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
Anaerobic ammonium oxidation (ANAMMOX) technology has potential technical superiority and economical efficiency for the nitrogen removal from landfill leachate, which contains high-strength ammonium nitrogen (NH4^...Anaerobic ammonium oxidation (ANAMMOX) technology has potential technical superiority and economical efficiency for the nitrogen removal from landfill leachate, which contains high-strength ammonium nitrogen (NH4^+-N) and refractory organics. To complete the ANAMMOX process, a preceding partial nitritation step to produce the appropriate ratio of nitrite/ammonium is a key stage. The objective of this study was to determine the optimal conditions to acquire constant partial nitritation for landfill leachate treatment, and a bench scale fixed bed bio-film reactor was used in this study to investigate the effects of the running factors on the partial nitritation. The results showed that both the dissolved oxygen (DO) concentration and the ammonium volumetric loading rate (Nv) had effects on the partial nitritation. In the controlling conditions with a temperature of 30±1℃, Nv of 0.2-1.0 kg NH4+-N/(m^3·d), and DO concentration of 0.8-2.3 mg/L, the steady partial nitritation was achieved as follows: more than 94% partial nitritation efficiency (nitrite as the main product), 60%-74% NH4^+-N removal efficiency, and NO2^--N/NH4^+-N ratio (concentration ratio) of 1.0-1.4 in the effluent.The impact of temperature was related to Nv at certain DO concentration, and the temperature range of 25-30℃ was suitable for treating high strength ammonium leachate. Ammonium-oxidizing bacteria (AOB) could be acclimated to higher FA (free ammonium) in the range of 122-224 mg/L. According to the denaturing gradient gel electrophoresis analysis result of the bio-film in the reactor, there were 25 kinds of 16S rRNA gene fragments, which indicated that abundant microbial communities existed in the bio-film, although high concentrations of ammonium and FA may inhibit the growth of the nitrite-oxidizing bacteria (NOB) and other microorganisms in the reactor.展开更多
Modeling for nitritation process was discussed and analyzed quantitatively for the factors that influence nitrite accumulation. The results indicated that pH, inorganic carbon source and Hydraulic Retention Time(HRT) ...Modeling for nitritation process was discussed and analyzed quantitatively for the factors that influence nitrite accumulation. The results indicated that pH, inorganic carbon source and Hydraulic Retention Time(HRT) as well as biomass concentration are the main factors that influenced the conversion ratio of ammonium to nitrite. A constant high pH can lead to a high nitritation rate and results in high conversion ratio on condition that free ammonia inhibition do not happen. In a CSTR system, without pH control, this conversion ratio can be monitored by pH variation in the reactor. The pH goes down far from the inlet level means a strongly nitrite accumulation. High concentration of alkalinity can promoted the conversion ratio by means of accelerating the nitritation rate through providing sufficient inorganic carbon source(carbon dioxide). When inorganic carbon source was depleted, the nitritation process stopped. HRT adjustment could be an efficient way to make the nitritation system run more flexible, which to some extent can meet the requirements of the fluctuant of inlet parameters such as ammonium concentration, pH, and temperature and so on. Biomass concentration is the key point, especially for a CSTR system in steady state, which was normally circumscribed by the characteristics of bacteria and may also affected by aeration mode and can be increased by prolonging the HRT on the condition of no nitrate accumulation when no recirculation available. The higher the biomass concentration is, the better the nitrite accumulation can be obtained.展开更多
This study employed multispectral techniques to evaluate fulvic acid(FA)compositional characteristic and elucidate its biodegradation mechanisms during partial nitritation(PN)process.Results showed that FA removal eff...This study employed multispectral techniques to evaluate fulvic acid(FA)compositional characteristic and elucidate its biodegradation mechanisms during partial nitritation(PN)process.Results showed that FA removal efficiency(FRE)decreased from 90.22 to 23.11%when FA concentrations in the reactor were increased from 0 to 162.30 mg/L,and that molecular size,degree of aromatization and humification of the effluent FA macromolecules all increased after treatment.Microbial population analysis indicated that the proliferation of the Comamonas,OLB12 and Thauera exhibit high FA utilization capacity in lower concentrations(<50.59 mg/L),promoting the degradation and removal of macromolecular FA.In addition,the sustained increase in external FA may decrease the abundance of above functional microorganisms,resulting in a rapid drop in FRE.Furthermore,from the genetic perspective,the elevated FA levels restricted carbohydrate(ko00620,ko00010 and ko00020)and nitrogen(HAO,AMO,NIR and NOR)metabolism-related pathways,thereby impeding FA removal and total nitrogen loss associated with N_(2)O emissions.展开更多
In this study,a modified continuous-flow nitrifying reactor was successfully operated for rapid cultivation of micro-granules and achieving robust nitritation.Results showed that sludge granulation with mean size of c...In this study,a modified continuous-flow nitrifying reactor was successfully operated for rapid cultivation of micro-granules and achieving robust nitritation.Results showed that sludge granulation with mean size of ca.100μm was achieved within three weeks by gradually increasing settling velocity-based selection pressure from 0.48 to 0.9 m/hr.Though Nitrospira like nitrite-oxidizing bacteria(NOB)were enriched in the micro-granules with a ratio between ammonia-oxidizing bacteria(AOB)and NOB of 5.7%/6.5% on day 21,fast nitritation was achieved within one-week by gradually increasing of influent ammonium concentration(from 50 to 200 mg/L).Maintaining ammonium in-excess was the key for repressing NOB in the micro-granules.Interestingly,when the influent ammonium concentration switched back to 50 mg/L still with the residual ammonium of 15–25 mg/L,the nitrite accumulation efficiency increased from 90%to 98%.Experimental results suggested that the NOB repression was intensified by both oxygen and nitrite unavailability in the inner layers of micro-granules.Unexpectedly,continuous operation with ammonium in excess resulted in overproduction of extracellular polysaccharides and overgrowth of some bacteria(e.g.,Nitrosomonas,Arenimonas,and Flavobacterium),which deteriorated the micro-granule stability and drove the micro-granules aggregation into larger ones with irregular morphology.However,efficient nitritation was stably maintained with extremely high ammonium oxidation potential(>50 mg/g VSS/hr)and nearly complete washout of NOB was obtained.This suggested that smooth and spherical granule was not a prerequisite for achieving NOB wash-out and maintaining effective nitritation in the granular reactor.Overall,the microgranules exhibited a great practical potential for high-rate nitritation.展开更多
