Climate warming and atmospheric nitrogen(N)deposition have profound influences on the terrestrial biosphere.However,how these two global change drivers affect phytoplankton which are important primary producers in wet...Climate warming and atmospheric nitrogen(N)deposition have profound influences on the terrestrial biosphere.However,how these two global change drivers affect phytoplankton which are important primary producers in wetlands with large carbon stocks and complex hydrological fluctuations remain largely unclear.As part of a two-year field experiment in a freshwater wetland,this study was conducted to investigate the effects of nighttime warming and N addition on phytoplankton biomass in the North China Plain.The results showed that neither nighttime warming nor N addition influenced the Shannon-Wiener index of phytoplankton community.Nighttime warming did not change phytoplankton biomass,likely due to the different warming impacts on dominant phyla and in different seasons.Decreased phytoplankton biomass in spring because of the increased water pH and submerged plant coverage was compensated by the enhanced biomass in autumn due to the reduced dissolved oxygen and submerged plant coverage,leading to the neutral change of phytoplankton biomass under warming.Nitrogen addition elevated phytoplankton biomass by 11.6%,which could be attributed to the enhanced nutrient availability and reduced submerged plant coverage.Positive relationships of methane(CH4)emission rates at the water-air interface with phytoplankton biomass indicated the potentially crucial role of phytoplankton in mediating wetland CH4 cycling through photosynthesis-driven metabolisms.The findings suggested the seasonal variation of phytoplankton and their potential responses to nighttime warming and N deposition,which may provide a more accurate basis for assessing the global change-carbon feedback in wetland ecosystems.展开更多
The Arno River Basin(Central Italy)is affected by a considerable anthropogenic pressure due to the presence of large cities and widespread industrial and agricultural practices.In this work,26 water samples from the A...The Arno River Basin(Central Italy)is affected by a considerable anthropogenic pressure due to the presence of large cities and widespread industrial and agricultural practices.In this work,26 water samples from the Arno River and its main tributaries were analyzed to assess the water pollution status.The geochemical composition of the Arno River changes from the source(dominated by a Ca-HCO_(3) facies)to the mouth(where a Na-Cl(SO4)chemistry prevails)with an increasing quality deterioration,as suggested by the Chemical Water Quality Index,due to anthropogenic contributions and seawater intrusion before flowing into the Ligurian Sea.The Ombrone and Usciana tributaries introduce anthropogenic pollutants into the Arno River,whilst Elsa tributary supplies significant contents of geogenic sulfate.The concentrations of dissolved nitrate and nitrite(up to 63 and 9 mg/L,respectively)and the respective isotopic values of𝛿15N and𝛿18O were also determined to understand origin and fate of the N-species in the Arno River Basin surface waters.The combined application of𝛿15N-NO_(3) and𝛿18O-NO_(3) and N-source apportionment modelling allowed the identification of soil organic nitrogen and sewage and domestic wastes as primary sources for dissolved NO_(3)-.The𝛿15N-NO_(2) and𝛿18O-NO_(2) values suggest that the nitrification process affects the ARB waters,thus controlling the abundances and proportion of the N-species.Our work indicates that additional efforts are needed to improve management strategies to reduce the release of nitrogenated species to the surface waters of the Arno River Basin,since little progress has been made from the early 2000s.展开更多
Here we firstly report a series of new deep eutectic solvents(DESs) induced by small amounts of crown ether complex and mainly formed by polyethylene glycol. These DESs not only presented the ultra-deep extraction of ...Here we firstly report a series of new deep eutectic solvents(DESs) induced by small amounts of crown ether complex and mainly formed by polyethylene glycol. These DESs not only presented the ultra-deep extraction of non-basic N-compounds from fuel oils, but also opened up the possibility of other new applications in chemistry and materials science.展开更多
Cryogenic rolling experiments have been conducted on the AZ31 magnesium(Mg)alloy sheet with bimodal non-basal texture,which is fabricated via the newly developed equal channel angular rolling and continuous bending pr...Cryogenic rolling experiments have been conducted on the AZ31 magnesium(Mg)alloy sheet with bimodal non-basal texture,which is fabricated via the newly developed equal channel angular rolling and continuous bending process with subsequent annealing(ECAR-CB-A)process.Results demonstrate that this sheet shows no edge cracks until the accumulated thickness reduction reaches about 18.5%,which is about 105.6%larger than that of the sheet with traditional basal texture.Characterization experiments including optical microstructure(OM),X-ray diffractometer(XRD),and electron backscatter diffraction(EBSD)measurements are then performed to explore the microstructure characteristics,texture evolution and deformation mechanisms during cryogenic rolling.Experimental observations confirm the occurrence of abundant{10–12}extension twins(ETs),twin-twin interactions among{10–12}ET variants and{10–12}-{10–12}double twins(DTs).The twinning behaviors as for{10–12}ETs are responsible for the concentration of c-axes of grains towards normal direction(ND)and the formation of transverse direction(TD)-component texture at the beginning of cryogenic rolling.The twinning behaviors with respect to{10–12}-{10–12}DTs are responsible for the disappearance of TD-component texture at the later stage of cryogenic rolling.The involved deformation mechanisms can be summarized as follows:Firstly{10–12}ETs dominate the plastic deformation.Subsequently,dislocation slip,especially basalslip,starts to sustain more plastic strain,while{10–12}ETs occur more frequently and enlarge continuously,resulting in the formation of twin-twin interaction among{10–12}ET variants.With the increasing rolling passes,{10–12}-{10–12}DTs incorporate in the plastic deformation and dislocation slip serves as the major one to sustain plastic strain.The activities of basalslip,{10–12}ETs and{10–12}-{10–12}DTs benefit in accommodating the plastic strain in sheet thickness,which contributes to the improved rolling formability in AZ31 Mg alloy sheet with bimodal non-basal texture during cryogenic rolling.展开更多
Since mid-2016,the low pathogenic H7N9 influenza virus has evolved into a highly pathogenic(HP)phenotype in China,raising many concerns about public health and poultry industry.The insertion of a“KRTA”motif at hemag...Since mid-2016,the low pathogenic H7N9 influenza virus has evolved into a highly pathogenic(HP)phenotype in China,raising many concerns about public health and poultry industry.The insertion of a“KRTA”motif at hemagglutinin cleavage site(HACS)occurred in the early stage of HP H7N9 variants.During the co-circulation,the HACS of HP-H7N9 variants were more polymorphic in birds and humans.Although HP-H7N9 variants,unlike the H5 subtype virus,exhibited the insertions of basic and non-basic amino acids,the underlying function of those insertions and substitutions remains unclear.The results of bioinformatics analysis indicated that the PEVPKRKRTAR/G motif of HACS had become the dominant motif in China.Then,we generated six H7N9 viruses bearing the PEIPKGR/G,PEVPKGR/G,PEVPKRKRTAR/G,PEVPKGKRTAR/G,PEVPKGKRIAR/G,and PEVPKRKRR/G motifs.Interestingly,after the deletion of threonine and alanine(TA)at HACS,the H7N9 viruses manifested decreased thermostability and virulence in mice,and the PEVPKRKRTAR/G-motif virus is prevalent in birds and humans probably due to its increased transmissibility and moderate virulence.By contrast,the insertion of non-basic amino acid isoleucine and alanine(IA)decreased the transmissibility in chickens and virulence in mice.Remarkably,the I335V substitution of H7N9 virus enhanced infectivity and transmission in chickens,suggesting that the combination of mutations and insertions of amino acids at the HACS promoted replication and pathogenicity in chickens and mice.The ongoing evolution of H7N9 increasingly threatens public health and poultry industry,so,its comprehensive surveillance and prevention of H7N9 viruses should be pursued.展开更多
