Polycyclic Aromatic Hydrocarbons(PAHs),along with their derivatives nitro-PAHs and oxy-PAHs,are globally recognized toxic pollutants.This research conducted daily PM_(2.5)sampling in winter 2021 at three urban(YNCE,SW...Polycyclic Aromatic Hydrocarbons(PAHs),along with their derivatives nitro-PAHs and oxy-PAHs,are globally recognized toxic pollutants.This research conducted daily PM_(2.5)sampling in winter 2021 at three urban(YNCE,SWP,and NG)and three suburban sites(HC,CTV,and YNE)in the Ili River Valley(IRV).For the first time in the IRV,a comprehensive study on 39 PAHs and derivatives was carried out.The results showed that the average∑_(16)PAHs concentration was 130.21±98.94 ng/m^(3),with 16PAHs constituting the dominant fraction(112.51±86.48 ng/m^(3)).The mean BaP and the total BaP equivalent quotient(TEQ)concentrations were 10.28±8.85 ng/m^(3)and 19.74±16.70 ng/m^(3),respectively.Approximately 88%of the daily BaP averages and 98%of the daily TEQ averages exceeded the national daily average standard of BaP(2.5 ng/m^(3)),indicating severe local BaP pollution.Urban sites had notably higher∑PAHs and TEQ concentrations than suburban sites,attributed to increased vehicular traffic and coal combustion in urban areas.PMF results showed that traffic emissions(32.7%-60.5%),coal combustion(13.9%-24.3%)and secondary formation(14.7%-22.7%)were the primary contributors to∑PAHs.Urban sites experienced a greater influence from traffic,while suburban sites were more impacted by coal and biomass burning.On polluted days,traffic sources’contributions increased significantly at HC,YNE,NG and YNCE sites,and secondary formation sources’contributions grew at CTV and YNCE sites.The sourcedependent BaPeq results underscored the role of secondary-formed PAH derivatives in TEQ.展开更多
Nitrated polycyclic aromatic hydrocarbons(NPAHs)have toxic potentials that are higher than those of their corresponding parent polycyclic aromatic hydrocarbons(PAHs)and thus have received increasing attention in recen...Nitrated polycyclic aromatic hydrocarbons(NPAHs)have toxic potentials that are higher than those of their corresponding parent polycyclic aromatic hydrocarbons(PAHs)and thus have received increasing attention in recent years.In this study,the occurrence,distribution,source,and human health risk assessment of 15 NPAHs and 16 PAHs were investigated in the surface water from 20 sampling sites of Lake Taihu during the dry,normal,and flood seasons of 2018.The PAH concentrations ranged from 255 to 7298 ng/L and the NPAH concentrations ranged from not-detected(ND)to 212 ng/L.Among the target analytes,2-nitrofluorene(2-n Flu)was the predominant NPAH,with a detection frequency ranging from 85%to 90%and a maximum concentration of 56.2 ng/L.The three-ringed and four-ringed NPAHs and PAHs comprised the majority of the detected compounds.In terms of seasonal variation,the highest levels of the NPAHs and PAHs were in the dry season and flood season,respectively.Diagnostic ratio analysis indicated that the prime source of NPAHs was direct combustion,whereas in the case of PAHs the contribution was predominantly from a mixed pattern including pollution from unburned petroleum and petroleum combustion.The human health risk of NPAHs and PAHs was evaluated using a lifetime carcinogenic risk assessment model.The carcinogenic risk level of the targets ranged from 2.09×10^(-7)to 5.75×10^(-5)and some surface water samples posed a potential health risk.展开更多
Polycyclic aromatic hydrocarbons(PAHs)and their nitrated derivatives(NPAHs)attract continuous attention due to their outstanding carcinogenicity and mutagenicity.In order to investigate the diurnal variations,sources,...Polycyclic aromatic hydrocarbons(PAHs)and their nitrated derivatives(NPAHs)attract continuous attention due to their outstanding carcinogenicity and mutagenicity.In order to investigate the diurnal variations,sources,formation mechanism,and health risk assessment of them in heating season,particulate matter(PM)were collected in Beijing urban area from December 26,2017 to January 17,2018.PAHs and NPAHs in PM were quantitatively analyzed via gas chromatography-mass spectrometry(GC-MS).Average daily concentrations of PAHs and NPAHs were(78±54)ng/m^(3)and(783±684)pg/m^(3),respectively.The concentrations of them were significantly higher at nighttime than at daytime,and NPAHs concentrations were 1-2 orders of magnitude lower than PAHs concentrations.In the heating season,the dominant species of PAHs include benzo[b]fluoranthene,fluoranthene,pyrene,and chrysene,while 9-nitroanthracene,2+3-nitrofluoranthene,and 2-nitropyrene were dominant species for NPAHs.NPAHs were found to have a single peak during heating and to be primarily distributed in the 0.4-0.7μm particle size.Primary emissions such as biomass burning,coal combustion,and traffic emissions were the major sources of PAHs.NPAHs were produced by the primary source of vehicle emissions and the secondary reaction triggered by OH radicals,as well as biomass burning during daytime.According to the health risk assessment,the total carcinogenic risk was higher in adults than in children.While upon oral ingestion,the carcinogenic risk in children was higher than that of adults,but the risk of adults was higher than children through skin contact and respiratory inhalation.展开更多
Intensive daytime and nighttime sampling was carried out from 23 Oct to 31 Dec 2008 to investigate the occurrence of nitrated polycyclic aromatic hydrocarbons （NPAHs） in PM1o at a roadside site in Xiamen, China. At ...Intensive daytime and nighttime sampling was carried out from 23 Oct to 31 Dec 2008 to investigate the occurrence of nitrated polycyclic aromatic hydrocarbons （NPAHs） in PM1o at a roadside site in Xiamen, China. At the same time, six PMt0 samples were collected from a nearby roadway tunnel for comparison. Six NPAHs, namely 9-nitroanthracene, 2- and 3-nitrofluoranthene, 1- nitropyrene, 7-nitrobenz[a]anthracene, and 6-nitrobenzo[a]pyrene, were identified and quantified using GC/MS in negative ion chemical ionization mode. The average total concentration of six NPAHs （~NPAHs） in the cold season （26 Nov-31 Dec） was 2.3 （daytime） and 9.9 （nighttime） times higher than those in the warm season. Significant statistical difference （p 〈 0.01, 2-tailed） of ∑NPAHs between daytime and nighttime was found during both the warm and cold seasons. NPAHs were significantly positively correlated with their parent PAHs and nitrogen dioxide but negatively correlated with ambient temperature. The ratio of 2 ＋ 3-nitrofluoranthene to 1- nitropyrene exhibited a similar diurnal pattern as ZNPAHs and was generally greater than 5, indicating the importance of secondary atmospheric formation. The diurnal variations of NPAHs were all influenced by the diurnal variations of PAHs, nitrogen dioxide, sunlight, and temperature. The daily inhalable exposure to the six NPAHs in the tunnel was much higher than the roadside values in the warm season but only slightly higher than those in the cold season.展开更多
Air pollutants can potentially lead to nitration of allergic proteins,thus promoting sensitization of these allergens.However,little is currently known about the nitration status of house dust mite(HDM)allergens.We id...Air pollutants can potentially lead to nitration of allergic proteins,thus promoting sensitization of these allergens.However,little is currently known about the nitration status of house dust mite(HDM)allergens.We identified the occurrence of nitrated products of two major HDM allergens Der f 1 and Der p 1 in dust samples collected from college dormitories in eastern China and assessed their associated health risk.The results showed that both non-nitrated and nitrated forms of the two allergens were detected in the dust in the range of non-detected(ND)-10.6,1.44-15.4,ND-22.4,ND-7.28μg/g for non-nitrated Der f 1,nitrated Der f 1,non-nitrated Der p 1 and nitrated Der p 1,respectively.The median rates of nitration were determined as 74.0%for Der f 1 and 20.4% for Der p 1 at consideration of one nitration site.Further analysis reveals that the levels of HDM allergens and their nitrated products were found to be generally higher during winter,in dormitories of lower altitude and with female occupants.Furthermore,the calculated risk indexes were at considerably high levels.Our findings suggest that nitrated HDM allergens have already accumulated in the environment at such significant levels and their associated health risk calls for our immediate attention.展开更多
