Nitrogen oxides(NO_(x))are crucial in tropospheric photochemical ozone(O_(3))production and oxidation capacity.Currently,the widely used NO_(x)measurement technique is chemiluminescence(CL)(CL-NO_(x)),which tends to o...Nitrogen oxides(NO_(x))are crucial in tropospheric photochemical ozone(O_(3))production and oxidation capacity.Currently,the widely used NO_(x)measurement technique is chemiluminescence(CL)(CL-NO_(x)),which tends to overestimate NO_(2)due to atmospheric oxidation products of NO_(x)(i.e.,NO_(z)).We developed and characterized a NO_(x)measurement system using the cavity attenuated phase shift(CAPS)technique(CAPS-NO_(x)),which is free from interferences with nitrogen-containing species.The NO_(x)measured by the CAPS-NO_(x)and CL-NO_(x)analyzers were compared.Results show that both analyzers showed consistent measurement results for NO,but the NO_(2)measured by the CAPS-NO_(x)analyzer(NO_(2)_CAPS)was mostly lower than that measured by the CL-NO_(x)analyzer(NO_(2)_CL),which led to the deviations in O_(3)formation sensitivity regime and O_(x)(=O_(3)+NO_(2))sources(i.e.,regional background and photochemically produced O_(x))determined by the ozone production efficiencies(OPE)calculated from NO_(2)_CL and NO_(2)_CAPS.Overall,OPE_CL exceeded OPE_CAPS by 18.9%,which shifted 3 out of 13 observation days from the VOCs-limited to the transition regime when judging using OPE_CL,as compared to calculations using OPE_CAPS.During the observation period,days dominated by regional background O_(x)accounted for 46%and 62%when determined using NO_(2)_CL and NO_(2)_CAPS,respectively.These findings suggest that the use of the CL-NO_(x)analyzer tends to underestimate both the VOCs-limited regime and the regional background O_(x)dominated days.The newly built CAPS-NO_(x)analyzer here can promote the accurate measurement of NO_(2),which is meaningful for diagnosing O_(3)formation regimes and O_(x)sources.展开更多
The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocata...The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocatalysts.However,the low solubility and limited diffusion of N_(2)significantly hinder the achievement of satisfactory performance.In this context,we report an effective strategy to enhance NRR activity by introducing a metal-organic framework(MOF)membrane,specifically MIL-53(Al),onto a perovskite oxide(LiNbO_(3)),denoted as LN@MIL-X(X=0.2,0.4 and 0.6).The MIL-53(Al)membrane selectively recognizes and concentrates N_(2)at the catalyst interface while simultaneously repelling water molecules,thereby inhibiting the hydrogen evolution reaction(HER).This ultrathin nanostructure significantly improves the NRR performance of LN@MIL-X compared to pristine LiNbO_(3).Notably,LN@MIL-0.4 exhibits a maximum NH_(3)yield of 45.25 mg h^(-1)mg_(cat.)^(-1)with an impressive Faradaic efficiency(FE)of 86.41%at-0.45 V versus RHE in 0.1 mol L^(-1)Na_(2)SO_(4).This work provides a universal strategy for the design and synthesis of perovskite oxide electrocatalysts,facilitating high-efficiency ammonia synthesis.展开更多
Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and re...Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.展开更多
It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,...It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).展开更多
Ecological floating bed is an important biological remediation method for water pollution control.During the removal of excess nutrients and pollutants,changes in environmental factors affect the characteristics of mi...Ecological floating bed is an important biological remediation method for water pollution control.During the removal of excess nutrients and pollutants,changes in environmental factors affect the characteristics of microorganisms in aquatic ecosystems.To understand the influences of ecological floating beds on size-fractionated microorganisms,we investigated the community assembly and nitrogen metabolic characteristics of three size-fractionated microorganism groups in the ecological floating bed area,using 18S rDNA,16S rDNA metabarcoding,and metagenomic sequencing techniques.Firstly,we discovered substantial differences between size-fractionated groups in the diversity and compositions of both microeukaryotic and bacterial communities,as well as the influences of floating beds on specific groups.The floating beds appeared to provide more habitats for heterotrophs and symbiotes while potentially inhibiting the growth of certain phytoplankton(cyanobacteria).Secondly,we observed that microeukaryotic and bacterial communities were predominantly influenced by stochastic and deterministic processes,respectively,and they both exhibited distinct patterns across different size-fractionated groups.Notably,microeukaryotic community assembly demonstrated a greater sensitivity to ecological floating beds,as indicated by an increase in dispersal limitation processes.Finally,the nitrogen metabolism functional genes revealed that microbes associated with large-sized particles played a crucial role in dissimilatory nitrate reduction to ammonium(DNRA)and denitrification processes within the floating bed area,thereby facilitating the removal of excess nitrogen nutrients from the water.In contrast,freeliving microorganisms from small-sized groups were linked mainly to the genes involved in nitrogen assimilation and assimilatory nitrate reduction to ammonium(ANRA)processes.These findings help understand the impact of ecological floating beds on the diversity and functional characteristics of microorganism communities in different size-fractionated groups.展开更多
Climate warming and atmospheric nitrogen(N)deposition have profound influences on the terrestrial biosphere.However,how these two global change drivers affect phytoplankton which are important primary producers in wet...Climate warming and atmospheric nitrogen(N)deposition have profound influences on the terrestrial biosphere.However,how these two global change drivers affect phytoplankton which are important primary producers in wetlands with large carbon stocks and complex hydrological fluctuations remain largely unclear.As part of a two-year field experiment in a freshwater wetland,this study was conducted to investigate the effects of nighttime warming and N addition on phytoplankton biomass in the North China Plain.The results showed that neither nighttime warming nor N addition influenced the Shannon-Wiener index of phytoplankton community.Nighttime warming did not change phytoplankton biomass,likely due to the different warming impacts on dominant phyla and in different seasons.Decreased phytoplankton biomass in spring because of the increased water pH and submerged plant coverage was compensated by the enhanced biomass in autumn due to the reduced dissolved oxygen and submerged plant coverage,leading to the neutral change of phytoplankton biomass under warming.Nitrogen addition elevated phytoplankton biomass by 11.6%,which could be attributed to the enhanced nutrient availability and reduced submerged plant coverage.Positive relationships of methane(CH4)emission rates at the water-air interface with phytoplankton biomass indicated the potentially crucial role of phytoplankton in mediating wetland CH4 cycling through photosynthesis-driven metabolisms.The findings suggested the seasonal variation of phytoplankton and their potential responses to nighttime warming and N deposition,which may provide a more accurate basis for assessing the global change-carbon feedback in wetland ecosystems.展开更多
