Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide.A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amou...Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide.A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amounts of extra-framework Al.EPR spectra and UV-vis spectra show that the percentage of iron ions in tetrahedral or octahedral coordination increases while those of clustered Fe species decrease by the addition of extra-framework Al species.Nitrous oxide titration reveals that more active Fe centers are formed,which promote the nitrous oxide consumption.The number of active centers in the catalyst with the introduction of extra-framework Al is about four times that of the catalyst without the addition of extra-framework Al.Due to this,there is an increase in the methane conversion,total selectivity and yield of oxygenates.展开更多
This paper monitors the differences of early rice yield and the emissions of methane and nitrous oxide in the paddy field, based on the different cultivation technologies(high-yield scattered-planting mode, transplan...This paper monitors the differences of early rice yield and the emissions of methane and nitrous oxide in the paddy field, based on the different cultivation technologies(high-yield scattered-planting mode, transplanting mode, farmer-planting mode). Results suggested that the rice yield by high-yield scattered-planting mode and transplanting mode was significantly higher than farmer-planting mode, and the increase reached 16.4% and 17.7%. The difference of high-yield scattered-planting mode and transplanting mode was insignificant. The potential contributions of the methane amount by these three patterns to the global contribution were all above90%. The emission of methane during the growth period by the high-yield scatteredplanting mode was dramatically lower than that by transplanting mode and farmerplanting mode, while the differences between the high-yield transplanting mode and the farmer mode were insignificant. The changes of global temperature increase and the emission of methane were the same. The greenhouse gas intensity of high-yield scattered-planting mode was the lowest, and the farmer-planting mode was the highest. Therefore, the scattered-planting with reasonable fertilizing method is the most essential way to realize high yield of rice and the reducing the greenhouse gas emission as well.展开更多
P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phas...P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.展开更多
Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na...Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na-ion cathodes.Here,we reveal the correlation between cationic ordering transition and OR degradation in ribbon-ordered P3-Na_(0.6)Li_(0.2)Mn_(0.8)O_(2) via in situ structural analysis.Comparing two different voltage windows,the OR capacity can be improved approximately twofold when suppressing the in-plane cationic ordering transition.We find that the intralayer cationic migration is promoted by electrochemical reduction from Mn^(4+)to Jahn–Teller Mn^(3+)and the concomitant NaO_(6) stacking transformation from triangular prisms to octahedra,resulting in the loss of ribbon ordering and electrochemical decay.First-principles calculations reveal that Mn^(4+)/Mn^(3+)charge ordering and alignment of the degenerate eg orbital induce lattice-level collective Jahn–Teller distortion,which favors intralayer Mn-ion migration and thereby accelerates OR degradation.These findings unravel the relationship between in-plane cationic ordering and OR reversibility and highlight the importance of superstructure protection for the rational design of reversible OR-active layered oxide cathodes.展开更多
Developing stable and efficient nonprecious-metal-based oxygen evolution catalysts in the neutral electrolyte is a challenging but essential goal for various electrochemical systems.Particularly,cobalt-based spinels h...Developing stable and efficient nonprecious-metal-based oxygen evolution catalysts in the neutral electrolyte is a challenging but essential goal for various electrochemical systems.Particularly,cobalt-based spinels have drawn a considerable amount of attention but most of them operate in alkali solutions.However,the frequently studied Co-Fe spinel system never exhibits appreciable stability in nonbasic conditions,not to mention attract further investigation on its key structural motif and transition states for activity loss.Herein,we report exceptional stable Co-Fe spinel oxygen evolution catalysts(~30%Fe is optimal)in a neutral electrolyte,owing to its unique metal ion arrangements in the crystal lattice.The introduced iron content enters both the octahedral and tetrahedral sites of the spinel as Fe^(2+)and Fe^(3+)(with Co ions having mixed distribution as well).Combining density functional theory calculations,we find that the introduction of Fe to Co_(3)O_(4)lowers the covalency of metal-oxygen bonds and can help suppress the oxidation of Co^(2+/3+)and 0^(2-).It implies that the Co-Fe spinel will have minor surface reconstruction and less lattice oxygen loss during the oxygen evolution reaction process in comparison with Co_(3)O_(4)and hence show much better stability.These findings suggest that there is still much chance for the spinel structures,especially using reasonable sublattices engineering via multimetal doping to develop advanced oxygen evolution catalysts.展开更多
The undesirable capacity loss after first cycle is universal among layered cathode materials,which results in the capacity and energy decay.The key to resolving this obstacle lies in understanding the effect and origi...The undesirable capacity loss after first cycle is universal among layered cathode materials,which results in the capacity and energy decay.The key to resolving this obstacle lies in understanding the effect and origin of specific active Li sites during discharge process.In this study,focusing on Ah-level pouch cells for reliability,an ultrahigh initial Coulombic efficiency(96.1%)is achieved in an archetypical Li-rich layered oxide material.Combining the structure and electrochemistry analysis,we demonstrate that the achievement of high-capacity reversibility is a kinetic effect,primarily related to the sluggish Li mobility during oxygen reduction.Activating oxygen reduction through small density would induce the oxygen framework contraction,which,according to Pauli repulsion,imposes a great repulsive force to hinder the transport of tetrahedral Li.The tetrahedral Li storage upon deep oxygen reduction is experimentally visualized and,more importantly,contributes to 6%Coulombic efficiency enhancement as well as 10%energy density improvement for pouch cells,which shows great potentials breaking through the capacity and energy limitation imposed by intercalation chemistry.展开更多
