Sequence hybrid biological reactor (SHBR) was proposed, and some key control parameters were investigated for nitrogen removal from wastewater by simultaneous nitrification and denitrification (SND) via nitrite. S...Sequence hybrid biological reactor (SHBR) was proposed, and some key control parameters were investigated for nitrogen removal from wastewater by simultaneous nitrification and denitrification (SND) via nitrite. SND via nitrite was achieved in SHBR by controlling demand oxygen (DO) concentration. There was a programmed decrease of the DO from 2.50 mg·L^-1 to 0.30 mg·L^-1, and the average nitrite accumulation rate (NAR) was increased from 16.5% to 95.5% in 3 weeks. Subsequently, further increase in DO concentration to 1.50 mg·L^-1 did not destroy the partial nitrification to nitrite. The results showed that limited air flow rate to cause oxygen deficiency in the reactor would eventually induce only nitrification to nitrite and not further to nitrate. Nitrogen removal efficiency was increased with the increase in NAR, that is, NAR was increased from 60% to 90%, and total nitrogen removal efficiency was increased from 68% to 85%. The SHBR could tolerate high organic loading rate (OLR), COD and ammonia-nitrogen removal efficiency were greater than 92% and 93.5%, respectively,, and it even operated under low DO concentration (0.5 mg·L^-1) and maintained high OLR (4.0 kg COD·m^-3·d^-1). The presence of biofilm positively affected the activated sludge settling capability, and sludge volume index (SVI) of activated sludge in SHBR never hit more than 90 ml·L^-1 throughout the experiments.展开更多
The gas-liquid phase equilibrium is used in controlling the nitrosation reaction process. Decomposition of nitrous acid and oxidation side reaction.are suppressed in a closed reaction system. The system pressure is us...The gas-liquid phase equilibrium is used in controlling the nitrosation reaction process. Decomposition of nitrous acid and oxidation side reaction.are suppressed in a closed reaction system. The system pressure is used as the criterion of the end of reaction, avoiding excessive feeding and reducing'the decomposition'of nitrous acid. The head space of the reactor is used as the gas buffer, stabilizing the feeding fluctuations and inhibiting the side reaction, decomposition of nitrous acid. Nitrogen oxide concentration is controlled at the minimum level.Thus the zero release ofnitrogen ox!de waste gas can be achieved without using any absorption process.展开更多
Dissociation of methyl nitrite is the first step during CO catalytic coupling to dimethyl oxalate followed by hydrogenation to ethyl glycol in a typical coal to liquid process. In this work, the first-principle calcul...Dissociation of methyl nitrite is the first step during CO catalytic coupling to dimethyl oxalate followed by hydrogenation to ethyl glycol in a typical coal to liquid process. In this work, the first-principle calculations based on density functional theory were performed to explore the reaction mechanism for the non-catalytic dissociation of methyl nitrite in the gas phase and the catalytic dissociation of methyl nitrite on Pd(111) surface since palladium supported on alpha-alumina is the most effective catalyst for the coupling. For the non-catalytic case, the calculated results show that the CH_3O–NO bond will break with a bond energy of 1.91 eV, and the produced CH_3O radicals easily decompose to formaldehyde, while the further dissociation of formaldehyde in the gas phase is difficult due to the strong C–H bond. On the other hand, the catalytic dissociation of methyl nitrite on Pd(111) to the adsorbed CH_3O and NO takes place with a small energy barrier of 0.03 eV. The calculated activation energies along the proposed reaction pathways indicate that(i) at low coverage, a successive dehydrogenation of the adsorbed CH_3O to CO and H is favored while(ii) at high coverage, hydrogenation of CH_3O to methanol and carbonylation of CH_3O to methyl formate are more preferred. On the basis of the proposed reaction mechanism,two meaningful ways are proposed to suppress the dissociation of methyl nitrate during the CO catalytic coupling to dimethyl oxalate.展开更多
