NO adsorption on Ag/Pt(110)-(1×2) bimetallic surfaces at room temperature was investigated by means of Auger electron spectroscopy, X-ray photoelectron spectroscopy and thermal desorption spectroscopy. An une...NO adsorption on Ag/Pt(110)-(1×2) bimetallic surfaces at room temperature was investigated by means of Auger electron spectroscopy, X-ray photoelectron spectroscopy and thermal desorption spectroscopy. An unexpected formation of nitrite/nitrate surface species on Ag/Pt(110)-(1 ×2) bimetallic surfaces is observed, then decompose at elevated temperatures to form N2. However, such nitrite/nitrate surface species do not form on clean Pt(110) and Ag-Pt alloy surfaces upon NO exposure at room temperature. The formation of nitrite/nitrate surface species on Ag/Pt(110)-(1×2) bimetallic surfaces is attributed to high reactivity of highly coordination-unsaturated Ag clusters and the synergetic effect between Ag clusters and Pt substrate.展开更多
Sulfur-limestone was used in the autotrophic denitrification process to remove the nitrate and nitrite in a lab scale upflow biofilter.Synthetic water with four levels of nitrate and nitrite concentrations of 10,40,70...Sulfur-limestone was used in the autotrophic denitrification process to remove the nitrate and nitrite in a lab scale upflow biofilter.Synthetic water with four levels of nitrate and nitrite concentrations of 10,40,70 and 100 mg N/L was tested.When treating the low concentration of nitrate-or nitrite-contaminated water(10,40 mg N/L),a high removal rate of about 90% was achieved at the hydraulic retention time(HRT) of 3 hr and temperature of 20-25°C.At the same HRT,50% of the nitrate or nitrite could be removed even at the low temperature of 5-10°C.For the higher concentration nitrate and nitrite(70,100 mg N/L),longer HRT was required.The batch test indicated that influent concentration,HRT and temperature are important factors afiecting the denitrification eficiency.Molecular analysis implied that nitrate and nitrite were denitrified into nitrogen by the same microorganisms.The sequential two-step-reactions from nitrate to nitrite and from nitrite to the next-step product might have taken place in the same cell during the autotrophic denitrification process.展开更多
The potential toxic effects of nitrate-nitrite-nitrosamine on pancreatic β cell have remained a controversial issue over the past two decades. In this study, we reviewed epidemiological studies investigated the assoc...The potential toxic effects of nitrate-nitrite-nitrosamine on pancreatic β cell have remained a controversial issue over the past two decades. In this study, we reviewed epidemiological studies investigated the associations between nitrate-nitrite-nitrosamines exposure, from both diet and drinking water to ascertain whether these compounds may contribute to development of type 1 diabetes. To identify relevant studies, a systematic search strategy of Pub Med, Scopus, and Science Direct was conducted using queries including the key words "nitrate", "nitrite", "nitrosamine" with "type 1 diabetes" or "insulin dependent diabetes mellitus". All searches were limited to studies published in English. Ecologic surveys, case-control and cohort studies have indicated conflicting results in relation to nitrate-nitrite exposure from drinking water and the risk of type 1 diabetes. A null, sometimes even negative association has been mainly reported in regions with a mean nitrate levels < 25 mg/L in drinking water, while increased risk of type 1 diabetes was observed in those with a maximum nitrate levels > 40-80 mg/L. Limited data are available regarding the potential diabetogenic effect of nitrite from drinking water, although there is evidence indicating dietary nitrite could be a risk factor for development of type 1 diabetes, an effect however that seems to be significant in a higher range of acceptable limit for nitrate/nitrite. Current data regarding dietary exposure of nitrosamine and development of type 1 diabetes is also inconsistent. Considering to an increasing trend of type 1 diabetes mellitus(T1DM) along with an elevated nitrate-nitrite exposure, additional research is critical to clarify potential harmful effects of nitrate-nitritenitrosamine exposure on β-cell autoimmunity and the risk of T1DM.展开更多
The qualitative and quantitative analyses of reactive oxygen species are essential to determine their steady-state concentration and related reaction mechanisms in environmental aquatic systems. In this study, salicyl...The qualitative and quantitative analyses of reactive oxygen species are essential to determine their steady-state concentration and related reaction mechanisms in environmental aquatic systems. In this study, salicylic acid was employed as an innovative molecular probe of hydroxyl radical(OH) generated in aqueous nitrate and nitrite solutions through photochemical reactions. Kinetic studies showed that the steady-state concentrations of OH in aqueous NO- 3(10 mmol/L, pH=5) and NO- 2(10 mmol/L, pH=5) solutions under ultraviolet irradiation were at a same magnitude, 10 -15 mol/L. Apparent quantum yields of OH at 313 nm were measured as 0.011 and 0.07 for NO- 3 and NO- 2 respectively, all comparable to the results of previous studies.展开更多
