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

摘要

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.