Ammonium and nitrite are two substrates of anammox bacteria, but they are also inhibitors under high concentrations. The performance of two anaerobic ammonium-oxidizing (anammox) upflow biofilm (UBF) reactors was inve...Ammonium and nitrite are two substrates of anammox bacteria, but they are also inhibitors under high concentrations. The performance of two anaerobic ammonium-oxidizing (anammox) upflow biofilm (UBF) reactors was investigated. The results show that anammox UBFs become unstable under nitrogen loading rate (NLR) applied higher than 1.0 g/(L·d). The consumptions of acidity in the anammox reaction lead to the increase of pH, which is as high as 8.70-9.05. Free nitrous acid concentration is accompanied to be lower than the affinity constant of anammox bacteria, and then starvation effect appears. Moreover, free ammonia concentration increases to 57-178 mg/L, resulting in inhibitory effect on the anammox bacteria. Both negative effects contribute to the instability of the anammox bioreactors.展开更多
Alkanolamines are widely used in the purification of the sourgas sweetening process. During the sour gas absorption process, CO_2 significantly degrades the amine solvent and creates enormous problems for plant operat...Alkanolamines are widely used in the purification of the sourgas sweetening process. During the sour gas absorption process, CO_2 significantly degrades the amine solvent and creates enormous problems for plant operation. In this work, CO_2 induced degradation of aqueous diethanolamine(DEA) solution was conducted in a 1.25 L jacketed glass reactor that functioned as an absorber and stripper at atmospheric conditions. Pure CO_2 was bubbled through the reactor until the solution became saturated. In this study, the concentrations of DEA used were in the range of concentrations between 2 mol·L^(-1) and 4 mol·L^(-1). In the degradation experiment, six generic cycles were conducted for each run. Each cycle was configured with the absorption and desorption of carbon dioxide at 55 ℃ and 100 ℃, respectively. Samples were collected after a predetermined experimental time and analyzed by ion chromatography(IC) to identify unknown ionic degradation products(DGPs). In the IC analysis, three different columns were used for anion, cation and ion exclusion systems, which are Metrosep A Supp 5150/4.0, Metrosep C Supp 4 150/4.0 and Metrosep Organic Acids, respectively. The major identified DGPs of D01 DEA2 M, D02 DEA3 M, and D03 DEA4 M are nitrite, acetate and ammonium. Phosphate product was found in the degraded amine samples which might be due to the contamination of water or chromatographic system.展开更多
Two lab-scale reactors, suspended-sludge and fluidized.bed, were conducted with the feed of ammonium-rich synthetic wastewater devoid of COD. Completely autotrophic nitrogen-removal process was fulfilled in both react...Two lab-scale reactors, suspended-sludge and fluidized.bed, were conducted with the feed of ammonium-rich synthetic wastewater devoid of COD. Completely autotrophic nitrogen-removal process was fulfilled in both reactors and the maximum efficiencies of nitrogen removal were achieved, 65% in the suspended-sludge reactor and 73% in the fluidized-bed reactor respectively. Different from the steady performance of the fluldized-bed reactor, the suspended-sludge reactor came to deteriorate constantly after a period of stable operation, resulting in almost complete loss of the N-removal ability in the suspending system. Molecular methods such as PCR and FISH were employed for describing the microbial characteristics in two systems. This study suggests that a biofllm system is a suitable configuration for completely autotrophic N-removal with more feasibility and stability than a suspending system.展开更多
A system consisting of a two-stage up-flow anaerobic sludge blanket (UASB) reactor and an anoxic/aerobic (A/O) reactor was used to treat municipal landfill leachate. Denitrification took place in the first stage o...A system consisting of a two-stage up-flow anaerobic sludge blanket (UASB) reactor and an anoxic/aerobic (A/O) reactor was used to treat municipal landfill leachate. Denitrification took place in the first stage of the UASB reactor (UASB1). The chemical oxygen demand of the UASB1 effluent was further decreased in the second stage (UASB2). Nitrification was accomplished in the A/O reactor. When diluted with tap water at a ratio of 1:1, the ammonia nitrogen concentration of the influent leachate was approximately 1200 mg· L^-1, whereas that of the system effluent was approximately 8-11 mg· L^-1, and the corresponding removal efficiency is about 99.08%. Stable partial nitrification was achieved in the A/O reactor with 88.61%-91.58% of the nitrite accumulation ratio, even at comparatively low temperature ( 16℃). The results demonstrate that free ammonia (FA) concentrations within a suitable range exhibit a positive effect on partial nitrification. In this experiment when FA was within the 1-30 mgmg· L^-1 range, partial nitrification could be achieved, whereas when FA exceeded 280 mgmg· L^-1, the nitrification process was entirely inhibited. Temperature was not the key factor leading to partial nitrification within the 16-29 ℃ range. The inhibitory influence of free nitrous acid (FNA) on nitrification was also minimal when pH was greater than 8.5. Thus, FA concentration was a major factor in achieving partial nitrification.展开更多