The increase in soil temperature associated with climate change has introduced considerable challenges to crop production.Split nitrogen application(SN)represents a potential strategy for improving crop nitrogen use e...The increase in soil temperature associated with climate change has introduced considerable challenges to crop production.Split nitrogen application(SN)represents a potential strategy for improving crop nitrogen use efficiency and enhancing crop stress resistance.Nevertheless,the precise interaction between soil warming(SW)and SN remains unclear.In order to ascertain the impact of SW on maize growth and whether SN can improve the tolerance of maize to SW,a two-year field experiment was conducted(2022-2023).The aim was to examine the influence of two SW ranges(MT,warming 1.40℃;HT,warming 2.75℃)and two nitrogen application methods(N1,one-time basal application of nitrogen fertilizer;N2,one third of base nitrogen fertilizer+two thirds of jointing stage supplemental nitrogen fertilizer)on maize root growth,photosynthetic characteristics,nitrogen use efficiency,and yield.The results demonstrated that SW impeded root growth and precipitated the premature aging of maize leaves following anthesis,particularly in the HT,which led to a notable reduction in maize yield.In comparison to N1,SN has been shown to increase root length density by 8.54%,root bleeding rate by 8.57%,and enhance root distribution ratio in the middle soil layers(20-60 cm).The interaction between SW and SN had a notable impact on maize growth and yield.The SN improved the absorption and utilization efficiency of nitrogen by promoting root development and downward canopy growth,thus improving the tolerance of maize to SW at the later stage of growth.In particular,the N2HT resulted in a 14.51%increase in the photosynthetic rate,a 18.58%increase in nitrogen absorption efficiency,and a 18.32%increase in maize yield compared with N1HT.It can be posited that the SN represents a viable nitrogen management measure with the potential to enhance maize tolerance to soil high-temperature stress.展开更多
Nitrogen(N)uptake is regulated by water availability,and a water deficit can limit crop N responses by reducing N uptake and utilization.The complex and multifaceted interplay between water availability and the crop N...Nitrogen(N)uptake is regulated by water availability,and a water deficit can limit crop N responses by reducing N uptake and utilization.The complex and multifaceted interplay between water availability and the crop N response makes it difficult to predict and quantify the effect of water deficit on crop N status.The nitrogen nutrition index(NNI)has been widely used to accurately diagnose crop N status and to evaluate the effectiveness of N application.The decline of NNI under water-limiting conditions has been documented,although the underlying mechanism governing this decline is not fully understood.This study aimed to elucidate the reason for the decline of NNI under waterlimiting conditions and to provide insights into the accurate utilization of NNI for assessing crop N status under different water-N interaction treatments.Rainout shelter experiments were conducted over three growing seasons from 2018 to 2021 under different N(75 and 225 kg N ha^(-1),low N and high N)and water(120 to 510 mm,W0 to W3)co-limitation treatments.Plant N accumulation,shoot biomass(SB),plant N concentration(%N),soil nitrate-N content,actual evapotranspiration(ET_a),and yield were recorded at the stem elongation,booting,anthesis and grain filling stages.Compared to W0,W1 to W3 treatments exhibited NNI values that were greater by 10.2 to 20.5%,12.6to 24.8%,14 to 24.8%,and 16.8 to 24.8%at stem elongation,booting,anthesis,and grain filling,respectively,across the 2018-2021 seasons.This decline in NNI under water-limiting conditions stemmed from two main factors.First,reduced ET_(a) and SB led to a greater critical N concentration(%N_(c))under water-limiting conditions,which contributed to the decline in NNI primarily under high N conditions.Second,changes in plant%N played a more significant role under low N conditions.Plant N accumulation exhibited a positive allometric relationship with SB and a negative relationship with soil nitrate-N content under water-limiting conditions,indicating co-regulation by SB and the soil nitrate-N content.However,this regulation was influenced by water availability.Plant N accumulation sourced from the soil nitrate-N content reflects soil N availability.Greater soil water availability facilitated greater absorption of soil nitrate-N into the plants,leading to a positive correlation between plant N accumulation and ET_(a)across the different water-N interaction treatments.Therefore,considering the impact of soil water availability is crucial when assessing soil N availability under water-limiting conditions.The findings of this study provide valuable insights into the factors contributing to the decline in NNI among different water-N interaction treatments and can contribute to the more accurate utilization of NNI for assessing winter wheat N status.展开更多
The trade-off between yield and environmental effects caused by nitrogen fertilizer application is an important issue in wheat production.A reduction in fertile florets is one of the main reasons for the lower yields ...The trade-off between yield and environmental effects caused by nitrogen fertilizer application is an important issue in wheat production.A reduction in fertile florets is one of the main reasons for the lower yields under low nitrogen application rates.Brassinosteroids(BRs)have been found to play a role in nitrogen-induced rice spikelet degeneration.However,whether BRs play a role in wheat floret development and the mechanisms involved are not clear.Therefore,a nitrogen gradient experiment and exogenous spraying experiment were conducted to investigate the role and mechanism of BRs in wheat floret development under low nitrogen stress.The results showed that as the nitrogen application decreased,the endogenous BRs content of the spikes decreased,photosynthesis weakened,and total carbon,soluble sugar and starch in the spikes decreased,leading to a reduction in the number of fertile florets.Under low nitrogen stress,exogenous spraying of 24-epibrassinolide promoted photosynthesis,and stimulated stem fructan hydrolysis and the utilization and storage of sucrose in spikes,which directed more carbohydrates to the spikes and increased the number of fertile florets.In conclusion,BRs mediate the effects of nitrogen fertilizer on wheat floret development,and under low nitrogen stress,foliar spraying of 24-epibrassinolide promotes the flow of carbohydrates from the stem to the spikes,alleviating wheat floret degeneration.展开更多
The thermochemical non-equilibrium phenomena encountered by hypersonic vehicles present significant challenges in their design.To investigate the thermochemical reaction flow behind shock waves,the non-equilibrium rad...The thermochemical non-equilibrium phenomena encountered by hypersonic vehicles present significant challenges in their design.To investigate the thermochemical reaction flow behind shock waves,the non-equilibrium radiation in the visible range using a shock tube was studied.Experiments were conducted with a shock velocity of 4.7 km/s,using nitrogen at a pressure of 20 Pa.To address measurement difficulties associated with weak radiation,a special square section shock tube with a side length of 380 mm was utilized.A high-speed camera characterized the shock wave’s morphology,and a spectrograph and a monochromator captured the radiation.The spectra were analyzed,and the numerical spectra were compared with experimental results,showing a close match.Temperature changes behind the shock wave were obtained and compared with numerical predictions.The findings indicate that the vibrational temperatures are overestimated,while the vibrational relaxation time is likely underestimated,due to the oversimplified portrayals of the non-equilibrium relaxation process in the models.Additionally,both experimental and simulated time-resolved profiles of radiation intensity at specific wavelengths were analyzed.The gathered data aims to enhance computational fluid dynamics codes and radiation models,improving their predictive accuracy.展开更多