Accurate quantification of dissolved organic nitrogen(DON) has been a challenge due to the cumulative analytical errors in the conventional method via subtracting dissolved inorganic nitrogen species(DIN) from total d...Accurate quantification of dissolved organic nitrogen(DON) has been a challenge due to the cumulative analytical errors in the conventional method via subtracting dissolved inorganic nitrogen species(DIN) from total dissolved nitrogen(TDN). Size exclusion chromatography coupled with an organic nitrogen detector(SEC-OND) has been developed as a direct method for quantification and characterization of DON. However, the applications of SECOND method still subject to poor separations between DON and DIN species and unsatisfied N recoveries of macromolecules. In this study, we packed a series of SEC columns with different lengths and resin materials for separation of different N species and designed an independent vacuum ultraviolet(VUV) oxidation device for complete oxidation converting N species to nitrate. To guarantee sufficient N recoveries, the operation conditions were optimized as oxidation time ≥ 30 min, injection mass(sample concentration × injection volume) < 1000 μL × mg-N/L for macromolecular proteins, and neutral p H mobile eluent. The dissolved O_(2)concentration in SEC mobile phase determined the upper limit of VUV oxidation at a specific oxidation time. Compared to conventional HW50S column(20 × 250 mm),HW40S column(20 × 350 mm) with mobile phase comprising of 1.5 g/L Na2HPO_(4)·2H_(2)O + 2.5g/L KH_(2)PO_(4)(p H = 6.85) could achieve a better separation of DON, nitrite, nitrate, and ammonia. When applied to river water, lake water, wastewater effluent, groundwater, and landfill leachate, the SEC-OND method could quantify DON as well as DIN species accurately and conveniently even the DIN/TDN ratio reached 0.98.展开更多
A spectrophotometric technique is developed to simultaneously quantify nitrate and nitrite in plasma treated water.The measurement is based on examining the inflection points(wavelengths)in the derivative absorbance o...A spectrophotometric technique is developed to simultaneously quantify nitrate and nitrite in plasma treated water.The measurement is based on examining the inflection points(wavelengths)in the derivative absorbance of the nitrate or nitrite solution.At the inflection points of the pure nitrate solution,the derivative absorbance is zero and independent of the nitrate’s concentration,and thus the nitrite’s concentration in a mixed nitrate and nitrite solution can be obtained by using the Beer’s law at these points.The nitrate’s concentration can also be achieved from the inflection points of nitrite in the same manner.The relation between the tested substance’s(nitrate or nitrite)concentration and the second-or the third-order absorbances is obtained at these inflection points.Test measurements for mixed aqueous solutions of nitrate and nitrite with or without hydrogen peroxide confirm the reliability of this technique.We applied this technique to quantify the nitrate and nitrite generated in air plasma treated aqueous solutions.The results indicate that both nitrate and nitrite concentrations increase with the plasma treatment time,and the nitrite species is found to be generated prior to the nitrate species in the air plasma treated aqueous solution.Moreover,the production rate of total nitrogen species is independent of the solutions’p H value.These results are relevant to diverse applications of plasma activated solutions in materials processing,biotechnology,medicine and other fields.展开更多
Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the...Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.展开更多
The levels of nitrate and nitrite were determined in 102 samples of Syrian white cheese which represents the major production of total cheeses, manufactured mainly from cow’s milk and sheep’s milk in a less degree. ...The levels of nitrate and nitrite were determined in 102 samples of Syrian white cheese which represents the major production of total cheeses, manufactured mainly from cow’s milk and sheep’s milk in a less degree. Determination of nitrate and nitrite levels has been made by spectrophotometric method. The results for nitrate in cow’s and sheep’s milk cheeses reveal an average of 5.10 and 6.25 mg/kg, respectively. The results for nitrite in cow’s and sheep’s milk cheese were found to contain 1.24 and 1.31 mg/kg as an average, respectively. Several factors can play a role in the interpretation of the high nitrate content, such as livestock nutrition by forge with high nitrate load and water contaminated with nitrogen fertilizer and domestic effluents, primitive production techniques in many cases, and adding nitrate salts to prevent the growth of gas-producing bacteria caused by failing in the hygienic conditions. There is a necessity to apply strict controls to reduce the presence of these two anions in the Syrian white cheese.展开更多
During 1985-1987, the concentration of nitrate nitrogen was higher in the Laizhou Bay and the Bohai Bay while that of nitrite nitrogen was higher in the Liaodong Bay and the Bohai Bay. The concentration of nitrate nit...During 1985-1987, the concentration of nitrate nitrogen was higher in the Laizhou Bay and the Bohai Bay while that of nitrite nitrogen was higher in the Liaodong Bay and the Bohai Bay. The concentration of nitrate nitrogen was highest in winter and lowest in summer while that of nitrite nitrogen was highest in autumn and lowest in spring. The seasonal variation of the concentration of nitrate nitrogen was maximum in the Laizhou Bay and the Bohai Bay while that of the concentration of nitrite nitrogen was maximum in the Liaodong Bay. There was a great difference in the concentration of nitrate nitrogen between the surface and the bottom in autumn and in the concentration of nitrite nitrogen between the surface and the bottom in summer. The main reason for the seasonal variations of the concentration of nitrate nitrogen and nitrite nitrogen was the marine biochemical process. The nitrate nitrogen and nitrite nitrogen in the Bohai Sea basically maintained a quasi-equilibrium state seasonal cycle. The quasi-equilibrium state seasonal cycle of nitrate nitrogen and nitrite nitrogen at the bottom was stable while that at the surface was liable to variations caused by other factors.展开更多
