Nitrogen oxides(NO_(x))are crucial in tropospheric photochemical ozone(O_(3))production and oxidation capacity.Currently,the widely used NO_(x)measurement technique is chemiluminescence(CL)(CL-NO_(x)),which tends to o...Nitrogen oxides(NO_(x))are crucial in tropospheric photochemical ozone(O_(3))production and oxidation capacity.Currently,the widely used NO_(x)measurement technique is chemiluminescence(CL)(CL-NO_(x)),which tends to overestimate NO_(2)due to atmospheric oxidation products of NO_(x)(i.e.,NO_(z)).We developed and characterized a NO_(x)measurement system using the cavity attenuated phase shift(CAPS)technique(CAPS-NO_(x)),which is free from interferences with nitrogen-containing species.The NO_(x)measured by the CAPS-NO_(x)and CL-NO_(x)analyzers were compared.Results show that both analyzers showed consistent measurement results for NO,but the NO_(2)measured by the CAPS-NO_(x)analyzer(NO_(2)_CAPS)was mostly lower than that measured by the CL-NO_(x)analyzer(NO_(2)_CL),which led to the deviations in O_(3)formation sensitivity regime and O_(x)(=O_(3)+NO_(2))sources(i.e.,regional background and photochemically produced O_(x))determined by the ozone production efficiencies(OPE)calculated from NO_(2)_CL and NO_(2)_CAPS.Overall,OPE_CL exceeded OPE_CAPS by 18.9%,which shifted 3 out of 13 observation days from the VOCs-limited to the transition regime when judging using OPE_CL,as compared to calculations using OPE_CAPS.During the observation period,days dominated by regional background O_(x)accounted for 46%and 62%when determined using NO_(2)_CL and NO_(2)_CAPS,respectively.These findings suggest that the use of the CL-NO_(x)analyzer tends to underestimate both the VOCs-limited regime and the regional background O_(x)dominated days.The newly built CAPS-NO_(x)analyzer here can promote the accurate measurement of NO_(2),which is meaningful for diagnosing O_(3)formation regimes and O_(x)sources.展开更多
The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocata...The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocatalysts.However,the low solubility and limited diffusion of N_(2)significantly hinder the achievement of satisfactory performance.In this context,we report an effective strategy to enhance NRR activity by introducing a metal-organic framework(MOF)membrane,specifically MIL-53(Al),onto a perovskite oxide(LiNbO_(3)),denoted as LN@MIL-X(X=0.2,0.4 and 0.6).The MIL-53(Al)membrane selectively recognizes and concentrates N_(2)at the catalyst interface while simultaneously repelling water molecules,thereby inhibiting the hydrogen evolution reaction(HER).This ultrathin nanostructure significantly improves the NRR performance of LN@MIL-X compared to pristine LiNbO_(3).Notably,LN@MIL-0.4 exhibits a maximum NH_(3)yield of 45.25 mg h^(-1)mg_(cat.)^(-1)with an impressive Faradaic efficiency(FE)of 86.41%at-0.45 V versus RHE in 0.1 mol L^(-1)Na_(2)SO_(4).This work provides a universal strategy for the design and synthesis of perovskite oxide electrocatalysts,facilitating high-efficiency ammonia synthesis.展开更多
Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and re...Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.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
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 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
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
Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great potential.We demonstrate the targeted synthesis and cation modulation of NiCo_(2)O_(4)spinel nanoboxes,sy...Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great potential.We demonstrate the targeted synthesis and cation modulation of NiCo_(2)O_(4)spinel nanoboxes,synthesized via cation exchange and calcination oxidation.These catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds,specifically 2-phenoxy-1-phenylethanol,into nitrogen-containing aromatics,achieving high conversion rates and selectivities.These catalysts were synthesized via a cation exchange and calcination oxidation process,using Prussian blue nanocubes as precursors.The porous architecture and polymetallic composition of the NiCo_(2)O_(4)spinel demonstrated superior performance in electrocatalytic oxidative coupling,achieving a 99.2 wt%conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt%for quinoline derivatives and 31.5 wt%for phenol.Key innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives,the elucidation of a multistage reaction pathway involving CAO bond cleavage,hydroxyaldol condensation,and CAN bond formation,and a deeper mechanistic understanding derived from DFT simulations.This work establishes a new strategy for lignin valorization,offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions,without the need for additional reagents.