Lodging is a major constraint limiting oil flax production efficiency in northern China.Crop lodging susceptibility is closely related to stem lignin content,and the regulatory mechanisms by which nitrogen and potassi...Lodging is a major constraint limiting oil flax production efficiency in northern China.Crop lodging susceptibility is closely related to stem lignin content,and the regulatory mechanisms by which nitrogen and potassium fertilization interactively influence lignin biosynthesis in oil flax stems require further investigation.Therefore,this study aimed to enhance lodging resistance and increase grain yield in oil flax.We examined the interactive effects of different nitrogen (75,150,and 225 kg N ha^(–1)) and potassium (60 and 90 kg K_(2)O ha^(–1)) fertilizer rates on lignin metabolism,lodging resistance,and grain yield during the 2022 and 2023 growing seasons.Results indicated that nitrogen and potassium fertilizer levels and their interactions promoted lignin accumulation,improved lodging resistance,and increased grain yield.Compared to the control (CK),the75–150 kg N ha^(–1) combined with 60 kg K_(2)O ha^(–1) treatments significantly enhanced the activities of key lignin-synthesizing enzymes (tyrosine ammonia-lyase (TAL),phenylalanine ammonia-lyase (PAL),cinnamyl alcohol dehydrogenase (CAD),and peroxidase (POD)) and upregulated the expression of 4CL1 and F5H3 genes,leading to a 29.63–43.30%increase in lignin content,improved stem bending strength and lodging resistance index,and a 23.27–32.34%increase in grain yield.Correlation analysis revealed that nitrogen and potassium fertilizers positively regulated enzyme activities and gene expression related to lignin biosynthesis,thereby facilitating lignin accumulation and enhancing stem mechanical strength and lodging resistance.Positive correlations were observed among lignin-related enzyme activities,gene expression,lodging resistance traits,and grain yield.In summary,the application of 75–150 kg N ha^(–1) in conjunction with 60 kg K_(2)O ha^(–1)promoted lignin biosynthesis and accumulation,enhanced lodging resistance,and increased grain yield in oil flax grown in the dryland farming region of central Gansu,China.Furthermore,this treatment provides a technical basis for cultivating stress-tolerant and high-yield oil flax in arid regions.展开更多
Green ammonia,produced by harnessing renewable solar energy to split nitrogen,plays a pivotal role in both agricultural practices and forthcoming energy configurations,driving the sustainable development of human soci...Green ammonia,produced by harnessing renewable solar energy to split nitrogen,plays a pivotal role in both agricultural practices and forthcoming energy configurations,driving the sustainable development of human society with zero-carbon emissions.However,nitrogen photoreduction currently faces the challenges of poor activation ability and low yield,and it is still challenging to unravel the intertwined problems in this field and provide direction for its development due to the complex reaction mechanism and multidisciplinary aspects such as photochemistry,catalysis,interface science,and technology.This review focuses on capturing the latest advances in photocatalytic nitrogen-to-ammonia conversion,delving into fundamental principles regarding the process,efficient photocatalysts for practical ammonia synthesis,and well-designed catalytic environments.Besides,this article provides insightful guidelines for analyzing complicated reaction mechanisms and identifying key bottlenecks or specific rate-determining steps,such as reactant activation,interfacial reaction engineering,and hydrogen evolution side reactions.By integrating perspectives from atomic mechanisms,nanoscale photocatalysts,microscale interfacial engineering,and macroscale reaction system design,this review advances the development of nitrogen photoreduction from proof-of-concept discoveries to viable solar-to-chemical conversion technologies,while also providing a valuable entry point for researchers into this burgeoning field.展开更多
Schizophrenia(SCZ) is a severe mental disorder with an unclear pathogenesis.Increasing evidence suggests that oxidative stress(OS) may contribute to the neuropathological processes underlying SCZ.Biothiols,key endogen...Schizophrenia(SCZ) is a severe mental disorder with an unclear pathogenesis.Increasing evidence suggests that oxidative stress(OS) may contribute to the neuropathological processes underlying SCZ.Biothiols,key endogenous antioxidants,have been proposed as potential biomarkers for the disease.However,due to the presence of the blood-brain barrier(BBB),fluorescent probes are rarely used to image biothiols in the brain of SCZ models.In this study,a series of fluorescent probes for biothiols were developed using dicyanoisophorone derivatives as fluorophores known for their excellent optical properties,and carboxylic esters as recognition units.A parallel synthesis and rapid screening strategy was employed to construct and optimize these probes.By introducing trifluoromethyl and benzothiazole groups into the fluorophore,the emission wavelength was successfully shifted into the near-infrared region.Additionally,various trifluoromethyl-substituted aromatic and nitrogen heterocyclic compounds were incorporated to optimize the carboxylic esters,thereby improving the probes' reactivity and lipophilicity.Systematic evaluation of the physicochemical characteristics,and optical performance led to the identification of DCIBT-11 as the most promising candidate.DCI-BT-11 demonstrated excellent BBB permeability and a good response to biothiols both in vitro and in vivo.Notably,DCI-BT-11 was used for the first time to visualize biothiol flux and assess the therapeutic effects of the antioxidant N-acetylcysteine(NAC) in the brains of SCZ mouse models,offering new insights into the role of OS in the pathogenesis and treatment of SCZ.展开更多