The influence of pollution from petroleum refining activities on the levels of nitrates and nitrites in five edible vegetable species was investigated. Besides, the kinetics of nitrite and nitrate was studied in vivo ...The influence of pollution from petroleum refining activities on the levels of nitrates and nitrites in five edible vegetable species was investigated. Besides, the kinetics of nitrite and nitrate was studied in vivo using albino rats with focus on the possible influence of concentration difference on kinetics and implications to toxicity. Leaf samples of the five vegetable species were collected randomly from various locations within Eleme, a host community of Port Harcourt Refinery Company and the Indorama Petrochemical Company. Also, samples were collected from Umuahia, which served as pollution-free control. The leaf samples were analyzed for their nitrite and nitrate contents. Nitrite was determined spectrophotometrically while nitrate was determined after cadmium column reduction. Results showed that samples from Eleme had higher mean nitrate (349.20 mg/100g dry leaf mass;P 0.05) as compared to the same samples from Umuahia. Solutions of nitrate and nitrite, equivalent in concentration to mean nitrate and nitrite content of the vegetable samples from the two locations were administered enterally to four groups of albino rats. Analysis of their blood levels were monitored five times at 30 minutes intervals following administration. Rates of change of blood nitrites and nitrates were found to be fairly constant in absorption as well as in the elimination phase. Their peak blood concentrations varied proportionately with their concentrations in administered solutions. However, peak blood nitrate was attained later in group of animals receiving higher amount of nitrate solution. Refining activities may pre-dispose people living within Eleme community to health hazards through contamination of edible vegetables.展开更多
This study aimed to evaluate the quality of water from village boreholes by measuring physicochemical parameters such as nitrates, nitrites, and total organic carbon (TOC). Forty-five (45) village pumps from the South...This study aimed to evaluate the quality of water from village boreholes by measuring physicochemical parameters such as nitrates, nitrites, and total organic carbon (TOC). Forty-five (45) village pumps from the Southern (Basse Côte) and the Northern (Korhogo) region of Cte d’Ivoire (west Africa) were sampled. Physicochemical parameters such as temperature, pH, conductivity at 25˚C, and turbidity were determined in situ, while nitrite and nitrate were analyzed according to ISO 10304-1 (2007) standard and total organic carbon (TOC) by NF EN 1484 (1997) standard. The results showed that the borehole waters of the Basse Côte and Korhogo analyzed are acidic, with an average temperature of 27.51˚C ± 0.16˚C and 29.95˚C ± 0.51˚C respectively for the Basse Côte and Korhogo regions. The borehole waters of the Basse Côtedo not contain nitrites, while those of Korhogo have average nitrite contents of 0.32 mg/l. The average nitrate rate in the waters of the Basse Côte and Korhogo are 12.08 ± 2.11 mg/l and 11.03 ± 3.18 mg/l respectively. The average TOC concentration of the waters of the Basse Côte is 1.28 ± 0.32 mg/l and that of Korhogo is 0.56 ± 0.09 mg/L. The study showed that the borehole waters of the Basse Côte and Korhogo have average temperatures between 27.4˚C and 29.95˚C with a slightly acidic pH value and acceptable salinity. The TOC concentrations obtained at the different sampling points were all below the French standard (2 mg/L) except for certains pumps of the Basse Côte. The water samples from the Basse Côte were devoid of nitrite. On the other hand, those from Korhogo revealed the presence of nitrite. Also, the borehole waters of the regions of the Basse Côte and Korhogo contain relatively high nitrate contents, presumably due to anthropometric activity. Overall, our study on the quality of drinking water showed that the waters analyzed are in compliance with international standards and safe for consumption.展开更多
This paper presents results of nitrites and nitrates determination in two types of baby foods: commercial products in jars and their homemade conventional counterparts. Nitrites levels in all analyzed samples were be...This paper presents results of nitrites and nitrates determination in two types of baby foods: commercial products in jars and their homemade conventional counterparts. Nitrites levels in all analyzed samples were below of the detection limit (〈 0.9 mg/kg) of applied spectrophotometric method with Griess reagent. Nitrates contents in commercial products ranged: 9.1-38.1 mg/kg while in homemade baby foods levels between 26.6 mg/kg and 118.8 mg/kg were obtained. All the contents of nitrates were lower than the EU legislation maximum limit (200 mg/kg). Comparison of each type of commercial product with its homemade counterpart baby food evidenced significant differences (p 〈 0.05) in average nitrates levels in favor of the first type. Apart from determining and comparing the levels of nitrates in the baby food samples also risk assessment for an average 6-months old infant to nitrates exposure was conducted. The estimated nitrates intake with a typical portion of 200g of baby food ranged between 6% and 25.7% of acceptable daily intake for commercial and from 18.0% to 80.3% for homemade ones.展开更多
