In the present study,we synthesized CeO2 catalysts doped with various transition metals(M=Co,Fe,or Cu)using a supercritical water hydrothermal route,which led to the incorporation of the metal ions in the CeO2 lattice...In the present study,we synthesized CeO2 catalysts doped with various transition metals(M=Co,Fe,or Cu)using a supercritical water hydrothermal route,which led to the incorporation of the metal ions in the CeO2 lattice,forming solid solutions.The catalysts were then used for the selective catalytic reduction(SCR)of NO by CO.The Cu‐doped catalyst exhibited the highest SCR activity;it had a T50(i.e.,50%NO conversion)of only 83°C and a T90(i.e.,90%NO conversion)of 126°C.Such an activity was also higher than in many state‐of‐the‐art catalysts.In situ diffuse reflectance Fourier transform infrared spectroscopy suggested that the MOx‐CeO2 catalysts(M=Co and Fe)mainly followed an Eley‐Rideal reaction mechanism for CO‐SCR.In contrast,a Langmuir‐Hinshelwood SCR reaction mechanism occurred in CuO‐CeO2 owing to the presence of Cu+species,which ensured effective adsorption of CO.This explains why CuO‐CeO2 exhibited the highest activity with regard to the SCR of NO by CO.展开更多
In this study, a hybrid process using non‐thermal plasma (NTP) and photocatalytic oxidation (PCO) was adopted for the degradation of gas‐phase toluene using TiO2 as the photocatalyst. To discover the synergetic effe...In this study, a hybrid process using non‐thermal plasma (NTP) and photocatalytic oxidation (PCO) was adopted for the degradation of gas‐phase toluene using TiO2 as the photocatalyst. To discover the synergetic effect between NTP and PCO, the performances of both sole (O3, UV, NTP, and PCO) and combined (O3 + TiO2, O3 + UV, NTP + UV, O3 + PCO, and NTP + PCO) processes were investigated from different perspectives, such as the toluene removal efficiency, selectivity of COx, mineralization rate, ozone utilization, and the generation of by‐products. The toluene removal efficiency of the combined NTP + PCO process was 80.2%, which was much higher than that of a sole degradation process such as NTP (18.8%) and PCO (13.4%). The selectivity of CO2 and the ozone utilization efficiency also significantly improved. The amount of by‐products in the gas phase and the carbon‐ based intermediates adsorbed on the catalyst surface dramatically reduced. The improvement in the overall performances of the combined NTP + PCO process was mainly ascribed to the efficient utilization of ozone in the photocatalytic oxidation, and the ozone further acting as an electron acceptor and scavenger, generating more hydroxyl radicals and reducing the recombination of electron‐ hole pairs.展开更多
α‐,β‐,γ‐andδ‐MnO2catalysts were synthesized by a one‐step hydrothermal method,and were utilized for the catalytic oxidation of toluene in a combined plasma‐catalytic process.The relationship between catalyti...α‐,β‐,γ‐andδ‐MnO2catalysts were synthesized by a one‐step hydrothermal method,and were utilized for the catalytic oxidation of toluene in a combined plasma‐catalytic process.The relationship between catalytic performance and MnO2crystal structures was investigated.It was noted that the toluene removal efficiency was32.5%at the specific input energy of160J/L when non‐thermal plasma was used alone.Theα‐MnO2catalyst showed the best activity among the investigated catalysts,yielding a toluene conversion of78.1%at the specific input energy of160J/L.Forβ‐MnO2,γ‐MnO2andδ‐MnO2,removal efficiencies of47.4%,66.1%and50.0%,respectively,were achieved.By powder X‐ray diffraction,Raman spectroscopy,transmission electron microscopy,scanning electron microscopy,Brunauer‐Emmett‐Teller,H2temperature‐programmed reduction and X‐ray photoelectron spectroscopy analyses,it was concluded that the tunnel structure,the stability of the crystal in plasma,the Mn-O bond strength of MnO2and the surface‐chemisorbed oxygen species played important roles in the plasma‐catalytic degradation of toluene.Additionally,the degradation routes of toluene in non‐thermal plasma and in the plasma‐catalytic process were also studied.It was concluded that the introduction of MnO2catalysts enabled O3,O2,electrons and radical species in the gas to be adsorbed on the MnO2surface via a facile interconversion among the Mn4+,Mn3+and Mn2+states.These four species could then be transported to the toluene or intermediate organic by‐products,which greatly improved the toluene removal efficiency and decreased the final output of by‐products.展开更多
A sample of sulfated anatase TiO2 with high‐energy(001)facets(TiO2‐001)was prepared by a simple one‐step hydrothermal route using SO42-as a morphology‐controlling agent.After doping ceria,Ce/TiO2‐001 was used as ...A sample of sulfated anatase TiO2 with high‐energy(001)facets(TiO2‐001)was prepared by a simple one‐step hydrothermal route using SO42-as a morphology‐controlling agent.After doping ceria,Ce/TiO2‐001 was used as the catalyst for selective catalytic reduction(SCR)of NO with NH3.Compared with Ce/P25(Degussa P25 TiO2)and Ce/P25‐S(sulfated P25)catalysts,Ce/TiO2‐001 was more suitable for medium‐and high‐temperature SCR of NO due to the high surface area,sulfation,and the excellent properties of the active‐energy(001)facets.All of these facilitated the generation of abundant acidity,chemisorbed oxygen,and activated NOx‐adsorption species,which were the important factors for the SCR reaction.展开更多
文摘In the present study,we synthesized CeO2 catalysts doped with various transition metals(M=Co,Fe,or Cu)using a supercritical water hydrothermal route,which led to the incorporation of the metal ions in the CeO2 lattice,forming solid solutions.The catalysts were then used for the selective catalytic reduction(SCR)of NO by CO.The Cu‐doped catalyst exhibited the highest SCR activity;it had a T50(i.e.,50%NO conversion)of only 83°C and a T90(i.e.,90%NO conversion)of 126°C.Such an activity was also higher than in many state‐of‐the‐art catalysts.In situ diffuse reflectance Fourier transform infrared spectroscopy suggested that the MOx‐CeO2 catalysts(M=Co and Fe)mainly followed an Eley‐Rideal reaction mechanism for CO‐SCR.In contrast,a Langmuir‐Hinshelwood SCR reaction mechanism occurred in CuO‐CeO2 owing to the presence of Cu+species,which ensured effective adsorption of CO.This explains why CuO‐CeO2 exhibited the highest activity with regard to the SCR of NO by CO.
