Sm_2 Fe_(17) prepared by reduction-diffusion method needs to be washed with water to remove calcium oxide. Electrochemical corrosion occurs when Sm_2 Fe_(17) powder is in contact with liquid water. Corrosion mechanism...Sm_2 Fe_(17) prepared by reduction-diffusion method needs to be washed with water to remove calcium oxide. Electrochemical corrosion occurs when Sm_2 Fe_(17) powder is in contact with liquid water. Corrosion mechanism of H_2 O on Sm_2 Fe_(17) powder and nitrogenation process of corroded Sm_2 Fe_(17) were studied by analyzing the structure and morphology. It is indicated that the metallic hydroxide forms and deposits on the Sm_2 Fe_(17) powder surfaces during water corrosion. At the same time, oxygen and hydrogen enter the unit cell of Sm2 Fe_(17), causing a slight increase in Curie temperature. In the subsequent nitriding process,the hydroxide is dehydrated and hydrogen is desorbed. The resulting oxide reacts with Sm_2 Fe_(17)N_x to form a-Fe and Sm_2 O_3. Thermodynamic calculations using the HSC Chemistry 6.0 software indicate that the reaction can occur spontaneously. The effect of water corrosion on the magnetic properties of the nitride can be eliminated by hydrogen reduction prior to nitriding.展开更多
Nitrogenation of SmFelolVIo2 powders was performed in a self-made furnace under a high-purity N2 atmo- sphere up to 40 MPa at 500 ℃. Upon nitrogenation at atmospheric pressure, the lattice parameters a and c increase...Nitrogenation of SmFelolVIo2 powders was performed in a self-made furnace under a high-purity N2 atmo- sphere up to 40 MPa at 500 ℃. Upon nitrogenation at atmospheric pressure, the lattice parameters a and c increase by 0.5% and 2.7%, respectively, whereas the Curie temperature Tc increases from 519 to 633 K. With further increasing the nitrogenation pressure to 20 and 40 MPa, the 1：12 main phase starts to decompose and a large amount of Mo and a-Fe precipitates. This leads to variation of Mo concentration in the 1：12 phase and causes a sharp decrease in Tc and in the coercivity. The relative complex permittivity and permeability of paraffin-SmFeloMO2 composites show multi-resonant behavior. After nitrogenation, the magnetic loss of the powders decreases, which may originate from the influence of eddy currents due to the increase in the particle size.展开更多
The reaction kinetics between nitrogen gas and Nd(Fe, Mo)_(12) intermetallic compound has been studied. The relationship between the reaction temperature, the reaction time with average mass fraction of N in samples h...The reaction kinetics between nitrogen gas and Nd(Fe, Mo)_(12) intermetallic compound has been studied. The relationship between the reaction temperature, the reaction time with average mass fraction of N in samples have been measured. The activation energy of first step reaction, E_f,(18.2 kJ/mol), is smaller than E_s (64.6 kJ /mol) of the second step during which nitrogen diffusion in the range 400～550℃ can be represented by an activated interstitial diffusion process. Heating above 550℃ leads to disproportion of the compound into NdN and α-Fe and the permanent properties will be damaged greatly.展开更多
An efficient KI catalyzed nitrogenation of aldehydes and alcohols for the direct synthesis of carbamoyl azides and ureas via a radical process has been developed. The simple operating procedures, the readily available...An efficient KI catalyzed nitrogenation of aldehydes and alcohols for the direct synthesis of carbamoyl azides and ureas via a radical process has been developed. The simple operating procedures, the readily available starting materials including aldehydes, alcohols and amines, as well as the utility of the products all make this strategy very attractive.展开更多
Amides are among the fundamental chemicals in organic chemistry.Compared to other carbonyl functional groups,the transformation of amide is relatively difficult and remains a challenge.The traditional deconstruction t...Amides are among the fundamental chemicals in organic chemistry.Compared to other carbonyl functional groups,the transformation of amide is relatively difficult and remains a challenge.The traditional deconstruction transformations of amides to other functional products are usually limited to twisted or electronically activated amides.Herein,we describe a direct nitrogenation approach to convert amides into nitriles.This chemistry provides a novel amide transformation pathway via both C–C and C–N bond cleavage.Interestingly,the simple,readily available,and inexpensive inorganic salt NaNO2 is successfully employed as a nitrogen source in this organic N-incorporation process.Applications of this study are demonstrated through the latestage modification of drug and natural product derivatives.展开更多
