A titania support with a large surface area was developed, which has a BET surface area of 380.5 m^2/g, four times that of a traditional titania support. The support was ultrasonically impregnated with 5 wt% vanadia. ...A titania support with a large surface area was developed, which has a BET surface area of 380.5 m^2/g, four times that of a traditional titania support. The support was ultrasonically impregnated with 5 wt% vanadia. A special heat treatment was used in the calcination to maintain the large surface area and high dispersion of vanadium species. This catalyst was compared to a common V2O5-TiO2 catalyst with the same vanadia loading prepared by a traditional method. The new catalyst has a surface area of 117.7 m^2/g, which was 38% higher than the traditional V2O5-TiO2 catalyst. The selective catalytic reduction（SCR） performance demonstrated that the new catalyst had a wider temperature window and better N2 selectivity compared to the traditional one. The NO conversion was 80% from 200 to 450 °C. The temperature window was 100 °C wider than the traditional catalyst. Raman spectra indicated that the vanadium species formed more V-O-V linkages on the catalyst prepared by the traditional method. The amount of V-O-Ti and V=O was larger for the new catalyst. Temperature programmed desorption of NH3, temperature programmed reduction by H2 and X-ray photoelectron spectroscopy results showed that its redox ability and total acidity were enhanced. The results are helpful for developing a more efficient SCR catalyst for the removal of NOx in flue gases.展开更多
A study was conducted to determine the effects of elevated CO2 on soil N process at Changbai Mountain in Jilin Province, northeastern China （42°24＂N, 128°06＂E, and 738 m elevation）. A randomized complete...A study was conducted to determine the effects of elevated CO2 on soil N process at Changbai Mountain in Jilin Province, northeastern China （42°24＂N, 128°06＂E, and 738 m elevation）. A randomized complete block design of ambient and elevated CO2 was established in an open-top chamber facility in the spring of 1999. Changpai Scotch pine （Pinus sylvestris var. sylvestriformis seeds were sowed in May, 1999 and CO2 fumigation treatments began after seeds germination. In each year, the exposure started at the end of April and stopped at the end of October. Soil samples were collected in June and August 2006 and in June 2007, and soil nitrifying, denitrifying and N2-fixing enzyme activities were measured. Results show that soil nitrifying enzyme activities （NEA） in the 5-10 cm soil layer were significantly increased at elevated CO2 by 30.3% in June 2006, by 30.9% in August 2006 and by 11.3% in June 2007. Soil denitrifying enzyme activities （DEA） were significantly decreased by elevated CO2 treatment in June 2006 （P 〈 0.012） and August 2006 （P 〈 0.005） samplings in our study; no significant difference was detected in June 2007, and no significant changes in N2-fixing enzyme activity were found. This study suggests that elevated CO2 can alter soil nitrifying enzyme and denitrifying enzyme activities.展开更多
The hydrogenation of m-dinitrobenzene to m-phenylenediamine in liquid phase was studied with the nickel catalysts supported on SiO2, TiO2, γ-Al2O3, MgO and diatomite carders. Based on the experiments of X-ray diffrac...The hydrogenation of m-dinitrobenzene to m-phenylenediamine in liquid phase was studied with the nickel catalysts supported on SiO2, TiO2, γ-Al2O3, MgO and diatomite carders. Based on the experiments of X-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS）, temperature-programmed reduction （TPR）, temperature-programmed desorption of hydrogen （H2-TPD） and activity evaluation, the physico-chemical and catalytic properties of the catalysts were investigated. Among the catalysts tested, the SiO2 supported nickel catalyst showed the highest activity and selectivity towards m-phenylenediamine, over which 97.3% m-dinitrobenzene conversion and 95.1% m-phenylenediamine yield were obtained at 373K under hydrogen pressure of 2.6MPa after reaction for 6 h when using ethanol as solvent. Although TiO2 and diatomite supported nickel catalysts also presented high activity, they had lower selectivity towards m-phenylenediamine. As for γ-Al2O3 and MgO supported catalysts were almost inactive for the object reaction. It was shown that both the activity and selectivity of the catalysts were strongly depended on the interaction between nickel and the support. The higher activities of Ni/SiO2, Ni/TiO2 and Ni/diatomite could be attributed to the weaker metal-support interaction, on which Ni species presented as crystallized Ni metal particles. On the other hand, there existed strong metal-support interaction in Ni/MgO and Ni γ-Al2O3, which causes these catalysts more difficult to be reduced and the availability of Ni active sites decreased, resulting in their low catalytic activity.展开更多
