It is still a lack of bifunctional catalysts for ammonia oxidation reaction(AOR)and hydrogen evolution reaction(HER)due to their different reaction mechanisms.In this work,P is doped into PtZn alloy by calcination wit...It is still a lack of bifunctional catalysts for ammonia oxidation reaction(AOR)and hydrogen evolution reaction(HER)due to their different reaction mechanisms.In this work,P is doped into PtZn alloy by calcination with NaH_(2)PO_(2) as P source to induce the lattice tensile strain of Pt and the electronic interaction between P and Zn,which optimizes the AOR and HER activity simultaneously.The sample with the optimal P content can drive the AOR peak current density of 293.6 mA·mgPt^(-1),which is almost 2.7 times of Pt.For HER,the overpotential at^(-1)0 mA·cm^(-2) is only 23 mV with Tafel slope of 34.1 mV·dec^(-1).Furthermore,only 0.59 V is needed to obtain 50 mA·mgPt^(-1) for ammonia electrolysis under a two-electrode system.Therefore,this work shows an ingenious method to design bifunctional catalysts for ammonia electrolysis.展开更多
Soil arsenic contamination is of great concern because of its toxicity to human,crops,and soil microorganisms.However,the impacts of arsenic on soil ammonia oxidizers communities remain unclear.Seven types of soil spi...Soil arsenic contamination is of great concern because of its toxicity to human,crops,and soil microorganisms.However,the impacts of arsenic on soil ammonia oxidizers communities remain unclear.Seven types of soil spiked with 0 or 100 mg arsenic per kg soil were incubated for 180 days and sampled at days 1,15,30,90 and 180.The changes in the community composition and abundance of ammonia oxidizing bacteria(AOB)and ammonia oxidizing archaea(AOA)were analyzed by terminal restriction fragment length polymorphism(TRFLP)analysis,clone library sequencing,and quantitative PCR(qPCR)targeting amoA gene.Results revealed considerable variations in the potential ammonia oxidation(PAO)rates in different soils,but soil PAO was not consistently significantly inhibited by arsenic,probably due to the low bioavailable arsenic contents or the existence of functional redundancy between AOB and AOA.The variations in AOB and AOA communities were closely associated with the changes in arsenic fractionations.The amoA gene abundances of AOA increased after arsenic addition,whereas AOB decreased,which corroborated the notion that AOA and AOB might occupy different niches in arsenic-contaminated soils.Phylogenetic analysis of amoA gene-encoded proteins revealed that all AOB clone sequences belonged to the genus Nitrosospira,among which those belonging to Nitrosospira cluster 3a were dominant.The main AOA sequence detected belonged to Thaumarchaeal Group 1.1b,which was considered to have a high ability to adapt to environmental changes.Our results provide new insights into the impacts of arsenic on the soil nitrogen cycling.展开更多
Mining,smelting and tailing deposition activities can cause metal(loid)contamination in surrounding soils,threatening ecosystems and human health.Microbial indicators are sensitive to environmental factors and have a ...Mining,smelting and tailing deposition activities can cause metal(loid)contamination in surrounding soils,threatening ecosystems and human health.Microbial indicators are sensitive to environmental factors and have a crucial role in soil ecological risk assessment.Xikuangshan,the largest active antimony(Sb)mine in the world,was taken as the research area.The soil properties,metal(loid)contents and microbial characteristics were investigated and their internal response relationships were explored by multivariate statistical analysis.The assessment of the single pollution index and Nemerow synthetic pollution index(PN)showed that the soils were mainly polluted by Sb,followed by Cd and As,in which sampling site S1 had a slight metal(loid)pollution and the other sampling sites suffered from severe synthetic metal(loid)pollution.The microbial characteristics were dissimilar among sampling points at different locations from the mining area according to hierarchical cluster analysis.The correlation analysis indicated that fluorescein diacetate hydrolase,acid phosphatase,soil basal respiration andmicrobial biomass carbonwere negatively correlatedwith PN,indicating their sensitivity to combined metal(loid)contamination;that dehydrogenase was positively correlated with pH;and that urease,potential ammonia oxidation and abundance of ammonia-oxidizing bacteria and archaea were correlated with N(nitrogen)contents.However,β-glucosidase activity had no significant correlations with physicochemical properties and metal(loid)contents.Principal components analysis suggested bioavailable Sb and pH were the dominant factors of soil environment in Xikuangshan Sb mining area.Our results can provide a theoretical basis for ecological risk assessment of contaminated soil.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
As a promising fuel candidate,ammonia has been successtully used as anode feed in alkaline fuel cells.However,current technology in catalysts for ammonia electro-oxidation reaction(AOR)with respect to both cost and pe...As a promising fuel candidate,ammonia has been successtully used as anode feed in alkaline fuel cells.However,current technology in catalysts for ammonia electro-oxidation reaction(AOR)with respect to both cost and performance is inadequate to ensure large scale commercial application of direct ammonia fuel cells.Recent studies found that alloying Pt with different transition metals and controlling the morphology of catalysts can improve the AOR activity,and thus potentially can solve the cost issue.Herein,(100)-terminated Pt-M nanocubes(M=3d-transition metals Fe,Co,Ni,Zn)are synthesized via wet-chemistry method and their catalytic activities toward AOR are evaluated.The addition of Fe,Co,Ni and Zn elements can enhance the AOR activity due to decrease in oxophilicity of platinum and bifunctional mechanism.Pt-Zn exhibits the maximum mass activity and specific ativity with values of 0.41 A/mgpt and 169 mA/cm2 that are 1.6 and 1.8 times higher than Pt nanocubes,respectively.Pt-Fe,Pt-Co and PI-Ni nanocubes also ilustrate higher mass and specific activities compared to Pt nanocubes.展开更多
Ammonia-oxidizing archaeon(AOA)could play important roles for nitrogen removal in the bioreactors under conditions such as low pH and low dissolved oxygen.Therefore,enhancing ammonia oxidation capability of AOA has gr...Ammonia-oxidizing archaeon(AOA)could play important roles for nitrogen removal in the bioreactors under conditions such as low pH and low dissolved oxygen.Therefore,enhancing ammonia oxidation capability of AOA has great significance for water and wastewater treatment,especially under conditions like low dissolved oxygen concentration.Utilizing a novel AOA strain SAT1,which was enriched from a wastewater treatment plant by our group,the effect of magnetic field on AOA’s ammonia oxidation capability,its magnetotaxis and heredity were investigated in this study.Compared with control experiment,AOA’s maximum nitrite-N formation rate during the cultivation increased by 56.8%(0.65 mgN/(L·d))with 20 mT magnetic field.Also,it was testified that AOA possessed a certain magnetotaxis.However,results manifested that the enhancement of AOA’s ammonia oxidation capability was not heritable,that is,lost once the magnetic field was removed.Additionally,the possible mechanism of improving AOA’s ammonia oxidation capability by magnetic field was owing to the promotion of AOA single cells’growth and fission,rather than the enhancement of their ammonia oxidation rates.The results shed light on the application of AOA and methods to enhance AOA’s ammonia oxidation capability,especially in wastewater treatment processes under certain conditions.展开更多