Coordinating light and nitrogen(N)distribution within a canopy is essential for improving rice yield and resource use efficiency.However,limited research has examined light and N distribution in response to planting d...Coordinating light and nitrogen(N)distribution within a canopy is essential for improving rice yield and resource use efficiency.However,limited research has examined light and N distribution in response to planting density and N rate,and their relationships with grain yield,radiation use efficiency(RUE),and N use efficiency for grain production(NUEg)in rice.A two-year field experiment was conducted with two hybrid varieties under three N levels,0 kg ha^(-1)(N1),90 kg ha^(-1)(N2)and 180 kg ha^(-1)(N3),and two planting densities,22.2 hills m-2(D1)and 33.3 hills m^(-2)(D2).Results showed 3.4%higher yield and 4.4%higher NUEg under N2D2 compared with N3D1.The extinction coefficient for N(K_(N))and light(K_(L))and their ratio(K_(N)/K_(L))at heading stage were significantly influenced by N rate,planting density,and their interaction.K_(N)decreased with the increase of N input or planting density.Compared to N1,K_(N)decreased by 43.5 and 58.8%under N2 and N3,respectively,while K_(N)under D2 decreased by 16.0%compared to D1.Higher K_(L)and K_(N)/K_(L)values occurred under low N rates,with opposite trends under high N rates.Increased planting density led to decreased K_(L)and K_(N)/K_(L)values.N2D2 demonstrated higher K_(L)and K_(N),and thus comparable K_(N)/K_(L),compared to N3D1.Correlation analysis revealed K_(L)negatively correlated with RUE,while K_(N)and K_(N)/K_(L)positively correlated with NUEg.These findings indicate that increasing planting density under reduced N input could maintain rice yield while enhancing resource use efficiency through regulation of canopy light and N distribution.展开更多
Long-term manure application has the potential to alleviate soil acidification, and increase carbon sequestration and nutrient availability, thus improving cropland fertility. However, the mechanisms behind greenhouse...Long-term manure application has the potential to alleviate soil acidification, and increase carbon sequestration and nutrient availability, thus improving cropland fertility. However, the mechanisms behind greenhouse gas N_(2)O emissions from acidic soil mediated by long-term manure application remain poorly understood. Herein, we investigated N_(2)O emission and its linkage with gross N mineralization and nitrification rates, as well as nitrifying and denitrifying microbes in an acidic upland soil subjected to 36-year fertilization treatments, including an unfertilized control(CK), inorganic fertilizer(F), 2× rate of inorganic fertilizer(2F), manure(M), and the combination of inorganic fertilizer and manure(FM) treatments. Compared to the CK treatment(1.34 μg N kg^(-1) d^(-1)), fertilization strongly increased N_(2)O emissions by 34-fold on average, with more pronounced increases in the manure-amendment(10.6-169 μg N kg^(-1) d^(-1)) than those in the inorganic fertilizer treatments(3.26-5.51 μg N kg^(-1) d^(-1)). The manure amendment-stimulated N_(2)O emissions were highly associated with increased soil pH, mean weight diameter of soil aggregates, substrate availability(e.g., particulate organic carbon, NO_(3)^(-)and available phosphorus), gross N mineralization rates, denitrifier abundances and the(nirK+nirS)/nosZ ratio. These findings suggest that the increased N_(2)O emissions primarily resulted from alleviated acidification, increased substrate availability and improved soil structure, thus enhancing microbial N mineralization and favoring N_(2)O^(-)producing denitrifiers over N_(2)O consumers. Moreover, ammonia-oxidizing bacteria(AOB) rather than ammonia-oxidizing archaea(AOA) positively correlated with soil NO_(3)^(-)concentration and N_(2)O emissions, indicating that nitrification indirectly contributed to N_(2)O production by supplying NO_(3)^(-)for denitrification. Collectively, manure amendment potentially stimulates N_(2)O emissions, primarily resulting from alleviated soil acidification and increased substrate availability, thus enhancing N mineralization and denitrifier-mediated N_(2)O production. Our findings suggest that consideration should be given to the greenhouse gas budgets of agricultural ecosystems when applying manure for managing the pH and fertility of acidic soils.展开更多
Nitrogen use efficiency in rice is lower than in upland crops,likely due to differences in soil nitrogen dynamics and crop nitrogen preferences.However,the specific nitrogen dynamics in paddy and upland systems and th...Nitrogen use efficiency in rice is lower than in upland crops,likely due to differences in soil nitrogen dynamics and crop nitrogen preferences.However,the specific nitrogen dynamics in paddy and upland systems and their impact on crop nitrogen uptake remain poorly understood.The N dynamics and impact on crop N uptake determine the downstream environmental pollution from nitrogen fertilizer.To address this poor understanding,we analyzed 2,044 observations of gross nitrogen transformation rates in soils from 136 studies to examine nitrogen dynamics in both systems and their effects on nitrogen uptake in rice and upland crops.Our findings revealed that nitrogen mineralization and autotrophic nitrification rates are lower in paddies than in upland soil,while dissimilatory nitrate reduction to ammonium is higher in paddies,these differences being driven by flooding and lower total nitrogen content in paddies.Rice exhibited higher ammonium uptake,while upland crops had over twice the nitrate uptake.Autotrophic nitrification stimulated by p H reduced rice nitrogen uptake,while heterotrophic nitrification enhanced nitrogen uptake of upland crops.Autotrophic nitrification played a key role in regulating the ammonium-to-nitrate ratio in soils,which further affected the balance of plant nitrogen uptake.These results highlight the need to align soil nitrogen dynamics with crop nitrogen preferences to maximize plant maximize productivity and reduce reactive nitrogen pollution.展开更多
We report first-principles predictions of a cage-like polymeric nitrogen phase(cage-N)composed of interlocked N10 clusters stabilized by mixed sp^(2)/sp^(3) hybridization.Under high pressure,cage-N exhibits exceptiona...We report first-principles predictions of a cage-like polymeric nitrogen phase(cage-N)composed of interlocked N10 clusters stabilized by mixed sp^(2)/sp^(3) hybridization.Under high pressure,cage-N exhibits exceptional mechanical performance,including an ideal compressive strength of 343 GPa at a pressure of 300 GPa,~33% higher than that of diamond.This ultrahigh strength arises from the synergistic interplay between its three-dimensional covalent framework and hybridized bonding topology,which enables isotropic stress accommodation and dynamic electronic rearrangement.These results establish cage-N as a promising non-carbon ultrahard material and provide a bonding-driven route toward designing superhard frameworks under extreme conditions.展开更多
In order to improve the total-dose radiation har dness of the buried oxides(BOX) in the structure of separation-by-implanted-oxygen(SIMOX) silicon-on-insulator(SOI),nitrogen ions are implanted into the buried oxides w...In order to improve the total-dose radiation har dness of the buried oxides(BOX) in the structure of separation-by-implanted-oxygen(SIMOX) silicon-on-insulator(SOI),nitrogen ions are implanted into the buried oxides with two different doses,2×10 15 and 3×10 15 cm -2 ,respectively.The experimental results show that the radiation hardness of the buried oxides is very sensitive to the doses of nitrogen implantation for a lower dose of irradiation with a Co-60 source.Despite the small difference between the doses of nitrogen implantation,the nitrogen-implanted 2×10 15 cm -2 BOX has a much higher hardness than the control sample (i.e.the buried oxide without receiving nitrogen implantation) for a total-dose irradiation of 5×104rad(Si),whereas the nitrogen-implanted 3×10 15 cm -2 BOX has a lower hardness than uhe control sample.However,this sensitivity of radiation hardness to the doses of nitrogen implantation reduces with the increasing total-dose of irradiation (from 5×104 to 5×105rad (Si)).The radiation hardness of BOX is characterized by MOS high-frequency (HF) capacitance-voltage (C-V) technique after the top silicon layers are removed.In addition,the abnormal HF C-V curve of the metal-silicon-BOX-silicon(MSOS) structure is observed and explained.展开更多