Although previous studies have demonstrated the involvement of nitrated a-synuclein in neurodegenerative disorders(synucleinopathies),the effects of nitrated α-synuclein and the molecular mechanisms underlying its t...Although previous studies have demonstrated the involvement of nitrated a-synuclein in neurodegenerative disorders(synucleinopathies),the effects of nitrated α-synuclein and the molecular mechanisms underlying its toxicity are still unclear.In the present study,nitrated α-synuclein with four 3-nitrotyrosines(Tyr^(39),Tyr^(125),Tyr^(133),and Tyr^(136))was obtained non-enzymatically by incubation with nitrite.The nitrated protein existed as a mixture of monomers,dimers,and polymers in solution.The nitrated a-synuclein could induce cell death in a time-and concentration-dependent manner when SH-SY5Y cells(a human neuroblastoma cell line)were incubated with the dimers and polymers.Treatment with anti-integrin α5β1 antibody partially rescued the SH-SY5Y cells from the cell death.Dot blotting and immunoprecipitation revealed that the nitrated protein bound to integrin on the cell membranes.Level of nitric oxide(NO)and calcium-independent inducible NO synthase(iNOS)activity increased during the initial stages of the treatment.The expression of phosphorylated focal adhesion kinase(FAK)decreased in the cells.Subsequently,an increase in caspase 3 activity was observed in SH-SY5Y cells.Our results demonstrate that activation of iNOS and inhibition of FAK may both be responsible for the cell death induced by nitrated α-synuclein.These data suggest that the cytotoxicity of nitrated a-synuclein is mediated via an integrin-iNOS/-FAK signaling pathway,and that the nitration of α-synuclein plays a role in neuronal degeneration.展开更多
The present work aims to stabilize the room temperature allotropic transition of ammonium nitrate(AN)particles utilizing a microencapsulation technique,which involves solvent/non-solvent in which nitrocellulose(NC)has...The present work aims to stabilize the room temperature allotropic transition of ammonium nitrate(AN)particles utilizing a microencapsulation technique,which involves solvent/non-solvent in which nitrocellulose(NC)has been employed as a coating agent.The SEM micrographs revealed distinct features of both pure AN and NC,contrasting with the irregular granular surface topography of the coated AN particles,demonstrating the adherence of NC on the AN surface.Structural analysis via infrared spectroscopy(IR)demonstrated a successful association of AN and NC,with slight shifts observed in IR bands indicating interfacial interactions.Powder X-ray Diffraction(PXRD)analysis further elucidated the structural changes induced by the coating process,revealing that the NC coating altered the crystallization pattern of its pure form.Thermal analysis demonstrates distinct profiles for pure and coated AN,for which the coated sample exhibits a temperature increase and an enthalpy decrease of the room temperature allotropic transition by 6℃,and 36%,respectively.Furthermore,the presence of NC coating alters the intermolecular forces within the composite system,leading to a reduction in melting enthalpy of coated AN by~39%compared to pure AN.The thermal decomposition analysis shows a two-step thermolysis process for coated AN,with a significant increase in the released heat by about 78%accompanied by an increase in the activation barrier of NC and AN thermolysis,demonstrating a stabilized reactivity of the AN-NC particles.These findings highlight the synergistic effect of NC coating on AN particles,which contributed to a structural and reactive stabilization of both AN and NC,proving the potential application of NC-coated AN as a strategically advantageous oxidizer in composite solid propellant formulations.展开更多
Ammonia is the cornerstone of modern agriculture,providing a critical nitrogen source for global food production and serving as a key raw material for numerous industrial chemicals.Electrocatalytic nitrate reduction,a...Ammonia is the cornerstone of modern agriculture,providing a critical nitrogen source for global food production and serving as a key raw material for numerous industrial chemicals.Electrocatalytic nitrate reduction,as an environmentally friendly method for synthesizing ammonia,not only mitigates the reliance on current ammonia synthesis processes fed by traditional fossil fuels but also effectively reduces nitrate pollution resulting from agricultural and industrial activities.This review explores the fundamental principles of electrocata lytic nitrate reduction,focusing on the key steps of electron transfer and ammonia formation.Additionally,it summarizes the critical factors influencing the performance and selectivity of the reaction,including the properties of the electrolyte,operating voltage,electrode materials,and design of the electrolytic cell.Further discussion of recent advances in electrocatalysts,including pure metal catalysts,metal oxide catalysts,non-metallic catalysts,and composite catalysts,highlights their significant roles in enhancing both the efficiency and selectivity of electrocata lytic nitrate to ammonia(NRA)reactions.Critical challenges for the industrial NRA trials and further outlooks are outlined to propel this strategy toward real-world applications.Overall,the review provides an in-depth overview and comprehensive understanding of electrocata lytic NRA technology,thereby promoting further advancements and innovations in this domain.展开更多
Nitrate contamination of groundwater is a worldwide problem, particularly in agricultural countries. Exposure to high levels of nitrates in groundwater can have adverse effects on the health of residents who use groun...Nitrate contamination of groundwater is a worldwide problem, particularly in agricultural countries. Exposure to high levels of nitrates in groundwater can have adverse effects on the health of residents who use groundwater for drinking. This study aims to assess the health risk associated with the ingestion of nitrates in well water in the town of M’bahiakro. Health risk maps were created on the basis of hazard quotients (HQ) using the US Environmental Protection Agency (USEPA) health risk assessment model. The results indicate that residents of the Koko, Dougouba and Baoulekro neighbourhoods, whatever their age, are potentially exposed to the toxic effects of NO3−during their daily intake of nitrate-contaminated well water, with reference to hazard quotients (HQ) greater than 1. Nitrate concentrations in the groundwater should therefore be controlled in order to prevent their harmful effects on the health of the population and guarantee its use in rice-growing activities in M’Bahiakro.展开更多
Electrocatalytic nitrate reduction reaction (NO_(3)-RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution issues.We report a CuO nanoparticles in...Electrocatalytic nitrate reduction reaction (NO_(3)-RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution issues.We report a CuO nanoparticles incorporated on nitrogen-doped porous carbon (CuO@NC) catalyst for NO_(3)-RR.Part of Cu(Ⅱ) is reduced to Cu(Ⅰ) during the NO_(3)-RR process to construct Cu(Ⅰ)-Cu(Ⅱ) pairs,confirmed by in situ X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy.Density functional theory (DFT) calculations indicated that the formation of Cu(Ⅰ) could provide a reaction path with smaller energy barrier for NO_(3)-RR,while Cu(Ⅱ) effectively suppressed the competition of hydrogen evolution reaction (HER).As a result,CuO@NC catalyst achieved a Faradaic efficiency of 84.2% at -0.49 V versus reversible hydrogen electrode (RHE),and a NH_(3)yield rate of 17.2 mg h^(-1)mg^(-1)cat.at -0.79 V vs.RHE,higher than the HaberBosch process (<3.4 g h^(-1)g^(-1)cat.).This work may open a new avenue for effective NO_(3)-RR by modulating oxidation states.展开更多
Scientific knowledge on the chemical compositions of fine particulate matter(PM_(2.5)) is essential for properly assessing its health and climate effects,and for decisionmakers to develop efficient mitigation strategi...Scientific knowledge on the chemical compositions of fine particulate matter(PM_(2.5)) is essential for properly assessing its health and climate effects,and for decisionmakers to develop efficient mitigation strategies.A high-resolution PM_(2.5) chemical composition dataset(CAQRA-aerosol)is developed in this study,which provides hourly maps of organic carbon,black carbon,ammonium,nitrate,and sulfate in China from 2013 to 2020 with a horizontal resolution of 15 km.This paper describes the method,access,and validation results of this dataset.It shows that CAQRA-aerosol has good consistency with observations and achieves higher or comparable accuracy with previous PM_(2.5) composition datasets.Based on CAQRA-aerosol,spatiotemporal changes of different PM_(2.5) compositions were investigated from a national viewpoint,which emphasizes different changes of nitrate from other compositions.The estimated annual rate of population-weighted concentrations of nitrate is 0.23μg m^(−3)yr^(−1) from 2015 to 2020,compared with−0.19 to−1.1μg m^(−3)yr^(−1) for other compositions.The whole dataset is freely available from the China Air Pollution Data Center(https://doi.org/10.12423/capdb_PKU.2023.DA).展开更多