Specific management of water regimes, soil and N in China might play an important role in regulating N2O and CH4 emissions in rice fields. Nitrous oxide and methane emissions from alternate non-flooded/flooded paddies...Specific management of water regimes, soil and N in China might play an important role in regulating N2O and CH4 emissions in rice fields. Nitrous oxide and methane emissions from alternate non-flooded/flooded paddies were monitored simultaneously during a 516-day incubation with lysimeter experiments. Two N sources (15N-(NH4)2SO4 and 15N-labeled milk vetch) were applied to two contrasting paddies: one derived from Xiashu loess (Loess) and one from Quaternary red clay (Clay). Both N2O and CH4 emissions were significantly higher in soil Clay than in soil Loess during the flooded period. For both soil, N2O emissions peaked at the transition periods shortly after the beginning of the flooded and non-flooded seasons. Soil type affected N2O emission patterns. In soil Clay, the emission peak during the transition period from non-flooded to flooded conditions was much higher than the peak during the transition period from flooded to non-flooded conditions. In soil Loess, the emission peak during the transition period from flooded to non-flooded conditions was obviously higher than the peak during the transition period from non-flooded to flooded conditions except for milk vetch treatment. Soil type also had a significant effect on CH4 emissions during the flooded season, over which the weighted average flux was 111 mg C m-2 h-1 and 2.2 mg C m-2 h-1 from Clay and Loess, respectively. Results indicated that it was the transition in the water regime that dominated N2O emissions while it was the soil type that dominated CH4 emissions during the flooded season. Anaerobic oxidation of methane possibly existed in soil Loess during the flooded season.展开更多
The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/TiO2 catalysts prepared by a liquid-phase chemical reduction method. The catalysts were characterized by inductively coupled plasm...The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/TiO2 catalysts prepared by a liquid-phase chemical reduction method. The catalysts were characterized by inductively coupled plasma (ICP), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS) and temperature-programmed reduction (TPR). Results show that the titania structure has favorable influence on physio-chemical and catalytic properties of Ni/TiO2 catalysts. Compared to commercial Raney nickel, the catalytic activity of Ni/TiO2 catalyst is much superior, irrespective of the titania structure. The catalytic activity of anatase titania supported nickel catalyst Ni/TiO2(A) is higher than that of rutile titania supported nickel catalyst Ni/TiO2(R), possibly because the reduction of nickel oxide to metallic nickel for Ni/TiO2(A) is easier than that for Ni/TiO2(R) at similar reaction conditions.展开更多
An experimental study of thermal de-NOx using NH3 as reductant in 02/C02 atmosphere with the effect of S02 and different additives was performed in a drop tube furnace. Results show that the optimum temperature win- d...An experimental study of thermal de-NOx using NH3 as reductant in 02/C02 atmosphere with the effect of S02 and different additives was performed in a drop tube furnace. Results show that the optimum temperature win- dow is 841-1184 ℃, and the optimum reaction temperature is about 900 ℃ with a de-NOx efficiency of 95.4%. A certain amount of S02 has an inhibiting effect on NO reduction. The effect of additives, including Na2C03, C2H5OH and FeCI3, on NO reduction by NH3 is also explored. The addition of Na2CO3 and FeCI3 is useful to widen the tem- perature window and shift the reaction to lower temperature for the efficiency is increased from 30.5% to 74.0% and 67.4% respectively at 800 ℃. Qualitatively, the modeling results using a detailed kinetic modeling mecha- nism represent well most of the process features. The effect of Na2CO3, C2H5OH and FeCI3 addition can be reproduced well by the Na2C03, C2H5OH and Fe（CO）5 sub-mechanism respectively. The reaction mechanism analysis shows that the effects of these additives on NO reduction are achieved mainly by promoting the produc- tion of OH radicals at lower temperature.展开更多
