Methane is one of the main components of atmospheric pollutants, which is challenging to be eliminated by catalytic oxidation under mild conditions because of its tetrahedral structure stability. In this work, the acidic sites of Pd-based catalysts are modified by introducing transition metals (Cr, Mo, W) to promote the cleavage of C-H bonds and therefore to enhance the catalytic oxidation performance of methane. The oxygen vacancies, acidity and redox property of prepared catalysts are systematically characterized by XRD, Raman, H2-TPR and NH3-TPD techniques. The results show that, the transition metal modification increases the acidic site of Pd catalysts obviously, and the modified PdM catalysts have a higher amount of oxygen vacancies. However, only Mo modified PdMo catalyst exhibits better redox performance, while Cr and W modified PdCr and PdW catalysts show slightly lower redox performance. The results of the methane oxidation reaction confirm that the PdMo catalyst with moderate acidic sites displays excellent performance in the methane oxidation reaction, and its T90 decreases by about 150 ℃, while the PdCr and PdW catalysts with more and less acidic sites show lower methane oxidation activity. The results indicate that the number of acid sites and the redox properties of the catalyst jointly determine the methane oxidation performance. This conclusion provides critical insights for design and preparation of catalysts for complete oxidation of methane at low temperatures.
| 科 Family | 属数 Number of genus | 种数 Number of species | 占总种数比例 Percentage of total species (%) | 属 Genus | 种数 Number of species | 占总种数比例 Percentage of total species (%) |
|---|---|---|---|---|---|---|
| 鹅膏菌科Amanitaceae | 2 | 11 | 5.26 | 鹅膏菌属 Amanita | 10 | 4.78 |
| 小菇科 Mycenaceae | 2 | 12 | 5.74 | 丝盖伞属 Inocybe | 5 | 2.39 |
| 多孔菌科 Polyporaceae | 8 | 14 | 6.70 | 蜡蘑属 Laccaria | 5 | 2.39 |
| 红菇科 Russulaceae | 3 | 23 | 11.00 | 小皮伞属 Marasmius | 6 | 2.87 |
| 小菇属 Mycena | 11 | 5.26 | ||||
| 光柄菇属 Pluteus | 5 | 2.39 | ||||
| 红菇属 Russula | 17 | 8.13 | ||||
| 栓菌属 Trametes | 5 | 2.39 |