The electrochemical conversion of nitrate,a widespread water pollutant,into valuable ammonia represents a green and decentralized approach to ammonia synthesis.However,the sluggish multielectronproton coupling path an...The electrochemical conversion of nitrate,a widespread water pollutant,into valuable ammonia represents a green and decentralized approach to ammonia synthesis.However,the sluggish multielectronproton coupling path and the low reactive species(nitrate and proton)concentration at the catalyst interface inhibit the efficiency of ammonia production from nitrate reduction reaction(NitRR).Herein,we introduce a novel iron-based tandem catalyst encapsulated by reduced graphene oxide(denoted as Fe-rGO),with a superior ammonia production rate of 47.815 mg h^(-1)mg_(ca)^(t-1)and a high Faraday efficiency(FE)of 96.51%at an applied potential of-0.5 V.It also delivers a robust stability with FE above90%under a current density of 250 mA cm^(-2)for 50 h.In situ X-ray absorption spectroscopy reveals that the FeO_(x)is dynamically translated to Fe~0 site concurrently with the enhancement of the NH_(3)production rate,suggesting the Fe^(0) site as hydrogenation active center.The asymmetric distribution of surface charges of rGO not only enriches nitrate ions at the catalytic interface and promotes the hydrogenation process in NitRR,but also protects the iron species and ensures their stability during electrolysis.The Zn-NO_(3)^(-)battery demonstrates an impressive FE of 88.6%,highlighting its exceptional potential for practical applications.展开更多
Nitrogen(N)uptake is regulated by water availability,and a water deficit can limit crop N responses by reducing N uptake and utilization.The complex and multifaceted interplay between water availability and the crop N...Nitrogen(N)uptake is regulated by water availability,and a water deficit can limit crop N responses by reducing N uptake and utilization.The complex and multifaceted interplay between water availability and the crop N response makes it difficult to predict and quantify the effect of water deficit on crop N status.The nitrogen nutrition index(NNI)has been widely used to accurately diagnose crop N status and to evaluate the effectiveness of N application.The decline of NNI under water-limiting conditions has been documented,although the underlying mechanism governing this decline is not fully understood.This study aimed to elucidate the reason for the decline of NNI under waterlimiting conditions and to provide insights into the accurate utilization of NNI for assessing crop N status under different water-N interaction treatments.Rainout shelter experiments were conducted over three growing seasons from 2018 to 2021 under different N(75 and 225 kg N ha^(-1),low N and high N)and water(120 to 510 mm,W0 to W3)co-limitation treatments.Plant N accumulation,shoot biomass(SB),plant N concentration(%N),soil nitrate-N content,actual evapotranspiration(ET_a),and yield were recorded at the stem elongation,booting,anthesis and grain filling stages.Compared to W0,W1 to W3 treatments exhibited NNI values that were greater by 10.2 to 20.5%,12.6to 24.8%,14 to 24.8%,and 16.8 to 24.8%at stem elongation,booting,anthesis,and grain filling,respectively,across the 2018-2021 seasons.This decline in NNI under water-limiting conditions stemmed from two main factors.First,reduced ET_(a) and SB led to a greater critical N concentration(%N_(c))under water-limiting conditions,which contributed to the decline in NNI primarily under high N conditions.Second,changes in plant%N played a more significant role under low N conditions.Plant N accumulation exhibited a positive allometric relationship with SB and a negative relationship with soil nitrate-N content under water-limiting conditions,indicating co-regulation by SB and the soil nitrate-N content.However,this regulation was influenced by water availability.Plant N accumulation sourced from the soil nitrate-N content reflects soil N availability.Greater soil water availability facilitated greater absorption of soil nitrate-N into the plants,leading to a positive correlation between plant N accumulation and ET_(a)across the different water-N interaction treatments.Therefore,considering the impact of soil water availability is crucial when assessing soil N availability under water-limiting conditions.The findings of this study provide valuable insights into the factors contributing to the decline in NNI among different water-N interaction treatments and can contribute to the more accurate utilization of NNI for assessing winter wheat N status.展开更多
The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation ...The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation and oxygen evolution competition,sluggish kinetics,low Faradaic efficiency,and limited nitrate yields.In this work,a novel two-dimensional(2D)layered MOF Mn-BCPPy(H_(2)BCPPy=3,5-di(4'-carboxyphenyl)pyridine)has been successfully synthesized.The framework is composed of a rod-manganese motifs and possesses abundant active sites including open metal sites(OMSs)and Lewis base sites(LBSs).The Mn-BCPPy is the first MOF catalyst applied in electrocatalytic NOR which NO_(3)^(-)exhibited relatively high activity with a yield of 99.75μg/(h·mg)and a Faraday efficiency(FE)of 32.09%.Furthermore,it can be used as fluorescent sensor for selectively and sensitively detect nitrofuran antibiotics(NFs).Therefore,this work explores the application of MOF materials in the field of electrocatalytic NOR,which reveals that manganese-based MOFs have great potential prospects.展开更多
A static corrosion experiment of 347H stainless steel alloyed with elements Cu and Mo was carried out in a nitrate molten salt(60%NaNO_(3)+40%KNO_(3))at 565℃ for 720 h.The effects of elements Cu and Mo on the corrosi...A static corrosion experiment of 347H stainless steel alloyed with elements Cu and Mo was carried out in a nitrate molten salt(60%NaNO_(3)+40%KNO_(3))at 565℃ for 720 h.The effects of elements Cu and Mo on the corrosion resistance of 347H stainless steel in molten salt were investigated by analyzing the phase composition,microstructure and chemical composition of the corrosion products.The results show that the grain refinement induced by element Mo imparts the stainless steel with optimal corrosion resistance at a medium grain size.Furthermore,the formation of MoC significantly enhances the intergranular corrosion resistance of the stainless steel.The stainless steel exhibits uniform corrosion in the nitrate solution.The corrosion layer displays a dual-layer structure,and the corrosion products protecting matrix are present in both the inner and outer layers.The outer layer consists of a mixture of Fe oxides(Fe_(2)O_(3),Fe_(3)O_(4)),NaFeO_(2),and a minor amount of MgFe_(2)O_(4).Conversely,the inner layer is primarily composed of a spinel layer(FeCr_(2)O_(4),MgCr_(2)O_(4))and a thin Cu_(2)O layer.The oxidation of Cu in the inner layer leads to the formation of a dense Cu_(2)O layer,effectively impeding O_(2)-plasma infiltration into the matrix.展开更多
Nitrate is the primary nitrogen source for plants and is a signaling molecule regulating various plant developmental processes. Despite its significance, limited information is available on nitrate signaling in Vitis ...Nitrate is the primary nitrogen source for plants and is a signaling molecule regulating various plant developmental processes. Despite its significance, limited information is available on nitrate signaling in Vitis vinifera. We identified nine Vv RWP-RK genes distributed across eight chromosomes using genome-wide identification and evolutionary analyses. Among these, Vv NLP1-4 and Vv RKD1-5 are associated with nitrate signaling and reproductive growth, respectively. To investigate their potential functions, structures, cis-acting promoter elements,functional structural domains, phylogenetic trees, spatiotemporal expression levels in different tissues at different developmental stages,potential protein-protein interaction networks, synteny(gene content), collinearity(gene order), and three-dimensional protein structure prediction were explored. We found that long-term nitrate application dramatically promoted grapevine plantlet development, including primary root length and leaf growth, and Vv NLP1.1, Vv NLP1.2, and Vv NLP2 were highly expressed in ‘Thompson Seedless' root tissues under nitrate-enriched conditions. To clarify the critical role of nitrate in grapevine growth, we observed that nuclear localization of Vv NLP1.1increased significantly following nitrate treatment. Vv NLP1.1 was found to bind to the promoter of the primary nitrate response gene Vv NRT1.1,driving its transcriptional activity. These findings indicate that Vv NLP1.1 is a core transcription factor of the nitrate signaling pathway in grapevine. Nitrate molecular docking analysis revealed that Vv NLP1.1 directly binds to nitrate ions, indicating its potential role as a nitrate sensor capable of directly perceiving nitrate concentration. We also discovered that short-term nitrate starvation impacts Vv NLP1.1 promoter activity, linked to the abscisic acid-binding element(ABRE) motif in its promoter region. Our results thus provide new insights into the molecular mechanisms underlying various physiological processes in grapevine, particularly the nitrate signaling pathway, and provide a theoretical basis for improving nitrogen use efficiency(NUE) in grapevine.展开更多