A laboratory incubation experiment was conducted to investigate nitrous oxide(N 2O) emission and reduction in a paddy soil(Stagnic Anthrosol) response to the pretreatment of water regime. The paddy soil was maintaine...A laboratory incubation experiment was conducted to investigate nitrous oxide(N 2O) emission and reduction in a paddy soil(Stagnic Anthrosol) response to the pretreatment of water regime. The paddy soil was maintained under either air dried(sample D) or submerged(sample F) conditions for 110 d before the soil was adjusted into soil moisture of 20%, 40%, 60%, 80% and 100% water holding capacity(WHC) respectively, and then incubated with or without 10%(v/v) acetylene for 138 h at 25℃. At lower soil water content (≤60% WHC), N 2O emission from the sample F was 2 29 times higher than that from the sample D( P <0 01). While, N 2O emission from the sample F was only 29 and 14 percent of that from the sample D at the soil moisture of 80% and 100% WHC, respectively( P <0 01). The maximal N 2O emissions observed at soil moisture of 80% WHC were about 24 and 186 times higher than the minima obtained at the soil moisture of 20% WHC for the sample F and D, respectively. But at the soil moisture of 80% and 100% WHC, N 2O emission from the sample F with acetylene(F+ACE) was comparable to that of the sample D with acetylene (D+ACE). The results showed that the F sample produced N 2O ability in denitrification was similar to the sample D, however, the sample F was in the better reduction of N 2O to N 2 than the sample D even after the soil moisture was adjusted into the same level of 80% or 100% WHC. Therefore, the pretreatment of water regime influenced the strength and product composition of denitrification and N 2O emission from the paddy soil.展开更多
Many studies have focused on various agricultural management measures to reduce agricultural nitrous oxide (N2O) emission. However, few studies have investigated soil N2O emissions in intercropping systems in the No...Many studies have focused on various agricultural management measures to reduce agricultural nitrous oxide (N2O) emission. However, few studies have investigated soil N2O emissions in intercropping systems in the North China Plain. Thus, we conducted a ifeld experiment to compare N2O emissions under monoculture and maize-legume intercropping systems. In 2010, ifve treatments, including monocultured maize (M), maize-peanut (MP), maize-alfalfa (MA), maize-soybean (MS), and maize-sweet clover (MSC) intercropping were designed to investigate this issue using the static chamber technique. In 2011, M, MP, and MS remained, and monocultured peanuts (P) and soybean (S) were added to the trial. The results showed that total production of N2O from different treatments ranged from (0.87&#177;0.12) to (1.17&#177;0.11) kg ha-1 in 2010, while those ranged from (3.35&#177;0.30) to (9.10&#177;2.09) kg ha-1 in 2011. MA and MSC had no signiifcant effect on soil N2O production compared to that of M (P&lt;0.05). Cumulative N2O emissions from MP in 2010 were signiifcantly lower than those from M, but the result was the opposite in 2011 (P&lt;0.05). MS signiifcantly reduced soil N2O emissions by 25.55 and 48.84%in 2010 and 2011, respectively (P&lt;0.05). Soil N2O emissions were signiifcantly correlated with soil water content, soil temperature, nitriifcation potential, soil NH4+, and soil NO3-content (R2=0.160-0.764, P&lt;0.01). A stepwise linear regression analysis indicated that soil N2O release was mainly controlled by the interaction between soil moisture and soil NO3-content (R2=0.828, P&lt;0.001). These results indicate that MS had a coincident effect on soil N2O lfux and signiifcantly reduced soil N2O production compared to that of M over two growing seasons.展开更多
Aquatic ecosystems have been identified as a globally significant source of nitrous oxide(N_2O) due to continuous active nitrogen involvement, but the processes and influencing factors that control N_2O production are...Aquatic ecosystems have been identified as a globally significant source of nitrous oxide(N_2O) due to continuous active nitrogen involvement, but the processes and influencing factors that control N_2O production are still poorly understood, especially in reservoirs. For that, monthly N_2O variations were monitored in Dongfeng reservoir(DFR)with a mesotrophic condition. The dissolved N_2O concentration in DFR displayed a distinct spatial–temporal pattern but lower than that in the eutrophic reservoirs. During the whole sampling year, N_2O saturation ranging from 144% to 640%, indicating that reservoir acted as source of atmospheric N_2O. N_2O production is induced by the introduction of nitrogen(NO_3^-, NH_4^+) in mesotrophic reservoirs, and is also affected by oxygen level and water temperature. Nitrification was the predominate process for N_2O production in DFR due to well-oxygenated longitudinal water layers.Mean values of estimated N_2O flux from the air–water interface averaged 0.19 μmol m^(-2)h^(-1) with a range of 0.01–0.61 μmol m^(-2)h^(-1). DFR exhibited less N_2O emission flux than that reported in a nearby eutrophic reservoir, but still acted as a moderate N_2O source compared with other reservoirs and lakes worldwide. Annual emissions from the water–air interface of DFR were estimated to be 0.32×10~5 mol N–N_2O, while N_2O degassing from releasing water behind the dam during power generation was nearly five times greater. Hence, N_2O degassing behind the dam should be taken into account for estimation of N_2O emissions from artificial reservoirs, an omission that historically has probably resulted in underestimates. IPCC methodology should consider more specifically N_2O emission estimation in aquatic ecosystems, especially in reservoirs, the default EF5 model will lead to an overestimation.展开更多
Increased precipitation during the vegetation periods was observed in and further predicted for Inner Mongolia. The changes in the associated soil moisture may affect the biosphere-atmosphere exchange of greenhouse ga...Increased precipitation during the vegetation periods was observed in and further predicted for Inner Mongolia. The changes in the associated soil moisture may affect the biosphere-atmosphere exchange of greenhouse gases. Therefore, we set up an irrigation experiment with one watered (W) and one unwatered plot (UW) at a winter-grazed Leymus chinensis-steppe site in the Xilin River catchment, Inner Mongolia. UW only received the natural precipitation of 2005 (129 mm), whereas W was additionally watered after the precipitation data of 1998 (in total 427 mm). In the 3-hour resolution, we determined nitrous oxide (N20), methane (CH4) and carbon dioxide (CO2) fluxes at both plots between May and September 2005, using a fully automated, chamber-based measuring system. N20 fluxes in the steppe were very low, with mean emissions (±s.e.) of 0.9-4-0.5 and 0.7-4-0.5 μg N m^-2 h^-1 at W and UW, respectively. The steppe soil always served as a CH4 sink, with mean fluxes of -24.1-4-3.9 and -31.1-4- 5.3 μg C m^-2 h^-1 at W and UW. Nighttime mean CO2 emissions were 82.6±8.7 and 26.3±1.7 mg C m^-2 h^-1 at W and UW, respectively, coinciding with an almost doubled aboveground plant biomass at W. Our results indicate that the ecosystem CO2 respiration responded sensitively to increased water input during the vegetation period, whereas the effects on CH4 and N2O fluxes were weak, most likely due to the high evapotranspiration and the lack of substrate for N2O producing processes. Based on our results, we hypothesize that with the gradual increase of summertime precipitation in Inner Mongolia, ecosystem CO2 respiration will be enhanced and CH4 uptake by the steppe soils will be lightly inhibited.展开更多
