Cu-Mn, Cu-Mn-Ce, and Cu-Ce mixed-oxide catalysts were prepared by a citric acid sol-gel method and then characterized by XRD, BET, H_2-TPR and XPS analyses. Their catalytic properties were investigated in the toluene ...Cu-Mn, Cu-Mn-Ce, and Cu-Ce mixed-oxide catalysts were prepared by a citric acid sol-gel method and then characterized by XRD, BET, H_2-TPR and XPS analyses. Their catalytic properties were investigated in the toluene combustion reaction. Results showed that the Cu-Mn-Ce ternary mixed-oxide catalyst with 1:2:4 mole ratios had the highest catalytic activity, and 99% toluene conversion was achieved at temperatures below 220°C. In the Cu-Mn-Ce catalyst, a portion of Cu and Mn species entered into the Ce O2 fluorite lattice, which led to the formation of a ceria-based solid solution. Excess Cu and Mn oxides existed on the surface of the ceria-based solid solution. The coexistence of Cu-Mn mixed oxides and the ceria-based solid solution resulted in a better synergetic interaction than the Cu-Mn and Cu-Ce catalysts, which promoted catalyst reducibility, increased oxygen mobility, and enhanced the formation of abundant active oxygen species.展开更多
The preparation of highly active supported noble metal catalysts with a low noble metal loading has always been the ultimate goal of researchers working on catalysis.Hydrothermally treated Pt/Al_(2)O_(3)(Pt/Al_(2)O_(3...The preparation of highly active supported noble metal catalysts with a low noble metal loading has always been the ultimate goal of researchers working on catalysis.Hydrothermally treated Pt/Al_(2)O_(3)(Pt/Al_(2)O_(3)-H)exhibits better catalytic activity than that(Pt/Al_(2)O_(3)-C)treated via the conventional calcination approach.At the high space velocity of100,000 m L/(g·hr),the temperature that correspond to 50%toluene conversion(T50)of Pt/Al_(2)O_(3)-H is 115℃ lower than that of Pt/Al_(2)O_(3)-C,and the turnover frequency(TOF)value can reach 0.0756 sec-1.The mechanism by which the hydrothermal approach enhances Pt/Al_(2)O_(3) activity has been investigated.The structure associated with the high catalytic activity of Pt nanoparticles(NPs)can be retained via hydrothermal treatment.Furthermore,the support is transformed to AlO(OH)with numerous surface hydroxyl groups,which in turn can facilitate the adsorption of toluene.And the synergistic effects of Pt NPs and AlO(OH)increases the contents of Pt in oxidation state and active oxygen,which are beneficial for toluene oxidation.展开更多
CeO2 is an important porous material with a wide range of applications in the abatement of volatile organic compounds (VOCs). In this paper, we prepared a series of novel three-dimensional (3D) micro/nanostructure...CeO2 is an important porous material with a wide range of applications in the abatement of volatile organic compounds (VOCs). In this paper, we prepared a series of novel three-dimensional (3D) micro/nanostructured CeO2 materials via a solvothermal method. Organic acid-assisted synthesis and inorganic acid post-treatment were used to adjust the Ce02 microstructures. The size of the 3D micro/nanostructures could be controlled in the range from 180nm to 1.5 μm and the surface morphology changed from rough to smooth with the use of different organic acids. The CeO2 synthesized with acetic acid featured a hierarchical porosity and showed good performance for toluene catalytic combustion: a T50 of 187 ℃ and a T90 of 195 ℃. Moreover, the crystallite size, textural properties, and surface chemical states could be tuned by inorganic acid modification. After treatment with HNO3, the modified CeO2 materials exhibited improved catalytic activity, with a T50 of-175 ℃ and a T90 of -187 ℃. We concluded that the toluene combustion activity is related to the porosity and the amount of surface active oxygen of the CeO2. Both these features can be tuned by the co-work of organic and inorganic acids.展开更多
