To achieve high efficiency of nitrogen and phosphorus removal and to investigate the rule of simultaneous nitrification and denitrification phosphorus removal (SNDPR), a whole course of SNDPR damage and recovery was...To achieve high efficiency of nitrogen and phosphorus removal and to investigate the rule of simultaneous nitrification and denitrification phosphorus removal (SNDPR), a whole course of SNDPR damage and recovery was studied in a pilot-scale, anaerobicanoxic oxidation ditch (OD), where the volumes of anaerobic zone, anoxic zone, and ditches zone of the OD system were 7, 21, and 280 L, respectively. The reactor was fed with municipal wastewater with a flow rate of 336 L/d. The concept of simultaneous nitrification and denitrification (SND) rate (rSND) was put forward to quantify SND. The results indicate that: (1) high nitrogen and phosphorus removal efficiencies were achieved during the stable SND phase, total nitrogen (TN) and total phosphate (TP) removal rates were 80% and 85%, respectively; (2) when the system was aerated excessively, the stability of SND was damaged, and rSND dropped from 80% to 20% or less; (3) the natural logarithm of the ratio of NOx to NH4^+ in the effluent had a linear correlation to oxidation-reduction potential (ORP); (4) when NO3^- was less than 6 mg/L, high phosphorus removal efficiency could be achieved; (5) denitrifying phosphorus removal (DNPR) could take place in the anaerobic-anoxic OD system. The major innovation was that the SND rate was devised and quantified.展开更多
Dielectric barrier discharge (DBD) plasma was utilized to oxidize NO contained in the exhaust gas to NO2, ultimately improve the selective catalytic reduction of nitrogen oxides (NOx). In the one case, DBD was cre...Dielectric barrier discharge (DBD) plasma was utilized to oxidize NO contained in the exhaust gas to NO2, ultimately improve the selective catalytic reduction of nitrogen oxides (NOx). In the one case, DBD was created directly in the exhaust gas (direct application), and in the an other case, ozone produced by DBD was injected into the exhaust gas (indirect application). A comparative study between such direct and indirect applications of DBD plasma was made in terms of the NOx removal efficiency and the energy consumption. The NO2 content in the exhaust gas was changed by the voltage applied to the DBD device (for direct application) or by the amount of ozone added to the exhaust gas (for indirect application). In both cases, NO was easily oxidized to NO2, and the change in NO2 content largely affected the NOx removal performance of the catalytic reactor placed downstream, where both NO and NO2 were reduced to N2 in the presence of ammonia as the reducing agent. The experiments were primarily concerned with the effect of reaction temperature on the catalytic NOx reduction at various NO2 contents. The direct and indirect applications of DBD were found to remarkably improve the catalytic NOx reduction, especially at low temperatures.展开更多
A single-stage plasma-catalytic reactor in which catalytic materials werepacked was used to remove nitrogen oxides. The packing material was scoria being made of variousmetal oxides including Al_2O_3, MgO, TiO_2, etc....A single-stage plasma-catalytic reactor in which catalytic materials werepacked was used to remove nitrogen oxides. The packing material was scoria being made of variousmetal oxides including Al_2O_3, MgO, TiO_2, etc. Scoria was able to act not only as dielectricpellets but also as a catalyst in the presence of reducing agent such as ethylene and ammonia.Without plasma discharge, scoria did not work well as a catalyst in the temperature range of 100 ℃to 200 ℃, showing less than 10% of NOx removal efficiency. When plasma is produced inside thereactor, the NOx removal efficiency could be increased to 60% in this temperature range.展开更多
The potential of using denitrifying and nitrifying concurrent biofilters for the removal of nitrogen oxides from synthetic gas streams was studied under the condition of high oxygen concentration. It was found that ...The potential of using denitrifying and nitrifying concurrent biofilters for the removal of nitrogen oxides from synthetic gas streams was studied under the condition of high oxygen concentration. It was found that more than 85% of nitric oxide was removed from synthetic combustion gas-streams which contained 20% oxygen and 350 μL/L NO, with a residence time of 60 seconds. In the process, it was found that the existing of oxygen showed no evident negative effect on the efficiency of nitrogen removal.展开更多
This paper reports the studies conducted on removal of oxides ofnitrogen (NOx) from diesel engine exhaust using electrical dischargeplasma combined with adsorbing materials such as molecular sieves.This study is being...This paper reports the studies conducted on removal of oxides ofnitrogen (NOx) from diesel engine exhaust using electrical dischargeplasma combined with adsorbing materials such as molecular sieves.This study is being reported for the first time. The exhaust is takenfrom a diesel engine of 6 kW under no load conditions. Thecharacteristic behavior of a pulse energized dielectric barrierdischarge reactor in the diesel exhaust treatment is reported. TheNOx removal was not significant (36/100) when the reactor without anypacking was used.展开更多
