blocks of Segmented Water Chains on Rutile RuO2(110). / Mu, Rentao; Cantu, David C.; Glezakou, Vassiliki Alexandra; Lyubinetsky, Igor; Rousseau, Roger; Dohnálek, Zdenek.
In: Journal of Physical Chemistry C, Vol. 119, No. 41, 15.10.2015, p. 23552-23558.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Deprotonated Water Dimers
T2 - The Building Blocks of Segmented Water Chains on Rutile RuO2(110)
AU - Mu, Rentao
AU - Cantu, David C.
AU - Glezakou, Vassiliki Alexandra
AU - Lyubinetsky, Igor
AU - Rousseau, Roger
AU - Dohnálek, Zdenek
PY - 2015/10/15
Y1 - 2015/10/15
N2 - Despite the importance of RuO2 in photocatalytic water splitting and catalysis in general, the interactions of water with even its most stable (110) surface are not well understood. In this study we employ a combination of high-resolution scanning tunneling microscopy imaging with density functional theory based ab initio molecular dynamics, and we follow the formation and binding of linear water clusters on coordinatively unsaturated ruthenium rows. We find that clusters of all sizes (dimers, trimers, tetramers, extended chains) are stabilized by donating one proton per every two water molecules to the surface bridge bonded oxygen sites, in contrast with water monomers that do not show a significant propensity for dissociation. The clusters with odd number of water molecules are less stable than the clusters with even number and are generally not observed under thermal equilibrium. For all clusters with even numbers, the dissociated dimers represent the fundamental building blocks with strong intradimer hydrogen bonds and only very weak interdimer interactions resulting in segmented water chains.
AB - Despite the importance of RuO2 in photocatalytic water splitting and catalysis in general, the interactions of water with even its most stable (110) surface are not well understood. In this study we employ a combination of high-resolution scanning tunneling microscopy imaging with density functional theory based ab initio molecular dynamics, and we follow the formation and binding of linear water clusters on coordinatively unsaturated ruthenium rows. We find that clusters of all sizes (dimers, trimers, tetramers, extended chains) are stabilized by donating one proton per every two water molecules to the surface bridge bonded oxygen sites, in contrast with water monomers that do not show a significant propensity for dissociation. The clusters with odd number of water molecules are less stable than the clusters with even number and are generally not observed under thermal equilibrium. For all clusters with even numbers, the dissociated dimers represent the fundamental building blocks with strong intradimer hydrogen bonds and only very weak interdimer interactions resulting in segmented water chains.
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U2 - 10.1021/acs.jpcc.5b07158
DO - 10.1021/acs.jpcc.5b07158
M3 - Article
VL - 119
SP - 23552
EP - 23558
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 41
ER -