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 objectives of this study which included two experiments were to investigate the effects of dietary inclusion of sorghum grain rich in condensed tannins(CT)(18.9 g kg^(–1)dry matter(DM))on nitrogen(N)metabolism an...The objectives of this study which included two experiments were to investigate the effects of dietary inclusion of sorghum grain rich in condensed tannins(CT)(18.9 g kg^(–1)dry matter(DM))on nitrogen(N)metabolism and urine nitrous oxide(N_(2)O)emissions of beef steers.In experiment 1,six Limousin×Luxi crossbreed steers with an initial liveweight of(245.0±18.7)kg were used as experimental animals.Three levels of sorghum grain,i.e.,0,167 and 338 g kg^(–1)DM were included in diets as experimental treatments.The animals and the treatments were randomly assigned to a replicated 3×3 Latin square design.In experiment 2,static incubation technique was used to determine the N_(2)O emissions of the urine samples collected in experiment 1.The results of experiment 1 showed that dietary inclusion of sorghum grain linearly increased the faecal N excretion(P=0.001),the total N excretion(P=0.010)and the faecal N to N intake ratio(P=0.021),but it did not affect the N retention and the N utilization efficiency(P>0.10).The plasma metabolomic data showed that dietary inclusion of sorghum grain increased the relative concentrations of phenolic acid(N1,N5,N10-tris-trans-p-coumaroylspermine and prenyl cis-caffeate)and carnitine(3-hydroxyisovalerylcarnitine and linoelaidyl carnitine).The results also showed that dietary inclusion of sorghum grain linearly increased the urinary urea excretion(P=0.010)and decreased the urinary excretion of purine derivatives(P=0.041)as well as the estimated rumen microbial N supply(P=0.012)based on urinary purine derivatives.The results of experiment 2 showed that including sorghum grain in the diet linearly increased the average concentrations of NH_(4)^(+)-N(P=0.012),NO_(2)^(–)-N(P=0.009),NO_(3)^(-)-N(P=0.001)and the total inorganic N(P<0.001)in the soil enriched with urine samples.The urine sample N_(2)O-N flux(P=0.001),the estimated steer urine N_(2)O-N flux(P=0.021)and the N_(2)O-N to urinary N ratio(P=0.038)linearly increased with increasing inclusion of sorghum grain in the diet.In conclusion,dietary inclusion of sorghum grain containing high CT at 167 and 338 g kg^(–1)DM did not affect the N utilization efficiency of steers but increased the urine N_(2)O-N emissions by 5.7 and 31.4%,respectively.For reducing the N_(2)O emissions to the environment,high levels of sorghum grain should not be included in the diet of steers.展开更多
Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-...Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-doping methods(one-step and two-step method),dried sludge(DS)/urea mass ratios(5:1,4:1,3:1,2:1,and 1:1),SC preparation procedures(pyrolysis only,pyrolysis with acid washing,and pyrolysis with KOH activation and acid washing),and different pyrolysis temperatures(500,600,700,and 800°C)on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation.The results indicated that N-doping could obviously promote the catalytic performance of SC.The one-step method with simultaneous sludge pyrolysis(at 700°C),KOH activation,and N-doping(DS/urea of 3:1)was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%,whereas the optimal NO conversion rate of SC without N-doping was only 47.3%.Urea worked both as carbon and nitrogen source,which could increase about 2.9%-16.5%of carbon and 24.8%-42.7%of nitrogen content in SC pyrolyzed at 700°C.N-doping significantly promoted microporosity of SC.The optimal N-doped SC showed specific surface areas of 571.38 m^(2)/g,much higher than 374.34 m^(2)/g of the optimal SC without N-doping.In addition,N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups.Finally,three reaction paths,i.e.microporous reactor,active sites,and basic site control path,were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.展开更多
