Abstract
Recently, a large quantity of research has been done on the conversion of CH4.(1) Compared to photo-catalysis and thermo-catalysis with precious metal catalysts and high reaction temperatures, the electro-catalysis path, which are always performed at room temperature, demonstrates more potential. In this regard, the electrochemical oxidation and conversion of CH4 to commodity chemicals, such as wide-application liquid alcohols, shows obvious economic benefit and high energy/ conversion-efficient. Zirconia (ZrO2) has rich Lewis acid active sites and huge electron acceptability, showing a remarkable adsorption capacity of CO32-.(2) Based on the above characters, zirconia-based hybrid has attracted a lot of attention and made some breakthroughs. In particular, transition metal oxide (TMO, such as NiO and Co3O4) doping ZrO2 forming TMO/ZrO2 compound demonstrates the potential of methane oxidation with CO32- at room temperature. Compared to NiO and Co3O4, copper-based (Cu) catalysts have a high activity and a long-term durability on forming liquid and gas organics of C1 catalysis reaction system (CO2 reduction reaction) at room temperature.(3-5) Hence, we present a facile strategy of using Cu ions doping ZrO2 to activate the hybrid activity by manipulating its crystal and electronic structure. As expected, the unique cylindrical ZrO2:CuOx catalyst shows remarkable CH4 oxidation performance with large current density differences (13.35 mA cm-2) and long-term electrochemical stability (negligible attenuation (10 %) after 48 hours). According to theoretical and experimental observations of the CH4 oxidation on ZrO2: CuOx hybrid, the high activity and durability of the hybrid should be attributed to 1) strong synergistic-coupling effect; 2) the unique doping structure forming favorable electronic and crystal structure; 3) fast oxidation reaction mechanism by shortening the reaction path. The mechanism could be described as that ZrO2 facilitating CO32- adsorption, then CO32- as the oxidizing agent source rapidly oxidizes CH4 adsorbed on the surface of Cu in zirconia.Keywords: ZrO2:CuOx, Methane conversion, high activity, Unique doping structure Uncategorized
Published Version
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