Electrocatalytic ammonia oxidation reaction(EAOR)provides an ideal solution for on-board hydrogen supply for fuel cells,while the lack of efficient and durable EAOR catalysts has been a long-standing obstacle for its ...Electrocatalytic ammonia oxidation reaction(EAOR)provides an ideal solution for on-board hydrogen supply for fuel cells,while the lack of efficient and durable EAOR catalysts has been a long-standing obstacle for its practical application.Herein,we reported that the defect engineering via in-situ electrochemically introducing oxygen vacancies(Vo)not only turns the inactive CuO into efficient EAOR catalyst but also achieves a high stability of over 400 h at a high current density of~200 mA·cm^(−2).Theoretical simulation reveals that the presence of Vo on the CuO surface induces a remarkable upshift of the d-band center of active Cu site closer to the Fermi level,which significantly stabilizes the reaction intermediates(*NHx)and efficiently oxidizes NH3 into N2.This Vo-modulated CuO shows a different catalytic mechanism from that on the conventional Pt-based catalysts,paving a new avenue to develop inexpensive,efficient,and robust catalysts,not limited to EAOR.展开更多
Measurement and predicted variations of ammonia oxidation rate(AOR)are critical for the optimization of biological nitrogen removal,however,it is difficult to predict accurate AOR based on current models.In this study...Measurement and predicted variations of ammonia oxidation rate(AOR)are critical for the optimization of biological nitrogen removal,however,it is difficult to predict accurate AOR based on current models.In this study,a modified model was developed to predict AOR based on laboratoryscale tests and verified through pilot-scale tests.In biological nitrogen removal reactors,the specific ammonia oxidation rate(SAOR)was affected by both mixed liquor volatile suspended solids(MLVSS)concentration and temperature.When MLVSS increased 1.6,4.2,and 7.1-fold(1.3‒8.9 g/L,at 20℃),the measured SAOR decreased by 21%,49%,and 56%,respectively.Thereby,the estimated SAOR was suggested to modify when MLVSS changed through a power equation fitting.In addition,temperature coefficient(θ)was modified based on MLVSS concentration.These results suggested that the prediction of variations ammonia oxidation rate in real wastewater treatment system could be more accurate when considering the effect of MLVSS variations on SAOR.展开更多
A range of plant species produce root exudates that inhibit ammonia-oxidizing microorganisms.This biological nitrification inhibition(BNI)capacity can decrease N loss and increase N uptake from the rhizosphere.This st...A range of plant species produce root exudates that inhibit ammonia-oxidizing microorganisms.This biological nitrification inhibition(BNI)capacity can decrease N loss and increase N uptake from the rhizosphere.This study sought evidence for the existence and magnitude of BNI capacity in canola(Brassica napus).Seedlings of three canola cultivars,Brachiaria humidicola(BNI positive)and wheat(Triticum aestivum)were grown in a hydroponic system.Root exudates were collected and their inhibition of the ammonia oxidizing bacterium,Nitrosospira multiformis,was tested.Subsequent pot experiments were used to test the inhibition of native nitrifying communities in soil.Root exudates from canola significantly reduced nitrification rates of both N.multiformis cultures and native soil microbial communities.The level of nitrification inhibition across the three cultivars was similar to the well-studied high-BNI species B.humidicola.BNI capacity of canola may have implications for the N dynamics in farming systems and the N uptake efficiency of crops in rotational farming systems.By reducing nitrification rates canola crops may decrease N losses,increase plant N uptake and encourage microbial N immobilization and subsequently increase the pool of organic N that is available for mineralization during the following cereal crops.展开更多
The ammonia electrolysis is a highly efficient and energy-saving method for ultra-pure hydrogen generation, which highly relies on electrocatalytic performance of electrocatalysts. In this work, high-quality platinum(...The ammonia electrolysis is a highly efficient and energy-saving method for ultra-pure hydrogen generation, which highly relies on electrocatalytic performance of electrocatalysts. In this work, high-quality platinum(Pt) nanocubes(Pt-NCs) with 4.5 nm size are achieved by facile hydrothermal synthesis. The physical morphology and structure of Pt-NCs are exhaustively characterized, revealing that Pt-NCs with special {100} facets have excellent uniformity, good dispersity and high crystallinity. Meanwhile, the electrocatalytic performance of Pt-NCs for ammonia electrolysis are carefully investigated in alkaline solutions, which display outstanding electroactivity and stability for both ammonia electrooxidation reaction(AEOR) and hydrogen evolution reaction(HER) in KOH solution. Furthermore, a symmetric Pt-NCs||Pt-NCs ammonia electrolyzer based on bifunctional Pt-NCs electrocatalyst is constructed, which only requires 0.68 V electrolysis voltage for hydrogen generation. Additionally, the symmetric Pt-NCs||Pt-NCs ammonia electrolyzer has excellent reversible switch capability for AEOR at anode and HER at cathode, showing outstanding alternating operation ability for ammonia electrolysis.展开更多
Ce1-xZrxO_(2) composite oxides(molar,x=0-1.0,interval of 0.2)were prepared by a cetyltrimethylammonium bromide-assisted precipitation method.The enhancement of silver-species modification and catalytic mechanism of ad...Ce1-xZrxO_(2) composite oxides(molar,x=0-1.0,interval of 0.2)were prepared by a cetyltrimethylammonium bromide-assisted precipitation method.The enhancement of silver-species modification and catalytic mechanism of adsorption-transformationdesorption process were investigated over the Ag-impregnated catalysts for lowtemperature selective catalytic oxidation of ammonia(NH_(3)-SCO).The optimal 5 wt.%Ag/Ce_(0.6)Zr_(0.4)O_(2) catalyst presented good NH_(3)-SCO performancewith>90% NH_(3) conversion at temperature(T)≥250°C and 89% N_(2) selectivity.Despite the irregular block shape and underdeveloped specific surface area(∼60m2/g),the naked and Ag-modified Ce_(0.6)Zr_(0.4)O_(2) solid solution still obtained highly dispersed distribution of surface elements analyzed by scanning electron microscope-energy dispersive spectrometer(SEM-EDS)(mapping),N_(2) adsorptiondesorption test and X-ray diffraction(XRD).H2 temperature programmed reduction(H2-TPR)and X-ray photoelectron spectroscopy(XPS)results indicated that Ag-modification enhanced the mobility and activation of oxygen-species leading to a promotion on CeO_(2) reducibility and synergistic Ag0/Ag+and Ce^(4+)/Ce^(3+)redox cycles.Besides,Ag+/Ag_(2)O clusters could facilitate the formation of surface oxygen vacancies that was beneficial to the adsorption and activation of ammonia.NH3-temperature programmed desorption(NH_(3)-TPD)showed more adsorption-desorption capacity to ammoniawere provided by physical,weakandmedium-strong acid sites.Diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments revealed the activation of ammonia might be the control step of NH3-SCO procedure,during which NH3 dehydrogenation derived from NHx-species and also internal selective catalytic reduction(i-SCR)reactions were proposed.展开更多