Total dissolved nitrogen(TDN) is an important parameter for assessing the nutrient cycling and status of natural waters.The accurate determination of TDN in natural waters is essential for assessing its contents and d...Total dissolved nitrogen(TDN) is an important parameter for assessing the nutrient cycling and status of natural waters.The accurate determination of TDN in natural waters is essential for assessing its contents and distinguishing different forms of nitrogen in the water.The TDN in various systems has been largely documented,and the concentrations of TDN are usually obtained using high-temperature catalytic(HTC) or persulfate oxidation(PO).However,the accuracy of these methods and their suitability for all types of natural waters are still unclear.To explore both methods in-depth,assorted samples were tested,including eight solutions composed of nitrogen-containing compounds(3 dissolved inorganic nitrogen fractions:NO_(3)^(-),NO_(2)^(-)and NH_(4)^(+);5 organic compounds:EDTA-2Na,vitamin B1,vitamin B12,amino acids,and urea) and 105 natural waters which were collected from an open ocean(Northwest Pacific Ocean,28),a marginal sea(Yellow Sea,34),an estuary(Huanghe River mouth,31),rivers(Huanghe River,4;Licun River,4),and precipitations(4 samples).The results showed that heterocycles and molecular dimensions had certain effects on the oxidation efficiency of the PO method but had little effect on HTC.There was no significant difference between the two methods for natural waters,but HTC was more suitable for deep-sea samples with low TDN concentrations(less than 10 μmol/L) and low organic activity.Overall,HTC has a relatively simple measurement process,a high degree of automation,and low error.Therefore,HTC can be recommended to determine the TDN of samples in freshwater and seawater.展开更多
We evaluate nitrogen oxides pollution in Takamatsu and Utazu area in Kagawa prefecture, Japan. Annually observations for nitrogen oxides (nitrogen dioxide;NO2, nitric oxide;NO) (1990-2007) were obtained from data base...We evaluate nitrogen oxides pollution in Takamatsu and Utazu area in Kagawa prefecture, Japan. Annually observations for nitrogen oxides (nitrogen dioxide;NO2, nitric oxide;NO) (1990-2007) were obtained from data base of Kagawa prefecture, Japan. Changes in NO2 and NO in Takamatsu and Utazu area were evaluated and compared. In 2007, NO2, NO and NO2 + NO (ppm) in Takamatsu area were higher than those in Utazu area. However, NO2 /NO + NO2 in Takamatsu area was lower than that in Utazu area. From 1990 to 2007, mean of NO2 in a day over the level of 0.06 ppm was 30 days in Takamatsu area and only one day in Utazu area. Mean of NO2, NO and NO2 + NO was significantly higher and NO2/NO + NO2 was lower in Takamatsu area than that in Utazu area. In addition, NO2, NO and NO2 + NO were negatively correlated and NO2/NO + NO2 was positively correlated with years (1990-2007) in Takamatsu area. The level of nitrogen oxides pollution in Utazu area was lower than Takamatsu area. Further observation is required for preventing nitrogen oxides pollution in Kagawa prefecture, Japan.展开更多
Ruminants play a critical role in our food system by converting plant biomass that humans cannot or choose not to consume into edible high-quality food.However,ruminant excreta is a significant source of nitrous oxide...Ruminants play a critical role in our food system by converting plant biomass that humans cannot or choose not to consume into edible high-quality food.However,ruminant excreta is a significant source of nitrous oxide(N_(2)O),a potent greenhouse gas with a long-term global warming potential 298 times that of carbon dioxide.Natural phytochemicals or forages containing phytochemicals have shown the potential to improve the efficiency of nitrogen(N)utilization and decrease N_(2)O emissions from the excreta of ruminants.Dietary inclusion of tannins can shift more of the excreted N to the feces,alter the urinary N composition and consequently reduce N_(2)O emissions from excreta.Essential oils or saponins could inhibit rumen ammonia production and decrease urinary N excretion.In grazed pastures,large amounts of glucosinolates or aucubin can be introduced into pasture soils when animals consume plants rich in these compounds and then excrete them or their metabolites in the urine or feces.If inhibitory compounds are excreted in the urine,they would be directly applied to the urine patch to reduce nitrification and subsequent N_(2)O emissions.The phytochemicals’role in sustainable ruminant production is undeniable,but much uncertainty remains.Inconsistency,transient effects,and adverse effects limit the effectiveness of these phytochemicals for reducing N losses.In this review,we will identify some current phytochemicals found in feed that have the potential to manipulate ruminant N excretion or mitigate N_(2)O production and deliberate the challenges and opportunities associated with using phytochemicals or forages rich in phytochemicals as dietary strategies for reducing N excretion and excreta-derived N_(2)O emissions.展开更多