基金supported by the National Key Research and Development Plan of China (2016YFC0204700)National Natural Science Foundation of China (NSFC-51578488)+3 种基金Zhejiang Provincial "151" Talents Program (2013)Key Project of Zhejiang Provincial Science and Technology Programthe Program for Zhejiang Leading Team of S&T Innovation (2013TD07)the Changjiang Scholar Incentive Program (2009)~~
文摘In this study, a hybrid process using non‐thermal plasma (NTP) and photocatalytic oxidation (PCO) was adopted for the degradation of gas‐phase toluene using TiO2 as the photocatalyst. To discover the synergetic effect between NTP and PCO, the performances of both sole (O3, UV, NTP, and PCO) and combined (O3 + TiO2, O3 + UV, NTP + UV, O3 + PCO, and NTP + PCO) processes were investigated from different perspectives, such as the toluene removal efficiency, selectivity of COx, mineralization rate, ozone utilization, and the generation of by‐products. The toluene removal efficiency of the combined NTP + PCO process was 80.2%, which was much higher than that of a sole degradation process such as NTP (18.8%) and PCO (13.4%). The selectivity of CO2 and the ozone utilization efficiency also significantly improved. The amount of by‐products in the gas phase and the carbon‐ based intermediates adsorbed on the catalyst surface dramatically reduced. The improvement in the overall performances of the combined NTP + PCO process was mainly ascribed to the efficient utilization of ozone in the photocatalytic oxidation, and the ozone further acting as an electron acceptor and scavenger, generating more hydroxyl radicals and reducing the recombination of electron‐ hole pairs.
基金supported by the National Key Research and Development Plan of China(2016YFC0204700)Zhejiang Provincial"151"Talents Program(2013)+2 种基金Key Project of Zhejiang Provincial Science and Technology Program,the Program for Zhejiang Leading Team of S&T Innovation(2013TD07)Special Program for Social Development of Key Science and Technology Project of Zhejiang Province(2014C03025)Changjiang Scholar Incentive Program(2009)~~
文摘α‐,β‐,γ‐andδ‐MnO2catalysts were synthesized by a one‐step hydrothermal method,and were utilized for the catalytic oxidation of toluene in a combined plasma‐catalytic process.The relationship between catalytic performance and MnO2crystal structures was investigated.It was noted that the toluene removal efficiency was32.5%at the specific input energy of160J/L when non‐thermal plasma was used alone.Theα‐MnO2catalyst showed the best activity among the investigated catalysts,yielding a toluene conversion of78.1%at the specific input energy of160J/L.Forβ‐MnO2,γ‐MnO2andδ‐MnO2,removal efficiencies of47.4%,66.1%and50.0%,respectively,were achieved.By powder X‐ray diffraction,Raman spectroscopy,transmission electron microscopy,scanning electron microscopy,Brunauer‐Emmett‐Teller,H2temperature‐programmed reduction and X‐ray photoelectron spectroscopy analyses,it was concluded that the tunnel structure,the stability of the crystal in plasma,the Mn-O bond strength of MnO2and the surface‐chemisorbed oxygen species played important roles in the plasma‐catalytic degradation of toluene.Additionally,the degradation routes of toluene in non‐thermal plasma and in the plasma‐catalytic process were also studied.It was concluded that the introduction of MnO2catalysts enabled O3,O2,electrons and radical species in the gas to be adsorbed on the MnO2surface via a facile interconversion among the Mn4+,Mn3+and Mn2+states.These four species could then be transported to the toluene or intermediate organic by‐products,which greatly improved the toluene removal efficiency and decreased the final output of by‐products.
基金supported by the National Key R&D Program of China(2016YFC0204100)the Zhejiang Provincial "151" Talents Program+1 种基金the Program for Zhejiang Leading Team of S&T Innovation(2013TD07)the Changjiang Scholar Incentive Program(2009)~~
文摘A sample of sulfated anatase TiO2 with high‐energy(001)facets(TiO2‐001)was prepared by a simple one‐step hydrothermal route using SO42-as a morphology‐controlling agent.After doping ceria,Ce/TiO2‐001 was used as the catalyst for selective catalytic reduction(SCR)of NO with NH3.Compared with Ce/P25(Degussa P25 TiO2)and Ce/P25‐S(sulfated P25)catalysts,Ce/TiO2‐001 was more suitable for medium‐and high‐temperature SCR of NO due to the high surface area,sulfation,and the excellent properties of the active‐energy(001)facets.All of these facilitated the generation of abundant acidity,chemisorbed oxygen,and activated NOx‐adsorption species,which were the important factors for the SCR reaction.