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
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
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
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
The development of the three-component catalytic system for constructing isoindolinones from simple feedstocks is both significant and challenging.In this study,a unique tartrate-linked dimeric samarium-antimonotungst...The development of the three-component catalytic system for constructing isoindolinones from simple feedstocks is both significant and challenging.In this study,a unique tartrate-linked dimeric samarium-antimonotungstate[Sm_(2)(H_(2)O)_(6)(tar)(Sb_(2)W_(21)O_(72))]_(2)^(20-)(Sm_(4)tar_(2),H_(4)tar=tartaric acid)was synthesized via a one-step method at room temperature using an acetate buffer solution.The dimeric polyanion of Sm4tar2shows a centrosymmetric structure with a parallelogram-like arrangement and comprises two enantiomeric{Sm_(2)(H_(2)O)_(6)(Sb_(2)W_(21)O_(72))}moieties connected by two enantiomeric tar ligands.Sm_(4)tar_(2)demonstrates efficient catalytic activity in the three-component reaction involving 2-acylbenzoic acids,primary amines,and phosphine oxides to form 3,3-disubstituted isoindolinones.The advantages of this catalytic system include simple feedstocks,green and reusable catalyst,and operational simplicity with water as the sole by-product.This finding enables an effective molecular fragment assembly strategy for synthesizing isoindolinone drug precursor skeletons.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
Introducing PT-symmetric generalized Scarf-Ⅱpotentials into the three-coupled nonlinear Gross-Pitaevskii equations offers a new way to seek stable soliton states in quasi-onedimensional spin-1 Bose-Einstein condensat...Introducing PT-symmetric generalized Scarf-Ⅱpotentials into the three-coupled nonlinear Gross-Pitaevskii equations offers a new way to seek stable soliton states in quasi-onedimensional spin-1 Bose-Einstein condensates.In scenarios where the spin-independent parameter c_(0)and the spin-dependent parameter c_(2)vary,we use both analytical and numerical methods to investigate the three-coupled nonlinear Gross-Pitaevskii equations with PT-symmetric generalized Scarf-Ⅱpotentials.We obtain analytical soliton states and find that simply modulating c_(2)may change the analytical soliton states from unstable to stable.Additionally,we obtain numerically stable double-hump soliton states propagating in the form of periodic oscillations,exhibiting distinct behavior in energy exchange.For further investigation,we discuss the interaction of numerical double-hump solitons with Gaussian solitons and observe the transfer of energy among the three components.These findings may contribute to a deeper understanding of solitons in Bose-Einstein condensates with PT-symmetric potentials and may hold significance for both theoretical understanding and experimental design in related physics experiments.展开更多
We presented the preparation and analysis of La_(1-x)K_(x)CoO_(3)(x=0.1-0.4)catalysts,supported on microwave-absorbing ceramic carriers,using the sol-gel method.We systematically investigated the effects of various re...We presented the preparation and analysis of La_(1-x)K_(x)CoO_(3)(x=0.1-0.4)catalysts,supported on microwave-absorbing ceramic carriers,using the sol-gel method.We systematically investigated the effects of various reaction conditions under microwave irradiation(0-50 W).These conditions included reaction temperatures(300-600℃),oxygen concentrations(0-6%),and varying K^(+)doping levels on the catalysts'activity.The crystalline phase,microstructure,and the catalytic activity of the catalyst were analyzed by XRD,TEM,H_2-TPR,and O_(2)-TPD.The experimental results reveal that La_(1-x)K_(x)CoO_(3)(x=0.1-0.4)catalysts consistently form homogeneous perovskite nanoparticles across different doping levels.The NO decomposition efficiency on these catalysts initially increases and then decreases with variations in doping amount,temperature,and microwave power.Additionally,an increase in oxygen concentration positively influences NO conversion rates.The optimal performance is observed with La_(0.7)K_(0.3)CoO_(3)catalyst under conditions of x=0.3,400℃,10 W microwave power,and 4%oxygen concentration,achieving a peak NO conversion rate of La_(0.7)K_(0.3)CoO_(3)catalyst is 93.1%.展开更多
As an independent thermodynamic parameter,pressure significantly influences interatomic distances,leading to an increase in material density.In this work,we employ the CALYPSO structure search and density functional t...As an independent thermodynamic parameter,pressure significantly influences interatomic distances,leading to an increase in material density.In this work,we employ the CALYPSO structure search and density functional theory calculations to explore the structural phase transitions and electronic properties of calcium-sulfur compounds(Ca_(x)S_(1-x),where x=1/4,1/3,1/2,2/3,3/4,4/5)under 0-1200 GPa.The calculated formation enthalpies suggest that Ca_(x)S_(1-x)compounds undergo multiple phase transitions and eventually decompose into elemental Ca and S,challenging