In the selective oxidation of biomass-based 1,2-propanediol(PDO)with oxygen as the terminal oxidant,it is challenging to improve the lactic acid(LA)selectivity for nonnoble metal nanoparticles(NPs)due to their limited...In the selective oxidation of biomass-based 1,2-propanediol(PDO)with oxygen as the terminal oxidant,it is challenging to improve the lactic acid(LA)selectivity for nonnoble metal nanoparticles(NPs)due to their limited oxygen reduction rate and easy C-C cleavage.Given the high economic feasibility of nonnoble metals,i.e.,Cu,in this work,copper and nitrogen codoped porous carbon nanosheets encapsulating ultrafine Cu nanoparticles(Cu@Cu-N-C)were developed to realize highly selective of PDO oxidation to LA.The carbon-encapsulated ultrasmall Cu^(0)NPs in Cu@Cu-N-C have high PDO dehydrogenation activity while N-coordinated Cu(Cu-N)sites are responsible for the high oxygen reduction efficacy.Therefore,the performance of catalytic PDO conversion to LA is optimized by a proposed pathway of PDO→hydroxylacetone→lactaldehyde→LA.Specifically,the enhanced LA selectivity is 88.5%,and the PDO conversion is up to 75.1%in an O_(2)-pressurized reaction system(1.0 MPa O_(2)),superior to other Cu-based catalysts,while in a milder nonpressurized system(O_(2)flow rate of 100 mL min-1),a remarkable LA selectivity(94.2%)is obtained with 39.8%PDO conversion,2.2 times higher than that of supported Au nanoparticles(1%Au/C).Moreover,carbon encapsulation offers Cu@Cu-N-C with strong leaching resistance for better recycling.展开更多
V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy ...V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy (XPS) and catalytic removal of ethanol, acetaldehyde and nitrogen oxides at low temperature (〈300 ?C) were used to assess the properties of the catalysts. The results showed that the sample with 1wt% vanadium exhibited an excellent catalytic performance for simultaneous removal of ethanol, acetaldehyde and nitrogen oxides. The conversions of ethanol, acetaldehyde and nitrogen oxides at 250 ?C were 100%, 74.4% and 98.7%, respectively. V-Pd/γ-Al2O3-TiO2 catalyst with 1 wt% vanadium showed the largest surface area and higher dispersion of vanadium oxide on the catalyst surface, and possessed a larger mole fraction of V4+ species and unique PdO species on the surface, which can be attributed to the strong synergistic effect among palladium, vanadium and the carriers. The higher activity of V-Pd/γ-Al2O3-TiO2 catalyst is related to the V4+ and Pd2+ species on the surface, which might be favorable for the formation of active sites.展开更多
The selective catalytic oxidation (SCO) of NO was studied on a catalyst consisting of iron-manganese oxide supported on mesoporous silica (MPS) with different Mn/Fe ratios. Effects of the amount of manganese and i...The selective catalytic oxidation (SCO) of NO was studied on a catalyst consisting of iron-manganese oxide supported on mesoporous silica (MPS) with different Mn/Fe ratios. Effects of the amount of manganese and iron, oxygen, and calcination temperature on NO conversion were also investigated. It was found that the Mn-Fe/MPS catalyst with a Mn/Fe molar ratio of 1 showed the highest activity at the calcination temperature of 400 °C. The results showed that over this catalyst, NO conversion reached 70% under the condition of 280 °C and a space velocity of 5000 h-1. SO2 and H2O had no adverse impact on the reaction activity when the SCO reaction temperature was above 240 °C. In addition, the SCO activity was suppressed gradually in the presence of SO2 and H2O below 240 °C, and such an effect was reversible after heating treatment.展开更多
The electrochemical methanol oxidation reaction(MOR) is of paramount importance for direct methanol fuel cell(DMFC) application, where efficient catalysts are required to facilitate the complicated multiple charge tra...The electrochemical methanol oxidation reaction(MOR) is of paramount importance for direct methanol fuel cell(DMFC) application, where efficient catalysts are required to facilitate the complicated multiple charge transfer process. The catalyst support not only determines the dispersion status of the catalysts particles, but also exerts great influence on the electronic structure of the catalysts, thereby altering its intrinsic activity. Herein, we demonstrated that nitrogen atoms, assisted by the pre-treatment of carbon matrix with oxidants, can be easily doped into carbon nanotubes at low temperature. The obtained nitrogen-doped carbon nanotubes can effectively improve the dispersion of the supported platinum nanoparticles and facilitate the MOR by modifying the electronic structure of platinum atoms,through catalyst-support interaction.展开更多
Tin/tin oxide materials are key electrocatalysts for selective conversion of CO;to formate/formic acid.Herein we report a tin oxide material with nitrogen doping by using ammonia treatment at elevated temperature. The...Tin/tin oxide materials are key electrocatalysts for selective conversion of CO;to formate/formic acid.Herein we report a tin oxide material with nitrogen doping by using ammonia treatment at elevated temperature. The N doped material demonstrated enhanced electrocatalytic CO;reduction activity, showing high Faradaic efficiency(90%) for formate at -0.65 V vs. RHE with partial current density of 4 mA/cm;.The catalysis was contributed to increased electron negativity of N atom compared to O atom. Additionally, the N-doped catalyst demonstrates sulfur tolerance with retained formate selectivity. The analysis after electrolysis shows that the catalyst structure partially converts to metallic Sn, and thus the combined Sn/N-SnO;is the key for the active CO;catalysis.展开更多