In order to address the evolving emission characteristics of oxygenated volatile organic compounds(OVOCs),it is essential to develop adsorbent materials specifically designed for the efficient adsorption of OVOCs with...In order to address the evolving emission characteristics of oxygenated volatile organic compounds(OVOCs),it is essential to develop adsorbent materials specifically designed for the efficient adsorption of OVOCs with large kinetic diameters.In this study,we used co-pyrolysis to prepare a series of graded porous carbon materials with well-developed micropores by adjusting the doping ratios of root nodules and pretreated cellulose.The material with root nodule to cellulose mass ratio of 1:1(TCC-RN-1)exhibited the highest saturated adsorption capacity for butyl acetate(834 mg/g).This can be attributed to enhanced pore size distribution from nodule doping,which facilitates the development of a micropore-graded structure.Additionally,the nodules acted as auxiliary activating agents that enhanced the KOH micropore regulation effect during the activation stage,resulting in the highest micropore volume(0.863 cm^(3)/g).The doping of root nodules facilitated the formation of additional defects on the surface of the porous carbon material,leading to a more disordered arrangement that improved pollutant adsorption.Furthermore,TCC-RN-1 demonstrated good thermal stability in an air atmosphere,main-taining a butyl acetate adsorption capacity exceeding 95%after five adsorption-desorption cycles.This indicates its favorable potential for industrial applications.展开更多
Osteoarthritis(OA),a debilitating joint disorder affecting millions worldwide,is characterized by persistent inflammation,oxidative stress,and irreversible cartilage breakdown,yet remains without diseasemodifying ther...Osteoarthritis(OA),a debilitating joint disorder affecting millions worldwide,is characterized by persistent inflammation,oxidative stress,and irreversible cartilage breakdown,yet remains without diseasemodifying therapies.Inspired by natural enzymatic cascades,we developed a bioinspired nanocomposite hydrogel,N,S-doped Mn-Nb(C-CeO),that mimics endogenous antioxidant pathways to reprogram the OA microenvironment.This system combines N,Sdoped Mn-Nb_(2)C MXene nanosheets with CeO_(2)nanozymes within a boronate ester-crosslinked hydrogel,forming an“immuno-redox circuitry”with four synergistic functions:(1)cascade reactive oxygen species(ROS)scavenging via superoxide dismutase-like Mn-Nb_(2)C and catalase-like CeO_(2),amplified by photothermal enhancement under near-infrared irradiation;(2)broad reactive nitrogen species clearance,removing peroxynitrite(ONOO^(-)),nitric oxide(NO),and nitroxyl(NO^(-))to mitigate inflammation;(3)immunomodulation through Mn^(2+)-activated cGAS-STING signaling,which promoted macrophage polarization toward the M2 phenotype,concomitantly reducing the levels of pro-inflammatory cytokines such as interleukin-1 beta(IL-1β)and tumor necrosis factor-alpha(TNF-α);(4)cartilage regeneration via pH/ROS-responsive simvastatin(SIM)release and nanocatalysis,upregulating SRY-box transcription factor 9(SOX9)and Col2a1 while inhibiting matrix metalloproteinase-13(MMP-13)and a disintegrin and metalloproteinase with thrombospondin motifs 5(ADAMTS5).In a murine OA model,the system reduced synovitis by 60%,restored 80% of cartilage thickness,and suppressed osteophyte formation,outperforming singlecomponent treatments.This strategy pioneers a“self-healing cartilage”approach by integrating nanocatalysis with immunoengineering for transformative OA therapy.展开更多
Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few importa...Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few important groups of organics including organic nitrogen(ON),organonitrates(OrgN),organosulfates(OS)and polycyclic aromatic hydrocarbons(PAHs),via online measurement of submicron aerosols(PM_(1))in Nanjing,China,during 2022 summer.The average PM_(1) concentration was 15.39μg/m^(3),dominated by secondary components(69.1%),which were even more important at higher PM_(1) levels.The primary organic aerosols(POA)were from traffic,industry and cooking;the two secondary OA factors were both closely linked with photochemistry,with one(OOA1)being relatively fresh and important in early afternoon and another(OOA2)being aged and important in late afternoon.Sulfate formation was also governed by photochemistry but resembled that of OOA2 not OOA1;nitrate formation was associated strongly with heterogeneous hydrolysis and thermodynamic equilibrium.Results also reveal a possible photochemical reaction channel from POA to OOA1,then to OOA2.Case studies show that formations of secondary components responded differently to different weather conditions and governed summer PM_(1) pollution.The average ON,OrgN,OS and PAHs concentrations were determined to be 122.8,84.4,45.6 and 3.3 ng/m^(3),respectively.ON was dominated by primary sources(53.8%).OrgN varied similarly to nitrate.OS formation was linked with aqueous-phase reactions,which were insignificant therefore its level was low.PAHs was mainly from traffic,and photochemical oxidation might be its important sink during afternoon.展开更多