BACKGROUND Nitrous oxide(N2O)has gained increasing popularity as a recreational drug,causing hallucinations,excitation,and psychological dependence.However,side effects have been reported in recent years.Our case repo...BACKGROUND Nitrous oxide(N2O)has gained increasing popularity as a recreational drug,causing hallucinations,excitation,and psychological dependence.However,side effects have been reported in recent years.Our case report proposes a correlation among N2O,pulmonary embolism(PE),and deep vein thrombosis(DVT)and emphasizes the role of homocysteine(Hcy)in thrombotic events.CASE SUMMARY A 29-year-old man with long-term N2O abuse sought evaluation after acute chest pain.A diagnostic workup revealed PE,DVT,and hyperhomocysteinemia.The patient was successfully treated with thrombolytic and anticoagulant therapy.Moreover,his Hcy level decreased and returned to normal after Hcy-lowering therapy.CONCLUSION Chronic N2O abuse might increase the risk of PE and DVT,although there have been few studies previously.展开更多
Rice-duck (RD) and rice-fish (RF) ecological systems are major complex planting and breeding models of rice paddy fields in southern China. Studying the methane (CH4) and nitrous oxide (N2O) emissions and thei...Rice-duck (RD) and rice-fish (RF) ecological systems are major complex planting and breeding models of rice paddy fields in southern China. Studying the methane (CH4) and nitrous oxide (N2O) emissions and their economic value from these two ecosystems can provide theoretical and practical basis for further development and utilization of these classical agricultural techniques. CH4 and N2O emissions from RD and RF ecological systems were measured in situ by using static chambers technique. Using global warming potentials (GWPs), we assessed the greenhouse effect of CH4 and N2O and their economic value. Results showed that the peaks of CH4 emission fluxes from RD and RF appeared at full tillering stage and at heading stage, and the average emission fluxes were significantly (P〈 0.05) lower than that from CK. N2O fluxes remained low when the field is flooded and high after draining the water. Compared with CK, the total amount of N2O emissions was significantly (P〈0.05) higher and slightly lower than those from RD and RF, respectively. In 2006 and 2007, the total greenhouse effect of CH4 and N20 from RD and RF were 4 728.3 and 4 611 kg CO2 ha^-1, 4 545 and 4 754.3 kg CO2 ha^-1, respectively. The costs of greenhouse effect were 970.89 and 946.81 RMB yuan ha^-1, and 933.25 and 976.23 RMB yuan ha^-1, respectively, which were significant lower than those from CK (5 997.6 and 5 391.5 RMB yuan ha^-1). Except for the environment cost of CH4 and N2O, the economic benefits from RD and RF were 2 210.64 and 4 881.92 RMB yuan ha^-1; 3 798.37 and 5 310.64 RMB yuan ha^-1, respectively, higher than those from CK. Therefore, RD and RF complex ecological planting and breeding models can effectively decrease and control CH4 and N2O emissions, and they are two of the effective strategies to reduce greenhouse gases from rice paddy fields and contribute in alleviating global warming. Thus, their adoption is important to the environment together with their economy benefits.展开更多
Paddy field is a primary agricultural landscape in the south of China and is often regarded as one of main sources emitting nitrous oxide to atmosphere. The nitrous oxide emissions under a variety of paddy field pract...Paddy field is a primary agricultural landscape in the south of China and is often regarded as one of main sources emitting nitrous oxide to atmosphere. The nitrous oxide emissions under a variety of paddy field practices, such as fertilization, flooding/draining management were investigated to study on agricultural activities on paddy field affect the dynamic process of the emission. Under no addition of fertilizers the average emission flux of nitrous oxide was 8 55 μg/(m 2·h) during the rice( Oryza Sativa L.) growth season. The results indicated that most of nitrous oxide emissions occurred during the crack forming and expansion period when paddy field was being drained. The diurnal emissions peak of nitrous oxide appeared at 20∶30 at night in cracked rice fields. The statistical analysis suggested that the correlation of nitrous oxide emissions flux( Y ) with soil water content( X 1), soil temperature( X 2), and E h( X 3), could be described in a regression equation: Y =-1498 95+2895 48 X 1+50 63 X 2-96 99 X 1· X 2+0 006 X 2· X 3 There were the different power equations to simulate the correlations between the everyday dynamic N 2O emissions and the mean surface area of cracks, mean volume and depth of cracks respectively during paddy soil drying by soil columns incubation experiments. Taken all together, the current study presented a dynamic analysis of nitrous oxide emission of paddy field under various conditions, therefore provided a basis for the management to balance between environmental effect and paddy field activities.展开更多
The concentrations of nitrous oxide varies between 57 and 329 nmol/dm3, saturation is 674%~4 134% in the Zhujiang River Estuary. This suggests that the area is an emissive source of nitrous oxide. The acetylene inhib...The concentrations of nitrous oxide varies between 57 and 329 nmol/dm3, saturation is 674%~4 134% in the Zhujiang River Estuary. This suggests that the area is an emissive source of nitrous oxide. The acetylene inhibition technique is employed to evaluate the rates of nitrification, denitrification and nitrate reduction by bacterial activities in the sediments at three sites. The average of nitrification, denitrification and nitrate reduction rates ranges from 0.32 to 2.43, 0.03 to 0.84 and 4.17 to 13.06 mmol/(m2·h), respectively. The ver- tical profiles of the sediments show that the nitrification and denitrification processes mainly take place in the depth from 0 to 4 cm and depend on regional conditions. The rates of nitrification, denitrification and nitrate reduction are dominated by Eh, nitrate and ammoni- um concentrations in sediments and DO in overlay water. There is a coupling between nitrification and denitrification.展开更多