Residual ammonium is a critical parameter affecting the stability of mainstream partial nitritation/anammox(PN/A), but the underlying mechanism remains unclear. In this study,mainstream PN/A was established and operat...Residual ammonium is a critical parameter affecting the stability of mainstream partial nitritation/anammox(PN/A), but the underlying mechanism remains unclear. In this study,mainstream PN/A was established and operated with progressively decreasing residual ammonium. PN/A deteriorated as the residual ammonium decreased to below 5 mg/L, and this was paralleled by a significant loss in anammox activity in situ and an increasing nitrite oxidation rate. Further analysis revealed that the low-ammonium condition directly decreased anammox activity in situ via two distinct mechanisms. First, anammox bacteria were located in the inner layer of the granular sludge, and thus were disadvantageous when competing for ammonium with ammonium-oxidizing bacteria(AOB) in the outer layer. Second, the complete ammonia oxidizer(comammox) was enriched at low residual ammonium concentrations because of its high ammonium affinity. Both AOB and comammox presented kinetic advantages over anammox bacteria. At high residual ammonium concentrations,nitrite-oxidizing bacteria(NOB) were effectively suppressed, even when their maximum activity was high due to competition for nitrite with anammox bacteria. At low residual ammonium concentrations, the decrease in anammox activity in situ led to an increase in nitrite availability for nitrite oxidation, facilitating the activation of NOB despite the dissolved oxygen limitation(0.15–0.35 mg/L) for NOB persisting throughout the operation. Therefore, the deterioration of mainstream PN/A at low residual ammonium was primarily triggered by a decline in anammox activity in situ. This study provides novel insights into the optimized design of mainstream PN/As in engineering applications.展开更多
The long-term impact of fulvic acid(FA)on partial nitritation(PN)systemwas initially examined in this study.The obtained results revealed that the FA lower than 50 mg/L had negligible effect on the nitrite accumulatio...The long-term impact of fulvic acid(FA)on partial nitritation(PN)systemwas initially examined in this study.The obtained results revealed that the FA lower than 50 mg/L had negligible effect on the nitrite accumulation rate(NAR nearly 100%)and ammonium removal rate(ARR 56.85%),while FA over 50 mg/L decreased ARR from 56.85%to 0.7%.Sludge characteristics analysis found that appropriate FA(<50 mg/L)exposure promoted the settling performance and granulation of PN sludge by removing Bacteroidetes and accumulating Chloroflexi.The analysis of metagenomics suggested that the presence of limited FA(0-50 mg/L)stimulated the generation of NADH,which favors the denitrification and nitrite reduction.The negative impact of FA on the PN system could be divided into two stages.Initially,limited FA(50-120 mg/L)was decomposed by Anaerolineae to stimulate the growth and propagation of heterotrophic bacteria(Thauera).Increasing heterotrophs competed with AOB(Nitrosomonas)for dissolved oxygen,causing AOB to be eliminated and ARR to declined.Subsequently,when FA dosage was over 120 mg/L,Anaerolineae were inhibited and heterotrophic bacteria reduced,resulting in the abundance of AOB recovered.Nevertheless,the ammonium transformation pathway was suppressed because genes amoABC and hao were obviously reduced,leading to the deterioration of reactor performance.Overall,these results provide theoretical guidance for the practical application of PN for the treatment of FA-containing sewage.展开更多
A continuous flow bioreactor was operated for 300 days to investigate partial nitritation(PN)of mature landfill leachate,establishing the long-term performance of the system in terms of the microbial community composi...A continuous flow bioreactor was operated for 300 days to investigate partial nitritation(PN)of mature landfill leachate,establishing the long-term performance of the system in terms of the microbial community composition,evolution,and interactions.The stable operation phase(31-300 d)began after a 30 days of start-up period,reaching an average nitrite accumulation ratio(NAR)of 94.43%and a ratio of nitrite nitrogen to ammonia nitrogen(NO_(2)^(−)-N/NH_(4)^(+)-N)of 1.16.Some fulvic-like and humic-like compounds and proteins were effectively degraded in anaerobic and anoxic tanks,which was consistent with the corresponding abundance of methanogens and syntrophic bacteria in the anaerobic tank,and organic matter degrading bacteria in the anoxic tank.The ammonia-oxidizing bacteria(AOB)Nitrosomonas was found to be the key functional bacteria,exhibiting an increase in abundance from 0.27%to 6.38%,due to its collaborative interactions with organic matter degrading bacteria.In-situ inhibition of nitrite-oxidizing bacteria(NOB)was achieved using a combination of free ammonia(FA)and free nitrous acid(FNA),low dissolved oxygen(DO)with fewer bioavailable organics conditions were employed to maintain stable PN and a specific ratio of NO_(2)^(−)-N/NH_(4)^(+)-N,without an adverse impact on AOB.The synergistic relationships between AOB and both denitrifying bacteria and organic matter degrading bacteria,were found to contribute to the enhanced PN performance and microbial community structure stability.These findings provide a theoretical guidance for the effective application of PN-Anammox for mature landfill leachate treatment.展开更多
Sanchuan ham is appreciated in Yunnan Province,China,for its characteristic flavor and taste,while the microbial community structure and biogenic amines content remain unclear during fermentation processes.In this stu...Sanchuan ham is appreciated in Yunnan Province,China,for its characteristic flavor and taste,while the microbial community structure and biogenic amines content remain unclear during fermentation processes.In this study,we explored the physicochemical property,biogenic amines concentration and microbial diversity of external and internal Sanchuan ham by high-throughput sequencing during the processing of Sanchuan ham.Results showed that the nitrite remained at a stable level of 0.15 mg/kg which was significantly lower than the national health standard safety level of 20 mg/kg.In addition,compared with fresh hams,the content of total free amino acids in ripe Sanchuan ham has grown 14 folds;sour and bitter were the main tastes of Sanchuan ham.Notably,the concentration of cadaverine was the highest of all biogenic amines during the entire fermentation period.At the bacterial phyla level,Firmicutes and Actinobacteria were the two main phyla,while at the genus level,Staphylococcus was a significant strain throughout the whole fermentation.Moreover,the dry stage has a great impact on the succession change of microbial community structure.Simultaneously,the change trends and composition of bacteria in the interior have slight discrepancies with those of the exterior of Sanchuan ham.展开更多