Ammonia and nitric acid,versatile industrial feedstocks,and burgeoning clean energy vectors hold immense promise for sustainable development.However,Haber–Bosch and Ostwald processes,which generates carbon dioxide as...Ammonia and nitric acid,versatile industrial feedstocks,and burgeoning clean energy vectors hold immense promise for sustainable development.However,Haber–Bosch and Ostwald processes,which generates carbon dioxide as massive by-product,contribute to greenhouse effects and pose environmental challenges.Thus,the pursuit of nitrogen fixation through carbon–neutral pathways under benign conditions is a frontier of scientific topics,with the harnessing of solar energy emerging as an enticing and viable option.This review delves into the refinement strategies for scale-up mild photocatalytic nitrogen fixation,fields ripe with potential for innovation.The narrative is centered on enhancing the intrinsic capabilities of catalysts to surmount current efficiency barriers.Key focus areas include the in-depth exploration of fundamental mechanisms underpinning photocatalytic procedures,rational element selection,and functional planning,state-of-the-art experimental protocols for understanding photo-fixation processes,valid photocatalytic activity evaluation,and the rational design of catalysts.Furthermore,the review offers a suite of forward-looking recommendations aimed at propelling the advancement of mild nitrogen photo-fixation.It scrutinizes the existing challenges and prospects within this burgeoning domain,aspiring to equip researchers with insightful perspectives that can catalyze the evolution of cutting-edge nitrogen fixation methodologies and steer the development of next-generation photocatalytic systems.展开更多
Macroalgae dominate nutrient dynamics and function as high-value foods for microbial,meio-and macrofaunal communities in coastal ecosystems.Because of this vital role,it is important to clarify the physiological infor...Macroalgae dominate nutrient dynamics and function as high-value foods for microbial,meio-and macrofaunal communities in coastal ecosystems.Because of this vital role,it is important to clarify the physiological information associated with environmental changes as it reflects their growth potential.To evaluate the effects of the changes in salinity and nutrients,the photosynthetic efficiency of a green macroalga Ulva fasciata from the Daya Bay was tested at a range of salinity(i.e.,31 to 10 psu)and nitrogen content(i.e.,5 to 60μmol L^(-1)).The results showed that cellular chlorophyll a(Chl a),carbohydrate and protein contents of U.fasciata were increased due to reduced salinity,and were decreased by interactive nitrogen enrichment.Within a short culture period(i.e.,18 h),the reduced salinity decreased the maximum photosynthetic efficiency(rETRmax and Pmax)derived from the rapid light response curve and photosynthetic oxygen evolution rate versus irradiance curve,respectively,as well as the saturation irradiance(E_(K)).This reducing effect diminished with enlonged cultivation time and reversed to a stimulating effect after 24 h of cultivation.The nitrogen enrichment stimulated the rETRmax and Pmax,as well as the E_(K),regardless of salinity,especially within short-term cultivation period(i.e.,<24 h).In addition,our results indicate that seawater freshening lowers the photosynthetic efficiency of U.fasciata in the short term,which is mitigated by nitrogen enrichment,but stimulates it in the long term,providing insight into how macroalgae thrive in coastal or estuarine waters where salinity and nutrients normally covary strongly.展开更多
In contrast to research on active sites in nanomaterials,lithium tantalate single crystals,known for their exceptional optical properties and long-range ordered lattice structure,present a promising avenue for in-dept...In contrast to research on active sites in nanomaterials,lithium tantalate single crystals,known for their exceptional optical properties and long-range ordered lattice structure,present a promising avenue for in-depth exploration of photocatalytic reaction systems with fewer constraints imposed by surface chemistry.Typically,the isotropy of a specific facet provides a perfect support for studying heteroatom doping.Herein,this work delves into the intrinsic catalytic sites for photocatalytic nitrogen fixation in iron-doped lithium tantalate single crystals.The presence of iron not only modifies the electronic structure of lithium tantalate,improving its light absorption capacity,but also functions as an active site for the nitrogen adsorption and activation.The photocatalytic ammonia production rate of the iron-doped lithium tantalate in pure water is maximum 26.95μg cm^(−2)h^(−1),which is three times higher than that of undoped lithium tantalate.The combination of first-principles simulations with in situ characterizations confirms that iron doping promotes the rate-determining step and changes the pathway of hydrogenation to associative alternating.This study provides a new perspective on in-depth investigation of intrinsic catalytic active sites in photocatalysis and other catalytic processes.展开更多
The application of organic fertilizers has become an increasingly popular practice in maize production to reduce thegaseous nitrogen(N) loss and soil degradation caused by inorganic fertilizers. Organic fertilizer pla...The application of organic fertilizers has become an increasingly popular practice in maize production to reduce thegaseous nitrogen(N) loss and soil degradation caused by inorganic fertilizers. Organic fertilizer plays a key rolein improving soil quality and stabilizing maize yields, but few studies have compared different substitution rates. Afield study was carried out in 2021 and 2022, based on a long-term trial initiated in 2016, which included five organicfertilizer N substitution rates with equal inputs of 200 kg N ha^(–1): 0% organic fertilizer(T1, 100% inorganic fertilizer),50.0% organic+50.0% inorganic fertilizer(T2), 37.5% organic+62.5% inorganic fertilizer(T3), 25.0% organic+75.0%inorganic fertilizer(T4), and 12.5% organic+87.5% inorganic fertilizer(T5), as well as a no fertilizer control(T6). Theresults of the two years showed that T3 and T1 had the highest grain yield and biomass, respectively, and there wasno significant difference between T1 and T3. Compared with T1, the 12.5, 25.0, 37.5, and 50.0% substitution rates in T5, T4, T3, and T2 significantly reduced total nitrogen losses(NH_(3), N_(2)O) by 8.3, 16.1, 18.7, and 27.0%, respectively.Nitrogen use efficiency(NUE) was higher in T5, T3, and T1, and there were no significant differences among them.Organic fertilizer substitution directly reduced NH_(3)volatilization and N_(2)O emission from farmland by lowering theammonium nitrogen and alkali-dissolved N contents and by increasing soil moisture. These substitution treatmentsreduced N_(2)O emissions indirectly by regulating the abundances of AOB and nirK-harboring genes by promotingsoil moisture. Specifically, the 37.5% organic fertilizer substitution reduces NH_(3)volatilization and N_(2)O emission from farmland by reducing the ammonium nitrogen and alkali-dissolved N contents and increasing moisture, which negatively regulate the abundance of AOB and nir K-harboring genes to reduce N_(2)O emissions indirectly in rainfed maize fields on the Loess Plateau of China.展开更多
To more accurately describe the coal damage and fracture evolution law during liquid nitrogen(LN_(2))fracturing under true triaxial stress,a thermal-hydraulic-mechanical-damage(THMD)coupling model for LN_(2) fracturin...To more accurately describe the coal damage and fracture evolution law during liquid nitrogen(LN_(2))fracturing under true triaxial stress,a thermal-hydraulic-mechanical-damage(THMD)coupling model for LN_(2) fracturing coal was developed,considering the coal heterogeneity and thermophysical parameters of nitrogen.The accuracy and applicability of model were verified by comparing with LN_(2) injection pre-cooling and fracturing experimental data.The effects of different pre-cooling times and horizontal stress ratios on coal damage evolution,permeability,temperature distribution,and fracture characteristics were analyzed.The results show that the permeability and damage of the coal increase exponentially,while the temperature decreases exponentially during the fracturing process.As the pre-cooling time increases,the damage range of the coal expands,and the fracture propagation becomes more pronounced.The initiation pressure and rupture pressure decrease and tend to stabilize with longer precooling times.As the horizontal stress ratio increases,fractures preferentially extend along the direction of maximum horizontal principal stress,leading to a significant decrease in both initiation and rupture pressures.At a horizontal stress ratio of 3,the initiation pressure drops by 48.07%,and the rupture pressure decreases by 41.36%.The results provide a theoretical basis for optimizing LN_(2) fracturing techniques and improving coal seam modification.展开更多
The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Cova...The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Covalent organic frameworks(COFs)offer a promising approach for CO_(2)transformation but lack high efficiency and selectivity in the absence of metals.Here,we have incorporated a pyridine nitrogen component into the imine-COF conjugated structure(Tp Pym).This innovative system has set a record of producing a CO yield of 1565μmol g^(-1)within 6 h.The soft X-ray absorption fine structure measurement proves that Tp Pym has both better conjugation and electron cloud enrichment.The electronic structure distribution delays the charge-carrier recombination,as evidenced by femtosecond transient absorption spectroscopy.The energy band diagram and theoretical calculation show that the conduction-band potential of Tp Pym is lower and the reduction reaction of CO_(2)to CO is more likely to occur.展开更多