Studies have demonstrated that the presence of nitrate and nitrite in drinking water can cause some disease such as cancer and blu baby in the infant. The Environmental Protection Agency (EPA) has since adopted the 10...Studies have demonstrated that the presence of nitrate and nitrite in drinking water can cause some disease such as cancer and blu baby in the infant. The Environmental Protection Agency (EPA) has since adopted the 10 mg/L standard as the maximum contaminant level (MCL) for nitrate-nitrogen and 1 mg/L for nitrite-nitrogen for regulated public water systems. Given the importance of nitrate and nitrite in drinking water as well as GIS ability in spatial analysis of various factors in the groundwater, this study aimed to evaluate concentration of nitrate and nitrite in the drinking water wells of Yazd using two IDW (Inverse Distance Weighting) and Kriging models. In this descriptive study, the applied data on the water quality of underground water of Yazd Environmental Health Office and the average annual nitrate and nitrite in 2015 were related to 24 wells in the studied area. The nitrate and nitrite rate in groundwater in wells was compared to the standard amount of Institute of Standard and Industrial Researches and then was analyzed via Arc GIS software using IDW and Kriging interpolation methods. The mean concentration of nitrate was 17.62 ± 3.08 mg/l and for nitrite was 0.011 ± 0.003 mg/l in the wells. In the all studied zone, the nitrate and nitrite rate was in the standard range according to the National Standard of Iran (No. 1053). In this study, Kriging interpolation method was more efficient than IDW method.展开更多
Phenolic compounds are emitted into earth’s atmosphere through industry and biomass burning events. These compounds may react in the gas or particle phase to form additional airborne pollutants. In this work, the aqu...Phenolic compounds are emitted into earth’s atmosphere through industry and biomass burning events. These compounds may react in the gas or particle phase to form additional airborne pollutants. In this work, the aqueous phase chemical reactions of syringol, guaiacol, and catechol were studied in the presence of nitrate (NO-3 ) or nitrite ( NO-2) with and without UV illumination. The reactions were found to yield light absorbing products and electrospray ionization mass spectrometry (ESI-MS) experiments indicate some of the compounds formed may be the nitrated analogues of the starting organic compounds. However, infrared absorption data suggests the reaction products are composed of a complicated mixture. This suggests additional reactions occur simultaneously in solution. Treatment of the isolated reaction products with ozone (O3) suggest they are unstable and will eventually chemically decompose if/when formed in the atmosphere.展开更多
An alternative methodology for simultaneous determination of nitrite and nitrate by capillary zone electrophoresis using direct detection UV at 210 nm under reverse electrosmotic flow is proposed. The choice of the el...An alternative methodology for simultaneous determination of nitrite and nitrate by capillary zone electrophoresis using direct detection UV at 210 nm under reverse electrosmotic flow is proposed. The choice of the electrolyte composition has taken account: the mobility of the anion buffer and of the solutes;the low absorbance of the buffer in 210 nm;high base line stability and analysis time. The electrolyte optimized has consisted of 100 mmol.L–1 TRIS/HCl buffer and 0.15 mmol.L–1 CTAB at pH 8.2. The proposed method was applied successfully in the analysis of nitrite and nitrate in samples from urban stream in the absence of usual sample pretreatment.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
Mining and tailings deposition can cause serious heavy metal(loids)pollution to the surrounding soil environment.Soil microorganisms adapt their metabolism to such conditions,driving alterations in soil function.This ...Mining and tailings deposition can cause serious heavy metal(loids)pollution to the surrounding soil environment.Soil microorganisms adapt their metabolism to such conditions,driving alterations in soil function.This study aims to elucidate the response patterns of nitrogen-cycling microorganisms under long-term heavy metal(loids)exposure.The results showed that the diversity and abundance of nitrogen-cyclingmicroorganisms showed negative feedback to heavy metal(loids)concentrations.Denitrifying microorganisms were shown to be the dominant microorganisms with over 60%of relative abundance and a complex community structure including 27 phyla.Further,the key bacterial species in the denitrification process were calculated using a random forest model,where the top three key species(Pseudomonas stutzei,Sphingobium japonicum and Leifsonia rubra)were found to play a prominent role in nitrite reduction.Functional gene analysis and qPCR revealed that nirK,which is involved in nitrite reduction,significantly accumulated in the most metal-rich soil with the increase of absolute abundance of 63.86%.The experimental results confirmed that the activity of nitrite reductase(Nir)encoded by nirK in the soil was increased at high concentrations of heavy metal(loids).Partial least squares-path model identified three potential modes of nitrite reduction processes being stimulated by heavy metal(loids),the most prominent of which contributed to enhanced nirK abundance and soil Nir activity through positive stimulation of key species.The results provide new insights and preliminary evidence on the stimulation of nitrite reduction processes by heavy metal(loids).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
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
基金This work was supported by the National Natural Science Foundation of China (No.20973161 and No.11079033), the Ministry of Science and Technology of China (No.2010CB923302), the Fundamental Research Funds for the Central Universities, and the MPG-CAS partner group program.