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
MXene derivatives are notable two-dimensional nanomaterials with numerous prospective applications in the domains of energy development.MXene derivative,MBene,diversifies its focus on energy storage and harvesting due...MXene derivatives are notable two-dimensional nanomaterials with numerous prospective applications in the domains of energy development.MXene derivative,MBene,diversifies its focus on energy storage and harvesting due to its exceptional electrical conductivity,structural flexibility,and mechanical properties.This comprehensive review describes the sandwich-like structure of the synthesized MBene,derived from its multilayered parent material and its distinct chemical framework to date.The fields of focus encompass the investigation of novel MBenes,the study of phase-changing mechanisms,and the examination of hex-MBenes,ortho-MBenes,tetra-MBenes,tri-MBenes,and MXenes with identical transition metal components.A critical analysis is also provided on the electrochemical mechanism and performance of MBene in energy storage(Li/Na/Mg/Ca/Li–S batteries and supercapacitors),as well as conversion and harvesting(CO_(2) reduction,and nitrogen reduction reactions).The persistent difficulties associated with conducting experimental synthesis and establishing artificial intelligence-based forecasts are extensively deliberated alongside the potential and forthcoming prospects of MBenes.This review provides a single platform for an overview of the MBene’s potential in energy storage and harvesting.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
In this work,ofloxacin(OFL),a kind of frequently detected antibiotic in groundwater,was selected to explore its impact(at ng/L-μg/L-level)on denitrification performance in an autotrophic denitrification system driven...In this work,ofloxacin(OFL),a kind of frequently detected antibiotic in groundwater,was selected to explore its impact(at ng/L-μg/L-level)on denitrification performance in an autotrophic denitrification system driven by pyrite/sulfur(FeS2/S0).Results showed that OFL restrained nitrate removal efficiency,and the inhibition degree was positively related to the concentration of OFL.After being exposed to increased OFL(200 ng/L-100μg/L)for 69 days,higher inhibition of electron transport activity(ETSA),enzyme activities of nitrate reductase(NAR),and nitrite reductase(NIR)were acquired.Meanwhile,the extracellular protein(PN)content of sludge samples was remarkably stimulated by OFL to resist the augmented toxicity.OFL contributed to increased microbial diversity and sulfur/sulfide oxidation functional genes in ng/L-level bioreactors,whereas led to a decline inμg/L level experiments.With OFL at concentrations of 200 ng/L and 100μg/L,the whole expression of 10 key denitrification functional genes was depressed,and the higher the OFL concentration,the lower the expression level.However,no significant proliferation of antibiotic resistance genes(ARGs)either in 200 ng/L-OFL or 100μg/L-OFL groups was observed.Two-factor correlation analysis results indicated that Thiobacillus,Anaerolineae,Anaerolineales,and Nitrospirae might be the main hosts of existing ARGs in this system.展开更多
A comprehensive insight into the evolution and molecular structure of basic and neutral nitrogen compounds during the residue hydrotreating(RHT)process was gained through ESI(+)/ESI(-)FT-ICR MS analysis of the feedsto...A comprehensive insight into the evolution and molecular structure of basic and neutral nitrogen compounds during the residue hydrotreating(RHT)process was gained through ESI(+)/ESI(-)FT-ICR MS analysis of the feedstock and its hydrogenated samples,with hydrodenitrogenation(HDN)ratios of 15.9%-70.1%.This study revealed that carbazoles,characterized by a double bond equivalent(DBE)of 9-11,were the refractory neutral nitrogen compounds during the RHT process.Their recalcitrant nature was primarily