Chemical warfare agents(CWAs)remain a persistent hazard in many parts of the world,necessitating a deeper exploration of their chemical and physical characteristics and reactions under diverse conditions.Diisopropyl m...Chemical warfare agents(CWAs)remain a persistent hazard in many parts of the world,necessitating a deeper exploration of their chemical and physical characteristics and reactions under diverse conditions.Diisopropyl methylphosphonate(DIMP),a commonly used CWA surrogate,is widely studied to enhance our understanding of CWA behavior.The prevailing thermal decomposition model for DIMP,developed approximately 25 years ago,is based on data collected in nitrogen atmospheres at temperatures ranging from 700 K to 800 K.Despite its limitations,this model continues to serve as a foundation for research across various thermal and reactive environments,including combustion studies.Our recent experiments have extended the scope of decomposition analysis by examining DIMP in both nitrogen and zero air across a lower temperature range of 175??C to 250??C.Infrared spectroscopy results under nitrogen align well with the established model;however,we observed that catalytic effects,stemming from decomposition byproducts and interactions with stainless steel surfaces,alter the reaction kinetics.In zero air environments,we observed a novel infrared absorption band.Spectral fitting suggests this band may represent a combination of propanal and acetone,while GCMS analysis points to vinyl formate and acetone as possible constituents.Although the precise identity of these new products remains unresolved,our findings clearly indicate that the existing decomposition model cannot be reliably extended to lower temperatures or non-nitrogen environments without further revisions.展开更多
The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.A...The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.Accordingly,comprehensive kinetic study by employing thermalgravimetric analysis at various heating rates was presented in this paper.Two main weight loss regions were observed during heating.The initial region corresponded to the dehydration of crystal water,whereas the subsequent region with overlapping peaks involved complex decomposition reactions.The overlapping peaks were separated into two individual reaction peaks and the activation energy of each peak was calculated using isoconversional kinetics methods.The activation energy of peak 1 exhibited a continual increase as the reaction conversion progressed,while that of peak 2 steadily decreased.The optimal kinetic models,identified as belonging to the random nucleation and subsequent growth category,provided valuable insights into the mechanism of the decomposition reactions.Furthermore,the adjustment factor was introduced to reconstruct the kinetic mechanism models,and the reconstructed models described the kinetic mechanism model more accurately for the decomposition reactions.This study enhanced the understanding of the thermochemical behavior and kinetic parameters of the lepidolite sulfation product decomposition reactions,further providing theoretical basis for promoting the selective extraction of lithium.展开更多
The microstructural evolution of Cu−19Ni−6Cr−7Mn alloy during aging treatment was investigated.After aging for 120 min at 500℃,the alloy exhibited excellent mechanical properties,including a tensile strength of 978 M...The microstructural evolution of Cu−19Ni−6Cr−7Mn alloy during aging treatment was investigated.After aging for 120 min at 500℃,the alloy exhibited excellent mechanical properties,including a tensile strength of 978 MPa and an elastic modulus of 145.8 GPa.After aging for 240 min at 500℃,the elastic modulus of the alloy reached 149.5 GPa,which was among the highest values reported for Cu alloys.It was worth mentioning that the tensile strength increased rapidly from 740 to 934 MPa after aging for 5 min at 500℃,which was close to the maximum tensile strength(978 MPa).Analysis of the underlying strengthening mechanisms and phase transformation behavior revealed that the Cu−19Ni−6Cr−7Mn alloy underwent spinodal decomposition and DO_(22) ordering during the first 5 min of aging at 500℃,and L1_(2) ordered phases and bcc-Cr precipitates appeared.Therefore,the enhanced mechanical properties of the Cu−19Ni−6Cr−7Mn alloy can be attributed to the stress field generated by spinodal decomposition and the presence of nanoscale ordered phase and Cr precipitates.展开更多
Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy convers...Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy conversion efficiency.In certain application scenarios,the use of N_(2)O(a potent greenhouse gas),as an alternative oxidant to air,presents a feasible strategy.Herein,we report for the first time the operation of PCFCs employing N_(2)O as the oxidant.A hybrid Pr_(2)Ni_(0.6)Co_(0.4)O_(4-δ)(PNCO-214)catalyst is developed,comprising Ruddlesden-Popper(R-P)structured Pr_(4)Ni_(1.8)Co_(1.2)O_(10-δ)(PNCO-4310)and fluorite structured Pr_(6)O_(11)(PO-611),which synergistically exhibits exceptional catalytic activity toward both N_(2)O decomposition and the oxygen reduction reaction,achieving a conversion over 92% and an area specific resistance of 1.301Ω·cm^(2) at 600℃.Quasi-insitu temperature-dependent Fourier transform infrared(FTIR)and electrochemical impedance spectroscopy analyses reveal that abundant oxygen vacancies in PNCO-214 facilitate rapid adsorption and dissociation of N_(2)O into N_(2) and O_(2),while also promoting the surface exchange kinetics of proton/oxygen during oxygen reduction reaction(ORR).When applied in an anode-supported single cell with PNCO-214 cathode operating under N_(2)O,outstanding power density and low resistance are achieved,delivering 0.801 W·cm^(-2) and 0.245Ω·cm^(2) at 600℃.Satisfactory performance is also maintained even when the temperature is reduced to 500℃.Furthermore,the single cell demonstrates relatively good stability with negligible degradation over 130 h at 600℃ and 0.7 V.These findings underscore the potential of PNCO-214 as a highly effective cathode catalyst for enabling the use of N_(2)O as a viable oxidant in PCFCs for specific industrial applications.展开更多
In recent years,ozone has become one of the key pollutants affecting the urban air qual-ity.Direct catalytic decomposition of ozone emerges as an effective method for ozone re-moval.Field experimentswere conducted to ...In recent years,ozone has become one of the key pollutants affecting the urban air qual-ity.Direct catalytic decomposition of ozone emerges as an effective method for ozone re-moval.Field experimentswere conducted to evaluate the effectiveness of exteriorwall coat-ings with ozone decomposition catalysts for ozone removal in practical applications.ANSYS 2020R1 software was first used for simulation and analysis of ozone concentration and flow fields to investigate the decomposition boundary of these wall coatings.The results show that the exterior wall coatings with manganese-based catalysts can effectively reduce the ozone concentration near the wall coating.The ozone decomposition efficiency is nega-tively correlated with the distance fromthe coating and the decomposition boundary range is around 18 m.The decomposition boundary will increase with the increase of tempera-ture,and decrease with the increase of the wind speed and the relative humidity.These results underscore the viability of using exterior wall coatings with catalysts for controlling ozone pollution in atmospheric environments.This approach presents a promising avenue for addressing ozone pollution through self-purifying materials on building external wall.展开更多