文摘NO adsorption on Ag/Pt(110)-(1×2) bimetallic surfaces at room temperature was investigated by means of Auger electron spectroscopy, X-ray photoelectron spectroscopy and thermal desorption spectroscopy. An unexpected formation of nitrite/nitrate surface species on Ag/Pt(110)-(1 ×2) bimetallic surfaces is observed, then decompose at elevated temperatures to form N2. However, such nitrite/nitrate surface species do not form on clean Pt(110) and Ag-Pt alloy surfaces upon NO exposure at room temperature. The formation of nitrite/nitrate surface species on Ag/Pt(110)-(1×2) bimetallic surfaces is attributed to high reactivity of highly coordination-unsaturated Ag clusters and the synergetic effect between Ag clusters and Pt substrate.
基金supported by the National Natural Science Foundation of China(No.50808121)the Chinese National Key Projects of Water Pollution Control and Reclamation(No.2008ZX07106-2-2)
文摘Sulfur-limestone was used in the autotrophic denitrification process to remove the nitrate and nitrite in a lab scale upflow biofilter.Synthetic water with four levels of nitrate and nitrite concentrations of 10,40,70 and 100 mg N/L was tested.When treating the low concentration of nitrate-or nitrite-contaminated water(10,40 mg N/L),a high removal rate of about 90% was achieved at the hydraulic retention time(HRT) of 3 hr and temperature of 20-25°C.At the same HRT,50% of the nitrate or nitrite could be removed even at the low temperature of 5-10°C.For the higher concentration nitrate and nitrite(70,100 mg N/L),longer HRT was required.The batch test indicated that influent concentration,HRT and temperature are important factors afiecting the denitrification eficiency.Molecular analysis implied that nitrate and nitrite were denitrified into nitrogen by the same microorganisms.The sequential two-step-reactions from nitrate to nitrite and from nitrite to the next-step product might have taken place in the same cell during the autotrophic denitrification process.
基金supported by the Research Institute for Endocrine Sciences of Shahid Beheshti University of Medical Sciences
文摘The potential toxic effects of nitrate-nitrite-nitrosamine on pancreatic β cell have remained a controversial issue over the past two decades. In this study, we reviewed epidemiological studies investigated the associations between nitrate-nitrite-nitrosamines exposure, from both diet and drinking water to ascertain whether these compounds may contribute to development of type 1 diabetes. To identify relevant studies, a systematic search strategy of Pub Med, Scopus, and Science Direct was conducted using queries including the key words "nitrate", "nitrite", "nitrosamine" with "type 1 diabetes" or "insulin dependent diabetes mellitus". All searches were limited to studies published in English. Ecologic surveys, case-control and cohort studies have indicated conflicting results in relation to nitrate-nitrite exposure from drinking water and the risk of type 1 diabetes. A null, sometimes even negative association has been mainly reported in regions with a mean nitrate levels < 25 mg/L in drinking water, while increased risk of type 1 diabetes was observed in those with a maximum nitrate levels > 40-80 mg/L. Limited data are available regarding the potential diabetogenic effect of nitrite from drinking water, although there is evidence indicating dietary nitrite could be a risk factor for development of type 1 diabetes, an effect however that seems to be significant in a higher range of acceptable limit for nitrate/nitrite. Current data regarding dietary exposure of nitrosamine and development of type 1 diabetes is also inconsistent. Considering to an increasing trend of type 1 diabetes mellitus(T1DM) along with an elevated nitrate-nitrite exposure, additional research is critical to clarify potential harmful effects of nitrate-nitritenitrosamine exposure on β-cell autoimmunity and the risk of T1DM.
文摘The qualitative and quantitative analyses of reactive oxygen species are essential to determine their steady-state concentration and related reaction mechanisms in environmental aquatic systems. In this study, salicylic acid was employed as an innovative molecular probe of hydroxyl radical(OH) generated in aqueous nitrate and nitrite solutions through photochemical reactions. Kinetic studies showed that the steady-state concentrations of OH in aqueous NO- 3(10 mmol/L, pH=5) and NO- 2(10 mmol/L, pH=5) solutions under ultraviolet irradiation were at a same magnitude, 10 -15 mol/L. Apparent quantum yields of OH at 313 nm were measured as 0.011 and 0.07 for NO- 3 and NO- 2 respectively, all comparable to the results of previous studies.