the traditional view that pressure stabilizes and densifies compounds.The analysis of formation enthalpy indicates that an increase in pressure leads to a rise in internal energy and the PV term,resulting in thermodynamic instability.Bader charge analysis reveals that this phenomenon is attributed to a decrease in charge transfer under high pressure.The activation of Ca-3d orbitals is significantly enhanced under pressure,leading to competition with Ca-4s orbitals and S-3p orbitals.This may cause the formation enthalpy minimum on the convex hull to shift sequentially from CaS to CaS_(3),then to Ca_(3)S and Ca_(2)S,and finally back to CaS.These findings provide critical insights into the behavior of alkaline-earth metal sulfides under high pressure,with implications for the synthesis and application of novel materials under extreme conditions and for understanding element distribution in planetary interiors.展开更多
Formalizing complex processes and phenomena of a real-world problem may require a large number of variables and constraints,resulting in what is termed a large-scale optimization problem.Nowadays,such large-scale opti...Formalizing complex processes and phenomena of a real-world problem may require a large number of variables and constraints,resulting in what is termed a large-scale optimization problem.Nowadays,such large-scale optimization problems are solved using computing machines,leading to an enormous computational time being required,which may delay deriving timely solutions.Decomposition methods,which partition a large-scale optimization problem into lower-dimensional subproblems,represent a key approach to addressing time-efficiency issues.There has been significant progress in both applied mathematics and emerging artificial intelligence approaches on this front.This work aims at providing an overview of the decomposition methods from both the mathematics and computer science points of view.We also remark on the state-of-the-art developments and recent applications of the decomposition methods,and discuss the future research and development perspectives.展开更多
Heterogeneous graphs generally refer to graphs with different types of nodes and edges.A common approach for extracting useful information from heterogeneous graphs is to use meta-graphs,which can be seen as a special...Heterogeneous graphs generally refer to graphs with different types of nodes and edges.A common approach for extracting useful information from heterogeneous graphs is to use meta-graphs,which can be seen as a special kind of directed acyclic graph with same node and edge types as the heterogeneous graph.However,how to design proper metagraphs is challenging.Recently,there have been many works on learning suitable metagraphs from a heterogeneous graph.Existing methods generally introduce continuous weights for edges that are independent of each other,which ignores the topological structures of meta-graphs and can be ineffective.To address this issue,the authors propose a new viewpoint from tensor on learning meta-graphs.Such a viewpoint not only helps interpret the limitation of existing works by CANDECOMP/PARAFAC(CP)decomposition,but also inspires us to propose a topology-aware tensor decomposition,called TENSUS,that reflects the structure of DAGs.The proposed topology-aware tensor decomposition is easy to use and simple to implement,and it can be taken as a plug-in part to upgrade many existing works,including node classification and recommendation on heterogeneous graphs.Experimental results on different tasks demonstrate that the proposed method can significantly improve the state-of-the-arts for all these tasks.展开更多
When plants respond to drought stress,dynamic cellular changes occur,accompanied by alterations in gene expression,which often act through trans-regulation.However,the detection of trans-acting genetic variants and ne...When plants respond to drought stress,dynamic cellular changes occur,accompanied by alterations in gene expression,which often act through trans-regulation.However,the detection of trans-acting genetic variants and networks of genes is challenged by the large number of genes and markers.Using a tensor decomposition method,we identify trans-acting expression quantitative trait loci(trans-eQTLs)linked to gene modules,rather than individual genes,which were associated with maize drought response.Module-to-trait association analysis demonstrates that half of the modules are relevant to drought-related traits.Genome-wide association studies of the expression patterns of each module identify 286 trans-eQTLs linked to drought-responsive modules,the majority of which cannot be detected based on individual gene expression.Notably,the trans-eQTLs located in the regions selected during maize improvement tend towards relatively strong selection.We further prioritize the genes that affect the transcriptional regulation of multiple genes in trans,as exemplified by two transcription factor genes.Our analyses highlight that multidimensional reduction could facilitate the identification of trans-acting variations in gene expression in response to dynamic environments and serve as a promising technique for high-order data processing in future crop breeding.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