A novel nitrogenous nickel-based deposited metal was prepared by gas metal arc welding.Subsequently,solid solution treatment as well as solution and aging treatments were conducted on the prepared metal to study the e...A novel nitrogenous nickel-based deposited metal was prepared by gas metal arc welding.Subsequently,solid solution treatment as well as solution and aging treatments were conducted on the prepared metal to study the evolution of microstructure and tensile properties at different states.Results show that the high-temperature tensile strength of the deposited metal exhibits good performance after the addition of W and N.The grain size of the sample is large,and petal-like Laves phase appears at the grain boundaries.After solid solution treatment,the grain size decreases,and the Laves phase disappears.However,both the yield strength and elongation of the deposited metal decrease.The grain size of the samples after solid solution and aging treatment is more uniform,nanoscale M(C,N)phases are precipitated within the crystals,and M_(23)C_(6) phase forms at grain boundaries.The yield strength and ultimate tensile strength of this sample are higher than those of the other samples,but its plasticity is the lowest.The main deformation mechanism is the unit dislocation a/2<110>cutting the precipitation phase.展开更多
The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation ...The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation and oxygen evolution competition,sluggish kinetics,low Faradaic efficiency,and limited nitrate yields.In this work,a novel two-dimensional(2D)layered MOF Mn-BCPPy(H_(2)BCPPy=3,5-di(4'-carboxyphenyl)pyridine)has been successfully synthesized.The framework is composed of a rod-manganese motifs and possesses abundant active sites including open metal sites(OMSs)and Lewis base sites(LBSs).The Mn-BCPPy is the first MOF catalyst applied in electrocatalytic NOR which NO_(3)^(-)exhibited relatively high activity with a yield of 99.75μg/(h·mg)and a Faraday efficiency(FE)of 32.09%.Furthermore,it can be used as fluorescent sensor for selectively and sensitively detect nitrofuran antibiotics(NFs).Therefore,this work explores the application of MOF materials in the field of electrocatalytic NOR,which reveals that manganese-based MOFs have great potential prospects.展开更多
Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.W...Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.We investigated the formation of nitrogen-induced diaph-ite structures(hybrid diamond-graphite phases)and their role in changing the conductivity.Nitrogen doping in a hy-drogen-rich plasma environment promotes the emergence of unique sp^(3)-sp^(2)bonding interfaces,where diamond grains are covalently integrated with graphitic domains,facilitating a structure-driven electronic transition.High-resolution transmis-sion electron microscopy and selected area electron diffraction reveal five-fold,six-fold and twelve-fold symmetries,along with an atypical{200}crystallographic reflection,confirming diaphite formation in 5%and 10%N-doped UNCD films,while high-er doping levels(15%and 20%)result in extensive graphitization.Raman spectroscopy tracks the evolution of sp^(2)bonding with increasing nitrogen content,while atomic force microscopy and X-ray diffraction indicate a consistent diamond grain size of~8 nm.Cryogenic electronic transport measurements reveal a conductivity increase from 8.72 to 708 S/cm as the nitrogen dop-ing level increases from 5%to 20%,which is attributed to defect-mediated carrier transport and 3D weak localization.The res-ulting conductivity is three orders of magnitude higher than previously reported.These findings establish a direct correlation between diaphite structural polymorphism and tunable electronic properties in nitrogen-doped UNCD films,offering new ways for defect-engineering diamond-based electronic materials.展开更多
Soil nitrogen(N)is the main limiting nutrient for plant growth,which is sensitive to variations in the soil oxygen environment.To provide insights into plant N accumulation and yield under aerated and drip irrigation,...Soil nitrogen(N)is the main limiting nutrient for plant growth,which is sensitive to variations in the soil oxygen environment.To provide insights into plant N accumulation and yield under aerated and drip irrigation,a greenhouse tomato experiment was conducted with six treatments,including three fertilization types:inorganic fertilizer(NPK);organic fertilizer(OM);chemical(75%of applied N)+organic fertilizer(25%)(NPK+OM)under drip irrigation(DI)and aerated irrigation(AI)methods.Under Al,total soil carbon mineralization(C_(min))was significantly higher(by 5.7-7.0%)than under DI irrigation.C_(min)in the fertilizer treatments followed the order NPK+OM>OM>NPK under both AI and DI.Potentially mineralizable C(C_(0))and N(N_(0))was greater under AI than under DI.Gross N mineralization,gross nitrification,and NH_(4)^(+)immobilization rates were significantly higher under the AINPK treatment than the DINPK treatment by 2.58-3.27-,1.25-1.44-,and 1-1.26-fold,respectively.These findings demonstrated that AI and the addition of organic fertilizer accelerated the turnover of soil organic matter and N transformation processes,thereby enhancing N availability.Moreover,the combination of AI and organic fertilizer application was found to promote root growth(8.4-10.6%),increase the duration of the period of rapid N accumulation(ΔT),and increase the maximum N accumulation rate(V_(max)),subsequently encouraging aboveground dry matter accumulation.Consequently,the AI treatment yield was significantly greater(by 6.3-12.4%)than under the DI treatment.Further,N partial factor productivity(NPFP)and N harvest index(NHI)were greater under AI than under DI,by 6.3 to 12.4%,and 4.6 to 8.1%,respectively.The rankings of yield and NPFP remained consistent,with NPK+OM>OM>NPK under both AI and DI treatments.These results highlighted the positive impacts of AI and organic fertilizer application on soil N availability,N uptake,and overall crop yield in tomato.The optimal management measure was identified as the AINPK+OM treatment,which led to more efficient N management,better crop growth,higher yield,and more sustainable agricultural practices.展开更多
In dryland ecosystems,nitrogen(N)is the primary limiting factor after water availability,constraining both plant productivity and organic matter decomposition while also regulating ecosystem function and service provi...In dryland ecosystems,nitrogen(N)is the primary limiting factor after water availability,constraining both plant productivity and organic matter decomposition while also regulating ecosystem function and service provision.However,the distributions of different soil N fraction stocks in drylands and the factors that influence them remain poorly understood.In this study,we collected 2076 soil samples from 173 sites across the drylands of northern China during the summers of 2021 and 2022.Using the best-performing eXtreme Gradient Boosting(XGBoost)model,we mapped the spatial distributions of the soil N fraction stocks and identified the key drivers of their variability.Our findings revealed that the stocks of total nitrogen(TN),inorganic nitrogen(IN),and microbial biomass nitrogen(MBN)in the top 30 cm soil layer were 1020.4,92.2,and 40.8 Tg,respectively,with corresponding mean densities of 164.6,14.9,and 6.6 g/m2.Climate variables-particularly mean annual temperature and aridity-along with human impacts emerged as the dominant drivers of soil N stock distribution.Notably,increased aridity and intensified human impacts exerted mutually counteracting effects on soil N fractions:aridity-driven moisture limitation generally suppressed N accumulation,whereas anthropogenic activities(e.g.,fertilization and grazing)promoted N enrichment.By identifying the key environmental and anthropogenic factors shaping the soil N distribution,this study improves the accuracy of regional and global N stock estimates.These insights provide a scientific foundation for developing more effective soil N management strategies in dryland ecosystems,contributing to sustainable land use and long-term ecosystem resilience in drylands.展开更多
基金supported by the Science and Technology Project of Hebei Education Department(No.QN2023028)the Natural Science Foundation of Hebei Province(No.C2022201042)+1 种基金the High-level Talent Research Funding Project of Hebei University(Nos.521000981405 and 521000981186)the Collaborative Innovation Center for Baiyangdian Basin Ecological Protection and Beijing-Tianjin-Hebei Sustainable Development.
