To deposit TiO2 films through plasma CVD, the partial pressure ratio of O2 to TIC14 should be greater than the stoichiometric ratio （PO2/PTiCl4 〉 1）. However, this may lead to the formation of powder instead of fil...To deposit TiO2 films through plasma CVD, the partial pressure ratio of O2 to TIC14 should be greater than the stoichiometric ratio （PO2/PTiCl4 〉 1）. However, this may lead to the formation of powder instead of film on the substrate when using volume dielectric barrier discharge （volume-DBD） at atmospheric pressure. In this study, by adding N2 into the working gas Ar, TiO2 photocatalytic films were successfully fabricated in the presence of excess O2 （PO2/PTiC14 = 2.6） by using a wire-to-plate atmospheric-pressure volume-DBD. The tuning effect of N2 on the deposition of TiO2 film was studied in detail. The results showed that by increasing the N2 content, the deposition rate and particle size of the TiO2 film were reduced, and its photocatalytic activity was enhanced. The tuning mechanism of N2 is further discussed.展开更多
Cold plasma generated by dielectric barrier discharge （DBD） at atmospheric pressure was adopted for preparation of commercial TiO2 Degussa P25 supported Au catalysts （Au/P25- P） with the assistance of the depositi...Cold plasma generated by dielectric barrier discharge （DBD） at atmospheric pressure was adopted for preparation of commercial TiO2 Degussa P25 supported Au catalysts （Au/P25- P） with the assistance of the deposition-precipitation procedure. The influences of the plasma reduction time and calcination on the performance of the Au/P25-P catalysts were investigated. CO oxidation was performed to investigate the catalytic activity of the Au/P25 catalysts. The results show that DBD cold plasma for the fabrication of Au/P25-P catalysts is a fast process, and Au/P25-P （4 min） exhibited the highest CO oxidation activity due to the complete reduction of Au compounds and less consumption of oxygen vacancies. In order to form more oxygen vacancies active species, Au/P25-P was calcined to obtain Au/P25-PC catalysts. Interestingly, Au/P25- PC exhibited the highest activity for CO oxidation among the Au/P25 samples. The results of transmission electron microscopy （TEM） indicated that the smaller size and high distribution of Au nanoparticles are the mean reasons for a high performance of Au/P25-PC. Atmospheric- pressure DBD cold plasma was proved to be of great efficiency in preparing high performance supported Au catalysts.展开更多
Dielectric barrier discharge （DBD） cold plasma at atmospheric pressure was used for preparation of copper nanoparticles by reduction of copper oxide （CuO）. Power X-ray diffraction （XRD） was used to characterize ...Dielectric barrier discharge （DBD） cold plasma at atmospheric pressure was used for preparation of copper nanoparticles by reduction of copper oxide （CuO）. Power X-ray diffraction （XRD） was used to characterize the structure of the copper oxide samples treated by DBD plasma. Influences of H2 content and the treating time on the reduction of copper oxide by DBD plasma were investigated. The results show that the reduction ratio of copper oxide was increased initially and then decreased with increasing H2 content, and the highest reduction ratio was achieved at 20% H2 content. Moreover, the copper oxide samples were gradually reduced by DBD plasma into copper nanoparticles with the increase in treating time. However, the average reduction rate was decreased as a result of the diffusion of the active hydrogen species. Optical emission spectra （OES） were observed during the reduction of the copper oxide samples by DBD plasma, and the reduction mechanism was explored accordingly. Instead of high-energy electrons, atomic hydrogen （H） radicals, and the heating effect, excited-state hydrogen molecules are suspected to be one kind of important reducing agents. Atmospheric-pressure DBD cold plasma is proved to be an efficient method for preparing copper nanoparticles.展开更多
As an important type of metal-organic framework(MOF),Zr-MOF shows excellent CO2 adsorption performance.In this work,a Zr-MOF was synthesized by a solvothennal method and adopted to support Ru through simple incipient-...As an important type of metal-organic framework(MOF),Zr-MOF shows excellent CO2 adsorption performance.In this work,a Zr-MOF was synthesized by a solvothennal method and adopted to support Ru through simple incipient-wetness impreg nation.Then the Ru/Zr-MOF was applied for CO2 hydrogenation(Vh2:VCO2=4:1)with the assistance of dielectric banner dischai'ge(DBD)plasma.The hydrogenation of Cd2 results showed that methane was produced selectively under the synergistic effect between plasma and the Ru/Zr-MOF catalyst,and the selectivity and yield of methane reached 94.6%and 39.1%,respectively.The XRD and SEM analyses indicate that the basic crystalline phase structure and morphology of the Zr-MOF and Ru/Zr-MOF remained the same after DBD plasma treatment,suggesting that the catalysts are stable in plasma.The guest molecules in the pores of the Zr-MOF are removed and the Ru"ions are reduced to metallic Ru()in the reduction atmosphere according to the BET and XPS results,which are responsible for the high performance of plasma with the Ru/Zr-MOF catalyst.In situ optical emission spectra of pure plasma,plasma with Zr-MOF,and plasma with Ru/Zr-MOF were measured,and the active species of C,H and CH for CO2 hydrogenation were detected.The plasma-assisted Ru/Zr-MOF exhibited high catalytic activity and stability in CO2 hydrogenation to methane,and it has great guiding significance for CO2 hydrogenation by using plasma and MOF materials.展开更多
基金supported by National Natural Science Foundation of China(Nos.10835004,51077009)the Fundamental Research Funds for the Central Universities
文摘To deposit TiO2 films through plasma CVD, the partial pressure ratio of O2 to TIC14 should be greater than the stoichiometric ratio （PO2/PTiCl4 〉 1）. However, this may lead to the formation of powder instead of film on the substrate when using volume dielectric barrier discharge （volume-DBD） at atmospheric pressure. In this study, by adding N2 into the working gas Ar, TiO2 photocatalytic films were successfully fabricated in the presence of excess O2 （PO2/PTiC14 = 2.6） by using a wire-to-plate atmospheric-pressure volume-DBD. The tuning effect of N2 on the deposition of TiO2 film was studied in detail. The results showed that by increasing the N2 content, the deposition rate and particle size of the TiO2 film were reduced, and its photocatalytic activity was enhanced. The tuning mechanism of N2 is further discussed.
