The electrochemical coupling of biomass oxidation and nitrogen conversion presents a potential strategy for high value-added chemicals and nitrogen cycling.Herein,in this work,CuO/Co_(3)O_(4)with heterogeneous interfa...The electrochemical coupling of biomass oxidation and nitrogen conversion presents a potential strategy for high value-added chemicals and nitrogen cycling.Herein,in this work,CuO/Co_(3)O_(4)with heterogeneous interface is successfully constructed as a bifunctional catalyst for the electrooxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid and the electroreduction of nitrate to ammonia(NH_(3)).The open-circuit potential spontaneous experiment shows that more 5-hydroxymethylfurfural molecules are adsorbed in the Helmholtz layer of the CuO/Co_(3)O_(4)composite,which certifies that the CuO/Co_(3)O_(4)heterostructure is conducive to the kinetic adsorption of 5-hydroxymethylfurfural.In situ electrochemical impedance spectroscopy further shows that CuO/Co_(3)O_(4)has faster reaction kinetics and lower reaction potential in oxygen evolution reaction and 5-hydroxymethylfurfural electrocatalytic oxidation.Moreover,CuO/Co_(3)O_(4)also has a good reduction effect on NO_(3)^(-).The ex-situ Raman spectroscopy shows that under the reduction potential,the metal oxide is reduced,and the generated Cu_(2)O can be used as a new active site for the reaction to promote the electrocatalytic conversion of NO_(3)^(-)to NH_(3) synthesis.This work provides valuable guidance for the synthesis of value-added chemicals by 5-hydroxymethylfurfural electrocatalytic oxidation coupled with NO_(3)^(-)while efficiently producing NH_(3).展开更多
The electrochemical oxidation degradation processes for artificial and actual wastewater containing ammonia were carried out with a Ti/RuO2-Pt anode and a Ti plate cathode. We studied the effects of different current ...The electrochemical oxidation degradation processes for artificial and actual wastewater containing ammonia were carried out with a Ti/RuO2-Pt anode and a Ti plate cathode. We studied the effects of different current densities, space sizes between the two electrodes, and amounts of added NaCl on ammonia-containing wastewater treatm.ent. It was shown that, after a 30-min treatment under the optimal conditions, which were a current density of 20 mA/cm2, a space size between the two electrodes of I cm, and an added amount of 0.5 g/L of NaC1, the COD concentration in municipal wastewater was 40 mg/L, a removal rate of 90%; and the NH3-N concentration was 7 mg/L, a removal rate of 88.3%. The effluent of municipal wastewater qualified for Class A of the Discharge Standard of Pollutants for Municipal Wastewater Treatment Plant (GB 18918-2002).展开更多
The influencing factors and kinetics of oxidative degradation of ammonia nitrogen in high salinity wastewater by sodium hypochlorite oxidation( Na Cl O) were studied. The results showed that the degradation process of...The influencing factors and kinetics of oxidative degradation of ammonia nitrogen in high salinity wastewater by sodium hypochlorite oxidation( Na Cl O) were studied. The results showed that the degradation process of ammonia nitrogen by sodium hypochlorite accorded with a pseudo first-order kinetics model,and the influencing factors included Na Cl O dosage,initial concentration of ammonia nitrogen,salinity,temperature,and so on. When Na Cl O dosage was 0. 6%( MCl∶ MN= 13. 76),the reaction rate constant was up to 0. 015 75 min^(-1). The higher the initial concentration of ammonia nitrogen was,the worse the effect of oxidation reaction was. When the initial concentration did not exceed 45 mg/L,the effect on oxidation reaction rate constant increased with the increase of the initial concentration. Low salinity had no effect on ammonia nitrogen oxidation.When salinity was higher than 2. 0%,the inhibition effect on ammonia nitrogen oxidation would increase,and the reaction rate constant decreased obviously with the increase of salinity. The improvement of reaction temperature was beneficial to ammonia oxidation degradation. As temperature increased from 10 to 35 ℃,the reaction rate constant rose from 0. 00188 to 0. 01043 min^(-1).展开更多
Ammonia is gaining increasing attention as a green alternative fuel for achieving large-scale carbon emission reduction. Despite its potential technical prospects, the harsh ignition conditions and slow flame propagat...Ammonia is gaining increasing attention as a green alternative fuel for achieving large-scale carbon emission reduction. Despite its potential technical prospects, the harsh ignition conditions and slow flame propagation speed of ammonia pose significant challenges to its application in engines. Non-equilibrium plasma has been identified as a promising method, but current research on plasma-enhanced ammonia combustion is limited and primarily focuses on ignition characteristics revealed by kinetic models. In this study, low-temperature and low-pressure chemistry in plasma-assisted ammonia oxidative pyrolysis is investigated by integrated studies of steady-state GC measurements and mathematical simulation. The detailed kinetic mechanism of NH_(3) decomposition in plasma-driven Ar/NH_(3) and Ar/NH_(3)/O_(2) mixtures has been developed. The numerical model has good agreements with the experimental measurements in NH_(3)/O_(2) consumption and N_(2)/H_(2) generation, which demonstrates the rationality of modelling. Based on the modelling results, species density profiles, path flux and sensitivity analysis for the key plasmaproduced species such as NH_(2), NH, H_(2), OH, H, O, O(^(1)D), O_(2)(a^(1)△_(g)), O_(2)(b^(1)∑_(g)^(+)), Ar^(*), H^(-), Ar^(+), NH_(3)^(+), O_(2)^(-) in the discharge and afterglow are analyzed in detail to illustrate the effectiveness of the active species on NH_(3) excitation and decomposition at low temperature and relatively higher E/N values. The results revealed that NH_(2), NH, H as well as H_(2) are primarily generated through the electron collision reactions e + NH_(3)→ e + NH_(2)+ H, e + NH_(3)→ e + NH + H_(2) and the excited-argon collision reaction Ar^(*) + NH_(3)+ H → Ar + NH_(2)+ 2H, which will then react with highly reactive oxidative species such as O_(2)^(*), O^(*), O, OH, and O_(2) to produce stable products of NOx and H_(2)O. NH_(3)→ NH is found a specific pathway for NH_(3) consumption with plasma assistance, which further highlights the enhanced kinetic effects.展开更多
Monte Carlo method is applied to investigate the kinetics of ammonia oxidative decomposition over the commercial propylene ammoxidation catalyst(Mo-Bi). The simulation is quite in agreement with experimental results. ...Monte Carlo method is applied to investigate the kinetics of ammonia oxidative decomposition over the commercial propylene ammoxidation catalyst(Mo-Bi). The simulation is quite in agreement with experimental results. Monte Carlo simulation proves that the process of ammonia oxidation decomposition is a two-step reaction.展开更多