Tyrosine residues in proteins can be nitrated to form 3-nitrotyrosine(3-NT)under the influence of ozone(O_(3))and nitrogen dioxide(NO_(2))in the air,which may introduce health impacts.A selective and sensitive enzyme-...Tyrosine residues in proteins can be nitrated to form 3-nitrotyrosine(3-NT)under the influence of ozone(O_(3))and nitrogen dioxide(NO_(2))in the air,which may introduce health impacts.A selective and sensitive enzyme-linked-immunoassay(ELISA)method was developed to determine 3-NT in modified model protein(bovine serum albumin,BSA)and ambient aerosol samples.The nitration degrees(NDs)of BSA in the exposure experiments with different durations were detected by both the ELISA and spectrophotometric methods(i.e.,ND_(ELISA) and ND_(SEC-PDA)),which show good coincidence.The kinetic investigation by both ΔND_(ELISA) and ΔND_(SEC-PDA) in the exposure experiments shows that the rate coefficients(k)of the pseudo-first-order kinetic rate reactions of protein nitration were comparable.These results indicate that direct detection of 3-NT by the ELISA method can be applied for laboratory exposure samples analysis for kinetic studies.Based on the selective detection of 3-NT,ND_(ELISA) provides a promising measure for the assessment of ND in model proteins.3-NT was alsomeasured in PM_(2.5) samples in summer in Guangzhou,southern China,ranging from 10.1 to 404 pg/m^(3),providing clear evidence of protein nitration in ambient aerosols.We further proposed that 3-NT/protein can be used as a proxy to evaluate protein nitration in ambient aerosols.A significant correlationwas observed between 3-NT/protein and O_(3),confirming the crucial role of O_(3) in protein nitration.Our results show that the direct detection of 3-NT by the ELISA method can be more widely applied in the laboratory and field-based studies for understanding the mechanisms of protein nitration.展开更多
The enrichment of low-grade phosphate rock is an important process to realize sustainable support of phosphorus resources. An aqueous solution containing Ca(NO_(3))_(2) and Mg(NO_(3))_(2) is produced during the enrich...The enrichment of low-grade phosphate rock is an important process to realize sustainable support of phosphorus resources. An aqueous solution containing Ca(NO_(3))_(2) and Mg(NO_(3))_(2) is produced during the enrichment of low-grade phosphate rock by leaching of HNO_(3) or calcination coupling with leaching of NH_(4)NO_(3) solution. Preparation liquid fertilizer is a preferential way to utilize it. The liquid−solid phase diagrams of Ca(NO_(3))_(2)-Mg(NO_(3))_(2)-H_(2)O, KNO_(3)-Mg(NO_(3))_(2)-H_(2)O, KNO_(3)-Ca(NO_(3))_(2)-H_(2)O and KNO_(3)-Ca(NO_(3))_(2)-Mg(NO_(3))_(2)-H_(2)O systems at 313.15 K were studied by isothermal dissolution equilibrium method. Two crystallization regions of Ca(NO_(3))_(2)·4H_(2)O and Mg(NO_(3))_(2)·6H_(2)O were observed in the phase diagram of the ternary system Ca(NO_(3))_(2)-Mg(NO_(3))_(2)-H_(2)O, a liquid fertilizer with a maximal total nutrient content of 27.46% and a nutrients ratio of N:Ca:Mg = 8.40:10.37:1 can be formed. A homogenous solution can be formed by mixing Ca(NO_(3))_(2)·4H_(2)O and Mg(NO_(3))_(2)·6H_(2)O. In the ternary system KNO_(3)-Mg(NO_(3))_(2)-H_(2)O, the crystallization regions of KNO_(3), Mg(NO_(3))_(2)·6H_(2)O and the co-crystallization region of KNO_(3) and Mg(NO_(3))_(2)·6H_(2)O were observed. The obtained maximal total nutrient content of liquid fertilizer is 23.32% with the ratio of N:K_(2)O = 1:3.39. In the ternary system KNO_(3)-Ca(NO_(3))_(2)-H_(2)O, the crystallization regions of Ca(NO_(3))_(2)·4H_(2)O and KNO_(3) were observed. The obtained maximal total nutrient content of liquid fertilizer is 38.41% with the ratio of N:K_(2)O:Ca = 1.05:1.18:1. A homogenous solution can also be formed by mixing Ca(NO_(3))_(2)·4H_(2)O and KNO_(3) directly. In the quaternary system KNO_(3)-Ca(NO_(3))_(2)-Mg(NO_(3))_(2)-H_(2)O, the crystallization regions of Ca(NO_(3))_(2)·4H_(2)O, Mg(NO_(3))_(2)·6H_(2)O and KNO_(3) and the co-crystallization region of KNO_(3) and Mg(NO_(3))_(2)·6H_(2)O were observed. The obtained maximal total nutrient content of liquid fertilizer is 38.41% with the ratio of N:K_(2)O:Ca = 1.05:1.18:1. The modified BET model was successfully used to fit the solubility curves. The results can provide a guidance for the formulation of water-soluble fertilizers of N-(K, Ca, Mg).展开更多
Cyclotella cryptica,a model diatom known for its robust adaptability to variable salinity and temperature conditions,is a promising candidate for large-scale biotechnological applications.Nutrient availability,particu...Cyclotella cryptica,a model diatom known for its robust adaptability to variable salinity and temperature conditions,is a promising candidate for large-scale biotechnological applications.Nutrient availability,particularly nitrogen and phosphorus,plays a crucial role in the metabolic activities of microalgae,influencing its industrial utility.Exploring the relationship between these essential nutrients and both the yield and biochemical composition of this microalga is crucial for optimizing cultivation strategies.However,research focusing on the effects of nitrogen and phosphorus on C.cryptica remains limited.We investigated the impacts of varying concentrations of nitrate(0.25-3.96 mmol/L)and phosphate(14.4-229.6μmol/L)on C.cryptica culture by analyzing its growth performance,photosynthetic activity,biochemical composition,and biosilica deposition.Results indicate that C.cryptica exhibited enhanced growth,photosynthetic efficiency,and carotenoid production under higher nutrient concentrations.However,the effects of nitrate on macronutrients composition and fatty acids profile differed from those of phosphate.Specifically,increased nitrate levels resulted in higher concentrations of polyunsaturated fatty acids(PUFAs)at the expense of saturated fatty acids(SFAs),while increased phosphate levels were associated with increased PUFAs and reduced monounsaturated fatty acids(MUFAs).Additionally,biosilica deposition was weakened by elevated nitrate but enhanced by increased phosphate levels.This study improved our understanding of nutrient-mediated regulatory mechanisms in diatoms and contributed valuable data to the broader field of algal biotechnology.Moreover,these findings are expected to advance the development of tailored nutrient management strategies,thereby enhancing the industrial potential of C.cryptica.展开更多
A novel Cu-t-ZrO_(2)catalyst with enhanced electronic metal-support interaction(EMSI)is designed for efficient electrocatalytic conversion of nitrate(NO_(3^(-)))to ammonia(NH_(3)),achieving a remarkable Faradaic effic...A novel Cu-t-ZrO_(2)catalyst with enhanced electronic metal-support interaction(EMSI)is designed for efficient electrocatalytic conversion of nitrate(NO_(3^(-)))to ammonia(NH_(3)),achieving a remarkable Faradaic efficiency and yield rate of 97.54%and 33.64 mg h^(-1)mg_(cat)^(-1),respectively.Electrons are more likely to be transferred from Cu to t-ZrO_(2)at the electron-rich interface due to the lower work function,which promotes the formation of highly active Cu species and facilitates NO_(3^(-))adsorption,ensuring selective conversion into NH_(3).展开更多
基金supported by the National Key R&D Program of China(No.2017YFC0212501)the Fundamental Research Funds for the Central Universities(No.2021YJSMT09)the research project on deep source apportionment of urban air pollution and pollution control strategies in the core area of the Ili River Valley。
文摘Polycyclic Aromatic Hydrocarbons(PAHs),along with their derivatives nitro-PAHs and oxy-PAHs,are globally recognized toxic pollutants.This research conducted daily PM_(2.5)sampling in winter 2021 at three urban(YNCE,SWP,and NG)and three suburban sites(HC,CTV,and YNE)in the Ili River Valley(IRV).For the first time in the IRV,a comprehensive study on 39 PAHs and derivatives was carried out.The results showed that the average∑_(16)PAHs concentration was 130.21±98.94 ng/m^(3),with 16PAHs constituting the dominant fraction(112.51±86.48 ng/m^(3)).The mean BaP and the total BaP equivalent quotient(TEQ)concentrations were 10.28±8.85 ng/m^(3)and 19.74±16.70 ng/m^(3),respectively.Approximately 88%of the daily BaP averages and 98%of the daily TEQ averages exceeded the national daily average standard of BaP(2.5 ng/m^(3)),indicating severe local BaP pollution.Urban sites had notably higher∑PAHs and TEQ concentrations than suburban sites,attributed to increased vehicular traffic and coal combustion in urban areas.PMF results showed that traffic emissions(32.7%-60.5%),coal combustion(13.9%-24.3%)and secondary formation(14.7%-22.7%)were the primary contributors to∑PAHs.Urban sites experienced a greater influence from traffic,while suburban sites were more impacted by coal and biomass burning.On polluted days,traffic sources’contributions increased significantly at HC,YNE,NG and YNCE sites,and secondary formation sources’contributions grew at CTV and YNCE sites.The sourcedependent BaPeq results underscored the role of secondary-formed PAH derivatives in TEQ.
