A mechanochemical redox reaction between KMnO4 and CoCl2 was developed to obtain a CoxMn1-xOy catalyst with a specific surface area of 479 m^2 g^-1,which was higher than that obtained using a co-precipitation(CP)metho...A mechanochemical redox reaction between KMnO4 and CoCl2 was developed to obtain a CoxMn1-xOy catalyst with a specific surface area of 479 m^2 g^-1,which was higher than that obtained using a co-precipitation(CP)method(34 m2 g^-1),sol-gel(SG)method(72 m^2 g^-1),or solution redox process(131 m^2 g^-1).During catalytic combustion,this CoxMn1-xOy catalyst exhibited better activity(T100 for propylene=~200℃)than the control catalysts obtained using the SG(325℃)or CP(450℃)methods.The mechanical action,mainly in the form of kinetic energy and frictional heating,may generate a high degree of interstitial porosity,while the redox reaction could contribute to good dispersion of cobalt and manganese species.Moreover,the as-prepared CoxMn1-xOy catalyst worked well in the presence of water vapor(H2O 4.2%,>60 h)or SO2(100 ppm)and at high temperature(400℃,>60 h).The structure MnO2·(CoOOH)2.93 was suggested for the current CoxMn1-xOy catalyst.This catalyst could be extended to the total oxidation of other typical hydrocarbons(T90=150°C for ethanol,T90=225°C for acetone,T90=250℃for toluene,T90=120℃for CO,and T90=540℃for CH4).Scale-up of the synthesis of CoxMn1-xOy catalyst(1 kg)can be achieved via ball milling,which may provide a potential strategy for real world catalysis.展开更多
文摘A mechanochemical redox reaction between KMnO4 and CoCl2 was developed to obtain a CoxMn1-xOy catalyst with a specific surface area of 479 m^2 g^-1,which was higher than that obtained using a co-precipitation(CP)method(34 m2 g^-1),sol-gel(SG)method(72 m^2 g^-1),or solution redox process(131 m^2 g^-1).During catalytic combustion,this CoxMn1-xOy catalyst exhibited better activity(T100 for propylene=~200℃)than the control catalysts obtained using the SG(325℃)or CP(450℃)methods.The mechanical action,mainly in the form of kinetic energy and frictional heating,may generate a high degree of interstitial porosity,while the redox reaction could contribute to good dispersion of cobalt and manganese species.Moreover,the as-prepared CoxMn1-xOy catalyst worked well in the presence of water vapor(H2O 4.2%,>60 h)or SO2(100 ppm)and at high temperature(400℃,>60 h).The structure MnO2·(CoOOH)2.93 was suggested for the current CoxMn1-xOy catalyst.This catalyst could be extended to the total oxidation of other typical hydrocarbons(T90=150°C for ethanol,T90=225°C for acetone,T90=250℃for toluene,T90=120℃for CO,and T90=540℃for CH4).Scale-up of the synthesis of CoxMn1-xOy catalyst(1 kg)can be achieved via ball milling,which may provide a potential strategy for real world catalysis.