The application of nitrogen(N) fertilizer to increase crop yields has a significant influence on soil methane(CH_4) and nitrous oxide(N_2O) emission/uptake.A meta-analysis was carried out on the effect of N appl...The application of nitrogen(N) fertilizer to increase crop yields has a significant influence on soil methane(CH_4) and nitrous oxide(N_2O) emission/uptake.A meta-analysis was carried out on the effect of N application on(i) CH_4 emissions in rice paddies,(ii) CH_4 uptake in upland fields and(iii) N_2O emissions.The responses of CH_4 emissions to N application in rice paddies were highly variable and overall no effects were found.CH_4 emissions were stimulated at low N application rates(〈100 kg N ha^(-1)) but inhibited at high N rates(〉200 kg N ha^(-1)) as compared to no N fertilizer(control).The response of CH_4 uptake to N application in upland fields was 15%lower than control,with a mean CH_4 uptake factor of-0.001 kg CH_4-C kg^(-1) N.The mean N_2O emission factors were 1.00 and 0.94%for maize(Zea mays) and wheat(Triticum aestivum),respectively,but significantly lower for the rice(Oryza sativa)(0.51%).Compared with controls,N addition overall increased global warming potential of CH_4 and N_2O emissions by 78%.Our result revealed that response of CH_4 emission to N input might depend on the CH_4concentration in rice paddy.The critical factors that affected CH_4 uptake and N_2O emission were N fertilizer application rate and the controls of CH_4 uptake and N_2O emission.The influences of application times,cropping systems and measurement frequency should all be considered when assessing CH_4 and N_2O emissions/uptake induced by N fertilizer.展开更多
The influencing factors and kinetics of oxidative degradation of ammonia nitrogen in high salinity wastewater by sodium hypochlorite oxidation( Na Cl O) were studied. The results showed that the degradation process of...The influencing factors and kinetics of oxidative degradation of ammonia nitrogen in high salinity wastewater by sodium hypochlorite oxidation( Na Cl O) were studied. The results showed that the degradation process of ammonia nitrogen by sodium hypochlorite accorded with a pseudo first-order kinetics model,and the influencing factors included Na Cl O dosage,initial concentration of ammonia nitrogen,salinity,temperature,and so on. When Na Cl O dosage was 0. 6%( MCl∶ MN= 13. 76),the reaction rate constant was up to 0. 015 75 min^(-1). The higher the initial concentration of ammonia nitrogen was,the worse the effect of oxidation reaction was. When the initial concentration did not exceed 45 mg/L,the effect on oxidation reaction rate constant increased with the increase of the initial concentration. Low salinity had no effect on ammonia nitrogen oxidation.When salinity was higher than 2. 0%,the inhibition effect on ammonia nitrogen oxidation would increase,and the reaction rate constant decreased obviously with the increase of salinity. The improvement of reaction temperature was beneficial to ammonia oxidation degradation. As temperature increased from 10 to 35 ℃,the reaction rate constant rose from 0. 00188 to 0. 01043 min^(-1).展开更多
A microreactor system and TPD techniques were used to study the reaction kinetics of the CO+ NO reaction and the adsorption of CO,NO,CO_2 and N_2O over Cu-Mn-O(Ⅰ)and Cu-Mn-Ce-O(Ⅱ) catalysts.The results show that the...A microreactor system and TPD techniques were used to study the reaction kinetics of the CO+ NO reaction and the adsorption of CO,NO,CO_2 and N_2O over Cu-Mn-O(Ⅰ)and Cu-Mn-Ce-O(Ⅱ) catalysts.The results show that the catalytic activity of(Ⅱ)is higher than that of(Ⅰ)for the CO+NO reac- tion,and the higher the conversion of NO,the larger was the activity difference between(Ⅰ)and(Ⅱ).For (Ⅰ)the rate of NO elimination is dependent on the partial pressures of NO,CO,CO_2 with the kinetics or- ders of 0.48,0.56,0.08,respectively.The TPD study shows that the presence of Ce in(Ⅱ)may promote the adsorption of NO,CO on the surface,i.e.an increase of the coverage θ_(NO),θ_(CO),which result in a decrease of the hindrance of the reaction products.For CO_2 and N_2O the situation is in the opposite,the presence of Ce makes the θ_(CO)_2)and θ_(NO)on(Ⅱ)decrease,which weakens the inhibition of CO_2 for the reaction.展开更多
