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Title: Combined soft and hard X-ray ambient pressure photoelectron spectroscopy studies of semiconductor/electrolyte interfaces

The development of solar fuel generating materials would greatly benefit from a molecular level understanding of the semiconductor/electrolyte interface and changes in the interface induced by an applied potential and illumination by solar light. Ambient pressure photoelectron spectroscopy techniques with both soft and hard X-rays, AP-XPS and AP-HAXPES respectively, have the potential to markedly contribute to this understanding. In this paper we initially provide two examples of current challenges in solar fuels material development that AP-XPS and AP-HAXPES can directly a ddress. This will be followed by a brief description of the distinguishing and complementary characteristics of soft and hard X-ray AP-XPS and AP-HAXPES and best approaches to achieving monolayer sensitivity in solid/aqueous electrolyte studies. In particular we focus on the detection of surface adsorbed hydroxyl groups in the presence of aqueous hydroxide anions in the electrolyte, a common situation when investigating photoanodes for solar fuel generating applications. Finally, the article concludes by providing an example of a combined AP-XPS and AP-HAXPES study of a semiconductor/aqueous electrolyte interface currently used in water splitting devices specifically the BiVO 4/aqueous potassium phosphate electrolyte interface.
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [4] ;  [1]
  1. Helmholtz-Zentrum Berlin (HZB), (Germany). Inst. for Solar Fuels
  2. Helmholtz-Zentrum Berlin (HZB), (Germany). Inst. for Solar Fuels; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Journal of Electron Spectroscopy and Related Phenomena
Additional Journal Information:
Journal Volume: 221; Journal Issue: C; Journal ID: ISSN 0368-2048
Publisher:
Elsevier
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
SC-22.1 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ambient pressure; Photoelectron spectroscopy; Solid liquid interface; HAXPES
OSTI Identifier:
1440005

Starr, David E., Favaro, Marco, Abdi, Fatwa F., Bluhm, Hendrik, Crumlin, Ethan J., and van de Krol, Roel. Combined soft and hard X-ray ambient pressure photoelectron spectroscopy studies of semiconductor/electrolyte interfaces. United States: N. p., Web. doi:10.1016/j.elspec.2017.05.003.
Starr, David E., Favaro, Marco, Abdi, Fatwa F., Bluhm, Hendrik, Crumlin, Ethan J., & van de Krol, Roel. Combined soft and hard X-ray ambient pressure photoelectron spectroscopy studies of semiconductor/electrolyte interfaces. United States. doi:10.1016/j.elspec.2017.05.003.
Starr, David E., Favaro, Marco, Abdi, Fatwa F., Bluhm, Hendrik, Crumlin, Ethan J., and van de Krol, Roel. 2017. "Combined soft and hard X-ray ambient pressure photoelectron spectroscopy studies of semiconductor/electrolyte interfaces". United States. doi:10.1016/j.elspec.2017.05.003. https://www.osti.gov/servlets/purl/1440005.
@article{osti_1440005,
title = {Combined soft and hard X-ray ambient pressure photoelectron spectroscopy studies of semiconductor/electrolyte interfaces},
author = {Starr, David E. and Favaro, Marco and Abdi, Fatwa F. and Bluhm, Hendrik and Crumlin, Ethan J. and van de Krol, Roel},
abstractNote = {The development of solar fuel generating materials would greatly benefit from a molecular level understanding of the semiconductor/electrolyte interface and changes in the interface induced by an applied potential and illumination by solar light. Ambient pressure photoelectron spectroscopy techniques with both soft and hard X-rays, AP-XPS and AP-HAXPES respectively, have the potential to markedly contribute to this understanding. In this paper we initially provide two examples of current challenges in solar fuels material development that AP-XPS and AP-HAXPES can directly a ddress. This will be followed by a brief description of the distinguishing and complementary characteristics of soft and hard X-ray AP-XPS and AP-HAXPES and best approaches to achieving monolayer sensitivity in solid/aqueous electrolyte studies. In particular we focus on the detection of surface adsorbed hydroxyl groups in the presence of aqueous hydroxide anions in the electrolyte, a common situation when investigating photoanodes for solar fuel generating applications. Finally, the article concludes by providing an example of a combined AP-XPS and AP-HAXPES study of a semiconductor/aqueous electrolyte interface currently used in water splitting devices specifically the BiVO4/aqueous potassium phosphate electrolyte interface.},
doi = {10.1016/j.elspec.2017.05.003},
journal = {Journal of Electron Spectroscopy and Related Phenomena},
number = C,
volume = 221,
place = {United States},
year = {2017},
month = {5}
}