A series of meso‐microporous copper‐supporting chabazite molecular sieve（CuSAPO‐34） catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction（NH3‐SCR）have been synthesized ...A series of meso‐microporous copper‐supporting chabazite molecular sieve（CuSAPO‐34） catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction（NH3‐SCR）have been synthesized via a one‐pot hydrothermal crystallization method. The physicochemical properties of the catalysts were characterized by scanning electron microscopy, transmission electron microscopy, N2 adsorption‐desorption measurements, X‐ray diffraction, 27 Al magic angle spinning nuclear magnetic resonance, diffuse reflectance ultraviolet‐visible spectroscopy, inductively coupled plasma‐atomic emission spectroscopy, X‐ray photoelectron spectroscopy, temperature‐programmed reduction measurements, and electron paramagnetic resonance analysis. The formation of micro‐mesopores in the Cu‐SAPO‐34 catalysts decreases diffusion resistance and greatly improves the accessibility of reactants to catalytic active sites. The main active sites for NH3‐SCR reaction are the isolated Cu^2＋ species displaced into the ellipsoidal cavity of the Cu‐SAPO‐34 catalysts.展开更多
Dielectric barrier discharge （DBD） plasma was utilized to oxidize NO contained in the exhaust gas to NO2, ultimately improve the selective catalytic reduction of nitrogen oxides （NOx）. In the one case, DBD was cre...Dielectric barrier discharge （DBD） plasma was utilized to oxidize NO contained in the exhaust gas to NO2, ultimately improve the selective catalytic reduction of nitrogen oxides （NOx）. In the one case, DBD was created directly in the exhaust gas （direct application）, and in the an other case, ozone produced by DBD was injected into the exhaust gas （indirect application）. A comparative study between such direct and indirect applications of DBD plasma was made in terms of the NOx removal efficiency and the energy consumption. The NO2 content in the exhaust gas was changed by the voltage applied to the DBD device （for direct application） or by the amount of ozone added to the exhaust gas （for indirect application）. In both cases, NO was easily oxidized to NO2, and the change in NO2 content largely affected the NOx removal performance of the catalytic reactor placed downstream, where both NO and NO2 were reduced to N2 in the presence of ammonia as the reducing agent. The experiments were primarily concerned with the effect of reaction temperature on the catalytic NOx reduction at various NO2 contents. The direct and indirect applications of DBD were found to remarkably improve the catalytic NOx reduction, especially at low temperatures.展开更多
A single-stage plasma-catalytic reactor in which catalytic materials werepacked was used to remove nitrogen oxides. The packing material was scoria being made of variousmetal oxides including Al_2O_3, MgO, TiO_2, etc....A single-stage plasma-catalytic reactor in which catalytic materials werepacked was used to remove nitrogen oxides. The packing material was scoria being made of variousmetal oxides including Al_2O_3, MgO, TiO_2, etc. Scoria was able to act not only as dielectricpellets but also as a catalyst in the presence of reducing agent such as ethylene and ammonia.Without plasma discharge, scoria did not work well as a catalyst in the temperature range of 100 ℃to 200 ℃, showing less than 10% of NOx removal efficiency. When plasma is produced inside thereactor, the NOx removal efficiency could be increased to 60% in this temperature range.展开更多
The potential of using denitrifying and nitrifying concurrent biofilters for the removal of nitrogen oxides from synthetic gas streams was studied under the condition of high oxygen concentration. It was found that ...The potential of using denitrifying and nitrifying concurrent biofilters for the removal of nitrogen oxides from synthetic gas streams was studied under the condition of high oxygen concentration. It was found that more than 85% of nitric oxide was removed from synthetic combustion gas-streams which contained 20% oxygen and 350 μL/L NO, with a residence time of 60 seconds. In the process, it was found that the existing of oxygen showed no evident negative effect on the efficiency of nitrogen removal.展开更多
This paper reports the studies conducted on removal of oxides ofnitrogen (NOx) from diesel engine exhaust using electrical dischargeplasma combined with adsorbing materials such as molecular sieves.This study is being...This paper reports the studies conducted on removal of oxides ofnitrogen (NOx) from diesel engine exhaust using electrical dischargeplasma combined with adsorbing materials such as molecular sieves.This study is being reported for the first time. The exhaust is takenfrom a diesel engine of 6 kW under no load conditions. Thecharacteristic behavior of a pulse energized dielectric barrierdischarge reactor in the diesel exhaust treatment is reported. TheNOx removal was not significant (36/100) when the reactor without anypacking was used.展开更多
Nitrogen oxides（NOx：NO,NO2）are a concern due to their adverse health effects.Diesel engine transport sector is the major emitter of NOx.The regulations have been strengthened and to comply with them,one of the two ...Nitrogen oxides（NOx：NO,NO2）are a concern due to their adverse health effects.Diesel engine transport sector is the major emitter of NOx.The regulations have been strengthened and to comply with them,one of the two methods commonly used is the selective catalytic reduction of NOxby NH3（NH3-SCR）,NH3being supplied by the in-situ hydrolysis of urea.Efficiency and durability of the catalyst for this process are highly required.Durability is evaluated by hydrothermal treatment of the catalysts at temperature above 800℃.In this study,very active catalysts for the NH3-SCR of NOxwere prepared by using a silicoaluminophosphate commercial zeolite as copper host structure.Characterizations by X-ray diffraction（XRD）,scanning electron microscopy（SEM）and temperature programmed desorption of ammonia（NH3-TPD）showed that this commercial zeolite was hydrothermally stable up to 850℃ and,was able to retain some structural properties up to950℃.After hydrothermal treatment at 850℃,the NOxreduction efficiency into NH3-SCR depends on the copper content.The catalyst with a copper content of 1.25 wt.%was the most active.The difference in activity was much more important when using NO than the fast NO/NO2reaction mixture.展开更多
基金supported by the Natural Science Foundation of Guangdong Province(No.2020A1515110526)the Key-Area Research and Development Programof Guangdong Province(No.2020B1111360003)the National Natural Science Foundation of China(No.42305096).