Over the last decades, nitric oxide(NO) has been definitively recognised as one of the key players involved in immunity and inflammation. NO generation was originally described in activated macrophages, which still re...Over the last decades, nitric oxide(NO) has been definitively recognised as one of the key players involved in immunity and inflammation. NO generation was originally described in activated macrophages, which still represent the prototype of NO-producing cells. Notwithstanding, additional cell subsets belonging to both innate and adaptive immunity have been documented to sustain NO propagation by means of the enzymatic activity of different nitric oxide synthase isoforms. Furthermore, due to its chemical characteristics, NO could rapidly react with other free radicals to generate different reactive nitrogen species(RNS), which have been intriguingly associated with many pathological conditions. Nonetheless, the plethora of NO/RNS-mediated effects still remains extremely puzzling. The aim of this manuscript is to dig into the broad literature on the topic to provide intriguing insights on NO-mediated circuits within immune system. We analysed NO and RNS immunological clues arising from their biochemical properties, immunomodulatory activities and finally dealing with their impact on different pathological scenarios with far prompting intriguing perspectives for their pharmacological targeting.展开更多
文摘To achieve high efficiency of nitrogen and phosphorus removal and to investigate the rule of simultaneous nitrification and denitrification phosphorus removal (SNDPR), a whole course of SNDPR damage and recovery was studied in a pilot-scale, anaerobicanoxic oxidation ditch (OD), where the volumes of anaerobic zone, anoxic zone, and ditches zone of the OD system were 7, 21, and 280 L, respectively. The reactor was fed with municipal wastewater with a flow rate of 336 L/d. The concept of simultaneous nitrification and denitrification (SND) rate (rSND) was put forward to quantify SND. The results indicate that: (1) high nitrogen and phosphorus removal efficiencies were achieved during the stable SND phase, total nitrogen (TN) and total phosphate (TP) removal rates were 80% and 85%, respectively; (2) when the system was aerated excessively, the stability of SND was damaged, and rSND dropped from 80% to 20% or less; (3) the natural logarithm of the ratio of NOx to NH4^+ in the effluent had a linear correlation to oxidation-reduction potential (ORP); (4) when NO3^- was less than 6 mg/L, high phosphorus removal efficiency could be achieved; (5) denitrifying phosphorus removal (DNPR) could take place in the anaerobic-anoxic OD system. The major innovation was that the SND rate was devised and quantified.
文摘Dielectric barrier discharge (DBD) plasma was utilized to oxidize NO contained in the exhaust gas to NO2, ultimately improve the selective catalytic reduction of nitrogen oxides (NOx). In the one case, DBD was created directly in the exhaust gas (direct application), and in the an other case, ozone produced by DBD was injected into the exhaust gas (indirect application). A comparative study between such direct and indirect applications of DBD plasma was made in terms of the NOx removal efficiency and the energy consumption. The NO2 content in the exhaust gas was changed by the voltage applied to the DBD device (for direct application) or by the amount of ozone added to the exhaust gas (for indirect application). In both cases, NO was easily oxidized to NO2, and the change in NO2 content largely affected the NOx removal performance of the catalytic reactor placed downstream, where both NO and NO2 were reduced to N2 in the presence of ammonia as the reducing agent. The experiments were primarily concerned with the effect of reaction temperature on the catalytic NOx reduction at various NO2 contents. The direct and indirect applications of DBD were found to remarkably improve the catalytic NOx reduction, especially at low temperatures.
基金The project supported by the Basic Research Program of the Korea Science & Engineering Foundation (KOSEF) (No. R05-2001-000-01247-0)
文摘A single-stage plasma-catalytic reactor in which catalytic materials werepacked was used to remove nitrogen oxides. The packing material was scoria being made of variousmetal oxides including Al_2O_3, MgO, TiO_2, etc. Scoria was able to act not only as dielectricpellets but also as a catalyst in the presence of reducing agent such as ethylene and ammonia.Without plasma discharge, scoria did not work well as a catalyst in the temperature range of 100 ℃to 200 ℃, showing less than 10% of NOx removal efficiency. When plasma is produced inside thereactor, the NOx removal efficiency could be increased to 60% in this temperature range.
基金supported by the National Natural Science Foundation of China(Grants No.20277009)
文摘The potential of using denitrifying and nitrifying concurrent biofilters for the removal of nitrogen oxides from synthetic gas streams was studied under the condition of high oxygen concentration. It was found that more than 85% of nitric oxide was removed from synthetic combustion gas-streams which contained 20% oxygen and 350 μL/L NO, with a residence time of 60 seconds. In the process, it was found that the existing of oxygen showed no evident negative effect on the efficiency of nitrogen removal.
文摘This paper reports the studies conducted on removal of oxides ofnitrogen (NOx) from diesel engine exhaust using electrical dischargeplasma combined with adsorbing materials such as molecular sieves.This study is being reported for the first time. The exhaust is takenfrom a diesel engine of 6 kW under no load conditions. Thecharacteristic behavior of a pulse energized dielectric barrierdischarge reactor in the diesel exhaust treatment is reported. TheNOx removal was not significant (36/100) when the reactor without anypacking was used.