In the realm of nonlinear integrable systems,the presence of decompositions facilitates the establishment of linear superposition solutions and the derivation of novel coupled systems exhibiting nonlinear integrabilit...In the realm of nonlinear integrable systems,the presence of decompositions facilitates the establishment of linear superposition solutions and the derivation of novel coupled systems exhibiting nonlinear integrability.By focusing on single-component decompositions within the potential BKP hierarchy,it has been observed that specific linear superpositions of decomposition solutions remain consistent with the underlying equations.Moreover,through the implementation of multi-component decompositions within the potential BKP hierarchy,successful endeavors have been undertaken to formulate linear superposition solutions and novel coupled Kd V-type systems that resist decoupling via alterations in dependent variables.展开更多
Earthquakes can cause significant hazards,leading to loss of human life and property damage.In this study,we applied the masking empirical mode decomposition(EMD)to the Gyeongju earthquake(ML 5.8)in South Korea and th...Earthquakes can cause significant hazards,leading to loss of human life and property damage.In this study,we applied the masking empirical mode decomposition(EMD)to the Gyeongju earthquake(ML 5.8)in South Korea and the Abe Pura earthquake(ML 7.0)in Indonesia and then revealed that the 7th intrinsic mode function(IMF7),composed of waveforms with a period band of approximately 150 to 750 minutes.展开更多
Machine-learning is a robust technique for understanding pollution characteristics of surface ozone,which are at high levels in urban China.This study introduced an innovative approach combining trend decomposition wi...Machine-learning is a robust technique for understanding pollution characteristics of surface ozone,which are at high levels in urban China.This study introduced an innovative approach combining trend decomposition with Random Forest algorithm to investigate ozone dynamics and formation regimes in a coastal area of China.During the period of 2017–2022,significant inter-annual fluctuations emerged,with peaks in mid-2017 attributed to volatile organic compounds(VOCs),and in late-2019 influenced by air temperature.Multifaceted periodicities(daily,weekly,holiday,and yearly)in ozone were revealed,elucidating substantial influences of daily and yearly components on ozone periodicity.A VOC-sensitive ozone formation regime was identified,characterized by lower VOCs/NO_(x) ratios(average=0.88)and significant positive correlations between ozone and VOCs.This interplay manifested in elevated ozone duringweekends,holidays,and pandemic lockdowns.Key variables influencing ozone across diverse timescaleswere uncovered,with solar radiation and temperature driving daily and yearly ozone variations,respectively.Precursor substances,particularly VOCs,significantly shaped weekly/holiday patterns and long-term trends of ozone.Specifically,acetone,ethane,hexanal,and toluene had a notable impact on the multi-year ozone trend,emphasizing the urgency of VOC regulation.Furthermore,our observations indicated that NO_(x) primarily drived the stochastic variations in ozone,a distinguishing characteristic of regions with heavy traffic.This research provides novel insights into ozone dynamics in coastal urban areas and highlights the importance of integrating statistical and machinelearning methods in atmospheric pollution studies,with implications for targeted mitigation strategies beyond this specific region and pollutant.展开更多
Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. Ho...Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. However, such fascinating properties do not bring long-term cyclability of h-LMBs. One of critical challenges is the interface instability in contacting with the Li metal anode, as fiuorinated solvents are highly susceptible to exceptionally reductive metallic Li attributed to its low lowest unoccupied molecular orbital(LUMO), which leads to significant consumption of the fiuorinated components upon cycling.Herein, attenuating reductive decomposition of fiuorinated electrolytes is proposed to circumvent rapid electrolyte consumption. Specifically, the vinylene carbonate(VC) is selected to tame the reduction decomposition by preferentially forming protective layer on the Li anode. This work, experimentally and computationally, demonstrates the importance of pre-passivation of Li metal anodes at high voltage to attenuate the decomposition of fiuoroethylene carbonate(FEC). It is expected to enrich the understanding of how VC attenuate the reactivity of FEC, thereby extending the cycle life of fiuorinated electrolytes in high-voltage Li-metal batteries.展开更多
Multivariate time series forecasting iswidely used in traffic planning,weather forecasting,and energy consumption.Series decomposition algorithms can help models better understand the underlying patterns of the origin...Multivariate time series forecasting iswidely used in traffic planning,weather forecasting,and energy consumption.Series decomposition algorithms can help models better understand the underlying patterns of the original series to improve the forecasting accuracy of multivariate time series.However,the decomposition kernel of previous decomposition-based models is fixed,and these models have not considered the differences in frequency fluctuations between components.These problems make it difficult to analyze the intricate temporal variations of real-world time series.In this paper,we propose a series decomposition-based Mamba model,DecMamba,to obtain the intricate temporal dependencies and the dependencies among different variables of multivariate time series.A variable-level adaptive kernel combination search module is designed to interact with information on different trends and periods between variables.Two backbone structures are proposed to emphasize the differences in frequency fluctuations of seasonal and trend components.Mamba with superior performance is used instead of a Transformer in backbone structures to capture the dependencies among different variables.A new embedding block is designed to capture the temporal features better,especially for the high-frequency seasonal component whose semantic information is difficult to acquire.A gating mechanism is introduced to the decoder in the seasonal backbone to improve the prediction accuracy.A comparison with ten state-of-the-art models on seven real-world datasets demonstrates that DecMamba can better model the temporal dependencies and the dependencies among different variables,guaranteeing better prediction performance for multivariate time series.展开更多
The multi-objective particle swarm optimization algorithm(MOPSO)is widely used to solve multi-objective optimization problems.In the article,amulti-objective particle swarm optimization algorithmbased on decomposition...The multi-objective particle swarm optimization algorithm(MOPSO)is widely used to solve multi-objective optimization problems.In the article,amulti-objective particle swarm optimization algorithmbased on decomposition and multi-selection strategy is proposed to improve the search efficiency.First,two update strategies based on decomposition are used to update the evolving population and external archive,respectively.Second,a multiselection strategy is designed.The first strategy is for the subspace without a non-dominated solution.Among the neighbor particles,the particle with the smallest penalty-based boundary intersection value is selected as the global optimal solution and the particle far away fromthe search particle and the global optimal solution is selected as the personal optimal solution to enhance global search.The second strategy is for the subspace with a non-dominated solution.In the neighbor particles,two particles are randomly selected,one as the global optimal solution and the other as the personal optimal solution,to enhance local search.The third strategy is for Pareto optimal front(PF)discontinuity,which is identified by the cumulative number of iterations of the subspace without non-dominated solutions.In the subsequent iteration,a new probability distribution is used to select from the remaining subspaces to search.Third,an adaptive inertia weight update strategy based on the dominated degree is designed to further improve the search efficiency.Finally,the proposed algorithmis compared with fivemulti-objective particle swarm optimization algorithms and five multi-objective evolutionary algorithms on 22 test problems.The results show that the proposed algorithm has better performance.展开更多