In this work,the CuAl-LDO/c-CNTs catalyst was fabricated via in situ oriented assembly of layered-double hydroxides(LDHs)and citric acid-modified carbon nanotubes(c-CNTs)followed by annealing treatment,and evaluated i...In this work,the CuAl-LDO/c-CNTs catalyst was fabricated via in situ oriented assembly of layered-double hydroxides(LDHs)and citric acid-modified carbon nanotubes(c-CNTs)followed by annealing treatment,and evaluated in the selective catalytic oxidation(SCO)of NH_(3)to N_(2).The CuAl-LDO/c-CNTs catalyst presented better catalytic performance(98%NH_(3)conversion with nearly 90%N_(2)selectivity at 513 K)than other catalysts,such as CuAlO_(x)/CNTs,CuAlO_(x)/c-CNTs and CuAl-LDO/CNTs.Multiple characterizations were utilized to analyze the difference of physicochemical properties among four catalysts.XRD,TEM and XPS analyses manifested that CuO and Cu_(2)O nanoparticles dispersed well on the surface of the Cu Al-LDO/c-CNTs catalyst.Compared with other catalysts,larger specific surface area and better dispersion of CuAl-LDO/c-CNTs catalyst were conducive to the exposure of more active sites,thus improving the redox capacity of the active site and NH_(3)adsorption capacity.In-situ DRIFTS results revealed that the internal selective catalytic reduction(iSCR)mechanism was found over CuAl-LDO/c-CNTs catalyst.展开更多
Active iron catalysts with 5A molecular sieve as the carrier were prepared firstly, and then were used in the treatment of ammonia nitrogen in landfill leachate pretreated by MBR by using CWPO, finally the effects of ...Active iron catalysts with 5A molecular sieve as the carrier were prepared firstly, and then were used in the treatment of ammonia nitrogen in landfill leachate pretreated by MBR by using CWPO, finally the effects of preparation process of catalysts, assistants and reaction conditions on the removal rate of ammonia nitrogen were analyzed. The results show that the preparation process of catalysts and assistants had great effects on catalytic activity; when steeping fluid concentration was 2 mol/L and 0.01 mol/L cerium nitrate was used as an assistant, Fe-Ce/5A catalyst roasted for 3 h at 400 ~C had a good catalytic effect. As 10 g of Fe-Ce/5A catalyst was added to water sample, and landfill leachate pretreated by MBR reacted with 15 ml of H2 02 for 30 min at 60 ~C, the removal rate of ammonia nitrogen was up to 90.8%, that is, ammonia nitrogen concentra- tion decreased from 253 to 23 mg/L, reaching the national emission standard. Besides, the kinetic analysis of ammonia nitrogen removal reveals that the removal reaction of ammonia nitrogen conformed with pseudo first order kinetic equation. Thus, it is feasible to use this method to deeply treat landfill leachate pretreated by MBR.展开更多
Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as...Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control,and practical ruthenium nanocatalysts are explored for ammonia synthesis.Graphite and graphitic carbons are of interest as supports for the nanocatalysts.Despite considerable literature on the catalytic processes on graphite and graphitic supports,reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood.Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation,and practical Ru nanocatalysts in ammonia synthesis,on graphite and related supports under controlled reaction environments using a novel in-situ environmental(scanning) transmission electron microscope with single atom resolution.By recording snapshots of the reaction dynamics,the behaviour of the catalysts is imaged.The images reveal single metal atoms,clusters of a few atoms on the graphitic supports and the support function.These all play key roles in the mobility,sintering and growth of the catalysts.The experimental findings provide new structural insights into atomic scale reaction dynamics,morphology and stability of the nanocatalysts.展开更多
Ammonia (NH<sub>3</sub>) dissociation and oxidation in a cylindrical quartz reactor has been experimentally studied for various inlet NH<sub>3</sub> concentrations (5%, 10%, and 15%) and reacto...Ammonia (NH<sub>3</sub>) dissociation and oxidation in a cylindrical quartz reactor has been experimentally studied for various inlet NH<sub>3</sub> concentrations (5%, 10%, and 15%) and reactor temperatures between 700 K and 1000 K. The thermal effects during both NH<sub>3</sub> dissociation (endothermic) and oxidation (exothermic) were observed using a bundle of thermocouples positioned along the central axis of the quartz reactor, while the corresponding NH<sub>3</sub> conversions and nitrogen oxides emissions were determined by analysing the gas composition of the reactor exit stream. A stronger endothermic effect, as indicated by a greater temperature drop during NH<sub>3</sub> dissociation, was observed as the NH<sub>3</sub> feed concentration and reactor temperature increased. During NH<sub>3</sub> oxidation, a predominantly greater exothermic effect with increasing NH<sub>3</sub> feed concentration and reactor temperature was also evident;however, it was apparent that NH<sub>3</sub> dissociation occurred near the reactor inlet, preceding the downstream NH<sub>3</sub> and H<sub>2</sub> oxidation. For both NH<sub>3</sub> dissociation and oxidation, NH<sub>3</sub> conversion increased with increasing temperature and decreasing initial NH<sub>3</sub> concentration. Significant levels of NO<sub>X</sub> emissions were observed during NH<sub>3</sub> oxidation, which increased with increasing temperature. From the experimental results, it is speculated that the stainless-steel in the thermocouple bundle may have catalysed NH<sub>3</sub> dissociation and thus changed the reaction chemistry during NH<sub>3</sub> oxidation.展开更多
By making the use of the processes which includes separating trash and solid materials from the wastewater-ammonia stripping tower-UASB-biological oxidation pond, we have treated the wastewater which comes from the sw...By making the use of the processes which includes separating trash and solid materials from the wastewater-ammonia stripping tower-UASB-biological oxidation pond, we have treated the wastewater which comes from the swine factory. The treated wastewater can meet the primary standard of The People's Republic of China based on sewage discharge standards and the wastewater treatment project design contract (GBl8596-2001), and the effluent will be used as irrigation-water. We introduce this project including the quality of influent and effluent and the flow scheme, the statement of every part, the investment and the effect, etc. The operation indicated that this process has many merits such as the stability in operation-effect and the convenience in management. So it will provide some help for the similar wastewater treatment.展开更多
Organic carbon,inorganic carbon,temperature,p H and ORP are all to have a certain influence on the anaerobic ammonia oxidation reaction.We can draw some conclusions on the optimum conditions of anaerobic ammonia oxida...Organic carbon,inorganic carbon,temperature,p H and ORP are all to have a certain influence on the anaerobic ammonia oxidation reaction.We can draw some conclusions on the optimum conditions of anaerobic ammonia oxidation reaction.The optimum temperature of the anaerobic ammonia oxidation reaction is 30-35℃.And the optimum p H of the anaerobic ammonia reaction is 7.5-8.3.The presence of organic matters can affect the anaerobic ammonia reaction,and different organic matters have different influence on it.The concentration of the inorganic carbon also exist great influence on the reaction.High inorganic carbon concentration also can inhibit anaerobic ammonia oxidation reaction.展开更多
