Enhanced Stability and Efficiency for Photoelectrochemical Iodide Oxidation by Methyl Termination and Electrochemical Pt Deposition on n-Type Si Microwire Arrays

Shane Ardo, Elizabeth A. Santori, Hal S. Emmer, Ronald L. Grimm, Matthew J. Bierman, Bruce S. Brunschwig, Harry A. Atwater, Nathan S. Lewis

Research output: Contribution to journalArticle

Abstract

Arrays of Si microwires doped n-type (n-Si) and surface-functionalized with methyl groups have been used, with or without deposition of Pt electrocatalysts, to photoelectrochemically oxidize I-(aq) to I3 -(aq) in 7.6 M HI(aq). Under conditions of iodide oxidation, methyl-terminated n-Si microwire arrays exhibited stable short-circuit photocurrents over a time scale of days, albeit with low energy-conversion efficiencies. In contrast, electrochemical deposition of Pt onto methyl-terminated n-Si microwire arrays consistently yielded energy-conversion efficiencies of ∼2% for iodide oxidation, with an open-circuit photovoltage of ∼400 mV and a short-circuit photocurrent density of ∼10 mA cm-2 under 100 mW cm-2 of simulated air mass 1.5G solar illumination. Platinized electrodes were stable for >200 h of continuous operation, with no discernible loss of Si or Pt. Pt deposited using electron-beam evaporation also resulted in stable photoanodic operation of the methyl-terminated n-Si microwire arrays but yielded substantially lower photovoltages than when Pt was deposited electrochemically.

Original languageEnglish
Pages (from-to)2308-2314
Number of pages7
JournalACS Energy Letters
Volume4
Issue number9
DOIs
Publication statusPublished - Sep 13 2019

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Iodides
Photocurrents
Energy conversion
Short circuit currents
Conversion efficiency
Oxidation
Electrocatalysts
Electron beams
Evaporation
Lighting
Electrodes
Networks (circuits)
Air

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

Cite this

Enhanced Stability and Efficiency for Photoelectrochemical Iodide Oxidation by Methyl Termination and Electrochemical Pt Deposition on n-Type Si Microwire Arrays. / Ardo, Shane; Santori, Elizabeth A.; Emmer, Hal S.; Grimm, Ronald L.; Bierman, Matthew J.; Brunschwig, Bruce S.; Atwater, Harry A.; Lewis, Nathan S.

In: ACS Energy Letters, Vol. 4, No. 9, 13.09.2019, p. 2308-2314.

Research output: Contribution to journalArticle

Ardo, Shane ; Santori, Elizabeth A. ; Emmer, Hal S. ; Grimm, Ronald L. ; Bierman, Matthew J. ; Brunschwig, Bruce S. ; Atwater, Harry A. ; Lewis, Nathan S. / Enhanced Stability and Efficiency for Photoelectrochemical Iodide Oxidation by Methyl Termination and Electrochemical Pt Deposition on n-Type Si Microwire Arrays. In: ACS Energy Letters. 2019 ; Vol. 4, No. 9. pp. 2308-2314.
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