Combinatorial discovery of bifunctional oxygen reduction - Water oxidation electrocatalysts for regenerative fuel cells

Guoying Chen; David A. Delafuente; S. Sarangapani; Thomas E. Mallouk

doi:10.1016/S0920-5861(01)00327-3

Combinatorial discovery of bifunctional oxygen reduction - Water oxidation electrocatalysts for regenerative fuel cells

Guoying Chen, David A. Delafuente, S. Sarangapani, Thomas E. Mallouk

Research output: Contribution to journal › Article › peer-review

204 Scopus citations

Abstract

Electrode arrays containing 715 unique combinations of five elements (Pt, Ru, Os, Ir, and Rh) were prepared by borohydride reaction of aqueous metal salts, and were screened for activity as oxygen reduction and water oxidation catalysts. Using a consensus map, catalysts that showed high activity for both reactions and good resistance to anodic corrosion were identified in the Pt-Ru rich region of the Pt-Ru-Ir ternary. The ternary catalyst Pt_4.5Ru₄Ir_0.5 (subscripts indicate atomic ratios) is significantly more active than the previously described Pt₁Ir₁ bifunctional catalyst for both reactions. While the best ternary catalyst is close to Pt₁Ru₁ in composition, the latter is unstable with respect to anodic corrosion. A detailed kinetic comparison of anodically stable catalysts Pt_4.5Ru₄Ir_0.5 and Pt₁Ir₁ showed that the addition of the oxophilic element Ru increases the reaction rate by stabilizing S-O bonds (S ≡ surface atom) and accelerating the oxidative deprotonation of S-OH groups.

Original language	English (US)
Pages (from-to)	341-355
Number of pages	15
Journal	Catalysis Today
Volume	67
Issue number	4
DOIs	https://doi.org/10.1016/S0920-5861(01)00327-3
State	Published - Jun 15 2001

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry

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10.1016/S0920-5861(01)00327-3

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title = "Combinatorial discovery of bifunctional oxygen reduction - Water oxidation electrocatalysts for regenerative fuel cells",

abstract = "Electrode arrays containing 715 unique combinations of five elements (Pt, Ru, Os, Ir, and Rh) were prepared by borohydride reaction of aqueous metal salts, and were screened for activity as oxygen reduction and water oxidation catalysts. Using a consensus map, catalysts that showed high activity for both reactions and good resistance to anodic corrosion were identified in the Pt-Ru rich region of the Pt-Ru-Ir ternary. The ternary catalyst Pt4.5Ru4Ir0.5 (subscripts indicate atomic ratios) is significantly more active than the previously described Pt1Ir1 bifunctional catalyst for both reactions. While the best ternary catalyst is close to Pt1Ru1 in composition, the latter is unstable with respect to anodic corrosion. A detailed kinetic comparison of anodically stable catalysts Pt4.5Ru4Ir0.5 and Pt1Ir1 showed that the addition of the oxophilic element Ru increases the reaction rate by stabilizing S-O bonds (S ≡ surface atom) and accelerating the oxidative deprotonation of S-OH groups.",

author = "Guoying Chen and Delafuente, {David A.} and S. Sarangapani and Mallouk, {Thomas E.}",

note = "Funding Information: We thank the Army Research Office for support of this work under grant DAAH04-94-G-0055, subcontract SA151-298 from Illinois Institute of Technology. DAD thanks the NSF Solid State Chemistry Program for support of his summer research at Penn State. We thank Prof. Eugene Smotkin for helpful discussions about kinetic isotope effects, and for providing a copy of Ref. [42] prior to publication. We also thank Dr. Renxuan Liu for designing the gas diffusion cell used to test bulk catalysts, and Mr. Chad Waraksa for writing the computer program used to analyze current–voltage data. We thank Dr. Rosemary Walsh and the electron microscope facility for the Life Sciences in the Biotechnology Institute at Pennsylvania State University for the use of the scanning electron microscope, and Dr. Jeffrey Shallenberger of the Penn State Materials Characterization Laboratory for obtaining XPS spectra.",

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AU - Chen, Guoying

AU - Delafuente, David A.

AU - Sarangapani, S.

AU - Mallouk, Thomas E.

N1 - Funding Information: We thank the Army Research Office for support of this work under grant DAAH04-94-G-0055, subcontract SA151-298 from Illinois Institute of Technology. DAD thanks the NSF Solid State Chemistry Program for support of his summer research at Penn State. We thank Prof. Eugene Smotkin for helpful discussions about kinetic isotope effects, and for providing a copy of Ref. [42] prior to publication. We also thank Dr. Renxuan Liu for designing the gas diffusion cell used to test bulk catalysts, and Mr. Chad Waraksa for writing the computer program used to analyze current–voltage data. We thank Dr. Rosemary Walsh and the electron microscope facility for the Life Sciences in the Biotechnology Institute at Pennsylvania State University for the use of the scanning electron microscope, and Dr. Jeffrey Shallenberger of the Penn State Materials Characterization Laboratory for obtaining XPS spectra.

PY - 2001/6/15

Y1 - 2001/6/15

N2 - Electrode arrays containing 715 unique combinations of five elements (Pt, Ru, Os, Ir, and Rh) were prepared by borohydride reaction of aqueous metal salts, and were screened for activity as oxygen reduction and water oxidation catalysts. Using a consensus map, catalysts that showed high activity for both reactions and good resistance to anodic corrosion were identified in the Pt-Ru rich region of the Pt-Ru-Ir ternary. The ternary catalyst Pt4.5Ru4Ir0.5 (subscripts indicate atomic ratios) is significantly more active than the previously described Pt1Ir1 bifunctional catalyst for both reactions. While the best ternary catalyst is close to Pt1Ru1 in composition, the latter is unstable with respect to anodic corrosion. A detailed kinetic comparison of anodically stable catalysts Pt4.5Ru4Ir0.5 and Pt1Ir1 showed that the addition of the oxophilic element Ru increases the reaction rate by stabilizing S-O bonds (S ≡ surface atom) and accelerating the oxidative deprotonation of S-OH groups.

AB - Electrode arrays containing 715 unique combinations of five elements (Pt, Ru, Os, Ir, and Rh) were prepared by borohydride reaction of aqueous metal salts, and were screened for activity as oxygen reduction and water oxidation catalysts. Using a consensus map, catalysts that showed high activity for both reactions and good resistance to anodic corrosion were identified in the Pt-Ru rich region of the Pt-Ru-Ir ternary. The ternary catalyst Pt4.5Ru4Ir0.5 (subscripts indicate atomic ratios) is significantly more active than the previously described Pt1Ir1 bifunctional catalyst for both reactions. While the best ternary catalyst is close to Pt1Ru1 in composition, the latter is unstable with respect to anodic corrosion. A detailed kinetic comparison of anodically stable catalysts Pt4.5Ru4Ir0.5 and Pt1Ir1 showed that the addition of the oxophilic element Ru increases the reaction rate by stabilizing S-O bonds (S ≡ surface atom) and accelerating the oxidative deprotonation of S-OH groups.

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Combinatorial discovery of bifunctional oxygen reduction - Water oxidation electrocatalysts for regenerative fuel cells

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