The effect of Zr on the catalytic performance of Pd/y-A1203 for the methane combustion was investigated. The results show that the addition of Zr can improve the activity and stability of Pd/γ-Al2O3 catalyst, which, ...The effect of Zr on the catalytic performance of Pd/y-A1203 for the methane combustion was investigated. The results show that the addition of Zr can improve the activity and stability of Pd/γ-Al2O3 catalyst, which, based on the catalyst characterization (N2 adsorption, XRD, CO- Chemisorption, XPS, CHa-TPR and O2-TPO), is ascribed to the interaction between Pd and Zr. The active phase of methane combustion over supported palladium catalyst is the Pd^0/Pd^2+ mixture. Zr addition inhibits Pd aggregation and enhances the redox properties of active phase Pd^0/ Pd^2+. H2 reduction could effectively reduce the oxidation degree of Pd species and regenerate the active sites (Pd^0/ pd^2+).展开更多
The organic matter degradation process during anaerobic co-digestion of municipal biomass waste (MBW) and waste-activated sludge (WAS) under different organic loading rates (OLRs) was investigated in bench-scale...The organic matter degradation process during anaerobic co-digestion of municipal biomass waste (MBW) and waste-activated sludge (WAS) under different organic loading rates (OLRs) was investigated in bench-scale and pilot-scale semi-continuous stirred tank reactors. To better understand the degradation process of MBW and WAS co-digestion and provide theoretical guidance for engineering application, anaerobic digestion model No. 1 was revised for the co-digestion of MBW and WAS. The results showed that the degradation of organic matter could be characterized into three different fractions, including readily hydrolyzable organics, easily degradable particulate organics, and recalcitrant particle organics. Hydrolysis was the rate-limiting step under lower OLRs, and methanogenesisis was the rate-limiting step for an OLR of 8.0 kg volatile solid (VS)/(m^3·day). The hydrolytic parameters of carbohydrate, protein, and lipids were 0.104, 0.083, and 0.084 kg chemical oxygen demand (COD)/(kg COD·hr), respectively, and the reaction rate parameters of lipid fermentation were 1 and 1.25 kg COD/(kg COD.hr) for OLRs of 4.0 and 6.0 kg VS/(m^3·day). A revised model was used to simulate methane yield, and the results fit well with the experimental data. Material balance data were acquired based on the revised model, which showed that 58.50% of total COD was converted to methane.展开更多
Activity and stability of 1%Pd-0.2%Pt/Al2O3 and 1%Pd-0.2%Pt/0.6%Ce/Al2O3 catalysts prepared by impregnation method for catalytic combustion of methane in air were investigated. The catalysts before and after reaction ...Activity and stability of 1%Pd-0.2%Pt/Al2O3 and 1%Pd-0.2%Pt/0.6%Ce/Al2O3 catalysts prepared by impregnation method for catalytic combustion of methane in air were investigated. The catalysts before and after reaction were characterized by BET, CO chemisorption, XRD and XPS techniques. Results showed that the presence of Ce significantly increased the activity and thermal stability of the Pd-Pt/Al2O3 catalyst towards methane combustion, which could be attributed to more highly-dispersed active PdO particles over the Pd-Pt/Ce/Al2O3 catalyst surface as well as the retarded sintering of PdO and the maintained oxidized state of surface Pd during the combustion process in the presence of Ce.展开更多
Effects of carrier gas composition(N2/air) on NH3 production, energy efficiency regarding NH3 production and byproducts formation from plasma-catalytic decomposition of urea were systematically investigated using an...Effects of carrier gas composition(N2/air) on NH3 production, energy efficiency regarding NH3 production and byproducts formation from plasma-catalytic decomposition of urea were systematically investigated using an Al2 O3-packed dielectric barrier discharge(DBD) reactor at room temperature. Results show that the presence of O2 in the carrier gas accelerates the conversion of urea but leads to less generation of NH3. The final yield of NH3 in the gas phase decreased from 70.5%, 78.7%, 66.6% and 67.2% to 54.1%, 51.7%, 49.6% and 53.4% for applied voltages of 17, 19, 21 and 23 kV, respectively when air was used as the carrier gas instead of N2.From the viewpoint of energy savings, however, air carrier gas is better than N2 due to reduced energy consumption and increased energy efficiency for decomposition of a fixed amount of urea. Carrier gas composition has little influence on the major decomposition pathways of urea under the synergetic effects of plasma and Al2 O3 catalyst to give NH3 and CO2 as the main products. Compared to a small amount of N2 O formed with N2 as the carrier gas, however,more byproducts including N2O and NO2 in the gas phase and NH4 NO3 in solid deposits were produced with air as the carrier gas, probably due to the unproductive consumption of NH3, the possible intermediate HNCO and even urea by the abundant active oxygen species and nitrogen oxides generated in air-DBD plasma.展开更多
