Engineering interfacial silicon dioxide for improved metal-insulator-semiconductor silicon photoanode water splitting performance

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Satterthwaite, Peter F.
Scheuermann, Andrew G.
Hurley, Paul K.
Chidsey, Christopher E. D.
McIntyre, Paul C.
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American Chemical Society
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Silicon photoanodes protected by atomic layer deposited (ALD) TiO2 show promise as components of water splitting devices that may enable the large-scale production of solar fuels and chemicals. Minimizing the resistance of the oxide corrosion protection layer is essential for fabricating efficient devices with good fill factor. Recent literature reports have shown that the interfacial SiO2 layer, interposed between the protective ALD-TiO2 and the Si anode, acts as a tunnel oxide that limits hole conduction from the photoabsorbing substrate to the surface oxygen evolution catalyst. Herein, we report a significant reduction of bilayer resistance, achieved by forming stable, ultrathin (<1.3 nm) SiO2 layers, allowing fabrication of water splitting photoanodes with hole conductances near the maximum achievable with the given catalyst and Si substrate. Three methods for controlling the SiO2 interlayer thickness on the Si(100) surface for ALD-TiO2 protected anodes were employed: (1) TiO2 deposition directly on an HF-etched Si(100) surface, (2) TiO2 deposition after SiO2 atomic layer deposition on an HF-etched Si(100) surface, and (3) oxygen scavenging, post-TiO2 deposition to decompose the SiO2 layer using a Ti overlayer. Each of these methods provides a progressively superior means of reliably thinning the interfacial SiO2 layer, enabling the fabrication of efficient and stable water oxidation silicon anodes.
Atomic-layer deposition , Photoelectrochemical cells , Electronic-properties , Oxygen , Oxide , Oxidation , Anodes , TiO2 , Conversion , Growth
Satterthwaite, Peter F.;Scheuermann, Andrew G.;Hurley, Paul K.;Chidsey, Christopher E. D.;McIntyre, Paul C. (2016) 'Engineering interfacial silicon dioxide for improved metal-insulator-semiconductor silicon photoanode water splitting performance'. Acs Applied Materials & Interfaces, 8 (20):13140-13149. doi: 10.1021/acsami.6b03029
This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see