To address the issues of peak overlap caused by complex matrices in agricultural product terahertz(THz)spectral signals and the dynamic,nonlinear interference induced by environmental and system noise,this study explo...To address the issues of peak overlap caused by complex matrices in agricultural product terahertz(THz)spectral signals and the dynamic,nonlinear interference induced by environmental and system noise,this study explores the feasibility of adaptive-signal-decomposition-based denoising methods to improve THz spectral quality.THz time-domain spectroscopy(THz-TDS)combined with an attenuated total reflection(ATR)accessory was used to collect THz absorbance spectra from 48 peanut samples.Taking the quantitative prediction model of peanut moisture content based on THz-ATR as an example,wavelet transform(WT),empirical mode decomposition(EMD),local mean decomposition(LMD),and its improved methods-segmented local mean decomposition(SLMD)and piecewise mirror extension local mean decomposition(PME-LMD)-were employed for spectral denoising.The applicability of different denoising methods was evaluated using a support vector regression(SVR)model.Experimental results show that the peanut moisture content prediction model constructed after PME-LMD denoising achieved the best performance,with a root mean square error(RMSE),coefficient of determination(R^(2)),and mean absolute percentage error(MAPE)of 0.010,0.912,and 0.040,respectively.Compared with traditional methods,PME-LMD significantly improved spectral quality and model prediction performance.The PME-LMD denoising strategy proposed in this study effectively suppresses non-uniform noise interference in THz spectral signals,providing an efficient and accurate preprocessing method for THz spectral analysis of agricultural products.This research provides theoretical support and technical guidance for the application of THz technology for detecting agricultural product quality.展开更多
In this paper,we prove that L(K_(x,y))(λ),theλ-fold line graph of the complete bipartite graph Ka,y,has a C_(6)-decomposition if and only if ry≥6,λxy(c+y-2)=0(mod 12)and(x+y)=0(mod 2),where x,y are nonnegative int...In this paper,we prove that L(K_(x,y))(λ),theλ-fold line graph of the complete bipartite graph Ka,y,has a C_(6)-decomposition if and only if ry≥6,λxy(c+y-2)=0(mod 12)and(x+y)=0(mod 2),where x,y are nonnegative integers and(x,y)≠(2,4)or(2,5).展开更多
The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste g...The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste gas but also recover clean energy H_(2),which has significant socio-economic and ecological advantages.However,the highly effective decomposition of H_(2)S at low temperatures is still a great challenge,because of the stringent thermodynamic equilibrium constraints(only 20% even at high temperature of 1010℃).Conventional microwave catalysts exhibit unsatisfactory performance at low temperatures(below 600℃).Herein,Mo_(2)C@CeO_(2) catalysts with a core-shell structure were successfully developed for robust microwave catalytic decomposition of H_(2)S at low temperatures.Two carbon precursors,para-phenylenediamine(Mo_(2)C-p)and meta-phenylenediamine(Mo_(2)C-m),were employed to tailor Mo_(2)C configurations.Remarkably,the H_(2)S conversion of Mo_(2)C-p@CeO_(2) catalyst at a low temperature of 550℃ is as high as 92.1%,which is much higher than the H_(2)S equilibrium conversion under the conventional thermal conditions(2.6% at 550℃).To our knowledge,this represents the most active catalyst for microwave catalytic decomposition of H_(2)S at low temperature of 550℃.Notably,Mo_(2)C-p demonstrated superior intrinsic activity(84%)compared to Mo_(2)C-m(6.4%),with XPS analysis revealing that its enhanced performance stems from a higher concentration of Mo_(2+)active sites.This work presents a substitute approach for the efficient utilization of H_(2)S waste gas and opens up a novel avenue for the rational design of microwave catalysts for microwave catalytic reaction at low-temperature.展开更多
Organic matter(OM)derived from the decomposition of crop residues plays a key role as a sorbent for cadmium(Cd)immobilization.Few studies have explored the straw decomposition processes with the presence of minerals,a...Organic matter(OM)derived from the decomposition of crop residues plays a key role as a sorbent for cadmium(Cd)immobilization.Few studies have explored the straw decomposition processes with the presence of minerals,and the effect of newly generated organomineral complexes on heavy metal adsorption.In this study,we investigated the variations in structure and composition during the rice straw decomposition with or without minerals(goethite and kaolinite),as well as the adsorption behavior and mechanisms by which straw decomposition affects Cd immobilization.The degree of humification of extracted straw organic matter was assessed using excitation-emission matrix(EEM)fluorescence and Ultraviolet-visible spectroscopy(UV-vis),while employing FTIR spectroscopy and XPS to characterize the adsorption mechanisms.The spectra analysis revealed the enrichment of highly aromatic and hydrophobic components,indicating that the degree of straw decomposition and humification were further intensified during incubation.Additionally,the existence of goethite(SG)accelerated the humification of OM.Sorption experiments revealed that the straw humification increased Cd adsorption capacity.Notably,SG exhibited significantly higher adsorption performance compared to the organic matter without minerals(RS)and the existence of kaolinite(SK).Further analysis using FT-IR spectroscopy and XPS verified that the primarymechanisms involved in Cd immobilization were complexion with—OH and—COOH,as well as the formation of Cd-πbinds with aromatic C=C on the surface of solid OMs.These findings will facilitate understanding the interactions of the rice straw decomposing with soil minerals and its remediation effect on Cd-contaminated farmland.展开更多
The deployment of non-precious metal catalysts for the production of COx-free hydrogen via the ammonia decomposition reaction(ADR)presents a promising yet great challenge.In the present study,two crystal structures of...The deployment of non-precious metal catalysts for the production of COx-free hydrogen via the ammonia decomposition reaction(ADR)presents a promising yet great challenge.In the present study,two crystal structures of α-MoC and β-Mo_(2)C catalysts with different Mo/C ratios were synthesized,and their ammonia decomposition performance as well as structural evolution in ADR was investigated.The β-Mo_(2)C catalyst,characterized by a higher Mo/C ratio,demonstrated a remarkable turnover frequency of 1.3 s^(-1),which is over tenfold higher than that ofα-MoC(0.1 s^(-1)).An increase in the Mo/C ratio of molybdenum carbide revealed a direct correlation between the surface Mo/C ratio and the hydrogen yield.The transient response surface reaction indicated that the combination of N*and N*derived from NH_(3) dissociation represents the rate-determining step in the ADR,andβ-Mo2C exhibited exceptional proficiency in facilitating this pivotal step.Concurrently,the accumulation of N*species on the carbide surface could induce the phase transition of molybdenum carbide to nitride,which follows a topological transformation.It is discovered that such phase evolution was affected by the Mo-C surface and reaction temperature simultaneously.When the kinetics of combination of N*was accelerated by rising temperatures and its accumulation on the carbide surface was mitigated,β-Mo_(2)C maintained its carbide phase,preventing nitridation during the ADR at 810℃.Our results contribute to an in-depth understanding of the molybdenum carbides’catalytic properties in ADR and highlight the nature of the carbide-nitride phase transition in the reaction.展开更多