文摘Climate warming and atmospheric nitrogen(N)deposition have profound influences on the terrestrial biosphere.However,how these two global change drivers affect phytoplankton which are important primary producers in wetlands with large carbon stocks and complex hydrological fluctuations remain largely unclear.As part of a two-year field experiment in a freshwater wetland,this study was conducted to investigate the effects of nighttime warming and N addition on phytoplankton biomass in the North China Plain.The results showed that neither nighttime warming nor N addition influenced the Shannon-Wiener index of phytoplankton community.Nighttime warming did not change phytoplankton biomass,likely due to the different warming impacts on dominant phyla and in different seasons.Decreased phytoplankton biomass in spring because of the increased water pH and submerged plant coverage was compensated by the enhanced biomass in autumn due to the reduced dissolved oxygen and submerged plant coverage,leading to the neutral change of phytoplankton biomass under warming.Nitrogen addition elevated phytoplankton biomass by 11.6%,which could be attributed to the enhanced nutrient availability and reduced submerged plant coverage.Positive relationships of methane(CH4)emission rates at the water-air interface with phytoplankton biomass indicated the potentially crucial role of phytoplankton in mediating wetland CH4 cycling through photosynthesis-driven metabolisms.The findings suggested the seasonal variation of phytoplankton and their potential responses to nighttime warming and N deposition,which may provide a more accurate basis for assessing the global change-carbon feedback in wetland ecosystems.
文摘The Arno River Basin(Central Italy)is affected by a considerable anthropogenic pressure due to the presence of large cities and widespread industrial and agricultural practices.In this work,26 water samples from the Arno River and its main tributaries were analyzed to assess the water pollution status.The geochemical composition of the Arno River changes from the source(dominated by a Ca-HCO_(3) facies)to the mouth(where a Na-Cl(SO4)chemistry prevails)with an increasing quality deterioration,as suggested by the Chemical Water Quality Index,due to anthropogenic contributions and seawater intrusion before flowing into the Ligurian Sea.The Ombrone and Usciana tributaries introduce anthropogenic pollutants into the Arno River,whilst Elsa tributary supplies significant contents of geogenic sulfate.The concentrations of dissolved nitrate and nitrite(up to 63 and 9 mg/L,respectively)and the respective isotopic values of𝛿15N and𝛿18O were also determined to understand origin and fate of the N-species in the Arno River Basin surface waters.The combined application of𝛿15N-NO_(3) and𝛿18O-NO_(3) and N-source apportionment modelling allowed the identification of soil organic nitrogen and sewage and domestic wastes as primary sources for dissolved NO_(3)-.The𝛿15N-NO_(2) and𝛿18O-NO_(2) values suggest that the nitrification process affects the ARB waters,thus controlling the abundances and proportion of the N-species.Our work indicates that additional efforts are needed to improve management strategies to reduce the release of nitrogenated species to the surface waters of the Arno River Basin,since little progress has been made from the early 2000s.
基金supported by the National Natrual Sciece Foundation of China (Nos. 21650110454, 21675164, 2 822407)the CAS-President International Fellowship Initiative (No. 2017PC0014)the Funds for Distinguished Young Scientists of Gansu (No. 1506RJDA281)
文摘Here we firstly report a series of new deep eutectic solvents(DESs) induced by small amounts of crown ether complex and mainly formed by polyethylene glycol. These DESs not only presented the ultra-deep extraction of non-basic N-compounds from fuel oils, but also opened up the possibility of other new applications in chemistry and materials science.
基金supported by the National Natural Science Foundation of China(Grant Nos.51805064,51822509)the Qingnian project of science and technology research program of Chongqing Education Commission of China(Grant No.KJQN202101141).
文摘Cryogenic rolling experiments have been conducted on the AZ31 magnesium(Mg)alloy sheet with bimodal non-basal texture,which is fabricated via the newly developed equal channel angular rolling and continuous bending process with subsequent annealing(ECAR-CB-A)process.Results demonstrate that this sheet shows no edge cracks until the accumulated thickness reduction reaches about 18.5%,which is about 105.6%larger than that of the sheet with traditional basal texture.Characterization experiments including optical microstructure(OM),X-ray diffractometer(XRD),and electron backscatter diffraction(EBSD)measurements are then performed to explore the microstructure characteristics,texture evolution and deformation mechanisms during cryogenic rolling.Experimental observations confirm the occurrence of abundant{10–12}extension twins(ETs),twin-twin interactions among{10–12}ET variants and{10–12}-{10–12}double twins(DTs).The twinning behaviors as for{10–12}ETs are responsible for the concentration of c-axes of grains towards normal direction(ND)and the formation of transverse direction(TD)-component texture at the beginning of cryogenic rolling.The twinning behaviors with respect to{10–12}-{10–12}DTs are responsible for the disappearance of TD-component texture at the later stage of cryogenic rolling.The involved deformation mechanisms can be summarized as follows:Firstly{10–12}ETs dominate the plastic deformation.Subsequently,dislocation slip,especially basalslip,starts to sustain more plastic strain,while{10–12}ETs occur more frequently and enlarge continuously,resulting in the formation of twin-twin interaction among{10–12}ET variants.With the increasing rolling passes,{10–12}-{10–12}DTs incorporate in the plastic deformation and dislocation slip serves as the major one to sustain plastic strain.The activities of basalslip,{10–12}ETs and{10–12}-{10–12}DTs benefit in accommodating the plastic strain in sheet thickness,which contributes to the improved rolling formability in AZ31 Mg alloy sheet with bimodal non-basal texture during cryogenic rolling.
基金supported by National Natural Science Foundation of China(31672586 and 31830097)the Key Research and Development Program of Guangdong Province(2019B020218004)+2 种基金Earmarked Found for China Agriculture Research System(CARS-41-G16)Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme(2018,Wenbao Qi)Young Scholars of Yangtze River Scholar Professor Program(2019,Wenbao Qi)
文摘Since mid-2016,the low pathogenic H7N9 influenza virus has evolved into a highly pathogenic(HP)phenotype in China,raising many concerns about public health and poultry industry.The insertion of a“KRTA”motif at hemagglutinin cleavage site(HACS)occurred in the early stage of HP H7N9 variants.During the co-circulation,the HACS of HP-H7N9 variants were more polymorphic in birds and humans.Although HP-H7N9 variants,unlike the H5 subtype virus,exhibited the insertions of basic and non-basic amino acids,the underlying function of those insertions and substitutions remains unclear.The results of bioinformatics analysis indicated that the PEVPKRKRTAR/G motif of HACS had become the dominant motif in China.Then,we generated six H7N9 viruses bearing the PEIPKGR/G,PEVPKGR/G,PEVPKRKRTAR/G,PEVPKGKRTAR/G,PEVPKGKRIAR/G,and PEVPKRKRR/G motifs.Interestingly,after the deletion of threonine and alanine(TA)at HACS,the H7N9 viruses manifested decreased thermostability and virulence in mice,and the PEVPKRKRTAR/G-motif virus is prevalent in birds and humans probably due to its increased transmissibility and moderate virulence.By contrast,the insertion of non-basic amino acid isoleucine and alanine(IA)decreased the transmissibility in chickens and virulence in mice.Remarkably,the I335V substitution of H7N9 virus enhanced infectivity and transmission in chickens,suggesting that the combination of mutations and insertions of amino acids at the HACS promoted replication and pathogenicity in chickens and mice.The ongoing evolution of H7N9 increasingly threatens public health and poultry industry,so,its comprehensive surveillance and prevention of H7N9 viruses should be pursued.
基金supported by the Natural Science Fund of China(31771724)the Key Research and Development Project of Shaanxi Province(2024NC-ZDCYL-01-10).
