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Title: Operando Analyses of Solar Fuels Light Absorbers and Catalysts

Operando synchrotron radiation photoelectron spectroscopy 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. TiO 2/electrolyte and Si/TiO 2 /Ni/electrolyte interfaces were then analyzed by synchrotron radiation photoelectron spectroscopy. The PES data allows for determination of the flat-band position and identification of potential regions in which Fermi level pinning, depletion, or accumulation 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 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.
Authors:
 [1] ; ORCiD logo [1] ;  [1] ;  [2] ;  [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [1] ;  [3] ;  [4] ;  [5] ;  [1] ;  [4]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Chinese Academy of Sciences, Shanghai (China); ShanghaiTech Univ., Shanghai (China)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Electrochimica Acta
Additional Journal Information:
Journal Volume: 211; Journal Issue: C; Journal ID: ISSN 0013-4686
Publisher:
Elsevier
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Catalysis; Semiconductors; Protection; operando spectroscopy; artificial photosynthesis
OSTI Identifier:
1377461

Lewerenz, Hans -Joachim, Lichterman, Michael F., Richter, Matthias H., Crumlin, Ethan J., Hu, Shu, Axnanda, Stephanus, Favaro, Marco, Drisdell, Walter, Hussain, Zahid, Brunschwig, Bruce S., Liu, Zhi, Nilsson, Anders, Bell, Alexis T., Lewis, Nathan S., and Friebel, Daniel. Operando Analyses of Solar Fuels Light Absorbers and Catalysts. United States: N. p., Web. doi:10.1016/j.electacta.2016.06.006.
Lewerenz, Hans -Joachim, Lichterman, Michael F., Richter, Matthias H., Crumlin, Ethan J., Hu, Shu, Axnanda, Stephanus, Favaro, Marco, Drisdell, Walter, Hussain, Zahid, Brunschwig, Bruce S., Liu, Zhi, Nilsson, Anders, Bell, Alexis T., Lewis, Nathan S., & Friebel, Daniel. Operando Analyses of Solar Fuels Light Absorbers and Catalysts. United States. doi:10.1016/j.electacta.2016.06.006.
Lewerenz, Hans -Joachim, Lichterman, Michael F., Richter, Matthias H., Crumlin, Ethan J., Hu, Shu, Axnanda, Stephanus, Favaro, Marco, Drisdell, Walter, Hussain, Zahid, Brunschwig, Bruce S., Liu, Zhi, Nilsson, Anders, Bell, Alexis T., Lewis, Nathan S., and Friebel, Daniel. 2016. "Operando Analyses of Solar Fuels Light Absorbers and Catalysts". United States. doi:10.1016/j.electacta.2016.06.006. https://www.osti.gov/servlets/purl/1377461.
@article{osti_1377461,
title = {Operando Analyses of Solar Fuels Light Absorbers and Catalysts},
author = {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},
abstractNote = {Operando synchrotron radiation photoelectron spectroscopy 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. TiO2/electrolyte and Si/TiO2 /Ni/electrolyte interfaces were then analyzed by synchrotron radiation photoelectron spectroscopy. The PES data allows for determination of the flat-band position and identification of potential regions in which Fermi level pinning, depletion, or accumulation 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 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.},
doi = {10.1016/j.electacta.2016.06.006},
journal = {Electrochimica Acta},
number = C,
volume = 211,
place = {United States},
year = {2016},
month = {6}
}