A group parameter approach using "total organic halogen" is effective for monitoring gaseous organic halogen compounds, including fluorine, chlorine, and bromine compounds, generated from combustion. We described th...A group parameter approach using "total organic halogen" is effective for monitoring gaseous organic halogen compounds, including fluorine, chlorine, and bromine compounds, generated from combustion. We described the use of barrier-discharge radiofrequency- helium-plasma/atomic emission spectrometry, for the detection of semi- and low-volatile organic halogen compounds (SLVOXs), which can be collected by CarbotrapTM adsorbents and analyzed using thermal desorpfion. The optimal carder gas flow rates at the injection and desorption lines were established to be 100 mL/min. The detection range for SLVOXs in the gaseous samples was from 10 ng to tens of micrograms. Measuring F was more difficult than measuring C1 or Br, because the wavelength of F is close to that of air. The barrier- discharge radiofrequency-helium-plasma/atomic emission spectrometry measured from 85% to 103% of the SLVOXs in the gas sample. It has been found that Carbotrap B is appropriate for high-boiling-point compounds, and Carbotrap C is suitable for the determination of organic halogen compounds with lower boiling points, in the range 200-230℃. Under optimal analysis conditions, a chlorine- containing plastic was destroyed using different oxygen concentrations. Lower oxygen concentrations resulted in the production of lower amounts of organic halogen compounds.展开更多
Exfoliated graphite(EG)is promising oil sorbent as well as an intermediate product for the preparation of flexible graphite films(FGFs).It has been a critical challenge to energy conservation and pollution abatement f...Exfoliated graphite(EG)is promising oil sorbent as well as an intermediate product for the preparation of flexible graphite films(FGFs).It has been a critical challenge to energy conservation and pollution abatement for the traditional EG production technique.Here,we propose a simple and effective preparation method to acquire EG in which flake graphite is intercalated and exfoliated at room temperature,not involving any pollutant emission.The influence factors in the preparation process were explored,such as the amount of H_(2)SO_(4)and H_(2)O_(2),the temperature for the preparation of room temperature exfoliated graphite(RTEG).In contrast to the EG by high temperature exfoliation(HTEG),RTEG exhibits a homogeneous structure and a significantly increased volume and surface area.Moreover,EG blocks with high oil sorption capacity and excellent reuse performance can be obtained by RTEG method.Especially,FGFs fabricated by RTEG has high flexibility,thermal conductivity and electrical conductivity.It suggests that this environment-friendly technology is suitable for large-scale industrial implementation of graphite-based oil sorbents and flexible materials.展开更多
基金Acknowledgements This research was supported by the National High Technology Research and Development Program of China (Nos. 2010AA064904 and 2012AA062702) and the National Natural Science Foundation of China (Grant No. 21177006).
文摘The effect of Zr on the catalytic performance of Pd/y-A1203 for the methane combustion was investigated. The results show that the addition of Zr can improve the activity and stability of Pd/γ-Al2O3 catalyst, which, based on the catalyst characterization (N2 adsorption, XRD, CO- Chemisorption, XPS, CHa-TPR and O2-TPO), is ascribed to the interaction between Pd and Zr. The active phase of methane combustion over supported palladium catalyst is the Pd^0/Pd^2+ mixture. Zr addition inhibits Pd aggregation and enhances the redox properties of active phase Pd^0/ Pd^2+. H2 reduction could effectively reduce the oxidation degree of Pd species and regenerate the active sites (Pd^0/ pd^2+).
基金supported by the Ministry of Science and Technology of China (No.2010DFA22770)the National Science and Technology Support Program of China (No.2010BAC66B04)the Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province (No.AE201003)
文摘The organic matter degradation process during anaerobic co-digestion of municipal biomass waste (MBW) and waste-activated sludge (WAS) under different organic loading rates (OLRs) was investigated in bench-scale and pilot-scale semi-continuous stirred tank reactors. To better understand the degradation process of MBW and WAS co-digestion and provide theoretical guidance for engineering application, anaerobic digestion model No. 1 was revised for the co-digestion of MBW and WAS. The results showed that the degradation of organic matter could be characterized into three different fractions, including readily hydrolyzable organics, easily degradable particulate organics, and recalcitrant particle organics. Hydrolysis was the rate-limiting step under lower OLRs, and methanogenesisis was the rate-limiting step for an OLR of 8.0 kg volatile solid (VS)/(m^3·day). The hydrolytic parameters of carbohydrate, protein, and lipids were 0.104, 0.083, and 0.084 kg chemical oxygen demand (COD)/(kg COD·hr), respectively, and the reaction rate parameters of lipid fermentation were 1 and 1.25 kg COD/(kg COD.hr) for OLRs of 4.0 and 6.0 kg VS/(m^3·day). A revised model was used to simulate methane yield, and the results fit well with the experimental data. Material balance data were acquired based on the revised model, which showed that 58.50% of total COD was converted to methane.