The amount of piggery wastewater as domestic livestock is increasing.The volume of piggery wastewater produced is less than the volume of other wastewaters,but piggery wastewater has a heavy impact on wastewater strea...The amount of piggery wastewater as domestic livestock is increasing.The volume of piggery wastewater produced is less than the volume of other wastewaters,but piggery wastewater has a heavy impact on wastewater streams due to an extremely high concentration of nitrogen and COD.In this study,laboratory reactors were operated using piggery wastewater and the effluent of anaerobic digester from piggery wastewater plants.The purpose of this study was to induce the nitritation process,which is an economically advantageous nitrogen removal method that converts ammonium nitrogen into nitrite.The results showed that the effluent of anaerobic digester from piggery wastewater was more efficient than raw piggery wastewater in terms of inducing nitritation.It can be deduced that nitritation is largely affected by an organic fraction of piggery wastewater.It can also be concluded that a small amount of biodegradable organic matter in piggery wastewater is efficient in inducing nitritation.展开更多
Free ammonia(FA) inhibition on nitrite-oxidized bacteria(NOB) and real-time control are used to achieve nitrogen removal from landfill leachate via nitrite pathway at low temperatures in sequencing batch reactor. ...Free ammonia(FA) inhibition on nitrite-oxidized bacteria(NOB) and real-time control are used to achieve nitrogen removal from landfill leachate via nitrite pathway at low temperatures in sequencing batch reactor. The inhibition of FA on NOB activity during the aerobic period was prolonged using real-time control. The degree of nitrite accumulation was monitored along with variations of the ammonia-oxidizing bacteria and NOB population using fluorescence in situ hybridization techniques. It is demonstrated that the end-point of ammonia oxidization is detected from the on-line measured dissolved oxygen,oxidization–reduction potential, and p H signals, which could avoid the loss the FA inhibition on NOB caused by excess aeration. At low temperature(13.0–17.6°C), the level of nitrite pathway rapidly increased from 19.8% to 90%, suggesting that nitritation was successfully started up at low temperature by applying syntrophic association of the FA inhibition and real-time control, and then this high level of nitrite pathway was stably maintained for as long as 233 days. Mechanism analysis shows that the establishment of nitritation was primarily the result of predominant ammonia-oxidizing bacteria developed in the nitrifying bacteria population compared to NOB. This was mainly due to a gradual reduction of nitrite amount that is available to provide energy for the growth of NOB,eventually leading to the elimination of NOB from the bacterial clusters in sequencing batch reactor sludge system.展开更多
Biological nitrogen removal process could be affected due to the presence of heavy metals owing to their toxicity and accumulation in the sludge.In this study,the impact of Cu2+shock on a long-term nitritation operati...Biological nitrogen removal process could be affected due to the presence of heavy metals owing to their toxicity and accumulation in the sludge.In this study,the impact of Cu2+shock on a long-term nitritation operation was investigated in an air-lift reactor with selfrecirculation.Both the dynamics of microbial community and inhibition kinetics under Cu2+stress were ascertained.The results showed that Cu2+exerted severe inhibition on nitritation performance of an air-lift reactor(ALR)at 25 mg/L.The corresponding NH4+-N removal efficiency decreased to below 50%,which was mainly due to the variation of microbial community structure,especially the inhibition of nitrifiers like Nitrosomonas(the relative abundance decreased from 30%to 1%after Cu2+inhibition).Kinetic parameters were obtained and compared after fitting the Haldane model.The long-term Cu2+stress on the ALR aggravated the ammonium affinity and the resistance to substrate self-inhibition of the nitritation sludge,but reduced the resistance to Cu2+inhibition.Furthermore,Cu2+acted as uncompetitive inhibitor on nitritation process.Our results provide new insights into the nitritation characteristics under long-term Cu2+stress.展开更多
The objective of this study was to investigate the nitritation performance in a biofilm reactor for treating domestic wastewater.The reactor was operated in continuous feed mode from phases 1 to 3.The dissolved oxygen...The objective of this study was to investigate the nitritation performance in a biofilm reactor for treating domestic wastewater.The reactor was operated in continuous feed mode from phases 1 to 3.The dissolved oxygen(DO)was controlled at 3.5–7 mg/L throughout the experiment.The biofilm reactor showed excellent nitritation performance after the inoculation of nitrifying sludge,with the hydraulic retention time being reduced from 24 to 7 hr.Above 90%nitrite accumulation ratio(NAR)was maintained in phase 1.Afterwards,nitratation occurred with the low NH4^+–N concentration in the reactor.The improvement of NH4^+–N concentration to 20–35 mg/L had a limited effect on the recovery of nitritation.However,nitritation recovered rapidly when sequencing batch feed mode was adopted in phase 4,with the effluent NH4^+-N concentration above 7 mg/L.The improvement of ammonia oxidizing bacteria(AOB)activity and the combined inhibition effect of free ammonia(FA)and free nitrous acid(FNA)on the nitrite oxidizing bacteria(NOB)were two key factors for the rapid recovery of nitritation.Sludge activity was obtained in batch tests.The results of batch tests had a good relationship with the long term operation performance of the biofilm reactor.展开更多
A combined nitritation–anammox reactor was developed to treat the digestion supernatant under various C/N ratios. Due to the difficulties for heterotroph to utilize the refractory organics, the reactor presented rela...A combined nitritation–anammox reactor was developed to treat the digestion supernatant under various C/N ratios. Due to the difficulties for heterotroph to utilize the refractory organics, the reactor presented relatively stable performance with increasing supernatant addition. Nevertheless, the adverse effects of supernatant would accumulate during the long-term operation and thus weakened the activity and shock resistance of microbes,which further led to the gradual decrease of reactor performance after 92 days' operation.Under this circumstance, supernatant with volatile fatty acids(VFAs) residuals was further introduced into the reactor to investigate the performance of combined nitritation–anammox process with VFA addition. With the appearance of VFAs, the nitrogen removal performance gradually restored and the reactor finally achieved stable and efficient performance with C/N ratio of 0.35. The VFA residuals within 150 mg/L in the supernatant served as the extra electron donors and stimulated the heterotrophic denitrification process, which was vital for the enhancement of reactor. The nitrogen removal rate and total nitrogen removal efficiency reached 0.49 kg N/(m^3·day) and 88.8% after 140 days' operation, respectively. The combined nitritation–anammox reactor was proved suitable to treat digestion supernatant.展开更多