due to their low aromaticity and high steric hindrance.Conversely,quinolines(DBEs 7 to 9)were the most abundant basic nitrogen compounds.Through a meticulous analysis of DBE evolution,we revealed the intricate reaction mechanisms of benzocarbazoles and dibenzocarbazoles in residual oil,highlighting the crucial role of quinolines as key intermediates in eliminating these compounds.Interestingly,nitrogen compounds with either low or high carbon numbers(for a given DBE)exhibited higher reactivity than those with medium carbon numbers,which can be attributed to the low steric hindrance resulting from short alkyl chains and more naphthenic-aromatic structures,respectively.After hydrotreatment,the molecular structures of the most refractory or abundant nitrogen compounds could consist of two main types:those with multiple naphthenic-aromatic rings and those with long side chains near the nitrogen atom.This research has revealed nitrogen compounds'evolutionary mechanisms and refractory nature,and the molecular structure of the most resistant or abundant basic and neutral nitrogen compounds,providing a deeper understanding of the HDN process and ultimately paving the way for the rational RHT catalyst design and process development.展开更多
Nitric oxide(NO)is a gaseous molecule produced by 3 different NO synthase(NOS)isoforms:Neural/brain NOS(nNOS/bNOS,type 1),endothelial NOS(eNOS,type 3)and inducible NOS(type 2).Type 1 and 3 NOS are constitutively expre...Nitric oxide(NO)is a gaseous molecule produced by 3 different NO synthase(NOS)isoforms:Neural/brain NOS(nNOS/bNOS,type 1),endothelial NOS(eNOS,type 3)and inducible NOS(type 2).Type 1 and 3 NOS are constitutively expressed.NO can serve different purposes:As a vasoactive molecule,as a neurotransmitter or as an immunomodulator.It plays a key role in cerebral ischemia/reperfusion injury(CIRI).Hypoxic episodes simulate the production of oxygen free radicals,leading to mitochondrial and phospholipid damage.Upon reperfusion,increased levels of oxygen trigger oxide synthases;whose products are associated with neuronal damage by promoting lipid peroxidation,nitrosylation and excitotoxicity.Molecular pathways in CIRI can be altered by NOS.Neuroprotective effects are observed with eNOS activity.While nNOS interplay is prone to endothelial inflammation,oxidative stress and apoptosis.Therefore,nNOS appears to be detrimental.The interaction between NO and other free radicals develops peroxynitrite;which is a cytotoxic agent.It plays a main role in the likelihood of hemorrhagic events by tissue plasminogen activator(t-PA).Peroxynitrite scavengers are currently being studied as potential targets to prevent hemorrhagic transformation in CIRI.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 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
Nitrogen removal from domestic sewage is usually limited by insufficient carbon source and electron donor.An economical solid carbon source was developed by composition of polyvinyl alcohol,sodium alginate,and corncob...Nitrogen removal from domestic sewage is usually limited by insufficient carbon source and electron donor.An economical solid carbon source was developed by composition of polyvinyl alcohol,sodium alginate,and corncob,which was utilized as external carbon source in the anaerobic anoxic oxic(AAO)-biofilter for the treatment of low carbon-to-nitrogen ratio domestic sewage,and the nitrogen removal was remarkably improved from 63.2%to 96.5%.Furthermore,the effluent chemical oxygen demand maintained at 35 mg/L or even lower,and the total nitrogenwas reduced to less than 2mg/L.Metagenomic analysis demonstrated that the microbial communities responsible for potential denitrification and organic matter degradation in both AAO and the biofilter reactors were mainly composed of Proteobacteria and Bacteroides,respectively.The solid carbon source addition resulted in relatively high abundance of functional enzymes responsible for NO_(3)^(−)-N to NO_(2)^(−)-N con-version in both AAO and the biofilter reactors,thus enabled stable reaction.The carbon source addition during glycolysis primarily led to the increase of genes associated with the metabolic conversion of fructose 1.6P2 to glycerol-3P The reactor maintained high abun-dance of genes related to the tricarboxylic acid cycle,and then guaranteed efficient carbon metabolism.The results indicate that the composite carbon source is feasible for denitri-fication enhancement of AAO-biofilter,which contribute to the theoretical foundation for practical nitrogen removal application.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
