Gd-Ni-Sb-SnO2 electrocatalysts for active and selective ozone production

James L. Lansing, Lingyan Zhao, Tana Siboonruang, Nuwan H. Attanayake, Angela B. Leo, Peter Fatouros, So Min Park, Kenneth R. Graham, John A. Keith, Maureen Tang

Research output: Contribution to journalArticlepeer-review

Abstract

Direct electrochemical production of dissolved ozone could potentially provide economic wastewater treatment and sanitation or a valuable chemical oxidant. Although Ni-Sb-SnO2 electrocatalysts have the highest known faradaic efficiencies for electrochemical ozone production, the activity and selectivity are not yet sufficient for commercial implementation. This work finds that co-doping Ni and Gd increases the ozone selectivity by a factor of three over Ni alone. These findings are the first demonstration of an active dopant other than Ni in SnO2. Electrochemical and physical characterization show that trends in ozone activity are caused by chemical catalysis, not morphology effects, and that conduction band alignment is not a catalytic descriptor for the system. Selective radical quenching experiments and quantum chemistry calculations of thermodynamic energies suggest that the kinetic barriers to form solution-phase intermediates are important for understanding the role of dopants in electrochemical ozone production.

Original languageEnglish
Article numbere17486
JournalAICHE Journal
Volume67
Issue number12
DOIs
StatePublished - Dec 2021

Bibliographical note

Funding Information:
We acknowledge support from the NSF (CHE-1856460/1855657 and EEC-1659324) and the Mascaro Center for Sustainable Innovation. Quantum chemistry calculations were run using resources provided by the University of Pittsburgh Center for Research Computing. So Min Park and Kenneth R. Graham gratefully acknowledge the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, and the EPSCoR program, under award no. DE-SC0018208 for supporting the UPS and XPS measurements and analysis.

Funding Information:
National Science Foundation, Grant/Award Numbers: 1659324, 1855657, 1856460; Department of Energy, Office of Science, Grant/Award Number: SC0018208 Funding information

Funding Information:
We acknowledge support from the NSF (CHE‐1856460/1855657 and EEC‐1659324) and the Mascaro Center for Sustainable Innovation. Quantum chemistry calculations were run using resources provided by the University of Pittsburgh Center for Research Computing. So Min Park and Kenneth R. Graham gratefully acknowledge the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, and the EPSCoR program, under award no. DE‐SC0018208 for supporting the UPS and XPS measurements and analysis.

Publisher Copyright:
© 2021 American Institute of Chemical Engineers.

Keywords

  • electrocatalysis
  • ozone

ASJC Scopus subject areas

  • Biotechnology
  • Environmental Engineering
  • Chemical Engineering (all)

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