The metal ion batteries have gained widespread attention for wearable electronics due to their competitive energy density and long cycling life.Exploring the advanced anode materials is significant for next generation...The metal ion batteries have gained widespread attention for wearable electronics due to their competitive energy density and long cycling life.Exploring the advanced anode materials is significant for next generation energy storage systems.However,severe electrode volume changes and sluggish redox kinetics are the critical problems for lithium/potassium ion batteries(LIBs/PIBs)towards large-scale applications.Herein,we prepare a novel anode material,which consists of reduced graphene oxide wrapping one-dimensional(1D)N-doped porous carbon nanotube with cobalt phosphoselenide(CoPSe)nanoparticles embedded inside them(r GO@Co PSe/NC).Benefited from the dual carbon decorations and ultrafine nanoparticles structure,it achieves a reversible capacity of 245 mAh/g at 5 A/g after 2000 cycles for LIBs and 215 mAh/g at 1 A/g after 500 cycles for PIBs.The pseudocapacitance and GITT measurements are used to investigate the electrochemical kinetics of r GO@Co PSe/NC for LIBs.In addition,the lithium ion full cell also shows good electrochemical performance when paired with high capacity LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode.This work provides a feasible electrode design strategy for high-efficiency metal ion batteries based on multidimensional nanoarchitecture engineering and composition tailoring.展开更多
The role of brassinosteroids(BRs)in enabling plants to respond effectively to adverse conditions is well known,though the precise mechanism of action that helps plants cope with arsenic(As)toxicity is still difficult ...The role of brassinosteroids(BRs)in enabling plants to respond effectively to adverse conditions is well known,though the precise mechanism of action that helps plants cope with arsenic(As)toxicity is still difficult to interpret.Therefore we tested the effect of brassinolide(BL)spray(0,0.5,and 1 mg·L^(-1))on As(0,and 10 mg·L^(-1))stressed tomato defense responses As stress led to the induction of oxidative stress,impaired chlorophyll and nitrogen metabolism,and Fe uptake,in conjunction with a reduction in plant growth and biomass.BL spray,on the contrary,protected the photo synthetic system and helped plants grow better under As stress.This was achieved by controlling the metabolism of chlorophyll and proline and lowering the amounts of methylglyoxal and H_(2)O_(2) through glyoxalaseⅠandⅡand antioxidant enzyme s.BL decreased arsenic accumulation by directing As sequestration towards vacuoles and increased Fe amount in the leaves and roots by regulating the expression of As(Lsil and Lsi2)and Fe(IRT1,IRT2,NRAMP1,and NRAMP3)transporters in As-stressed tomatoes.Furthermore,BL boosted adaptability against As phytotoxicity,while reducing the damaging impacts on photosynthesis,nitrogen metabolism,sulfur asimilation,and Fe absorption.These results offer a solid framework for the development of exogenous BRs-based breeding strategies for safer agricultural development.展开更多
The inhibitory effects of zinc oxide nanoparticles(ZnO NPs)and impacts of N-acylhomoserine lactone(AHL)-based quorum sensing(QS)on biological nitrogen removal(BNR)performance have beenwell-investigated.However,the eff...The inhibitory effects of zinc oxide nanoparticles(ZnO NPs)and impacts of N-acylhomoserine lactone(AHL)-based quorum sensing(QS)on biological nitrogen removal(BNR)performance have beenwell-investigated.However,the effects of ammonia nitrogen(NH_(4)^(+)-N)concentrations on NP toxicity and AHL regulation have seldom been addressed yet.This study consulted on the impacts of ZnO NPs on BNR systems when high NH_(4)^(+)-N concentrationwas available.The synergistic toxic effects of high-strength NH_(4)^(+)-N(200 mg/L)and ZnO NPs resulted in decreased ammonia oxidation rates and dropped the nitrogen removal efficiencies by 17.5%±0.2%.The increased extracellular polymeric substances(EPS)production was observed in response to the high NH_(4)^(+)-N and ZnO NP stress,which indicated the defensemechanism against the toxic effects in the BNR systemswas stimulated.Furthermore,the regulatory effects of exogenous N-decanoyl-homoserine lactone(C_(10)-HSL)-mediated QS system on NP-stressed BNR systems were revealed to improve the BNR performance under different NH_(4)^(+)-N concentrations.The C_(10)-HSL regulated the intracellular reactive oxygen species levels,denitrification functional enzyme activities,and antioxidant enzyme activities,respectively.This probably synergistically enhanced the defense mechanism against NP toxicity.However,compared to the low NH_(4)^(+)-N concentration of 60 mg/L,the efficacy of C_(10)-HSL was inhibited at high NH_(4)^(+)-N levels of 200 mg/L.The findings provided the significant application potential of QS system for BNR when facing toxic compound shock threats.