基金The National Key Research and Development Project of China under contract No.2019YFC1407802the Fund of State Environmental Protection Key Laboratory of Coastal Ecosystem under contract No.202112+3 种基金the Open Fund of Key Laboratory of Marine Ecological Environment Science and EngineeringMinistry of Natural Resources under contract No.MESE-2019-06the National Natural Science Foundation of China under contract No.41876078the Shandong Provincial Natural Science Foundation of China under contract No.ZR2018MD016。
文摘Total dissolved nitrogen(TDN) is an important parameter for assessing the nutrient cycling and status of natural waters.The accurate determination of TDN in natural waters is essential for assessing its contents and distinguishing different forms of nitrogen in the water.The TDN in various systems has been largely documented,and the concentrations of TDN are usually obtained using high-temperature catalytic(HTC) or persulfate oxidation(PO).However,the accuracy of these methods and their suitability for all types of natural waters are still unclear.To explore both methods in-depth,assorted samples were tested,including eight solutions composed of nitrogen-containing compounds(3 dissolved inorganic nitrogen fractions:NO_(3)^(-),NO_(2)^(-)and NH_(4)^(+);5 organic compounds:EDTA-2Na,vitamin B1,vitamin B12,amino acids,and urea) and 105 natural waters which were collected from an open ocean(Northwest Pacific Ocean,28),a marginal sea(Yellow Sea,34),an estuary(Huanghe River mouth,31),rivers(Huanghe River,4;Licun River,4),and precipitations(4 samples).The results showed that heterocycles and molecular dimensions had certain effects on the oxidation efficiency of the PO method but had little effect on HTC.There was no significant difference between the two methods for natural waters,but HTC was more suitable for deep-sea samples with low TDN concentrations(less than 10 μmol/L) and low organic activity.Overall,HTC has a relatively simple measurement process,a high degree of automation,and low error.Therefore,HTC can be recommended to determine the TDN of samples in freshwater and seawater.
文摘We evaluate nitrogen oxides pollution in Takamatsu and Utazu area in Kagawa prefecture, Japan. Annually observations for nitrogen oxides (nitrogen dioxide;NO2, nitric oxide;NO) (1990-2007) were obtained from data base of Kagawa prefecture, Japan. Changes in NO2 and NO in Takamatsu and Utazu area were evaluated and compared. In 2007, NO2, NO and NO2 + NO (ppm) in Takamatsu area were higher than those in Utazu area. However, NO2 /NO + NO2 in Takamatsu area was lower than that in Utazu area. From 1990 to 2007, mean of NO2 in a day over the level of 0.06 ppm was 30 days in Takamatsu area and only one day in Utazu area. Mean of NO2, NO and NO2 + NO was significantly higher and NO2/NO + NO2 was lower in Takamatsu area than that in Utazu area. In addition, NO2, NO and NO2 + NO were negatively correlated and NO2/NO + NO2 was positively correlated with years (1990-2007) in Takamatsu area. The level of nitrogen oxides pollution in Utazu area was lower than Takamatsu area. Further observation is required for preventing nitrogen oxides pollution in Kagawa prefecture, Japan.
基金supported by Beijing Captial Agribusiness&Food Group Co.,Ltd.‘Integrated Innovation and Industrial Application of"Green Digital Intelligence"Technology in the Whole Dairy Industry Chain’(SNSPKJ2022)National Natural Science Foundation of China(32302767).
文摘Ruminants play a critical role in our food system by converting plant biomass that humans cannot or choose not to consume into edible high-quality food.However,ruminant excreta is a significant source of nitrous oxide(N_(2)O),a potent greenhouse gas with a long-term global warming potential 298 times that of carbon dioxide.Natural phytochemicals or forages containing phytochemicals have shown the potential to improve the efficiency of nitrogen(N)utilization and decrease N_(2)O emissions from the excreta of ruminants.Dietary inclusion of tannins can shift more of the excreted N to the feces,alter the urinary N composition and consequently reduce N_(2)O emissions from excreta.Essential oils or saponins could inhibit rumen ammonia production and decrease urinary N excretion.In grazed pastures,large amounts of glucosinolates or aucubin can be introduced into pasture soils when animals consume plants rich in these compounds and then excrete them or their metabolites in the urine or feces.If inhibitory compounds are excreted in the urine,they would be directly applied to the urine patch to reduce nitrification and subsequent N_(2)O emissions.The phytochemicals’role in sustainable ruminant production is undeniable,but much uncertainty remains.Inconsistency,transient effects,and adverse effects limit the effectiveness of these phytochemicals for reducing N losses.In this review,we will identify some current phytochemicals found in feed that have the potential to manipulate ruminant N excretion or mitigate N_(2)O production and deliberate the challenges and opportunities associated with using phytochemicals or forages rich in phytochemicals as dietary strategies for reducing N excretion and excreta-derived N_(2)O emissions.