[Objective] This study aimed to investigate the abundance and composition of ammonia-oxidizing bacteria and ammonia-oxidizing archaea in Pearl River Estuary sediment.[Method] Firstly,the amoA gene library was construc...[Objective] This study aimed to investigate the abundance and composition of ammonia-oxidizing bacteria and ammonia-oxidizing archaea in Pearl River Estuary sediment.[Method] Firstly,the amoA gene library was constructed;then based on that,the content and diversity of amoA genes of ammonia-oxidizing bacteria and ammonia-oxidizing archaea in Pearl River Estuary sediment were detected by using quantitative real-time polymerase chain reaction(Q-PCR).[Result] The results of Q-PCR presented that ammonia-oxidizing archaea(AOA) were more abundant than ammonia-oxidizing bacteria(AOB) in the top of sediment cores,with ratios of AOA to AOB of 22 and 9 at the two sites.It suggested that ammonia-oxidizing archaea may play more important roles than ammonia-oxidizing bacteria in the process of ammonia oxidation in the Pearl River Estuary sediment.The phylogenetic tree based on amoA gene sequences revealed that the amoA sequences of both AOA and AOB shared high similarity with the clones from uncultured environment.In the top sediment layer at site Q7,AOB amoA-like gene sequences were dominated by Nitrosomonas-like sequence types,which could be classified into five groups(clusters A,B,C,D and E).Cluster A accounted for 72.1% of the library.In the top sediment layer,the AOA amoA gene fell into two groups "water column/sediment" cluster(52.2%) and "soil/sediment" cluster(47.8%).But in the bottom sediment layer of Q7,most of the AOA amoA sequences(93.3%) fell into "soil/sediment" cluster,and a little part(6.7%) fell into the "water/sediment" cluster.In addition,the total amount of amoA genes in the bottom sediment was higher than that in top sediment.[Conclusion] This study helps to realize the cycle of nitrogen in Pearl River Estuary Region,and thus to provide theoretical support for the treatment of nitrogen eutrophication.展开更多
OLAND(oxygen limited autotrophic nitrification and denitrification) nitrogen removal system was constructed by coupling with oxygen limited nitritation stage and anaerobic ammonium oxidation stage. Ammonia oxidizer, a...OLAND(oxygen limited autotrophic nitrification and denitrification) nitrogen removal system was constructed by coupling with oxygen limited nitritation stage and anaerobic ammonium oxidation stage. Ammonia oxidizer, as a kind of key bacteria in N cycle, plays an important role at the oxygen limited nitritation stage of OLAND nitrogen removal system. In this study, specific amplification of 16S rDNA fragment of ammonia oxidizer by nested PCR, separation of mixed PCR samples by denaturing gradient gel electrophoresis(DGGE), and the quantification of ammonia oxidizer by fluorescence in situ hybridization(FISH) were combined to investigate the shifts of community composition and quantity of ammonia oxidizer of the oxygen limited nitritation stage in OLAND system. It showed that the community composition of ammonia oxidizer changed drastically when dissolved oxygen was decreased gradually, and the dominant ammonia oxidizer of the steady nitrite accumulation stage were completely different from that of the early stage of oxygen limited nitritation identified by DGGE . It was concluded that the Nitrosomonas may be the dominant genus of ammonia oxidizer at the oxygen limited nitritation stage of OLAND system characterized by nested PCR-DGGE and FISH, and the percentage of Nitrosomonas was 72.5% ±0.8% of ammonia oxidizer at the steady nitrite accumulation stage detected by FISH.展开更多
Ammonia oxidizing (AOB) and denitrifying bacteria (DNB) play an important role in soil nitrogen transformation in natural and agricultural ecosystems. Effects of long-term fertilization on abundance and community ...Ammonia oxidizing (AOB) and denitrifying bacteria (DNB) play an important role in soil nitrogen transformation in natural and agricultural ecosystems. Effects of long-term fertilization on abundance and community composition of AOB and DNB were studied with targeting ammonia monooxygenase (amoA) and nitrite reductase (nirK) genes using polymerase chain reaction- denaturing gradient gel electrophoresis (PCR-DGGE) and real-time PCR, respectively. A field trial with different fertilization treatments in a rice paddy from Tai Lake region, centre East China was used in this study, including no fertilizer application (NF), balanced chemical fertilizers (CF), combined organic/inorganic fertilizer of balanced chemical fertilizers plus pig manure (CFM), and plus rice straw return (CFS). The abundances and riehnesses of amoA and nirK were increased in CF, CFM and CFS compared to NF. Principle component analysis of DGGE profiles showed significant difference in nirK and amoA genes composition between organic amended (CFS and CFM) and the non-organic amended (CF and NF) plots. Number of amoA copies was significantly positively correlated with normalized soil nutrient richness (NSNR) of soil organic carbon (SOC) and total nitrogen (T-N), and that of nirK copies was with NSNR of SOC, T-N plus total phosphorus. Moreover, nitrification potential showed a positive correlation with SOC content, while a significantly lower denitrification potential was found under CFM compared to under CFS. Therefore, SOC accumulation accompanied with soil nutrient richness under long-term balanced and organic/inorganic combined fertilization promoted abundance and diversity of AOB and DNB in the rice paddy.展开更多
The short-term effects of temperature and free ammonia (FA) on ammonium oxidization were investigated in this study by operating several batch tests with two different partial nitrification aggregates, formed as eithe...The short-term effects of temperature and free ammonia (FA) on ammonium oxidization were investigated in this study by operating several batch tests with two different partial nitrification aggregates, formed as either granules or flocs. The results showed that the rate of ammonium oxidation in both cultures increased significantly as temperature increased from 10 to 30 °C. The specific ammonium oxidation rate with the granules was 2-3 times higher than that with flocs at the same temperature. Nitrification at various FA concentrations and temperatures combination exhibited obvious inhibition in ammonium oxidation rate when FA was 90 mg·L 1 and tempera- ture dropped to 10 °C in the two systems. However, the increase in substrate oxidation rate of ammonia at 30 °C was observed. The results suggested that higher reaction temperature was helpful to reduce the toxicity of FA. Granules appeared to be more tolerant to FA attributed to the much fraction of ammonia oxidizing bacteria (AOB) and higher resistance to the transfer of ammonia into the bacterial aggregates, whereas in the floc system, the bacteria distributed throughout the entire aggregate. These results may contribute to the applicability of the nitrifying granules in wastewater treatment operated at high ammonium concentration.展开更多