基金supported by the National Natural Science Foundation of China(No.41671493)the State Key Laboratory of Pollution Control and Resource Reuse Foundation(No.PCRRF17030)the National Major Project of the Science and Technology Ministry of China(No.2017ZX07202-004 and 2017X07301002-3)。
文摘Nitrated polycyclic aromatic hydrocarbons(NPAHs)have toxic potentials that are higher than those of their corresponding parent polycyclic aromatic hydrocarbons(PAHs)and thus have received increasing attention in recent years.In this study,the occurrence,distribution,source,and human health risk assessment of 15 NPAHs and 16 PAHs were investigated in the surface water from 20 sampling sites of Lake Taihu during the dry,normal,and flood seasons of 2018.The PAH concentrations ranged from 255 to 7298 ng/L and the NPAH concentrations ranged from not-detected(ND)to 212 ng/L.Among the target analytes,2-nitrofluorene(2-n Flu)was the predominant NPAH,with a detection frequency ranging from 85%to 90%and a maximum concentration of 56.2 ng/L.The three-ringed and four-ringed NPAHs and PAHs comprised the majority of the detected compounds.In terms of seasonal variation,the highest levels of the NPAHs and PAHs were in the dry season and flood season,respectively.Diagnostic ratio analysis indicated that the prime source of NPAHs was direct combustion,whereas in the case of PAHs the contribution was predominantly from a mixed pattern including pollution from unburned petroleum and petroleum combustion.The human health risk of NPAHs and PAHs was evaluated using a lifetime carcinogenic risk assessment model.The carcinogenic risk level of the targets ranged from 2.09×10^(-7)to 5.75×10^(-5)and some surface water samples posed a potential health risk.
基金supported by the National Natural Science Foundation of China(No.41907197)the Fundamental Research Funds for Central Public Welfare Scientific Research Institutes of China,Chinese Research Academy of Environmental Sciences(No.2019YSKY-018)+1 种基金the National Key R&D Program of China(No.2019YFC0214800)the Standard System and Key Standards Research of National Ecological Environment Protection and Risk Prevention(No.2020YFC18063)。
文摘Polycyclic aromatic hydrocarbons(PAHs)and their nitrated derivatives(NPAHs)attract continuous attention due to their outstanding carcinogenicity and mutagenicity.In order to investigate the diurnal variations,sources,formation mechanism,and health risk assessment of them in heating season,particulate matter(PM)were collected in Beijing urban area from December 26,2017 to January 17,2018.PAHs and NPAHs in PM were quantitatively analyzed via gas chromatography-mass spectrometry(GC-MS).Average daily concentrations of PAHs and NPAHs were(78±54)ng/m^(3)and(783±684)pg/m^(3),respectively.The concentrations of them were significantly higher at nighttime than at daytime,and NPAHs concentrations were 1-2 orders of magnitude lower than PAHs concentrations.In the heating season,the dominant species of PAHs include benzo[b]fluoranthene,fluoranthene,pyrene,and chrysene,while 9-nitroanthracene,2+3-nitrofluoranthene,and 2-nitropyrene were dominant species for NPAHs.NPAHs were found to have a single peak during heating and to be primarily distributed in the 0.4-0.7μm particle size.Primary emissions such as biomass burning,coal combustion,and traffic emissions were the major sources of PAHs.NPAHs were produced by the primary source of vehicle emissions and the secondary reaction triggered by OH radicals,as well as biomass burning during daytime.According to the health risk assessment,the total carcinogenic risk was higher in adults than in children.While upon oral ingestion,the carcinogenic risk in children was higher than that of adults,but the risk of adults was higher than children through skin contact and respiratory inhalation.
基金supported by the National Natural Science Foundation of China (No. 40971257,41171365)the Environmental Nonprofit Research and Special Project of China (No. 201009004)the Program for Changjiang Scholars and Innovative Research Team in University (No.IRT0941)
文摘Intensive daytime and nighttime sampling was carried out from 23 Oct to 31 Dec 2008 to investigate the occurrence of nitrated polycyclic aromatic hydrocarbons （NPAHs） in PM1o at a roadside site in Xiamen, China. At the same time, six PMt0 samples were collected from a nearby roadway tunnel for comparison. Six NPAHs, namely 9-nitroanthracene, 2- and 3-nitrofluoranthene, 1- nitropyrene, 7-nitrobenz[a]anthracene, and 6-nitrobenzo[a]pyrene, were identified and quantified using GC/MS in negative ion chemical ionization mode. The average total concentration of six NPAHs （~NPAHs） in the cold season （26 Nov-31 Dec） was 2.3 （daytime） and 9.9 （nighttime） times higher than those in the warm season. Significant statistical difference （p 〈 0.01, 2-tailed） of ∑NPAHs between daytime and nighttime was found during both the warm and cold seasons. NPAHs were significantly positively correlated with their parent PAHs and nitrogen dioxide but negatively correlated with ambient temperature. The ratio of 2 ＋ 3-nitrofluoranthene to 1- nitropyrene exhibited a similar diurnal pattern as ZNPAHs and was generally greater than 5, indicating the importance of secondary atmospheric formation. The diurnal variations of NPAHs were all influenced by the diurnal variations of PAHs, nitrogen dioxide, sunlight, and temperature. The daily inhalable exposure to the six NPAHs in the tunnel was much higher than the roadside values in the warm season but only slightly higher than those in the cold season.
基金financially supported by the National Natural Science Foundation of China (No. 41977341)Natural Science Foundation of Zhejiang Province, China (No. LGF21B070007)Research Center for Air Pollution and Health, Zhejiang University (No. I21405-11)
文摘Air pollutants can potentially lead to nitration of allergic proteins,thus promoting sensitization of these allergens.However,little is currently known about the nitration status of house dust mite(HDM)allergens.We identified the occurrence of nitrated products of two major HDM allergens Der f 1 and Der p 1 in dust samples collected from college dormitories in eastern China and assessed their associated health risk.The results showed that both non-nitrated and nitrated forms of the two allergens were detected in the dust in the range of non-detected(ND)-10.6,1.44-15.4,ND-22.4,ND-7.28μg/g for non-nitrated Der f 1,nitrated Der f 1,non-nitrated Der p 1 and nitrated Der p 1,respectively.The median rates of nitration were determined as 74.0%for Der f 1 and 20.4% for Der p 1 at consideration of one nitration site.Further analysis reveals that the levels of HDM allergens and their nitrated products were found to be generally higher during winter,in dormitories of lower altitude and with female occupants.Furthermore,the calculated risk indexes were at considerably high levels.Our findings suggest that nitrated HDM allergens have already accumulated in the environment at such significant levels and their associated health risk calls for our immediate attention.
基金supported by the grants from the China Postdoctoral Science Foundation(20070410153,200801120)the National Science Foundation of China(30970695)+1 种基金the Major State Basic Research Development Program of China(973 Program)(2010CB912303)the Chinese Academy of Sciences(KSCX2-YW-R-119,KSCX2-YW-R-256).