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
With the aim to effectively depolymerize polyethylene terephthalate(PET)under mild reaction conditions,PET methanolysis and dimethyl terephthalate(DMT)hydrolysis are integrated in a catalyst system.Firstly,methanolysi...With the aim to effectively depolymerize polyethylene terephthalate(PET)under mild reaction conditions,PET methanolysis and dimethyl terephthalate(DMT)hydrolysis are integrated in a catalyst system.Firstly,methanolysis of PET to DMT is achieved over Cu-Mg-Al oxide catalyst.Next,terephthalic acid(TPA)is prepared by DMT hydrolysis.It is found that hydrolysis of DMT to TPA can be promoted by introducing trace amount of water in this catalyst system.CuO-MgO-4.5Al_2O_(3)catalyst demonstrates the excellent catalytic performance for the depolymerization of PET with high conversion rate and TPA yield(100%and 99.5%,respectively)after reaction at 160℃for 6 h,which provides a new idea for the depolymerization of PET.展开更多
Layered transition metal oxides have emerged as promising cathode materials for sodium ion batteries.However,irreversible phase transitions cause structural distortion and cation rearrangement,leading to sluggish Na+d...Layered transition metal oxides have emerged as promising cathode materials for sodium ion batteries.However,irreversible phase transitions cause structural distortion and cation rearrangement,leading to sluggish Na+dynamics and rapid capacity decay.In this study,we propose a medium-entropy cathode by simultaneously introducing Fe,Mg,and Li dopants into a typical P2-type Na_(0.75)Ni_(0.25)Mn_(0.75)O_(2)cathode.The modified Na_(0.75)Ni_(0.2125)Mn_(0.6375)Fe_(0.05)Mg_(0.05)Li_(0.05)O_(2)cathode predominantly exhibits a main P2 phase(93.5%)with a minor O3 phase(6.5%).Through spectroscopy techniques and electrochemical investigations,we elucidate the redox mechanisms of Ni^(2+/3+/4+),Mn^(3+/4+),Fe^(3+/4+),and O_(2)-/O_(2)^(n-)during charging/discharging.The medium-entropy doping mitigates the detrimental P2-O_(2)phase transition at high-voltage,replacing it with a moderate and reversible structural evolution(P2-OP4),thereby enhancing structural stability.Consequently,the modified cathode exhibits a remarkable rate capacity of 108.4 mAh·g^(-1)at 10C,with a capacity retention of 99.0%after 200 cycles at 1C,82.5%after 500 cycles at 5C,and 76.7%after 600 cycles at 10C.Furthermore,it also demonstrates superior electrochemical performance at high cutoff voltage of 4.5 V and extreme temperature(55 and 0℃).This work offers solutions to critical challenges in sodium ion batteries cathode materials.展开更多
In the paper,we report a highly robust and porous bimetallic Ti-MOF(designated Mg_(2)Ti-ABTC)by utiliz-ing a trinuclear[Mg_(2)TiO(COO)_(6)]cluster and a tetradentate H_(4)ABTC(3,3′,5,5′-azobenzene tetracarboxylic ac...In the paper,we report a highly robust and porous bimetallic Ti-MOF(designated Mg_(2)Ti-ABTC)by utiliz-ing a trinuclear[Mg_(2)TiO(COO)_(6)]cluster and a tetradentate H_(4)ABTC(3,3′,5,5′-azobenzene tetracarboxylic acid)ligand.Mg_(2)Ti-ABTC exhibited permanent porosity for N_(2),CO_(2),CH_(4),C_(2)H_(2),C_(2)H_(4),and C_(2)H_(6)gas adsorption.Further-more,Mg_(2)Ti-ABTC exhibited outstanding photocatalytic activity in the oxidation of aromatic sulfides to the corre-sponding sulfoxides under ambient air conditions.Mechanism studies reveal that photoinduced holes(h^(+)),the super-oxide radical(·O_(2)^(-)),and singlet oxygen(^(1)O_(2))are pivotal species involved in the photocatalytic oxidation reaction.展开更多
基金supported by the Natural Science Foundation of Guangdong Province(No.2020A1515110526)the Key-Area Research and Development Programof Guangdong Province(No.2020B1111360003)the National Natural Science Foundation of China(No.42305096).
