Nitrous acid, HNO2, is an important precursor of OH radicals in the troposphere. Measurements of HNO2 and NO2, using differential optical absorption spectroscopy （DOAS）, were performed in Shanghai, China for a perio...Nitrous acid, HNO2, is an important precursor of OH radicals in the troposphere. Measurements of HNO2 and NO2, using differential optical absorption spectroscopy （DOAS）, were performed in Shanghai, China for a period from October 22, 2004 to January 4, 2005. The mean （and median） hourly concentrations of HNO2 and NO2 during this period were 1.1 （0.7） ppb and 24 （21.4） ppb respectively. A correlation between HNO2/NO2 and PM10 mass concentrations was obtained. This correlation suggests that significant heterogeneous chemical production of HNO2 may occur through NO2 reactions on aerosol surfaces. This hypothesis was further supported by detailed analysis of selected pollution episodes in this study. At the same time, the water dependence of HNO2 formation was studied by analysis of relative humidity （RH）. It showed that the maximum HNO2/NO2 ratio was increased along with RH below 70% and inhibited at RH〉70%.展开更多
Digested wastewater contains pathogenic microorganisms and high ammonia concentrations,which can pose a potential risk to public health.Effective removal of pathogens and nitrogen is crucial for the post-treatment of ...Digested wastewater contains pathogenic microorganisms and high ammonia concentrations,which can pose a potential risk to public health.Effective removal of pathogens and nitrogen is crucial for the post-treatment of digested wastewater.Partial nitrification-anammox is an energy-saving nitrogen removal process.Free nitrous acid(FNA),an intermediate product of partial nitrification,has the potential to inactivate microorganisms.However,the efficiency and mechanisms of FNA-related inactivation in pathogens during partial nitrification remains unclear.In this study,Enterococcus and Escherichia coli(E.coli)were selected to investigate the efficiency and mechanisms of FNA-related inactivation in partial nitrification process.The results revealed that 83%±13%and 59%±27%of E.coli and Enterococcus were removed,respectively,in partial nitrification process at FNA concentrations of 0.023−0.028 mg/L.When the concentration of FNA increased from 0 to 0.5 mg/L,the inactivation efficiencies of E.coli and Enterococcus increased from 0 to 99.9%and 89.9%,respectively.Enterococcus exhibited a higher resistance to FNA attack compared to E.coli.3D-laser scanning microscopy(3D-LSM)and scanning electron microscopy(SEM)revealed that FNA exposure caused the surface collapse of E.coli and Enterococcus,as well as visible pore formation on the surface of E.coli cells.4',6-Diamidino-2-phenylindole dihydrochloride n-hydrate(DAPI)/propidium iodide(PI)and biomolecule leakage confirmed that inactivation of E.coli and Enterococcus occurred due to breakdown of cell walls and cell membranes.These findings indicate that partial nitrification process can be used for the removal of residual pathogenic microorganisms.展开更多
The biocidal effects of free nitrous acid (FNA) have found applications in multiple units in an urban wastewater system, including sewer networks, wastewater treatment processes, and sludge treatment processes. Howeve...The biocidal effects of free nitrous acid (FNA) have found applications in multiple units in an urban wastewater system, including sewer networks, wastewater treatment processes, and sludge treatment processes. However, these applications are associated with chemical costs as both nitrite and acid are needed to produce FNA at the required levels. The recent discovery of novel acid-tolerant ammonia oxidizers offers the possibility to produce FNA from domestic wastewater, enabling the development of next-generation FNA-based technologies capable of achieving self-sustaining FNA production. In this study, we focus on the concept of in situ FNA generation facilitated by acid-tolerant ammonia oxidizers and highlight the multiple benefits it creates, after a brief review of the historical development of FNA-based technologies. We will discuss how wastewater systems can be made more energy-efficient and sustainable by leveraging the potential of acid-tolerant ammonia oxidizers.展开更多
Nitrous oxide is one of the most commonly used inhalational anesthetic agents used in practice.It is a cost-effective,pleasant,safe,and versatile anesthetic agent with many desirable properties like good quality analg...Nitrous oxide is one of the most commonly used inhalational anesthetic agents used in practice.It is a cost-effective,pleasant,safe,and versatile anesthetic agent with many desirable properties like good quality analgesia,decreased awareness,accelerated induction and recovery from anesthesia,and reduced utilization of other expensive inhalational agents with potential cost savings.The use of nitrous oxide has been questioned by a lot of studies and case reports perceiving its adverse systemic,hematological,immune,and neurologic adverse effects.However,the literature in the recent past has tried to resolve the controversies related to its use.The concerns over an increase in cardiovascular complications and mortality following nitrous oxide use have been negated by recent data.However,its use in certain vulnerable populations like children with cobalamin and folate deficiency or defects in their metabolic pathways remains a cause of concern for its toxic effects.In this narrative review,we aim to discuss the pharmacological properties of nitrous oxide,the potential advantages and drawbacks of the use of nitrous oxide in children,address the neurodevelopmental and other systemic effects,and throw light on the evidence regarding the safety of nitrous oxide use and its current role in pediatric procedural sedation and anesthesia practice.The literature related to its use in the pediatric population for painful procedures and surgeries has been summarized.展开更多
