Robust electrografted interfaces on metal oxides for electrocatalysis-an in situ spectroelectrochemical study

Harris TGAA, Goetz R, Wrzolek P, Davis V, Knapp CE, Ly K, Hildebrandt P, Schwalbe M, Weidinger IM, Zebger I, Fischer A (2018)

Publication Type: Journal article

Publication year: 2018

Journal

Journal of Materials Chemistry A Royal Society of Chemistry

Book Volume: 6

Pages Range: 15200-15212

Journal Issue: 31

DOI: 10.1039/c8ta02983k

Abstract

Diazonium salts were electrografted onto transparent conductive oxides as stable alternatives to conventional anchoring groups for the surface immobilisation of molecular species, such as molecular electrocatalysts and/or photosensitisers. Surface sensitive in situ ATR-IR spectroscopy, in combination with spectroelectrochemistry, was used as tool to provide unprecedented information on the interface formation, structure and stability, which is not possible using conventional approaches. Electrografted interfaces deposited on model oxides were thereby shown to be stable in an extraordinarily wide pH range (2.5-12) and electrochemical potential window (-0.73 to 2.23 V vs. RHE in aqueous media, and -1.3 V to 1.6 V vs. Fc/Fc+ in organic media). As a model electrocatalyst, an Fe porphyrin active for the oxygen reduction reaction (ORR) was immobilised on both mesoporous antimony doped tin oxide (me-ATO) and planar tin doped indium oxide (pl-ITO) using this electrografting approach. Surface coverages comparable to those previously reported using phosphonate anchoring groups were achieved. In addition, fast electron transfer rates were demonstrated, while in situ resonance Raman spectroelectrochemistry proved the co-ordination of the immobilised species and demonstrated its excellent electrochemical accessibility.

Involved external institutions

Technische Universität Berlin DE Germany (DE) Humboldt-Universität zu Berlin DE Germany (DE) Albert-Ludwigs-Universität Freiburg DE Germany (DE) University College London (UCL) GB United Kingdom (GB) University of Cambridge GB United Kingdom (GB) Technische Universität Dresden DE Germany (DE)

How to cite

APA:

Harris, T.G.A.A., Goetz, R., Wrzolek, P., Davis, V., Knapp, C.E., Ly, K.,... Fischer, A. (2018). Robust electrografted interfaces on metal oxides for electrocatalysis-an in situ spectroelectrochemical study. Journal of Materials Chemistry A, 6(31), 15200-15212. https://doi.org/10.1039/c8ta02983k

MLA:

Harris, Tomos G. A. A., et al. "Robust electrografted interfaces on metal oxides for electrocatalysis-an in situ spectroelectrochemical study." Journal of Materials Chemistry A 6.31 (2018): 15200-15212.

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