基金supported by the National Natural Science Foundation of China(32371407,82160421)the Natural Science Foundation of Jiangsu Province(BK20211322)。
文摘In the selective oxidation of biomass-based 1,2-propanediol(PDO)with oxygen as the terminal oxidant,it is challenging to improve the lactic acid(LA)selectivity for nonnoble metal nanoparticles(NPs)due to their limited oxygen reduction rate and easy C-C cleavage.Given the high economic feasibility of nonnoble metals,i.e.,Cu,in this work,copper and nitrogen codoped porous carbon nanosheets encapsulating ultrafine Cu nanoparticles(Cu@Cu-N-C)were developed to realize highly selective of PDO oxidation to LA.The carbon-encapsulated ultrasmall Cu^(0)NPs in Cu@Cu-N-C have high PDO dehydrogenation activity while N-coordinated Cu(Cu-N)sites are responsible for the high oxygen reduction efficacy.Therefore,the performance of catalytic PDO conversion to LA is optimized by a proposed pathway of PDO→hydroxylacetone→lactaldehyde→LA.Specifically,the enhanced LA selectivity is 88.5%,and the PDO conversion is up to 75.1%in an O_(2)-pressurized reaction system(1.0 MPa O_(2)),superior to other Cu-based catalysts,while in a milder nonpressurized system(O_(2)flow rate of 100 mL min-1),a remarkable LA selectivity(94.2%)is obtained with 39.8%PDO conversion,2.2 times higher than that of supported Au nanoparticles(1%Au/C).Moreover,carbon encapsulation offers Cu@Cu-N-C with strong leaching resistance for better recycling.
基金supported by the National Natural Science Foundation of China (No. 21073131)the Shanxi Natural Science Foundation(No. 2009011011-3)
文摘V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy (XPS) and catalytic removal of ethanol, acetaldehyde and nitrogen oxides at low temperature (〈300 ?C) were used to assess the properties of the catalysts. The results showed that the sample with 1wt% vanadium exhibited an excellent catalytic performance for simultaneous removal of ethanol, acetaldehyde and nitrogen oxides. The conversions of ethanol, acetaldehyde and nitrogen oxides at 250 ?C were 100%, 74.4% and 98.7%, respectively. V-Pd/γ-Al2O3-TiO2 catalyst with 1 wt% vanadium showed the largest surface area and higher dispersion of vanadium oxide on the catalyst surface, and possessed a larger mole fraction of V4+ species and unique PdO species on the surface, which can be attributed to the strong synergistic effect among palladium, vanadium and the carriers. The higher activity of V-Pd/γ-Al2O3-TiO2 catalyst is related to the V4+ and Pd2+ species on the surface, which might be favorable for the formation of active sites.
基金the Hunan Provincial Natural Science Foundation of China (No. 07 JJ4003)
文摘The selective catalytic oxidation (SCO) of NO was studied on a catalyst consisting of iron-manganese oxide supported on mesoporous silica (MPS) with different Mn/Fe ratios. Effects of the amount of manganese and iron, oxygen, and calcination temperature on NO conversion were also investigated. It was found that the Mn-Fe/MPS catalyst with a Mn/Fe molar ratio of 1 showed the highest activity at the calcination temperature of 400 °C. The results showed that over this catalyst, NO conversion reached 70% under the condition of 280 °C and a space velocity of 5000 h-1. SO2 and H2O had no adverse impact on the reaction activity when the SCO reaction temperature was above 240 °C. In addition, the SCO activity was suppressed gradually in the presence of SO2 and H2O below 240 °C, and such an effect was reversible after heating treatment.
基金supported by the National Natural Science Foundation of China (21433003, 21633008)the Jilin Province Science and Technology Development Program (20150101066JC, 20160622037JC, 20170203003SF, and 20170520150JH)the Hundred Talents Program of the Chinese Academy of Sciences and the Recruitment Program of Foreign Experts (WQ20122200077)
文摘The electrochemical methanol oxidation reaction(MOR) is of paramount importance for direct methanol fuel cell(DMFC) application, where efficient catalysts are required to facilitate the complicated multiple charge transfer process. The catalyst support not only determines the dispersion status of the catalysts particles, but also exerts great influence on the electronic structure of the catalysts, thereby altering its intrinsic activity. Herein, we demonstrated that nitrogen atoms, assisted by the pre-treatment of carbon matrix with oxidants, can be easily doped into carbon nanotubes at low temperature. The obtained nitrogen-doped carbon nanotubes can effectively improve the dispersion of the supported platinum nanoparticles and facilitate the MOR by modifying the electronic structure of platinum atoms,through catalyst-support interaction.
基金financially supported by Key Research Program of the Chinese Academy of Sciences (ZDRW-ZS-2016-3)the National Key Research and Development Program of China (2016YFB0600901)the Instrument Developing Project of the Chinese Academy of Sciences
文摘Tin/tin oxide materials are key electrocatalysts for selective conversion of CO;to formate/formic acid.Herein we report a tin oxide material with nitrogen doping by using ammonia treatment at elevated temperature. The N doped material demonstrated enhanced electrocatalytic CO;reduction activity, showing high Faradaic efficiency(90%) for formate at -0.65 V vs. RHE with partial current density of 4 mA/cm;.The catalysis was contributed to increased electron negativity of N atom compared to O atom. Additionally, the N-doped catalyst demonstrates sulfur tolerance with retained formate selectivity. The analysis after electrolysis shows that the catalyst structure partially converts to metallic Sn, and thus the combined Sn/N-SnO;is the key for the active CO;catalysis.