This paper introduces dynamic mode decomposition(DMD)as a novel approach to model the breakage kinetics of particulate systems.DMD provides a data-driven framework to identify a best-fit linear dynamics model from a s...This paper introduces dynamic mode decomposition(DMD)as a novel approach to model the breakage kinetics of particulate systems.DMD provides a data-driven framework to identify a best-fit linear dynamics model from a sequence of system measurement snapshots,bypassing the nontrivial task of determining appropriate mathemat-ical forms for the breakage kernel functions.A key innovation of our method is the instilling of physics-informed constraints into the DMD eigenmodes and eigenvalues,ensuring they adhere to the physical structure of particle breakage processes even under sparse measurement data.The integration of eigen-constraints is computationally aided by a zeroth-order global optimizer for solving the nonlinear,nonconvex optimization problem that elicits system dynamics from data.Our method is evaluated against the state-of-the-art optimized DMD algorithm using both generated data and real-world data of a batch grinding mill,showcasing over an order of magnitude lower prediction errors in data reconstruction and forecasting.展开更多
The land application of livestock manure has been widely acknowledged as a beneficial approach for nutrient recycling and environmental protection.However,the impact of residual antibiotics,a common contaminant of man...The land application of livestock manure has been widely acknowledged as a beneficial approach for nutrient recycling and environmental protection.However,the impact of residual antibiotics,a common contaminant of manure,on the degradation of organic compounds and nutrient release in Eutric Regosol is not well understood.Here,we studied,how oxytetracycline(OTC)and ciprofloxacin(CIP)affect the decomposition,microbial community structure,extracellular enzyme activities and nutrient release from cattle and pig manure using litterbag incubation experiments.Results showed that OTC and CIP greatly inhibited livestock manure decomposition,causing a decreased rate of carbon(28%-87%),nitrogen(15%-44%)and phosphorus(26%-43%)release.The relative abundance of gramnegative(G-)bacteria was reduced by 4.0%-13%while fungi increased by 7.0%-71%during a 28-day incubation period.Co-occurrence network analysis showed that antibiotic exposure disrupted microbial interactions,particularly among G-bacteria,G+bacteria,and actinomycetes.These changes in microbial community structure and function resulted in decreased activity of urease,β-1,4-N-acetyl-glucosaminidase,alkaline protease,chitinase,and catalase,causing reduced decomposition and nutrient release in cattle and pig ma-nures.These findings advance our understanding of decomposition and nutrient recycling from manure-contaminated antibiotics,which will help facilitate sustainable agricultural production and soil carbon sequestration.展开更多
Monolithic catalysts with excellent O_(3)catalytic decomposition performance were prepared by in situ loading of Co-doped KMn_(8)O_(16)on the surface of nickel foam.The triple-layer structure with Co-doped KMn_(8)O_(1...Monolithic catalysts with excellent O_(3)catalytic decomposition performance were prepared by in situ loading of Co-doped KMn_(8)O_(16)on the surface of nickel foam.The triple-layer structure with Co-doped KMn_(8)O_(16)/Ni6MnO_(8)/Ni foam was grown spontaneously on the surface of nickel foam by tuning the molar ratio of KMnO_(4)to Co(NO_(3))_(2)·6H_(2)O precursors.Importantly,the formed Ni6MnO_(8)structure between KMn_(8)O_(16)and nickel foam during in situ synthesis process effectively protected nickel foam from further etching,which significantly enhanced the reaction stability of catalyst.The optimum amount of Co doping in KMn_(8)O_(16)was available when the molar ratio of Mn to Co species in the precursor solution was 2:1.And the Mn2Co1 catalyst had abundant oxygen vacancies and excellent hydrophobicity,thus creating outstanding O_(3)decomposition activity.The O_(3)conversion under dry conditions and relative humidity of 65%,90%over a period of 5 hr was 100%,94%and 80%with the space velocity of 28,000 hr^(−1),respectively.The in situ constructed Co-doped KMn_(8)O_(16)/Ni foam catalyst showed the advantages of low price and gradual applicability of the preparation process,which provided an opportunity for the design of monolithic catalyst for O_(3)catalytic decomposition.展开更多
The catalytic performance of supported metal catalysts is highly dependent on the interfacial contact between the metal centers and support materials,which could dynamically adapt to the chemical environment in the re...The catalytic performance of supported metal catalysts is highly dependent on the interfacial contact between the metal centers and support materials,which could dynamically adapt to the chemical environment in the reactions.Herein,the well-known Ru/TiO_(x)interface of the Ru/TiO_(2)catalyst is shown to be transformed into Ru/TiO_(x)N_(y)during the NH_(3)decomposition,which is derived from the nitridation of the support by N^(*)species.Through a series of characterizations and density functional theory(DFT)calculations,it is found that such a nitrogenous interface primarily blocks the cleavage of N-H bonds with a higher energy barrier,leading to the deactivation of Ru/TiO_(2)in NH_(3)decomposition.Nevertheless,the Ru/TiO_(x)interface can be easily restored by oxidation and a subsequent H2 reduction,contributing to the recovery of the catalytic activity toward NH_(3)decomposition.Our study provides a new insight into the deactivation mechanism of Ru/TiO_(2)in NH_(3)decomposition and highlights the significance of the dynamic evolution of the metal-support interfaces in the reactions.展开更多
基金sponsored by the Department of Defense,Defense Threat Reduction Agency under the Materials Science in Extreme Environments University Research Alliance,HDTRA1-20-2-0001。
文摘Chemical warfare agents(CWAs)remain a persistent hazard in many parts of the world,necessitating a deeper exploration of their chemical and physical characteristics and reactions under diverse conditions.Diisopropyl methylphosphonate(DIMP),a commonly used CWA surrogate,is widely studied to enhance our understanding of CWA behavior.The prevailing thermal decomposition model for DIMP,developed approximately 25 years ago,is based on data collected in nitrogen atmospheres at temperatures ranging from 700 K to 800 K.Despite its limitations,this model continues to serve as a foundation for research across various thermal and reactive environments,including combustion studies.Our recent experiments have extended the scope of decomposition analysis by examining DIMP in both nitrogen and zero air across a lower temperature range of 175??C to 250??C.Infrared spectroscopy results under nitrogen align well with the established model;however,we observed that catalytic effects,stemming from decomposition byproducts and interactions with stainless steel surfaces,alter the reaction kinetics.In zero air environments,we observed a novel infrared absorption band.Spectral fitting suggests this band may represent a combination of propanal and acetone,while GCMS analysis points to vinyl formate and acetone as possible constituents.Although the precise identity of these new products remains unresolved,our findings clearly indicate that the existing decomposition model cannot be reliably extended to lower temperatures or non-nitrogen environments without further revisions.