基金supported by the Basic Research Program of Jiangsu Province (No.BK20211557)the National Key R&D Program (No.2016YFE0112300)+1 种基金the National Natural Science Foundation of China (No.51708279)the High-level Talent Team Project of Quanzhou City (No. 2018CT006)。
文摘Accurate quantification of dissolved organic nitrogen(DON) has been a challenge due to the cumulative analytical errors in the conventional method via subtracting dissolved inorganic nitrogen species(DIN) from total dissolved nitrogen(TDN). Size exclusion chromatography coupled with an organic nitrogen detector(SEC-OND) has been developed as a direct method for quantification and characterization of DON. However, the applications of SECOND method still subject to poor separations between DON and DIN species and unsatisfied N recoveries of macromolecules. In this study, we packed a series of SEC columns with different lengths and resin materials for separation of different N species and designed an independent vacuum ultraviolet(VUV) oxidation device for complete oxidation converting N species to nitrate. To guarantee sufficient N recoveries, the operation conditions were optimized as oxidation time ≥ 30 min, injection mass(sample concentration × injection volume) < 1000 μL × mg-N/L for macromolecular proteins, and neutral p H mobile eluent. The dissolved O_(2)concentration in SEC mobile phase determined the upper limit of VUV oxidation at a specific oxidation time. Compared to conventional HW50S column(20 × 250 mm),HW40S column(20 × 350 mm) with mobile phase comprising of 1.5 g/L Na2HPO_(4)·2H_(2)O + 2.5g/L KH_(2)PO_(4)(p H = 6.85) could achieve a better separation of DON, nitrite, nitrate, and ammonia. When applied to river water, lake water, wastewater effluent, groundwater, and landfill leachate, the SEC-OND method could quantify DON as well as DIN species accurately and conveniently even the DIN/TDN ratio reached 0.98.
基金National Natural Science Foundation of China(No.52077185)the Basic Research Program of Science and Technology of Shenzhen,China(No.JCYJ20190809162617137)for partial financial support。
文摘A spectrophotometric technique is developed to simultaneously quantify nitrate and nitrite in plasma treated water.The measurement is based on examining the inflection points(wavelengths)in the derivative absorbance of the nitrate or nitrite solution.At the inflection points of the pure nitrate solution,the derivative absorbance is zero and independent of the nitrate’s concentration,and thus the nitrite’s concentration in a mixed nitrate and nitrite solution can be obtained by using the Beer’s law at these points.The nitrate’s concentration can also be achieved from the inflection points of nitrite in the same manner.The relation between the tested substance’s(nitrate or nitrite)concentration and the second-or the third-order absorbances is obtained at these inflection points.Test measurements for mixed aqueous solutions of nitrate and nitrite with or without hydrogen peroxide confirm the reliability of this technique.We applied this technique to quantify the nitrate and nitrite generated in air plasma treated aqueous solutions.The results indicate that both nitrate and nitrite concentrations increase with the plasma treatment time,and the nitrite species is found to be generated prior to the nitrate species in the air plasma treated aqueous solution.Moreover,the production rate of total nitrogen species is independent of the solutions’p H value.These results are relevant to diverse applications of plasma activated solutions in materials processing,biotechnology,medicine and other fields.
基金supported by the National Natural Science Foundation of China[Nos.U21A20332,52103226,52202275,52203314,and 12204253]the Distinguished Young Scholars Fund of Jiangsu Province[No.BK20220061]the Fellowship of China Postdoctoral Science Foundation[No.2021M702382]。
文摘Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.
文摘The levels of nitrate and nitrite were determined in 102 samples of Syrian white cheese which represents the major production of total cheeses, manufactured mainly from cow’s milk and sheep’s milk in a less degree. Determination of nitrate and nitrite levels has been made by spectrophotometric method. The results for nitrate in cow’s and sheep’s milk cheeses reveal an average of 5.10 and 6.25 mg/kg, respectively. The results for nitrite in cow’s and sheep’s milk cheese were found to contain 1.24 and 1.31 mg/kg as an average, respectively. Several factors can play a role in the interpretation of the high nitrate content, such as livestock nutrition by forge with high nitrate load and water contaminated with nitrogen fertilizer and domestic effluents, primitive production techniques in many cases, and adding nitrate salts to prevent the growth of gas-producing bacteria caused by failing in the hygienic conditions. There is a necessity to apply strict controls to reduce the presence of these two anions in the Syrian white cheese.
