The catalysts of iron-doped Mn-Ce/TiO2 （Fe-Mn-Ce/TiO2） prepared by sol-gel method were investigated for low temperature selective catalytic reduction （SCR） of NO with NH3. It was found that the NO conversion over ...The catalysts of iron-doped Mn-Ce/TiO2 （Fe-Mn-Ce/TiO2） prepared by sol-gel method were investigated for low temperature selective catalytic reduction （SCR） of NO with NH3. It was found that the NO conversion over Fe-Mn-Ce/TiO2 was obviously improved after iron doping compared with that over Mn-Ce/TiO2. Fe-Mn-Ce/TiO2 with the molar ratio of Fe/Ti = 0.1 exhibited the highest activity. The results showed that 96.8% NO conversion was obtained over Fe（0.1）-Mn-Ce/TiO2 at 180~C at a space velocity of 50,000 hr-1. Fe-Mn-Ce/TiO2 exhibited much higher resistance to H2O and SO2 than that of Mn-Ce/TiO2. The properties of the catalysts were characterized using X-ray diffraction （XRD）, N2 adsorption, temperature programmed desorption （NH3-TPD and NOx-TPD）, and X- ray photoelectron spectroscopy （XPS） techniques. BET, NH3-TPD and NOx-TPD results showed that the specific surface area and NH3 and NOx adsorption capacity of the catalysts increased with iron doping. It was known from XPS analysis that iron valence state on the surface of the catalysts were in Fe^3＋ state. The doping of iron enhanced the dispersion and oxidation state of Mn and Ce on the surface of the catalysts. The oxygen concentrations on the surface of the catalysts were found to increase after iron doping. Fe-Mn-Ce/TiO2 represented a promising catalyst for low temperature SCR of NO with NH3 in the presence of H20 and SO2.展开更多
This work examines the influence of preparation methods on the physicochemical properties and catalytic performance of MnOx‐CeO2 catalysts for selective catalytic reduction of NO by NH3 (NH3‐SCR) at low temperature....This work examines the influence of preparation methods on the physicochemical properties and catalytic performance of MnOx‐CeO2 catalysts for selective catalytic reduction of NO by NH3 (NH3‐SCR) at low temperature. Five different methods, namely, mechanical mixing, impregnation,hydrothermal treatment, co‐precipitation, and a sol‐gel technique, were used to synthesizeMnOx‐CeO2 catalysts. The catalysts were characterized in detail, and an NH3‐SCR model reaction waschosen to evaluate the catalytic performance. The results showed that the preparation methodsaffected the catalytic performance in the order: hydrothermal treatment > sol‐gel > co‐precipitation> impregnation > mechanical mixing. This order correlated with the surface Ce3+ and Mn4+ content,oxygen vacancies and surface adsorbed oxygen species concentration, and the amount of acidic sitesand acidic strength. This trend is related to redox interactions between MnOx and CeO2. The catalystformed by a hydrothermal treatment exhibited excellent physicochemical properties, optimal catalyticperformance, and good H2O resistance in NH3‐SCR reaction. This was attributed to incorporationof Mnn+ into the CeO2 lattice to form a uniform ceria‐based solid solution (containing Mn‐O‐Cestructures). Strengthening of the electronic interactions between MnOx and CeO2, driven by thehigh‐temperature and high‐pressure conditions during the hydrothermal treatment also improved the catalyst characteristics. Thus, the hydrothermal treatment method is an efficient and environment‐friendly route to synthesizing low‐temperature denitrification (deNOx) catalysts.展开更多
Formaldehyde（HCHO）is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The developme...Formaldehyde（HCHO）is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The development of highly efficient and stable catalysts that can completely convert HCHO at low temperatures,even room temperature,is important.Supported Pt and Pd catalysts can completely convert HCHO at room temperature,but their industrial applications are limited because they are expensive.The catalytic activities in HCHO oxidation of transition-metal oxide catalysts such as manganese and cobalt oxides with unusual morphologies are better than those of traditional MnO2,Co3O4,or other metal oxides.This is attributed to their