文摘The increase in soil temperature associated with climate change has introduced considerable challenges to crop production.Split nitrogen application(SN)represents a potential strategy for improving crop nitrogen use efficiency and enhancing crop stress resistance.Nevertheless,the precise interaction between soil warming(SW)and SN remains unclear.In order to ascertain the impact of SW on maize growth and whether SN can improve the tolerance of maize to SW,a two-year field experiment was conducted(2022-2023).The aim was to examine the influence of two SW ranges(MT,warming 1.40℃;HT,warming 2.75℃)and two nitrogen application methods(N1,one-time basal application of nitrogen fertilizer;N2,one third of base nitrogen fertilizer+two thirds of jointing stage supplemental nitrogen fertilizer)on maize root growth,photosynthetic characteristics,nitrogen use efficiency,and yield.The results demonstrated that SW impeded root growth and precipitated the premature aging of maize leaves following anthesis,particularly in the HT,which led to a notable reduction in maize yield.In comparison to N1,SN has been shown to increase root length density by 8.54%,root bleeding rate by 8.57%,and enhance root distribution ratio in the middle soil layers(20-60 cm).The interaction between SW and SN had a notable impact on maize growth and yield.The SN improved the absorption and utilization efficiency of nitrogen by promoting root development and downward canopy growth,thus improving the tolerance of maize to SW at the later stage of growth.In particular,the N2HT resulted in a 14.51%increase in the photosynthetic rate,a 18.58%increase in nitrogen absorption efficiency,and a 18.32%increase in maize yield compared with N1HT.It can be posited that the SN represents a viable nitrogen management measure with the potential to enhance maize tolerance to soil high-temperature stress.
基金supported by the National Natural Science Foundation of China(51609247)the Henan Provincial Natural Science Foundation,China(222300420589,202300410553)+4 种基金the Central Public-interest Scientific Institution Basal Research Fund,China(FIRI2022-22)the Science&Technology Fundamental Resources Investigation Program,China(2022FY101601)the Science and Technology Project of Xinxiang City,Henan Province,China(GG2021024)the Major Special Science and Technology Project of Henan Province,China(221100110700)the Joint Fund of Science and Technology Research and Development Plan of Henan Province,China(Superior Discipline Cultivation)(222301420104)。
文摘Nitrogen(N)uptake is regulated by water availability,and a water deficit can limit crop N responses by reducing N uptake and utilization.The complex and multifaceted interplay between water availability and the crop N response makes it difficult to predict and quantify the effect of water deficit on crop N status.The nitrogen nutrition index(NNI)has been widely used to accurately diagnose crop N status and to evaluate the effectiveness of N application.The decline of NNI under water-limiting conditions has been documented,although the underlying mechanism governing this decline is not fully understood.This study aimed to elucidate the reason for the decline of NNI under waterlimiting conditions and to provide insights into the accurate utilization of NNI for assessing crop N status under different water-N interaction treatments.Rainout shelter experiments were conducted over three growing seasons from 2018 to 2021 under different N(75 and 225 kg N ha^(-1),low N and high N)and water(120 to 510 mm,W0 to W3)co-limitation treatments.Plant N accumulation,shoot biomass(SB),plant N concentration(%N),soil nitrate-N content,actual evapotranspiration(ET_a),and yield were recorded at the stem elongation,booting,anthesis and grain filling stages.Compared to W0,W1 to W3 treatments exhibited NNI values that were greater by 10.2 to 20.5%,12.6to 24.8%,14 to 24.8%,and 16.8 to 24.8%at stem elongation,booting,anthesis,and grain filling,respectively,across the 2018-2021 seasons.This decline in NNI under water-limiting conditions stemmed from two main factors.First,reduced ET_(a) and SB led to a greater critical N concentration(%N_(c))under water-limiting conditions,which contributed to the decline in NNI primarily under high N conditions.Second,changes in plant%N played a more significant role under low N conditions.Plant N accumulation exhibited a positive allometric relationship with SB and a negative relationship with soil nitrate-N content under water-limiting conditions,indicating co-regulation by SB and the soil nitrate-N content.However,this regulation was influenced by water availability.Plant N accumulation sourced from the soil nitrate-N content reflects soil N availability.Greater soil water availability facilitated greater absorption of soil nitrate-N into the plants,leading to a positive correlation between plant N accumulation and ET_(a)across the different water-N interaction treatments.Therefore,considering the impact of soil water availability is crucial when assessing soil N availability under water-limiting conditions.The findings of this study provide valuable insights into the factors contributing to the decline in NNI among different water-N interaction treatments and can contribute to the more accurate utilization of NNI for assessing winter wheat N status.
基金supported by the Key Research and Development Program of Shaanxi,China(2021NY-083)the National Natural Science Foundation of China(31871567)。
文摘The trade-off between yield and environmental effects caused by nitrogen fertilizer application is an important issue in wheat production.A reduction in fertile florets is one of the main reasons for the lower yields under low nitrogen application rates.Brassinosteroids(BRs)have been found to play a role in nitrogen-induced rice spikelet degeneration.However,whether BRs play a role in wheat floret development and the mechanisms involved are not clear.Therefore,a nitrogen gradient experiment and exogenous spraying experiment were conducted to investigate the role and mechanism of BRs in wheat floret development under low nitrogen stress.The results showed that as the nitrogen application decreased,the endogenous BRs content of the spikes decreased,photosynthesis weakened,and total carbon,soluble sugar and starch in the spikes decreased,leading to a reduction in the number of fertile florets.Under low nitrogen stress,exogenous spraying of 24-epibrassinolide promoted photosynthesis,and stimulated stem fructan hydrolysis and the utilization and storage of sucrose in spikes,which directed more carbohydrates to the spikes and increased the number of fertile florets.In conclusion,BRs mediate the effects of nitrogen fertilizer on wheat floret development,and under low nitrogen stress,foliar spraying of 24-epibrassinolide promotes the flow of carbohydrates from the stem to the spikes,alleviating wheat floret degeneration.
基金supported by the Key-Area Research and Development Program of Guangdong Province(Grant No.2021B0909060004)the National Natural Science Foundation of China(Grant Nos.12072355 and 92271117)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0620202).
文摘The thermochemical non-equilibrium phenomena encountered by hypersonic vehicles present significant challenges in their design.To investigate the thermochemical reaction flow behind shock waves,the non-equilibrium radiation in the visible range using a shock tube was studied.Experiments were conducted with a shock velocity of 4.7 km/s,using nitrogen at a pressure of 20 Pa.To address measurement difficulties associated with weak radiation,a special square section shock tube with a side length of 380 mm was utilized.A high-speed camera characterized the shock wave’s morphology,and a spectrograph and a monochromator captured the radiation.The spectra were analyzed,and the numerical spectra were compared with experimental results,showing a close match.Temperature changes behind the shock wave were obtained and compared with numerical predictions.The findings indicate that the vibrational temperatures are overestimated,while the vibrational relaxation time is likely underestimated,due to the oversimplified portrayals of the non-equilibrium relaxation process in the models.Additionally,both experimental and simulated time-resolved profiles of radiation intensity at specific wavelengths were analyzed.The gathered data aims to enhance computational fluid dynamics codes and radiation models,improving their predictive accuracy.
基金financially supported by the National Natural Science Foundation of China(No.21675131)the Volkswagen Foundation(Freigeist Fellowship No.89592)+1 种基金the Natural Science Foundation of Chongqing(No.2020jcyj-zdxmX0003,CSTB2023NSCQ-MSX0924)the National Research Foundation,Singapore,and A*STAR(Agency for Science Technology and Research)under its LCER Phase 2 Programme Hydrogen&Emerging Technologies FI,Directed Hydrogen Programme(Award No.U2305D4003).
文摘Ammonia and nitric acid,versatile industrial feedstocks,and burgeoning clean energy vectors hold immense promise for sustainable development.However,Haber–Bosch and Ostwald processes,which generates carbon dioxide as massive by-product,contribute to greenhouse effects and pose environmental challenges.Thus,the pursuit of nitrogen fixation through carbon–neutral pathways under benign conditions is a frontier of scientific topics,with the harnessing of solar energy emerging as an enticing and viable option.This review delves into the refinement strategies for scale-up mild photocatalytic nitrogen fixation,fields ripe with potential for innovation.The narrative is centered on enhancing the intrinsic capabilities of catalysts to surmount current efficiency barriers.Key focus areas include the in-depth exploration of fundamental mechanisms underpinning photocatalytic procedures,rational element selection,and functional planning,state-of-the-art experimental protocols for understanding photo-fixation processes,valid photocatalytic activity evaluation,and the rational design of catalysts.Furthermore,the review offers a suite of forward-looking recommendations aimed at propelling the advancement of mild nitrogen photo-fixation.It scrutinizes the existing challenges and prospects within this burgeoning domain,aspiring to equip researchers with insightful perspectives that can catalyze the evolution of cutting-edge nitrogen fixation methodologies and steer the development of next-generation photocatalytic systems.