文摘During 1985-1987, the concentration of nitrate nitrogen was higher in the Laizhou Bay and the Bohai Bay while that of nitrite nitrogen was higher in the Liaodong Bay and the Bohai Bay. The concentration of nitrate nitrogen was highest in winter and lowest in summer while that of nitrite nitrogen was highest in autumn and lowest in spring. The seasonal variation of the concentration of nitrate nitrogen was maximum in the Laizhou Bay and the Bohai Bay while that of the concentration of nitrite nitrogen was maximum in the Liaodong Bay. There was a great difference in the concentration of nitrate nitrogen between the surface and the bottom in autumn and in the concentration of nitrite nitrogen between the surface and the bottom in summer. The main reason for the seasonal variations of the concentration of nitrate nitrogen and nitrite nitrogen was the marine biochemical process. The nitrate nitrogen and nitrite nitrogen in the Bohai Sea basically maintained a quasi-equilibrium state seasonal cycle. The quasi-equilibrium state seasonal cycle of nitrate nitrogen and nitrite nitrogen at the bottom was stable while that at the surface was liable to variations caused by other factors.
文摘The influence of pollution from petroleum refining activities on the levels of nitrates and nitrites in five edible vegetable species was investigated. Besides, the kinetics of nitrite and nitrate was studied in vivo using albino rats with focus on the possible influence of concentration difference on kinetics and implications to toxicity. Leaf samples of the five vegetable species were collected randomly from various locations within Eleme, a host community of Port Harcourt Refinery Company and the Indorama Petrochemical Company. Also, samples were collected from Umuahia, which served as pollution-free control. The leaf samples were analyzed for their nitrite and nitrate contents. Nitrite was determined spectrophotometrically while nitrate was determined after cadmium column reduction. Results showed that samples from Eleme had higher mean nitrate (349.20 mg/100g dry leaf mass;P 0.05) as compared to the same samples from Umuahia. Solutions of nitrate and nitrite, equivalent in concentration to mean nitrate and nitrite content of the vegetable samples from the two locations were administered enterally to four groups of albino rats. Analysis of their blood levels were monitored five times at 30 minutes intervals following administration. Rates of change of blood nitrites and nitrates were found to be fairly constant in absorption as well as in the elimination phase. Their peak blood concentrations varied proportionately with their concentrations in administered solutions. However, peak blood nitrate was attained later in group of animals receiving higher amount of nitrate solution. Refining activities may pre-dispose people living within Eleme community to health hazards through contamination of edible vegetables.
文摘This study aimed to evaluate the quality of water from village boreholes by measuring physicochemical parameters such as nitrates, nitrites, and total organic carbon (TOC). Forty-five (45) village pumps from the Southern (Basse Côte) and the Northern (Korhogo) region of Cte d’Ivoire (west Africa) were sampled. Physicochemical parameters such as temperature, pH, conductivity at 25˚C, and turbidity were determined in situ, while nitrite and nitrate were analyzed according to ISO 10304-1 (2007) standard and total organic carbon (TOC) by NF EN 1484 (1997) standard. The results showed that the borehole waters of the Basse Côte and Korhogo analyzed are acidic, with an average temperature of 27.51˚C ± 0.16˚C and 29.95˚C ± 0.51˚C respectively for the Basse Côte and Korhogo regions. The borehole waters of the Basse Côtedo not contain nitrites, while those of Korhogo have average nitrite contents of 0.32 mg/l. The average nitrate rate in the waters of the Basse Côte and Korhogo are 12.08 ± 2.11 mg/l and 11.03 ± 3.18 mg/l respectively. The average TOC concentration of the waters of the Basse Côte is 1.28 ± 0.32 mg/l and that of Korhogo is 0.56 ± 0.09 mg/L. The study showed that the borehole waters of the Basse Côte and Korhogo have average temperatures between 27.4˚C and 29.95˚C with a slightly acidic pH value and acceptable salinity. The TOC concentrations obtained at the different sampling points were all below the French standard (2 mg/L) except for certains pumps of the Basse Côte. The water samples from the Basse Côte were devoid of nitrite. On the other hand, those from Korhogo revealed the presence of nitrite. Also, the borehole waters of the regions of the Basse Côte and Korhogo contain relatively high nitrate contents, presumably due to anthropometric activity. Overall, our study on the quality of drinking water showed that the waters analyzed are in compliance with international standards and safe for consumption.
文摘This paper presents results of nitrites and nitrates determination in two types of baby foods: commercial products in jars and their homemade conventional counterparts. Nitrites levels in all analyzed samples were below of the detection limit (〈 0.9 mg/kg) of applied spectrophotometric method with Griess reagent. Nitrates contents in commercial products ranged: 9.1-38.1 mg/kg while in homemade baby foods levels between 26.6 mg/kg and 118.8 mg/kg were obtained. All the contents of nitrates were lower than the EU legislation maximum limit (200 mg/kg). Comparison of each type of commercial product with its homemade counterpart baby food evidenced significant differences (p 〈 0.05) in average nitrates levels in favor of the first type. Apart from determining and comparing the levels of nitrates in the baby food samples also risk assessment for an average 6-months old infant to nitrates exposure was conducted. The estimated nitrates intake with a typical portion of 200g of baby food ranged between 6% and 25.7% of acceptable daily intake for commercial and from 18.0% to 80.3% for homemade ones.