文摘Although previous studies have demonstrated the involvement of nitrated a-synuclein in neurodegenerative disorders(synucleinopathies),the effects of nitrated α-synuclein and the molecular mechanisms underlying its toxicity are still unclear.In the present study,nitrated α-synuclein with four 3-nitrotyrosines(Tyr^(39),Tyr^(125),Tyr^(133),and Tyr^(136))was obtained non-enzymatically by incubation with nitrite.The nitrated protein existed as a mixture of monomers,dimers,and polymers in solution.The nitrated a-synuclein could induce cell death in a time-and concentration-dependent manner when SH-SY5Y cells(a human neuroblastoma cell line)were incubated with the dimers and polymers.Treatment with anti-integrin α5β1 antibody partially rescued the SH-SY5Y cells from the cell death.Dot blotting and immunoprecipitation revealed that the nitrated protein bound to integrin on the cell membranes.Level of nitric oxide(NO)and calcium-independent inducible NO synthase(iNOS)activity increased during the initial stages of the treatment.The expression of phosphorylated focal adhesion kinase(FAK)decreased in the cells.Subsequently,an increase in caspase 3 activity was observed in SH-SY5Y cells.Our results demonstrate that activation of iNOS and inhibition of FAK may both be responsible for the cell death induced by nitrated α-synuclein.These data suggest that the cytotoxicity of nitrated a-synuclein is mediated via an integrin-iNOS/-FAK signaling pathway,and that the nitration of α-synuclein plays a role in neuronal degeneration.
文摘The present work aims to stabilize the room temperature allotropic transition of ammonium nitrate(AN)particles utilizing a microencapsulation technique,which involves solvent/non-solvent in which nitrocellulose(NC)has been employed as a coating agent.The SEM micrographs revealed distinct features of both pure AN and NC,contrasting with the irregular granular surface topography of the coated AN particles,demonstrating the adherence of NC on the AN surface.Structural analysis via infrared spectroscopy(IR)demonstrated a successful association of AN and NC,with slight shifts observed in IR bands indicating interfacial interactions.Powder X-ray Diffraction(PXRD)analysis further elucidated the structural changes induced by the coating process,revealing that the NC coating altered the crystallization pattern of its pure form.Thermal analysis demonstrates distinct profiles for pure and coated AN,for which the coated sample exhibits a temperature increase and an enthalpy decrease of the room temperature allotropic transition by 6℃,and 36%,respectively.Furthermore,the presence of NC coating alters the intermolecular forces within the composite system,leading to a reduction in melting enthalpy of coated AN by~39%compared to pure AN.The thermal decomposition analysis shows a two-step thermolysis process for coated AN,with a significant increase in the released heat by about 78%accompanied by an increase in the activation barrier of NC and AN thermolysis,demonstrating a stabilized reactivity of the AN-NC particles.These findings highlight the synergistic effect of NC coating on AN particles,which contributed to a structural and reactive stabilization of both AN and NC,proving the potential application of NC-coated AN as a strategically advantageous oxidizer in composite solid propellant formulations.
基金supported by the National Key Research and Development Program of China(2023YFE0120900)the National Natural Science Foundation of China(52377160)+2 种基金the National Natural Science Foundation of China National Young Talents Project(GYKP010)Shaanxi Provincial Natural Science Program(2023-JCYB-425)Xi’an Jiaotong University Young Top Talents Program。
文摘Ammonia is the cornerstone of modern agriculture,providing a critical nitrogen source for global food production and serving as a key raw material for numerous industrial chemicals.Electrocatalytic nitrate reduction,as an environmentally friendly method for synthesizing ammonia,not only mitigates the reliance on current ammonia synthesis processes fed by traditional fossil fuels but also effectively reduces nitrate pollution resulting from agricultural and industrial activities.This review explores the fundamental principles of electrocata lytic nitrate reduction,focusing on the key steps of electron transfer and ammonia formation.Additionally,it summarizes the critical factors influencing the performance and selectivity of the reaction,including the properties of the electrolyte,operating voltage,electrode materials,and design of the electrolytic cell.Further discussion of recent advances in electrocatalysts,including pure metal catalysts,metal oxide catalysts,non-metallic catalysts,and composite catalysts,highlights their significant roles in enhancing both the efficiency and selectivity of electrocata lytic nitrate to ammonia(NRA)reactions.Critical challenges for the industrial NRA trials and further outlooks are outlined to propel this strategy toward real-world applications.Overall,the review provides an in-depth overview and comprehensive understanding of electrocata lytic NRA technology,thereby promoting further advancements and innovations in this domain.
文摘Nitrate contamination of groundwater is a worldwide problem, particularly in agricultural countries. Exposure to high levels of nitrates in groundwater can have adverse effects on the health of residents who use groundwater for drinking. This study aims to assess the health risk associated with the ingestion of nitrates in well water in the town of M’bahiakro. Health risk maps were created on the basis of hazard quotients (HQ) using the US Environmental Protection Agency (USEPA) health risk assessment model. The results indicate that residents of the Koko, Dougouba and Baoulekro neighbourhoods, whatever their age, are potentially exposed to the toxic effects of NO3−during their daily intake of nitrate-contaminated well water, with reference to hazard quotients (HQ) greater than 1. Nitrate concentrations in the groundwater should therefore be controlled in order to prevent their harmful effects on the health of the population and guarantee its use in rice-growing activities in M’Bahiakro.
基金National Natural Science Foundation of China (52371228, 52402045)fund of Key Laboratory of Advanced Materials of Ministry of Education(Advmat-2414)。
文摘Electrocatalytic nitrate reduction reaction (NO_(3)-RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution issues.We report a CuO nanoparticles incorporated on nitrogen-doped porous carbon (CuO@NC) catalyst for NO_(3)-RR.Part of Cu(Ⅱ) is reduced to Cu(Ⅰ) during the NO_(3)-RR process to construct Cu(Ⅰ)-Cu(Ⅱ) pairs,confirmed by in situ X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy.Density functional theory (DFT) calculations indicated that the formation of Cu(Ⅰ) could provide a reaction path with smaller energy barrier for NO_(3)-RR,while Cu(Ⅱ) effectively suppressed the competition of hydrogen evolution reaction (HER).As a result,CuO@NC catalyst achieved a Faradaic efficiency of 84.2% at -0.49 V versus reversible hydrogen electrode (RHE),and a NH_(3)yield rate of 17.2 mg h^(-1)mg^(-1)cat.at -0.79 V vs.RHE,higher than the HaberBosch process (<3.4 g h^(-1)g^(-1)cat.).This work may open a new avenue for effective NO_(3)-RR by modulating oxidation states.
基金support from the National Key Scientific and Technological Infrastructure project “Earth System Science Numerical Simulator Facility” (Earth Lab)sponsored by the National Natural Science Foundation of China (Grant Nos. 42175132, 92044303, and 42205119)+2 种基金the National Key R&D Program (Grant Nos. 2020YFA0607802 and 2022YFC3703003)the CAS Information Technology Program (Grant No. CAS-WX2021SF-0107-02)the fellowship of China Postdoctoral Science Foundation (Grant No. 2022M723093)
文摘Scientific knowledge on the chemical compositions of fine particulate matter(PM_(2.5)) is essential for properly assessing its health and climate effects,and for decisionmakers to develop efficient mitigation strategies.A high-resolution PM_(2.5) chemical composition dataset(CAQRA-aerosol)is developed in this study,which provides hourly maps of organic carbon,black carbon,ammonium,nitrate,and sulfate in China from 2013 to 2020 with a horizontal resolution of 15 km.This paper describes the method,access,and validation results of this dataset.It shows that CAQRA-aerosol has good consistency with observations and achieves higher or comparable accuracy with previous PM_(2.5) composition datasets.Based on CAQRA-aerosol,spatiotemporal changes of different PM_(2.5) compositions were investigated from a national viewpoint,which emphasizes different changes of nitrate from other compositions.The estimated annual rate of population-weighted concentrations of nitrate is 0.23μg m^(−3)yr^(−1) from 2015 to 2020,compared with−0.19 to−1.1μg m^(−3)yr^(−1) for other compositions.The whole dataset is freely available from the China Air Pollution Data Center(https://doi.org/10.12423/capdb_PKU.2023.DA).