Zinc extraction from crude zinc oxide(CZO)is beneficial to the full utilization of secondary resources and environmental protection.In this paper,a systematic investigation was carried out to study the leaching behavi...Zinc extraction from crude zinc oxide(CZO)is beneficial to the full utilization of secondary resources and environmental protection.In this paper,a systematic investigation was carried out to study the leaching behavior of CZO by using ammonia-ammonium carbonate solution.It was found that the maximum leaching rate of zinc from CZO dust was 95.7%under the conditions of[Zn]T:[NH 3]T:[CO_(3)^(2−)]=1:7.00:1.75,liquid to solid ratio 5:1,leaching temperature 30℃ and leaching time 60 min.Compared with pure zinc oxide(PZO)leaching,the CZO leaching required longer time and more leaching agents,which is caused by the Cd^(2+),Pb^(2+) and other metal cationic impurities in CZO.The metal cationic impurities dissolved in the leaching solution and combined with ammonium to form complexes,consuming leaching agents and affecting zinc leaching.展开更多
Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assi...Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assisted co-precipitation(FP-CP)process.Compared to the Mn/Mg Al-LDO obtained via slow drop assisted coprecipitation(SD-CP)method,the Mn/Mg Al-LDO(FP-CP)has excellent activity.The Mn/Mg Al-LDO(FP-CP)catalyst was shown to possess a high NO conversion rate of 76%-100%from 25 to 150℃,which is much better than the control Mn/Mg Al-LDO(SD-CP)(29.4%-75.8%).In addition,the Mn/Mg Al-LDO(FP-CP)offered an enhanced NO conversion rate of 97%and a N2selectivity of 97.3%at 100℃;the NO conversion rate was 100%and the N2selectivity was 90%at 150℃with a GHSV of 60,000 h^-1.The Mn/Mg Al-LDO(FP-CP)catalyst exhibited a smaller fragment nano-sheet structure(sheet thickness of 7.23 nm).An apparent lattice disorder was observed in the HRTEM image confirming the presence of many defects.The H2-TPR curves show that the Mn/Mg Al-LDO(FP-CP)catalyst has abundant reducing substances.Furthermore,the enhanced surface acidity makes the NH3concentration of the Mn/Mg Al-LDO(FP-CP)catalyst lower than 100 ml·m^-3after the reaction from 25 to 400℃.This can effectively reduce the ammonia escape rate in the SCR reaction.Thus,the Mn/Mg Al-LDO(FP-CP)catalyst has potential applications in stationary industrial installations for environmentally friendly ultra-low temperature SCR.展开更多
The diversification of ammonia-oxidizing bacteria (AOB) and ammonia-oxidizing archaea (AOA) communities and their potential nitrification activity (PNA) on a large scale have not been well documented. In this work, se...The diversification of ammonia-oxidizing bacteria (AOB) and ammonia-oxidizing archaea (AOA) communities and their potential nitrification activity (PNA) on a large scale have not been well documented. In this work, seven paddy soils from different geographic regions in Sichuan, P. R. China were selected to determine the spatial distribution of the activities, abundances and community compositions of AOB and AOA. PNA varied greatly among paddy soils, and was positively correlated with soil pH (P< 0.05). The abundance of AOA was 81.1 to 1 670.0 times more than that of AOB, which indicates paddy soil environments favor the growth of AOA. Denaturing gradient gel electrophoresis fingerprints of amoA genes exhibited distinct spatial differences in AOA compositions rather than in AOB compositions. Sequencing analysis revealed that acidic soils were dominated by AOA within marine group 1.1 a-associated lineage, whereas the soil group 1.1b lineage AOA predominated in neutral and alkaline soils. Both nitrosopira cluster 3-like and Nitrosomonas cluster 7-like AOB dominated the AOB communities in the paddy soils. Redundancy analysis suggested that soil NH4^+-N content was the most significant driver determining the AOB community structure, while no significant correlation between AOA community structure and soil properties was found. The findings highlight that the activity and composition of ammonia oxidizers exhibit spatial variations in complex paddy fields due to the joint influence of soil variables associated with pH and N availability.展开更多
Electrochemical nitrate reduction to ammonia(NRA) can realize the green synthesis of ammonia(NH3) at ambient conditions, and also remove nitrate contamination in water. However, the current catalysts for NRA still fac...Electrochemical nitrate reduction to ammonia(NRA) can realize the green synthesis of ammonia(NH3) at ambient conditions, and also remove nitrate contamination in water. However, the current catalysts for NRA still face relatively low NH3yield rate and poor stability. We present here a core-shell heterostructure comprising cobalt oxide anchored on copper oxide nanowire arrays(CuO NWAs@Co_(3)O_(4)) for efficient NRA. The CuO NWAs@Co_(3)O_(4)demonstrates significantly enhanced NRA performance in alkaline media in comparison with plain CuO NWAs and Co_(3)O_(4)flocs. Especially, at-0.23 V vs. RHE, NH_(3) yield rate of the CuO NWAs@Co_(3)O_(4)reaches 1.915 mmol h^(-1)cm^(-2),much higher than those of CuO NWAs(1.472 mmol h^(-1)cm^(-2)), Co_(3)O_(4)flocs(1.222 mmol h^(-1)cm^(-2)) and recent reported Cu-based catalysts.It is proposed that the synergetic effects of the heterostructure combing atom hydrogen adsorption and nitrate reduction lead to the enhanced NRA performance.展开更多
Ammonia oxidation, the first and rate-limiting step of nitrification, is carried out by both ammonia-oxidizing bacteria (AOB) and ammonia-oxidizing archaea (AOA). However, the relative importance of AOB and AOA to...Ammonia oxidation, the first and rate-limiting step of nitrification, is carried out by both ammonia-oxidizing bacteria (AOB) and ammonia-oxidizing archaea (AOA). However, the relative importance of AOB and AOA to nitrification in terrestrial ecosystems is not well understood. The aim of this study was to investigate the effect of the nitrogen input amount on abundance and community composition of AOB and AOA in red paddy soil. Soil samples of 10-20 cm (root layer soil) and 0-5 cm (surface soil) depths were taken from a red paddy. Rice in the paddy was fertilized with different rates of N as urea of N1 (75 kg N ha" yr-1), N2 (150 kg N ha~ yrl), N3 (225 kg N ha1 yrl) and CK (without fertilizers) in 2009, 2010 and 2011. Abundance and community composition of ammonia oxidizers was analyzed by real-time PCR and denaturing gradient gel electrophoresis (DGGE) based on amoA (the unit A of ammonia monooxygenase) gene. Archaeal amoA copies in N3 and N2 were significantly (P〈0.05) higher than those in CK and N1 in root layer soil or in surface soil under tillering and heading stages of rice, while the enhancement in bacterial amoA gene copies with increasing of N fertilizer rates only took on in root layer soil. N availability and soil NO3--N content increased but soil NH4+-N content didn't change with increasing of N fertilizer rates. Otherwise, the copy numbers of archaeal amoA gene were higher (P〈0.05) than those of bacterial amoA gene in root lary soil or in surface soil. Redundancy discriminate analysis based on DGGE bands showed that there were no obvious differs in composition of AOA or AOB communities in the field among different N fertilizer rates. Results of this study suggested that the abundance of ammonia-oxidizers had active response to N fertilizer rates and the response of AOA was more obvious than that of AOB. Similarity in the community composition of AOA or AOB among different N fertilizer rates indicate that the community composition of ammonia-oxidizers was relatively stable in the paddy soil at least in short term for three years.展开更多