文摘Nitrogen oxides(NO_(x))are crucial in tropospheric photochemical ozone(O_(3))production and oxidation capacity.Currently,the widely used NO_(x)measurement technique is chemiluminescence(CL)(CL-NO_(x)),which tends to overestimate NO_(2)due to atmospheric oxidation products of NO_(x)(i.e.,NO_(z)).We developed and characterized a NO_(x)measurement system using the cavity attenuated phase shift(CAPS)technique(CAPS-NO_(x)),which is free from interferences with nitrogen-containing species.The NO_(x)measured by the CAPS-NO_(x)and CL-NO_(x)analyzers were compared.Results show that both analyzers showed consistent measurement results for NO,but the NO_(2)measured by the CAPS-NO_(x)analyzer(NO_(2)_CAPS)was mostly lower than that measured by the CL-NO_(x)analyzer(NO_(2)_CL),which led to the deviations in O_(3)formation sensitivity regime and O_(x)(=O_(3)+NO_(2))sources(i.e.,regional background and photochemically produced O_(x))determined by the ozone production efficiencies(OPE)calculated from NO_(2)_CL and NO_(2)_CAPS.Overall,OPE_CL exceeded OPE_CAPS by 18.9%,which shifted 3 out of 13 observation days from the VOCs-limited to the transition regime when judging using OPE_CL,as compared to calculations using OPE_CAPS.During the observation period,days dominated by regional background O_(x)accounted for 46%and 62%when determined using NO_(2)_CL and NO_(2)_CAPS,respectively.These findings suggest that the use of the CL-NO_(x)analyzer tends to underestimate both the VOCs-limited regime and the regional background O_(x)dominated days.The newly built CAPS-NO_(x)analyzer here can promote the accurate measurement of NO_(2),which is meaningful for diagnosing O_(3)formation regimes and O_(x)sources.
基金supported by the National Natural Science Foundation of China(No.U22A20418,22075196)the Research Project Supported by Shanxi Scholarship Council of China(2022–050).
文摘The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocatalysts.However,the low solubility and limited diffusion of N_(2)significantly hinder the achievement of satisfactory performance.In this context,we report an effective strategy to enhance NRR activity by introducing a metal-organic framework(MOF)membrane,specifically MIL-53(Al),onto a perovskite oxide(LiNbO_(3)),denoted as LN@MIL-X(X=0.2,0.4 and 0.6).The MIL-53(Al)membrane selectively recognizes and concentrates N_(2)at the catalyst interface while simultaneously repelling water molecules,thereby inhibiting the hydrogen evolution reaction(HER).This ultrathin nanostructure significantly improves the NRR performance of LN@MIL-X compared to pristine LiNbO_(3).Notably,LN@MIL-0.4 exhibits a maximum NH_(3)yield of 45.25 mg h^(-1)mg_(cat.)^(-1)with an impressive Faradaic efficiency(FE)of 86.41%at-0.45 V versus RHE in 0.1 mol L^(-1)Na_(2)SO_(4).This work provides a universal strategy for the design and synthesis of perovskite oxide electrocatalysts,facilitating high-efficiency ammonia synthesis.
基金supported by National Natural Science Fundation of China(Nos.52170086,22308194,U22A20423)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+1 种基金Taishan Scholars Program of Shandong Province(No.tsqn202211012)Shandong Provincial Excellent Youth(No.ZR2022YQ47)。
文摘Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.
文摘It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).
基金Supported by the National Natural Science Foundation of China(Nos.42141003,42176147)the National Key Research and Development Program of China(No.2022YFF0802204)the Xiamen Key Laboratory of Urban Sea Ecological Conservation and Restoration(USER)(Nos.USER2021-1,USER2021-5)。
文摘Ecological floating bed is an important biological remediation method for water pollution control.During the removal of excess nutrients and pollutants,changes in environmental factors affect the characteristics of microorganisms in aquatic ecosystems.To understand the influences of ecological floating beds on size-fractionated microorganisms,we investigated the community assembly and nitrogen metabolic characteristics of three size-fractionated microorganism groups in the ecological floating bed area,using 18S rDNA,16S rDNA metabarcoding,and metagenomic sequencing techniques.Firstly,we discovered substantial differences between size-fractionated groups in the diversity and compositions of both microeukaryotic and bacterial communities,as well as the influences of floating beds on specific groups.The floating beds appeared to provide more habitats for heterotrophs and symbiotes while potentially inhibiting the growth of certain phytoplankton(cyanobacteria).Secondly,we observed that microeukaryotic and bacterial communities were predominantly influenced by stochastic and deterministic processes,respectively,and they both exhibited distinct patterns across different size-fractionated groups.Notably,microeukaryotic community assembly demonstrated a greater sensitivity to ecological floating beds,as indicated by an increase in dispersal limitation processes.Finally,the nitrogen metabolism functional genes revealed that microbes associated with large-sized particles played a crucial role in dissimilatory nitrate reduction to ammonium(DNRA)and denitrification processes within the floating bed area,thereby facilitating the removal of excess nitrogen nutrients from the water.In contrast,freeliving microorganisms from small-sized groups were linked mainly to the genes involved in nitrogen assimilation and assimilatory nitrate reduction to ammonium(ANRA)processes.These findings help understand the impact of ecological floating beds on the diversity and functional characteristics of microorganism communities in different size-fractionated groups.
基金supported by the Science and Technology Project of Hebei Education Department(No.QN2023028)the Natural Science Foundation of Hebei Province(No.C2022201042)+1 种基金the High-level Talent Research Funding Project of Hebei University(Nos.521000981405 and 521000981186)the Collaborative Innovation Center for Baiyangdian Basin Ecological Protection and Beijing-Tianjin-Hebei Sustainable Development.
文摘Climate warming and atmospheric nitrogen(N)deposition have profound influences on the terrestrial biosphere.However,how these two global change drivers affect phytoplankton which are important primary producers in wetlands with large carbon stocks and complex hydrological fluctuations remain largely unclear.As part of a two-year field experiment in a freshwater wetland,this study was conducted to investigate the effects of nighttime warming and N addition on phytoplankton biomass in the North China Plain.The results showed that neither nighttime warming nor N addition influenced the Shannon-Wiener index of phytoplankton community.Nighttime warming did not change phytoplankton biomass,likely due to the different warming impacts on dominant phyla and in different seasons.Decreased phytoplankton biomass in spring because of the increased water pH and submerged plant coverage was compensated by the enhanced biomass in autumn due to the reduced dissolved oxygen and submerged plant coverage,leading to the neutral change of phytoplankton biomass under warming.Nitrogen addition elevated phytoplankton biomass by 11.6%,which could be attributed to the enhanced nutrient availability and reduced submerged plant coverage.Positive relationships of methane(CH4)emission rates at the water-air interface with phytoplankton biomass indicated the potentially crucial role of phytoplankton in mediating wetland CH4 cycling through photosynthesis-driven metabolisms.The findings suggested the seasonal variation of phytoplankton and their potential responses to nighttime warming and N deposition,which may provide a more accurate basis for assessing the global change-carbon feedback in wetland ecosystems.