基金financially supported by the National Natural Science Foundation of China(Nos.52034002 and U2202254)the Fundamental Research Funds for the Central Universities,China(No.FRF-TT-19-001)。
文摘The sulfation and decomposition process has proven effective in selectively extracting lithium from lepidolite.It is essential to clarify the thermochemical behavior and kinetic parameters of decomposition reactions.Accordingly,comprehensive kinetic study by employing thermalgravimetric analysis at various heating rates was presented in this paper.Two main weight loss regions were observed during heating.The initial region corresponded to the dehydration of crystal water,whereas the subsequent region with overlapping peaks involved complex decomposition reactions.The overlapping peaks were separated into two individual reaction peaks and the activation energy of each peak was calculated using isoconversional kinetics methods.The activation energy of peak 1 exhibited a continual increase as the reaction conversion progressed,while that of peak 2 steadily decreased.The optimal kinetic models,identified as belonging to the random nucleation and subsequent growth category,provided valuable insights into the mechanism of the decomposition reactions.Furthermore,the adjustment factor was introduced to reconstruct the kinetic mechanism models,and the reconstructed models described the kinetic mechanism model more accurately for the decomposition reactions.This study enhanced the understanding of the thermochemical behavior and kinetic parameters of the lepidolite sulfation product decomposition reactions,further providing theoretical basis for promoting the selective extraction of lithium.
基金supported by the National Key R&D Program of China (No. 2021YFB3700700)the Henan Province Top Talent Training Program Project, China (No. 244500510020)the High-level Talent Research Start-up Project Funding of Henan Academy of Sciences, China (No. 242017001)。
文摘The microstructural evolution of Cu−19Ni−6Cr−7Mn alloy during aging treatment was investigated.After aging for 120 min at 500℃,the alloy exhibited excellent mechanical properties,including a tensile strength of 978 MPa and an elastic modulus of 145.8 GPa.After aging for 240 min at 500℃,the elastic modulus of the alloy reached 149.5 GPa,which was among the highest values reported for Cu alloys.It was worth mentioning that the tensile strength increased rapidly from 740 to 934 MPa after aging for 5 min at 500℃,which was close to the maximum tensile strength(978 MPa).Analysis of the underlying strengthening mechanisms and phase transformation behavior revealed that the Cu−19Ni−6Cr−7Mn alloy underwent spinodal decomposition and DO_(22) ordering during the first 5 min of aging at 500℃,and L1_(2) ordered phases and bcc-Cr precipitates appeared.Therefore,the enhanced mechanical properties of the Cu−19Ni−6Cr−7Mn alloy can be attributed to the stress field generated by spinodal decomposition and the presence of nanoscale ordered phase and Cr precipitates.
基金financially supported by the National Key R&D Program of China(No.2024YFF0506300)National Natural Science Foundation of China(No.52336009)+5 种基金Key Research and Development Program of Shaanxi(No.2024CY2-GJHX-66)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515010429)Natural Science Basic Research Plan in Shaanxi Province of China(No.2024JC-YBQN-0475)Xidian University Specially Funded Project for Interdisciplinary Exploration(No.TZJH2024063)the Fundamental Research Funds for the Central Universities(No.QTZX23061)the Innovation Center of Nuclear Power Technology(No.HDLCXZX-2022-ZH-013).
文摘Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy conversion efficiency.In certain application scenarios,the use of N_(2)O(a potent greenhouse gas),as an alternative oxidant to air,presents a feasible strategy.Herein,we report for the first time the operation of PCFCs employing N_(2)O as the oxidant.A hybrid Pr_(2)Ni_(0.6)Co_(0.4)O_(4-δ)(PNCO-214)catalyst is developed,comprising Ruddlesden-Popper(R-P)structured Pr_(4)Ni_(1.8)Co_(1.2)O_(10-δ)(PNCO-4310)and fluorite structured Pr_(6)O_(11)(PO-611),which synergistically exhibits exceptional catalytic activity toward both N_(2)O decomposition and the oxygen reduction reaction,achieving a conversion over 92% and an area specific resistance of 1.301Ω·cm^(2) at 600℃.Quasi-insitu temperature-dependent Fourier transform infrared(FTIR)and electrochemical impedance spectroscopy analyses reveal that abundant oxygen vacancies in PNCO-214 facilitate rapid adsorption and dissociation of N_(2)O into N_(2) and O_(2),while also promoting the surface exchange kinetics of proton/oxygen during oxygen reduction reaction(ORR).When applied in an anode-supported single cell with PNCO-214 cathode operating under N_(2)O,outstanding power density and low resistance are achieved,delivering 0.801 W·cm^(-2) and 0.245Ω·cm^(2) at 600℃.Satisfactory performance is also maintained even when the temperature is reduced to 500℃.Furthermore,the single cell demonstrates relatively good stability with negligible degradation over 130 h at 600℃ and 0.7 V.These findings underscore the potential of PNCO-214 as a highly effective cathode catalyst for enabling the use of N_(2)O as a viable oxidant in PCFCs for specific industrial applications.
基金supported by the National Natural Science Foundation of China(Nos.52470114 and 52022104)the National Key R&D Program of China(No.2022YFC3702802)the Youth Innovation Promotion Association,CAS(No.Y2021020).
文摘In recent years,ozone has become one of the key pollutants affecting the urban air qual-ity.Direct catalytic decomposition of ozone emerges as an effective method for ozone re-moval.Field experimentswere conducted to evaluate the effectiveness of exteriorwall coat-ings with ozone decomposition catalysts for ozone removal in practical applications.ANSYS 2020R1 software was first used for simulation and analysis of ozone concentration and flow fields to investigate the decomposition boundary of these wall coatings.The results show that the exterior wall coatings with manganese-based catalysts can effectively reduce the ozone concentration near the wall coating.The ozone decomposition efficiency is nega-tively correlated with the distance fromthe coating and the decomposition boundary range is around 18 m.The decomposition boundary will increase with the increase of tempera-ture,and decrease with the increase of the wind speed and the relative humidity.These results underscore the viability of using exterior wall coatings with catalysts for controlling ozone pollution in atmospheric environments.This approach presents a promising avenue for addressing ozone pollution through self-purifying materials on building external wall.