基金the support received from the National Natural Science Foundation of China(Grant No.22372012,22261160640,and 22002009)the Natural Science Foundation of Hunan Province(Grant No.2023JJ20037 and 2021JJ40565)the Scientific Research Project of Hunan Provincial Department of Education(Grant No.22B0293)
文摘The electrochemical coupling of biomass oxidation and nitrogen conversion presents a potential strategy for high value-added chemicals and nitrogen cycling.Herein,in this work,CuO/Co_(3)O_(4)with heterogeneous interface is successfully constructed as a bifunctional catalyst for the electrooxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid and the electroreduction of nitrate to ammonia(NH_(3)).The open-circuit potential spontaneous experiment shows that more 5-hydroxymethylfurfural molecules are adsorbed in the Helmholtz layer of the CuO/Co_(3)O_(4)composite,which certifies that the CuO/Co_(3)O_(4)heterostructure is conducive to the kinetic adsorption of 5-hydroxymethylfurfural.In situ electrochemical impedance spectroscopy further shows that CuO/Co_(3)O_(4)has faster reaction kinetics and lower reaction potential in oxygen evolution reaction and 5-hydroxymethylfurfural electrocatalytic oxidation.Moreover,CuO/Co_(3)O_(4)also has a good reduction effect on NO_(3)^(-).The ex-situ Raman spectroscopy shows that under the reduction potential,the metal oxide is reduced,and the generated Cu_(2)O can be used as a new active site for the reaction to promote the electrocatalytic conversion of NO_(3)^(-)to NH_(3) synthesis.This work provides valuable guidance for the synthesis of value-added chemicals by 5-hydroxymethylfurfural electrocatalytic oxidation coupled with NO_(3)^(-)while efficiently producing NH_(3).
基金supported by the Eleventh Five-Year Key Technology Research and Development Program in China (Grant No. 2006BAJ08B04)
文摘The electrochemical oxidation degradation processes for artificial and actual wastewater containing ammonia were carried out with a Ti/RuO2-Pt anode and a Ti plate cathode. We studied the effects of different current densities, space sizes between the two electrodes, and amounts of added NaCl on ammonia-containing wastewater treatm.ent. It was shown that, after a 30-min treatment under the optimal conditions, which were a current density of 20 mA/cm2, a space size between the two electrodes of I cm, and an added amount of 0.5 g/L of NaC1, the COD concentration in municipal wastewater was 40 mg/L, a removal rate of 90%; and the NH3-N concentration was 7 mg/L, a removal rate of 88.3%. The effluent of municipal wastewater qualified for Class A of the Discharge Standard of Pollutants for Municipal Wastewater Treatment Plant (GB 18918-2002).
基金Supported by Project for Achievement Transformation of High and New Technology in Shanghai City(201405267)
文摘The influencing factors and kinetics of oxidative degradation of ammonia nitrogen in high salinity wastewater by sodium hypochlorite oxidation( Na Cl O) were studied. The results showed that the degradation process of ammonia nitrogen by sodium hypochlorite accorded with a pseudo first-order kinetics model,and the influencing factors included Na Cl O dosage,initial concentration of ammonia nitrogen,salinity,temperature,and so on. When Na Cl O dosage was 0. 6%( MCl∶ MN= 13. 76),the reaction rate constant was up to 0. 015 75 min^(-1). The higher the initial concentration of ammonia nitrogen was,the worse the effect of oxidation reaction was. When the initial concentration did not exceed 45 mg/L,the effect on oxidation reaction rate constant increased with the increase of the initial concentration. Low salinity had no effect on ammonia nitrogen oxidation.When salinity was higher than 2. 0%,the inhibition effect on ammonia nitrogen oxidation would increase,and the reaction rate constant decreased obviously with the increase of salinity. The improvement of reaction temperature was beneficial to ammonia oxidation degradation. As temperature increased from 10 to 35 ℃,the reaction rate constant rose from 0. 00188 to 0. 01043 min^(-1).
基金the grant support from the National Natural Science Foundation of China (No. 21975018, 22278032)。
文摘Ammonia is gaining increasing attention as a green alternative fuel for achieving large-scale carbon emission reduction. Despite its potential technical prospects, the harsh ignition conditions and slow flame propagation speed of ammonia pose significant challenges to its application in engines. Non-equilibrium plasma has been identified as a promising method, but current research on plasma-enhanced ammonia combustion is limited and primarily focuses on ignition characteristics revealed by kinetic models. In this study, low-temperature and low-pressure chemistry in plasma-assisted ammonia oxidative pyrolysis is investigated by integrated studies of steady-state GC measurements and mathematical simulation. The detailed kinetic mechanism of NH_(3) decomposition in plasma-driven Ar/NH_(3) and Ar/NH_(3)/O_(2) mixtures has been developed. The numerical model has good agreements with the experimental measurements in NH_(3)/O_(2) consumption and N_(2)/H_(2) generation, which demonstrates the rationality of modelling. Based on the modelling results, species density profiles, path flux and sensitivity analysis for the key plasmaproduced species such as NH_(2), NH, H_(2), OH, H, O, O(^(1)D), O_(2)(a^(1)△_(g)), O_(2)(b^(1)∑_(g)^(+)), Ar^(*), H^(-), Ar^(+), NH_(3)^(+), O_(2)^(-) in the discharge and afterglow are analyzed in detail to illustrate the effectiveness of the active species on NH_(3) excitation and decomposition at low temperature and relatively higher E/N values. The results revealed that NH_(2), NH, H as well as H_(2) are primarily generated through the electron collision reactions e + NH_(3)→ e + NH_(2)+ H, e + NH_(3)→ e + NH + H_(2) and the excited-argon collision reaction Ar^(*) + NH_(3)+ H → Ar + NH_(2)+ 2H, which will then react with highly reactive oxidative species such as O_(2)^(*), O^(*), O, OH, and O_(2) to produce stable products of NOx and H_(2)O. NH_(3)→ NH is found a specific pathway for NH_(3) consumption with plasma assistance, which further highlights the enhanced kinetic effects.
文摘Monte Carlo method is applied to investigate the kinetics of ammonia oxidative decomposition over the commercial propylene ammoxidation catalyst(Mo-Bi). The simulation is quite in agreement with experimental results. Monte Carlo simulation proves that the process of ammonia oxidation decomposition is a two-step reaction.