The reuse of treated wastewater in agricultural systems could partially help alleviate water resource shortages in developing countries. Treated wastewater differs from fresh water in that it has higher concentrations...The reuse of treated wastewater in agricultural systems could partially help alleviate water resource shortages in developing countries. Treated wastewater differs from fresh water in that it has higher concentrations of salts, Escherichia coli and presence of dissolved organic matter, and inorganic N after secondary treatment, among others. Its application could thus cause environmental consequences such as soil salinization, ammonia volatilization, and greenhouse gas emissions. In an incubation experiment, we evaluated the characteristics and effects of water-filled pore space (WFPS) and N input on the emissions of nitrous oxide (N2O) and carbon dioxide (CO2) from silt loam soil receiving treated wastewater. Irrigation with treated wastewater (vs. distilled water) significantly increased cumulative N2O emission in soil (117.97 μg N kg-1). Cumulative N2O emissions showed an exponentially increase with the increasing WFPS in unamended soil, but the maximum occurred in the added urea soil incubated at 60% WFPS. N2O emissions caused by irrigation with treated wastewater combined with urea-N fertilization did not simply add linearly, but significant interaction (P〈0.05) caused lower emissions than the production of N2O from the cumulative effects of treated wastewater and fertilizer N. Moreover, a significant impact on cumulative CO2 emission was measured in soil irrigated with treated wastewater. When treated wastewater was applied, there was significant interaction between WFPS and N input on N2O emission. Hence, our results indicated that irrigation with treated wastewater should cause great concern for increasing global warming potential due to enhanced emission of N2O and CO2.展开更多
The absorption spectrum of the C1Ⅱ state of N2O molecule in the wavelength range of 142.5-147.5 nm has been measured under the jet-cooled condition, and the clear spectral features are displayed. A vibrational progre...The absorption spectrum of the C1Ⅱ state of N2O molecule in the wavelength range of 142.5-147.5 nm has been measured under the jet-cooled condition, and the clear spectral features are displayed. A vibrational progression is observed with a frequency interval of about 500 cm-1. With the aid of potential energy surfaces (PES) of the low-lying electronic states of N2O, the vibrational progression is assigned as the bending mode of the repulsive C1Ⅱ state. From the Fourier transformation analysis, the recurrence period of the periodic orbit near the transition state region is derived to be 65 fs. Through the least-square Lorentzian fitting, the lifetimes of the resonance levels are estimated from their profile widths to be about 20 fs, which is shorter than the recurrence period. Therefore, a new explanation is suggested for the observed diffuse spectral structure, based on the behavior of dissociating N20 on PES of the C1Ⅱ state in the present excitation energy range.展开更多
The results of a system analysis of the efficiency of nitrous oxide(N_2O) as a propellant component for small space vehicles(SSV) were presented. A criterion for mass efficiency of the SSV propulsion system(PS) is det...The results of a system analysis of the efficiency of nitrous oxide(N_2O) as a propellant component for small space vehicles(SSV) were presented. A criterion for mass efficiency of the SSV propulsion system(PS) is determined. The current global state-of-the-art of SSV PSs is shown. The application field of nitrous oxide in SSV PSs is calculated and mass efficiency of N_2O application is quantitatively determined. An overview of physical and chemical as well as operational properties of nitrous oxide as a promising, non-toxic component of rocket propellant is provided. Main physical and chemical constants of gaseous and liquid nitrous oxide; chemical properties of N_2O, thermal stability of N_2O, catalytic decomposition of N_2O, a mechanism of decomposition of N_2O, catalysts for decomposition of N_2O, ballast additives to N_2O, application of nitrous oxide, nitrous oxide as a rocket propellant, production of nitrous oxide, toxicity of nitrous oxide, fire hazard of N_2O, requirements to equipment when handling N_2O; storage and transportation of N_2O are considered. It is demonstrated that nitrous oxide is a chemical compound meeting the requirements to rocket propellants, including those related to the environmental friendliness of propellants. With 75 references.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
Direct nitrous oxide(N2O) emissions(DNEs) from croplands are required in national inventories of greenhouse gases. The Intergovernmental Panel on Climate Change(IPCC) guidelines provide an approach using direct emissi...Direct nitrous oxide(N2O) emissions(DNEs) from croplands are required in national inventories of greenhouse gases. The Intergovernmental Panel on Climate Change(IPCC) guidelines provide an approach using direct emission factors(EFds) to estimate DNEs, which are constants for large regions. The goal of this paper is to establish empirical models to account for the temporal and spatial variations of EFds, which, apart from the nitrogen addition rate, also vary with a range of environmental factors, so as to enhance the accuracy of regional/national DNE estimates. Therefore, the seasonal/annual DNEs(n = 71) from upland croplands, which are the differences in N2 O emissions between fields with and without fertilizer-nitrogen addition, were used to statistically relate DNEs to regulating factors including the fertilizer-nitrogen addition rate(FN), and environmental(climate and soil) factors. The multivariate stepwise linear regression results showed positive combined effects of FN and clay fraction on DNEs(R2 = 0.61, p < 0.001). Furthermore, the nonlinear regression of FN, precipitation, and clay fraction was also adopted for prediction(R2 = 0.50, p < 0.001). Validation with an independent dataset(n = 31) suggested that both models were better predictors of DNEs than the IPCC model, which only depends on FN. These empirical models may provide simple but reliable approaches for compiling regional/national, and even global inventories of DNEs from croplands. However, both models were restricted to a limited sample size. Understandably, more field observations are still required to further validate the global applicability of these simple approaches.展开更多
The rate of nitrous oxide emission from a laboratory sequence batch reactor (SBR) wastewater treatment system using synthetic wastewater was measured under controlled conditions. The SBR was operated in the mode of ...The rate of nitrous oxide emission from a laboratory sequence batch reactor (SBR) wastewater treatment system using synthetic wastewater was measured under controlled conditions. The SBR was operated in the mode of 4 h for aeration, 3.5 h for stirring without aeration, 0.5 h for settling and drainage, and 4 h of idle. The sludge was acclimated by running the system to achieve a stable running state as chemical oxygen demand, NO2^-, NO3^-, NH4^+, pH, and N2O. indicated by rhythmic changes of total N, dissolved oxygen, Under the present experimental conditions measured nitrous oxide emitted from the off-gas in the aerobic and anaerobic phases, respectively, accounted for 8.6%-16.1% and 0-0.05% of N removed, indicating that the aerobic phase was the main source of N2O emission from the system. N2O dissolved in discharged water was considerable in term of concentration. Thus, measures to be developed for the purpose of reducing N2O emission from the system should be effective in the aeration phase.展开更多
基金This research was supported by the Zhejiang Provincial Natural Science Foundation of China(LR18B060001)Basic Research Project of Sinopec Group(415025)the Fundamental Research Funds for the Central Universities.