基金sponsored by the National Natural Science Foundations of China under Grant Nos.12301315,12235007,11975131the Zhejiang Provincial Natural Science Foundation of China under Grant No.LQ20A010009。
文摘In the realm of nonlinear integrable systems,the presence of decompositions facilitates the establishment of linear superposition solutions and the derivation of novel coupled systems exhibiting nonlinear integrability.By focusing on single-component decompositions within the potential BKP hierarchy,it has been observed that specific linear superpositions of decomposition solutions remain consistent with the underlying equations.Moreover,through the implementation of multi-component decompositions within the potential BKP hierarchy,successful endeavors have been undertaken to formulate linear superposition solutions and novel coupled Kd V-type systems that resist decoupling via alterations in dependent variables.
基金supported as part of the"2024 Groundwater Basic Survey Project,"funded by the Ministry of Environment(Project No.20240123-001)。
文摘Earthquakes can cause significant hazards,leading to loss of human life and property damage.In this study,we applied the masking empirical mode decomposition(EMD)to the Gyeongju earthquake(ML 5.8)in South Korea and the Abe Pura earthquake(ML 7.0)in Indonesia and then revealed that the 7th intrinsic mode function(IMF7),composed of waveforms with a period band of approximately 150 to 750 minutes.
基金supported by Ningbo Natural Science Foundation(No.2023J059)Ningbo Commonweal Programme Key Project(No.2023S038)Guangxi Key Research and Development Programme(No.GuikeAB21220063).
文摘Machine-learning is a robust technique for understanding pollution characteristics of surface ozone,which are at high levels in urban China.This study introduced an innovative approach combining trend decomposition with Random Forest algorithm to investigate ozone dynamics and formation regimes in a coastal area of China.During the period of 2017–2022,significant inter-annual fluctuations emerged,with peaks in mid-2017 attributed to volatile organic compounds(VOCs),and in late-2019 influenced by air temperature.Multifaceted periodicities(daily,weekly,holiday,and yearly)in ozone were revealed,elucidating substantial influences of daily and yearly components on ozone periodicity.A VOC-sensitive ozone formation regime was identified,characterized by lower VOCs/NO_(x) ratios(average=0.88)and significant positive correlations between ozone and VOCs.This interplay manifested in elevated ozone duringweekends,holidays,and pandemic lockdowns.Key variables influencing ozone across diverse timescaleswere uncovered,with solar radiation and temperature driving daily and yearly ozone variations,respectively.Precursor substances,particularly VOCs,significantly shaped weekly/holiday patterns and long-term trends of ozone.Specifically,acetone,ethane,hexanal,and toluene had a notable impact on the multi-year ozone trend,emphasizing the urgency of VOC regulation.Furthermore,our observations indicated that NO_(x) primarily drived the stochastic variations in ozone,a distinguishing characteristic of regions with heavy traffic.This research provides novel insights into ozone dynamics in coastal urban areas and highlights the importance of integrating statistical and machinelearning methods in atmospheric pollution studies,with implications for targeted mitigation strategies beyond this specific region and pollutant.
基金supported by the National Natural Science Foundation of China (Nos. 22379121, 62005216)Basic Public Welfare Research Program of Zhejiang (No. LQ22F050013)+1 种基金Zhejiang Province Key Laboratory of Flexible Electronics Open Fund (2023FE005)Shenzhen Foundation Research Program (No. JCYJ20220530112812028)。
文摘Fluoride-based electrolyte exhibits extraordinarily high oxidative stability in high-voltage lithium metal batteries(h-LMBs) due to the inherent low highest occupied molecular orbital(HOMO) of fiuorinated solvents. However, such fascinating properties do not bring long-term cyclability of h-LMBs. One of critical challenges is the interface instability in contacting with the Li metal anode, as fiuorinated solvents are highly susceptible to exceptionally reductive metallic Li attributed to its low lowest unoccupied molecular orbital(LUMO), which leads to significant consumption of the fiuorinated components upon cycling.Herein, attenuating reductive decomposition of fiuorinated electrolytes is proposed to circumvent rapid electrolyte consumption. Specifically, the vinylene carbonate(VC) is selected to tame the reduction decomposition by preferentially forming protective layer on the Li anode. This work, experimentally and computationally, demonstrates the importance of pre-passivation of Li metal anodes at high voltage to attenuate the decomposition of fiuoroethylene carbonate(FEC). It is expected to enrich the understanding of how VC attenuate the reactivity of FEC, thereby extending the cycle life of fiuorinated electrolytes in high-voltage Li-metal batteries.
基金supported in part by the Interdisciplinary Project of Dalian University(DLUXK-2023-ZD-001).
文摘Multivariate time series forecasting iswidely used in traffic planning,weather forecasting,and energy consumption.Series decomposition algorithms can help models better understand the underlying patterns of the original series to improve the forecasting accuracy of multivariate time series.However,the decomposition kernel of previous decomposition-based models is fixed,and these models have not considered the differences in frequency fluctuations between components.These problems make it difficult to analyze the intricate temporal variations of real-world time series.In this paper,we propose a series decomposition-based Mamba model,DecMamba,to obtain the intricate temporal dependencies and the dependencies among different variables of multivariate time series.A variable-level adaptive kernel combination search module is designed to interact with information on different trends and periods between variables.Two backbone structures are proposed to emphasize the differences in frequency fluctuations of seasonal and trend components.Mamba with superior performance is used instead of a Transformer in backbone structures to capture the dependencies among different variables.A new embedding block is designed to capture the temporal features better,especially for the high-frequency seasonal component whose semantic information is difficult to acquire.A gating mechanism is introduced to the decoder in the seasonal backbone to improve the prediction accuracy.A comparison with ten state-of-the-art models on seven real-world datasets demonstrates that DecMamba can better model the temporal dependencies and the dependencies among different variables,guaranteeing better prediction performance for multivariate time series.
基金supported by National Natural Science Foundations of China(nos.12271326,62102304,61806120,61502290,61672334,61673251)China Postdoctoral Science Foundation(no.2015M582606)+2 种基金Industrial Research Project of Science and Technology in Shaanxi Province(nos.2015GY016,2017JQ6063)Fundamental Research Fund for the Central Universities(no.GK202003071)Natural Science Basic Research Plan in Shaanxi Province of China(no.2022JM-354).
