Solar Cell-Powered Electrochemical Methane-To-Methanol Conversion With Cuo/Ceo2 Catalysts

ACS ENERGY LETTERS(2021)

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摘要
Electrochemical CH4 oxidation is attractive as a strategy capable of conversion with high selectivity, but improving productivity remains a challenge. We demonstrate that CuO/CeO2 can serve as a catalyst for the room-temperature conversion of CH4 to CH3OH in the presence of CO32-. At an optimized ratio of CuO/CeO2 (Cu:Ce = 6:4), we achieve the highest production rate of 752.9 mu mol/g(cat)/h (6 h reaction) at ambient pressure; among the oxygenates, a CH3OH selectivity of 79% is obtained. In an experiment using isotopes, we confirm that CH4 is activated by active oxygen on the catalyst surface provided from CO32- to form CH3OH. Furthermore, we demonstrate a solar cell-powered electrochemical CH4 conversion. In the 12 h reaction, a CH3OH production of 7165.0 mu mol/g(cat) at ambient pressure and 21986.6 mu mol/g(cat) at 10 bar is obtained.
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