full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban si...full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.展开更多
The sustainable recovery and utilization of sludge bioenergy within a circular economy context has drawn increasing attention,but there is currently a shortage of reliable technology.This study presents an innovative ...The sustainable recovery and utilization of sludge bioenergy within a circular economy context has drawn increasing attention,but there is currently a shortage of reliable technology.This study presents an innovative biotechnology based on free nitrous acid(FNA)to realize sustainable organics recovery from waste activated sludge(WAS)in-situ,driving efficient nitrogen removal from ammonia rich mature landfill leachate by integrating partial nitrification,fermentation,and denitrification process(PN/DN-F/DN).First,ammonia((1708.5±142.9)mg·L^(-1))in mature landfill leachate is oxidized to nitrite in the aerobic stage of a partial nitrification coupling denitrification(PN/DN)sequencing batch reactor(SBR),with nitrite accumulation ratio of 95.4%±2.5%.Then,intermediate effluent(NO_(2)^(-)-N=(1196.9±184.2)mg·L^(-1))of the PN/DN-SBR,along with concentrated WAS(volatile solids(VSs)=(15119.8±2484.2)mg·L^(-1)),is fed into an anoxic reactor for fermentation coupling denitrification process(F/DN).FNA,the protonated form of nitrite,degrades organics in the WAS to the soluble fraction by the biocidal effect,and the released organics are utilized by denitrifiers to drive NOx-reduction.An ultra-fast sludge reduction rate of 4.89 kg·m^(-3)·d^(-1) and nitrogen removal rate of 0.46 kg·m^(-3)·d^(-1) were realized in the process.Finally,F/DN-SBR effluent containing organics is refluxed to PN/DN-SBR for secondary denitrification in the post anoxic stage.After 175 d operation,an average of 19350.6 mg chemical oxygen demand organics were recovered per operational cycle,with 95.2%nitrogen removal and 53.4%sludge reduction.PN/DN-F/DN is of great significance for promoting a paradigm transformation from energy consumption to energy neutral,specifically,the total benefit in equivalent terms of energy was 291.8 kW·h·t^(-1) total solid.展开更多
Two series of ZSM-5 and beta zeolites were pretreated in 1.0 mol/L HNO3 solution at room temper-ature for various time periods. The catalytic performances of their Fe-exchanged products in N2O decomposition were evalu...Two series of ZSM-5 and beta zeolites were pretreated in 1.0 mol/L HNO3 solution at room temper-ature for various time periods. The catalytic performances of their Fe-exchanged products in N2O decomposition were evaluated. The Fe-zeolite catalysts were characterized using N2 adsorp-tion-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, ultra-violet-visible spectroscopy, temperature-programmed desorption of NH3, and scanning and trans-mission electron microscopies. For the ZSM-5 zeolite, acid leaching primarily takes place on the crystal surface and the particle size is reduced, therefore the pore channels are shortened. However, because of the good stability of MFI zeolites, the acid does not greatly penetrate the pore channels and new mesopores are not created. For the beta zeolite, because the amorphous material is in-clined to dissolve（deagglomerate）, some of the micropores are slightly dilated. The improved cata-lytic activities can be explained by the increased active Fe loading as a result of structural changes.展开更多
Alpha radiolysis of nitric acid aqueous solution by a ^(238)Pu source is investigated experimentally and theoretically.The time dependence of the nitrous acid yield on dose rate,nitric acid concentration,and nitrate i...Alpha radiolysis of nitric acid aqueous solution by a ^(238)Pu source is investigated experimentally and theoretically.The time dependence of the nitrous acid yield on dose rate,nitric acid concentration,and nitrate ion concentration is studied.A novel kinetic model for the α-radiolysis of nitric acid aqueous solution is established,by considering the direct and indirect effects.The simulation results agree well with the experimental data,indicating the validity of our model to treat the reaction paths for generation and consumption of nitrous acid.It is shown that the redox reactions involving Pu cannot be neglected in theα-radiolysis of the solution.The results provide a better understanding of the α-ray radiolysis of aqueous nitric acid.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
