Platinum-macrocycle co-catalysts for the electrochemical oxidation of methanol

J. S. Bett; H. R. Kunz; A. J. Aldykiewicz; J. M. Fenton; W. F. Bailey; D. V. McGrath

doi:10.1016/S0013-4686(98)00122-4

Platinum-macrocycle co-catalysts for the electrochemical oxidation of methanol

J. S. Bett, H. R. Kunz, A. J. Aldykiewicz, J. M. Fenton, W. F. Bailey, D. V. McGrath

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68 Scopus citations

Abstract

Metal phthalocyanines (Fe, Co, Ni and Sn) and ruthenium tetramethylcyclam 14 and 15 were studied as cocatalysts for methanol oxidation on platinum supported catalysts. The formation of well defined monolayers of the adsorbed complexes was inferred from the Langmuirian form of the adsorption isotherms in solutions of macrocycles. The coverage at monolayer levels was low, e.g. 1.25 to 2.25 × 10¹³ molecules cm^-2 or 400 to 800 Å² molecule^-1. Enhancement for the methanol oxidation reaction was observed for Pt co-catalyzed with Sn phthalocyanine and Ru tetramethylcyclam. Ru tetramethylcyclam showed an enhancement for methanol oxidation on a per unit weight basis over pure Pt, approaching the activity of PtRu at lower potentials. Increasing the size of the nitrogen ring from 14 to 15 resulted in a lower redox potential and increase in the activity of methanol oxidation. The activity of Pt co-catalyzed with Ru TMC 15 decreased with time suggesting that the macrocycle was desorbing from the supported catalyst surface.

Original language	English (US)
Pages (from-to)	3645-3655
Number of pages	11
Journal	Electrochimica Acta
Volume	43
Issue number	24
DOIs	https://doi.org/10.1016/S0013-4686(98)00122-4
State	Published - Aug 21 1998
Externally published	Yes

Keywords

Methanol oxidation
Platinum
Ruthenium tetramethylcyclams

ASJC Scopus subject areas

General Chemical Engineering
Electrochemistry

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10.1016/S0013-4686(98)00122-4

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title = "Platinum-macrocycle co-catalysts for the electrochemical oxidation of methanol",

abstract = "Metal phthalocyanines (Fe, Co, Ni and Sn) and ruthenium tetramethylcyclam 14 and 15 were studied as cocatalysts for methanol oxidation on platinum supported catalysts. The formation of well defined monolayers of the adsorbed complexes was inferred from the Langmuirian form of the adsorption isotherms in solutions of macrocycles. The coverage at monolayer levels was low, e.g. 1.25 to 2.25 × 1013 molecules cm-2 or 400 to 800 {\AA}2 molecule-1. Enhancement for the methanol oxidation reaction was observed for Pt co-catalyzed with Sn phthalocyanine and Ru tetramethylcyclam. Ru tetramethylcyclam showed an enhancement for methanol oxidation on a per unit weight basis over pure Pt, approaching the activity of PtRu at lower potentials. Increasing the size of the nitrogen ring from 14 to 15 resulted in a lower redox potential and increase in the activity of methanol oxidation. The activity of Pt co-catalyzed with Ru TMC 15 decreased with time suggesting that the macrocycle was desorbing from the supported catalyst surface.",

keywords = "Methanol oxidation, Platinum, Ruthenium tetramethylcyclams",

author = "Bett, {J. S.} and Kunz, {H. R.} and Aldykiewicz, {A. J.} and Fenton, {J. M.} and Bailey, {W. F.} and McGrath, {D. V.}",

note = "Funding Information: This work was supported by the United States Department of Energy under contract number DE-AC08-96NV11984.",

year = "1998",

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doi = "10.1016/S0013-4686(98)00122-4",

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T1 - Platinum-macrocycle co-catalysts for the electrochemical oxidation of methanol

AU - Bett, J. S.

AU - Kunz, H. R.

AU - Aldykiewicz, A. J.

AU - Fenton, J. M.

AU - Bailey, W. F.

AU - McGrath, D. V.

N1 - Funding Information: This work was supported by the United States Department of Energy under contract number DE-AC08-96NV11984.

PY - 1998/8/21

Y1 - 1998/8/21

N2 - Metal phthalocyanines (Fe, Co, Ni and Sn) and ruthenium tetramethylcyclam 14 and 15 were studied as cocatalysts for methanol oxidation on platinum supported catalysts. The formation of well defined monolayers of the adsorbed complexes was inferred from the Langmuirian form of the adsorption isotherms in solutions of macrocycles. The coverage at monolayer levels was low, e.g. 1.25 to 2.25 × 1013 molecules cm-2 or 400 to 800 Å2 molecule-1. Enhancement for the methanol oxidation reaction was observed for Pt co-catalyzed with Sn phthalocyanine and Ru tetramethylcyclam. Ru tetramethylcyclam showed an enhancement for methanol oxidation on a per unit weight basis over pure Pt, approaching the activity of PtRu at lower potentials. Increasing the size of the nitrogen ring from 14 to 15 resulted in a lower redox potential and increase in the activity of methanol oxidation. The activity of Pt co-catalyzed with Ru TMC 15 decreased with time suggesting that the macrocycle was desorbing from the supported catalyst surface.

AB - Metal phthalocyanines (Fe, Co, Ni and Sn) and ruthenium tetramethylcyclam 14 and 15 were studied as cocatalysts for methanol oxidation on platinum supported catalysts. The formation of well defined monolayers of the adsorbed complexes was inferred from the Langmuirian form of the adsorption isotherms in solutions of macrocycles. The coverage at monolayer levels was low, e.g. 1.25 to 2.25 × 1013 molecules cm-2 or 400 to 800 Å2 molecule-1. Enhancement for the methanol oxidation reaction was observed for Pt co-catalyzed with Sn phthalocyanine and Ru tetramethylcyclam. Ru tetramethylcyclam showed an enhancement for methanol oxidation on a per unit weight basis over pure Pt, approaching the activity of PtRu at lower potentials. Increasing the size of the nitrogen ring from 14 to 15 resulted in a lower redox potential and increase in the activity of methanol oxidation. The activity of Pt co-catalyzed with Ru TMC 15 decreased with time suggesting that the macrocycle was desorbing from the supported catalyst surface.

KW - Methanol oxidation

KW - Platinum

KW - Ruthenium tetramethylcyclams

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Platinum-macrocycle co-catalysts for the electrochemical oxidation of methanol

Abstract

Keywords

ASJC Scopus subject areas

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