文摘The multi-objective particle swarm optimization algorithm(MOPSO)is widely used to solve multi-objective optimization problems.In the article,amulti-objective particle swarm optimization algorithmbased on decomposition and multi-selection strategy is proposed to improve the search efficiency.First,two update strategies based on decomposition are used to update the evolving population and external archive,respectively.Second,a multiselection strategy is designed.The first strategy is for the subspace without a non-dominated solution.Among the neighbor particles,the particle with the smallest penalty-based boundary intersection value is selected as the global optimal solution and the particle far away fromthe search particle and the global optimal solution is selected as the personal optimal solution to enhance global search.The second strategy is for the subspace with a non-dominated solution.In the neighbor particles,two particles are randomly selected,one as the global optimal solution and the other as the personal optimal solution,to enhance local search.The third strategy is for Pareto optimal front(PF)discontinuity,which is identified by the cumulative number of iterations of the subspace without non-dominated solutions.In the subsequent iteration,a new probability distribution is used to select from the remaining subspaces to search.Third,an adaptive inertia weight update strategy based on the dominated degree is designed to further improve the search efficiency.Finally,the proposed algorithmis compared with fivemulti-objective particle swarm optimization algorithms and five multi-objective evolutionary algorithms on 22 test problems.The results show that the proposed algorithm has better performance.
基金Supported by the National Key R&D Program of China(2023YFD2101001)National Natural Science Foundation of China(32202144,61807001)。
文摘To address the issues of peak overlap caused by complex matrices in agricultural product terahertz(THz)spectral signals and the dynamic,nonlinear interference induced by environmental and system noise,this study explores the feasibility of adaptive-signal-decomposition-based denoising methods to improve THz spectral quality.THz time-domain spectroscopy(THz-TDS)combined with an attenuated total reflection(ATR)accessory was used to collect THz absorbance spectra from 48 peanut samples.Taking the quantitative prediction model of peanut moisture content based on THz-ATR as an example,wavelet transform(WT),empirical mode decomposition(EMD),local mean decomposition(LMD),and its improved methods-segmented local mean decomposition(SLMD)and piecewise mirror extension local mean decomposition(PME-LMD)-were employed for spectral denoising.The applicability of different denoising methods was evaluated using a support vector regression(SVR)model.Experimental results show that the peanut moisture content prediction model constructed after PME-LMD denoising achieved the best performance,with a root mean square error(RMSE),coefficient of determination(R^(2)),and mean absolute percentage error(MAPE)of 0.010,0.912,and 0.040,respectively.Compared with traditional methods,PME-LMD significantly improved spectral quality and model prediction performance.The PME-LMD denoising strategy proposed in this study effectively suppresses non-uniform noise interference in THz spectral signals,providing an efficient and accurate preprocessing method for THz spectral analysis of agricultural products.This research provides theoretical support and technical guidance for the application of THz technology for detecting agricultural product quality.
文摘In this paper,we prove that L(K_(x,y))(λ),theλ-fold line graph of the complete bipartite graph Ka,y,has a C_(6)-decomposition if and only if ry≥6,λxy(c+y-2)=0(mod 12)and(x+y)=0(mod 2),where x,y are nonnegative integers and(x,y)≠(2,4)or(2,5).
基金supported by the National Natural Science Foundation of China(22178295,21706225)Natural Science Foundation of Hunan Province(2025JJ50085)Hunan Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization.
文摘The new technology of direct decomposition of H_(2)S into high value-added H_(2) and S,as an alternative to the Claus process in industry,is an ideal route that can not only deal with toxic and abundant H_(2)S waste gas but also recover clean energy H_(2),which has significant socio-economic and ecological advantages.However,the highly effective decomposition of H_(2)S at low temperatures is still a great challenge,because of the stringent thermodynamic equilibrium constraints(only 20% even at high temperature of 1010℃).Conventional microwave catalysts exhibit unsatisfactory performance at low temperatures(below 600℃).Herein,Mo_(2)C@CeO_(2) catalysts with a core-shell structure were successfully developed for robust microwave catalytic decomposition of H_(2)S at low temperatures.Two carbon precursors,para-phenylenediamine(Mo_(2)C-p)and meta-phenylenediamine(Mo_(2)C-m),were employed to tailor Mo_(2)C configurations.Remarkably,the H_(2)S conversion of Mo_(2)C-p@CeO_(2) catalyst at a low temperature of 550℃ is as high as 92.1%,which is much higher than the H_(2)S equilibrium conversion under the conventional thermal conditions(2.6% at 550℃).To our knowledge,this represents the most active catalyst for microwave catalytic decomposition of H_(2)S at low temperature of 550℃.Notably,Mo_(2)C-p demonstrated superior intrinsic activity(84%)compared to Mo_(2)C-m(6.4%),with XPS analysis revealing that its enhanced performance stems from a higher concentration of Mo_(2+)active sites.This work presents a substitute approach for the efficient utilization of H_(2)S waste gas and opens up a novel avenue for the rational design of microwave catalysts for microwave catalytic reaction at low-temperature.
基金supported by the National Key Research and Development Program of China(No.2022YFD1700102)the National Natural Science Foundation of China(No.U20A20108)the Hunan Provincial Natural Science Foundation of China(No.2021JJ30357).
文摘Organic matter(OM)derived from the decomposition of crop residues plays a key role as a sorbent for cadmium(Cd)immobilization.Few studies have explored the straw decomposition processes with the presence of minerals,and the effect of newly generated organomineral complexes on heavy metal adsorption.In this study,we investigated the variations in structure and composition during the rice straw decomposition with or without minerals(goethite and kaolinite),as well as the adsorption behavior and mechanisms by which straw decomposition affects Cd immobilization.The degree of humification of extracted straw organic matter was assessed using excitation-emission matrix(EEM)fluorescence and Ultraviolet-visible spectroscopy(UV-vis),while employing FTIR spectroscopy and XPS to characterize the adsorption mechanisms.The spectra analysis revealed the enrichment of highly aromatic and hydrophobic components,indicating that the degree of straw decomposition and humification were further intensified during incubation.Additionally,the existence of goethite(SG)accelerated the humification of OM.Sorption experiments revealed that the straw humification increased Cd adsorption capacity.Notably,SG exhibited significantly higher adsorption performance compared to the organic matter without minerals(RS)and the existence of kaolinite(SK).Further analysis using FT-IR spectroscopy and XPS verified that the primarymechanisms involved in Cd immobilization were complexion with—OH and—COOH,as well as the formation of Cd-πbinds with aromatic C=C on the surface of solid OMs.These findings will facilitate understanding the interactions of the rice straw decomposing with soil minerals and its remediation effect on Cd-contaminated farmland.