The inhibition of nitrification by mixing nitrification inhibitors(NI)with fertilizers is emerging as an effective method to reduce fertilizer-induced nitrous oxide(N_(2)O)emissions.The additive 3,4-dimethylpyrazole p...The inhibition of nitrification by mixing nitrification inhibitors(NI)with fertilizers is emerging as an effective method to reduce fertilizer-induced nitrous oxide(N_(2)O)emissions.The additive 3,4-dimethylpyrazole phosphate(DMPP)apparently inhibits ammonia oxidizing bacteria(AOB)more than ammonia oxidizing archaea(AOA),which dominate the nitrification in alkaline and acid soil,respectively.However,the efficacy of DMPP in terms of nitrogen sources interacting with soil properties remains unclear.We therefore conducted a microcosm experiment using three typical Chinese agricultural soils with contrasting pH values(fluvo-aquic soil,black soil and red soil),which were fertilized with either digestate or urea in conjunction with a range of DMPP concentrations.In the alkaline fluvo-aquic soil,fertilization with either urea or digestate induced a peak in N_(2)O emission(60μg N kg^(-1)d^(-1))coinciding with the rapid nitrification within 3 d following fertilization.DMPP almost eliminated this peak in N_(2)O emission,reducing it by nearly 90%,despite the fact that the nitrification rate was only reduced by 50%.In the acid black soil,only the digestate induced an N_(2)O emission that increased gradually,reaching its maximum(20μg N kg^(-1)d^(-1))after 5–7 d.The nitrification rate and N_(2)O emission were both marginally reduced by DMPP in the black soil,and the N_(2)O yield(N_(2)O-N per NO2–+NO3–-N produced)was exceptionally high at 3.5%,suggesting that the digestate induced heterotrophic denitrification.In the acid red soil,the N_(2)O emission spiked in the digestate and urea treatments at 50 and 10μg N kg^(-1)d^(-1),respectively,and DMPP reduced the rates substantially by nearly 70%.Compared with 0.5%DMPP,the higher concentrations of DMPP(1.0 to 1.5%)did not exert a significantly(P<0.05)better inhibition effect on the N_(2)O emissions in these soils(either with digestate or urea).This study highlights the importance of matching the nitrogen sources,soil properties and NIs to achieve a high efficiency of N_(2)O emission reduction.展开更多
基金The National Natural Science Foundation of China (No. 20277006) and the Fudan University Foundation for Young Scientists (No.EXH 6286301)
文摘Nitrous acid, HNO2, is an important precursor of OH radicals in the troposphere. Measurements of HNO2 and NO2, using differential optical absorption spectroscopy （DOAS）, were performed in Shanghai, China for a period from October 22, 2004 to January 4, 2005. The mean （and median） hourly concentrations of HNO2 and NO2 during this period were 1.1 （0.7） ppb and 24 （21.4） ppb respectively. A correlation between HNO2/NO2 and PM10 mass concentrations was obtained. This correlation suggests that significant heterogeneous chemical production of HNO2 may occur through NO2 reactions on aerosol surfaces. This hypothesis was further supported by detailed analysis of selected pollution episodes in this study. At the same time, the water dependence of HNO2 formation was studied by analysis of relative humidity （RH）. It showed that the maximum HNO2/NO2 ratio was increased along with RH below 70% and inhibited at RH〉70%.
基金supported by the Natural Science Foundation of Anhui Province(China)(No.2208085ME145)the Key Project of Science and Technology in Anhui Province(China)(No.1801041130)the National Key R&D Program of China(No.2019YFC0408502).
文摘Digested wastewater contains pathogenic microorganisms and high ammonia concentrations,which can pose a potential risk to public health.Effective removal of pathogens and nitrogen is crucial for the post-treatment of digested wastewater.Partial nitrification-anammox is an energy-saving nitrogen removal process.Free nitrous acid(FNA),an intermediate product of partial nitrification,has the potential to inactivate microorganisms.However,the efficiency and mechanisms of FNA-related inactivation in pathogens during partial nitrification remains unclear.In this study,Enterococcus and Escherichia coli(E.coli)were selected to investigate the efficiency and mechanisms of FNA-related inactivation in partial nitrification process.The results revealed that 83%±13%and 59%±27%of E.coli and Enterococcus were removed,respectively,in partial nitrification process at FNA concentrations of 0.023−0.028 mg/L.When the concentration of FNA increased from 0 to 0.5 mg/L,the inactivation efficiencies of E.coli and Enterococcus increased from 0 to 99.9%and 89.9%,respectively.Enterococcus exhibited a higher resistance to FNA attack compared to E.coli.3D-laser scanning microscopy(3D-LSM)and scanning electron microscopy(SEM)revealed that FNA exposure caused the surface collapse of E.coli and Enterococcus,as well as visible pore formation on the surface of E.coli cells.4',6-Diamidino-2-phenylindole dihydrochloride n-hydrate(DAPI)/propidium iodide(PI)and biomolecule leakage confirmed that inactivation of E.coli and Enterococcus occurred due to breakdown of cell walls and cell membranes.These findings indicate that partial nitrification process can be used for the removal of residual pathogenic microorganisms.