文摘Iron-containing zeolites play an important role in the selective oxidation of methane to oxygenates by nitrous oxide.A solid-state ion exchange method is adopted to prepare Fe-MOR zeolite catalysts with different amounts of extra-framework Al.EPR spectra and UV-vis spectra show that the percentage of iron ions in tetrahedral or octahedral coordination increases while those of clustered Fe species decrease by the addition of extra-framework Al species.Nitrous oxide titration reveals that more active Fe centers are formed,which promote the nitrous oxide consumption.The number of active centers in the catalyst with the introduction of extra-framework Al is about four times that of the catalyst without the addition of extra-framework Al.Due to this,there is an increase in the methane conversion,total selectivity and yield of oxygenates.
基金Supported by National"Twelfth Five-Year Plan"of Scientific and Technological Support Plan(No.2011BAD16B04)~~
文摘This paper monitors the differences of early rice yield and the emissions of methane and nitrous oxide in the paddy field, based on the different cultivation technologies(high-yield scattered-planting mode, transplanting mode, farmer-planting mode). Results suggested that the rice yield by high-yield scattered-planting mode and transplanting mode was significantly higher than farmer-planting mode, and the increase reached 16.4% and 17.7%. The difference of high-yield scattered-planting mode and transplanting mode was insignificant. The potential contributions of the methane amount by these three patterns to the global contribution were all above90%. The emission of methane during the growth period by the high-yield scatteredplanting mode was dramatically lower than that by transplanting mode and farmerplanting mode, while the differences between the high-yield transplanting mode and the farmer mode were insignificant. The changes of global temperature increase and the emission of methane were the same. The greenhouse gas intensity of high-yield scattered-planting mode was the lowest, and the farmer-planting mode was the highest. Therefore, the scattered-planting with reasonable fertilizing method is the most essential way to realize high yield of rice and the reducing the greenhouse gas emission as well.
基金supported by the National Natural Science Foundation of China (22169002)the Chongzuo Key Research and Development Program of China (20220603)the Counterpart Aid Project for Discipline Construction from Guangxi University(2023M02)
文摘P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.
基金funding supports from the National Key R&D Program of China(Grant Nos.2022YFB2404400 and 2019YFA0308500)Beijing Natural Science Foundation(Z190010)National Natural Science Foundation of China(Grant Nos.51991344,52025025,52072400,and 52002394)。
文摘Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na-ion cathodes.Here,we reveal the correlation between cationic ordering transition and OR degradation in ribbon-ordered P3-Na_(0.6)Li_(0.2)Mn_(0.8)O_(2) via in situ structural analysis.Comparing two different voltage windows,the OR capacity can be improved approximately twofold when suppressing the in-plane cationic ordering transition.We find that the intralayer cationic migration is promoted by electrochemical reduction from Mn^(4+)to Jahn–Teller Mn^(3+)and the concomitant NaO_(6) stacking transformation from triangular prisms to octahedra,resulting in the loss of ribbon ordering and electrochemical decay.First-principles calculations reveal that Mn^(4+)/Mn^(3+)charge ordering and alignment of the degenerate eg orbital induce lattice-level collective Jahn–Teller distortion,which favors intralayer Mn-ion migration and thereby accelerates OR degradation.These findings unravel the relationship between in-plane cationic ordering and OR reversibility and highlight the importance of superstructure protection for the rational design of reversible OR-active layered oxide cathodes.
基金the financial support by the National Natural Science Foundation of China(NSFC,grant nos.21905288 and 51904288)Zhejiang Provincial Natural Science Foundation(LZ21B030001)+3 种基金K.C.Wong Education Foundation(GJTD-2019-13)Ningbo major special projects of the Plan“Science and Technology Innovation 2025”(grant nos.2018B10056 and 2019B10046)Ningbo 3315 ProgramYongjiang Talent Introduction Program(no.2021A-115-G)
文摘Developing stable and efficient nonprecious-metal-based oxygen evolution catalysts in the neutral electrolyte is a challenging but essential goal for various electrochemical systems.Particularly,cobalt-based spinels have drawn a considerable amount of attention but most of them operate in alkali solutions.However,the frequently studied Co-Fe spinel system never exhibits appreciable stability in nonbasic conditions,not to mention attract further investigation on its key structural motif and transition states for activity loss.Herein,we report exceptional stable Co-Fe spinel oxygen evolution catalysts(~30%Fe is optimal)in a neutral electrolyte,owing to its unique metal ion arrangements in the crystal lattice.The introduced iron content enters both the octahedral and tetrahedral sites of the spinel as Fe^(2+)and Fe^(3+)(with Co ions having mixed distribution as well).Combining density functional theory calculations,we find that the introduction of Fe to Co_(3)O_(4)lowers the covalency of metal-oxygen bonds and can help suppress the oxidation of Co^(2+/3+)and 0^(2-).It implies that the Co-Fe spinel will have minor surface reconstruction and less lattice oxygen loss during the oxygen evolution reaction process in comparison with Co_(3)O_(4)and hence show much better stability.These findings suggest that there is still much chance for the spinel structures,especially using reasonable sublattices engineering via multimetal doping to develop advanced oxygen evolution catalysts.
基金financially supported by the National Natural Science Foundation of China(Grant No.52272253)“Lingyan”Research and Development Plan of Zhejiang Province(Grant No.2022C01071)+2 种基金Low Cost Cathode Material(Grant No.TC220H06P)the Natural Science Foundation of Ningbo(Grant No.202003N4030)the Youth Innovation Promotion Association of Chinese Academy of Sciences(Grant No.2022299)
文摘The undesirable capacity loss after first cycle is universal among layered cathode materials,which results in the capacity and energy decay.The key to resolving this obstacle lies in understanding the effect and origin of specific active Li sites during discharge process.In this study,focusing on Ah-level pouch cells for reliability,an ultrahigh initial Coulombic efficiency(96.1%)is achieved in an archetypical Li-rich layered oxide material.Combining the structure and electrochemistry analysis,we demonstrate that the achievement of high-capacity reversibility is a kinetic effect,primarily related to the sluggish Li mobility during oxygen reduction.Activating oxygen reduction through small density would induce the oxygen framework contraction,which,according to Pauli repulsion,imposes a great repulsive force to hinder the transport of tetrahedral Li.The tetrahedral Li storage upon deep oxygen reduction is experimentally visualized and,more importantly,contributes to 6%Coulombic efficiency enhancement as well as 10%energy density improvement for pouch cells,which shows great potentials breaking through the capacity and energy limitation imposed by intercalation chemistry.