To feed an increasing population, large amounts of chemical nitrogen fertilizer have been used to produce much of our food, feed and fiber thereby increasing nitrogen levels in soils, natural waters, crop residues, li...To feed an increasing population, large amounts of chemical nitrogen fertilizer have been used to produce much of our food, feed and fiber thereby increasing nitrogen levels in soils, natural waters, crop residues, livestock wastes,and municipal and agricultural wastes, with national and international concern about its potential adverse effects on environmental quality and public health. To understand these phenomena and problems, first the nitrogen cycle and the environment are described. Then recent trends for nitrogen cycling through the food and feed system, N2O emissions from fertilized upland and paddy soils, and NO-3 pollution in ground water in Japan are reported. Finally, mitigation strategies in Japan for reducing N2O emission and NO-3 pollution are proposed, including nitrification inhibitors, controlled release fertilizers, utilization of plant species that could suppress nitrification, utilizing the toposequence, government policy, and appropriate agricultural practices. Of all the technologies presented, use of nitrification inhibitors and controlled release fertilizers are deemed the most important with further development of these aspects of technologies being expected. These practices, if employed worldwide, could help reduce the load, or environmental deterioration, on the Earth's biosphere.展开更多
Isolation of new bacterial strains and recognition of their metabolic activities are highly desirable for sustainability of natural ecosystems. Biodegradation of dimethyl phthalate （DMP） under anoxic conditions has ...Isolation of new bacterial strains and recognition of their metabolic activities are highly desirable for sustainability of natural ecosystems. Biodegradation of dimethyl phthalate （DMP） under anoxic conditions has been shown to occur as a series of sequential steps using strain CW-1 isolated from digested sludge of Sibao Wastewater Treatment Plant in Hangzhou, China. The microbial colony on LB medium was yellowish, 3-5 mm in diameter, convex in the center, and embedded in mucous externally. The individual cells of strain CW-1 are irregular rods, measuring （0.6-0.7）×（0.9-1.0） pm, V-shaped, with clubbed ends, Gram positive and without any filaments. 16S rDNA （ 1438 bp） sequence analysis showed that the strain was related to Arthrobacter sp. CW-1 and can degrade PAEs utilizing nitrate as electron acceptor, but cannot mineralize DMP completely. The degradation pathway was recommended as： dimethyl phthalate （DMP）→monomethyl phthalate （MMP）--,phthalic acid （PA）. DMP biodegradation was a first order reaction with degradation rate constant of 0.3033 d 1 and half-life 2.25 d. The DMP conversion to PA by CW-1 could be described by using sequential kinetic model.展开更多
基金supported by the National Natural Science Foundation of China(21325731,21221004)the National High Technology Research and Development Program of China(863 Program)the State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex
文摘A titania support with a large surface area was developed, which has a BET surface area of 380.5 m^2/g, four times that of a traditional titania support. The support was ultrasonically impregnated with 5 wt% vanadia. A special heat treatment was used in the calcination to maintain the large surface area and high dispersion of vanadium species. This catalyst was compared to a common V2O5-TiO2 catalyst with the same vanadia loading prepared by a traditional method. The new catalyst has a surface area of 117.7 m^2/g, which was 38% higher than the traditional V2O5-TiO2 catalyst. The selective catalytic reduction（SCR） performance demonstrated that the new catalyst had a wider temperature window and better N2 selectivity compared to the traditional one. The NO conversion was 80% from 200 to 450 °C. The temperature window was 100 °C wider than the traditional catalyst. Raman spectra indicated that the vanadium species formed more V-O-V linkages on the catalyst prepared by the traditional method. The amount of V-O-Ti and V=O was larger for the new catalyst. Temperature programmed desorption of NH3, temperature programmed reduction by H2 and X-ray photoelectron spectroscopy results showed that its redox ability and total acidity were enhanced. The results are helpful for developing a more efficient SCR catalyst for the removal of NOx in flue gases.
基金supported by the National Natural Science Foundation of China (No.90411020)Major State Basic Research Development Program of China (973 Program)(2002CB412502).