文摘The biocidal effects of free nitrous acid (FNA) have found applications in multiple units in an urban wastewater system, including sewer networks, wastewater treatment processes, and sludge treatment processes. However, these applications are associated with chemical costs as both nitrite and acid are needed to produce FNA at the required levels. The recent discovery of novel acid-tolerant ammonia oxidizers offers the possibility to produce FNA from domestic wastewater, enabling the development of next-generation FNA-based technologies capable of achieving self-sustaining FNA production. In this study, we focus on the concept of in situ FNA generation facilitated by acid-tolerant ammonia oxidizers and highlight the multiple benefits it creates, after a brief review of the historical development of FNA-based technologies. We will discuss how wastewater systems can be made more energy-efficient and sustainable by leveraging the potential of acid-tolerant ammonia oxidizers.
文摘Nitrous oxide is one of the most commonly used inhalational anesthetic agents used in practice.It is a cost-effective,pleasant,safe,and versatile anesthetic agent with many desirable properties like good quality analgesia,decreased awareness,accelerated induction and recovery from anesthesia,and reduced utilization of other expensive inhalational agents with potential cost savings.The use of nitrous oxide has been questioned by a lot of studies and case reports perceiving its adverse systemic,hematological,immune,and neurologic adverse effects.However,the literature in the recent past has tried to resolve the controversies related to its use.The concerns over an increase in cardiovascular complications and mortality following nitrous oxide use have been negated by recent data.However,its use in certain vulnerable populations like children with cobalamin and folate deficiency or defects in their metabolic pathways remains a cause of concern for its toxic effects.In this narrative review,we aim to discuss the pharmacological properties of nitrous oxide,the potential advantages and drawbacks of the use of nitrous oxide in children,address the neurodevelopmental and other systemic effects,and throw light on the evidence regarding the safety of nitrous oxide use and its current role in pediatric procedural sedation and anesthesia practice.The literature related to its use in the pediatric population for painful procedures and surgeries has been summarized.
基金supported by the National Natural Science Foundation of China[grant numbers 42275120 and 42075111]the National Key Research and Development Program[grant number 2023YFC3706101]。
文摘full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.
基金supported by the Beijing Natural Science Foundation (8222040)Key Program of National Natural Science Foundation of China (52131004)+4 种基金Young Elite Scientists Sponsorship Program by China association for science and technology (CAST,YESS20220508)Young Elite Scientists Sponsorship Program by Beijing Association for Science and Technology (BAST,BYESS2023183)Innovation and Entrepreneurship Leading Team Project in Guangzhou (CYLJTD-201607)Key Research and Developmental Program of Shandong Province (2020CXGC011404)Cultivating Fund of Faculty of Environment and Life,Beijing University of Technology (PY202302).
文摘The sustainable recovery and utilization of sludge bioenergy within a circular economy context has drawn increasing attention,but there is currently a shortage of reliable technology.This study presents an innovative biotechnology based on free nitrous acid(FNA)to realize sustainable organics recovery from waste activated sludge(WAS)in-situ,driving efficient nitrogen removal from ammonia rich mature landfill leachate by integrating partial nitrification,fermentation,and denitrification process(PN/DN-F/DN).First,ammonia((1708.5±142.9)mg·L^(-1))in mature landfill leachate is oxidized to nitrite in the aerobic stage of a partial nitrification coupling denitrification(PN/DN)sequencing batch reactor(SBR),with nitrite accumulation ratio of 95.4%±2.5%.Then,intermediate effluent(NO_(2)^(-)-N=(1196.9±184.2)mg·L^(-1))of the PN/DN-SBR,along with concentrated WAS(volatile solids(VSs)=(15119.8±2484.2)mg·L^(-1)),is fed into an anoxic reactor for fermentation coupling denitrification process(F/DN).FNA,the protonated form of nitrite,degrades organics in the WAS to the soluble fraction by the biocidal effect,and the released organics are utilized by denitrifiers to drive NOx-reduction.An ultra-fast sludge reduction rate of 4.89 kg·m^(-3)·d^(-1) and nitrogen removal rate of 0.46 kg·m^(-3)·d^(-1) were realized in the process.Finally,F/DN-SBR effluent containing organics is refluxed to PN/DN-SBR for secondary denitrification in the post anoxic stage.After 175 d operation,an average of 19350.6 mg chemical oxygen demand organics were recovered per operational cycle,with 95.2%nitrogen removal and 53.4%sludge reduction.PN/DN-F/DN is of great significance for promoting a paradigm transformation from energy consumption to energy neutral,specifically,the total benefit in equivalent terms of energy was 291.8 kW·h·t^(-1) total solid.