To study the HONO formation mechanisms during a pollution period, a continuous measurement was performed in both urban and suburban aeras of Beijing. During this period, the PM2.5 concentrations increased to 201 and 1...To study the HONO formation mechanisms during a pollution period, a continuous measurement was performed in both urban and suburban aeras of Beijing. During this period, the PM2.5 concentrations increased to 201 and 137 ?g/m3 in urban and suburban areas, respectively. The concentrations of HONO, CO, SO2, O3, NO, NO2, NOx were 1.45 ppbv, 0.61 ppmv, 8.7 ppbv, 4.3 ppbv, 44.4 ppbv, 37.4 ppbv, 79.4 ppbv and 0.72 ppbv, 1.00 ppmv, 1.2 ppbv, 7.9 ppbv, 3.7 ppbv, 8.2 ppbv, 11.9 ppbv, in urban and suburban areas, respectively. To compare possible pathways of HONO formation in both sites, the contributions of direct emissions, heterogeneous formations, and homogeneous productions were studied. HONO/NO2 ratios in the two sites indicated that heterogeneous reactions of NO2 were more efficient in suburban areas. And in both urban and suburban areas, the increase of PM2.5 concentrations and RH would promote the conversion efficiency in RH that ranged from 0% to 85%. However, when RH was above 85%, the HONO formation slowed down. Moreover, the study of direct emissions and homogeneous reactions showed that they contributed to a majority of HONO increase in urban areas than the 20% contributions in suburban areas. It implied that the high NOx concentrations and NO concentrations in urban areas or in pollution periods would make direct emissions and homogeneous reactions become dominant in HONO formations.展开更多
基金the National Key Project of Scientific and Technical Supporting Program of Ministry of Science and Technology ofChina(2006BAC19B03)Academic Human Resources Development in Institutions of Higher Leading under the Jurisdiction ofBeijing Municipalitythe Specialized Research Fund for the Doctoral Program of Higher Education of China(20060005002).
文摘Sequence hybrid biological reactor (SHBR) was proposed, and some key control parameters were investigated for nitrogen removal from wastewater by simultaneous nitrification and denitrification (SND) via nitrite. SND via nitrite was achieved in SHBR by controlling demand oxygen (DO) concentration. There was a programmed decrease of the DO from 2.50 mg·L^-1 to 0.30 mg·L^-1, and the average nitrite accumulation rate (NAR) was increased from 16.5% to 95.5% in 3 weeks. Subsequently, further increase in DO concentration to 1.50 mg·L^-1 did not destroy the partial nitrification to nitrite. The results showed that limited air flow rate to cause oxygen deficiency in the reactor would eventually induce only nitrification to nitrite and not further to nitrate. Nitrogen removal efficiency was increased with the increase in NAR, that is, NAR was increased from 60% to 90%, and total nitrogen removal efficiency was increased from 68% to 85%. The SHBR could tolerate high organic loading rate (OLR), COD and ammonia-nitrogen removal efficiency were greater than 92% and 93.5%, respectively,, and it even operated under low DO concentration (0.5 mg·L^-1) and maintained high OLR (4.0 kg COD·m^-3·d^-1). The presence of biofilm positively affected the activated sludge settling capability, and sludge volume index (SVI) of activated sludge in SHBR never hit more than 90 ml·L^-1 throughout the experiments.
文摘The gas-liquid phase equilibrium is used in controlling the nitrosation reaction process. Decomposition of nitrous acid and oxidation side reaction.are suppressed in a closed reaction system. The system pressure is used as the criterion of the end of reaction, avoiding excessive feeding and reducing'the decomposition'of nitrous acid. The head space of the reactor is used as the gas buffer, stabilizing the feeding fluctuations and inhibiting the side reaction, decomposition of nitrous acid. Nitrogen oxide concentration is controlled at the minimum level.Thus the zero release ofnitrogen ox!de waste gas can be achieved without using any absorption process.