基金supported by the National High Technology Research and Development Program (863) of China (No.2010AA064904)
文摘Activity and stability of 1%Pd-0.2%Pt/Al2O3 and 1%Pd-0.2%Pt/0.6%Ce/Al2O3 catalysts prepared by impregnation method for catalytic combustion of methane in air were investigated. The catalysts before and after reaction were characterized by BET, CO chemisorption, XRD and XPS techniques. Results showed that the presence of Ce significantly increased the activity and thermal stability of the Pd-Pt/Al2O3 catalyst towards methane combustion, which could be attributed to more highly-dispersed active PdO particles over the Pd-Pt/Ce/Al2O3 catalyst surface as well as the retarded sintering of PdO and the maintained oxidized state of surface Pd during the combustion process in the presence of Ce.
基金supported by the National Natural Science Foundation of China (Nos. 21547004, 51638001)the Beijing Natural Science Foundation (No. 8152011)the Scientific Research Program of Beijing Municipal Education Commission (No. KM201510005009)
文摘Effects of carrier gas composition(N2/air) on NH3 production, energy efficiency regarding NH3 production and byproducts formation from plasma-catalytic decomposition of urea were systematically investigated using an Al2 O3-packed dielectric barrier discharge(DBD) reactor at room temperature. Results show that the presence of O2 in the carrier gas accelerates the conversion of urea but leads to less generation of NH3. The final yield of NH3 in the gas phase decreased from 70.5%, 78.7%, 66.6% and 67.2% to 54.1%, 51.7%, 49.6% and 53.4% for applied voltages of 17, 19, 21 and 23 kV, respectively when air was used as the carrier gas instead of N2.From the viewpoint of energy savings, however, air carrier gas is better than N2 due to reduced energy consumption and increased energy efficiency for decomposition of a fixed amount of urea. Carrier gas composition has little influence on the major decomposition pathways of urea under the synergetic effects of plasma and Al2 O3 catalyst to give NH3 and CO2 as the main products. Compared to a small amount of N2 O formed with N2 as the carrier gas, however,more byproducts including N2O and NO2 in the gas phase and NH4 NO3 in solid deposits were produced with air as the carrier gas, probably due to the unproductive consumption of NH3, the possible intermediate HNCO and even urea by the abundant active oxygen species and nitrogen oxides generated in air-DBD plasma.
基金Acknowledgements This research was supported by the National Natural Science Foundation of China (Grant Nos. 21277010 and 51078013), Special Research Funding for Public Benefit Industries from National Ministry of Environmental Protection (No. 201209005), the National Science and Technology Support Program of China (No. 2010BAC66B04), and Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province (No. AE201003).
基金supported by the National Natural Science Foundation of China (No. 21277010, 51078013)the National Science and Technology Support Program of China (No. 2010BAC66B04)+1 种基金the Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province (No. AE201003)the Key Laboratory for Solid Waste Management and Environment Safety,Ministry of Education of China (No. SWMES 2010-05)
文摘A group parameter approach using "total organic halogen" is effective for monitoring gaseous organic halogen compounds, including fluorine, chlorine, and bromine compounds, generated from combustion. We described the use of barrier-discharge radiofrequency- helium-plasma/atomic emission spectrometry, for the detection of semi- and low-volatile organic halogen compounds (SLVOXs), which can be collected by CarbotrapTM adsorbents and analyzed using thermal desorpfion. The optimal carder gas flow rates at the injection and desorption lines were established to be 100 mL/min. The detection range for SLVOXs in the gaseous samples was from 10 ng to tens of micrograms. Measuring F was more difficult than measuring C1 or Br, because the wavelength of F is close to that of air. The barrier- discharge radiofrequency-helium-plasma/atomic emission spectrometry measured from 85% to 103% of the SLVOXs in the gas sample. It has been found that Carbotrap B is appropriate for high-boiling-point compounds, and Carbotrap C is suitable for the determination of organic halogen compounds with lower boiling points, in the range 200-230℃. Under optimal analysis conditions, a chlorine- containing plastic was destroyed using different oxygen concentrations. Lower oxygen concentrations resulted in the production of lower amounts of organic halogen compounds.
文摘Exfoliated graphite(EG)is promising oil sorbent as well as an intermediate product for the preparation of flexible graphite films(FGFs).It has been a critical challenge to energy conservation and pollution abatement for the traditional EG production technique.Here,we propose a simple and effective preparation method to acquire EG in which flake graphite is intercalated and exfoliated at room temperature,not involving any pollutant emission.The influence factors in the preparation process were explored,such as the amount of H_(2)SO_(4)and H_(2)O_(2),the temperature for the preparation of room temperature exfoliated graphite(RTEG).In contrast to the EG by high temperature exfoliation(HTEG),RTEG exhibits a homogeneous structure and a significantly increased volume and surface area.Moreover,EG blocks with high oil sorption capacity and excellent reuse performance can be obtained by RTEG method.Especially,FGFs fabricated by RTEG has high flexibility,thermal conductivity and electrical conductivity.It suggests that this environment-friendly technology is suitable for large-scale industrial implementation of graphite-based oil sorbents and flexible materials.