AVS 65th International Symposium & Exhibition | |
Thin Films Division | Tuesday Sessions |
Session TF-TuM |
Session: | Emerging Applications for ALD |
Presenter: | Jon Baker, Stanford University |
Authors: | J.G. Baker, Stanford University J.R. Schneider, Stanford University J.A. Singh, Stanford University A.J. Mackus, Stanford University S.F. Bent, Stanford University |
Correspondent: | Click to Email |
Electrical energy storage has emerged as an important challenge for societies moving away from fossil fuels toward more renewable sources (e.g. solar and wind) that are intermittent in nature. To rely only on solar and wind for electricity, large scale energy storage systems are required. Among several potential solutions, one promising strategy is to store excess electrical energy in the form of chemical bonds, through electrochemical production of fuels. In particular, electrochemical water splitting enables the production of hydrogen gas as a chemical fuel from excess electrical energy. However, a major drawback of this strategy is the low efficiency of the oxygen evolution reaction (OER).
To improve the efficiency of the OER, understanding why certain catalysts perform well is a powerful tool in designing new catalysts with better properties. Atomic layer deposition (ALD) has emerged as a strong platform to study catalysts due to its ability to deposit films that are compositionally well-defined. For electrochemical systems, ALD has the added benefit of high uniformity, conformality and precise thickness control; these attributes can minimize potential confounding effects like resistive and mass transport losses, which may affect measurement of a catalyst’s intrinsic activity. In this work, we study the effect of aluminum on Ni-Fe-OOH catalysts. While Ni-Fe-OOH catalysts have been reported to have high activity for the OER (nearly independent of synthesis method), the impact of aluminum on this catalyst is not yet well understood, with a wide range of OER activities reported. By using ALD, ternary films of Ni-Al-O were deposited. Introduction of iron was achieved through electrolyte iron-doping, enabling the formation of the quaternary Ni-Al-Fe-OOH catalyst. Electrochemical characterization of sufficiently thin films found that aluminum improved the turnover frequency of Ni-Fe-OOH catalysts by a factor of 3-4. By carefully controlling composition of the catalyst, the effects of aluminum and iron were independently studied. In iron-free catalysts, aluminum was found to improve OER activity; however, its improvement in activity was small compared to the effect of iron. In addition, thickness dependent studies were performed to understand how morphology and synthesis method may impact observed activity. For Ni-Al-Fe-OOH catalysts, a strong thickness dependence in the OER activity was observed. Characterization of the catalysts ex situ and under OER operating conditions reveal the likely cause of this thickness dependence is the observed changing morphology of the film with increasing thicknesses.