La2O3助剂对CH4部分氧化制氢Ni-Cu/ZrSiO催化剂的影响
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Abstract
ZrO2-SiO2 (ZrSiO) supported Ni-Cu-La2O3 catalyst for CH4 partial oxidation to produce hydrogen was prepared by isovolumetric impregnation. By using TPR, XPS, IR, TPD and microreactor techniques, the effect of La2O3 on adsorption and reaction of CH4 with H2O and O2 on the catalyst were studied. The results showed that the addition of La2O3 has obvious influence on the electronic charge distribution of metal active sites Ni, Cu on Ni-Cu/ZrSiO catalyst, and increases the chemisorption intensity of CH4 and H2O. The main reaction products of CH4 partial oxidation with H2O and O2 on Ni-Cu-La2O3/ZrSiO catalyst are H2 and CO2. Under condition of 450 ℃, nCH4∶nO2∶nH2O=1∶0-5∶2-5 and SV(CH4)=1 200 h-1, conversion of CH4 (xCH4) is greater than 90%, selectivity of H2 (SH2) is more than 99%, and SCO is merely 1.% on Ni-Cu-La2O3/MgSiO catalyst. Moreover, the catalysis mechanism of promoter La2O3 was discussed.
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