文摘Nitrogen oxides(NO_(x))are crucial in tropospheric photochemical ozone(O_(3))production and oxidation capacity.Currently,the widely used NO_(x)measurement technique is chemiluminescence(CL)(CL-NO_(x)),which tends to overestimate NO_(2)due to atmospheric oxidation products of NO_(x)(i.e.,NO_(z)).We developed and characterized a NO_(x)measurement system using the cavity attenuated phase shift(CAPS)technique(CAPS-NO_(x)),which is free from interferences with nitrogen-containing species.The NO_(x)measured by the CAPS-NO_(x)and CL-NO_(x)analyzers were compared.Results show that both analyzers showed consistent measurement results for NO,but the NO_(2)measured by the CAPS-NO_(x)analyzer(NO_(2)_CAPS)was mostly lower than that measured by the CL-NO_(x)analyzer(NO_(2)_CL),which led to the deviations in O_(3)formation sensitivity regime and O_(x)(=O_(3)+NO_(2))sources(i.e.,regional background and photochemically produced O_(x))determined by the ozone production efficiencies(OPE)calculated from NO_(2)_CL and NO_(2)_CAPS.Overall,OPE_CL exceeded OPE_CAPS by 18.9%,which shifted 3 out of 13 observation days from the VOCs-limited to the transition regime when judging using OPE_CL,as compared to calculations using OPE_CAPS.During the observation period,days dominated by regional background O_(x)accounted for 46%and 62%when determined using NO_(2)_CL and NO_(2)_CAPS,respectively.These findings suggest that the use of the CL-NO_(x)analyzer tends to underestimate both the VOCs-limited regime and the regional background O_(x)dominated days.The newly built CAPS-NO_(x)analyzer here can promote the accurate measurement of NO_(2),which is meaningful for diagnosing O_(3)formation regimes and O_(x)sources.
基金supported by the National Natural Science Foundation of China(No.U22A20418,22075196)the Research Project Supported by Shanxi Scholarship Council of China(2022–050).
文摘The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocatalysts.However,the low solubility and limited diffusion of N_(2)significantly hinder the achievement of satisfactory performance.In this context,we report an effective strategy to enhance NRR activity by introducing a metal-organic framework(MOF)membrane,specifically MIL-53(Al),onto a perovskite oxide(LiNbO_(3)),denoted as LN@MIL-X(X=0.2,0.4 and 0.6).The MIL-53(Al)membrane selectively recognizes and concentrates N_(2)at the catalyst interface while simultaneously repelling water molecules,thereby inhibiting the hydrogen evolution reaction(HER).This ultrathin nanostructure significantly improves the NRR performance of LN@MIL-X compared to pristine LiNbO_(3).Notably,LN@MIL-0.4 exhibits a maximum NH_(3)yield of 45.25 mg h^(-1)mg_(cat.)^(-1)with an impressive Faradaic efficiency(FE)of 86.41%at-0.45 V versus RHE in 0.1 mol L^(-1)Na_(2)SO_(4).This work provides a universal strategy for the design and synthesis of perovskite oxide electrocatalysts,facilitating high-efficiency ammonia synthesis.
基金supported by National Natural Science Fundation of China(Nos.52170086,22308194,U22A20423)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+1 种基金Taishan Scholars Program of Shandong Province(No.tsqn202211012)Shandong Provincial Excellent Youth(No.ZR2022YQ47)。
文摘Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.
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.
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-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National Natural Science Foundation of China (U23A6005 and 22078069)Project funded by China Postdoctoral Science Foundation (GZB20230172 and 2023M740748)。
文摘Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great potential.We demonstrate the targeted synthesis and cation modulation of NiCo_(2)O_(4)spinel nanoboxes,synthesized via cation exchange and calcination oxidation.These catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds,specifically 2-phenoxy-1-phenylethanol,into nitrogen-containing aromatics,achieving high conversion rates and selectivities.These catalysts were synthesized via a cation exchange and calcination oxidation process,using Prussian blue nanocubes as precursors.The porous architecture and polymetallic composition of the NiCo_(2)O_(4)spinel demonstrated superior performance in electrocatalytic oxidative coupling,achieving a 99.2 wt%conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt%for quinoline derivatives and 31.5 wt%for phenol.Key innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives,the elucidation of a multistage reaction pathway involving CAO bond cleavage,hydroxyaldol condensation,and CAN bond formation,and a deeper mechanistic understanding derived from DFT simulations.This work establishes a new strategy for lignin valorization,offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions,without the need for additional reagents.