基金funded by the National Natural Science Foundation of China (31760363)the Earmarked Fund for CARS (CARS-14-1-16)+1 种基金the Gansu Education Science and Technology Innovation Industry Support Program,China (2021CYZC-38)the Gansu Provincial Key Laboratory of Arid Land Crop Science,Gansu Agricultural University,China (GSCS-2020-Z6)。
文摘Lodging is a major constraint limiting oil flax production efficiency in northern China.Crop lodging susceptibility is closely related to stem lignin content,and the regulatory mechanisms by which nitrogen and potassium fertilization interactively influence lignin biosynthesis in oil flax stems require further investigation.Therefore,this study aimed to enhance lodging resistance and increase grain yield in oil flax.We examined the interactive effects of different nitrogen (75,150,and 225 kg N ha^(–1)) and potassium (60 and 90 kg K_(2)O ha^(–1)) fertilizer rates on lignin metabolism,lodging resistance,and grain yield during the 2022 and 2023 growing seasons.Results indicated that nitrogen and potassium fertilizer levels and their interactions promoted lignin accumulation,improved lodging resistance,and increased grain yield.Compared to the control (CK),the75–150 kg N ha^(–1) combined with 60 kg K_(2)O ha^(–1) treatments significantly enhanced the activities of key lignin-synthesizing enzymes (tyrosine ammonia-lyase (TAL),phenylalanine ammonia-lyase (PAL),cinnamyl alcohol dehydrogenase (CAD),and peroxidase (POD)) and upregulated the expression of 4CL1 and F5H3 genes,leading to a 29.63–43.30%increase in lignin content,improved stem bending strength and lodging resistance index,and a 23.27–32.34%increase in grain yield.Correlation analysis revealed that nitrogen and potassium fertilizers positively regulated enzyme activities and gene expression related to lignin biosynthesis,thereby facilitating lignin accumulation and enhancing stem mechanical strength and lodging resistance.Positive correlations were observed among lignin-related enzyme activities,gene expression,lodging resistance traits,and grain yield.In summary,the application of 75–150 kg N ha^(–1) in conjunction with 60 kg K_(2)O ha^(–1)promoted lignin biosynthesis and accumulation,enhanced lodging resistance,and increased grain yield in oil flax grown in the dryland farming region of central Gansu,China.Furthermore,this treatment provides a technical basis for cultivating stress-tolerant and high-yield oil flax in arid regions.
基金financially supported by the National Energy Green Hydrogen Refining Research&Development Center,National Natural Science Foundation of China(No.22476222)Natural Science Funds of Guangdong for Distinguished Young Scholar(No.2022B1515020098).
文摘Green ammonia,produced by harnessing renewable solar energy to split nitrogen,plays a pivotal role in both agricultural practices and forthcoming energy configurations,driving the sustainable development of human society with zero-carbon emissions.However,nitrogen photoreduction currently faces the challenges of poor activation ability and low yield,and it is still challenging to unravel the intertwined problems in this field and provide direction for its development due to the complex reaction mechanism and multidisciplinary aspects such as photochemistry,catalysis,interface science,and technology.This review focuses on capturing the latest advances in photocatalytic nitrogen-to-ammonia conversion,delving into fundamental principles regarding the process,efficient photocatalysts for practical ammonia synthesis,and well-designed catalytic environments.Besides,this article provides insightful guidelines for analyzing complicated reaction mechanisms and identifying key bottlenecks or specific rate-determining steps,such as reactant activation,interfacial reaction engineering,and hydrogen evolution side reactions.By integrating perspectives from atomic mechanisms,nanoscale photocatalysts,microscale interfacial engineering,and macroscale reaction system design,this review advances the development of nitrogen photoreduction from proof-of-concept discoveries to viable solar-to-chemical conversion technologies,while also providing a valuable entry point for researchers into this burgeoning field.
基金supported by the National Natural Science Foundation of China (Nos.22177025,21807021,22177026)the Science Fund for Creative Research Groups of the Natural Science Foundation of Hebei Province (No.B2021201038)+1 种基金the Foundation of Hebei University (No.050001-513300201004)the Director’s Foundation of the Key Laboratory of Medicinal Chemistry and Molecular Diagnosis,Ministry of Education,Hebei University (No.MCMDZR2024003)。
文摘Schizophrenia(SCZ) is a severe mental disorder with an unclear pathogenesis.Increasing evidence suggests that oxidative stress(OS) may contribute to the neuropathological processes underlying SCZ.Biothiols,key endogenous antioxidants,have been proposed as potential biomarkers for the disease.However,due to the presence of the blood-brain barrier(BBB),fluorescent probes are rarely used to image biothiols in the brain of SCZ models.In this study,a series of fluorescent probes for biothiols were developed using dicyanoisophorone derivatives as fluorophores known for their excellent optical properties,and carboxylic esters as recognition units.A parallel synthesis and rapid screening strategy was employed to construct and optimize these probes.By introducing trifluoromethyl and benzothiazole groups into the fluorophore,the emission wavelength was successfully shifted into the near-infrared region.Additionally,various trifluoromethyl-substituted aromatic and nitrogen heterocyclic compounds were incorporated to optimize the carboxylic esters,thereby improving the probes' reactivity and lipophilicity.Systematic evaluation of the physicochemical characteristics,and optical performance led to the identification of DCIBT-11 as the most promising candidate.DCI-BT-11 demonstrated excellent BBB permeability and a good response to biothiols both in vitro and in vivo.Notably,DCI-BT-11 was used for the first time to visualize biothiol flux and assess the therapeutic effects of the antioxidant N-acetylcysteine(NAC) in the brains of SCZ mouse models,offering new insights into the role of OS in the pathogenesis and treatment of SCZ.