specific structures,high specific surface areas,and other factors such as active phase,reducibility,and amount of surface active oxygens.Such catalysts with various morphologies have great potential and can also be used as catalyst supports.The loading of relatively cheap Ag or Au on transition-metal oxides with special morphologies potentially improves the catalytic activity in HCHO removal at room temperature.The preparation and development of new nanocatalysts with various morphologies and structures is important for HCHO removal.In this paper,research progress on precious-metal and transition-metal oxide catalyst systems for HCHO oxidation is reviewed; topics such as oxidation properties,structure–activity relationships,and factors influencing the catalytic activity and reaction mechanism are discussed.Future prospects and directions for the development of such catalysts are also covered.展开更多
A detailed thermodynamic and techno-economic comparison is presented for a CO2-based transcritical Rankine cycle and a subcritical organic Rankine cycle (ORC) using HFC245fa (1,1,1,3,3-pentafluoro-propane) as the work...A detailed thermodynamic and techno-economic comparison is presented for a CO2-based transcritical Rankine cycle and a subcritical organic Rankine cycle (ORC) using HFC245fa (1,1,1,3,3-pentafluoro-propane) as the working fluid driven by the low-temperature geothermal source,in order to determine the configuration that presents the maximum net power output with a minimum investment.The evaluations of both Rankine cycles have been performed based on equal thermodynamic mean heat rejection temperature by varying certain system operating parameters to achieve each Rankine cycle's optimum design at various geothermal source temperature levels ranging from 80oC to 120oC.The results obtained show that the optimum ther-modynamic mean heat injection temperatures of both Rankine cycles are distributed in the scope of 55% to 65% of a given geothermal source temperature level,and that the CO2-based transcritical Rankine cycle presents 3% to 7% higher net power output,84% reduction of turbine inlet volume flow rate,47% reduction of expansion ratio and 1.68 times higher total heat transfer capacity compared with the HFC245fa-based subcritical ORC.It is also indicated that using the CO2-based transcritical system can reduce the dimension of turbine design.However,it requires larger heat transfer areas with higher strength heat exchanger materials because of the higher system pressure.展开更多
基金supported by the National Natural Science Foundation of China (No. 90610018,50976050)the New Century Excellent Talents in University (No. NCET-07-0457)the National Key Technologies R&D Program of Tianjin (No. 09ZCKFSH01900)
文摘The catalysts of iron-doped Mn-Ce/TiO2 （Fe-Mn-Ce/TiO2） prepared by sol-gel method were investigated for low temperature selective catalytic reduction （SCR） of NO with NH3. It was found that the NO conversion over Fe-Mn-Ce/TiO2 was obviously improved after iron doping compared with that over Mn-Ce/TiO2. Fe-Mn-Ce/TiO2 with the molar ratio of Fe/Ti = 0.1 exhibited the highest activity. The results showed that 96.8% NO conversion was obtained over Fe（0.1）-Mn-Ce/TiO2 at 180~C at a space velocity of 50,000 hr-1. Fe-Mn-Ce/TiO2 exhibited much higher resistance to H2O and SO2 than that of Mn-Ce/TiO2. The properties of the catalysts were characterized using X-ray diffraction （XRD）, N2 adsorption, temperature programmed desorption （NH3-TPD and NOx-TPD）, and X- ray photoelectron spectroscopy （XPS） techniques. BET, NH3-TPD and NOx-TPD results showed that the specific surface area and NH3 and NOx adsorption capacity of the catalysts increased with iron doping. It was known from XPS analysis that iron valence state on the surface of the catalysts were in Fe^3＋ state. The doping of iron enhanced the dispersion and oxidation state of Mn and Ce on the surface of the catalysts. The oxygen concentrations on the surface of the catalysts were found to increase after iron doping. Fe-Mn-Ce/TiO2 represented a promising catalyst for low temperature SCR of NO with NH3 in the presence of H20 and SO2.