For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions...For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions to drive the water splitting reaction.Because of the lower thermodynamic requirements to oxidize ammonia compared to water,solar cells with smaller open circuit voltages can provide the required potential for ammonia splitting.In this work,a single perovskite solar cell with an open-circuit potential of 1.08 V is coupled to a 2-electrode electrochemical cell employing hybrid electroanodes functionalized with Ru-based molecular catalysts.The device is active for more than 30 min,producing N_(2) and H_(2) in a 1:2.9 ratio with 89%faradaic efficiency with no external applied bias.This work illustrates that hydrogen production from ammonia can be driven by conventional semiconductors.展开更多
The upland agricultural soils in North China are distributed north of a line between the Kunlun Mountains, the Qinling Mountains and the Huaihe River. They occur in arid, semi-arid and semi-humid regions and crop prod...The upland agricultural soils in North China are distributed north of a line between the Kunlun Mountains, the Qinling Mountains and the Huaihe River. They occur in arid, semi-arid and semi-humid regions and crop production often depends on rain-fed or irrigation to supplement rainfall. This paper summarizes the characteristics of gross nitrogen(N) transformation, the fate of N fertilizer and soil N as well as the N loss pathway, and makes suggestions for proper N management in the region. The soils of the region are characterized by strong N mineralization and nitrification, and weak immobilization and denitrification ability, which lead to the production and accumulation of nitrate in the soil profile. Large amounts of accumulated nitrate have been observed in the vadose-zone in soils due to excess N fertilization in the past three decades, and this nitrate is subject to occasional leaching which leads to groundwater nitrate contamination. Under farmer's conventional high N fertilization practice in the winter wheat-summer maize rotation system(N application rate was approximately 600 kg ha–1 yr–1), crop N uptake, soil residual N, NH_3 volatilization, NO_3~– leaching, and denitrification loss accounted for around 27, 30, 23, 18 and 2% of the applied fertilizer N, respectively. NH_3 volatilization and NO_3~– leaching were the most important N loss pathways while soil residual N was an important fate of N fertilizer for replenishing soil N depletion from crop production. The upland agricultural soils in North China are a large source of N_2O and total emissions in this region make up a large proportion(approximately 54%) of Chinese cropland N_2O emissions. The "non-coupled strong ammonia oxidation" process is an important mechanism of N_2O production. Slowing down ammonia oxidation after ammonium-N fertilizer or urea application and avoiding transient high soil NH4+ concentrations are key measures for reducing N_2O emissions in this region. Further N management should aim to minimize N losses from crop and livestock production, and increase the recycling of manure and straw back to cropland. We also recommend adoption of the 4 R(Right soure, Right rate, Right time, Right place) fertilization techniques to realize proper N fertilizer management, and improving application methods or modifying fertilizer types to reduce NH_3 volatilization, improving water management to reduce NO_3~– leaching, and controlling the strong ammonia oxidation process to abate N_2O emission. Future research should focus on the study of the trade-off effects among different N loss pathways under different N application methods or fertilizer products.展开更多
Electrochemical reduction of water to hydrogen(H2) offers a promising strategy for production of clean energy,but the design and optimization of electrochemical apparatus present challenges in terms of H2 recovery and...Electrochemical reduction of water to hydrogen(H2) offers a promising strategy for production of clean energy,but the design and optimization of electrochemical apparatus present challenges in terms of H2 recovery and energy consumption.Using cobalt phosphide nanoarrays(Co2 P/CoP NAs) as a charge mediator,we effectively separated the H2 and O2 evolution of alkaline water electrolysis in time,thereby achieving a membrane-free pathway for H2 purification.The hierarchical array structure and synergistic optimization of the electronic configuration of metallic Co2 P and metalloid CoP make the Co2 P/CoP NAs high-efficiency bifunctional electrocatalysts for both charge storage and hydrogen evolution.Theoretical investigations revealed that the introduction of Co2 P into CoP leads to a moderate hydrogen adsorption free energy and low water dissociation barrier,which are beneficial for boosting HER activity.Meanwhile,Co2 P/CoP NAs with high capacitance could maintain a cathodic H2 evolution time of 1500 s at 10 mA cm^(-2) driven by a low average voltage of 1.38 V.Alternatively,the energy stored in the mediator could be exhausted via coupling with the anodic oxidation of ammonia,whereby only 0.21 V was required to hold the current for 1188 s.This membrane-free architecture demonstrates the potential for developing hydrogen purification technology at low cost.展开更多
In situ and simultaneous remediation of a variety of pollutants in sediments remains a challenge.In this study,we report that the combination of electrocoagulation(EC)and electrooxidation(EO)is efficient in the immobi...In situ and simultaneous remediation of a variety of pollutants in sediments remains a challenge.In this study,we report that the combination of electrocoagulation(EC)and electrooxidation(EO)is efficient in the immobilization of phosphorus and heavymetals and in the oxidation of ammonium and toxic organicmatter.The integratedmixed metal oxide(MMO)/Fe anode system allowed the facile removal of ammonium and phosphorus in the overlying water(99% of 10 mg/L NH_(4)^(+)-N and 95% of 10 mg/L P disappeared in 15 and 30 min,respectively).Compared with the controls of the single Fe anode and single MMO anode systems,the dual MMO/Fe anode system significantly improved the removal of phenanthrene and promoted the transition of Pb and Cu from the mobile species to the immobile species.The concentrations of Pb and Cu in the toxicity characteristic leaching procedure extracts were reduced by 99%and 97% after an 8 hr operation.Further tests with four real polluted samples indicated that substantial proportions of acid-soluble fraction Pb and Cu were reduced(30%-31% for Pb and 16%–23% for Cu),and the amounts of total organic carbon and NH_(4)^(+)-N decreased by 56%–71% and 32%–63%,respectively.It was proposed that the in situ electrogenerated Fe(II)at the Fe anode and the active oxygen/chlorine species at the MMO anode are conducive to outstanding performance in the co-treatment of multiple pollutants.The results suggest that the EC/EO method is a powerful technology for the in situ remediation of sediments contaminated with different pollutants.展开更多