基金supported by the Hubei Provincial Science and Technology Project,China(2025CSA039)the National Natural Science Foundation of China(32001467)。
文摘Coordinating light and nitrogen(N)distribution within a canopy is essential for improving rice yield and resource use efficiency.However,limited research has examined light and N distribution in response to planting density and N rate,and their relationships with grain yield,radiation use efficiency(RUE),and N use efficiency for grain production(NUEg)in rice.A two-year field experiment was conducted with two hybrid varieties under three N levels,0 kg ha^(-1)(N1),90 kg ha^(-1)(N2)and 180 kg ha^(-1)(N3),and two planting densities,22.2 hills m-2(D1)and 33.3 hills m^(-2)(D2).Results showed 3.4%higher yield and 4.4%higher NUEg under N2D2 compared with N3D1.The extinction coefficient for N(K_(N))and light(K_(L))and their ratio(K_(N)/K_(L))at heading stage were significantly influenced by N rate,planting density,and their interaction.K_(N)decreased with the increase of N input or planting density.Compared to N1,K_(N)decreased by 43.5 and 58.8%under N2 and N3,respectively,while K_(N)under D2 decreased by 16.0%compared to D1.Higher K_(L)and K_(N)/K_(L)values occurred under low N rates,with opposite trends under high N rates.Increased planting density led to decreased K_(L)and K_(N)/K_(L)values.N2D2 demonstrated higher K_(L)and K_(N),and thus comparable K_(N)/K_(L),compared to N3D1.Correlation analysis revealed K_(L)negatively correlated with RUE,while K_(N)and K_(N)/K_(L)positively correlated with NUEg.These findings indicate that increasing planting density under reduced N input could maintain rice yield while enhancing resource use efficiency through regulation of canopy light and N distribution.
基金financially supported by the National Science & Technology Fundamental Resources Investigation Project of China (2021FY100501)the Youth Innovation of Chinese Academy of Agricultural Sciences (Y2023QC16)。
文摘Long-term manure application has the potential to alleviate soil acidification, and increase carbon sequestration and nutrient availability, thus improving cropland fertility. However, the mechanisms behind greenhouse gas N_(2)O emissions from acidic soil mediated by long-term manure application remain poorly understood. Herein, we investigated N_(2)O emission and its linkage with gross N mineralization and nitrification rates, as well as nitrifying and denitrifying microbes in an acidic upland soil subjected to 36-year fertilization treatments, including an unfertilized control(CK), inorganic fertilizer(F), 2× rate of inorganic fertilizer(2F), manure(M), and the combination of inorganic fertilizer and manure(FM) treatments. Compared to the CK treatment(1.34 μg N kg^(-1) d^(-1)), fertilization strongly increased N_(2)O emissions by 34-fold on average, with more pronounced increases in the manure-amendment(10.6-169 μg N kg^(-1) d^(-1)) than those in the inorganic fertilizer treatments(3.26-5.51 μg N kg^(-1) d^(-1)). The manure amendment-stimulated N_(2)O emissions were highly associated with increased soil pH, mean weight diameter of soil aggregates, substrate availability(e.g., particulate organic carbon, NO_(3)^(-)and available phosphorus), gross N mineralization rates, denitrifier abundances and the(nirK+nirS)/nosZ ratio. These findings suggest that the increased N_(2)O emissions primarily resulted from alleviated acidification, increased substrate availability and improved soil structure, thus enhancing microbial N mineralization and favoring N_(2)O^(-)producing denitrifiers over N_(2)O consumers. Moreover, ammonia-oxidizing bacteria(AOB) rather than ammonia-oxidizing archaea(AOA) positively correlated with soil NO_(3)^(-)concentration and N_(2)O emissions, indicating that nitrification indirectly contributed to N_(2)O production by supplying NO_(3)^(-)for denitrification. Collectively, manure amendment potentially stimulates N_(2)O emissions, primarily resulting from alleviated soil acidification and increased substrate availability, thus enhancing N mineralization and denitrifier-mediated N_(2)O production. Our findings suggest that consideration should be given to the greenhouse gas budgets of agricultural ecosystems when applying manure for managing the pH and fertility of acidic soils.
基金funded by the National Key Research and Development Program of China(2024YFD1501602)the National Natural Science Foundation of China(42407437)conducted as part of the Coordinated Research Project D1.50.16,implemented by the Soil and Water Management and Crop Nutrition Section of the Joint FAO/IAEA Division of Nuclear Techniques in Food and Agriculture,Department of Nuclear Sciences and Applications,Vienna,Austria。
文摘Nitrogen use efficiency in rice is lower than in upland crops,likely due to differences in soil nitrogen dynamics and crop nitrogen preferences.However,the specific nitrogen dynamics in paddy and upland systems and their impact on crop nitrogen uptake remain poorly understood.The N dynamics and impact on crop N uptake determine the downstream environmental pollution from nitrogen fertilizer.To address this poor understanding,we analyzed 2,044 observations of gross nitrogen transformation rates in soils from 136 studies to examine nitrogen dynamics in both systems and their effects on nitrogen uptake in rice and upland crops.Our findings revealed that nitrogen mineralization and autotrophic nitrification rates are lower in paddies than in upland soil,while dissimilatory nitrate reduction to ammonium is higher in paddies,these differences being driven by flooding and lower total nitrogen content in paddies.Rice exhibited higher ammonium uptake,while upland crops had over twice the nitrate uptake.Autotrophic nitrification stimulated by p H reduced rice nitrogen uptake,while heterotrophic nitrification enhanced nitrogen uptake of upland crops.Autotrophic nitrification played a key role in regulating the ammonium-to-nitrate ratio in soils,which further affected the balance of plant nitrogen uptake.These results highlight the need to align soil nitrogen dynamics with crop nitrogen preferences to maximize plant maximize productivity and reduce reactive nitrogen pollution.
基金supported by the Natural Science Foundation of China(Grant Nos.T2325013,52288102,52090024,12034009,12474004,and 12304036)the National Key R&D Program of China Grant No.2023YFA1610000+1 种基金the Fundamental Research Funds for the Central Universitiesthe Program for Jilin University and Sun Yat-sen University.
文摘We report first-principles predictions of a cage-like polymeric nitrogen phase(cage-N)composed of interlocked N10 clusters stabilized by mixed sp^(2)/sp^(3) hybridization.Under high pressure,cage-N exhibits exceptional mechanical performance,including an ideal compressive strength of 343 GPa at a pressure of 300 GPa,~33% higher than that of diamond.This ultrahigh strength arises from the synergistic interplay between its three-dimensional covalent framework and hybridized bonding topology,which enables isotropic stress accommodation and dynamic electronic rearrangement.These results establish cage-N as a promising non-carbon ultrahard material and provide a bonding-driven route toward designing superhard frameworks under extreme conditions.