基金Supported by the National Natural Science Foundation of China(21303102)China Postdoctoral Science Foundation funded project(2012M520900 and 2013T60449)
文摘Dissociation of methyl nitrite is the first step during CO catalytic coupling to dimethyl oxalate followed by hydrogenation to ethyl glycol in a typical coal to liquid process. In this work, the first-principle calculations based on density functional theory were performed to explore the reaction mechanism for the non-catalytic dissociation of methyl nitrite in the gas phase and the catalytic dissociation of methyl nitrite on Pd(111) surface since palladium supported on alpha-alumina is the most effective catalyst for the coupling. For the non-catalytic case, the calculated results show that the CH_3O–NO bond will break with a bond energy of 1.91 eV, and the produced CH_3O radicals easily decompose to formaldehyde, while the further dissociation of formaldehyde in the gas phase is difficult due to the strong C–H bond. On the other hand, the catalytic dissociation of methyl nitrite on Pd(111) to the adsorbed CH_3O and NO takes place with a small energy barrier of 0.03 eV. The calculated activation energies along the proposed reaction pathways indicate that(i) at low coverage, a successive dehydrogenation of the adsorbed CH_3O to CO and H is favored while(ii) at high coverage, hydrogenation of CH_3O to methanol and carbonylation of CH_3O to methyl formate are more preferred. On the basis of the proposed reaction mechanism,two meaningful ways are proposed to suppress the dissociation of methyl nitrate during the CO catalytic coupling to dimethyl oxalate.
基金Project(2006AA06Z332) supported by the National High-Tech Research and Development Program of ChinaProject(30770039) supported by the National Natural Science Foundation of ChinaProject(2008BADC4B05) supported by the National Science and Technology Pillar Program
文摘Ammonium and nitrite are two substrates of anammox bacteria, but they are also inhibitors under high concentrations. The performance of two anaerobic ammonium-oxidizing (anammox) upflow biofilm (UBF) reactors was investigated. The results show that anammox UBFs become unstable under nitrogen loading rate (NLR) applied higher than 1.0 g/(L·d). The consumptions of acidity in the anammox reaction lead to the increase of pH, which is as high as 8.70-9.05. Free nitrous acid concentration is accompanied to be lower than the affinity constant of anammox bacteria, and then starvation effect appears. Moreover, free ammonia concentration increases to 57-178 mg/L, resulting in inhibitory effect on the anammox bacteria. Both negative effects contribute to the instability of the anammox bioreactors.
基金the Ministry of Science,Technology and Innovation,Malaysia(MOSTI),for funding the project:RG003/09AET as well as the University of Malaya for allowing full access to several key laboratories to perform experimental work
文摘Alkanolamines are widely used in the purification of the sourgas sweetening process. During the sour gas absorption process, CO_2 significantly degrades the amine solvent and creates enormous problems for plant operation. In this work, CO_2 induced degradation of aqueous diethanolamine(DEA) solution was conducted in a 1.25 L jacketed glass reactor that functioned as an absorber and stripper at atmospheric conditions. Pure CO_2 was bubbled through the reactor until the solution became saturated. In this study, the concentrations of DEA used were in the range of concentrations between 2 mol·L^(-1) and 4 mol·L^(-1). In the degradation experiment, six generic cycles were conducted for each run. Each cycle was configured with the absorption and desorption of carbon dioxide at 55 ℃ and 100 ℃, respectively. Samples were collected after a predetermined experimental time and analyzed by ion chromatography(IC) to identify unknown ionic degradation products(DGPs). In the IC analysis, three different columns were used for anion, cation and ion exclusion systems, which are Metrosep A Supp 5150/4.0, Metrosep C Supp 4 150/4.0 and Metrosep Organic Acids, respectively. The major identified DGPs of D01 DEA2 M, D02 DEA3 M, and D03 DEA4 M are nitrite, acetate and ammonium. Phosphate product was found in the degraded amine samples which might be due to the contamination of water or chromatographic system.