基金Project supported by Natural Science Foundation of Ningbo,China(2017A610079)Technology Innovation&Achievement Industrialization Project of Ningbo China(2014B11010)
文摘Sm_2 Fe_(17) prepared by reduction-diffusion method needs to be washed with water to remove calcium oxide. Electrochemical corrosion occurs when Sm_2 Fe_(17) powder is in contact with liquid water. Corrosion mechanism of H_2 O on Sm_2 Fe_(17) powder and nitrogenation process of corroded Sm_2 Fe_(17) were studied by analyzing the structure and morphology. It is indicated that the metallic hydroxide forms and deposits on the Sm_2 Fe_(17) powder surfaces during water corrosion. At the same time, oxygen and hydrogen enter the unit cell of Sm2 Fe_(17), causing a slight increase in Curie temperature. In the subsequent nitriding process,the hydroxide is dehydrated and hydrogen is desorbed. The resulting oxide reacts with Sm_2 Fe_(17)N_x to form a-Fe and Sm_2 O_3. Thermodynamic calculations using the HSC Chemistry 6.0 software indicate that the reaction can occur spontaneously. The effect of water corrosion on the magnetic properties of the nitride can be eliminated by hydrogen reduction prior to nitriding.
基金financially supported by the National Natural Science Foundation of China (No. 51261001)Liaoning Provincial Natural Science Foundation (No. 2013020105)Shenyang Science and Technology Foundation (No. F13-316-139)
文摘Nitrogenation of SmFelolVIo2 powders was performed in a self-made furnace under a high-purity N2 atmo- sphere up to 40 MPa at 500 ℃. Upon nitrogenation at atmospheric pressure, the lattice parameters a and c increase by 0.5% and 2.7%, respectively, whereas the Curie temperature Tc increases from 519 to 633 K. With further increasing the nitrogenation pressure to 20 and 40 MPa, the 1：12 main phase starts to decompose and a large amount of Mo and a-Fe precipitates. This leads to variation of Mo concentration in the 1：12 phase and causes a sharp decrease in Tc and in the coercivity. The relative complex permittivity and permeability of paraffin-SmFeloMO2 composites show multi-resonant behavior. After nitrogenation, the magnetic loss of the powders decreases, which may originate from the influence of eddy currents due to the increase in the particle size.
文摘The reaction kinetics between nitrogen gas and Nd(Fe, Mo)_(12) intermetallic compound has been studied. The relationship between the reaction temperature, the reaction time with average mass fraction of N in samples have been measured. The activation energy of first step reaction, E_f,(18.2 kJ/mol), is smaller than E_s (64.6 kJ /mol) of the second step during which nitrogen diffusion in the range 400～550℃ can be represented by an activated interstitial diffusion process. Heating above 550℃ leads to disproportion of the compound into NdN and α-Fe and the permanent properties will be damaged greatly.
基金Financial support from National Basic Research Program of China （973 Program） （No. 2015CB856600）, the National Natural Science Foundation of China （Nos. 21325206, 21632001）, National Young Top-notch Talent Support Program, CAS Interdisciplinary Innovation Team, and Peking University Health Science Center （Nos. BMU20150505, BMU20160541） is greatly ap- preciated. We thank Bencong Zhu and Ao Sun in this group for reproducing the results of 2a and 2k.
文摘An efficient KI catalyzed nitrogenation of aldehydes and alcohols for the direct synthesis of carbamoyl azides and ureas via a radical process has been developed. The simple operating procedures, the readily available starting materials including aldehydes, alcohols and amines, as well as the utility of the products all make this strategy very attractive.
基金the National Key R&D Program of China(grant no.2021YFA1501700)the NSFC(grant nos.22131002,22161142019,81821004),and the Tencent Foundation for financial support.
文摘Amides are among the fundamental chemicals in organic chemistry.Compared to other carbonyl functional groups,the transformation of amide is relatively difficult and remains a challenge.The traditional deconstruction transformations of amides to other functional products are usually limited to twisted or electronically activated amides.Herein,we describe a direct nitrogenation approach to convert amides into nitriles.This chemistry provides a novel amide transformation pathway via both C–C and C–N bond cleavage.Interestingly,the simple,readily available,and inexpensive inorganic salt NaNO2 is successfully employed as a nitrogen source in this organic N-incorporation process.Applications of this study are demonstrated through the latestage modification of drug and natural product derivatives.