The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving t...The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving the NH_(3) selectivity is to facilitate adsorption and activation of NO_(2)^(−),which is generally undesirable in unitary species.In this work,an efficient NO_(2)^(−)RR catalyst is constructed by cooperating Pd with In2O3,in which NO_(2)^(−)could adsorb on interfacial dual-site through“Pd–N–O–In”linkage,leading to strengthened NO_(2)^(−)adsorption and easier N=O bond cleavage than that on unitary Pd or In2O3.Moreover,the Pd/In_(2)O_(3)composite exhibits moderate H^(*)adsorption,which may facilitate protonation kinetics while inhibiting competitive HER.As a result,it exhibits a fairly high NH_(3)yield rate of 622.76 mmol h^(−1)g^(−1)cat with a Faradaic efficiency(FE)of 95.72%,good selectivity of 91.96%,and cycling stability towards the NO_(2)^(−)RR,surpassing unitary In_(2)O_(3)and Pd/C electrocatalysts.Besides,computed results indicate that NH_(3)production on Pd/In_(2)O_(3)follows the deoxidation to hydrogenation pathway.This work highlights the significance of H^(*)and NO_(2)^(−)adsorption modulation and N=O activation in NO_(2)^(−)RR electrochemistry by creating synergy between a mediocre catalyst with an appropriate cooperator.展开更多
Human saliva is an indispensable fluid that maintains a healthy oral cavity which otherwise can lead to oral diseases(dental caries and periodontitis).In addition,salivary metabolites and microbiome profile provide ea...Human saliva is an indispensable fluid that maintains a healthy oral cavity which otherwise can lead to oral diseases(dental caries and periodontitis).In addition,salivary metabolites and microbiome profile provide early detection of systemic diseases such as cancer and obesity.Salivary diagnostic has gained popularity due to its non-invasive sampling technique.Fasting(abstinence from food or drink or both)research for weight loss and improve health is common,but studies using fasting saliva are scarce.Some metabolites in fasting saliva have been reported with interesting results,which can be enhanced by considering different confounding factors.For example,fasting saliva contains higher salivary nitrite,which is related to nitric oxide(NO).NO is a vasodilator supporting the healthy function of endothelial cells and its deficiency is connected to many diseases.The timely supply of NO through exogenous and endogenous means is highlighted and the potential advantage of fasting salivary composition changes in relation to COVID-19 infection is speculated.This review aims to provide a general discussion on the salivary composition,properties,and functions of the whole saliva,including the health benefits of fasting.展开更多
Electrochemical nitrite reduction reaction(NO_(2)^(-)RR) is a potential sustainable route for regulating the nitrogen cycle and ambient ammonia(NH_(3)) synthesis.However,it remains a challenge to precisely regulate th...Electrochemical nitrite reduction reaction(NO_(2)^(-)RR) is a potential sustainable route for regulating the nitrogen cycle and ambient ammonia(NH_(3)) synthesis.However,it remains a challenge to precisely regulate the reaction pathways and inhibit competing reactions(e.g.hydrogenolysis) for efficient and selective NH_(3) production in an aqueous solution environment.Here,we utilize the Schottky barrier-induced surface electric field to construct high-density electron-deficient Pd nanoparticles by modulating the N content in the carbon carrier to promote the enrichment and immobilization of NO_(2)^(-)on the electrode surface,which ensures the ultimate selectivity for NH_(3).With these properties,Pd@N_(0.14)C with the highest N content achieved excellent catalytic performance for the reduction of NO_(2)^(-)to NH_(3) with the 100% Faraday efficiency at-0.5 and-0.6 V vs,reversible hydrogen electrode(RHE) for NH_(3) production,which was significantly better than Pd/C and Pd@N_(x)C samples with lower N content.This study opens new avenues for rational construction of efficient electrocatalysts for nitrite removal and NH_(3) electrosynthesis.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
Highly efficient and green ammonia production is an important demand for modern agriculture.In this study,a two-step ammonia production method is developed using a gliding arc discharge in combination with Cu/Cu_(2)O ...Highly efficient and green ammonia production is an important demand for modern agriculture.In this study,a two-step ammonia production method is developed using a gliding arc discharge in combination with Cu/Cu_(2)O electrocatalysis.In this method,NO_(x)is provided by the gliding arc discharge and then electrolyzed by Cu/Cu_(2)O after alkaline absorption.The electrical characteristics,the optical characteristics and the NO_(x)production are investigated in discharges at different input voltage and the gas flow.The dependence of ammonia production through Cu/Cu_(2)O electrocatalysis on pH value and reduction potential are determined by colorimetric method.In our study,two discharge modes are observed.At high input voltage and low gas flow,the discharge is operated with a stable plasma channel which is called the steady arc gliding discharge mode(A-G mode).As lowering input voltage and raising gas flow,the plasma channel is destroyed and high frequency breakdown occurs instead,which is known as the breakdown gliding discharge mode(B-G mode).The optimal NO_(x)production of 7.34 mmol h^(-1)is obtained in the transition stage of the two discharge modes.The ammonia yield reaches0.402 mmol h^(-1)cm^(-2)at pH value of 12.7 and reduction potential of-1.0 V versus reversible hydrogen electrode(RHE).展开更多
BACKGROUND The common cause of sodium nitrite poisoning has shifted from previous accidental intoxication by exposure or ingestion of contaminated water and food to recent alarming intentional intoxication as an emplo...BACKGROUND The common cause of sodium nitrite poisoning has shifted from previous accidental intoxication by exposure or ingestion of contaminated water and food to recent alarming intentional intoxication as an employed method of suicide/exit.The subsequent formation of methemoglobin(MetHb)restricts oxygen transport and utilization in the body,resulting in functional hypoxia at the tissue level.In clinical practice,a mismatch of cyanotic appearance and oxygen partial pressure usually contributes to the identification of methemoglobinemia.Prompt recognition of characteristic mismatch and accurate diagnosis of sodium nitrite poisoning are prerequisites for the implementation of standardized systemic interventions.CASE SUMMARY A pregnant woman was admitted to the Department of Critical Care Medicine at the First Affiliated Hospital of Harbin Medical University due to consciousness disorders and drowsiness 2 h before admission.Subsequently,she developed vomiting and cyanotic skin.The woman underwent orotracheal intubation,invasive mechanical ventilation(IMV),and correction of internal environment disturbance in the ICU.Her premature infant was born with a higher-than-normal MetHb level of 3.3%,and received detoxification with methylene blue and vitamin C,supplemental vitamin K1,an infusion of fresh frozen plasma,as well as respiratory support via orotracheal intubation and IMV.On day 3 after admission,the puerpera regained consciousness,evacuated the IMV,and resumed enteral nutrition.She was then transferred to the maternity ward 24 h later.On day 7 after admission,the woman recovered and was discharged without any sequelae.CONCLUSION MetHb can cross through the placental barrier.Level of MetHb both reflects severity of the sodium nitrite poisoning and serves as feedback on therapeutic effectiveness.展开更多
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Project supported by the National Natural Science Foundation of China (No. 50238050)the Hi-Tech Research and Development Program (863) of China (No. 2002AA649250).