文摘A laboratory incubation experiment was conducted to investigate nitrous oxide(N 2O) emission and reduction in a paddy soil(Stagnic Anthrosol) response to the pretreatment of water regime. The paddy soil was maintained under either air dried(sample D) or submerged(sample F) conditions for 110 d before the soil was adjusted into soil moisture of 20%, 40%, 60%, 80% and 100% water holding capacity(WHC) respectively, and then incubated with or without 10%(v/v) acetylene for 138 h at 25℃. At lower soil water content (≤60% WHC), N 2O emission from the sample F was 2 29 times higher than that from the sample D( P <0 01). While, N 2O emission from the sample F was only 29 and 14 percent of that from the sample D at the soil moisture of 80% and 100% WHC, respectively( P <0 01). The maximal N 2O emissions observed at soil moisture of 80% WHC were about 24 and 186 times higher than the minima obtained at the soil moisture of 20% WHC for the sample F and D, respectively. But at the soil moisture of 80% and 100% WHC, N 2O emission from the sample F with acetylene(F+ACE) was comparable to that of the sample D with acetylene (D+ACE). The results showed that the F sample produced N 2O ability in denitrification was similar to the sample D, however, the sample F was in the better reduction of N 2O to N 2 than the sample D even after the soil moisture was adjusted into the same level of 80% or 100% WHC. Therefore, the pretreatment of water regime influenced the strength and product composition of denitrification and N 2O emission from the paddy soil.
基金supported by the National Key Technologies R&D Program of China (2011BAD16B15 and 2012BAD14B03)
文摘Many studies have focused on various agricultural management measures to reduce agricultural nitrous oxide (N2O) emission. However, few studies have investigated soil N2O emissions in intercropping systems in the North China Plain. Thus, we conducted a ifeld experiment to compare N2O emissions under monoculture and maize-legume intercropping systems. In 2010, ifve treatments, including monocultured maize (M), maize-peanut (MP), maize-alfalfa (MA), maize-soybean (MS), and maize-sweet clover (MSC) intercropping were designed to investigate this issue using the static chamber technique. In 2011, M, MP, and MS remained, and monocultured peanuts (P) and soybean (S) were added to the trial. The results showed that total production of N2O from different treatments ranged from (0.87&#177;0.12) to (1.17&#177;0.11) kg ha-1 in 2010, while those ranged from (3.35&#177;0.30) to (9.10&#177;2.09) kg ha-1 in 2011. MA and MSC had no signiifcant effect on soil N2O production compared to that of M (P&lt;0.05). Cumulative N2O emissions from MP in 2010 were signiifcantly lower than those from M, but the result was the opposite in 2011 (P&lt;0.05). MS signiifcantly reduced soil N2O emissions by 25.55 and 48.84%in 2010 and 2011, respectively (P&lt;0.05). Soil N2O emissions were signiifcantly correlated with soil water content, soil temperature, nitriifcation potential, soil NH4+, and soil NO3-content (R2=0.160-0.764, P&lt;0.01). A stepwise linear regression analysis indicated that soil N2O release was mainly controlled by the interaction between soil moisture and soil NO3-content (R2=0.828, P&lt;0.001). These results indicate that MS had a coincident effect on soil N2O lfux and signiifcantly reduced soil N2O production compared to that of M over two growing seasons.
基金financially supported by the National Key Research and Development Program of China through grant 2016YFA0601000the National Major Scientific Research Program Grant No.2013CB956401+1 种基金the National Natural Science Foundation of China through Grants Nos.41325010,41403082,and 41302285the Tianjin Research Program of Application Foundation and Advanced Technology Grant No.14JCQNJC08800
文摘Aquatic ecosystems have been identified as a globally significant source of nitrous oxide(N_2O) due to continuous active nitrogen involvement, but the processes and influencing factors that control N_2O production are still poorly understood, especially in reservoirs. For that, monthly N_2O variations were monitored in Dongfeng reservoir(DFR)with a mesotrophic condition. The dissolved N_2O concentration in DFR displayed a distinct spatial–temporal pattern but lower than that in the eutrophic reservoirs. During the whole sampling year, N_2O saturation ranging from 144% to 640%, indicating that reservoir acted as source of atmospheric N_2O. N_2O production is induced by the introduction of nitrogen(NO_3^-, NH_4^+) in mesotrophic reservoirs, and is also affected by oxygen level and water temperature. Nitrification was the predominate process for N_2O production in DFR due to well-oxygenated longitudinal water layers.Mean values of estimated N_2O flux from the air–water interface averaged 0.19 μmol m^(-2)h^(-1) with a range of 0.01–0.61 μmol m^(-2)h^(-1). DFR exhibited less N_2O emission flux than that reported in a nearby eutrophic reservoir, but still acted as a moderate N_2O source compared with other reservoirs and lakes worldwide. Annual emissions from the water–air interface of DFR were estimated to be 0.32×10~5 mol N–N_2O, while N_2O degassing from releasing water behind the dam during power generation was nearly five times greater. Hence, N_2O degassing behind the dam should be taken into account for estimation of N_2O emissions from artificial reservoirs, an omission that historically has probably resulted in underestimates. IPCC methodology should consider more specifically N_2O emission estimation in aquatic ecosystems, especially in reservoirs, the default EF5 model will lead to an overestimation.