基金supported by the National Natural Science Foundation of China(No.52370112).
文摘In order to address the evolving emission characteristics of oxygenated volatile organic compounds(OVOCs),it is essential to develop adsorbent materials specifically designed for the efficient adsorption of OVOCs with large kinetic diameters.In this study,we used co-pyrolysis to prepare a series of graded porous carbon materials with well-developed micropores by adjusting the doping ratios of root nodules and pretreated cellulose.The material with root nodule to cellulose mass ratio of 1:1(TCC-RN-1)exhibited the highest saturated adsorption capacity for butyl acetate(834 mg/g).This can be attributed to enhanced pore size distribution from nodule doping,which facilitates the development of a micropore-graded structure.Additionally,the nodules acted as auxiliary activating agents that enhanced the KOH micropore regulation effect during the activation stage,resulting in the highest micropore volume(0.863 cm^(3)/g).The doping of root nodules facilitated the formation of additional defects on the surface of the porous carbon material,leading to a more disordered arrangement that improved pollutant adsorption.Furthermore,TCC-RN-1 demonstrated good thermal stability in an air atmosphere,main-taining a butyl acetate adsorption capacity exceeding 95%after five adsorption-desorption cycles.This indicates its favorable potential for industrial applications.
基金supported by the National Natural Science Foundation of China(Nos.82101647 and 82203446)Natural Science Fund of Zhejiang Province(Nos.LY24H250001,LQN25H060003,and LY23H060011)+2 种基金the Postdoctoral Fellowship Program of CPSF(No.188020-170257701/136)the Regional Innovation and Development Joint Fund of the National Natural Science Foundation of China(No.U22A20282)the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515220225).
文摘Osteoarthritis(OA),a debilitating joint disorder affecting millions worldwide,is characterized by persistent inflammation,oxidative stress,and irreversible cartilage breakdown,yet remains without diseasemodifying therapies.Inspired by natural enzymatic cascades,we developed a bioinspired nanocomposite hydrogel,N,S-doped Mn-Nb(C-CeO),that mimics endogenous antioxidant pathways to reprogram the OA microenvironment.This system combines N,Sdoped Mn-Nb_(2)C MXene nanosheets with CeO_(2)nanozymes within a boronate ester-crosslinked hydrogel,forming an“immuno-redox circuitry”with four synergistic functions:(1)cascade reactive oxygen species(ROS)scavenging via superoxide dismutase-like Mn-Nb_(2)C and catalase-like CeO_(2),amplified by photothermal enhancement under near-infrared irradiation;(2)broad reactive nitrogen species clearance,removing peroxynitrite(ONOO^(-)),nitric oxide(NO),and nitroxyl(NO^(-))to mitigate inflammation;(3)immunomodulation through Mn^(2+)-activated cGAS-STING signaling,which promoted macrophage polarization toward the M2 phenotype,concomitantly reducing the levels of pro-inflammatory cytokines such as interleukin-1 beta(IL-1β)and tumor necrosis factor-alpha(TNF-α);(4)cartilage regeneration via pH/ROS-responsive simvastatin(SIM)release and nanocatalysis,upregulating SRY-box transcription factor 9(SOX9)and Col2a1 while inhibiting matrix metalloproteinase-13(MMP-13)and a disintegrin and metalloproteinase with thrombospondin motifs 5(ADAMTS5).In a murine OA model,the system reduced synovitis by 60%,restored 80% of cartilage thickness,and suppressed osteophyte formation,outperforming singlecomponent treatments.This strategy pioneers a“self-healing cartilage”approach by integrating nanocatalysis with immunoengineering for transformative OA therapy.
基金supported by the National Natural Science Foundation of China(Nos.22361162668 and 42021004)the National Key Research and Development Program of China(No.2023YFC3706203).