基金supported by the National Natural Science Foundation of China(12205300(H.S.),12405377(M.H.L))the Postdoctoral Science Foundation of China(2024M763694(M.H.L))+3 种基金the Natural Science Foundation of Hunan Province(2024JJ4027(H.S.))the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20240859(M.H.L)financial support from the Hunan Normal University Program(grant05311204666)financial support from the 2024 Large Instrument Testing Open Fund of Hunan Normal University(24CSY033,24CSY086)。
文摘The electrochemical conversion of nitrate,a widespread water pollutant,into valuable ammonia represents a green and decentralized approach to ammonia synthesis.However,the sluggish multielectronproton coupling path and the low reactive species(nitrate and proton)concentration at the catalyst interface inhibit the efficiency of ammonia production from nitrate reduction reaction(NitRR).Herein,we introduce a novel iron-based tandem catalyst encapsulated by reduced graphene oxide(denoted as Fe-rGO),with a superior ammonia production rate of 47.815 mg h^(-1)mg_(ca)^(t-1)and a high Faraday efficiency(FE)of 96.51%at an applied potential of-0.5 V.It also delivers a robust stability with FE above90%under a current density of 250 mA cm^(-2)for 50 h.In situ X-ray absorption spectroscopy reveals that the FeO_(x)is dynamically translated to Fe~0 site concurrently with the enhancement of the NH_(3)production rate,suggesting the Fe^(0) site as hydrogenation active center.The asymmetric distribution of surface charges of rGO not only enriches nitrate ions at the catalytic interface and promotes the hydrogenation process in NitRR,but also protects the iron species and ensures their stability during electrolysis.The Zn-NO_(3)^(-)battery demonstrates an impressive FE of 88.6%,highlighting its exceptional potential for practical applications.
基金supported by the National Natural Science Foundation of China(51609247)the Henan Provincial Natural Science Foundation,China(222300420589,202300410553)+4 种基金the Central Public-interest Scientific Institution Basal Research Fund,China(FIRI2022-22)the Science&Technology Fundamental Resources Investigation Program,China(2022FY101601)the Science and Technology Project of Xinxiang City,Henan Province,China(GG2021024)the Major Special Science and Technology Project of Henan Province,China(221100110700)the Joint Fund of Science and Technology Research and Development Plan of Henan Province,China(Superior Discipline Cultivation)(222301420104)。
文摘Nitrogen(N)uptake is regulated by water availability,and a water deficit can limit crop N responses by reducing N uptake and utilization.The complex and multifaceted interplay between water availability and the crop N response makes it difficult to predict and quantify the effect of water deficit on crop N status.The nitrogen nutrition index(NNI)has been widely used to accurately diagnose crop N status and to evaluate the effectiveness of N application.The decline of NNI under water-limiting conditions has been documented,although the underlying mechanism governing this decline is not fully understood.This study aimed to elucidate the reason for the decline of NNI under waterlimiting conditions and to provide insights into the accurate utilization of NNI for assessing crop N status under different water-N interaction treatments.Rainout shelter experiments were conducted over three growing seasons from 2018 to 2021 under different N(75 and 225 kg N ha^(-1),low N and high N)and water(120 to 510 mm,W0 to W3)co-limitation treatments.Plant N accumulation,shoot biomass(SB),plant N concentration(%N),soil nitrate-N content,actual evapotranspiration(ET_a),and yield were recorded at the stem elongation,booting,anthesis and grain filling stages.Compared to W0,W1 to W3 treatments exhibited NNI values that were greater by 10.2 to 20.5%,12.6to 24.8%,14 to 24.8%,and 16.8 to 24.8%at stem elongation,booting,anthesis,and grain filling,respectively,across the 2018-2021 seasons.This decline in NNI under water-limiting conditions stemmed from two main factors.First,reduced ET_(a) and SB led to a greater critical N concentration(%N_(c))under water-limiting conditions,which contributed to the decline in NNI primarily under high N conditions.Second,changes in plant%N played a more significant role under low N conditions.Plant N accumulation exhibited a positive allometric relationship with SB and a negative relationship with soil nitrate-N content under water-limiting conditions,indicating co-regulation by SB and the soil nitrate-N content.However,this regulation was influenced by water availability.Plant N accumulation sourced from the soil nitrate-N content reflects soil N availability.Greater soil water availability facilitated greater absorption of soil nitrate-N into the plants,leading to a positive correlation between plant N accumulation and ET_(a)across the different water-N interaction treatments.Therefore,considering the impact of soil water availability is crucial when assessing soil N availability under water-limiting conditions.The findings of this study provide valuable insights into the factors contributing to the decline in NNI among different water-N interaction treatments and can contribute to the more accurate utilization of NNI for assessing winter wheat N status.
基金supported by Natural Science Foundation of Shandong Province(ZR2021MB075)Fundamental Research Funds for the Central Universities,Ocean University of China(202461021).
文摘The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation and oxygen evolution competition,sluggish kinetics,low Faradaic efficiency,and limited nitrate yields.In this work,a novel two-dimensional(2D)layered MOF Mn-BCPPy(H_(2)BCPPy=3,5-di(4'-carboxyphenyl)pyridine)has been successfully synthesized.The framework is composed of a rod-manganese motifs and possesses abundant active sites including open metal sites(OMSs)and Lewis base sites(LBSs).The Mn-BCPPy is the first MOF catalyst applied in electrocatalytic NOR which NO_(3)^(-)exhibited relatively high activity with a yield of 99.75μg/(h·mg)and a Faraday efficiency(FE)of 32.09%.Furthermore,it can be used as fluorescent sensor for selectively and sensitively detect nitrofuran antibiotics(NFs).Therefore,this work explores the application of MOF materials in the field of electrocatalytic NOR,which reveals that manganese-based MOFs have great potential prospects.
基金Science and Technology Program Project of Gansu Province(21ZD3GB001)。
文摘A static corrosion experiment of 347H stainless steel alloyed with elements Cu and Mo was carried out in a nitrate molten salt(60%NaNO_(3)+40%KNO_(3))at 565℃ for 720 h.The effects of elements Cu and Mo on the corrosion resistance of 347H stainless steel in molten salt were investigated by analyzing the phase composition,microstructure and chemical composition of the corrosion products.The results show that the grain refinement induced by element Mo imparts the stainless steel with optimal corrosion resistance at a medium grain size.Furthermore,the formation of MoC significantly enhances the intergranular corrosion resistance of the stainless steel.The stainless steel exhibits uniform corrosion in the nitrate solution.The corrosion layer displays a dual-layer structure,and the corrosion products protecting matrix are present in both the inner and outer layers.The outer layer consists of a mixture of Fe oxides(Fe_(2)O_(3),Fe_(3)O_(4)),NaFeO_(2),and a minor amount of MgFe_(2)O_(4).Conversely,the inner layer is primarily composed of a spinel layer(FeCr_(2)O_(4),MgCr_(2)O_(4))and a thin Cu_(2)O layer.The oxidation of Cu in the inner layer leads to the formation of a dense Cu_(2)O layer,effectively impeding O_(2)-plasma infiltration into the matrix.
基金supported by the National Natural Science Foundation of China(Grant Nos.32260727,32472670,and 32371924)the Natural Science Foundation of Ningxia(Grant Nos.2024AAC02039 and 2022AAC02024)+2 种基金the Key Research and Development Program of Xinjiang Uygur Autonomous Region(Grant No.2022B02034-3)the Key Research and Development Program of Ningxia Hui Autonomous Region(Grant No.2024BBF01003)the Science and Technology Plan Project of Xi'an City(Grant No.23NYGG0028).
文摘Nitrate is the primary nitrogen source for plants and is a signaling molecule regulating various plant developmental processes. Despite its significance, limited information is available on nitrate signaling in Vitis vinifera. We identified nine Vv RWP-RK genes distributed across eight chromosomes using genome-wide identification and evolutionary analyses. Among these, Vv NLP1-4 and Vv RKD1-5 are associated with nitrate signaling and reproductive growth, respectively. To investigate their potential functions, structures, cis-acting promoter elements,functional structural domains, phylogenetic trees, spatiotemporal expression levels in different tissues at different developmental stages,potential protein-protein interaction networks, synteny(gene content), collinearity(gene order), and three-dimensional protein structure prediction were explored. We found that long-term nitrate application dramatically promoted grapevine plantlet development, including primary root length and leaf growth, and Vv NLP1.1, Vv NLP1.2, and Vv NLP2 were highly expressed in ‘Thompson Seedless' root tissues under nitrate-enriched conditions. To clarify the critical role of nitrate in grapevine growth, we observed that nuclear localization of Vv NLP1.1increased significantly following nitrate treatment. Vv NLP1.1 was found to bind to the promoter of the primary nitrate response gene Vv NRT1.1,driving its transcriptional activity. These findings indicate that Vv NLP1.1 is a core transcription factor of the nitrate signaling pathway in grapevine. Nitrate molecular docking analysis revealed that Vv NLP1.1 directly binds to nitrate ions, indicating its potential role as a nitrate sensor capable of directly perceiving nitrate concentration. We also discovered that short-term nitrate starvation impacts Vv NLP1.1 promoter activity, linked to the abscisic acid-binding element(ABRE) motif in its promoter region. Our results thus provide new insights into the molecular mechanisms underlying various physiological processes in grapevine, particularly the nitrate signaling pathway, and provide a theoretical basis for improving nitrogen use efficiency(NUE) in grapevine.