文摘A study was conducted to determine the effects of elevated CO2 on soil N process at Changbai Mountain in Jilin Province, northeastern China （42°24＂N, 128°06＂E, and 738 m elevation）. A randomized complete block design of ambient and elevated CO2 was established in an open-top chamber facility in the spring of 1999. Changpai Scotch pine （Pinus sylvestris var. sylvestriformis seeds were sowed in May, 1999 and CO2 fumigation treatments began after seeds germination. In each year, the exposure started at the end of April and stopped at the end of October. Soil samples were collected in June and August 2006 and in June 2007, and soil nitrifying, denitrifying and N2-fixing enzyme activities were measured. Results show that soil nitrifying enzyme activities （NEA） in the 5-10 cm soil layer were significantly increased at elevated CO2 by 30.3% in June 2006, by 30.9% in August 2006 and by 11.3% in June 2007. Soil denitrifying enzyme activities （DEA） were significantly decreased by elevated CO2 treatment in June 2006 （P 〈 0.012） and August 2006 （P 〈 0.005） samplings in our study; no significant difference was detected in June 2007, and no significant changes in N2-fixing enzyme activity were found. This study suggests that elevated CO2 can alter soil nitrifying enzyme and denitrifying enzyme activities.
文摘The hydrogenation of m-dinitrobenzene to m-phenylenediamine in liquid phase was studied with the nickel catalysts supported on SiO2, TiO2, γ-Al2O3, MgO and diatomite carders. Based on the experiments of X-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS）, temperature-programmed reduction （TPR）, temperature-programmed desorption of hydrogen （H2-TPD） and activity evaluation, the physico-chemical and catalytic properties of the catalysts were investigated. Among the catalysts tested, the SiO2 supported nickel catalyst showed the highest activity and selectivity towards m-phenylenediamine, over which 97.3% m-dinitrobenzene conversion and 95.1% m-phenylenediamine yield were obtained at 373K under hydrogen pressure of 2.6MPa after reaction for 6 h when using ethanol as solvent. Although TiO2 and diatomite supported nickel catalysts also presented high activity, they had lower selectivity towards m-phenylenediamine. As for γ-Al2O3 and MgO supported catalysts were almost inactive for the object reaction. It was shown that both the activity and selectivity of the catalysts were strongly depended on the interaction between nickel and the support. The higher activities of Ni/SiO2, Ni/TiO2 and Ni/diatomite could be attributed to the weaker metal-support interaction, on which Ni species presented as crystallized Ni metal particles. On the other hand, there existed strong metal-support interaction in Ni/MgO and Ni γ-Al2O3, which causes these catalysts more difficult to be reduced and the availability of Ni active sites decreased, resulting in their low catalytic activity.
基金Project supported by the National Natural Science Foundation of China (Nos. 30390080 and 30390081).
文摘Specific management of water regimes, soil and N in China might play an important role in regulating N2O and CH4 emissions in rice fields. Nitrous oxide and methane emissions from alternate non-flooded/flooded paddies were monitored simultaneously during a 516-day incubation with lysimeter experiments. Two N sources (15N-(NH4)2SO4 and 15N-labeled milk vetch) were applied to two contrasting paddies: one derived from Xiashu loess (Loess) and one from Quaternary red clay (Clay). Both N2O and CH4 emissions were significantly higher in soil Clay than in soil Loess during the flooded period. For both soil, N2O emissions peaked at the transition periods shortly after the beginning of the flooded and non-flooded seasons. Soil type affected N2O emission patterns. In soil Clay, the emission peak during the transition period from non-flooded to flooded conditions was much higher than the peak during the transition period from flooded to non-flooded conditions. In soil Loess, the emission peak during the transition period from flooded to non-flooded conditions was obviously higher than the peak during the transition period from non-flooded to flooded conditions except for milk vetch treatment. Soil type also had a significant effect on CH4 emissions during the flooded season, over which the weighted average flux was 111 mg C m-2 h-1 and 2.2 mg C m-2 h-1 from Clay and Loess, respectively. Results indicated that it was the transition in the water regime that dominated N2O emissions while it was the soil type that dominated CH4 emissions during the flooded season. Anaerobic oxidation of methane possibly existed in soil Loess during the flooded season.
基金Supported by the National Basic Research Program (No.2003CB615702) and the National Natural Science Foundation of Chin(No.20436030).
