A first-principles analysis of electrocatalytic oxidation of Co at the Dmfc anode

Michael John Janik, Matthew Neurock

Research output: Chapter in Book/Report/Conference proceedingConference contribution

Abstract

A key factor limiting the anode performance in the direct methanol fuel cell is the poisoning of Pt by CO, an abundant surface intermediate that forms in methanol oxidation. The energetics of CO oxidation over Pt and different Pt-Ru alloys were studied. The influences of solution and electrochemical potential on the overall reaction energies and activation barriers were examined. The addition of ruthenium to a Pt surface significantly reduced the equilibrium potential of water activation, thus indicating that the bifunctional mechanism contributes substantially to the oxidation of CO. The introduction of Ru into Pt, however, also acted to increase the equilibrium potential for the overall reaction of CO and H2O to form CO2, two protons and two electrons. The equilibrium overpotential for the overall oxidation of CO with H2O was substantially reduced in the overlayer system due to decreased binding energies of both species. A combined alloy system, with a mixed Pt/Ru layer over a Ru bulk substrate was shown to combine both the bifunctional and ligand effects. This is an abstract of a paper presented at the AIChE Annual Meeting (San Francisco, CA 11/12-17/2006).

Original languageEnglish (US)
Title of host publication2006 AIChE Annual Meeting
StatePublished - 2006
Event2006 AIChE Annual Meeting - San Francisco, CA, United States
Duration: Nov 12 2006Nov 17 2006

Other

Other2006 AIChE Annual Meeting
CountryUnited States
CitySan Francisco, CA
Period11/12/0611/17/06

Fingerprint

Carbon Monoxide
Anodes
Electrodes
Oxidation
Chemical activation
Methanol
Direct methanol fuel cells (DMFC)
Binding energy
Ruthenium
San Francisco
Protons
Poisoning
Ligands
Electrons
Substrates
Water

All Science Journal Classification (ASJC) codes

  • Biotechnology
  • Chemical Engineering(all)
  • Bioengineering
  • Safety, Risk, Reliability and Quality

Cite this

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title = "A first-principles analysis of electrocatalytic oxidation of Co at the Dmfc anode",
abstract = "A key factor limiting the anode performance in the direct methanol fuel cell is the poisoning of Pt by CO, an abundant surface intermediate that forms in methanol oxidation. The energetics of CO oxidation over Pt and different Pt-Ru alloys were studied. The influences of solution and electrochemical potential on the overall reaction energies and activation barriers were examined. The addition of ruthenium to a Pt surface significantly reduced the equilibrium potential of water activation, thus indicating that the bifunctional mechanism contributes substantially to the oxidation of CO. The introduction of Ru into Pt, however, also acted to increase the equilibrium potential for the overall reaction of CO and H2O to form CO2, two protons and two electrons. The equilibrium overpotential for the overall oxidation of CO with H2O was substantially reduced in the overlayer system due to decreased binding energies of both species. A combined alloy system, with a mixed Pt/Ru layer over a Ru bulk substrate was shown to combine both the bifunctional and ligand effects. This is an abstract of a paper presented at the AIChE Annual Meeting (San Francisco, CA 11/12-17/2006).",
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}

Janik, MJ & Neurock, M 2006, A first-principles analysis of electrocatalytic oxidation of Co at the Dmfc anode. in 2006 AIChE Annual Meeting. 2006 AIChE Annual Meeting, San Francisco, CA, United States, 11/12/06.

A first-principles analysis of electrocatalytic oxidation of Co at the Dmfc anode. / Janik, Michael John; Neurock, Matthew.

2006 AIChE Annual Meeting. 2006.

Research output: Chapter in Book/Report/Conference proceedingConference contribution

TY - GEN

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AU - Janik, Michael John

AU - Neurock, Matthew

PY - 2006

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N2 - A key factor limiting the anode performance in the direct methanol fuel cell is the poisoning of Pt by CO, an abundant surface intermediate that forms in methanol oxidation. The energetics of CO oxidation over Pt and different Pt-Ru alloys were studied. The influences of solution and electrochemical potential on the overall reaction energies and activation barriers were examined. The addition of ruthenium to a Pt surface significantly reduced the equilibrium potential of water activation, thus indicating that the bifunctional mechanism contributes substantially to the oxidation of CO. The introduction of Ru into Pt, however, also acted to increase the equilibrium potential for the overall reaction of CO and H2O to form CO2, two protons and two electrons. The equilibrium overpotential for the overall oxidation of CO with H2O was substantially reduced in the overlayer system due to decreased binding energies of both species. A combined alloy system, with a mixed Pt/Ru layer over a Ru bulk substrate was shown to combine both the bifunctional and ligand effects. This is an abstract of a paper presented at the AIChE Annual Meeting (San Francisco, CA 11/12-17/2006).

AB - A key factor limiting the anode performance in the direct methanol fuel cell is the poisoning of Pt by CO, an abundant surface intermediate that forms in methanol oxidation. The energetics of CO oxidation over Pt and different Pt-Ru alloys were studied. The influences of solution and electrochemical potential on the overall reaction energies and activation barriers were examined. The addition of ruthenium to a Pt surface significantly reduced the equilibrium potential of water activation, thus indicating that the bifunctional mechanism contributes substantially to the oxidation of CO. The introduction of Ru into Pt, however, also acted to increase the equilibrium potential for the overall reaction of CO and H2O to form CO2, two protons and two electrons. The equilibrium overpotential for the overall oxidation of CO with H2O was substantially reduced in the overlayer system due to decreased binding energies of both species. A combined alloy system, with a mixed Pt/Ru layer over a Ru bulk substrate was shown to combine both the bifunctional and ligand effects. This is an abstract of a paper presented at the AIChE Annual Meeting (San Francisco, CA 11/12-17/2006).

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