文摘Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few important groups of organics including organic nitrogen(ON),organonitrates(OrgN),organosulfates(OS)and polycyclic aromatic hydrocarbons(PAHs),via online measurement of submicron aerosols(PM_(1))in Nanjing,China,during 2022 summer.The average PM_(1) concentration was 15.39μg/m^(3),dominated by secondary components(69.1%),which were even more important at higher PM_(1) levels.The primary organic aerosols(POA)were from traffic,industry and cooking;the two secondary OA factors were both closely linked with photochemistry,with one(OOA1)being relatively fresh and important in early afternoon and another(OOA2)being aged and important in late afternoon.Sulfate formation was also governed by photochemistry but resembled that of OOA2 not OOA1;nitrate formation was associated strongly with heterogeneous hydrolysis and thermodynamic equilibrium.Results also reveal a possible photochemical reaction channel from POA to OOA1,then to OOA2.Case studies show that formations of secondary components responded differently to different weather conditions and governed summer PM_(1) pollution.The average ON,OrgN,OS and PAHs concentrations were determined to be 122.8,84.4,45.6 and 3.3 ng/m^(3),respectively.ON was dominated by primary sources(53.8%).OrgN varied similarly to nitrate.OS formation was linked with aqueous-phase reactions,which were insignificant therefore its level was low.PAHs was mainly from traffic,and photochemical oxidation might be its important sink during afternoon.
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.
基金supported by the National Natural Science Foundation of China(No.52302241 and 22225801)the Major Science and Technology Programs of Henan Province(241100240200)the China Postdoctoral Science Foundation(No.2023M730940).
文摘MXene derivatives are notable two-dimensional nanomaterials with numerous prospective applications in the domains of energy development.MXene derivative,MBene,diversifies its focus on energy storage and harvesting due to its exceptional electrical conductivity,structural flexibility,and mechanical properties.This comprehensive review describes the sandwich-like structure of the synthesized MBene,derived from its multilayered parent material and its distinct chemical framework to date.The fields of focus encompass the investigation of novel MBenes,the study of phase-changing mechanisms,and the examination of hex-MBenes,ortho-MBenes,tetra-MBenes,tri-MBenes,and MXenes with identical transition metal components.A critical analysis is also provided on the electrochemical mechanism and performance of MBene in energy storage(Li/Na/Mg/Ca/Li–S batteries and supercapacitors),as well as conversion and harvesting(CO_(2) reduction,and nitrogen reduction reactions).The persistent difficulties associated with conducting experimental synthesis and establishing artificial intelligence-based forecasts are extensively deliberated alongside the potential and forthcoming prospects of MBenes.This review provides a single platform for an overview of the MBene’s potential in energy storage and harvesting.
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 Natural Science Foundation of China(No.42377083)the Natural Science Foundation of Sichuan Province,China(No.2025 ZNSFSC0433).
文摘In this work,ofloxacin(OFL),a kind of frequently detected antibiotic in groundwater,was selected to explore its impact(at ng/L-μg/L-level)on denitrification performance in an autotrophic denitrification system driven by pyrite/sulfur(FeS2/S0).Results showed that OFL restrained nitrate removal efficiency,and the inhibition degree was positively related to the concentration of OFL.After being exposed to increased OFL(200 ng/L-100μg/L)for 69 days,higher inhibition of electron transport activity(ETSA),enzyme activities of nitrate reductase(NAR),and nitrite reductase(NIR)were acquired.Meanwhile,the extracellular protein(PN)content of sludge samples was remarkably stimulated by OFL to resist the augmented toxicity.OFL contributed to increased microbial diversity and sulfur/sulfide oxidation functional genes in ng/L-level bioreactors,whereas led to a decline inμg/L level experiments.With OFL at concentrations of 200 ng/L and 100μg/L,the whole expression of 10 key denitrification functional genes was depressed,and the higher the OFL concentration,the lower the expression level.However,no significant proliferation of antibiotic resistance genes(ARGs)either in 200 ng/L-OFL or 100μg/L-OFL groups was observed.Two-factor correlation analysis results indicated that Thiobacillus,Anaerolineae,Anaerolineales,and Nitrospirae might be the main hosts of existing ARGs in this system.