基金supported by the National Natural Science Foundation of China(51978436,52000092,22272116)Fundamental Research Program of Shanxi Province(202103021224043)。
文摘In this work,the CuAl-LDO/c-CNTs catalyst was fabricated via in situ oriented assembly of layered-double hydroxides(LDHs)and citric acid-modified carbon nanotubes(c-CNTs)followed by annealing treatment,and evaluated in the selective catalytic oxidation(SCO)of NH_(3)to N_(2).The CuAl-LDO/c-CNTs catalyst presented better catalytic performance(98%NH_(3)conversion with nearly 90%N_(2)selectivity at 513 K)than other catalysts,such as CuAlO_(x)/CNTs,CuAlO_(x)/c-CNTs and CuAl-LDO/CNTs.Multiple characterizations were utilized to analyze the difference of physicochemical properties among four catalysts.XRD,TEM and XPS analyses manifested that CuO and Cu_(2)O nanoparticles dispersed well on the surface of the Cu Al-LDO/c-CNTs catalyst.Compared with other catalysts,larger specific surface area and better dispersion of CuAl-LDO/c-CNTs catalyst were conducive to the exposure of more active sites,thus improving the redox capacity of the active site and NH_(3)adsorption capacity.In-situ DRIFTS results revealed that the internal selective catalytic reduction(iSCR)mechanism was found over CuAl-LDO/c-CNTs catalyst.
基金Supported by the Project of Agricultural Key Programs for Science and Technology Development of Ningbo (2011C11006)Key Spark Program Project of Science and Technology Ministry (2012GA7010011)the Science and Technology Plan Project of Ningbo City,Zhejiang Province
文摘Active iron catalysts with 5A molecular sieve as the carrier were prepared firstly, and then were used in the treatment of ammonia nitrogen in landfill leachate pretreated by MBR by using CWPO, finally the effects of preparation process of catalysts, assistants and reaction conditions on the removal rate of ammonia nitrogen were analyzed. The results show that the preparation process of catalysts and assistants had great effects on catalytic activity; when steeping fluid concentration was 2 mol/L and 0.01 mol/L cerium nitrate was used as an assistant, Fe-Ce/5A catalyst roasted for 3 h at 400 ~C had a good catalytic effect. As 10 g of Fe-Ce/5A catalyst was added to water sample, and landfill leachate pretreated by MBR reacted with 15 ml of H2 02 for 30 min at 60 ~C, the removal rate of ammonia nitrogen was up to 90.8%, that is, ammonia nitrogen concentra- tion decreased from 253 to 23 mg/L, reaching the national emission standard. Besides, the kinetic analysis of ammonia nitrogen removal reveals that the removal reaction of ammonia nitrogen conformed with pseudo first order kinetic equation. Thus, it is feasible to use this method to deeply treat landfill leachate pretreated by MBR.
基金the Engineering and Physical Science Research Council(EPSRC),U.K.for the award of a research grant EP/J0118058/1 and postdoctoral research assistantships(PDRAs) to M.R.W.and R.W.M.from the grant。
文摘Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control,and practical ruthenium nanocatalysts are explored for ammonia synthesis.Graphite and graphitic carbons are of interest as supports for the nanocatalysts.Despite considerable literature on the catalytic processes on graphite and graphitic supports,reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood.Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation,and practical Ru nanocatalysts in ammonia synthesis,on graphite and related supports under controlled reaction environments using a novel in-situ environmental(scanning) transmission electron microscope with single atom resolution.By recording snapshots of the reaction dynamics,the behaviour of the catalysts is imaged.The images reveal single metal atoms,clusters of a few atoms on the graphitic supports and the support function.These all play key roles in the mobility,sintering and growth of the catalysts.The experimental findings provide new structural insights into atomic scale reaction dynamics,morphology and stability of the nanocatalysts.
文摘Ammonia (NH<sub>3</sub>) dissociation and oxidation in a cylindrical quartz reactor has been experimentally studied for various inlet NH<sub>3</sub> concentrations (5%, 10%, and 15%) and reactor temperatures between 700 K and 1000 K. The thermal effects during both NH<sub>3</sub> dissociation (endothermic) and oxidation (exothermic) were observed using a bundle of thermocouples positioned along the central axis of the quartz reactor, while the corresponding NH<sub>3</sub> conversions and nitrogen oxides emissions were determined by analysing the gas composition of the reactor exit stream. A stronger endothermic effect, as indicated by a greater temperature drop during NH<sub>3</sub> dissociation, was observed as the NH<sub>3</sub> feed concentration and reactor temperature increased. During NH<sub>3</sub> oxidation, a predominantly greater exothermic effect with increasing NH<sub>3</sub> feed concentration and reactor temperature was also evident;however, it was apparent that NH<sub>3</sub> dissociation occurred near the reactor inlet, preceding the downstream NH<sub>3</sub> and H<sub>2</sub> oxidation. For both NH<sub>3</sub> dissociation and oxidation, NH<sub>3</sub> conversion increased with increasing temperature and decreasing initial NH<sub>3</sub> concentration. Significant levels of NO<sub>X</sub> emissions were observed during NH<sub>3</sub> oxidation, which increased with increasing temperature. From the experimental results, it is speculated that the stainless-steel in the thermocouple bundle may have catalysed NH<sub>3</sub> dissociation and thus changed the reaction chemistry during NH<sub>3</sub> oxidation.
文摘By making the use of the processes which includes separating trash and solid materials from the wastewater-ammonia stripping tower-UASB-biological oxidation pond, we have treated the wastewater which comes from the swine factory. The treated wastewater can meet the primary standard of The People's Republic of China based on sewage discharge standards and the wastewater treatment project design contract (GBl8596-2001), and the effluent will be used as irrigation-water. We introduce this project including the quality of influent and effluent and the flow scheme, the statement of every part, the investment and the effect, etc. The operation indicated that this process has many merits such as the stability in operation-effect and the convenience in management. So it will provide some help for the similar wastewater treatment.
文摘Organic carbon,inorganic carbon,temperature,p H and ORP are all to have a certain influence on the anaerobic ammonia oxidation reaction.We can draw some conclusions on the optimum conditions of anaerobic ammonia oxidation reaction.The optimum temperature of the anaerobic ammonia oxidation reaction is 30-35℃.And the optimum p H of the anaerobic ammonia reaction is 7.5-8.3.The presence of organic matters can affect the anaerobic ammonia reaction,and different organic matters have different influence on it.The concentration of the inorganic carbon also exist great influence on the reaction.High inorganic carbon concentration also can inhibit anaerobic ammonia oxidation reaction.
