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Title: Importance of Surface IrOx in Stabilizing RuO2 for Oxygen Evolution

Abstract

The high precious metal loading and high overpotential of the oxygen evolution reaction (OER) prevents the widespread utilization of polymer electrolyte membrane (PEM) water electrolyzers. In this paper, we explore the OER activity and stability in acidic electrolyte of a combined IrOx/RuO2 system consisting of RuO2 thin films with submonolayer (1, 2, and 4 Å) amounts of IrOx deposited on top. Operando extended X-ray absorption fine structure (EXAFS) on the Ir L-3 edge revealed a rutile type IrO2 structure with some Ir sites occupied by Ru, IrOx being at the surface of the RuO2 thin film. We monitor corrosion on IrOx/RuO2 thin films by combining electrochemical quartz crystal microbalance (EQCM) with inductively coupled mass spectrometry (ICP-MS). We elucidate the importance of submonolayer surface IrOx in minimizing Ru dissolution. Finally, our work shows that we can tune the surface properties of active OER catalysts, such as RuO2, aiming to achieve higher electrocatalytic stability in PEM electrolyzers.

Authors:
 [1];  [2];  [2];  [2];  [3];  [2];  [4];  [5]; ORCiD logo [2]
  1. Univ. of Copenhagen (Denmark). Nano-Science Centre. Dept. of Chemistry; Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis. Dept. of Chemical Engineering
  2. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics
  3. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis. Dept. of Chemical Engineering
  4. Univ. of Copenhagen (Denmark). Nano-Science Centre. Dept. of Chemistry
  5. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; Imperial College London (United Kingdom). Dept. of Materials
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Copenhagen (Denmark); Technical Univ. of Denmark, Lyngby (Denmark)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Danish Council for Independent Research (Denmark); Danish Ministry of Higher Education and Science (Denmark); Villum Foundation (Denmark)
OSTI Identifier:
1471514
Grant/Contract Number:  
AC02-76SF00515; 9455
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 122; Journal Issue: 2; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Escudero-Escribano, María, Pedersen, Anders F., Paoli, Elisa A., Frydendal, Rasmus, Friebel, Daniel, Malacrida, Paolo, Rossmeisl, Jan, Stephens, Ifan E. L., and Chorkendorff, Ib. Importance of Surface IrOx in Stabilizing RuO2 for Oxygen Evolution. United States: N. p., 2017. Web. https://doi.org/10.1021/acs.jpcb.7b07047.
Escudero-Escribano, María, Pedersen, Anders F., Paoli, Elisa A., Frydendal, Rasmus, Friebel, Daniel, Malacrida, Paolo, Rossmeisl, Jan, Stephens, Ifan E. L., & Chorkendorff, Ib. Importance of Surface IrOx in Stabilizing RuO2 for Oxygen Evolution. United States. https://doi.org/10.1021/acs.jpcb.7b07047
Escudero-Escribano, María, Pedersen, Anders F., Paoli, Elisa A., Frydendal, Rasmus, Friebel, Daniel, Malacrida, Paolo, Rossmeisl, Jan, Stephens, Ifan E. L., and Chorkendorff, Ib. Wed . "Importance of Surface IrOx in Stabilizing RuO2 for Oxygen Evolution". United States. https://doi.org/10.1021/acs.jpcb.7b07047. https://www.osti.gov/servlets/purl/1471514.
@article{osti_1471514,
title = {Importance of Surface IrOx in Stabilizing RuO2 for Oxygen Evolution},
author = {Escudero-Escribano, María and Pedersen, Anders F. and Paoli, Elisa A. and Frydendal, Rasmus and Friebel, Daniel and Malacrida, Paolo and Rossmeisl, Jan and Stephens, Ifan E. L. and Chorkendorff, Ib},
abstractNote = {The high precious metal loading and high overpotential of the oxygen evolution reaction (OER) prevents the widespread utilization of polymer electrolyte membrane (PEM) water electrolyzers. In this paper, we explore the OER activity and stability in acidic electrolyte of a combined IrOx/RuO2 system consisting of RuO2 thin films with submonolayer (1, 2, and 4 Å) amounts of IrOx deposited on top. Operando extended X-ray absorption fine structure (EXAFS) on the Ir L-3 edge revealed a rutile type IrO2 structure with some Ir sites occupied by Ru, IrOx being at the surface of the RuO2 thin film. We monitor corrosion on IrOx/RuO2 thin films by combining electrochemical quartz crystal microbalance (EQCM) with inductively coupled mass spectrometry (ICP-MS). We elucidate the importance of submonolayer surface IrOx in minimizing Ru dissolution. Finally, our work shows that we can tune the surface properties of active OER catalysts, such as RuO2, aiming to achieve higher electrocatalytic stability in PEM electrolyzers.},
doi = {10.1021/acs.jpcb.7b07047},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 2,
volume = 122,
place = {United States},
year = {2017},
month = {10}
}

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