Ammonia has emerged as a promising energy carrier owing to its carbon neutral content and low expense in long-range transportation.Therefore,development of a specific pathway to release the energy stored in ammonia is...Ammonia has emerged as a promising energy carrier owing to its carbon neutral content and low expense in long-range transportation.Therefore,development of a specific pathway to release the energy stored in ammonia is therefore in urgent demand.Electrochemical oxidation provides a convenient and reliable route to attain efficient utilization of ammonia.Here,we report that the high entropy(Mn,Fe,Co,Ni,Cu)_(3)O_(4)oxides can achieve high electrocatalytic activity for ammonia oxidation reaction(AOR)in non-aqueous solutions.The AOR onset overpotential of(Mn,Fe,Co,Ni,Cu)_(3)O_(4)is 0.70 V,which is nearly 0.2 V lower than that of their most active single metal cation counterpart.The mass spectroscopy study reveals that(Mn,Fe,Co,Ni,Cu)_(3)O_(4)preferentially oxidizes ammonia to environmentally friendly diatomic nitrogen with a Faradic efficiency of over 85%.The Xray photoelectron spectroscopy(XPS)result indicates that the balancing metal d-band of Mn and Cu cations helps retain a longlasting electrocatalytic activity.Overall,this work introduces a new family of earth-abundant transition metal high entropy oxide electrocatalysts for AOR,thus heralding a new paradigm of catalyst design for enabling ammonia as an energy carrier.展开更多
Nitrification is a key step in the global nitrogen cycle.Compared with autotrophic nitrification,heterotrophic nitrification remains poorly understood.In this study,Halomonas venusta MA-ZP17-13,isolated from seawater ...Nitrification is a key step in the global nitrogen cycle.Compared with autotrophic nitrification,heterotrophic nitrification remains poorly understood.In this study,Halomonas venusta MA-ZP17-13,isolated from seawater in shrimp aquaculture (Penaeus vannamei),could simultaneously undertake nitrification and denitrification.With the initial ammonium concentration at 100 mg/L,the maximum ammonium-nitrogen removal rate reached98.7%under the optimal conditions including C/N concentration ratio at 5.95,p H at 8.93,and Na Cl at 2.33%.The corresponding average removal rate was 1.37 mg/(L·h)(according to nitrogen) in 3 d at 11.2℃.By whole genome sequencing and analysis,nitrification-and denitrification-related genes were identified,including ammonia monooxygenase,nitrate reductase,nitrite reductase,nitric oxide dioxygenase and nitric oxide synthase;while no gene encoding hydroxylamine oxidase was identified,it implied the existence of a novel nitrification pathway from hydroxylamine to nitrate.These results indicate heterotrophic bacterium H.venusta MA-ZP17-13 can undertake simultaneous nitrification and denitrification at low temperature and has potential for NH_(4)^(+)-N/NH_(3)-N removal in marine aquaculture systems.展开更多
Introduction:Biological soil crusts(BSCs)can dominate surface cover in dry lands worldwide,playing an integral role in arid land biogeochemistry,particularly in N fertilization through fixation and cycling.Nitrificati...Introduction:Biological soil crusts(BSCs)can dominate surface cover in dry lands worldwide,playing an integral role in arid land biogeochemistry,particularly in N fertilization through fixation and cycling.Nitrification is a characteristic and universal N transformation in BSCs that becomes important for the export of N beyond the microscopic bounds of the crust itself.The contribution of ammonia-oxidizing bacteria(AOB)in BSCs has been shown,but the role and extent of the recently discovered ammonia-oxidizing archaea(AOA)have not.Methods:We sampled various types of crusts in four desert regions across the western United States and characterized the composition and size of ammonia-oxidizing communities using clone libraries and quantitative PCR targeting the amoA gene,which codes for the ammonia monooxygenase enzyme,universally present in ammonia-oxidizing microbes.Results:All archaeal amoA sequences retrieved from BSCs belonged to the Thaumarchaeota(Nitrososphaera associated Group I.1b).Sequences from the Sonoran Desert,Colorado Plateau,and Great Basin were indistinguishable from each other but distinct from those of the Chihuahuan Desert.Based on amoA gene abundances,archaeal and bacterial ammonia oxidizers were ubiquitous in our survey,but the ratios of archaeal to bacterial ammonia oxidizers shifted from bacterially dominated in northern,cooler deserts to archaeally dominated in southern,warmer deserts.Conclusions:Archaea are shown to be potentially important biogeochemical agents of biological soil crust N cycling.Conditions associated with different types of BSCs and biogeographical factors reveal a niche differentiation between AOA and AOB,possibly driven by temperature.展开更多
Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational performance.To address these drawbacks,this study inves...Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational performance.To address these drawbacks,this study investigated the effect of low intensity ultrasound treatment combined with hydroxylamine(NH2OH)on the performance of partial nitrification.Results showthat compared with the control group,low-intensity ultrasound treatment(0.10W/mL,15 min)combined with NH2OH(5 mg/L)reduced the time required for partial nitrification initiation by 6 days,increasing the nitrite accumulation rate(NAR)and ammonia nitro-gen removal rate(NRR)by 20.4% and 6.7%,respectively,achieving 96.48% NRR.Mechanis-tic analysis showed that NH2OH enhanced ammonia oxidation,inhibited nitrite-oxidizing bacteria(NOB)activity and shortened the time required for partial nitrification initiation.Furthermore,ultrasonication combined with NH2OH dosing stimulated EPS(extracellular polymeric substances)secretion,increased carbonyl,hydroxyl and amine functional group abundances and enhanced mass transfer.In addition,16S rRNA gene sequencing results showed that ultrasonication-sensitive Nitrospira disappeared from the ultrasound+NH_(2)OH system,while Nitrosomonas gradually became the dominant group.Collectively,the results of this study provide valuable insight into the enhancement of partial nitrification start-up during the process of wastewater nitrogen removal.展开更多
Complete ammonia oxidizing bacteria,or comammox bacteria(CAOB),can oxidize ammonium to nitrate on its own.Its discovery revolutionized our understanding of biological nitrification,and its distribution in both natural...Complete ammonia oxidizing bacteria,or comammox bacteria(CAOB),can oxidize ammonium to nitrate on its own.Its discovery revolutionized our understanding of biological nitrification,and its distribution in both natural and artificial systems has enabled a reevaluation of the relative contribution of microorganisms to the nitrogen cycle.Its wide distribution,adaptation to oligotrophic medium,and diverse metabolic pathways,means extensive research on CAOB and its application in water treatment can be promoted.Furthermore,the energy-saving characteristics of high oxygen affinity and low sludge production may also become frontier directions for wastewater treatment.This paper provides an overview of the discovery and environmental distribution of CAOB,as well as the physiological characteristics of the microorganisms,such as nutrient medium,environmental factors,enzymes,and metabolism,focusing on future research and the application of CAOB in wastewater treatment.Further research should be carried out on the physiological characteristics of CAOB,to analyze its ecological niche and impact factors,and explore its application potential in wastewater treatment nitrogen cycle improvement.展开更多
基金supported by the National Natural Science Foundation of China(No.22162004)the Natural Science Foundation of Guangxi Province(No.2022JJD120011)the Opening Project of Guangxi Key Laboratory of Information Materials(No.211025-K).