基金the financial support from the Natural Science Foundation of China (No. 21107096)Zhejiang Provincial Natural Science Foundation of China (No. Y14E080008)+1 种基金the Commission of Science and Technology of Zhejiang province (No. 2013C03021)the Specialized Research Fund for the Doctoral Program of Higher Education (No. 20133317110004)
文摘Cu-Mn, Cu-Mn-Ce, and Cu-Ce mixed-oxide catalysts were prepared by a citric acid sol-gel method and then characterized by XRD, BET, H_2-TPR and XPS analyses. Their catalytic properties were investigated in the toluene combustion reaction. Results showed that the Cu-Mn-Ce ternary mixed-oxide catalyst with 1:2:4 mole ratios had the highest catalytic activity, and 99% toluene conversion was achieved at temperatures below 220°C. In the Cu-Mn-Ce catalyst, a portion of Cu and Mn species entered into the Ce O2 fluorite lattice, which led to the formation of a ceria-based solid solution. Excess Cu and Mn oxides existed on the surface of the ceria-based solid solution. The coexistence of Cu-Mn mixed oxides and the ceria-based solid solution resulted in a better synergetic interaction than the Cu-Mn and Cu-Ce catalysts, which promoted catalyst reducibility, increased oxygen mobility, and enhanced the formation of abundant active oxygen species.
基金supported by the National Natural Science Foundation of China(Nos.21506194,21676255)the Zhejiang Provincial Natural Science Foundation of China(Nos.LZ21E080001,2017C03007,2017C33106)。
文摘The preparation of highly active supported noble metal catalysts with a low noble metal loading has always been the ultimate goal of researchers working on catalysis.Hydrothermally treated Pt/Al_(2)O_(3)(Pt/Al_(2)O_(3)-H)exhibits better catalytic activity than that(Pt/Al_(2)O_(3)-C)treated via the conventional calcination approach.At the high space velocity of100,000 m L/(g·hr),the temperature that correspond to 50%toluene conversion(T50)of Pt/Al_(2)O_(3)-H is 115℃ lower than that of Pt/Al_(2)O_(3)-C,and the turnover frequency(TOF)value can reach 0.0756 sec-1.The mechanism by which the hydrothermal approach enhances Pt/Al_(2)O_(3) activity has been investigated.The structure associated with the high catalytic activity of Pt nanoparticles(NPs)can be retained via hydrothermal treatment.Furthermore,the support is transformed to AlO(OH)with numerous surface hydroxyl groups,which in turn can facilitate the adsorption of toluene.And the synergistic effects of Pt NPs and AlO(OH)increases the contents of Pt in oxidation state and active oxygen,which are beneficial for toluene oxidation.
基金This work was financially supported by the Natural Science Foundation of China (21576054), the Scientific Project of Guangdong Province (2014A010106030, 2016A010104017,2016B020241003), and the Foundation of Higher Education of Guangdong Province (201 SICFSCX027) of China.
文摘CeO2 is an important porous material with a wide range of applications in the abatement of volatile organic compounds (VOCs). In this paper, we prepared a series of novel three-dimensional (3D) micro/nanostructured CeO2 materials via a solvothermal method. Organic acid-assisted synthesis and inorganic acid post-treatment were used to adjust the Ce02 microstructures. The size of the 3D micro/nanostructures could be controlled in the range from 180nm to 1.5 μm and the surface morphology changed from rough to smooth with the use of different organic acids. The CeO2 synthesized with acetic acid featured a hierarchical porosity and showed good performance for toluene catalytic combustion: a T50 of 187 ℃ and a T90 of 195 ℃. Moreover, the crystallite size, textural properties, and surface chemical states could be tuned by inorganic acid modification. After treatment with HNO3, the modified CeO2 materials exhibited improved catalytic activity, with a T50 of-175 ℃ and a T90 of -187 ℃. We concluded that the toluene combustion activity is related to the porosity and the amount of surface active oxygen of the CeO2. Both these features can be tuned by the co-work of organic and inorganic acids.