文摘Anaerobic ammonium oxidation (ANAMMOX) technology has potential technical superiority and economical efficiency for the nitrogen removal from landfill leachate, which contains high-strength ammonium nitrogen (NH4^+-N) and refractory organics. To complete the ANAMMOX process, a preceding partial nitritation step to produce the appropriate ratio of nitrite/ammonium is a key stage. The objective of this study was to determine the optimal conditions to acquire constant partial nitritation for landfill leachate treatment, and a bench scale fixed bed bio-film reactor was used in this study to investigate the effects of the running factors on the partial nitritation. The results showed that both the dissolved oxygen (DO) concentration and the ammonium volumetric loading rate (Nv) had effects on the partial nitritation. In the controlling conditions with a temperature of 30±1℃, Nv of 0.2-1.0 kg NH4+-N/(m^3·d), and DO concentration of 0.8-2.3 mg/L, the steady partial nitritation was achieved as follows: more than 94% partial nitritation efficiency (nitrite as the main product), 60%-74% NH4^+-N removal efficiency, and NO2^--N/NH4^+-N ratio (concentration ratio) of 1.0-1.4 in the effluent.The impact of temperature was related to Nv at certain DO concentration, and the temperature range of 25-30℃ was suitable for treating high strength ammonium leachate. Ammonium-oxidizing bacteria (AOB) could be acclimated to higher FA (free ammonium) in the range of 122-224 mg/L. According to the denaturing gradient gel electrophoresis analysis result of the bio-film in the reactor, there were 25 kinds of 16S rRNA gene fragments, which indicated that abundant microbial communities existed in the bio-film, although high concentrations of ammonium and FA may inhibit the growth of the nitrite-oxidizing bacteria (NOB) and other microorganisms in the reactor.
文摘Modeling for nitritation process was discussed and analyzed quantitatively for the factors that influence nitrite accumulation. The results indicated that pH, inorganic carbon source and Hydraulic Retention Time(HRT) as well as biomass concentration are the main factors that influenced the conversion ratio of ammonium to nitrite. A constant high pH can lead to a high nitritation rate and results in high conversion ratio on condition that free ammonia inhibition do not happen. In a CSTR system, without pH control, this conversion ratio can be monitored by pH variation in the reactor. The pH goes down far from the inlet level means a strongly nitrite accumulation. High concentration of alkalinity can promoted the conversion ratio by means of accelerating the nitritation rate through providing sufficient inorganic carbon source(carbon dioxide). When inorganic carbon source was depleted, the nitritation process stopped. HRT adjustment could be an efficient way to make the nitritation system run more flexible, which to some extent can meet the requirements of the fluctuant of inlet parameters such as ammonium concentration, pH, and temperature and so on. Biomass concentration is the key point, especially for a CSTR system in steady state, which was normally circumscribed by the characteristics of bacteria and may also affected by aeration mode and can be increased by prolonging the HRT on the condition of no nitrate accumulation when no recirculation available. The higher the biomass concentration is, the better the nitrite accumulation can be obtained.
基金supported by the Key Research and Development Project of Shandong (Nos.2021CXGC011202,2020CXGC011404,and 2022CXGC021002)the National Natural Science Foundation of China (No.22276006)。
文摘This study employed multispectral techniques to evaluate fulvic acid(FA)compositional characteristic and elucidate its biodegradation mechanisms during partial nitritation(PN)process.Results showed that FA removal efficiency(FRE)decreased from 90.22 to 23.11%when FA concentrations in the reactor were increased from 0 to 162.30 mg/L,and that molecular size,degree of aromatization and humification of the effluent FA macromolecules all increased after treatment.Microbial population analysis indicated that the proliferation of the Comamonas,OLB12 and Thauera exhibit high FA utilization capacity in lower concentrations(<50.59 mg/L),promoting the degradation and removal of macromolecular FA.In addition,the sustained increase in external FA may decrease the abundance of above functional microorganisms,resulting in a rapid drop in FRE.Furthermore,from the genetic perspective,the elevated FA levels restricted carbohydrate(ko00620,ko00010 and ko00020)and nitrogen(HAO,AMO,NIR and NOR)metabolism-related pathways,thereby impeding FA removal and total nitrogen loss associated with N_(2)O emissions.
基金supported by the National Natural Science Foundation of China (Nos. 51808367 and 51878430)
文摘In this study,a modified continuous-flow nitrifying reactor was successfully operated for rapid cultivation of micro-granules and achieving robust nitritation.Results showed that sludge granulation with mean size of ca.100μm was achieved within three weeks by gradually increasing settling velocity-based selection pressure from 0.48 to 0.9 m/hr.Though Nitrospira like nitrite-oxidizing bacteria(NOB)were enriched in the micro-granules with a ratio between ammonia-oxidizing bacteria(AOB)and NOB of 5.7%/6.5% on day 21,fast nitritation was achieved within one-week by gradually increasing of influent ammonium concentration(from 50 to 200 mg/L).Maintaining ammonium in-excess was the key for repressing NOB in the micro-granules.Interestingly,when the influent ammonium concentration switched back to 50 mg/L still with the residual ammonium of 15–25 mg/L,the nitrite accumulation efficiency increased from 90%to 98%.Experimental results suggested that the NOB repression was intensified by both oxygen and nitrite unavailability in the inner layers of micro-granules.Unexpectedly,continuous operation with ammonium in excess resulted in overproduction of extracellular polysaccharides and overgrowth of some bacteria(e.g.,Nitrosomonas,Arenimonas,and Flavobacterium),which deteriorated the micro-granule stability and drove the micro-granules aggregation into larger ones with irregular morphology.However,efficient nitritation was stably maintained with extremely high ammonium oxidation potential(>50 mg/g VSS/hr)and nearly complete washout of NOB was obtained.This suggested that smooth and spherical granule was not a prerequisite for achieving NOB wash-out and maintaining effective nitritation in the granular reactor.Overall,the microgranules exhibited a great practical potential for high-rate nitritation.
