To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstru...To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstructure,the specific surface area,the pore volume,the crystal structure,and functional groups presented in the prepared Cu2O/AC catalysts were thoroughly characterized.By using scanning electron microscopy(SEM),nitrogen adsorption/desorption isotherms,Fourier-transform infrared(FTIR)spectroscopy and X-ray diffractometry(XRD),the effects of Cu2O loading and calcination temperature on Cu2O/AC catalysts were investigated at low temperature(150℃).The research shows that Cu on the Cu2O/AC catalyst is in the form of Cu2O with good crystalline performance and is spherical and uniformly dispersed on the AC surface.The loading of Cu2O increases the active sites and the specific surface area of the reaction gas contact,which is conducive to the rapid progress of the carbon monoxide selective catalytic reduction(CO-SCR)reaction.When the loading of Cu2O was 8%and the calcination temperature was 500℃,the removal rate of NOx facilitated by the Cu2O/AC catalyst reached 97.9%.These findings provide a theoretical basis for understanding the denitrification of sintering flue gas.展开更多
Activated sludge process has been widely used to remove phosphorus and nitrogen from wastewater. However,the nitrogen and phosphorus removal is sometimes unsatisfactory due to the low influent COD.Another problem with...Activated sludge process has been widely used to remove phosphorus and nitrogen from wastewater. However,the nitrogen and phosphorus removal is sometimes unsatisfactory due to the low influent COD.Another problem with the activated sludge process is that large amount of waste activated sludge is produced,which needs further treatment.In this study,the waste activated sludge alkaline fermentation liquid was used as the main carbon source for phosphorus and nitrogen removal under anaerobic followed by alternating aerobic-anoxic conditions,and the results were compared with those using acetic acid as the carbon source.The use of alkaline fermentation liquid not only affected the transformations of phosphorus,nitrogen,intracellular polyhydroxyalkanoates and glycogen, but also led to higher removal efficiencies for phosphorus and nitrogen compared with acetic acid.It was observed that ammonium was completely removed with either alkaline fermentation liquid or acetic acid as the carbon source. However,the former resulted in higher removal efficiencies for phosphorus(95%)and nitrogen(82%),while the latter showed lower ones(87%and 74%,respectively).The presence of a large amount of propionic acid in the alkaline fermentation liquid was one possible reason for its higher phosphorus removal efficiency.Exogenous instead of endogenous denitrification was the main pathway for nitrogen removal with the alkaline fermentation liquid as the carbon source,which was responsible for its higher nitrogen removal efficiency.It seems that the alkaline fermentation liquid can replace acetic acid as the carbon source for phosphorus and nitrogen removal in anaerobic fol- lowed by alternating aerobic-anoxic sequencing batch reactor.展开更多
Flue gas pollution is a serious environmental problem that needs to be solved for the sustainable development of China.The surface chemical properties of carbon have great influence on its desulphurization performance...Flue gas pollution is a serious environmental problem that needs to be solved for the sustainable development of China.The surface chemical properties of carbon have great influence on its desulphurization performance.A series of activated carbons (ACs) were prepared using HNO3,H2O2,NH3·H2O and steam as activation agents with the aim to introduce functional groups to carbon surface in the ACs preparation process.The ACs were physically and chemically characterized by iodine and SO2 adsorption,ultimate analysis,Boehm titration,and temperature-programmed reduction (TPR).Results showed that the iodine number and desulphurization capacity of NH3·H2O activated carbon (AC-NH3) increase with both activation time,and its desulphurization capacity also