基金supported by the National Natural Science Foundation of China(No.41975156).
文摘Tyrosine residues in proteins can be nitrated to form 3-nitrotyrosine(3-NT)under the influence of ozone(O_(3))and nitrogen dioxide(NO_(2))in the air,which may introduce health impacts.A selective and sensitive enzyme-linked-immunoassay(ELISA)method was developed to determine 3-NT in modified model protein(bovine serum albumin,BSA)and ambient aerosol samples.The nitration degrees(NDs)of BSA in the exposure experiments with different durations were detected by both the ELISA and spectrophotometric methods(i.e.,ND_(ELISA) and ND_(SEC-PDA)),which show good coincidence.The kinetic investigation by both ΔND_(ELISA) and ΔND_(SEC-PDA) in the exposure experiments shows that the rate coefficients(k)of the pseudo-first-order kinetic rate reactions of protein nitration were comparable.These results indicate that direct detection of 3-NT by the ELISA method can be applied for laboratory exposure samples analysis for kinetic studies.Based on the selective detection of 3-NT,ND_(ELISA) provides a promising measure for the assessment of ND in model proteins.3-NT was alsomeasured in PM_(2.5) samples in summer in Guangzhou,southern China,ranging from 10.1 to 404 pg/m^(3),providing clear evidence of protein nitration in ambient aerosols.We further proposed that 3-NT/protein can be used as a proxy to evaluate protein nitration in ambient aerosols.A significant correlationwas observed between 3-NT/protein and O_(3),confirming the crucial role of O_(3) in protein nitration.Our results show that the direct detection of 3-NT by the ELISA method can be more widely applied in the laboratory and field-based studies for understanding the mechanisms of protein nitration.
基金support from the National Key Research and Development Program of China(2022YFC2904704)the Fundamental Research Funds for the Central Universities(SCU2024D009)。
文摘The enrichment of low-grade phosphate rock is an important process to realize sustainable support of phosphorus resources. An aqueous solution containing Ca(NO_(3))_(2) and Mg(NO_(3))_(2) is produced during the enrichment of low-grade phosphate rock by leaching of HNO_(3) or calcination coupling with leaching of NH_(4)NO_(3) solution. Preparation liquid fertilizer is a preferential way to utilize it. The liquid−solid phase diagrams of Ca(NO_(3))_(2)-Mg(NO_(3))_(2)-H_(2)O, KNO_(3)-Mg(NO_(3))_(2)-H_(2)O, KNO_(3)-Ca(NO_(3))_(2)-H_(2)O and KNO_(3)-Ca(NO_(3))_(2)-Mg(NO_(3))_(2)-H_(2)O systems at 313.15 K were studied by isothermal dissolution equilibrium method. Two crystallization regions of Ca(NO_(3))_(2)·4H_(2)O and Mg(NO_(3))_(2)·6H_(2)O were observed in the phase diagram of the ternary system Ca(NO_(3))_(2)-Mg(NO_(3))_(2)-H_(2)O, a liquid fertilizer with a maximal total nutrient content of 27.46% and a nutrients ratio of N:Ca:Mg = 8.40:10.37:1 can be formed. A homogenous solution can be formed by mixing Ca(NO_(3))_(2)·4H_(2)O and Mg(NO_(3))_(2)·6H_(2)O. In the ternary system KNO_(3)-Mg(NO_(3))_(2)-H_(2)O, the crystallization regions of KNO_(3), Mg(NO_(3))_(2)·6H_(2)O and the co-crystallization region of KNO_(3) and Mg(NO_(3))_(2)·6H_(2)O were observed. The obtained maximal total nutrient content of liquid fertilizer is 23.32% with the ratio of N:K_(2)O = 1:3.39. In the ternary system KNO_(3)-Ca(NO_(3))_(2)-H_(2)O, the crystallization regions of Ca(NO_(3))_(2)·4H_(2)O and KNO_(3) were observed. The obtained maximal total nutrient content of liquid fertilizer is 38.41% with the ratio of N:K_(2)O:Ca = 1.05:1.18:1. A homogenous solution can also be formed by mixing Ca(NO_(3))_(2)·4H_(2)O and KNO_(3) directly. In the quaternary system KNO_(3)-Ca(NO_(3))_(2)-Mg(NO_(3))_(2)-H_(2)O, the crystallization regions of Ca(NO_(3))_(2)·4H_(2)O, Mg(NO_(3))_(2)·6H_(2)O and KNO_(3) and the co-crystallization region of KNO_(3) and Mg(NO_(3))_(2)·6H_(2)O were observed. The obtained maximal total nutrient content of liquid fertilizer is 38.41% with the ratio of N:K_(2)O:Ca = 1.05:1.18:1. The modified BET model was successfully used to fit the solubility curves. The results can provide a guidance for the formulation of water-soluble fertilizers of N-(K, Ca, Mg).
基金Supported by the National Natural Science Foundation of China(No.31902370)the Ningbo Public Welfare Science and Technology Program(No.2022S161)the Zhejiang Provincial Natural Science Foundation of China(No.LY22C190001)。
文摘Cyclotella cryptica,a model diatom known for its robust adaptability to variable salinity and temperature conditions,is a promising candidate for large-scale biotechnological applications.Nutrient availability,particularly nitrogen and phosphorus,plays a crucial role in the metabolic activities of microalgae,influencing its industrial utility.Exploring the relationship between these essential nutrients and both the yield and biochemical composition of this microalga is crucial for optimizing cultivation strategies.However,research focusing on the effects of nitrogen and phosphorus on C.cryptica remains limited.We investigated the impacts of varying concentrations of nitrate(0.25-3.96 mmol/L)and phosphate(14.4-229.6μmol/L)on C.cryptica culture by analyzing its growth performance,photosynthetic activity,biochemical composition,and biosilica deposition.Results indicate that C.cryptica exhibited enhanced growth,photosynthetic efficiency,and carotenoid production under higher nutrient concentrations.However,the effects of nitrate on macronutrients composition and fatty acids profile differed from those of phosphate.Specifically,increased nitrate levels resulted in higher concentrations of polyunsaturated fatty acids(PUFAs)at the expense of saturated fatty acids(SFAs),while increased phosphate levels were associated with increased PUFAs and reduced monounsaturated fatty acids(MUFAs).Additionally,biosilica deposition was weakened by elevated nitrate but enhanced by increased phosphate levels.This study improved our understanding of nutrient-mediated regulatory mechanisms in diatoms and contributed valuable data to the broader field of algal biotechnology.Moreover,these findings are expected to advance the development of tailored nutrient management strategies,thereby enhancing the industrial potential of C.cryptica.
基金supported by the Natural Scientific Foundation of China(Nos.22127803,22174110,22203050)Natural Scientific Foundation of Shandong(No.ZR2022QB002)China Postdoctoral Science Foundation(No.2020T130331)。
文摘A novel Cu-t-ZrO_(2)catalyst with enhanced electronic metal-support interaction(EMSI)is designed for efficient electrocatalytic conversion of nitrate(NO_(3^(-)))to ammonia(NH_(3)),achieving a remarkable Faradaic efficiency and yield rate of 97.54%and 33.64 mg h^(-1)mg_(cat)^(-1),respectively.Electrons are more likely to be transferred from Cu to t-ZrO_(2)at the electron-rich interface due to the lower work function,which promotes the formation of highly active Cu species and facilitates NO_(3^(-))adsorption,ensuring selective conversion into NH_(3).