基金the financial support from the National Key Research and Development Program of China(2021YFA1501204)the project of SINOPEC RIPP Co.Ltd(PR20230230)。
文摘A comprehensive insight into the evolution and molecular structure of basic and neutral nitrogen compounds during the residue hydrotreating(RHT)process was gained through ESI(+)/ESI(-)FT-ICR MS analysis of the feedstock and its hydrogenated samples,with hydrodenitrogenation(HDN)ratios of 15.9%-70.1%.This study revealed that carbazoles,characterized by a double bond equivalent(DBE)of 9-11,were the refractory neutral nitrogen compounds during the RHT process.Their recalcitrant nature was primarily due to their low aromaticity and high steric hindrance.Conversely,quinolines(DBEs 7 to 9)were the most abundant basic nitrogen compounds.Through a meticulous analysis of DBE evolution,we revealed the intricate reaction mechanisms of benzocarbazoles and dibenzocarbazoles in residual oil,highlighting the crucial role of quinolines as key intermediates in eliminating these compounds.Interestingly,nitrogen compounds with either low or high carbon numbers(for a given DBE)exhibited higher reactivity than those with medium carbon numbers,which can be attributed to the low steric hindrance resulting from short alkyl chains and more naphthenic-aromatic structures,respectively.After hydrotreatment,the molecular structures of the most refractory or abundant nitrogen compounds could consist of two main types:those with multiple naphthenic-aromatic rings and those with long side chains near the nitrogen atom.This research has revealed nitrogen compounds'evolutionary mechanisms and refractory nature,and the molecular structure of the most resistant or abundant basic and neutral nitrogen compounds,providing a deeper understanding of the HDN process and ultimately paving the way for the rational RHT catalyst design and process development.
文摘Nitric oxide(NO)is a gaseous molecule produced by 3 different NO synthase(NOS)isoforms:Neural/brain NOS(nNOS/bNOS,type 1),endothelial NOS(eNOS,type 3)and inducible NOS(type 2).Type 1 and 3 NOS are constitutively expressed.NO can serve different purposes:As a vasoactive molecule,as a neurotransmitter or as an immunomodulator.It plays a key role in cerebral ischemia/reperfusion injury(CIRI).Hypoxic episodes simulate the production of oxygen free radicals,leading to mitochondrial and phospholipid damage.Upon reperfusion,increased levels of oxygen trigger oxide synthases;whose products are associated with neuronal damage by promoting lipid peroxidation,nitrosylation and excitotoxicity.Molecular pathways in CIRI can be altered by NOS.Neuroprotective effects are observed with eNOS activity.While nNOS interplay is prone to endothelial inflammation,oxidative stress and apoptosis.Therefore,nNOS appears to be detrimental.The interaction between NO and other free radicals develops peroxynitrite;which is a cytotoxic agent.It plays a main role in the likelihood of hemorrhagic events by tissue plasminogen activator(t-PA).Peroxynitrite scavengers are currently being studied as potential targets to prevent hemorrhagic transformation in CIRI.
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 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.
基金supported by the Special Funds for Chengde national innovation demonstration area construction of science and technology special project sustainable development agenda(No.202104F001)the National Basic Research Program of China(No.2019YFC0408602).
文摘Nitrogen removal from domestic sewage is usually limited by insufficient carbon source and electron donor.An economical solid carbon source was developed by composition of polyvinyl alcohol,sodium alginate,and corncob,which was utilized as external carbon source in the anaerobic anoxic oxic(AAO)-biofilter for the treatment of low carbon-to-nitrogen ratio domestic sewage,and the nitrogen removal was remarkably improved from 63.2%to 96.5%.Furthermore,the effluent chemical oxygen demand maintained at 35 mg/L or even lower,and the total nitrogenwas reduced to less than 2mg/L.Metagenomic analysis demonstrated that the microbial communities responsible for potential denitrification and organic matter degradation in both AAO and the biofilter reactors were mainly composed of Proteobacteria and Bacteroides,respectively.The solid carbon source addition resulted in relatively high abundance of functional enzymes responsible for NO_(3)^(−)-N to NO_(2)^(−)-N con-version in both AAO and the biofilter reactors,thus enabled stable reaction.The carbon source addition during glycolysis primarily led to the increase of genes associated with the metabolic conversion of fructose 1.6P2 to glycerol-3P The reactor maintained high abun-dance of genes related to the tricarboxylic acid cycle,and then guaranteed efficient carbon metabolism.The results indicate that the composite carbon source is feasible for denitri-fication enhancement of AAO-biofilter,which contribute to the theoretical foundation for practical nitrogen removal application.
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.