基金financially supported by the Natural Science Foundation of Shandong Province, China (No. ZR2019BEE070)a Project of Shandong Province Higher Educational Science and Technology Program (No. J18KA207)。
文摘Residual ammonium is a critical parameter affecting the stability of mainstream partial nitritation/anammox(PN/A), but the underlying mechanism remains unclear. In this study,mainstream PN/A was established and operated with progressively decreasing residual ammonium. PN/A deteriorated as the residual ammonium decreased to below 5 mg/L, and this was paralleled by a significant loss in anammox activity in situ and an increasing nitrite oxidation rate. Further analysis revealed that the low-ammonium condition directly decreased anammox activity in situ via two distinct mechanisms. First, anammox bacteria were located in the inner layer of the granular sludge, and thus were disadvantageous when competing for ammonium with ammonium-oxidizing bacteria(AOB) in the outer layer. Second, the complete ammonia oxidizer(comammox) was enriched at low residual ammonium concentrations because of its high ammonium affinity. Both AOB and comammox presented kinetic advantages over anammox bacteria. At high residual ammonium concentrations,nitrite-oxidizing bacteria(NOB) were effectively suppressed, even when their maximum activity was high due to competition for nitrite with anammox bacteria. At low residual ammonium concentrations, the decrease in anammox activity in situ led to an increase in nitrite availability for nitrite oxidation, facilitating the activation of NOB despite the dissolved oxygen limitation(0.15–0.35 mg/L) for NOB persisting throughout the operation. Therefore, the deterioration of mainstream PN/A at low residual ammonium was primarily triggered by a decline in anammox activity in situ. This study provides novel insights into the optimized design of mainstream PN/As in engineering applications.
基金supported by the Key Research&Developmental Program of Shandong Province(Nos.2021CXGC011202,2020CXGC011404)the Beijing Natural Science Foundation(No.8192004)the Beijing Major Science and Technology Projects(No.Z181100005318001)
文摘The long-term impact of fulvic acid(FA)on partial nitritation(PN)systemwas initially examined in this study.The obtained results revealed that the FA lower than 50 mg/L had negligible effect on the nitrite accumulation rate(NAR nearly 100%)and ammonium removal rate(ARR 56.85%),while FA over 50 mg/L decreased ARR from 56.85%to 0.7%.Sludge characteristics analysis found that appropriate FA(<50 mg/L)exposure promoted the settling performance and granulation of PN sludge by removing Bacteroidetes and accumulating Chloroflexi.The analysis of metagenomics suggested that the presence of limited FA(0-50 mg/L)stimulated the generation of NADH,which favors the denitrification and nitrite reduction.The negative impact of FA on the PN system could be divided into two stages.Initially,limited FA(50-120 mg/L)was decomposed by Anaerolineae to stimulate the growth and propagation of heterotrophic bacteria(Thauera).Increasing heterotrophs competed with AOB(Nitrosomonas)for dissolved oxygen,causing AOB to be eliminated and ARR to declined.Subsequently,when FA dosage was over 120 mg/L,Anaerolineae were inhibited and heterotrophic bacteria reduced,resulting in the abundance of AOB recovered.Nevertheless,the ammonium transformation pathway was suppressed because genes amoABC and hao were obviously reduced,leading to the deterioration of reactor performance.Overall,these results provide theoretical guidance for the practical application of PN for the treatment of FA-containing sewage.
基金financially supported by the National Natural Science Foundation of China(No.52170049).
文摘A continuous flow bioreactor was operated for 300 days to investigate partial nitritation(PN)of mature landfill leachate,establishing the long-term performance of the system in terms of the microbial community composition,evolution,and interactions.The stable operation phase(31-300 d)began after a 30 days of start-up period,reaching an average nitrite accumulation ratio(NAR)of 94.43%and a ratio of nitrite nitrogen to ammonia nitrogen(NO_(2)^(−)-N/NH_(4)^(+)-N)of 1.16.Some fulvic-like and humic-like compounds and proteins were effectively degraded in anaerobic and anoxic tanks,which was consistent with the corresponding abundance of methanogens and syntrophic bacteria in the anaerobic tank,and organic matter degrading bacteria in the anoxic tank.The ammonia-oxidizing bacteria(AOB)Nitrosomonas was found to be the key functional bacteria,exhibiting an increase in abundance from 0.27%to 6.38%,due to its collaborative interactions with organic matter degrading bacteria.In-situ inhibition of nitrite-oxidizing bacteria(NOB)was achieved using a combination of free ammonia(FA)and free nitrous acid(FNA),low dissolved oxygen(DO)with fewer bioavailable organics conditions were employed to maintain stable PN and a specific ratio of NO_(2)^(−)-N/NH_(4)^(+)-N,without an adverse impact on AOB.The synergistic relationships between AOB and both denitrifying bacteria and organic matter degrading bacteria,were found to contribute to the enhanced PN performance and microbial community structure stability.These findings provide a theoretical guidance for the effective application of PN-Anammox for mature landfill leachate treatment.
基金funded by National Natural Science Foundation of China(31460445)Science and Technology Talents and Platform Program of Yunnan Province,No.202105AF150049Yunnan University Key Laboratory of Food Microbial Resources and Utilization(Yunjiaofa[2018]No.135)。
文摘Sanchuan ham is appreciated in Yunnan Province,China,for its characteristic flavor and taste,while the microbial community structure and biogenic amines content remain unclear during fermentation processes.In this study,we explored the physicochemical property,biogenic amines concentration and microbial diversity of external and internal Sanchuan ham by high-throughput sequencing during the processing of Sanchuan ham.Results showed that the nitrite remained at a stable level of 0.15 mg/kg which was significantly lower than the national health standard safety level of 20 mg/kg.In addition,compared with fresh hams,the content of total free amino acids in ripe Sanchuan ham has grown 14 folds;sour and bitter were the main tastes of Sanchuan ham.Notably,the concentration of cadaverine was the highest of all biogenic amines during the entire fermentation period.At the bacterial phyla level,Firmicutes and Actinobacteria were the two main phyla,while at the genus level,Staphylococcus was a significant strain throughout the whole fermentation.Moreover,the dry stage has a great impact on the succession change of microbial community structure.Simultaneously,the change trends and composition of bacteria in the interior have slight discrepancies with those of the exterior of Sanchuan ham.
文摘The amount of piggery wastewater as domestic livestock is increasing.The volume of piggery wastewater produced is less than the volume of other wastewaters,but piggery wastewater has a heavy impact on wastewater streams due to an extremely high concentration of nitrogen and COD.In this study,laboratory reactors were operated using piggery wastewater and the effluent of anaerobic digester from piggery wastewater plants.The purpose of this study was to induce the nitritation process,which is an economically advantageous nitrogen removal method that converts ammonium nitrogen into nitrite.The results showed that the effluent of anaerobic digester from piggery wastewater was more efficient than raw piggery wastewater in terms of inducing nitritation.It can be deduced that nitritation is largely affected by an organic fraction of piggery wastewater.It can also be concluded that a small amount of biodegradable organic matter in piggery wastewater is efficient in inducing nitritation.