基金Supported by National Natural Science Foundation of China(40532011)~~
文摘[Objective] This study aimed to investigate the abundance and composition of ammonia-oxidizing bacteria and ammonia-oxidizing archaea in Pearl River Estuary sediment.[Method] Firstly,the amoA gene library was constructed;then based on that,the content and diversity of amoA genes of ammonia-oxidizing bacteria and ammonia-oxidizing archaea in Pearl River Estuary sediment were detected by using quantitative real-time polymerase chain reaction(Q-PCR).[Result] The results of Q-PCR presented that ammonia-oxidizing archaea(AOA) were more abundant than ammonia-oxidizing bacteria(AOB) in the top of sediment cores,with ratios of AOA to AOB of 22 and 9 at the two sites.It suggested that ammonia-oxidizing archaea may play more important roles than ammonia-oxidizing bacteria in the process of ammonia oxidation in the Pearl River Estuary sediment.The phylogenetic tree based on amoA gene sequences revealed that the amoA sequences of both AOA and AOB shared high similarity with the clones from uncultured environment.In the top sediment layer at site Q7,AOB amoA-like gene sequences were dominated by Nitrosomonas-like sequence types,which could be classified into five groups(clusters A,B,C,D and E).Cluster A accounted for 72.1% of the library.In the top sediment layer,the AOA amoA gene fell into two groups "water column/sediment" cluster(52.2%) and "soil/sediment" cluster(47.8%).But in the bottom sediment layer of Q7,most of the AOA amoA sequences(93.3%) fell into "soil/sediment" cluster,and a little part(6.7%) fell into the "water/sediment" cluster.In addition,the total amount of amoA genes in the bottom sediment was higher than that in top sediment.[Conclusion] This study helps to realize the cycle of nitrogen in Pearl River Estuary Region,and thus to provide theoretical support for the treatment of nitrogen eutrophication.
文摘OLAND(oxygen limited autotrophic nitrification and denitrification) nitrogen removal system was constructed by coupling with oxygen limited nitritation stage and anaerobic ammonium oxidation stage. Ammonia oxidizer, as a kind of key bacteria in N cycle, plays an important role at the oxygen limited nitritation stage of OLAND nitrogen removal system. In this study, specific amplification of 16S rDNA fragment of ammonia oxidizer by nested PCR, separation of mixed PCR samples by denaturing gradient gel electrophoresis(DGGE), and the quantification of ammonia oxidizer by fluorescence in situ hybridization(FISH) were combined to investigate the shifts of community composition and quantity of ammonia oxidizer of the oxygen limited nitritation stage in OLAND system. It showed that the community composition of ammonia oxidizer changed drastically when dissolved oxygen was decreased gradually, and the dominant ammonia oxidizer of the steady nitrite accumulation stage were completely different from that of the early stage of oxygen limited nitritation identified by DGGE . It was concluded that the Nitrosomonas may be the dominant genus of ammonia oxidizer at the oxygen limited nitritation stage of OLAND system characterized by nested PCR-DGGE and FISH, and the percentage of Nitrosomonas was 72.5% ±0.8% of ammonia oxidizer at the steady nitrite accumulation stage detected by FISH.
基金supported by the National Natural Science Foundation of China(40830528 and 40710019002)
文摘Ammonia oxidizing (AOB) and denitrifying bacteria (DNB) play an important role in soil nitrogen transformation in natural and agricultural ecosystems. Effects of long-term fertilization on abundance and community composition of AOB and DNB were studied with targeting ammonia monooxygenase (amoA) and nitrite reductase (nirK) genes using polymerase chain reaction- denaturing gradient gel electrophoresis (PCR-DGGE) and real-time PCR, respectively. A field trial with different fertilization treatments in a rice paddy from Tai Lake region, centre East China was used in this study, including no fertilizer application (NF), balanced chemical fertilizers (CF), combined organic/inorganic fertilizer of balanced chemical fertilizers plus pig manure (CFM), and plus rice straw return (CFS). The abundances and riehnesses of amoA and nirK were increased in CF, CFM and CFS compared to NF. Principle component analysis of DGGE profiles showed significant difference in nirK and amoA genes composition between organic amended (CFS and CFM) and the non-organic amended (CF and NF) plots. Number of amoA copies was significantly positively correlated with normalized soil nutrient richness (NSNR) of soil organic carbon (SOC) and total nitrogen (T-N), and that of nirK copies was with NSNR of SOC, T-N plus total phosphorus. Moreover, nitrification potential showed a positive correlation with SOC content, while a significantly lower denitrification potential was found under CFM compared to under CFS. Therefore, SOC accumulation accompanied with soil nutrient richness under long-term balanced and organic/inorganic combined fertilization promoted abundance and diversity of AOB and DNB in the rice paddy.
基金Supported by the Project of Scientific Research Base and Scientific Innovation Platform of Beijing Municipal Education CommissionNational Key Science and Technology Special Projects
文摘The short-term effects of temperature and free ammonia (FA) on ammonium oxidization were investigated in this study by operating several batch tests with two different partial nitrification aggregates, formed as either granules or flocs. The results showed that the rate of ammonium oxidation in both cultures increased significantly as temperature increased from 10 to 30 °C. The specific ammonium oxidation rate with the granules was 2-3 times higher than that with flocs at the same temperature. Nitrification at various FA concentrations and temperatures combination exhibited obvious inhibition in ammonium oxidation rate when FA was 90 mg·L 1 and tempera- ture dropped to 10 °C in the two systems. However, the increase in substrate oxidation rate of ammonia at 30 °C was observed. The results suggested that higher reaction temperature was helpful to reduce the toxicity of FA. Granules appeared to be more tolerant to FA attributed to the much fraction of ammonia oxidizing bacteria (AOB) and higher resistance to the transfer of ammonia into the bacterial aggregates, whereas in the floc system, the bacteria distributed throughout the entire aggregate. These results may contribute to the applicability of the nitrifying granules in wastewater treatment operated at high ammonium concentration.
基金Project(2020YFC1909805)supported by the National Key Research and Development Program of ChinaProjects(51504293,51574284)supported by the National Natural Science Foundation of China+2 种基金Project(2018-GX-A7)supported by Qinghai Provincial Major Scientific and Technological Special Project of ChinaProject(2020SK2125)supported by the Key Research and Development Program of Hunan Province,ChinaProject(CSUZC202129)supported by Open Sharing Fund for the Large-scale Instruments and Equipments of Central South University,China。
文摘Zinc extraction from crude zinc oxide(CZO)is beneficial to the full utilization of secondary resources and environmental protection.In this paper,a systematic investigation was carried out to study the leaching behavior of CZO by using ammonia-ammonium carbonate solution.It was found that the maximum leaching rate of zinc from CZO dust was 95.7%under the conditions of[Zn]T:[NH 3]T:[CO_(3)^(2−)]=1:7.00:1.75,liquid to solid ratio 5:1,leaching temperature 30℃ and leaching time 60 min.Compared with pure zinc oxide(PZO)leaching,the CZO leaching required longer time and more leaching agents,which is caused by the Cd^(2+),Pb^(2+) and other metal cationic impurities in CZO.The metal cationic impurities dissolved in the leaching solution and combined with ammonium to form complexes,consuming leaching agents and affecting zinc leaching.