文摘The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/TiO2 catalysts prepared by a liquid-phase chemical reduction method. The catalysts were characterized by inductively coupled plasma (ICP), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS) and temperature-programmed reduction (TPR). Results show that the titania structure has favorable influence on physio-chemical and catalytic properties of Ni/TiO2 catalysts. Compared to commercial Raney nickel, the catalytic activity of Ni/TiO2 catalyst is much superior, irrespective of the titania structure. The catalytic activity of anatase titania supported nickel catalyst Ni/TiO2(A) is higher than that of rutile titania supported nickel catalyst Ni/TiO2(R), possibly because the reduction of nickel oxide to metallic nickel for Ni/TiO2(A) is easier than that for Ni/TiO2(R) at similar reaction conditions.
基金Supported by the National Natural Science Foundation of China(51206096)
文摘An experimental study of thermal de-NOx using NH3 as reductant in 02/C02 atmosphere with the effect of S02 and different additives was performed in a drop tube furnace. Results show that the optimum temperature win- dow is 841-1184 ℃, and the optimum reaction temperature is about 900 ℃ with a de-NOx efficiency of 95.4%. A certain amount of S02 has an inhibiting effect on NO reduction. The effect of additives, including Na2C03, C2H5OH and FeCI3, on NO reduction by NH3 is also explored. The addition of Na2CO3 and FeCI3 is useful to widen the tem- perature window and shift the reaction to lower temperature for the efficiency is increased from 30.5% to 74.0% and 67.4% respectively at 800 ℃. Qualitatively, the modeling results using a detailed kinetic modeling mecha- nism represent well most of the process features. The effect of Na2CO3, C2H5OH and FeCI3 addition can be reproduced well by the Na2C03, C2H5OH and Fe（CO）5 sub-mechanism respectively. The reaction mechanism analysis shows that the effects of these additives on NO reduction are achieved mainly by promoting the produc- tion of OH radicals at lower temperature.
基金Project supported by the Canadian International Development Agency, Canada and the Chinese Academy of Scicences, China (No. KZCX2-413)
文摘To feed an increasing population, large amounts of chemical nitrogen fertilizer have been used to produce much of our food, feed and fiber thereby increasing nitrogen levels in soils, natural waters, crop residues, livestock wastes,and municipal and agricultural wastes, with national and international concern about its potential adverse effects on environmental quality and public health. To understand these phenomena and problems, first the nitrogen cycle and the environment are described. Then recent trends for nitrogen cycling through the food and feed system, N2O emissions from fertilized upland and paddy soils, and NO-3 pollution in ground water in Japan are reported. Finally, mitigation strategies in Japan for reducing N2O emission and NO-3 pollution are proposed, including nitrification inhibitors, controlled release fertilizers, utilization of plant species that could suppress nitrification, utilizing the toposequence, government policy, and appropriate agricultural practices. Of all the technologies presented, use of nitrification inhibitors and controlled release fertilizers are deemed the most important with further development of these aspects of technologies being expected. These practices, if employed worldwide, could help reduce the load, or environmental deterioration, on the Earth's biosphere.
文摘Isolation of new bacterial strains and recognition of their metabolic activities are highly desirable for sustainability of natural ecosystems. Biodegradation of dimethyl phthalate （DMP） under anoxic conditions has been shown to occur as a series of sequential steps using strain CW-1 isolated from digested sludge of Sibao Wastewater Treatment Plant in Hangzhou, China. The microbial colony on LB medium was yellowish, 3-5 mm in diameter, convex in the center, and embedded in mucous externally. The individual cells of strain CW-1 are irregular rods, measuring （0.6-0.7）×（0.9-1.0） pm, V-shaped, with clubbed ends, Gram positive and without any filaments. 16S rDNA （ 1438 bp） sequence analysis showed that the strain was related to Arthrobacter sp. CW-1 and can degrade PAEs utilizing nitrate as electron acceptor, but cannot mineralize DMP completely. The degradation pathway was recommended as： dimethyl phthalate （DMP）→monomethyl phthalate （MMP）--,phthalic acid （PA）. DMP biodegradation was a first order reaction with degradation rate constant of 0.3033 d 1 and half-life 2.25 d. The DMP conversion to PA by CW-1 could be described by using sequential kinetic model.