基金supported by the National Natural Science Foundation of China (Nos. 51168028, 51168027)the Science and Technique Foundation Project for Youth of Gansu Province (No. 1107RJYA279)
文摘Free ammonia(FA) inhibition on nitrite-oxidized bacteria(NOB) and real-time control are used to achieve nitrogen removal from landfill leachate via nitrite pathway at low temperatures in sequencing batch reactor. The inhibition of FA on NOB activity during the aerobic period was prolonged using real-time control. The degree of nitrite accumulation was monitored along with variations of the ammonia-oxidizing bacteria and NOB population using fluorescence in situ hybridization techniques. It is demonstrated that the end-point of ammonia oxidization is detected from the on-line measured dissolved oxygen,oxidization–reduction potential, and p H signals, which could avoid the loss the FA inhibition on NOB caused by excess aeration. At low temperature(13.0–17.6°C), the level of nitrite pathway rapidly increased from 19.8% to 90%, suggesting that nitritation was successfully started up at low temperature by applying syntrophic association of the FA inhibition and real-time control, and then this high level of nitrite pathway was stably maintained for as long as 233 days. Mechanism analysis shows that the establishment of nitritation was primarily the result of predominant ammonia-oxidizing bacteria developed in the nitrifying bacteria population compared to NOB. This was mainly due to a gradual reduction of nitrite amount that is available to provide energy for the growth of NOB,eventually leading to the elimination of NOB from the bacterial clusters in sequencing batch reactor sludge system.
基金supported by the National Natural Science Foundation of China(Nos.51878662,51674305)the Key Project of Science and Technology Program of Hunan Province(No.2017SK2420)+1 种基金the Fundamental Research Funds for the CentralUniversities of Central South University(No.2017zzts599)supported by the 2017 Huxiang Provincial Scholar Program and the 2018 Distinguished Youth Program of the Natural Science Foundation of Hunan Province(No.2019JJ20033)
文摘Biological nitrogen removal process could be affected due to the presence of heavy metals owing to their toxicity and accumulation in the sludge.In this study,the impact of Cu2+shock on a long-term nitritation operation was investigated in an air-lift reactor with selfrecirculation.Both the dynamics of microbial community and inhibition kinetics under Cu2+stress were ascertained.The results showed that Cu2+exerted severe inhibition on nitritation performance of an air-lift reactor(ALR)at 25 mg/L.The corresponding NH4+-N removal efficiency decreased to below 50%,which was mainly due to the variation of microbial community structure,especially the inhibition of nitrifiers like Nitrosomonas(the relative abundance decreased from 30%to 1%after Cu2+inhibition).Kinetic parameters were obtained and compared after fitting the Haldane model.The long-term Cu2+stress on the ALR aggravated the ammonium affinity and the resistance to substrate self-inhibition of the nitritation sludge,but reduced the resistance to Cu2+inhibition.Furthermore,Cu2+acted as uncompetitive inhibitor on nitritation process.Our results provide new insights into the nitritation characteristics under long-term Cu2+stress.
基金funded by the National Water Pollution Control and Management Technology Major Projects(No.2014ZX 07201-011)the Beijing Natural Science Foundation(No.8122005)of Chinathe Beijing Municipal EducationCommission General Program(No.KM2012-10005028)
文摘The objective of this study was to investigate the nitritation performance in a biofilm reactor for treating domestic wastewater.The reactor was operated in continuous feed mode from phases 1 to 3.The dissolved oxygen(DO)was controlled at 3.5–7 mg/L throughout the experiment.The biofilm reactor showed excellent nitritation performance after the inoculation of nitrifying sludge,with the hydraulic retention time being reduced from 24 to 7 hr.Above 90%nitrite accumulation ratio(NAR)was maintained in phase 1.Afterwards,nitratation occurred with the low NH4^+–N concentration in the reactor.The improvement of NH4^+–N concentration to 20–35 mg/L had a limited effect on the recovery of nitritation.However,nitritation recovered rapidly when sequencing batch feed mode was adopted in phase 4,with the effluent NH4^+-N concentration above 7 mg/L.The improvement of ammonia oxidizing bacteria(AOB)activity and the combined inhibition effect of free ammonia(FA)and free nitrous acid(FNA)on the nitrite oxidizing bacteria(NOB)were two key factors for the rapid recovery of nitritation.Sludge activity was obtained in batch tests.The results of batch tests had a good relationship with the long term operation performance of the biofilm reactor.
基金supported by the Mega-Projects of Science Research for Water Environment Improvement (No. 2012ZX07205-001)
文摘A combined nitritation–anammox reactor was developed to treat the digestion supernatant under various C/N ratios. Due to the difficulties for heterotroph to utilize the refractory organics, the reactor presented relatively stable performance with increasing supernatant addition. Nevertheless, the adverse effects of supernatant would accumulate during the long-term operation and thus weakened the activity and shock resistance of microbes,which further led to the gradual decrease of reactor performance after 92 days' operation.Under this circumstance, supernatant with volatile fatty acids(VFAs) residuals was further introduced into the reactor to investigate the performance of combined nitritation–anammox process with VFA addition. With the appearance of VFAs, the nitrogen removal performance gradually restored and the reactor finally achieved stable and efficient performance with C/N ratio of 0.35. The VFA residuals within 150 mg/L in the supernatant served as the extra electron donors and stimulated the heterotrophic denitrification process, which was vital for the enhancement of reactor. The nitrogen removal rate and total nitrogen removal efficiency reached 0.49 kg N/(m^3·day) and 88.8% after 140 days' operation, respectively. The combined nitritation–anammox reactor was proved suitable to treat digestion supernatant.
基金supported by the National Key R&D Program of China(Nos.2022YFA1503104 and 2022YFA1503102)the Natural Science Foundation of Shandong Province(No.2022HWYQ-009)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20230243)Taishan Scholars Project(No.tspd20230601)Qilu Young Scholars Program of Shandong University.
