A series of Co–Cr–O mixed oxides with different Co/Cr molar ratios are synthesized and tested for the total oxidation of propane.The reaction behaviors are closely related to the structural features of the mixed oxi...A series of Co–Cr–O mixed oxides with different Co/Cr molar ratios are synthesized and tested for the total oxidation of propane.The reaction behaviors are closely related to the structural features of the mixed oxides.The catalyst with a Co/Cr molar ratio of 1:2(1 Co2 Cr)and a spinel structure has the best activity(with a reaction rate of 1.38μmol g^–1 s^–1 at 250℃),which is attributed to the synergistic roles of its high surface acidity and good low-temperature reducibility,as evidenced by the temperature-programmed desorption of ammonia,reduction of hydrogen,and surface reaction of propane.Kinetic study shows that the reaction orders of propane and oxygen on the 1 Co2 Cr catalyst(0.58±0.03 and 0.34±0.05,respectively)are lower than those on the 2 Co1 Cr catalyst(0.77±0.02 and 0.98±0.16,respectively)and 1 Co5 Cr(0.66±0.05 and 1.30±0.11,respectively),indicating that the coverages of propane and oxygen on 1 Co2 Cr are higher than those on the other catalysts due to its higher surface acidity and higher reducibility.In addition,in-situ diffuse reflectance infrared spectroscopic investigation reveals that the main surface species on 1 Co2 Cr during the reaction are polydentate carbonate species,which accumulate on the surface at low temperatures(<250℃)but decompose at relatively high temperatures.展开更多
基金financially supported by the National Natural Science Foundation of China(21773212,21872124)~~
文摘A series of Co–Cr–O mixed oxides with different Co/Cr molar ratios are synthesized and tested for the total oxidation of propane.The reaction behaviors are closely related to the structural features of the mixed oxides.The catalyst with a Co/Cr molar ratio of 1:2(1 Co2 Cr)and a spinel structure has the best activity(with a reaction rate of 1.38μmol g^–1 s^–1 at 250℃),which is attributed to the synergistic roles of its high surface acidity and good low-temperature reducibility,as evidenced by the temperature-programmed desorption of ammonia,reduction of hydrogen,and surface reaction of propane.Kinetic study shows that the reaction orders of propane and oxygen on the 1 Co2 Cr catalyst(0.58±0.03 and 0.34±0.05,respectively)are lower than those on the 2 Co1 Cr catalyst(0.77±0.02 and 0.98±0.16,respectively)and 1 Co5 Cr(0.66±0.05 and 1.30±0.11,respectively),indicating that the coverages of propane and oxygen on 1 Co2 Cr are higher than those on the other catalysts due to its higher surface acidity and higher reducibility.In addition,in-situ diffuse reflectance infrared spectroscopic investigation reveals that the main surface species on 1 Co2 Cr during the reaction are polydentate carbonate species,which accumulate on the surface at low temperatures(<250℃)but decompose at relatively high temperatures.