基金financed by the Chinese Academy of Sciences for Strategic Priority Research Program(XDA05050602)the Key Technologies R&D Program of China during the 12th Five-Year Plan period of China(2012BAD14B01-1)
文摘The application of nitrogen(N) fertilizer to increase crop yields has a significant influence on soil methane(CH_4) and nitrous oxide(N_2O) emission/uptake.A meta-analysis was carried out on the effect of N application on(i) CH_4 emissions in rice paddies,(ii) CH_4 uptake in upland fields and(iii) N_2O emissions.The responses of CH_4 emissions to N application in rice paddies were highly variable and overall no effects were found.CH_4 emissions were stimulated at low N application rates(〈100 kg N ha^(-1)) but inhibited at high N rates(〉200 kg N ha^(-1)) as compared to no N fertilizer(control).The response of CH_4 uptake to N application in upland fields was 15%lower than control,with a mean CH_4 uptake factor of-0.001 kg CH_4-C kg^(-1) N.The mean N_2O emission factors were 1.00 and 0.94%for maize(Zea mays) and wheat(Triticum aestivum),respectively,but significantly lower for the rice(Oryza sativa)(0.51%).Compared with controls,N addition overall increased global warming potential of CH_4 and N_2O emissions by 78%.Our result revealed that response of CH_4 emission to N input might depend on the CH_4concentration in rice paddy.The critical factors that affected CH_4 uptake and N_2O emission were N fertilizer application rate and the controls of CH_4 uptake and N_2O emission.The influences of application times,cropping systems and measurement frequency should all be considered when assessing CH_4 and N_2O emissions/uptake induced by N fertilizer.
基金Supported by Project for Achievement Transformation of High and New Technology in Shanghai City(201405267)
文摘The influencing factors and kinetics of oxidative degradation of ammonia nitrogen in high salinity wastewater by sodium hypochlorite oxidation( Na Cl O) were studied. The results showed that the degradation process of ammonia nitrogen by sodium hypochlorite accorded with a pseudo first-order kinetics model,and the influencing factors included Na Cl O dosage,initial concentration of ammonia nitrogen,salinity,temperature,and so on. When Na Cl O dosage was 0. 6%( MCl∶ MN= 13. 76),the reaction rate constant was up to 0. 015 75 min^(-1). The higher the initial concentration of ammonia nitrogen was,the worse the effect of oxidation reaction was. When the initial concentration did not exceed 45 mg/L,the effect on oxidation reaction rate constant increased with the increase of the initial concentration. Low salinity had no effect on ammonia nitrogen oxidation.When salinity was higher than 2. 0%,the inhibition effect on ammonia nitrogen oxidation would increase,and the reaction rate constant decreased obviously with the increase of salinity. The improvement of reaction temperature was beneficial to ammonia oxidation degradation. As temperature increased from 10 to 35 ℃,the reaction rate constant rose from 0. 00188 to 0. 01043 min^(-1).
文摘A microreactor system and TPD techniques were used to study the reaction kinetics of the CO+ NO reaction and the adsorption of CO,NO,CO_2 and N_2O over Cu-Mn-O(Ⅰ)and Cu-Mn-Ce-O(Ⅱ) catalysts.The results show that the catalytic activity of(Ⅱ)is higher than that of(Ⅰ)for the CO+NO reac- tion,and the higher the conversion of NO,the larger was the activity difference between(Ⅰ)and(Ⅱ).For (Ⅰ)the rate of NO elimination is dependent on the partial pressures of NO,CO,CO_2 with the kinetics or- ders of 0.48,0.56,0.08,respectively.The TPD study shows that the presence of Ce in(Ⅱ)may promote the adsorption of NO,CO on the surface,i.e.an increase of the coverage θ_(NO),θ_(CO),which result in a decrease of the hindrance of the reaction products.For CO_2 and N_2O the situation is in the opposite,the presence of Ce makes the θ_(CO)_2)and θ_(NO)on(Ⅱ)decrease,which weakens the inhibition of CO_2 for the reaction.
基金Supported by Grant from the Italian Ministry of Health,BANDO GIOVANI RICERCATORI,No.2009-GR-2009-1558698Agnellini AHR was granted by Cariparo Fundation Fellowship
文摘Over the last decades, nitric oxide(NO) has been definitively recognised as one of the key players involved in immunity and inflammation. NO generation was originally described in activated macrophages, which still represent the prototype of NO-producing cells. Notwithstanding, additional cell subsets belonging to both innate and adaptive immunity have been documented to sustain NO propagation by means of the enzymatic activity of different nitric oxide synthase isoforms. Furthermore, due to its chemical characteristics, NO could rapidly react with other free radicals to generate different reactive nitrogen species(RNS), which have been intriguingly associated with many pathological conditions. Nonetheless, the plethora of NO/RNS-mediated effects still remains extremely puzzling. The aim of this manuscript is to dig into the broad literature on the topic to provide intriguing insights on NO-mediated circuits within immune system. We analysed NO and RNS immunological clues arising from their biochemical properties, immunomodulatory activities and finally dealing with their impact on different pathological scenarios with far prompting intriguing perspectives for their pharmacological targeting.