文摘It is still a lack of bifunctional catalysts for ammonia oxidation reaction(AOR)and hydrogen evolution reaction(HER)due to their different reaction mechanisms.In this work,P is doped into PtZn alloy by calcination with NaH_(2)PO_(2) as P source to induce the lattice tensile strain of Pt and the electronic interaction between P and Zn,which optimizes the AOR and HER activity simultaneously.The sample with the optimal P content can drive the AOR peak current density of 293.6 mA·mgPt^(-1),which is almost 2.7 times of Pt.For HER,the overpotential at^(-1)0 mA·cm^(-2) is only 23 mV with Tafel slope of 34.1 mV·dec^(-1).Furthermore,only 0.59 V is needed to obtain 50 mA·mgPt^(-1) for ammonia electrolysis under a two-electrode system.Therefore,this work shows an ingenious method to design bifunctional catalysts for ammonia electrolysis.
基金supported by the National Natural Science Foundation of China(Nos.41877061,41671308)Central Public-interest Scientific Institution Basal Research Fund(No.BSRF202101)the Agricultural Science and Technology Innovation Program of the Chinese Academy of Agricultural Sciences(No.CAAS-ASTIP-2016-IEDA).
文摘Soil arsenic contamination is of great concern because of its toxicity to human,crops,and soil microorganisms.However,the impacts of arsenic on soil ammonia oxidizers communities remain unclear.Seven types of soil spiked with 0 or 100 mg arsenic per kg soil were incubated for 180 days and sampled at days 1,15,30,90 and 180.The changes in the community composition and abundance of ammonia oxidizing bacteria(AOB)and ammonia oxidizing archaea(AOA)were analyzed by terminal restriction fragment length polymorphism(TRFLP)analysis,clone library sequencing,and quantitative PCR(qPCR)targeting amoA gene.Results revealed considerable variations in the potential ammonia oxidation(PAO)rates in different soils,but soil PAO was not consistently significantly inhibited by arsenic,probably due to the low bioavailable arsenic contents or the existence of functional redundancy between AOB and AOA.The variations in AOB and AOA communities were closely associated with the changes in arsenic fractionations.The amoA gene abundances of AOA increased after arsenic addition,whereas AOB decreased,which corroborated the notion that AOA and AOB might occupy different niches in arsenic-contaminated soils.Phylogenetic analysis of amoA gene-encoded proteins revealed that all AOB clone sequences belonged to the genus Nitrosospira,among which those belonging to Nitrosospira cluster 3a were dominant.The main AOA sequence detected belonged to Thaumarchaeal Group 1.1b,which was considered to have a high ability to adapt to environmental changes.Our results provide new insights into the impacts of arsenic on the soil nitrogen cycling.
基金supported by the National Natural Science Foundation of China(No.42030706).
文摘Mining,smelting and tailing deposition activities can cause metal(loid)contamination in surrounding soils,threatening ecosystems and human health.Microbial indicators are sensitive to environmental factors and have a crucial role in soil ecological risk assessment.Xikuangshan,the largest active antimony(Sb)mine in the world,was taken as the research area.The soil properties,metal(loid)contents and microbial characteristics were investigated and their internal response relationships were explored by multivariate statistical analysis.The assessment of the single pollution index and Nemerow synthetic pollution index(PN)showed that the soils were mainly polluted by Sb,followed by Cd and As,in which sampling site S1 had a slight metal(loid)pollution and the other sampling sites suffered from severe synthetic metal(loid)pollution.The microbial characteristics were dissimilar among sampling points at different locations from the mining area according to hierarchical cluster analysis.The correlation analysis indicated that fluorescein diacetate hydrolase,acid phosphatase,soil basal respiration andmicrobial biomass carbonwere negatively correlatedwith PN,indicating their sensitivity to combined metal(loid)contamination;that dehydrogenase was positively correlated with pH;and that urease,potential ammonia oxidation and abundance of ammonia-oxidizing bacteria and archaea were correlated with N(nitrogen)contents.However,β-glucosidase activity had no significant correlations with physicochemical properties and metal(loid)contents.Principal components analysis suggested bioavailable Sb and pH were the dominant factors of soil environment in Xikuangshan Sb mining area.Our results can provide a theoretical basis for ecological risk assessment of contaminated soil.
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Research Grant Council(Nos.26206115 and 16304117)of the Hong Kong Special Administrative Region.
文摘As a promising fuel candidate,ammonia has been successtully used as anode feed in alkaline fuel cells.However,current technology in catalysts for ammonia electro-oxidation reaction(AOR)with respect to both cost and performance is inadequate to ensure large scale commercial application of direct ammonia fuel cells.Recent studies found that alloying Pt with different transition metals and controlling the morphology of catalysts can improve the AOR activity,and thus potentially can solve the cost issue.Herein,(100)-terminated Pt-M nanocubes(M=3d-transition metals Fe,Co,Ni,Zn)are synthesized via wet-chemistry method and their catalytic activities toward AOR are evaluated.The addition of Fe,Co,Ni and Zn elements can enhance the AOR activity due to decrease in oxophilicity of platinum and bifunctional mechanism.Pt-Zn exhibits the maximum mass activity and specific ativity with values of 0.41 A/mgpt and 169 mA/cm2 that are 1.6 and 1.8 times higher than Pt nanocubes,respectively.Pt-Fe,Pt-Co and PI-Ni nanocubes also ilustrate higher mass and specific activities compared to Pt nanocubes.
基金the National Natural Science Foundation of China(Grant No.51678335)the China Postdoctoral Science Foundation(No.2015M57105).
文摘Ammonia-oxidizing archaeon(AOA)could play important roles for nitrogen removal in the bioreactors under conditions such as low pH and low dissolved oxygen.Therefore,enhancing ammonia oxidation capability of AOA has great significance for water and wastewater treatment,especially under conditions like low dissolved oxygen concentration.Utilizing a novel AOA strain SAT1,which was enriched from a wastewater treatment plant by our group,the effect of magnetic field on AOA’s ammonia oxidation capability,its magnetotaxis and heredity were investigated in this study.Compared with control experiment,AOA’s maximum nitrite-N formation rate during the cultivation increased by 56.8%(0.65 mgN/(L·d))with 20 mT magnetic field.Also,it was testified that AOA possessed a certain magnetotaxis.However,results manifested that the enhancement of AOA’s ammonia oxidation capability was not heritable,that is,lost once the magnetic field was removed.Additionally,the possible mechanism of improving AOA’s ammonia oxidation capability by magnetic field was owing to the promotion of AOA single cells’growth and fission,rather than the enhancement of their ammonia oxidation rates.The results shed light on the application of AOA and methods to enhance AOA’s ammonia oxidation capability,especially in wastewater treatment processes under certain conditions.
基金This work was supported by Westlake Education Foundation.