基金funded by the National Key Research and Development Program of China(No.20022YFC3102405)the National Natural Science Foundation of China(Nos.42425004,32371665)the Natural Science Foundation of Guangdong Province(Nos.2022A1515011461,2022A1515011831)。
文摘Macroalgae dominate nutrient dynamics and function as high-value foods for microbial,meio-and macrofaunal communities in coastal ecosystems.Because of this vital role,it is important to clarify the physiological information associated with environmental changes as it reflects their growth potential.To evaluate the effects of the changes in salinity and nutrients,the photosynthetic efficiency of a green macroalga Ulva fasciata from the Daya Bay was tested at a range of salinity(i.e.,31 to 10 psu)and nitrogen content(i.e.,5 to 60μmol L^(-1)).The results showed that cellular chlorophyll a(Chl a),carbohydrate and protein contents of U.fasciata were increased due to reduced salinity,and were decreased by interactive nitrogen enrichment.Within a short culture period(i.e.,18 h),the reduced salinity decreased the maximum photosynthetic efficiency(rETRmax and Pmax)derived from the rapid light response curve and photosynthetic oxygen evolution rate versus irradiance curve,respectively,as well as the saturation irradiance(E_(K)).This reducing effect diminished with enlonged cultivation time and reversed to a stimulating effect after 24 h of cultivation.The nitrogen enrichment stimulated the rETRmax and Pmax,as well as the E_(K),regardless of salinity,especially within short-term cultivation period(i.e.,<24 h).In addition,our results indicate that seawater freshening lowers the photosynthetic efficiency of U.fasciata in the short term,which is mitigated by nitrogen enrichment,but stimulates it in the long term,providing insight into how macroalgae thrive in coastal or estuarine waters where salinity and nutrients normally covary strongly.
基金supported by Natural Science Foundation of Shandong Province(Nos.ZR2022YQ42,ZR2021JQ15,ZR2021QE011,ZR2021ZD20,2022GJJLJRC-01)Innovative Team Project of Jinan(No.2021GXRC019)the National Natural Science Foundation of China(Nos.52022037,52202366).
文摘In contrast to research on active sites in nanomaterials,lithium tantalate single crystals,known for their exceptional optical properties and long-range ordered lattice structure,present a promising avenue for in-depth exploration of photocatalytic reaction systems with fewer constraints imposed by surface chemistry.Typically,the isotropy of a specific facet provides a perfect support for studying heteroatom doping.Herein,this work delves into the intrinsic catalytic sites for photocatalytic nitrogen fixation in iron-doped lithium tantalate single crystals.The presence of iron not only modifies the electronic structure of lithium tantalate,improving its light absorption capacity,but also functions as an active site for the nitrogen adsorption and activation.The photocatalytic ammonia production rate of the iron-doped lithium tantalate in pure water is maximum 26.95μg cm^(−2)h^(−1),which is three times higher than that of undoped lithium tantalate.The combination of first-principles simulations with in situ characterizations confirms that iron doping promotes the rate-determining step and changes the pathway of hydrogenation to associative alternating.This study provides a new perspective on in-depth investigation of intrinsic catalytic active sites in photocatalysis and other catalytic processes.
基金supported by the State Key Laboratory of Arid Land Crop Science, Gansu Agricultural University,China (GSCS-2022-Z02)the National Key R&D Program of China (2022YFD1900300)+2 种基金the National Natural Science Foundation of China (32260549)the Innovation Group of Basic Research in Gansu Province, China (25JRRA807)the Major Special Research Projects in Gansu Province, China (22ZD6NA009)。
文摘The application of organic fertilizers has become an increasingly popular practice in maize production to reduce thegaseous nitrogen(N) loss and soil degradation caused by inorganic fertilizers. Organic fertilizer plays a key rolein improving soil quality and stabilizing maize yields, but few studies have compared different substitution rates. Afield study was carried out in 2021 and 2022, based on a long-term trial initiated in 2016, which included five organicfertilizer N substitution rates with equal inputs of 200 kg N ha^(–1): 0% organic fertilizer(T1, 100% inorganic fertilizer),50.0% organic+50.0% inorganic fertilizer(T2), 37.5% organic+62.5% inorganic fertilizer(T3), 25.0% organic+75.0%inorganic fertilizer(T4), and 12.5% organic+87.5% inorganic fertilizer(T5), as well as a no fertilizer control(T6). Theresults of the two years showed that T3 and T1 had the highest grain yield and biomass, respectively, and there wasno significant difference between T1 and T3. Compared with T1, the 12.5, 25.0, 37.5, and 50.0% substitution rates in T5, T4, T3, and T2 significantly reduced total nitrogen losses(NH_(3), N_(2)O) by 8.3, 16.1, 18.7, and 27.0%, respectively.Nitrogen use efficiency(NUE) was higher in T5, T3, and T1, and there were no significant differences among them.Organic fertilizer substitution directly reduced NH_(3)volatilization and N_(2)O emission from farmland by lowering theammonium nitrogen and alkali-dissolved N contents and by increasing soil moisture. These substitution treatmentsreduced N_(2)O emissions indirectly by regulating the abundances of AOB and nirK-harboring genes by promotingsoil moisture. Specifically, the 37.5% organic fertilizer substitution reduces NH_(3)volatilization and N_(2)O emission from farmland by reducing the ammonium nitrogen and alkali-dissolved N contents and increasing moisture, which negatively regulate the abundance of AOB and nir K-harboring genes to reduce N_(2)O emissions indirectly in rainfed maize fields on the Loess Plateau of China.
基金financially supported by the National Natural Science Foundation of China(Nos.51874236 and 52174207)Shaanxi Science and Technology Innovation Team(No.2022TD02)Henan University of Science and Technology PhD Funded Projects(No.B2025-9)。
文摘To more accurately describe the coal damage and fracture evolution law during liquid nitrogen(LN_(2))fracturing under true triaxial stress,a thermal-hydraulic-mechanical-damage(THMD)coupling model for LN_(2) fracturing coal was developed,considering the coal heterogeneity and thermophysical parameters of nitrogen.The accuracy and applicability of model were verified by comparing with LN_(2) injection pre-cooling and fracturing experimental data.The effects of different pre-cooling times and horizontal stress ratios on coal damage evolution,permeability,temperature distribution,and fracture characteristics were analyzed.The results show that the permeability and damage of the coal increase exponentially,while the temperature decreases exponentially during the fracturing process.As the pre-cooling time increases,the damage range of the coal expands,and the fracture propagation becomes more pronounced.The initiation pressure and rupture pressure decrease and tend to stabilize with longer precooling times.As the horizontal stress ratio increases,fractures preferentially extend along the direction of maximum horizontal principal stress,leading to a significant decrease in both initiation and rupture pressures.At a horizontal stress ratio of 3,the initiation pressure drops by 48.07%,and the rupture pressure decreases by 41.36%.The results provide a theoretical basis for optimizing LN_(2) fracturing techniques and improving coal seam modification.
基金supported by the National Natural Science Foundation of China(Nos.22375031,22202037,22472023)the Fundamental Research Funds for the Central Universities(Nos.2412023YQ001,2412023QD019,2412024QD014)+1 种基金supported by grants from the seventh batch of Jilin Province Youth Science and Technology Talent Lifting Project(No.QT202305)Science and Technology Development Plan Project of Jilin Province,China(No.20240101192JC)。
文摘The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Covalent organic frameworks(COFs)offer a promising approach for CO_(2)transformation but lack high efficiency and selectivity in the absence of metals.Here,we have incorporated a pyridine nitrogen component into the imine-COF conjugated structure(Tp Pym).This innovative system has set a record of producing a CO yield of 1565μmol g^(-1)within 6 h.The soft X-ray absorption fine structure measurement proves that Tp Pym has both better conjugation and electron cloud enrichment.The electronic structure distribution delays the charge-carrier recombination,as evidenced by femtosecond transient absorption spectroscopy.The energy band diagram and theoretical calculation show that the conduction-band potential of Tp Pym is lower and the reduction reaction of CO_(2)to CO is more likely to occur.