基金supported by the National Natural Science Foundation of China (No. 21507130)the Open Project Program of Beijing National Laboratory for Molecular Sciences (No. 20140142)+3 种基金the Open Project Program of Chongqing Key Laboratory of Environmental Materials and Remediation Technology from Chongqing University of Arts and Sciences (No. CEK1405)the Open Project Program of Jiangsu Key Laboratory of Vehicle Emissions Control (No. OVEC001)the Open Project Program of Chongqing Key Laboratory of Catalysis and Functional Organic Molecules from Chongqing Technology and Business University (1456029)the Chongqing Science & Technology Commission (Nos. cstc2016jcyj A0070, cstc2014pt-gc20002, cstckjcxljrc13)~~
文摘This work examines the influence of preparation methods on the physicochemical properties and catalytic performance of MnOx‐CeO2 catalysts for selective catalytic reduction of NO by NH3 (NH3‐SCR) at low temperature. Five different methods, namely, mechanical mixing, impregnation,hydrothermal treatment, co‐precipitation, and a sol‐gel technique, were used to synthesizeMnOx‐CeO2 catalysts. The catalysts were characterized in detail, and an NH3‐SCR model reaction waschosen to evaluate the catalytic performance. The results showed that the preparation methodsaffected the catalytic performance in the order: hydrothermal treatment > sol‐gel > co‐precipitation> impregnation > mechanical mixing. This order correlated with the surface Ce3+ and Mn4+ content,oxygen vacancies and surface adsorbed oxygen species concentration, and the amount of acidic sitesand acidic strength. This trend is related to redox interactions between MnOx and CeO2. The catalystformed by a hydrothermal treatment exhibited excellent physicochemical properties, optimal catalyticperformance, and good H2O resistance in NH3‐SCR reaction. This was attributed to incorporationof Mnn+ into the CeO2 lattice to form a uniform ceria‐based solid solution (containing Mn‐O‐Cestructures). Strengthening of the electronic interactions between MnOx and CeO2, driven by thehigh‐temperature and high‐pressure conditions during the hydrothermal treatment also improved the catalyst characteristics. Thus, the hydrothermal treatment method is an efficient and environment‐friendly route to synthesizing low‐temperature denitrification (deNOx) catalysts.
基金supported by the National Natural Science Foundation of China(21325731,51478241,21221004)~~
文摘Formaldehyde（HCHO）is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The development of highly efficient and stable catalysts that can completely convert HCHO at low temperatures,even room temperature,is important.Supported Pt and Pd catalysts can completely convert HCHO at room temperature,but their industrial applications are limited because they are expensive.The catalytic activities in HCHO oxidation of transition-metal oxide catalysts such as manganese and cobalt oxides with unusual morphologies are better than those of traditional MnO2,Co3O4,or other metal oxides.This is attributed to their specific structures,high specific surface areas,and other factors such as active phase,reducibility,and amount of surface active oxygens.Such catalysts with various morphologies have great potential and can also be used as catalyst supports.The loading of relatively cheap Ag or Au on transition-metal oxides with special morphologies potentially improves the catalytic activity in HCHO removal at room temperature.The preparation and development of new nanocatalysts with various morphologies and structures is important for HCHO removal.In this paper,research progress on precious-metal and transition-metal oxide catalyst systems for HCHO oxidation is reviewed; topics such as oxidation properties,structure–activity relationships,and factors influencing the catalytic activity and reaction mechanism are discussed.Future prospects and directions for the development of such catalysts are also covered.
基金supported by the National Natural Science Foundation of China (Grant No.50976079)
文摘A detailed thermodynamic and techno-economic comparison is presented for a CO2-based transcritical Rankine cycle and a subcritical organic Rankine cycle (ORC) using HFC245fa (1,1,1,3,3-pentafluoro-propane) as the working fluid driven by the low-temperature geothermal source,in order to determine the configuration that presents the maximum net power output with a minimum investment.The evaluations of both Rankine cycles have been performed based on equal thermodynamic mean heat rejection temperature by varying certain system operating parameters to achieve each Rankine cycle's optimum design at various geothermal source temperature levels ranging from 80oC to 120oC.The results obtained show that the optimum ther-modynamic mean heat injection temperatures of both Rankine cycles are distributed in the scope of 55% to 65% of a given geothermal source temperature level,and that the CO2-based transcritical Rankine cycle presents 3% to 7% higher net power output,84% reduction of turbine inlet volume flow rate,47% reduction of expansion ratio and 1.68 times higher total heat transfer capacity compared with the HFC245fa-based subcritical ORC.It is also indicated that using the CO2-based transcritical system can reduce the dimension of turbine design.However,it requires larger heat transfer areas with higher strength heat exchanger materials because of the higher system pressure.
