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  • Structure–property relationships describing the buried interface between silicon oxide overlayers and electrocatalytic platinum thin films
Title: Structure–property relationships describing the buried interface between silicon oxide overlayers and electrocatalytic platinum thin films
Encapsulation of an active electrocatalyst with a permeable overlayer is an attractive approach to simultaneously enhance its stability, activity, and selectivity. However, the structure–property relationships that govern the performance of encapsulated electrocatalysts are poorly understood, especially those describing the electrocatalytic behavior of the buried interface between the overlayer and active electrocatalyst. Using planar silicon oxide (SiO x )-encapsulated platinum (Pt)/titanium (Ti) bilayer thin films as model electrodes, the present study investigates the physical and electrochemical properties of the SiO x |Pt buried interface. Through a combination of X-ray photoelectron spectroscopy and electroanalytical measurements, it is revealed that a platinum oxide (PtO x ) interlayer can exist between the SiO x overlayer and Pt thin film. The thickness and properties of the PtO x interlayer can be altered by modifying (i) the thickness of the SiO x overlayer or (ii) the thickness of the Pt layer, which may expose the buried interface to oxophilic Ti. Importantly, SiO x |Pt electrodes based on ultrathin Pt/Ti bilayers possess thinner PtO x interlayers while exhibiting reduced permeabilities for Cu 2+ and H + and enhanced stability during cycling in 0.5 M H 2 SO 4 . These findings highlight the tunability of buried interfaces while providing new insights that are needed to guide the design of complex electrocatalysts that contain them.  more » « less
Award ID(s):
1752340
NSF-PAR ID:
10082423
Author(s) / Creator(s):
; ; ; ;
Date Published:
Journal Name:
Journal of Materials Chemistry A
Volume:
6
Issue:
44
ISSN:
2050-7488
Page Range / eLocation ID:
22287 to 22300
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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    References

    Lee, D. H.; Park, H.; Clevenger, M.; Kim, H.; Kim, C. S.; Liu, M.; Kim, G.; Song, H. W.; No, K.; Kim, S. Y.; Ko, D.-K.; Lucietto, A.; Park, H.; Lee, S., High-Performance Oxide-Based p–n Heterojunctions Integrating p-SnOx and n-InGaZnO.ACS Applied Materials & Interfaces2021,13(46), 55676-55686.

    Hautier, G.; Miglio, A.; Ceder, G.; Rignanese, G.-M.; Gonze, X., Identification and design principles of low hole effective mass p-type transparent conducting oxides.Nat Commun2013,4.

    Yim, K.; Youn, Y.; Lee, M.; Yoo, D.; Lee, J.; Cho, S. H.; Han, S., Computational discovery of p-type transparent oxide semiconductors using hydrogen descriptor.npj Computational Materials2018,4(1), 17.

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