文摘A novel nitrogenous nickel-based deposited metal was prepared by gas metal arc welding.Subsequently,solid solution treatment as well as solution and aging treatments were conducted on the prepared metal to study the evolution of microstructure and tensile properties at different states.Results show that the high-temperature tensile strength of the deposited metal exhibits good performance after the addition of W and N.The grain size of the sample is large,and petal-like Laves phase appears at the grain boundaries.After solid solution treatment,the grain size decreases,and the Laves phase disappears.However,both the yield strength and elongation of the deposited metal decrease.The grain size of the samples after solid solution and aging treatment is more uniform,nanoscale M(C,N)phases are precipitated within the crystals,and M_(23)C_(6) phase forms at grain boundaries.The yield strength and ultimate tensile strength of this sample are higher than those of the other samples,but its plasticity is the lowest.The main deformation mechanism is the unit dislocation a/2<110>cutting the precipitation phase.
基金supported by Natural Science Foundation of Shandong Province(ZR2021MB075)Fundamental Research Funds for the Central Universities,Ocean University of China(202461021).
文摘The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation and oxygen evolution competition,sluggish kinetics,low Faradaic efficiency,and limited nitrate yields.In this work,a novel two-dimensional(2D)layered MOF Mn-BCPPy(H_(2)BCPPy=3,5-di(4'-carboxyphenyl)pyridine)has been successfully synthesized.The framework is composed of a rod-manganese motifs and possesses abundant active sites including open metal sites(OMSs)and Lewis base sites(LBSs).The Mn-BCPPy is the first MOF catalyst applied in electrocatalytic NOR which NO_(3)^(-)exhibited relatively high activity with a yield of 99.75μg/(h·mg)and a Faraday efficiency(FE)of 32.09%.Furthermore,it can be used as fluorescent sensor for selectively and sensitively detect nitrofuran antibiotics(NFs).Therefore,this work explores the application of MOF materials in the field of electrocatalytic NOR,which reveals that manganese-based MOFs have great potential prospects.
文摘Nitrogen doping in chemical vapor deposition-derived ultrananocrystalline diamond(UNCD)films in-creases the electronic conductivity,yet its microstructural effects on electron transport are insufficiently understood.We investigated the formation of nitrogen-induced diaph-ite structures(hybrid diamond-graphite phases)and their role in changing the conductivity.Nitrogen doping in a hy-drogen-rich plasma environment promotes the emergence of unique sp^(3)-sp^(2)bonding interfaces,where diamond grains are covalently integrated with graphitic domains,facilitating a structure-driven electronic transition.High-resolution transmis-sion electron microscopy and selected area electron diffraction reveal five-fold,six-fold and twelve-fold symmetries,along with an atypical{200}crystallographic reflection,confirming diaphite formation in 5%and 10%N-doped UNCD films,while high-er doping levels(15%and 20%)result in extensive graphitization.Raman spectroscopy tracks the evolution of sp^(2)bonding with increasing nitrogen content,while atomic force microscopy and X-ray diffraction indicate a consistent diamond grain size of~8 nm.Cryogenic electronic transport measurements reveal a conductivity increase from 8.72 to 708 S/cm as the nitrogen dop-ing level increases from 5%to 20%,which is attributed to defect-mediated carrier transport and 3D weak localization.The res-ulting conductivity is three orders of magnitude higher than previously reported.These findings establish a direct correlation between diaphite structural polymorphism and tunable electronic properties in nitrogen-doped UNCD films,offering new ways for defect-engineering diamond-based electronic materials.
基金supported by the National Natural Science Foundation of China for Young Scholars(52109066)the Postdoctoral Science Foundation of Shaanxi Province,China(2023BSHTBZZ29)the China Postdoctoral Science Foundation(2022M712604 and 2023T160534).
文摘Soil nitrogen(N)is the main limiting nutrient for plant growth,which is sensitive to variations in the soil oxygen environment.To provide insights into plant N accumulation and yield under aerated and drip irrigation,a greenhouse tomato experiment was conducted with six treatments,including three fertilization types:inorganic fertilizer(NPK);organic fertilizer(OM);chemical(75%of applied N)+organic fertilizer(25%)(NPK+OM)under drip irrigation(DI)and aerated irrigation(AI)methods.Under Al,total soil carbon mineralization(C_(min))was significantly higher(by 5.7-7.0%)than under DI irrigation.C_(min)in the fertilizer treatments followed the order NPK+OM>OM>NPK under both AI and DI.Potentially mineralizable C(C_(0))and N(N_(0))was greater under AI than under DI.Gross N mineralization,gross nitrification,and NH_(4)^(+)immobilization rates were significantly higher under the AINPK treatment than the DINPK treatment by 2.58-3.27-,1.25-1.44-,and 1-1.26-fold,respectively.These findings demonstrated that AI and the addition of organic fertilizer accelerated the turnover of soil organic matter and N transformation processes,thereby enhancing N availability.Moreover,the combination of AI and organic fertilizer application was found to promote root growth(8.4-10.6%),increase the duration of the period of rapid N accumulation(ΔT),and increase the maximum N accumulation rate(V_(max)),subsequently encouraging aboveground dry matter accumulation.Consequently,the AI treatment yield was significantly greater(by 6.3-12.4%)than under the DI treatment.Further,N partial factor productivity(NPFP)and N harvest index(NHI)were greater under AI than under DI,by 6.3 to 12.4%,and 4.6 to 8.1%,respectively.The rankings of yield and NPFP remained consistent,with NPK+OM>OM>NPK under both AI and DI treatments.These results highlighted the positive impacts of AI and organic fertilizer application on soil N availability,N uptake,and overall crop yield in tomato.The optimal management measure was identified as the AINPK+OM treatment,which led to more efficient N management,better crop growth,higher yield,and more sustainable agricultural practices.
基金supported by the Xinjiang Outstanding Youth Fund(2021D01E03)the Natural Science Foundation of Xinjiang Uygur Autonomous Region(2022D01D083)the National Natural Science Foundation of China(U2003214,41977099).
文摘In dryland ecosystems,nitrogen(N)is the primary limiting factor after water availability,constraining both plant productivity and organic matter decomposition while also regulating ecosystem function and service provision.However,the distributions of different soil N fraction stocks in drylands and the factors that influence them remain poorly understood.In this study,we collected 2076 soil samples from 173 sites across the drylands of northern China during the summers of 2021 and 2022.Using the best-performing eXtreme Gradient Boosting(XGBoost)model,we mapped the spatial distributions of the soil N fraction stocks and identified the key drivers of their variability.Our findings revealed that the stocks of total nitrogen(TN),inorganic nitrogen(IN),and microbial biomass nitrogen(MBN)in the top 30 cm soil layer were 1020.4,92.2,and 40.8 Tg,respectively,with corresponding mean densities of 164.6,14.9,and 6.6 g/m2.Climate variables-particularly mean annual temperature and aridity-along with human impacts emerged as the dominant drivers of soil N stock distribution.Notably,increased aridity and intensified human impacts exerted mutually counteracting effects on soil N fractions:aridity-driven moisture limitation generally suppressed N accumulation,whereas anthropogenic activities(e.g.,fertilization and grazing)promoted N enrichment.By identifying the key environmental and anthropogenic factors shaping the soil N distribution,this study improves the accuracy of regional and global N stock estimates.These insights provide a scientific foundation for developing more effective soil N management strategies in dryland ecosystems,contributing to sustainable land use and long-term ecosystem resilience in drylands.