文摘Electrocatalytic ammonia oxidation reaction(EAOR)provides an ideal solution for on-board hydrogen supply for fuel cells,while the lack of efficient and durable EAOR catalysts has been a long-standing obstacle for its practical application.Herein,we reported that the defect engineering via in-situ electrochemically introducing oxygen vacancies(Vo)not only turns the inactive CuO into efficient EAOR catalyst but also achieves a high stability of over 400 h at a high current density of~200 mA·cm^(−2).Theoretical simulation reveals that the presence of Vo on the CuO surface induces a remarkable upshift of the d-band center of active Cu site closer to the Fermi level,which significantly stabilizes the reaction intermediates(*NHx)and efficiently oxidizes NH3 into N2.This Vo-modulated CuO shows a different catalytic mechanism from that on the conventional Pt-based catalysts,paving a new avenue to develop inexpensive,efficient,and robust catalysts,not limited to EAOR.
基金financially supported by National Natural Science Foundation of China(Grant No.51978007)Research Project of Education Department of Liaoning Province(2020jy009 and 2020jy011).
文摘Measurement and predicted variations of ammonia oxidation rate(AOR)are critical for the optimization of biological nitrogen removal,however,it is difficult to predict accurate AOR based on current models.In this study,a modified model was developed to predict AOR based on laboratoryscale tests and verified through pilot-scale tests.In biological nitrogen removal reactors,the specific ammonia oxidation rate(SAOR)was affected by both mixed liquor volatile suspended solids(MLVSS)concentration and temperature.When MLVSS increased 1.6,4.2,and 7.1-fold(1.3‒8.9 g/L,at 20℃),the measured SAOR decreased by 21%,49%,and 56%,respectively.Thereby,the estimated SAOR was suggested to modify when MLVSS changed through a power equation fitting.In addition,temperature coefficient(θ)was modified based on MLVSS concentration.These results suggested that the prediction of variations ammonia oxidation rate in real wastewater treatment system could be more accurate when considering the effect of MLVSS variations on SAOR.
文摘A range of plant species produce root exudates that inhibit ammonia-oxidizing microorganisms.This biological nitrification inhibition(BNI)capacity can decrease N loss and increase N uptake from the rhizosphere.This study sought evidence for the existence and magnitude of BNI capacity in canola(Brassica napus).Seedlings of three canola cultivars,Brachiaria humidicola(BNI positive)and wheat(Triticum aestivum)were grown in a hydroponic system.Root exudates were collected and their inhibition of the ammonia oxidizing bacterium,Nitrosospira multiformis,was tested.Subsequent pot experiments were used to test the inhibition of native nitrifying communities in soil.Root exudates from canola significantly reduced nitrification rates of both N.multiformis cultures and native soil microbial communities.The level of nitrification inhibition across the three cultivars was similar to the well-studied high-BNI species B.humidicola.BNI capacity of canola may have implications for the N dynamics in farming systems and the N uptake efficiency of crops in rotational farming systems.By reducing nitrification rates canola crops may decrease N losses,increase plant N uptake and encourage microbial N immobilization and subsequently increase the pool of organic N that is available for mineralization during the following cereal crops.
基金sponsored by the National Natural Science Foundation of China (21875133 and 51873100)the Fundamental Research Funds for the Central Universities (GK201901002 and GK201902014)the 111 Project (B14041)。
文摘The ammonia electrolysis is a highly efficient and energy-saving method for ultra-pure hydrogen generation, which highly relies on electrocatalytic performance of electrocatalysts. In this work, high-quality platinum(Pt) nanocubes(Pt-NCs) with 4.5 nm size are achieved by facile hydrothermal synthesis. The physical morphology and structure of Pt-NCs are exhaustively characterized, revealing that Pt-NCs with special {100} facets have excellent uniformity, good dispersity and high crystallinity. Meanwhile, the electrocatalytic performance of Pt-NCs for ammonia electrolysis are carefully investigated in alkaline solutions, which display outstanding electroactivity and stability for both ammonia electrooxidation reaction(AEOR) and hydrogen evolution reaction(HER) in KOH solution. Furthermore, a symmetric Pt-NCs||Pt-NCs ammonia electrolyzer based on bifunctional Pt-NCs electrocatalyst is constructed, which only requires 0.68 V electrolysis voltage for hydrogen generation. Additionally, the symmetric Pt-NCs||Pt-NCs ammonia electrolyzer has excellent reversible switch capability for AEOR at anode and HER at cathode, showing outstanding alternating operation ability for ammonia electrolysis.
基金financially supported by National Natural Science Foundation of China (No.U20A20130)Fundamental Research Funds for the Central Universities (No.06500152)
文摘Ce1-xZrxO_(2) composite oxides(molar,x=0-1.0,interval of 0.2)were prepared by a cetyltrimethylammonium bromide-assisted precipitation method.The enhancement of silver-species modification and catalytic mechanism of adsorption-transformationdesorption process were investigated over the Ag-impregnated catalysts for lowtemperature selective catalytic oxidation of ammonia(NH_(3)-SCO).The optimal 5 wt.%Ag/Ce_(0.6)Zr_(0.4)O_(2) catalyst presented good NH_(3)-SCO performancewith>90% NH_(3) conversion at temperature(T)≥250°C and 89% N_(2) selectivity.Despite the irregular block shape and underdeveloped specific surface area(∼60m2/g),the naked and Ag-modified Ce_(0.6)Zr_(0.4)O_(2) solid solution still obtained highly dispersed distribution of surface elements analyzed by scanning electron microscope-energy dispersive spectrometer(SEM-EDS)(mapping),N_(2) adsorptiondesorption test and X-ray diffraction(XRD).H2 temperature programmed reduction(H2-TPR)and X-ray photoelectron spectroscopy(XPS)results indicated that Ag-modification enhanced the mobility and activation of oxygen-species leading to a promotion on CeO_(2) reducibility and synergistic Ag0/Ag+and Ce^(4+)/Ce^(3+)redox cycles.Besides,Ag+/Ag_(2)O clusters could facilitate the formation of surface oxygen vacancies that was beneficial to the adsorption and activation of ammonia.NH3-temperature programmed desorption(NH_(3)-TPD)showed more adsorption-desorption capacity to ammoniawere provided by physical,weakandmedium-strong acid sites.Diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments revealed the activation of ammonia might be the control step of NH3-SCO procedure,during which NH3 dehydrogenation derived from NHx-species and also internal selective catalytic reduction(i-SCR)reactions were proposed.
基金Financial support from Ministerio de Ciencia e Innovación through projects PID2022-140143OB-I00(MCIN/AEI/10.13039/501100011033)and SO-CEX2019-000925-S(MCIN/AEI/10.13039/5011000110)supported by Marie Sk?odowska-Curie Actions Individual Fellowship grant funding to AMB,grant 101031365-SolTIMEthe support from the MSCA-COFUND I2:ICIQ Impulsion(GA 801474)。
文摘For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions to drive the water splitting reaction.Because of the lower thermodynamic requirements to oxidize ammonia compared to water,solar cells with smaller open circuit voltages can provide the required potential for ammonia splitting.In this work,a single perovskite solar cell with an open-circuit potential of 1.08 V is coupled to a 2-electrode electrochemical cell employing hybrid electroanodes functionalized with Ru-based molecular catalysts.The device is active for more than 30 min,producing N_(2) and H_(2) in a 1:2.9 ratio with 89%faradaic efficiency with no external applied bias.This work illustrates that hydrogen production from ammonia can be driven by conventional semiconductors.