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(31572428)。
文摘The objectives of this study which included two experiments were to investigate the effects of dietary inclusion of sorghum grain rich in condensed tannins(CT)(18.9 g kg^(–1)dry matter(DM))on nitrogen(N)metabolism and urine nitrous oxide(N_(2)O)emissions of beef steers.In experiment 1,six Limousin×Luxi crossbreed steers with an initial liveweight of(245.0±18.7)kg were used as experimental animals.Three levels of sorghum grain,i.e.,0,167 and 338 g kg^(–1)DM were included in diets as experimental treatments.The animals and the treatments were randomly assigned to a replicated 3×3 Latin square design.In experiment 2,static incubation technique was used to determine the N_(2)O emissions of the urine samples collected in experiment 1.The results of experiment 1 showed that dietary inclusion of sorghum grain linearly increased the faecal N excretion(P=0.001),the total N excretion(P=0.010)and the faecal N to N intake ratio(P=0.021),but it did not affect the N retention and the N utilization efficiency(P>0.10).The plasma metabolomic data showed that dietary inclusion of sorghum grain increased the relative concentrations of phenolic acid(N1,N5,N10-tris-trans-p-coumaroylspermine and prenyl cis-caffeate)and carnitine(3-hydroxyisovalerylcarnitine and linoelaidyl carnitine).The results also showed that dietary inclusion of sorghum grain linearly increased the urinary urea excretion(P=0.010)and decreased the urinary excretion of purine derivatives(P=0.041)as well as the estimated rumen microbial N supply(P=0.012)based on urinary purine derivatives.The results of experiment 2 showed that including sorghum grain in the diet linearly increased the average concentrations of NH_(4)^(+)-N(P=0.012),NO_(2)^(–)-N(P=0.009),NO_(3)^(-)-N(P=0.001)and the total inorganic N(P<0.001)in the soil enriched with urine samples.The urine sample N_(2)O-N flux(P=0.001),the estimated steer urine N_(2)O-N flux(P=0.021)and the N_(2)O-N to urinary N ratio(P=0.038)linearly increased with increasing inclusion of sorghum grain in the diet.In conclusion,dietary inclusion of sorghum grain containing high CT at 167 and 338 g kg^(–1)DM did not affect the N utilization efficiency of steers but increased the urine N_(2)O-N emissions by 5.7 and 31.4%,respectively.For reducing the N_(2)O emissions to the environment,high levels of sorghum grain should not be included in the diet of steers.
基金supported by Shanghai Pujiang Program(No.22PJD001)the Fundamental Research Funds for the Central Universities(No.2232021G-11).
文摘Catalytic oxidation of NO at room temperature was carried out over nitrogen(N)-doped sludge char(SC)prepared from pyrolysis ofmunicipal sewage sludge,and urea was adopted as nitrogen source.The effects of different N-doping methods(one-step and two-step method),dried sludge(DS)/urea mass ratios(5:1,4:1,3:1,2:1,and 1:1),SC preparation procedures(pyrolysis only,pyrolysis with acid washing,and pyrolysis with KOH activation and acid washing),and different pyrolysis temperatures(500,600,700,and 800°C)on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation.The results indicated that N-doping could obviously promote the catalytic performance of SC.The one-step method with simultaneous sludge pyrolysis(at 700°C),KOH activation,and N-doping(DS/urea of 3:1)was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%,whereas the optimal NO conversion rate of SC without N-doping was only 47.3%.Urea worked both as carbon and nitrogen source,which could increase about 2.9%-16.5%of carbon and 24.8%-42.7%of nitrogen content in SC pyrolyzed at 700°C.N-doping significantly promoted microporosity of SC.The optimal N-doped SC showed specific surface areas of 571.38 m^(2)/g,much higher than 374.34 m^(2)/g of the optimal SC without N-doping.In addition,N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups.Finally,three reaction paths,i.e.microporous reactor,active sites,and basic site control path,were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.