基金the German Research Foundation (DFG, Research UnitNo. 536, "Matter fluxes in grasslands of Inner Mongo-lia as influenced by stocking rate", MAGIM) (BU 1173/6-2)the National Natural Science Foundation of China(NSFC) (Grant Nos. 40425010, 40331014)
文摘Increased precipitation during the vegetation periods was observed in and further predicted for Inner Mongolia. The changes in the associated soil moisture may affect the biosphere-atmosphere exchange of greenhouse gases. Therefore, we set up an irrigation experiment with one watered (W) and one unwatered plot (UW) at a winter-grazed Leymus chinensis-steppe site in the Xilin River catchment, Inner Mongolia. UW only received the natural precipitation of 2005 (129 mm), whereas W was additionally watered after the precipitation data of 1998 (in total 427 mm). In the 3-hour resolution, we determined nitrous oxide (N20), methane (CH4) and carbon dioxide (CO2) fluxes at both plots between May and September 2005, using a fully automated, chamber-based measuring system. N20 fluxes in the steppe were very low, with mean emissions (±s.e.) of 0.9-4-0.5 and 0.7-4-0.5 μg N m^-2 h^-1 at W and UW, respectively. The steppe soil always served as a CH4 sink, with mean fluxes of -24.1-4-3.9 and -31.1-4- 5.3 μg C m^-2 h^-1 at W and UW. Nighttime mean CO2 emissions were 82.6±8.7 and 26.3±1.7 mg C m^-2 h^-1 at W and UW, respectively, coinciding with an almost doubled aboveground plant biomass at W. Our results indicate that the ecosystem CO2 respiration responded sensitively to increased water input during the vegetation period, whereas the effects on CH4 and N2O fluxes were weak, most likely due to the high evapotranspiration and the lack of substrate for N2O producing processes. Based on our results, we hypothesize that with the gradual increase of summertime precipitation in Inner Mongolia, ecosystem CO2 respiration will be enhanced and CH4 uptake by the steppe soils will be lightly inhibited.
文摘BACKGROUND Nitrous oxide(N2O)has gained increasing popularity as a recreational drug,causing hallucinations,excitation,and psychological dependence.However,side effects have been reported in recent years.Our case report proposes a correlation among N2O,pulmonary embolism(PE),and deep vein thrombosis(DVT)and emphasizes the role of homocysteine(Hcy)in thrombotic events.CASE SUMMARY A 29-year-old man with long-term N2O abuse sought evaluation after acute chest pain.A diagnostic workup revealed PE,DVT,and hyperhomocysteinemia.The patient was successfully treated with thrombolytic and anticoagulant therapy.Moreover,his Hcy level decreased and returned to normal after Hcy-lowering therapy.CONCLUSION Chronic N2O abuse might increase the risk of PE and DVT,although there have been few studies previously.
基金supported by Important National Science&Technoligy Specific Projects, China (2004BA520A02)
文摘Rice-duck (RD) and rice-fish (RF) ecological systems are major complex planting and breeding models of rice paddy fields in southern China. Studying the methane (CH4) and nitrous oxide (N2O) emissions and their economic value from these two ecosystems can provide theoretical and practical basis for further development and utilization of these classical agricultural techniques. CH4 and N2O emissions from RD and RF ecological systems were measured in situ by using static chambers technique. Using global warming potentials (GWPs), we assessed the greenhouse effect of CH4 and N2O and their economic value. Results showed that the peaks of CH4 emission fluxes from RD and RF appeared at full tillering stage and at heading stage, and the average emission fluxes were significantly (P〈 0.05) lower than that from CK. N2O fluxes remained low when the field is flooded and high after draining the water. Compared with CK, the total amount of N2O emissions was significantly (P〈0.05) higher and slightly lower than those from RD and RF, respectively. In 2006 and 2007, the total greenhouse effect of CH4 and N20 from RD and RF were 4 728.3 and 4 611 kg CO2 ha^-1, 4 545 and 4 754.3 kg CO2 ha^-1, respectively. The costs of greenhouse effect were 970.89 and 946.81 RMB yuan ha^-1, and 933.25 and 976.23 RMB yuan ha^-1, respectively, which were significant lower than those from CK (5 997.6 and 5 391.5 RMB yuan ha^-1). Except for the environment cost of CH4 and N2O, the economic benefits from RD and RF were 2 210.64 and 4 881.92 RMB yuan ha^-1; 3 798.37 and 5 310.64 RMB yuan ha^-1, respectively, higher than those from CK. Therefore, RD and RF complex ecological planting and breeding models can effectively decrease and control CH4 and N2O emissions, and they are two of the effective strategies to reduce greenhouse gases from rice paddy fields and contribute in alleviating global warming. Thus, their adoption is important to the environment together with their economy benefits.
文摘Paddy field is a primary agricultural landscape in the south of China and is often regarded as one of main sources emitting nitrous oxide to atmosphere. The nitrous oxide emissions under a variety of paddy field practices, such as fertilization, flooding/draining management were investigated to study on agricultural activities on paddy field affect the dynamic process of the emission. Under no addition of fertilizers the average emission flux of nitrous oxide was 8 55 μg/(m 2·h) during the rice( Oryza Sativa L.) growth season. The results indicated that most of nitrous oxide emissions occurred during the crack forming and expansion period when paddy field was being drained. The diurnal emissions peak of nitrous oxide appeared at 20∶30 at night in cracked rice fields. The statistical analysis suggested that the correlation of nitrous oxide emissions flux( Y ) with soil water content( X 1), soil temperature( X 2), and E h( X 3), could be described in a regression equation: Y =-1498 95+2895 48 X 1+50 63 X 2-96 99 X 1· X 2+0 006 X 2· X 3 There were the different power equations to simulate the correlations between the everyday dynamic N 2O emissions and the mean surface area of cracks, mean volume and depth of cracks respectively during paddy soil drying by soil columns incubation experiments. Taken all together, the current study presented a dynamic analysis of nitrous oxide emission of paddy field under various conditions, therefore provided a basis for the management to balance between environmental effect and paddy field activities.
基金supported by the Knowledge Innovation Engineering of Chinese Academy of Sciences under contract No.KZCX3-SW-214,KSCX2-SW-132the Natural Science Foundation of Guangdong Province under contract No.032622.
文摘The concentrations of nitrous oxide varies between 57 and 329 nmol/dm3, saturation is 674%~4 134% in the Zhujiang River Estuary. This suggests that the area is an emissive source of nitrous oxide. The acetylene inhibition technique is employed to evaluate the rates of nitrification, denitrification and nitrate reduction by bacterial activities in the sediments at three sites. The average of nitrification, denitrification and nitrate reduction rates ranges from 0.32 to 2.43, 0.03 to 0.84 and 4.17 to 13.06 mmol/(m2·h), respectively. The ver- tical profiles of the sediments show that the nitrification and denitrification processes mainly take place in the depth from 0 to 4 cm and depend on regional conditions. The rates of nitrification, denitrification and nitrate reduction are dominated by Eh, nitrate and ammoni- um concentrations in sediments and DO in overlay water. There is a coupling between nitrification and denitrification.