基金supported by National Natural Science Foundation of China(Nos.11505019,21173028)the Science and Technology Research Project of Liaoning Provincial Education Department(No.L2013464)+1 种基金the Scientific Research Foundation for the Doctor of Liaoning Province(No.20131004)the Dalian Jinzhou New District Science and Technology Plan Project(No.KJCX-ZTPY-2014-0001)
文摘Cold plasma generated by dielectric barrier discharge （DBD） at atmospheric pressure was adopted for preparation of commercial TiO2 Degussa P25 supported Au catalysts （Au/P25- P） with the assistance of the deposition-precipitation procedure. The influences of the plasma reduction time and calcination on the performance of the Au/P25-P catalysts were investigated. CO oxidation was performed to investigate the catalytic activity of the Au/P25 catalysts. The results show that DBD cold plasma for the fabrication of Au/P25-P catalysts is a fast process, and Au/P25-P （4 min） exhibited the highest CO oxidation activity due to the complete reduction of Au compounds and less consumption of oxygen vacancies. In order to form more oxygen vacancies active species, Au/P25-P was calcined to obtain Au/P25-PC catalysts. Interestingly, Au/P25- PC exhibited the highest activity for CO oxidation among the Au/P25 samples. The results of transmission electron microscopy （TEM） indicated that the smaller size and high distribution of Au nanoparticles are the mean reasons for a high performance of Au/P25-PC. Atmospheric- pressure DBD cold plasma was proved to be of great efficiency in preparing high performance supported Au catalysts.
基金supported by National Natural Science Foundation of China(No.21173028)the Science and Technology Research Project of Liaoning Provincial Education Department of China(No.L2013464)the Scientific Research Foundation for the Doctor of Liaoning Province of China(No.20131004)
文摘Dielectric barrier discharge （DBD） cold plasma at atmospheric pressure was used for preparation of copper nanoparticles by reduction of copper oxide （CuO）. Power X-ray diffraction （XRD） was used to characterize the structure of the copper oxide samples treated by DBD plasma. Influences of H2 content and the treating time on the reduction of copper oxide by DBD plasma were investigated. The results show that the reduction ratio of copper oxide was increased initially and then decreased with increasing H2 content, and the highest reduction ratio was achieved at 20% H2 content. Moreover, the copper oxide samples were gradually reduced by DBD plasma into copper nanoparticles with the increase in treating time. However, the average reduction rate was decreased as a result of the diffusion of the active hydrogen species. Optical emission spectra （OES） were observed during the reduction of the copper oxide samples by DBD plasma, and the reduction mechanism was explored accordingly. Instead of high-energy electrons, atomic hydrogen （H） radicals, and the heating effect, excited-state hydrogen molecules are suspected to be one kind of important reducing agents. Atmospheric-pressure DBD cold plasma is proved to be an efficient method for preparing copper nanoparticles.
文摘As an important type of metal-organic framework(MOF),Zr-MOF shows excellent CO2 adsorption performance.In this work,a Zr-MOF was synthesized by a solvothennal method and adopted to support Ru through simple incipient-wetness impreg nation.Then the Ru/Zr-MOF was applied for CO2 hydrogenation(Vh2:VCO2=4:1)with the assistance of dielectric banner dischai'ge(DBD)plasma.The hydrogenation of Cd2 results showed that methane was produced selectively under the synergistic effect between plasma and the Ru/Zr-MOF catalyst,and the selectivity and yield of methane reached 94.6%and 39.1%,respectively.The XRD and SEM analyses indicate that the basic crystalline phase structure and morphology of the Zr-MOF and Ru/Zr-MOF remained the same after DBD plasma treatment,suggesting that the catalysts are stable in plasma.The guest molecules in the pores of the Zr-MOF are removed and the Ru"ions are reduced to metallic Ru()in the reduction atmosphere according to the BET and XPS results,which are responsible for the high performance of plasma with the Ru/Zr-MOF catalyst.In situ optical emission spectra of pure plasma,plasma with Zr-MOF,and plasma with Ru/Zr-MOF were measured,and the active species of C,H and CH for CO2 hydrogenation were detected.The plasma-assisted Ru/Zr-MOF exhibited high catalytic activity and stability in CO2 hydrogenation to methane,and it has great guiding significance for CO2 hydrogenation by using plasma and MOF materials.