基金supported by the National Natural Science Foundation of China (41471190)the National Key Research and Development Program of China (2016YFD0800102)+2 种基金the Special Fund for the Agricultural Public Welfare Profession of China (201503106)the Newton Fund, United Kingdom (BB/N013484/1)the GEF on the ‘Towards INMS’
文摘The upland agricultural soils in North China are distributed north of a line between the Kunlun Mountains, the Qinling Mountains and the Huaihe River. They occur in arid, semi-arid and semi-humid regions and crop production often depends on rain-fed or irrigation to supplement rainfall. This paper summarizes the characteristics of gross nitrogen(N) transformation, the fate of N fertilizer and soil N as well as the N loss pathway, and makes suggestions for proper N management in the region. The soils of the region are characterized by strong N mineralization and nitrification, and weak immobilization and denitrification ability, which lead to the production and accumulation of nitrate in the soil profile. Large amounts of accumulated nitrate have been observed in the vadose-zone in soils due to excess N fertilization in the past three decades, and this nitrate is subject to occasional leaching which leads to groundwater nitrate contamination. Under farmer's conventional high N fertilization practice in the winter wheat-summer maize rotation system(N application rate was approximately 600 kg ha–1 yr–1), crop N uptake, soil residual N, NH_3 volatilization, NO_3~– leaching, and denitrification loss accounted for around 27, 30, 23, 18 and 2% of the applied fertilizer N, respectively. NH_3 volatilization and NO_3~– leaching were the most important N loss pathways while soil residual N was an important fate of N fertilizer for replenishing soil N depletion from crop production. The upland agricultural soils in North China are a large source of N_2O and total emissions in this region make up a large proportion(approximately 54%) of Chinese cropland N_2O emissions. The "non-coupled strong ammonia oxidation" process is an important mechanism of N_2O production. Slowing down ammonia oxidation after ammonium-N fertilizer or urea application and avoiding transient high soil NH4+ concentrations are key measures for reducing N_2O emissions in this region. Further N management should aim to minimize N losses from crop and livestock production, and increase the recycling of manure and straw back to cropland. We also recommend adoption of the 4 R(Right soure, Right rate, Right time, Right place) fertilization techniques to realize proper N fertilizer management, and improving application methods or modifying fertilizer types to reduce NH_3 volatilization, improving water management to reduce NO_3~– leaching, and controlling the strong ammonia oxidation process to abate N_2O emission. Future research should focus on the study of the trade-off effects among different N loss pathways under different N application methods or fertilizer products.
基金financially supported by the National Natural Science Foundation of China (Nos. 51708543, 51438011 and 51722811)Water Pollution Control and Treatment National Science and Technology Major Project (Nos. 2017ZX07402001 and 2018ZX07110-007)。
文摘Electrochemical reduction of water to hydrogen(H2) offers a promising strategy for production of clean energy,but the design and optimization of electrochemical apparatus present challenges in terms of H2 recovery and energy consumption.Using cobalt phosphide nanoarrays(Co2 P/CoP NAs) as a charge mediator,we effectively separated the H2 and O2 evolution of alkaline water electrolysis in time,thereby achieving a membrane-free pathway for H2 purification.The hierarchical array structure and synergistic optimization of the electronic configuration of metallic Co2 P and metalloid CoP make the Co2 P/CoP NAs high-efficiency bifunctional electrocatalysts for both charge storage and hydrogen evolution.Theoretical investigations revealed that the introduction of Co2 P into CoP leads to a moderate hydrogen adsorption free energy and low water dissociation barrier,which are beneficial for boosting HER activity.Meanwhile,Co2 P/CoP NAs with high capacitance could maintain a cathodic H2 evolution time of 1500 s at 10 mA cm^(-2) driven by a low average voltage of 1.38 V.Alternatively,the energy stored in the mediator could be exhausted via coupling with the anodic oxidation of ammonia,whereby only 0.21 V was required to hold the current for 1188 s.This membrane-free architecture demonstrates the potential for developing hydrogen purification technology at low cost.
基金supported by the National Key Research and Development Program of China (Nos. 2020YFC1808502 and2018YFC1802804)the Open Project Program of the Key Laboratory of Environmental Protection & Safety of Communication Foundation Engineering,China Communications Construction Co.,Ltd
文摘In situ and simultaneous remediation of a variety of pollutants in sediments remains a challenge.In this study,we report that the combination of electrocoagulation(EC)and electrooxidation(EO)is efficient in the immobilization of phosphorus and heavymetals and in the oxidation of ammonium and toxic organicmatter.The integratedmixed metal oxide(MMO)/Fe anode system allowed the facile removal of ammonium and phosphorus in the overlying water(99% of 10 mg/L NH_(4)^(+)-N and 95% of 10 mg/L P disappeared in 15 and 30 min,respectively).Compared with the controls of the single Fe anode and single MMO anode systems,the dual MMO/Fe anode system significantly improved the removal of phenanthrene and promoted the transition of Pb and Cu from the mobile species to the immobile species.The concentrations of Pb and Cu in the toxicity characteristic leaching procedure extracts were reduced by 99%and 97% after an 8 hr operation.Further tests with four real polluted samples indicated that substantial proportions of acid-soluble fraction Pb and Cu were reduced(30%-31% for Pb and 16%–23% for Cu),and the amounts of total organic carbon and NH_(4)^(+)-N decreased by 56%–71% and 32%–63%,respectively.It was proposed that the in situ electrogenerated Fe(II)at the Fe anode and the active oxygen/chlorine species at the MMO anode are conducive to outstanding performance in the co-treatment of multiple pollutants.The results suggest that the EC/EO method is a powerful technology for the in situ remediation of sediments contaminated with different pollutants.
基金supported by the Energy Research Seed Grant from Duke Energy Initiative,the National Science Foundation(Nos.CHE-1565657 and CHE-1954838)the Army Research Office(W911NFN-18-2-004)+2 种基金S.H.and P.N.are both supported by fellowships from Department of Chemistry at Duke UniversityThis work was performed in part at the Duke University Shared Materials Instrumentation Facility(SMIF),a member of the North Carolina Research Triangle Nanotechnology Network(RTNN)which is supported by the National Science Foundation(award number ECCS-2025064)as part of the National Nanotechnology Coordinated Infrastructure(NNCI).