基金financially supported by the National Natural Science Foundation of China(No.22204028)Young Talent Support Project of Guangzhou Association for Science and Technology(No.QT-2023-003)+3 种基金Guangdong Basic and Applied Basic Research Fund Project(No.2022A1515110451)Guangzhou University Graduate Student Innovation Ability Cultivation Funding Program(No.2022GDJC-M06)Science and Technology Projects in Guangzhou(Nos.202201010245,2023A03J0029)Double-Thousand Talents Plan of Jiangxi Province(No.jxsq2023102005)。
文摘The metal ion batteries have gained widespread attention for wearable electronics due to their competitive energy density and long cycling life.Exploring the advanced anode materials is significant for next generation energy storage systems.However,severe electrode volume changes and sluggish redox kinetics are the critical problems for lithium/potassium ion batteries(LIBs/PIBs)towards large-scale applications.Herein,we prepare a novel anode material,which consists of reduced graphene oxide wrapping one-dimensional(1D)N-doped porous carbon nanotube with cobalt phosphoselenide(CoPSe)nanoparticles embedded inside them(r GO@Co PSe/NC).Benefited from the dual carbon decorations and ultrafine nanoparticles structure,it achieves a reversible capacity of 245 mAh/g at 5 A/g after 2000 cycles for LIBs and 215 mAh/g at 1 A/g after 500 cycles for PIBs.The pseudocapacitance and GITT measurements are used to investigate the electrochemical kinetics of r GO@Co PSe/NC for LIBs.In addition,the lithium ion full cell also shows good electrochemical performance when paired with high capacity LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode.This work provides a feasible electrode design strategy for high-efficiency metal ion batteries based on multidimensional nanoarchitecture engineering and composition tailoring.
基金financial support from the National Key Research and Development Program of China(Grant No.2023YFD220120302)supported by RUDN University Strategic Academic Leadership Program。
文摘The role of brassinosteroids(BRs)in enabling plants to respond effectively to adverse conditions is well known,though the precise mechanism of action that helps plants cope with arsenic(As)toxicity is still difficult to interpret.Therefore we tested the effect of brassinolide(BL)spray(0,0.5,and 1 mg·L^(-1))on As(0,and 10 mg·L^(-1))stressed tomato defense responses As stress led to the induction of oxidative stress,impaired chlorophyll and nitrogen metabolism,and Fe uptake,in conjunction with a reduction in plant growth and biomass.BL spray,on the contrary,protected the photo synthetic system and helped plants grow better under As stress.This was achieved by controlling the metabolism of chlorophyll and proline and lowering the amounts of methylglyoxal and H_(2)O_(2) through glyoxalaseⅠandⅡand antioxidant enzyme s.BL decreased arsenic accumulation by directing As sequestration towards vacuoles and increased Fe amount in the leaves and roots by regulating the expression of As(Lsil and Lsi2)and Fe(IRT1,IRT2,NRAMP1,and NRAMP3)transporters in As-stressed tomatoes.Furthermore,BL boosted adaptability against As phytotoxicity,while reducing the damaging impacts on photosynthesis,nitrogen metabolism,sulfur asimilation,and Fe absorption.These results offer a solid framework for the development of exogenous BRs-based breeding strategies for safer agricultural development.
基金supported by the National Natural Science Foundation of China(No.52270119).
文摘The inhibitory effects of zinc oxide nanoparticles(ZnO NPs)and impacts of N-acylhomoserine lactone(AHL)-based quorum sensing(QS)on biological nitrogen removal(BNR)performance have beenwell-investigated.However,the effects of ammonia nitrogen(NH_(4)^(+)-N)concentrations on NP toxicity and AHL regulation have seldom been addressed yet.This study consulted on the impacts of ZnO NPs on BNR systems when high NH_(4)^(+)-N concentrationwas available.The synergistic toxic effects of high-strength NH_(4)^(+)-N(200 mg/L)and ZnO NPs resulted in decreased ammonia oxidation rates and dropped the nitrogen removal efficiencies by 17.5%±0.2%.The increased extracellular polymeric substances(EPS)production was observed in response to the high NH_(4)^(+)-N and ZnO NP stress,which indicated the defensemechanism against the toxic effects in the BNR systemswas stimulated.Furthermore,the regulatory effects of exogenous N-decanoyl-homoserine lactone(C_(10)-HSL)-mediated QS system on NP-stressed BNR systems were revealed to improve the BNR performance under different NH_(4)^(+)-N concentrations.The C_(10)-HSL regulated the intracellular reactive oxygen species levels,denitrification functional enzyme activities,and antioxidant enzyme activities,respectively.This probably synergistically enhanced the defense mechanism against NP toxicity.However,compared to the low NH_(4)^(+)-N concentration of 60 mg/L,the efficacy of C_(10)-HSL was inhibited at high NH_(4)^(+)-N levels of 200 mg/L.The findings provided the significant application potential of QS system for BNR when facing toxic compound shock threats.