文摘The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving the NH_(3) selectivity is to facilitate adsorption and activation of NO_(2)^(−),which is generally undesirable in unitary species.In this work,an efficient NO_(2)^(−)RR catalyst is constructed by cooperating Pd with In2O3,in which NO_(2)^(−)could adsorb on interfacial dual-site through“Pd–N–O–In”linkage,leading to strengthened NO_(2)^(−)adsorption and easier N=O bond cleavage than that on unitary Pd or In2O3.Moreover,the Pd/In_(2)O_(3)composite exhibits moderate H^(*)adsorption,which may facilitate protonation kinetics while inhibiting competitive HER.As a result,it exhibits a fairly high NH_(3)yield rate of 622.76 mmol h^(−1)g^(−1)cat with a Faradaic efficiency(FE)of 95.72%,good selectivity of 91.96%,and cycling stability towards the NO_(2)^(−)RR,surpassing unitary In_(2)O_(3)and Pd/C electrocatalysts.Besides,computed results indicate that NH_(3)production on Pd/In_(2)O_(3)follows the deoxidation to hydrogenation pathway.This work highlights the significance of H^(*)and NO_(2)^(−)adsorption modulation and N=O activation in NO_(2)^(−)RR electrochemistry by creating synergy between a mediocre catalyst with an appropriate cooperator.
文摘Human saliva is an indispensable fluid that maintains a healthy oral cavity which otherwise can lead to oral diseases(dental caries and periodontitis).In addition,salivary metabolites and microbiome profile provide early detection of systemic diseases such as cancer and obesity.Salivary diagnostic has gained popularity due to its non-invasive sampling technique.Fasting(abstinence from food or drink or both)research for weight loss and improve health is common,but studies using fasting saliva are scarce.Some metabolites in fasting saliva have been reported with interesting results,which can be enhanced by considering different confounding factors.For example,fasting saliva contains higher salivary nitrite,which is related to nitric oxide(NO).NO is a vasodilator supporting the healthy function of endothelial cells and its deficiency is connected to many diseases.The timely supply of NO through exogenous and endogenous means is highlighted and the potential advantage of fasting salivary composition changes in relation to COVID-19 infection is speculated.This review aims to provide a general discussion on the salivary composition,properties,and functions of the whole saliva,including the health benefits of fasting.
文摘Electrochemical nitrite reduction reaction(NO_(2)^(-)RR) is a potential sustainable route for regulating the nitrogen cycle and ambient ammonia(NH_(3)) synthesis.However,it remains a challenge to precisely regulate the reaction pathways and inhibit competing reactions(e.g.hydrogenolysis) for efficient and selective NH_(3) production in an aqueous solution environment.Here,we utilize the Schottky barrier-induced surface electric field to construct high-density electron-deficient Pd nanoparticles by modulating the N content in the carbon carrier to promote the enrichment and immobilization of NO_(2)^(-)on the electrode surface,which ensures the ultimate selectivity for NH_(3).With these properties,Pd@N_(0.14)C with the highest N content achieved excellent catalytic performance for the reduction of NO_(2)^(-)to NH_(3) with the 100% Faraday efficiency at-0.5 and-0.6 V vs,reversible hydrogen electrode(RHE) for NH_(3) production,which was significantly better than Pd/C and Pd@N_(x)C samples with lower N content.This study opens new avenues for rational construction of efficient electrocatalysts for nitrite removal and NH_(3) electrosynthesis.
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Highly efficient and green ammonia production is an important demand for modern agriculture.In this study,a two-step ammonia production method is developed using a gliding arc discharge in combination with Cu/Cu_(2)O electrocatalysis.In this method,NO_(x)is provided by the gliding arc discharge and then electrolyzed by Cu/Cu_(2)O after alkaline absorption.The electrical characteristics,the optical characteristics and the NO_(x)production are investigated in discharges at different input voltage and the gas flow.The dependence of ammonia production through Cu/Cu_(2)O electrocatalysis on pH value and reduction potential are determined by colorimetric method.In our study,two discharge modes are observed.At high input voltage and low gas flow,the discharge is operated with a stable plasma channel which is called the steady arc gliding discharge mode(A-G mode).As lowering input voltage and raising gas flow,the plasma channel is destroyed and high frequency breakdown occurs instead,which is known as the breakdown gliding discharge mode(B-G mode).The optimal NO_(x)production of 7.34 mmol h^(-1)is obtained in the transition stage of the two discharge modes.The ammonia yield reaches0.402 mmol h^(-1)cm^(-2)at pH value of 12.7 and reduction potential of-1.0 V versus reversible hydrogen electrode(RHE).
基金Supported by the National Natural Science Foundation of China,No.82372172the Key Research and Development Plan Project of Heilongjiang Province,No.GA23C007+3 种基金the Heilongjiang Province Postdoctoral Start-up Fund,No.LBH-Q20037the Research Project of Heilongjiang Provincial Health Commission,No.20231717010461the Special Fund for Clinical Research of Wu Jie-ping Medical Foundation,No.320.6750.2022-02-16the Scientific Research Innovation Fund of the First Affiliated Hospital of Harbin Medical University,No.2021M08.
文摘BACKGROUND The common cause of sodium nitrite poisoning has shifted from previous accidental intoxication by exposure or ingestion of contaminated water and food to recent alarming intentional intoxication as an employed method of suicide/exit.The subsequent formation of methemoglobin(MetHb)restricts oxygen transport and utilization in the body,resulting in functional hypoxia at the tissue level.In clinical practice,a mismatch of cyanotic appearance and oxygen partial pressure usually contributes to the identification of methemoglobinemia.Prompt recognition of characteristic mismatch and accurate diagnosis of sodium nitrite poisoning are prerequisites for the implementation of standardized systemic interventions.CASE SUMMARY A pregnant woman was admitted to the Department of Critical Care Medicine at the First Affiliated Hospital of Harbin Medical University due to consciousness disorders and drowsiness 2 h before admission.Subsequently,she developed vomiting and cyanotic skin.The woman underwent orotracheal intubation,invasive mechanical ventilation(IMV),and correction of internal environment disturbance in the ICU.Her premature infant was born with a higher-than-normal MetHb level of 3.3%,and received detoxification with methylene blue and vitamin C,supplemental vitamin K1,an infusion of fresh frozen plasma,as well as respiratory support via orotracheal intubation and IMV.On day 3 after admission,the puerpera regained consciousness,evacuated the IMV,and resumed enteral nutrition.She was then transferred to the maternity ward 24 h later.On day 7 after admission,the woman recovered and was discharged without any sequelae.CONCLUSION MetHb can cross through the placental barrier.Level of MetHb both reflects severity of the sodium nitrite poisoning and serves as feedback on therapeutic effectiveness.