文摘Ammonia has emerged as a promising energy carrier owing to its carbon neutral content and low expense in long-range transportation.Therefore,development of a specific pathway to release the energy stored in ammonia is therefore in urgent demand.Electrochemical oxidation provides a convenient and reliable route to attain efficient utilization of ammonia.Here,we report that the high entropy(Mn,Fe,Co,Ni,Cu)_(3)O_(4)oxides can achieve high electrocatalytic activity for ammonia oxidation reaction(AOR)in non-aqueous solutions.The AOR onset overpotential of(Mn,Fe,Co,Ni,Cu)_(3)O_(4)is 0.70 V,which is nearly 0.2 V lower than that of their most active single metal cation counterpart.The mass spectroscopy study reveals that(Mn,Fe,Co,Ni,Cu)_(3)O_(4)preferentially oxidizes ammonia to environmentally friendly diatomic nitrogen with a Faradic efficiency of over 85%.The Xray photoelectron spectroscopy(XPS)result indicates that the balancing metal d-band of Mn and Cu cations helps retain a longlasting electrocatalytic activity.Overall,this work introduces a new family of earth-abundant transition metal high entropy oxide electrocatalysts for AOR,thus heralding a new paradigm of catalyst design for enabling ammonia as an energy carrier.
基金The COMRA Program under contract No. DY135-B2-01the Xiamen Ocean Economic Innovation and Development Demonstration Project under contract No. 16PZP001SF16the National Infrastructure of Natural Resources for Science and Technology Program of China under contract No. NIMR-2017-9。
文摘Nitrification is a key step in the global nitrogen cycle.Compared with autotrophic nitrification,heterotrophic nitrification remains poorly understood.In this study,Halomonas venusta MA-ZP17-13,isolated from seawater in shrimp aquaculture (Penaeus vannamei),could simultaneously undertake nitrification and denitrification.With the initial ammonium concentration at 100 mg/L,the maximum ammonium-nitrogen removal rate reached98.7%under the optimal conditions including C/N concentration ratio at 5.95,p H at 8.93,and Na Cl at 2.33%.The corresponding average removal rate was 1.37 mg/(L·h)(according to nitrogen) in 3 d at 11.2℃.By whole genome sequencing and analysis,nitrification-and denitrification-related genes were identified,including ammonia monooxygenase,nitrate reductase,nitrite reductase,nitric oxide dioxygenase and nitric oxide synthase;while no gene encoding hydroxylamine oxidase was identified,it implied the existence of a novel nitrification pathway from hydroxylamine to nitrate.These results indicate heterotrophic bacterium H.venusta MA-ZP17-13 can undertake simultaneous nitrification and denitrification at low temperature and has potential for NH_(4)^(+)-N/NH_(3)-N removal in marine aquaculture systems.
基金We thank Moria Nagy and G.S.N.Reddy for sharing their experiences with crust archaea.We are grateful to the staff of Sevilleta and Jornada LTER sites as well as the National Park Service(Canyonlands N.P.and Organ Pipe N.M.)for providing sampling permits,guidance,and hospitality.Finally,we thank Scott Bingham for assistance with qPCR and sequencing.This research was funded by an NSF grant from the Biodiversity Surveys and Inventories Program and by a USDA grant from the Soil Processes Program to FGP.
文摘Introduction:Biological soil crusts(BSCs)can dominate surface cover in dry lands worldwide,playing an integral role in arid land biogeochemistry,particularly in N fertilization through fixation and cycling.Nitrification is a characteristic and universal N transformation in BSCs that becomes important for the export of N beyond the microscopic bounds of the crust itself.The contribution of ammonia-oxidizing bacteria(AOB)in BSCs has been shown,but the role and extent of the recently discovered ammonia-oxidizing archaea(AOA)have not.Methods:We sampled various types of crusts in four desert regions across the western United States and characterized the composition and size of ammonia-oxidizing communities using clone libraries and quantitative PCR targeting the amoA gene,which codes for the ammonia monooxygenase enzyme,universally present in ammonia-oxidizing microbes.Results:All archaeal amoA sequences retrieved from BSCs belonged to the Thaumarchaeota(Nitrososphaera associated Group I.1b).Sequences from the Sonoran Desert,Colorado Plateau,and Great Basin were indistinguishable from each other but distinct from those of the Chihuahuan Desert.Based on amoA gene abundances,archaeal and bacterial ammonia oxidizers were ubiquitous in our survey,but the ratios of archaeal to bacterial ammonia oxidizers shifted from bacterially dominated in northern,cooler deserts to archaeally dominated in southern,warmer deserts.Conclusions:Archaea are shown to be potentially important biogeochemical agents of biological soil crust N cycling.Conditions associated with different types of BSCs and biogeographical factors reveal a niche differentiation between AOA and AOB,possibly driven by temperature.
文摘Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational performance.To address these drawbacks,this study investigated the effect of low intensity ultrasound treatment combined with hydroxylamine(NH2OH)on the performance of partial nitrification.Results showthat compared with the control group,low-intensity ultrasound treatment(0.10W/mL,15 min)combined with NH2OH(5 mg/L)reduced the time required for partial nitrification initiation by 6 days,increasing the nitrite accumulation rate(NAR)and ammonia nitro-gen removal rate(NRR)by 20.4% and 6.7%,respectively,achieving 96.48% NRR.Mechanis-tic analysis showed that NH2OH enhanced ammonia oxidation,inhibited nitrite-oxidizing bacteria(NOB)activity and shortened the time required for partial nitrification initiation.Furthermore,ultrasonication combined with NH2OH dosing stimulated EPS(extracellular polymeric substances)secretion,increased carbonyl,hydroxyl and amine functional group abundances and enhanced mass transfer.In addition,16S rRNA gene sequencing results showed that ultrasonication-sensitive Nitrospira disappeared from the ultrasound+NH_(2)OH system,while Nitrosomonas gradually became the dominant group.Collectively,the results of this study provide valuable insight into the enhancement of partial nitrification start-up during the process of wastewater nitrogen removal.
基金supported by the Foundation for Innovation Research Groups of the National Natural Science Foundation of China(No.62021003)Biological Wastewater Treatment and Process Control Technology,Beijing International Science and technology Cooperation Baseand the Founding projects of Beijing Municipal Commission of Education.
文摘Complete ammonia oxidizing bacteria,or comammox bacteria(CAOB),can oxidize ammonium to nitrate on its own.Its discovery revolutionized our understanding of biological nitrification,and its distribution in both natural and artificial systems has enabled a reevaluation of the relative contribution of microorganisms to the nitrogen cycle.Its wide distribution,adaptation to oligotrophic medium,and diverse metabolic pathways,means extensive research on CAOB and its application in water treatment can be promoted.Furthermore,the energy-saving characteristics of high oxygen affinity and low sludge production may also become frontier directions for wastewater treatment.This paper provides an overview of the discovery and environmental distribution of CAOB,as well as the physiological characteristics of the microorganisms,such as nutrient medium,environmental factors,enzymes,and metabolism,focusing on future research and the application of CAOB in wastewater treatment.Further research should be carried out on the physiological characteristics of CAOB,to analyze its ecological niche and impact factors,and explore its application potential in wastewater treatment nitrogen cycle improvement.