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With the aim to effectively depolymerize polyethylene terephthalate(PET)under mild reaction conditions,PET methanolysis and dimethyl terephthalate(DMT)hydrolysis are integrated in a catalyst system.Firstly,methanolysis of PET to DMT is achieved over Cu-Mg-Al oxide catalyst.Next,terephthalic acid(TPA)is prepared by DMT hydrolysis.It is found that hydrolysis of DMT to TPA can be promoted by introducing trace amount of water in this catalyst system.CuO-MgO-4.5Al_2O_(3)catalyst demonstrates the excellent catalytic performance for the depolymerization of PET with high conversion rate and TPA yield(100%and 99.5%,respectively)after reaction at 160℃for 6 h,which provides a new idea for the depolymerization of PET.
基金supported by the National Natural Science Foundation of China(No.21805018)by Sichuan Science and Technology Program(Nos.2022ZHCG0018,2023NSFSC0117 and 2023ZHCG0060)Yibin Science and Technology Program(No.2022JB005)and China Postdoctoral Science Foundation(No.2022M722704).
文摘Layered transition metal oxides have emerged as promising cathode materials for sodium ion batteries.However,irreversible phase transitions cause structural distortion and cation rearrangement,leading to sluggish Na+dynamics and rapid capacity decay.In this study,we propose a medium-entropy cathode by simultaneously introducing Fe,Mg,and Li dopants into a typical P2-type Na_(0.75)Ni_(0.25)Mn_(0.75)O_(2)cathode.The modified Na_(0.75)Ni_(0.2125)Mn_(0.6375)Fe_(0.05)Mg_(0.05)Li_(0.05)O_(2)cathode predominantly exhibits a main P2 phase(93.5%)with a minor O3 phase(6.5%).Through spectroscopy techniques and electrochemical investigations,we elucidate the redox mechanisms of Ni^(2+/3+/4+),Mn^(3+/4+),Fe^(3+/4+),and O_(2)-/O_(2)^(n-)during charging/discharging.The medium-entropy doping mitigates the detrimental P2-O_(2)phase transition at high-voltage,replacing it with a moderate and reversible structural evolution(P2-OP4),thereby enhancing structural stability.Consequently,the modified cathode exhibits a remarkable rate capacity of 108.4 mAh·g^(-1)at 10C,with a capacity retention of 99.0%after 200 cycles at 1C,82.5%after 500 cycles at 5C,and 76.7%after 600 cycles at 10C.Furthermore,it also demonstrates superior electrochemical performance at high cutoff voltage of 4.5 V and extreme temperature(55 and 0℃).This work offers solutions to critical challenges in sodium ion batteries cathode materials.
文摘In the paper,we report a highly robust and porous bimetallic Ti-MOF(designated Mg_(2)Ti-ABTC)by utiliz-ing a trinuclear[Mg_(2)TiO(COO)_(6)]cluster and a tetradentate H_(4)ABTC(3,3′,5,5′-azobenzene tetracarboxylic acid)ligand.Mg_(2)Ti-ABTC exhibited permanent porosity for N_(2),CO_(2),CH_(4),C_(2)H_(2),C_(2)H_(4),and C_(2)H_(6)gas adsorption.Further-more,Mg_(2)Ti-ABTC exhibited outstanding photocatalytic activity in the oxidation of aromatic sulfides to the corre-sponding sulfoxides under ambient air conditions.Mechanism studies reveal that photoinduced holes(h^(+)),the super-oxide radical(·O_(2)^(-)),and singlet oxygen(^(1)O_(2))are pivotal species involved in the photocatalytic oxidation reaction.