文摘The deployment of non-precious metal catalysts for the production of COx-free hydrogen via the ammonia decomposition reaction(ADR)presents a promising yet great challenge.In the present study,two crystal structures of α-MoC and β-Mo_(2)C catalysts with different Mo/C ratios were synthesized,and their ammonia decomposition performance as well as structural evolution in ADR was investigated.The β-Mo_(2)C catalyst,characterized by a higher Mo/C ratio,demonstrated a remarkable turnover frequency of 1.3 s^(-1),which is over tenfold higher than that ofα-MoC(0.1 s^(-1)).An increase in the Mo/C ratio of molybdenum carbide revealed a direct correlation between the surface Mo/C ratio and the hydrogen yield.The transient response surface reaction indicated that the combination of N*and N*derived from NH_(3) dissociation represents the rate-determining step in the ADR,andβ-Mo2C exhibited exceptional proficiency in facilitating this pivotal step.Concurrently,the accumulation of N*species on the carbide surface could induce the phase transition of molybdenum carbide to nitride,which follows a topological transformation.It is discovered that such phase evolution was affected by the Mo-C surface and reaction temperature simultaneously.When the kinetics of combination of N*was accelerated by rising temperatures and its accumulation on the carbide surface was mitigated,β-Mo_(2)C maintained its carbide phase,preventing nitridation during the ADR at 810℃.Our results contribute to an in-depth understanding of the molybdenum carbides’catalytic properties in ADR and highlight the nature of the carbide-nitride phase transition in the reaction.
基金supported by the Ramanujan Fellowship from the Science and Engineering Research Board,Government of India(Grant No.RJF/2022/000115).
文摘This paper introduces dynamic mode decomposition(DMD)as a novel approach to model the breakage kinetics of particulate systems.DMD provides a data-driven framework to identify a best-fit linear dynamics model from a sequence of system measurement snapshots,bypassing the nontrivial task of determining appropriate mathemat-ical forms for the breakage kernel functions.A key innovation of our method is the instilling of physics-informed constraints into the DMD eigenmodes and eigenvalues,ensuring they adhere to the physical structure of particle breakage processes even under sparse measurement data.The integration of eigen-constraints is computationally aided by a zeroth-order global optimizer for solving the nonlinear,nonconvex optimization problem that elicits system dynamics from data.Our method is evaluated against the state-of-the-art optimized DMD algorithm using both generated data and real-world data of a batch grinding mill,showcasing over an order of magnitude lower prediction errors in data reconstruction and forecasting.
基金supported by the National Natural Science Foundation of China(No.U20A2047)the Key Research and Development Project for Tibet Autonomous Region(No.XZ202201ZY0003N)+2 种基金the National Key Research and Development Program of China(No.2022YFD1901402)the Lasa Science and Technology Bureau(No.LSKJ202206)the Foundation of Graduate Research and Innovation in Chongqing(No.CYB22127).
文摘The land application of livestock manure has been widely acknowledged as a beneficial approach for nutrient recycling and environmental protection.However,the impact of residual antibiotics,a common contaminant of manure,on the degradation of organic compounds and nutrient release in Eutric Regosol is not well understood.Here,we studied,how oxytetracycline(OTC)and ciprofloxacin(CIP)affect the decomposition,microbial community structure,extracellular enzyme activities and nutrient release from cattle and pig manure using litterbag incubation experiments.Results showed that OTC and CIP greatly inhibited livestock manure decomposition,causing a decreased rate of carbon(28%-87%),nitrogen(15%-44%)and phosphorus(26%-43%)release.The relative abundance of gramnegative(G-)bacteria was reduced by 4.0%-13%while fungi increased by 7.0%-71%during a 28-day incubation period.Co-occurrence network analysis showed that antibiotic exposure disrupted microbial interactions,particularly among G-bacteria,G+bacteria,and actinomycetes.These changes in microbial community structure and function resulted in decreased activity of urease,β-1,4-N-acetyl-glucosaminidase,alkaline protease,chitinase,and catalase,causing reduced decomposition and nutrient release in cattle and pig ma-nures.These findings advance our understanding of decomposition and nutrient recycling from manure-contaminated antibiotics,which will help facilitate sustainable agricultural production and soil carbon sequestration.
基金supported by the National Natural Science Foundation of China (Nos.21876019 and 22276022)the National Key Research and Development Program of China (No.2019YFC1903903).
文摘Monolithic catalysts with excellent O_(3)catalytic decomposition performance were prepared by in situ loading of Co-doped KMn_(8)O_(16)on the surface of nickel foam.The triple-layer structure with Co-doped KMn_(8)O_(16)/Ni6MnO_(8)/Ni foam was grown spontaneously on the surface of nickel foam by tuning the molar ratio of KMnO_(4)to Co(NO_(3))_(2)·6H_(2)O precursors.Importantly,the formed Ni6MnO_(8)structure between KMn_(8)O_(16)and nickel foam during in situ synthesis process effectively protected nickel foam from further etching,which significantly enhanced the reaction stability of catalyst.The optimum amount of Co doping in KMn_(8)O_(16)was available when the molar ratio of Mn to Co species in the precursor solution was 2:1.And the Mn2Co1 catalyst had abundant oxygen vacancies and excellent hydrophobicity,thus creating outstanding O_(3)decomposition activity.The O_(3)conversion under dry conditions and relative humidity of 65%,90%over a period of 5 hr was 100%,94%and 80%with the space velocity of 28,000 hr^(−1),respectively.The in situ constructed Co-doped KMn_(8)O_(16)/Ni foam catalyst showed the advantages of low price and gradual applicability of the preparation process,which provided an opportunity for the design of monolithic catalyst for O_(3)catalytic decomposition.
基金supported by the National Key R&D Program of China(2022YFB4300700)National Natural Science Foundation of China(22008230,22208021,21925803)+6 种基金China Postdoctoral Science Foundation funded project(2020M670807)the Doctoral Scientific Research Foundation of Liaoning Province(2022-BS-014)the Innovation Research Fund Project of Dalian Institute of Chemical Physics(DICP I202224)CAS Specific Research Assistant Funding Programthe fund of the State Key Laboratory of Catalysis in Dalian Institute of Chemical Physics(N-22-08)the Youth Innovation Promotion Association CAS(Y2022061)the Young Topnotch Talents of Liaoning Province(XLYC2203108)。
文摘The catalytic performance of supported metal catalysts is highly dependent on the interfacial contact between the metal centers and support materials,which could dynamically adapt to the chemical environment in the reactions.Herein,the well-known Ru/TiO_(x)interface of the Ru/TiO_(2)catalyst is shown to be transformed into Ru/TiO_(x)N_(y)during the NH_(3)decomposition,which is derived from the nitridation of the support by N^(*)species.Through a series of characterizations and density functional theory(DFT)calculations,it is found that such a nitrogenous interface primarily blocks the cleavage of N-H bonds with a higher energy barrier,leading to the deactivation of Ru/TiO_(2)in NH_(3)decomposition.Nevertheless,the Ru/TiO_(x)interface can be easily restored by oxidation and a subsequent H2 reduction,contributing to the recovery of the catalytic activity toward NH_(3)decomposition.Our study provides a new insight into the deactivation mechanism of Ru/TiO_(2)in NH_(3)decomposition and highlights the significance of the dynamic evolution of the metal-support interfaces in the reactions.