文摘In order to improve the total-dose radiation har dness of the buried oxides(BOX) in the structure of separation-by-implanted-oxygen(SIMOX) silicon-on-insulator(SOI),nitrogen ions are implanted into the buried oxides with two different doses,2×10 15 and 3×10 15 cm -2 ,respectively.The experimental results show that the radiation hardness of the buried oxides is very sensitive to the doses of nitrogen implantation for a lower dose of irradiation with a Co-60 source.Despite the small difference between the doses of nitrogen implantation,the nitrogen-implanted 2×10 15 cm -2 BOX has a much higher hardness than the control sample (i.e.the buried oxide without receiving nitrogen implantation) for a total-dose irradiation of 5×104rad(Si),whereas the nitrogen-implanted 3×10 15 cm -2 BOX has a lower hardness than uhe control sample.However,this sensitivity of radiation hardness to the doses of nitrogen implantation reduces with the increasing total-dose of irradiation (from 5×104 to 5×105rad (Si)).The radiation hardness of BOX is characterized by MOS high-frequency (HF) capacitance-voltage (C-V) technique after the top silicon layers are removed.In addition,the abnormal HF C-V curve of the metal-silicon-BOX-silicon(MSOS) structure is observed and explained.
基金supported by the National Natural Science Foundation of China(2137626121173270)+4 种基金the National High Technology Research and Development Program of China(863 Program2015AA034603)the Beijing Natural Science Foundation(2142027)the China University of Petroleum Fund(201300071100072462015QZDX04)~~
文摘A series of meso‐microporous copper‐supporting chabazite molecular sieve（CuSAPO‐34） catalysts with excellent performance in low‐temperature ammonia selective catalytic reduction（NH3‐SCR）have been synthesized via a one‐pot hydrothermal crystallization method. The physicochemical properties of the catalysts were characterized by scanning electron microscopy, transmission electron microscopy, N2 adsorption‐desorption measurements, X‐ray diffraction, 27 Al magic angle spinning nuclear magnetic resonance, diffuse reflectance ultraviolet‐visible spectroscopy, inductively coupled plasma‐atomic emission spectroscopy, X‐ray photoelectron spectroscopy, temperature‐programmed reduction measurements, and electron paramagnetic resonance analysis. The formation of micro‐mesopores in the Cu‐SAPO‐34 catalysts decreases diffusion resistance and greatly improves the accessibility of reactants to catalytic active sites. The main active sites for NH3‐SCR reaction are the isolated Cu^2＋ species displaced into the ellipsoidal cavity of the Cu‐SAPO‐34 catalysts.
文摘Dielectric barrier discharge （DBD） plasma was utilized to oxidize NO contained in the exhaust gas to NO2, ultimately improve the selective catalytic reduction of nitrogen oxides （NOx）. In the one case, DBD was created directly in the exhaust gas （direct application）, and in the an other case, ozone produced by DBD was injected into the exhaust gas （indirect application）. A comparative study between such direct and indirect applications of DBD plasma was made in terms of the NOx removal efficiency and the energy consumption. The NO2 content in the exhaust gas was changed by the voltage applied to the DBD device （for direct application） or by the amount of ozone added to the exhaust gas （for indirect application）. In both cases, NO was easily oxidized to NO2, and the change in NO2 content largely affected the NOx removal performance of the catalytic reactor placed downstream, where both NO and NO2 were reduced to N2 in the presence of ammonia as the reducing agent. The experiments were primarily concerned with the effect of reaction temperature on the catalytic NOx reduction at various NO2 contents. The direct and indirect applications of DBD were found to remarkably improve the catalytic NOx reduction, especially at low temperatures.
基金The project supported by the Basic Research Program of the Korea Science & Engineering Foundation (KOSEF) (No. R05-2001-000-01247-0)
文摘A single-stage plasma-catalytic reactor in which catalytic materials werepacked was used to remove nitrogen oxides. The packing material was scoria being made of variousmetal oxides including Al_2O_3, MgO, TiO_2, etc. Scoria was able to act not only as dielectricpellets but also as a catalyst in the presence of reducing agent such as ethylene and ammonia.Without plasma discharge, scoria did not work well as a catalyst in the temperature range of 100 ℃to 200 ℃, showing less than 10% of NOx removal efficiency. When plasma is produced inside thereactor, the NOx removal efficiency could be increased to 60% in this temperature range.
基金supported by the National Natural Science Foundation of China(Grants No.20277009)
文摘The potential of using denitrifying and nitrifying concurrent biofilters for the removal of nitrogen oxides from synthetic gas streams was studied under the condition of high oxygen concentration. It was found that more than 85% of nitric oxide was removed from synthetic combustion gas-streams which contained 20% oxygen and 350 μL/L NO, with a residence time of 60 seconds. In the process, it was found that the existing of oxygen showed no evident negative effect on the efficiency of nitrogen removal.
文摘This paper reports the studies conducted on removal of oxides ofnitrogen (NOx) from diesel engine exhaust using electrical dischargeplasma combined with adsorbing materials such as molecular sieves.This study is being reported for the first time. The exhaust is takenfrom a diesel engine of 6 kW under no load conditions. Thecharacteristic behavior of a pulse energized dielectric barrierdischarge reactor in the diesel exhaust treatment is reported. TheNOx removal was not significant (36/100) when the reactor without anypacking was used.
基金the UREENOX project (ANR-11-VPTT-002) funded by the French ANR (L'Agence National de la Recherche)the French ANR for financial supportThe Institute of Chemistry of Poitiers (IC2MP) for the management of the UREENOX project
文摘Nitrogen oxides（NOx：NO,NO2）are a concern due to their adverse health effects.Diesel engine transport sector is the major emitter of NOx.The regulations have been strengthened and to comply with them,one of the two methods commonly used is the selective catalytic reduction of NOxby NH3（NH3-SCR）,NH3being supplied by the in-situ hydrolysis of urea.Efficiency and durability of the catalyst for this process are highly required.Durability is evaluated by hydrothermal treatment of the catalysts at temperature above 800℃.In this study,very active catalysts for the NH3-SCR of NOxwere prepared by using a silicoaluminophosphate commercial zeolite as copper host structure.Characterizations by X-ray diffraction（XRD）,scanning electron microscopy（SEM）and temperature programmed desorption of ammonia（NH3-TPD）showed that this commercial zeolite was hydrothermally stable up to 850℃ and,was able to retain some structural properties up to950℃.After hydrothermal treatment at 850℃,the NOxreduction efficiency into NH3-SCR depends on the copper content.The catalyst with a copper content of 1.25 wt.%was the most active.The difference in activity was much more important when using NO than the fast NO/NO2reaction mixture.
