Abstract
We synthesized nickel-iron layered double hydroxide ([NiFe]-LDH) nanosheets with different interlayer anions to probe their role in water oxidation catalysis. In alkaline electrolyte in ambient air, carbonate rapidly replaced other interlayer anions and catalytic activity was highest. Electrocatalytic water oxidation in virtually carbonate-free alkaline electrolyte revealed that activity was a function of anion basicity. Our [NiFe]-LDH nanosheets, prepared by pulsed laser ablation in liquids, were regenerated in carbonate-containing aqueous KOH. Anion binding motifs were assessed by X-ray photoelectron spectroscopy in combination with density functional theory calculations, suggesting that nitrite species bound to edge-site Fe in the precatalyst correlated with higher water oxidation activity.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 1734-1743 |
| Number of pages | 10 |
| Journal | Energy and Environmental Science |
| Volume | 9 |
| Issue number | 5 |
| DOIs | |
| State | Published - May 2016 |
Funding
We thank George Rossman for help with solid-state IR spectroscopy. Research was carried out in the Laser Resource Center and the Molecular Materials Research Center of the Beckman Institute of the California Institute of Technology. This work was supported by the NSF CCI Solar Fuels Program (CHE-1305124) and the Arnold and Mabel Beckman Foundation. B. M. H. is a Fellow of the Resnick Sustainability Institute at Caltech. W. H. thanks the Deutsche Forschungsgemeinschaft and the Cluster of Excellence "Engineering of AdvancedMaterials" at the University of Erlangen-N?rnberg for support.
ASJC Scopus subject areas
- Environmental Chemistry
- Renewable Energy, Sustainability and the Environment
- Nuclear Energy and Engineering
- Pollution