文摘Studies have demonstrated that the presence of nitrate and nitrite in drinking water can cause some disease such as cancer and blu baby in the infant. The Environmental Protection Agency (EPA) has since adopted the 10 mg/L standard as the maximum contaminant level (MCL) for nitrate-nitrogen and 1 mg/L for nitrite-nitrogen for regulated public water systems. Given the importance of nitrate and nitrite in drinking water as well as GIS ability in spatial analysis of various factors in the groundwater, this study aimed to evaluate concentration of nitrate and nitrite in the drinking water wells of Yazd using two IDW (Inverse Distance Weighting) and Kriging models. In this descriptive study, the applied data on the water quality of underground water of Yazd Environmental Health Office and the average annual nitrate and nitrite in 2015 were related to 24 wells in the studied area. The nitrate and nitrite rate in groundwater in wells was compared to the standard amount of Institute of Standard and Industrial Researches and then was analyzed via Arc GIS software using IDW and Kriging interpolation methods. The mean concentration of nitrate was 17.62 ± 3.08 mg/l and for nitrite was 0.011 ± 0.003 mg/l in the wells. In the all studied zone, the nitrate and nitrite rate was in the standard range according to the National Standard of Iran (No. 1053). In this study, Kriging interpolation method was more efficient than IDW method.
文摘Phenolic compounds are emitted into earth’s atmosphere through industry and biomass burning events. These compounds may react in the gas or particle phase to form additional airborne pollutants. In this work, the aqueous phase chemical reactions of syringol, guaiacol, and catechol were studied in the presence of nitrate (NO-3 ) or nitrite ( NO-2) with and without UV illumination. The reactions were found to yield light absorbing products and electrospray ionization mass spectrometry (ESI-MS) experiments indicate some of the compounds formed may be the nitrated analogues of the starting organic compounds. However, infrared absorption data suggests the reaction products are composed of a complicated mixture. This suggests additional reactions occur simultaneously in solution. Treatment of the isolated reaction products with ozone (O3) suggest they are unstable and will eventually chemically decompose if/when formed in the atmosphere.
基金The authors wish to acknowledge Conselho Nacional de Desenvolvimento Científico e Tecnológico(CNPq-476386/2007-1 and 300593/2008-2)Fundacao de Am-paroàPesquisa do Estado de Minas Gerais of Brazil(FA-PEMIG-CEX-APQ 1906-502/07,CEX APQ 01837/08 and CEX PPM 00326/09)Coordenacao de Aper-feicoamento de Pessoal de Nível Superior(CAPES)for fellowships and financial support.
文摘An alternative methodology for simultaneous determination of nitrite and nitrate by capillary zone electrophoresis using direct detection UV at 210 nm under reverse electrosmotic flow is proposed. The choice of the electrolyte composition has taken account: the mobility of the anion buffer and of the solutes;the low absorbance of the buffer in 210 nm;high base line stability and analysis time. The electrolyte optimized has consisted of 100 mmol.L–1 TRIS/HCl buffer and 0.15 mmol.L–1 CTAB at pH 8.2. The proposed method was applied successfully in the analysis of nitrite and nitrate in samples from urban stream in the absence of usual sample pretreatment.
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supported by the National Natural Science Foundation of China(No.41977029).
文摘Mining and tailings deposition can cause serious heavy metal(loids)pollution to the surrounding soil environment.Soil microorganisms adapt their metabolism to such conditions,driving alterations in soil function.This study aims to elucidate the response patterns of nitrogen-cycling microorganisms under long-term heavy metal(loids)exposure.The results showed that the diversity and abundance of nitrogen-cyclingmicroorganisms showed negative feedback to heavy metal(loids)concentrations.Denitrifying microorganisms were shown to be the dominant microorganisms with over 60%of relative abundance and a complex community structure including 27 phyla.Further,the key bacterial species in the denitrification process were calculated using a random forest model,where the top three key species(Pseudomonas stutzei,Sphingobium japonicum and Leifsonia rubra)were found to play a prominent role in nitrite reduction.Functional gene analysis and qPCR revealed that nirK,which is involved in nitrite reduction,significantly accumulated in the most metal-rich soil with the increase of absolute abundance of 63.86%.The experimental results confirmed that the activity of nitrite reductase(Nir)encoded by nirK in the soil was increased at high concentrations of heavy metal(loids).Partial least squares-path model identified three potential modes of nitrite reduction processes being stimulated by heavy metal(loids),the most prominent of which contributed to enhanced nirK abundance and soil Nir activity through positive stimulation of key species.The results provide new insights and preliminary evidence on the stimulation of nitrite reduction processes by heavy metal(loids).
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.
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.