文摘Two lab-scale reactors, suspended-sludge and fluidized.bed, were conducted with the feed of ammonium-rich synthetic wastewater devoid of COD. Completely autotrophic nitrogen-removal process was fulfilled in both reactors and the maximum efficiencies of nitrogen removal were achieved, 65% in the suspended-sludge reactor and 73% in the fluidized-bed reactor respectively. Different from the steady performance of the fluldized-bed reactor, the suspended-sludge reactor came to deteriorate constantly after a period of stable operation, resulting in almost complete loss of the N-removal ability in the suspending system. Molecular methods such as PCR and FISH were employed for describing the microbial characteristics in two systems. This study suggests that a biofllm system is a suitable configuration for completely autotrophic N-removal with more feasibility and stability than a suspending system.
基金Supported by the National Natural Science Foundation of China(51208040)a General Financial Grant from the China Postdoctoral Science Foundation(2013M541382)the National or Beijing Level College Students Innovation Training Projects-‘Free ammonia and free nitrous acid combined with inhibition of nitrification of landfill leachate’(14010221065)and‘Anaerobic–aerobic treatment of landfill leachate’(13010282007)
文摘A system consisting of a two-stage up-flow anaerobic sludge blanket (UASB) reactor and an anoxic/aerobic (A/O) reactor was used to treat municipal landfill leachate. Denitrification took place in the first stage of the UASB reactor (UASB1). The chemical oxygen demand of the UASB1 effluent was further decreased in the second stage (UASB2). Nitrification was accomplished in the A/O reactor. When diluted with tap water at a ratio of 1:1, the ammonia nitrogen concentration of the influent leachate was approximately 1200 mg· L^-1, whereas that of the system effluent was approximately 8-11 mg· L^-1, and the corresponding removal efficiency is about 99.08%. Stable partial nitrification was achieved in the A/O reactor with 88.61%-91.58% of the nitrite accumulation ratio, even at comparatively low temperature ( 16℃). The results demonstrate that free ammonia (FA) concentrations within a suitable range exhibit a positive effect on partial nitrification. In this experiment when FA was within the 1-30 mgmg· L^-1 range, partial nitrification could be achieved, whereas when FA exceeded 280 mgmg· L^-1, the nitrification process was entirely inhibited. Temperature was not the key factor leading to partial nitrification within the 16-29 ℃ range. The inhibitory influence of free nitrous acid (FNA) on nitrification was also minimal when pH was greater than 8.5. Thus, FA concentration was a major factor in achieving partial nitrification.
基金supported by the Strategic Priority Research Program(B)of the Chinese Academy of Sciences(XDB05010400)the Key Research Program of Chinese Academy of Sciences(KJZD-EW-TZ-G06-01)the National Natural Science Foundation of China(41475114)
文摘To study the HONO formation mechanisms during a pollution period, a continuous measurement was performed in both urban and suburban aeras of Beijing. During this period, the PM2.5 concentrations increased to 201 and 137 ?g/m3 in urban and suburban areas, respectively. The concentrations of HONO, CO, SO2, O3, NO, NO2, NOx were 1.45 ppbv, 0.61 ppmv, 8.7 ppbv, 4.3 ppbv, 44.4 ppbv, 37.4 ppbv, 79.4 ppbv and 0.72 ppbv, 1.00 ppmv, 1.2 ppbv, 7.9 ppbv, 3.7 ppbv, 8.2 ppbv, 11.9 ppbv, in urban and suburban areas, respectively. To compare possible pathways of HONO formation in both sites, the contributions of direct emissions, heterogeneous formations, and homogeneous productions were studied. HONO/NO2 ratios in the two sites indicated that heterogeneous reactions of NO2 were more efficient in suburban areas. And in both urban and suburban areas, the increase of PM2.5 concentrations and RH would promote the conversion efficiency in RH that ranged from 0% to 85%. However, when RH was above 85%, the HONO formation slowed down. Moreover, the study of direct emissions and homogeneous reactions showed that they contributed to a majority of HONO increase in urban areas than the 20% contributions in suburban areas. It implied that the high NOx concentrations and NO concentrations in urban areas or in pollution periods would make direct emissions and homogeneous reactions become dominant in HONO formations.