Nanostructured PdO/CeO supported on mesoporous SBA-15 silica was synthesized using a combination of incipient wetness impregnation and surface-assisted reduction. After calcination, the materials showed good activity as catalysts for the low-temperature oxidation of methane, with a sample having 5 wt % Pd loading showing 50% conversion to CO at ∼290 °C and complete conversion below 360 °C. The stability of catalysts in the presence of water was studied. The formation of Pd(0) during the methane oxidation reaction increases the oxygen vacancies on the surface of catalysts, improving the catalytic activity.
Bowtie-shaped NiCo 2 O 4 nanostructures are prepared using a hydrothermal method. Variation of the synthesis parameters, including reaction time, additives, and calcination temperature, allows an understanding of the origin of the bowtie-shaped structure to be developed. Methane oxidation experiments performed using temperature-programed oxidation (TPO) show that the new materials, which do not contain precious metals, have excellent activity for low-temperature methane combustion, with 100% conversion at ≈410 °C (gas hourly space velocity (GHSV): 90 000 mL (STP) g −1 h −1 ). The structure-activity relationships of the bowtie-shaped nanostructures are explored. The relatively low exhaust temperature in NGVs means that the activation of methane, which has the strongest CH bond of any hydrocarbon, is challenging from a chemical perspective. It is not surprising that the quest for effective lowtemperature methane oxidation catalysts has focused mainly on systems involving precious metals, such as platinum and palladium. [11][12][13][14][15] Metal oxidesupported PdO catalysts are generally considered to represent the state of the art for methane combustion catalysts. [16][17][18][19][20] Recent research in this field has focused on improving activity at low temperatures, [21,22] reducing the required loading of metal [23,24] and improving the thermal and hydrothermal stability of PdO catalysts. [25][26][27][28][29][30] Exciting recent advances include the development of core-shell Pd@CeO 2 catalysts with high activity and thermal stability, demonstrating complete conversion to CO 2 below 400 °C (gas hourly space velocity (GHSV) = 200 000 mL g −1 h −1 ). [21] Pd@ZrO 2 /Si-Al 2 O 3 catalysts that are stable in the presence of high concentrations of water vapor have also been proposed recently. [25] NiO@PdO/Al 2 O 3 catalysts that show good activity and stability with only 0.2 wt% Pd loading have been prepared [23] as well as Pd-based bimetallic nanocrystalline catalysts, in which the promotional effects of different transition metals have been examined. [26] Although Pd-based catalysts show excellent activity, the high price and low abundance of palladium are limiting factors to practical application, [31] and both the hydrothermal stability and SO 2 tolerance for these catalysts need to be improved. For this reason, the development of alternative catalysts based on non-noble metals is attractive. [32] These include single metal oxide-based catalysts (CuO, [33] Co 3 O 4 , [34] and MnO 2 [35] ), perovskite, [36,37] spinel, [38,39] and hexaaluminate [40] catalysts. Among these, Co 3 O 4 exhibits good activity for methane combustion attributed to a spinel-type structure with variable Co oxidation states and a high density of oxygen vacancies on the surface. [41] Additionally, the specific exposed facets and morphology of Co 3 O 4 plays an important role in the catalysis. [42,43] Materials with exposed (110) planes show enhanced catalytic activity for methane oxidation compared with those only exposing (100) or (111) face...
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