Direct observation of the energetics at a semiconductor/liquid junction by operando X-ray photoelectron spectroscopy

Michael F. Lichterman, Shu Hu, Matthias H. Richter, Ethan J. Crumlin, Stephanus Axnanda, Marco Favaro, Walter Drisdell, Zahid Hussain, Thomas Mayer, Bruce S. Brunschwig, Nathan S. Lewis, Zhi Liu, Hans Joachim Lewerenz

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Abstract

Photoelectrochemical (PEC) cells based on semiconductor/liquid interfaces provide a method of converting solar energy to electricity or fuels. Currently, the understanding of semiconductor/liquid interfaces is inferred from experiments and models. Operando ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) has been used herein to directly characterize the semiconductor/liquid junction at room temperature under real-time electrochemical control. X-ray synchrotron radiation in conjunction with AP-XPS has enabled simultaneous monitoring of the solid surface, the solid/electrolyte interface, and the bulk electrolyte of a PEC cell as a function of the applied potential, U. The observed shifts in binding energy with respect to the applied potential have directly revealed ohmic and rectifying junction behavior on metallized and semiconducting samples, respectively. Additionally, the non-linear response of the core level binding energies to changes in the applied electrode potential has revealed the influence of defect-derived electronic states on the Galvani potential across the complete cell.

Original languageEnglish
Pages (from-to)2409-2416
Number of pages8
JournalEnergy and Environmental Science
Volume8
Issue number8
DOIs
Publication statusPublished - Jan 1 2015

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ASJC Scopus subject areas

  • Environmental Chemistry
  • Renewable Energy, Sustainability and the Environment
  • Nuclear Energy and Engineering
  • Pollution

Cite this

Lichterman, M. F., Hu, S., Richter, M. H., Crumlin, E. J., Axnanda, S., Favaro, M., Drisdell, W., Hussain, Z., Mayer, T., Brunschwig, B. S., Lewis, N. S., Liu, Z., & Lewerenz, H. J. (2015). Direct observation of the energetics at a semiconductor/liquid junction by operando X-ray photoelectron spectroscopy. Energy and Environmental Science, 8(8), 2409-2416. https://doi.org/10.1039/c5ee01014d