基金supported by the National Natural Science Foundation of China (21307144,21307007)Science of Technology Development Plan of Jilin Province of China (20140520150JH)~~
文摘Two series of ZSM-5 and beta zeolites were pretreated in 1.0 mol/L HNO3 solution at room temper-ature for various time periods. The catalytic performances of their Fe-exchanged products in N2O decomposition were evaluated. The Fe-zeolite catalysts were characterized using N2 adsorp-tion-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, ultra-violet-visible spectroscopy, temperature-programmed desorption of NH3, and scanning and trans-mission electron microscopies. For the ZSM-5 zeolite, acid leaching primarily takes place on the crystal surface and the particle size is reduced, therefore the pore channels are shortened. However, because of the good stability of MFI zeolites, the acid does not greatly penetrate the pore channels and new mesopores are not created. For the beta zeolite, because the amorphous material is in-clined to dissolve（deagglomerate）, some of the micropores are slightly dilated. The improved cata-lytic activities can be explained by the increased active Fe loading as a result of structural changes.
基金partly supported by the National Natural Science Foundation of China(No.21377122)
文摘Alpha radiolysis of nitric acid aqueous solution by a ^(238)Pu source is investigated experimentally and theoretically.The time dependence of the nitrous acid yield on dose rate,nitric acid concentration,and nitrate ion concentration is studied.A novel kinetic model for the α-radiolysis of nitric acid aqueous solution is established,by considering the direct and indirect effects.The simulation results agree well with the experimental data,indicating the validity of our model to treat the reaction paths for generation and consumption of nitrous acid.It is shown that the redox reactions involving Pu cannot be neglected in theα-radiolysis of the solution.The results provide a better understanding of the α-ray radiolysis of aqueous nitric acid.
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.
基金supported by the National Natural Science Foundation of China(31861133018,41830751,42107320)the Hainan University Startup Fund,China(KYQD(ZR)-20098).
文摘The inhibition of nitrification by mixing nitrification inhibitors(NI)with fertilizers is emerging as an effective method to reduce fertilizer-induced nitrous oxide(N_(2)O)emissions.The additive 3,4-dimethylpyrazole phosphate(DMPP)apparently inhibits ammonia oxidizing bacteria(AOB)more than ammonia oxidizing archaea(AOA),which dominate the nitrification in alkaline and acid soil,respectively.However,the efficacy of DMPP in terms of nitrogen sources interacting with soil properties remains unclear.We therefore conducted a microcosm experiment using three typical Chinese agricultural soils with contrasting pH values(fluvo-aquic soil,black soil and red soil),which were fertilized with either digestate or urea in conjunction with a range of DMPP concentrations.In the alkaline fluvo-aquic soil,fertilization with either urea or digestate induced a peak in N_(2)O emission(60μg N kg^(-1)d^(-1))coinciding with the rapid nitrification within 3 d following fertilization.DMPP almost eliminated this peak in N_(2)O emission,reducing it by nearly 90%,despite the fact that the nitrification rate was only reduced by 50%.In the acid black soil,only the digestate induced an N_(2)O emission that increased gradually,reaching its maximum(20μg N kg^(-1)d^(-1))after 5–7 d.The nitrification rate and N_(2)O emission were both marginally reduced by DMPP in the black soil,and the N_(2)O yield(N_(2)O-N per NO2–+NO3–-N produced)was exceptionally high at 3.5%,suggesting that the digestate induced heterotrophic denitrification.In the acid red soil,the N_(2)O emission spiked in the digestate and urea treatments at 50 and 10μg N kg^(-1)d^(-1),respectively,and DMPP reduced the rates substantially by nearly 70%.Compared with 0.5%DMPP,the higher concentrations of DMPP(1.0 to 1.5%)did not exert a significantly(P<0.05)better inhibition effect on the N_(2)O emissions in these soils(either with digestate or urea).This study highlights the importance of matching the nitrogen sources,soil properties and NIs to achieve a high efficiency of N_(2)O emission reduction.
