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Operando Analyses of Solar Fuels Light Absorbers and Catalysts

Lewerenz, Hans-Joachim and Lichterman, Michael F. and Richter, Matthias H. and Crumlin, Ethan J. and Hu, Shu and Axnanda, Stephanus and Favaro, Marco and Drisdell, Walter and Hussain, Zahid and Brunschwig, Bruce S. and Liu, Zhi and Nilsson, Anders and Bell, Alexis T. and Lewis, Nathan S. and Friebel, Daniel (2016) Operando Analyses of Solar Fuels Light Absorbers and Catalysts. Electrochimica Acta, 211 . pp. 711-719. ISSN 0013-4686. doi:10.1016/j.electacta.2016.06.006.

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Operando synchrotron radiation photoelectron spectroscopy (SRPES) in the tender X-ray energy range has been used to obtain information on the energy-band relations of semiconductor and metal-covered semiconductor surfaces while in direct contact with aqueous electrolytes under potentiostatic control. The system that was investigated consists of highly doped Si substrates that were conformally coated with ∼70 nm titania films produced by atomic-layer deposition. The TiO2/electrolyte and the Si/TiO2/Ni electrolyte interfaces were then analyzed by synchrotron radiation photoelectron spectroscopy. The PES data provided a determination of the flat-band position and identified regions of applied potential in which Fermi level pinning, depletion, or accumulation conditions occurred. Operando X-ray absorption spectroscopy (XAS) techniques were additionally used to investigate the properties of heterogeneous electrocatalysts for the oxygen-evolution reaction. Operando XAS including the pre-edge, edge and EXAFS regions allowed the development of a detailed picture of the catalysts under operating conditions, and elucidated the changes that in the physical and electronic structure of the catalyst that accompanied increases in the applied potential. Specifically, XAS data, combined with DFT studies, indicated that the activity of the electrocatalyst correlated with the formation of Fe dopant sites in γ-NiOOH.

Item Type:Article
Related URLs:
URLURL TypeDescription
Lewerenz, Hans-Joachim0000-0001-8433-9471
Lichterman, Michael F.0000-0002-0710-7068
Richter, Matthias H.0000-0003-0091-2045
Crumlin, Ethan J.0000-0003-3132-190X
Hu, Shu0000-0002-5041-0169
Drisdell, Walter0000-0002-8693-4562
Brunschwig, Bruce S.0000-0002-6135-6727
Bell, Alexis T.0000-0002-5738-4645
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2016 Elsevier Ltd. Received 11 December 2015, Revised 31 May 2016, Accepted 1 June 2016, Available online 6 June 2016. This work was supported by the Office of Science of the U.S. Department of Energy (DOE) through award no. DE-SC0004993 to the Joint Center for Artificial Photosynthesis. The Advanced Light Source acknowledges support by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. XAS data collection was carried out at Stanford Synchrotron Radiation Lightsource, a National User Facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences. Computational work was carried out through NERSC computational resources under DOE Contract No. DE-AC02-05CH11231.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
Subject Keywords:Catalysis; Semiconductors; Protection; operando spectroscopy; artificial photosynthesis
Record Number:CaltechAUTHORS:20160629-130400375
Persistent URL:
Official Citation:Hans-Joachim Lewerenz, Michael F. Lichterman, Matthias H. Richter, Ethan J. Crumlin, Shu Hu, Stephanus Axnanda, Marco Favaro, Walter Drisdell, Zahid Hussain, Bruce S. Brunschwig, Zhi Liu, Anders Nilsson, Alexis T. Bell, Nathan S. Lewis, Daniel Friebel, Operando Analyses of Solar Fuels Light Absorbers and Catalysts, Electrochimica Acta, Volume 211, 1 September 2016, Pages 711-719, ISSN 0013-4686, (
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:68756
Deposited By: Donna Wrublewski
Deposited On:29 Jun 2016 22:18
Last Modified:11 Nov 2021 04:04

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