increases with the concentration of activation agent.However,HNO3 activated carbon (AC-HNO3) and H2O2 activated carbon (AC-H2O2) exhibit more complex behavior.Only their iodine numbers increase monotonously with activation time.Compared with steam activated AC (AC-H2O),the nitrogen content increases 0.232% in AC-NH3 and 0.077% in AC-HNO3.The amount of total basic site on AC-HNO3 is 0.19 mmol·g-1 higher than that on AC-H2O.H2O2 activation introduces an additional 0.08 mmol·g-1 carboxyl groups to AC surface than that introduced by steam activation.The desulphurization capacity of ACs in simulate flue gas desulphurization decreases as follows: AC-NH3 】 AC-HNO3 】 AC-H2O2 】 AC-H2O.This sequence is in accord with the SO2 catalytic oxidation/oxidation ratio in the absence of oxygen and the oxidation property reflected by TPR.In the presence of oxygen,all adsorbed SO2 on ACs can be oxidized into SO3.The desulphurization capacity increases differently according to the activation agents;the desulphurization capacity of AC-NH3 and AC-HNO3 improves by 4.8 times,yet AC-H2O increases only by 2.62 as compared with the desulphurization of corresponding ACs in absence of oxygen.展开更多
Since the ammonia in the effluent of the tradi-tional water purification process could not meet the supply demand,the advanced treatment of a high concentration of NH4+-N micro-polluted source water by biological acti...Since the ammonia in the effluent of the tradi-tional water purification process could not meet the supply demand,the advanced treatment of a high concentration of NH4+-N micro-polluted source water by biological activated carbon filter(BACF)was tested.The filter was operated in the downflow manner and the results showed that the remov-ing rate of NH_(4)^(+)-N was related to the influent concentration of NH_(4)^(+)-N.Its removing rate could be higher than 95%when influent concentration was under 1.0 mg/L.It could also decrease with the increasing influent concentration when the NH_(4)^(+)-N concentration was in the range from 1.5 to 4.9 mg/L and the dissolved oxygen(DO)in the influent was under 10 mg/L,and the minimum removing rate could be 30%.The key factor of restricting nitrification in BACF was the influent DO.When the influent NH_(4)^(+)-N concentration was high,the DO in water was almost depleted entirely by the nitrifying and hetetrophic bacteria in the depth of 0.4 m filter and the filter layer was divided into aerobic and anoxic zones.The nitrification and degradation of organic matters existed in the aerobic zone,while the denitrification occurred in the anoxic zone.Due to the limited carbon source,the denitrifica-tion could not be carried out properly,which led to the accu-mulation of the denitrification intermediates such as NO_(2)^(−).In addition to the denitrification bacteria,the nitrification and the heterotrophic bacteria existed in the anoxic zone.展开更多
Denitrification in subsoil(to a depth of 12 m) is an important mechanism to reduce nitrate(NO3^-) leaching into groundwater.However, regulating mechanisms of subsoil denitrification, especially those in the deep subso...Denitrification in subsoil(to a depth of 12 m) is an important mechanism to reduce nitrate(NO3^-) leaching into groundwater.However, regulating mechanisms of subsoil denitrification, especially those in the deep subsoil beneath the crop root zone, have not been well documented. In this study, soil columns of 0–12 m depth were collected from intensively farmed fields in the North China Plain. The fields had received long-term nitrogen(N) fertilizer inputs at 0(N0), 200(N200) and 600(N600) kg N ha^-1 year^-1. Main soil properties related to denitrification, i.e., soil water content, NO3^-, dissolved organic carbon(DOC), soil organic carbon(SOC),pH, denitrifying enzyme activity(DEA), and anaerobic denitrification rate(ADR), were determined. Statistical comparisons among the treatments were performed. The results showed that NO3^- was more heavily accumulated in the entire soil profile of the N600 treatment, compared to the N0 and N200 treatments. The SOC, DOC, and ADR decreased with increasing soil depth in all treatments,whereas considerable DEA was observed throughout the subsoil. The long-term fertilizer rates affected ADR only in the upper 4 m soil layers. The ADRs in the N200 and N600 treatments were significantly correlated with DOC. Multiple regression analysis indicated that DOC rather than DEA was the key factor regulating denitrification beneath the root zone. Additional research is required to determine if carbon addition into subsoil can be a promising approach to enhance NO3^- denitrification in the subsoil and consequently to mitigate groundwater NO3^- contamination in the intensive farmlands.展开更多
