Conversion of Methane to Methanol: Nickel, Palladium, and Platinum (d9) Cations as Catalysts for the Oxidation of Methane by Ozone at Room Temperature

The room‐temperature chemical kinetics has been measured for the catalytic activity of Group 10 atomic cations in the oxidation of methane to methanol by ozone. Ni+ is observed to be the most efficient catalyst. The complete catalytic cycle with Ni+ is interpreted with a computed potential energy la...

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Veröffentlicht in:Chemistry : a European journal 2010-10, Vol.16 (38), p.11605-11610
Hauptverfasser: Božović, Andrea, Feil, Stefan, Koyanagi, Gregory K., Viggiano, Albert A., Zhang, Xinhao, Schlangen, Maria, Schwarz, Helmut, Bohme, Diethard K.
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Sprache:eng
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Zusammenfassung:The room‐temperature chemical kinetics has been measured for the catalytic activity of Group 10 atomic cations in the oxidation of methane to methanol by ozone. Ni+ is observed to be the most efficient catalyst. The complete catalytic cycle with Ni+ is interpreted with a computed potential energy landscape and, in principle, has an infinite turnover number for the oxidation of methane, without poisoning side reactions. The somewhat lower catalytic activity of Pd+ is reported for the first time and also explored with DFT calculations. Pt+ is seen to be ineffective as a catalyst because of the observed failure of PtO+ to convert methane to methanol. Nickel is the best: The catalytic activity of M+ (M=Ni, Pd and Pt) in the oxidation of methane to methanol by ozone has been studied both experimentally and computationally. Ni+ is found to be the most efficient catalyst. The complete catalytic cycle with Ni+ has no poisoning side reactions and so proceeds, in principle, with an infinite turnover number.
ISSN:0947-6539
1521-3765
DOI:10.1002/chem.201000627