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Sustained Water Oxidation by Direct Electrosynthesis of Ultrathin Organic Protection Films on Silicon

Azarpia, Anahita and Schedel-Niedrig, Thomas and Lewerenz, H.-J. and Lublow, Michael (2016) Sustained Water Oxidation by Direct Electrosynthesis of Ultrathin Organic Protection Films on Silicon. Advanced Energy Materials, 6 (10). p. 1502314. ISSN 1614-6832. doi:10.1002/aenm.201502314.

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Artificial photosynthesis allows exceeding the efficiency and stability limits of natural photosynthesis. Based on the use of semiconducting absorbers, high efficiency in water photolysis has been achieved in various photoelectrode configurations. However, integrated systems are limited in their stability, and more stable half-cell electrodes use protection films prepared by laborious methods. Herein, the facile low-temperature preparation of ultrathin organic protection coatings is demonstrated. The formation is based on the catalytic properties of water oxidation catalysts toward alcohol-polymerization reactions, which results in the formation of hitherto unknown protection layers on silicon. The interfacial layers are generated via iodine-mediated electro-reductive polymerization of ethanol, concomitantly forming during electrophoretic transport of RuO_2 onto silicon supports. Reaction chemistry analyses show that the RuO_2-induced catalysis introduces E2-elimination reactions which result in a carbon sp^3 –sp^2 transformation of the film. For the two modes of photoelectrochemical operation, the photovoltaic and the photoelectrocatalytic mode, 20 and 15 mA cm^(−2) photocurrent densities, respectively, are obtained with unaltered output for 8 and 24 h. The interfacial layer enables Si photovoltages of 500 mV, demonstrating extraordinary electronic interface quality. Since only hydrogen termination of the surface is a prerequisite for growth of the organic protection layer, the method is applicable to a wide range of semiconductors.

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Lewerenz, H.-J.0000-0001-8433-9471
Additional Information:© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Received: November 19, 2015 Revised: January 17, 2016 Published online: March 11, 2016 The authors are thankful for fruitful discussion with R. van de Krol. They gratefully acknowledge the financial support provided by the Deutsche Forschungsgemeinschaft (DFG), project No. SCHE 533/3-1 within the priority program SPP 1613-“Solar-H 2." M.L. acknowledges temporary financial support granted by Freiburg University, Germany (group A. Fischer). The joint discussion and interpretation of the data and contributions to the manuscript (H.J.L.) was also supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under Award Number DE-SC0004993.
Funding AgencyGrant Number
Deutsche Forschungsgemeinschaft (DFG)SCHE 533/3-1
Deutsche Forschungsgemeinschaft (DFG)SPP 1613-“Solar-H_2"
Freiburg UniversityUNSPECIFIED
Department of Energy (DOE)DE-SC0004993
Subject Keywords:organic protection layer;oxygen evolution reaction;photoelectrocatalysis;RuO2;silicon supports
Non-Subject Keywords:organic protection layer;oxygen evolution reaction;photoelectrocatalysis;RuO2;silicon supports
Issue or Number:10
Record Number:CaltechAUTHORS:20160629-084424702
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Official Citation:Azarpira A., Schedel-Niedrig T., Lewerenz H.-J., Lublow M. (2016). Sustained Water Oxidation by Direct Electrosynthesis of Ultrathin Organic Protection Films on Silicon. Adv. Energy Mater., 6: . doi: 10.1002/aenm.201502314
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:68732
Deposited By: Donna Wrublewski
Deposited On:29 Jun 2016 16:50
Last Modified:11 Nov 2021 04:04

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