基金supported by Science and Technology Innovation Talents Program of Bingtuan(No.2019CB025)Major Scientific and Technological Project of Bingtuan(No.2018AA002)。
文摘Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assisted co-precipitation(FP-CP)process.Compared to the Mn/Mg Al-LDO obtained via slow drop assisted coprecipitation(SD-CP)method,the Mn/Mg Al-LDO(FP-CP)has excellent activity.The Mn/Mg Al-LDO(FP-CP)catalyst was shown to possess a high NO conversion rate of 76%-100%from 25 to 150℃,which is much better than the control Mn/Mg Al-LDO(SD-CP)(29.4%-75.8%).In addition,the Mn/Mg Al-LDO(FP-CP)offered an enhanced NO conversion rate of 97%and a N2selectivity of 97.3%at 100℃;the NO conversion rate was 100%and the N2selectivity was 90%at 150℃with a GHSV of 60,000 h^-1.The Mn/Mg Al-LDO(FP-CP)catalyst exhibited a smaller fragment nano-sheet structure(sheet thickness of 7.23 nm).An apparent lattice disorder was observed in the HRTEM image confirming the presence of many defects.The H2-TPR curves show that the Mn/Mg Al-LDO(FP-CP)catalyst has abundant reducing substances.Furthermore,the enhanced surface acidity makes the NH3concentration of the Mn/Mg Al-LDO(FP-CP)catalyst lower than 100 ml·m^-3after the reaction from 25 to 400℃.This can effectively reduce the ammonia escape rate in the SCR reaction.Thus,the Mn/Mg Al-LDO(FP-CP)catalyst has potential applications in stationary industrial installations for environmentally friendly ultra-low temperature SCR.
基金Funded by the National Natural Science Foundation of China (No.41606142)the Fundamental Research Funds of China West Normal University (No.463140 and No.412554)
文摘The diversification of ammonia-oxidizing bacteria (AOB) and ammonia-oxidizing archaea (AOA) communities and their potential nitrification activity (PNA) on a large scale have not been well documented. In this work, seven paddy soils from different geographic regions in Sichuan, P. R. China were selected to determine the spatial distribution of the activities, abundances and community compositions of AOB and AOA. PNA varied greatly among paddy soils, and was positively correlated with soil pH (P< 0.05). The abundance of AOA was 81.1 to 1 670.0 times more than that of AOB, which indicates paddy soil environments favor the growth of AOA. Denaturing gradient gel electrophoresis fingerprints of amoA genes exhibited distinct spatial differences in AOA compositions rather than in AOB compositions. Sequencing analysis revealed that acidic soils were dominated by AOA within marine group 1.1 a-associated lineage, whereas the soil group 1.1b lineage AOA predominated in neutral and alkaline soils. Both nitrosopira cluster 3-like and Nitrosomonas cluster 7-like AOB dominated the AOB communities in the paddy soils. Redundancy analysis suggested that soil NH4^+-N content was the most significant driver determining the AOB community structure, while no significant correlation between AOA community structure and soil properties was found. The findings highlight that the activity and composition of ammonia oxidizers exhibit spatial variations in complex paddy fields due to the joint influence of soil variables associated with pH and N availability.
基金the financial support from National Natural Science Foundation of China (No. 21972102)National Key Research and Development Program of China (2021YFA0910400)+3 种基金Natural Science Foundation of Jiangsu Province (BK20200991)Suzhou Science and Technology Planning Project (SS202016)the USTS starting fund (No.332012104)the Natural Science Foundation of Suzhou University of Science and Technology (No.342134401)。
文摘Electrochemical nitrate reduction to ammonia(NRA) can realize the green synthesis of ammonia(NH3) at ambient conditions, and also remove nitrate contamination in water. However, the current catalysts for NRA still face relatively low NH3yield rate and poor stability. We present here a core-shell heterostructure comprising cobalt oxide anchored on copper oxide nanowire arrays(CuO NWAs@Co_(3)O_(4)) for efficient NRA. The CuO NWAs@Co_(3)O_(4)demonstrates significantly enhanced NRA performance in alkaline media in comparison with plain CuO NWAs and Co_(3)O_(4)flocs. Especially, at-0.23 V vs. RHE, NH_(3) yield rate of the CuO NWAs@Co_(3)O_(4)reaches 1.915 mmol h^(-1)cm^(-2),much higher than those of CuO NWAs(1.472 mmol h^(-1)cm^(-2)), Co_(3)O_(4)flocs(1.222 mmol h^(-1)cm^(-2)) and recent reported Cu-based catalysts.It is proposed that the synergetic effects of the heterostructure combing atom hydrogen adsorption and nitrate reduction lead to the enhanced NRA performance.
基金the National Natural Science Foundation of China(40801097)the Natural Science Foundation of Fujian Province,China(2012J01107)
文摘Ammonia oxidation, the first and rate-limiting step of nitrification, is carried out by both ammonia-oxidizing bacteria (AOB) and ammonia-oxidizing archaea (AOA). However, the relative importance of AOB and AOA to nitrification in terrestrial ecosystems is not well understood. The aim of this study was to investigate the effect of the nitrogen input amount on abundance and community composition of AOB and AOA in red paddy soil. Soil samples of 10-20 cm (root layer soil) and 0-5 cm (surface soil) depths were taken from a red paddy. Rice in the paddy was fertilized with different rates of N as urea of N1 (75 kg N ha" yr-1), N2 (150 kg N ha~ yrl), N3 (225 kg N ha1 yrl) and CK (without fertilizers) in 2009, 2010 and 2011. Abundance and community composition of ammonia oxidizers was analyzed by real-time PCR and denaturing gradient gel electrophoresis (DGGE) based on amoA (the unit A of ammonia monooxygenase) gene. Archaeal amoA copies in N3 and N2 were significantly (P〈0.05) higher than those in CK and N1 in root layer soil or in surface soil under tillering and heading stages of rice, while the enhancement in bacterial amoA gene copies with increasing of N fertilizer rates only took on in root layer soil. N availability and soil NO3--N content increased but soil NH4+-N content didn't change with increasing of N fertilizer rates. Otherwise, the copy numbers of archaeal amoA gene were higher (P〈0.05) than those of bacterial amoA gene in root lary soil or in surface soil. Redundancy discriminate analysis based on DGGE bands showed that there were no obvious differs in composition of AOA or AOB communities in the field among different N fertilizer rates. Results of this study suggested that the abundance of ammonia-oxidizers had active response to N fertilizer rates and the response of AOA was more obvious than that of AOB. Similarity in the community composition of AOA or AOB among different N fertilizer rates indicate that the community composition of ammonia-oxidizers was relatively stable in the paddy soil at least in short term for three years.