基金Open Fund of Key Laboratory of Ministry of Education for Metallurgical Emission Reduction and Comprehensive Utilization of Resources,China(No.JKF19-08)General Project of Science and Technology Plan of Yunnan Science and Technology Department,China(No.2019FB077)+1 种基金Industrialization Cultivation Project of Scientific Research Fund of Yunnan Provincial Department of Education,China(No.2016CYH07)Top Young Talents of Yunnan Ten Thousand Talents Plan,China(No.YNWR-QNBJ-2019-263)。
文摘To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstructure,the specific surface area,the pore volume,the crystal structure,and functional groups presented in the prepared Cu2O/AC catalysts were thoroughly characterized.By using scanning electron microscopy(SEM),nitrogen adsorption/desorption isotherms,Fourier-transform infrared(FTIR)spectroscopy and X-ray diffractometry(XRD),the effects of Cu2O loading and calcination temperature on Cu2O/AC catalysts were investigated at low temperature(150℃).The research shows that Cu on the Cu2O/AC catalyst is in the form of Cu2O with good crystalline performance and is spherical and uniformly dispersed on the AC surface.The loading of Cu2O increases the active sites and the specific surface area of the reaction gas contact,which is conducive to the rapid progress of the carbon monoxide selective catalytic reduction(CO-SCR)reaction.When the loading of Cu2O was 8%and the calcination temperature was 500℃,the removal rate of NOx facilitated by the Cu2O/AC catalyst reached 97.9%.These findings provide a theoretical basis for understanding the denitrification of sintering flue gas.
基金Supported by the National High Technology Research and Development Program of China(2007AA06Z326)the Programfor New Century Excellent Talents(06-0373)in University
文摘Activated sludge process has been widely used to remove phosphorus and nitrogen from wastewater. However,the nitrogen and phosphorus removal is sometimes unsatisfactory due to the low influent COD.Another problem with the activated sludge process is that large amount of waste activated sludge is produced,which needs further treatment.In this study,the waste activated sludge alkaline fermentation liquid was used as the main carbon source for phosphorus and nitrogen removal under anaerobic followed by alternating aerobic-anoxic conditions,and the results were compared with those using acetic acid as the carbon source.The use of alkaline fermentation liquid not only affected the transformations of phosphorus,nitrogen,intracellular polyhydroxyalkanoates and glycogen, but also led to higher removal efficiencies for phosphorus and nitrogen compared with acetic acid.It was observed that ammonium was completely removed with either alkaline fermentation liquid or acetic acid as the carbon source. However,the former resulted in higher removal efficiencies for phosphorus(95%)and nitrogen(82%),while the latter showed lower ones(87%and 74%,respectively).The presence of a large amount of propionic acid in the alkaline fermentation liquid was one possible reason for its higher phosphorus removal efficiency.Exogenous instead of endogenous denitrification was the main pathway for nitrogen removal with the alkaline fermentation liquid as the carbon source,which was responsible for its higher nitrogen removal efficiency.It seems that the alkaline fermentation liquid can replace acetic acid as the carbon source for phosphorus and nitrogen removal in anaerobic fol- lowed by alternating aerobic-anoxic sequencing batch reactor.