基金funded by the National Natural Science Foundation of China (50979107)
文摘The reuse of treated wastewater in agricultural systems could partially help alleviate water resource shortages in developing countries. Treated wastewater differs from fresh water in that it has higher concentrations of salts, Escherichia coli and presence of dissolved organic matter, and inorganic N after secondary treatment, among others. Its application could thus cause environmental consequences such as soil salinization, ammonia volatilization, and greenhouse gas emissions. In an incubation experiment, we evaluated the characteristics and effects of water-filled pore space (WFPS) and N input on the emissions of nitrous oxide (N2O) and carbon dioxide (CO2) from silt loam soil receiving treated wastewater. Irrigation with treated wastewater (vs. distilled water) significantly increased cumulative N2O emission in soil (117.97 μg N kg-1). Cumulative N2O emissions showed an exponentially increase with the increasing WFPS in unamended soil, but the maximum occurred in the added urea soil incubated at 60% WFPS. N2O emissions caused by irrigation with treated wastewater combined with urea-N fertilization did not simply add linearly, but significant interaction (P〈0.05) caused lower emissions than the production of N2O from the cumulative effects of treated wastewater and fertilizer N. Moreover, a significant impact on cumulative CO2 emission was measured in soil irrigated with treated wastewater. When treated wastewater was applied, there was significant interaction between WFPS and N input on N2O emission. Hence, our results indicated that irrigation with treated wastewater should cause great concern for increasing global warming potential due to enhanced emission of N2O and CO2.
基金This work was supported by the National Natural Science Foundation of China (No.10979042 and No.21073173), the National Key Basic Research Special Foundation of China (No.2007CB815204), and the Fundamental Research Funds for the Central Universities. Authors also would like to thank Prof. J. B. Nee to provide his experimental data for our reference.
文摘The absorption spectrum of the C1Ⅱ state of N2O molecule in the wavelength range of 142.5-147.5 nm has been measured under the jet-cooled condition, and the clear spectral features are displayed. A vibrational progression is observed with a frequency interval of about 500 cm-1. With the aid of potential energy surfaces (PES) of the low-lying electronic states of N2O, the vibrational progression is assigned as the bending mode of the repulsive C1Ⅱ state. From the Fourier transformation analysis, the recurrence period of the periodic orbit near the transition state region is derived to be 65 fs. Through the least-square Lorentzian fitting, the lifetimes of the resonance levels are estimated from their profile widths to be about 20 fs, which is shorter than the recurrence period. Therefore, a new explanation is suggested for the observed diffuse spectral structure, based on the behavior of dissociating N20 on PES of the C1Ⅱ state in the present excitation energy range.
文摘The results of a system analysis of the efficiency of nitrous oxide(N_2O) as a propellant component for small space vehicles(SSV) were presented. A criterion for mass efficiency of the SSV propulsion system(PS) is determined. The current global state-of-the-art of SSV PSs is shown. The application field of nitrous oxide in SSV PSs is calculated and mass efficiency of N_2O application is quantitatively determined. An overview of physical and chemical as well as operational properties of nitrous oxide as a promising, non-toxic component of rocket propellant is provided. Main physical and chemical constants of gaseous and liquid nitrous oxide; chemical properties of N_2O, thermal stability of N_2O, catalytic decomposition of N_2O, a mechanism of decomposition of N_2O, catalysts for decomposition of N_2O, ballast additives to N_2O, application of nitrous oxide, nitrous oxide as a rocket propellant, production of nitrous oxide, toxicity of nitrous oxide, fire hazard of N_2O, requirements to equipment when handling N_2O; storage and transportation of N_2O are considered. It is demonstrated that nitrous oxide is a chemical compound meeting the requirements to rocket propellants, including those related to the environmental friendliness of propellants. With 75 references.
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 the Ministry of Science and Technology(Grant No. 2012CB417106)the National Natural Science Foundation of China(Grant No. 41321064)
文摘Direct nitrous oxide(N2O) emissions(DNEs) from croplands are required in national inventories of greenhouse gases. The Intergovernmental Panel on Climate Change(IPCC) guidelines provide an approach using direct emission factors(EFds) to estimate DNEs, which are constants for large regions. The goal of this paper is to establish empirical models to account for the temporal and spatial variations of EFds, which, apart from the nitrogen addition rate, also vary with a range of environmental factors, so as to enhance the accuracy of regional/national DNE estimates. Therefore, the seasonal/annual DNEs(n = 71) from upland croplands, which are the differences in N2 O emissions between fields with and without fertilizer-nitrogen addition, were used to statistically relate DNEs to regulating factors including the fertilizer-nitrogen addition rate(FN), and environmental(climate and soil) factors. The multivariate stepwise linear regression results showed positive combined effects of FN and clay fraction on DNEs(R2 = 0.61, p < 0.001). Furthermore, the nonlinear regression of FN, precipitation, and clay fraction was also adopted for prediction(R2 = 0.50, p < 0.001). Validation with an independent dataset(n = 31) suggested that both models were better predictors of DNEs than the IPCC model, which only depends on FN. These empirical models may provide simple but reliable approaches for compiling regional/national, and even global inventories of DNEs from croplands. However, both models were restricted to a limited sample size. Understandably, more field observations are still required to further validate the global applicability of these simple approaches.
基金Project supported by the National Natural Science Foundation of China (Nos. 40471072 and 30470060) and the Knowledge Innovation Program of Chinese Academy of Sciences (No. KZCX2-413-3-1).
文摘The rate of nitrous oxide emission from a laboratory sequence batch reactor (SBR) wastewater treatment system using synthetic wastewater was measured under controlled conditions. The SBR was operated in the mode of 4 h for aeration, 3.5 h for stirring without aeration, 0.5 h for settling and drainage, and 4 h of idle. The sludge was acclimated by running the system to achieve a stable running state as chemical oxygen demand, NO2^-, NO3^-, NH4^+, pH, and N2O. indicated by rhythmic changes of total N, dissolved oxygen, Under the present experimental conditions measured nitrous oxide emitted from the off-gas in the aerobic and anaerobic phases, respectively, accounted for 8.6%-16.1% and 0-0.05% of N removed, indicating that the aerobic phase was the main source of N2O emission from the system. N2O dissolved in discharged water was considerable in term of concentration. Thus, measures to be developed for the purpose of reducing N2O emission from the system should be effective in the aeration phase.