Details
| Original language | English |
|---|---|
| Pages (from-to) | 277-282 |
| Number of pages | 6 |
| Journal | Chemistry - A European Journal |
| Volume | 18 |
| Issue number | 1 |
| Early online date | 8 Dec 2011 |
| Publication status | Published - 2 Jan 2012 |
Abstract
With Car-Parrinello molecular dynamics simulations the elementary reaction steps of the electrolysis of bulk water are investigated. To simulate the reactions occurring near the anode and near the cathode, electrons are removed or added, respectively. The study focuses on the reactions in pure water. Effects depending on a particular electrode surface or a particular electrolyte are ignored. Under anodic conditions, the reaction continues till molecular oxygen is formed, under cathodic conditions the formation of molecular hydrogen is observed. In addition the formation of hydrogen peroxide is observed as an intermediate of the anodic reaction. The simulations demonstrate that the electrochemistry of oxygen formation without direct electrode contact can be explained by radical reactions in a solvent. These reactions may involve the intermediate formation of ions. The hydrogen formation is governed by rapid proton transfers between water molecules.
Keywords
- density functional theory, electrolysis of water, molecular dynamics, reaction mechanisms, redox chemistry
ASJC Scopus subject areas
- Chemical Engineering(all)
- Catalysis
- Chemistry(all)
- Organic Chemistry
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In: Chemistry - A European Journal, Vol. 18, No. 1, 02.01.2012, p. 277-282.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Electrolysis of water in the diffusion layer
T2 - First-principles molecular dynamics simulation
AU - Hofbauer, Florian
AU - Frank, Irmgard
PY - 2012/1/2
Y1 - 2012/1/2
N2 - With Car-Parrinello molecular dynamics simulations the elementary reaction steps of the electrolysis of bulk water are investigated. To simulate the reactions occurring near the anode and near the cathode, electrons are removed or added, respectively. The study focuses on the reactions in pure water. Effects depending on a particular electrode surface or a particular electrolyte are ignored. Under anodic conditions, the reaction continues till molecular oxygen is formed, under cathodic conditions the formation of molecular hydrogen is observed. In addition the formation of hydrogen peroxide is observed as an intermediate of the anodic reaction. The simulations demonstrate that the electrochemistry of oxygen formation without direct electrode contact can be explained by radical reactions in a solvent. These reactions may involve the intermediate formation of ions. The hydrogen formation is governed by rapid proton transfers between water molecules.
AB - With Car-Parrinello molecular dynamics simulations the elementary reaction steps of the electrolysis of bulk water are investigated. To simulate the reactions occurring near the anode and near the cathode, electrons are removed or added, respectively. The study focuses on the reactions in pure water. Effects depending on a particular electrode surface or a particular electrolyte are ignored. Under anodic conditions, the reaction continues till molecular oxygen is formed, under cathodic conditions the formation of molecular hydrogen is observed. In addition the formation of hydrogen peroxide is observed as an intermediate of the anodic reaction. The simulations demonstrate that the electrochemistry of oxygen formation without direct electrode contact can be explained by radical reactions in a solvent. These reactions may involve the intermediate formation of ions. The hydrogen formation is governed by rapid proton transfers between water molecules.
KW - density functional theory
KW - electrolysis of water
KW - molecular dynamics
KW - reaction mechanisms
KW - redox chemistry
UR - http://www.scopus.com/inward/record.url?scp=84555217795&partnerID=8YFLogxK
U2 - 10.1002/chem.201002094
DO - 10.1002/chem.201002094
M3 - Article
AN - SCOPUS:84555217795
VL - 18
SP - 277
EP - 282
JO - Chemistry - A European Journal
JF - Chemistry - A European Journal
SN - 0947-6539
IS - 1
ER -