基金supported by the National Natural Science Foundation of China (Grant No. 50204011)the Chemical and Environmental Engineering Lab for the TP-5000(II) adsorption instrument
文摘Flue gas pollution is a serious environmental problem that needs to be solved for the sustainable development of China.The surface chemical properties of carbon have great influence on its desulphurization performance.A series of activated carbons (ACs) were prepared using HNO3,H2O2,NH3·H2O and steam as activation agents with the aim to introduce functional groups to carbon surface in the ACs preparation process.The ACs were physically and chemically characterized by iodine and SO2 adsorption,ultimate analysis,Boehm titration,and temperature-programmed reduction (TPR).Results showed that the iodine number and desulphurization capacity of NH3·H2O activated carbon (AC-NH3) increase with both activation time,and its desulphurization capacity also increases with the concentration of activation agent.However,HNO3 activated carbon (AC-HNO3) and H2O2 activated carbon (AC-H2O2) exhibit more complex behavior.Only their iodine numbers increase monotonously with activation time.Compared with steam activated AC (AC-H2O),the nitrogen content increases 0.232% in AC-NH3 and 0.077% in AC-HNO3.The amount of total basic site on AC-HNO3 is 0.19 mmol·g-1 higher than that on AC-H2O.H2O2 activation introduces an additional 0.08 mmol·g-1 carboxyl groups to AC surface than that introduced by steam activation.The desulphurization capacity of ACs in simulate flue gas desulphurization decreases as follows: AC-NH3 】 AC-HNO3 】 AC-H2O2 】 AC-H2O.This sequence is in accord with the SO2 catalytic oxidation/oxidation ratio in the absence of oxygen and the oxidation property reflected by TPR.In the presence of oxygen,all adsorbed SO2 on ACs can be oxidized into SO3.The desulphurization capacity increases differently according to the activation agents;the desulphurization capacity of AC-NH3 and AC-HNO3 improves by 4.8 times,yet AC-H2O increases only by 2.62 as compared with the desulphurization of corresponding ACs in absence of oxygen.
文摘Since the ammonia in the effluent of the tradi-tional water purification process could not meet the supply demand,the advanced treatment of a high concentration of NH4+-N micro-polluted source water by biological activated carbon filter(BACF)was tested.The filter was operated in the downflow manner and the results showed that the remov-ing rate of NH_(4)^(+)-N was related to the influent concentration of NH_(4)^(+)-N.Its removing rate could be higher than 95%when influent concentration was under 1.0 mg/L.It could also decrease with the increasing influent concentration when the NH_(4)^(+)-N concentration was in the range from 1.5 to 4.9 mg/L and the dissolved oxygen(DO)in the influent was under 10 mg/L,and the minimum removing rate could be 30%.The key factor of restricting nitrification in BACF was the influent DO.When the influent NH_(4)^(+)-N concentration was high,the DO in water was almost depleted entirely by the nitrifying and hetetrophic bacteria in the depth of 0.4 m filter and the filter layer was divided into aerobic and anoxic zones.The nitrification and degradation of organic matters existed in the aerobic zone,while the denitrification occurred in the anoxic zone.Due to the limited carbon source,the denitrifica-tion could not be carried out properly,which led to the accu-mulation of the denitrification intermediates such as NO_(2)^(−).In addition to the denitrification bacteria,the nitrification and the heterotrophic bacteria existed in the anoxic zone.
基金supported by the National Natural Science Foundation of China(Nos.31270554 and41301323)the Key Program of National Natural Science Foundation of China(No.41530859)
文摘Denitrification in subsoil(to a depth of 12 m) is an important mechanism to reduce nitrate(NO3^-) leaching into groundwater.However, regulating mechanisms of subsoil denitrification, especially those in the deep subsoil beneath the crop root zone, have not been well documented. In this study, soil columns of 0–12 m depth were collected from intensively farmed fields in the North China Plain. The fields had received long-term nitrogen(N) fertilizer inputs at 0(N0), 200(N200) and 600(N600) kg N ha^-1 year^-1. Main soil properties related to denitrification, i.e., soil water content, NO3^-, dissolved organic carbon(DOC), soil organic carbon(SOC),pH, denitrifying enzyme activity(DEA), and anaerobic denitrification rate(ADR), were determined. Statistical comparisons among the treatments were performed. The results showed that NO3^- was more heavily accumulated in the entire soil profile of the N600 treatment, compared to the N0 and N200 treatments. The SOC, DOC, and ADR decreased with increasing soil depth in all treatments,whereas considerable DEA was observed throughout the subsoil. The long-term fertilizer rates affected ADR only in the upper 4 m soil layers. The ADRs in the N200 and N600 treatments were significantly correlated with DOC. Multiple regression analysis indicated that DOC rather than DEA was the key factor regulating denitrification beneath the root zone. Additional research is required to determine if carbon addition into subsoil can be a promising approach to enhance NO3^- denitrification in the subsoil and consequently to mitigate groundwater NO3^- contamination in the intensive farmlands.