High entropy alloys(HEAs)constituted of single solid solution phase,but remains chemical inhomogeneity in nature due to its multi-principal composition.Currently,existence of nanoscale spinodal decomposition(SD)phase ...High entropy alloys(HEAs)constituted of single solid solution phase,but remains chemical inhomogeneity in nature due to its multi-principal composition.Currently,existence of nanoscale spinodal decomposition(SD)phase in matrix was found to have significant impact on the properties of HEAs.Nevertheless,the morphology evolution and the kinetics of SD is not clear,which hinders in-depth understanding of the structure-property relationship.In this study,we examine the spinodal structures in(FeCoCrNi)85(AlCu)15 HEAs at different states using in-situ small-angle neutron scattering(SANS),in conjunction with transmission electron microscopy technique.The result demonstrates that SD occurred when aging the HEA samples at temperatures ranging from 500 to 800℃,which leads to the phase constitution of NiAlCu-rich and FeCoCr-rich spinodal phases,L1_(2)ordered phases,and FCC matrix.The characteristic wavelength of SD(λ_(SD))grows from 5.31 to 51.26 nm when aging temperature rises from 500 to 800℃,which explains the enhancement of the alloy’s microhardness.The SD kinetics was unraveled by fitting the time-dependentλ_(SD)through in-situ SANS measurement at 700℃.During isothermal treatment at 700℃,theλ_(SD)increases from 10.42 to 17.43 nm with prolonged time,and SD is in the late stage from the exponential trend of theλ_(SD)over time.Moreover,comparing with aging temperature,the aging time has a relatively minor impact on the coarsening of SD.展开更多
Exploring the factors driving the decoupling of China’s sulfur dioxide(SO_(2))emissions from economic growth(DEI)is crucial for achieving sustainable development.By analyzing the decoupling indicators and driving fac...Exploring the factors driving the decoupling of China’s sulfur dioxide(SO_(2))emissions from economic growth(DEI)is crucial for achieving sustainable development.By analyzing the decoupling indicators and driving factors at both the generation and treatment stages of SO_(2),more effective targeted mitigation strategies can be developed.We employ the Tapio decoupling model and propose a two-stage method to examine the decoupling issues related to SO_(2).Our findings indicate that:①DEI shows a steady and significant improvement,with SO_(2)emission intensity identified as the primary driver.②for the decoupling of economic growth and SO_(2)generation,energy scale serves as the largest stimulator,while the effect of energy intensity changes from negative to positive,and pollution intensity is first positive and then negative.③For the decoupling of SO_(2)generation and SO_(2)removal,treatment efficiency leads as the largest promoter,followed by treatment intensity.Based on these results,this study recommends that China focuses more on enhancing clean energy utilization and the effectiveness of treatment processes.展开更多
The Mountain Pass mine is recognized as one of the world's primary sources of rare earth minerals.These rare earth minerals mainly consist of bastnaesite and a small amount of monazite phosphate,which cannot be de...The Mountain Pass mine is recognized as one of the world's primary sources of rare earth minerals.These rare earth minerals mainly consist of bastnaesite and a small amount of monazite phosphate,which cannot be decomposed and recovered through conventional oxidative roasting and hydrochloric acid leaching process.An efficient,clean,and economical process called the"combined method"was proposed for the utilization of the Mountain Pass mine to extract rare earths from Mountain Pass rare earth concentrate(MPREC).The main steps of this process include weak oxidation atmosphere roasting,step leaching of hydrochloric acid,solid-liquid separation,the monazite slag with sulfuric acid roasting water leaching,etc.In this paper,the roasting process of MPREC under a weak oxidation atmosphere was investigated.The study examines the thermal decomposition kinetics,phase transition process,and leaching behavior of MPREC in air/CO_(2)atmosphere.Results show that,the activation energy(Ea)for MPREC thermal decomposition in air and CO_(2)atmosphere are 146 and 320 kJ/mol,respectively.At temperature above 500℃in air or above 700℃in CO_(2)atmosphere,REOF are generated from bastnaesite through an in-situ reaction with CaO,which is decomposed from CaCO_(3),to form CaF_(2)and rare earth oxide(REO).Thus,F is regulated into solid phase.In an oxidizing atmosphere,the thermal decomposition of bastnaesite is accompanied by the rapid oxidation of Ce(Ⅲ).In co ntrast,the oxidation of Ce(Ⅲ)in a CO_(2)atmosphere is significantly inhibited.At 700℃,the oxidation rate of Ce in air is 74.09%,while in a CO_(2)atmosphere,it is only 33.83%.The hydrochloric acid leaching experiment shows that,the leaching rate of rare earth after roasting at 600℃under an air atmosphere reaches to 82.9%,and it reaches 87%after roasting at 800℃under a CO_(2)atmosphere.The reduction of Ce oxidation in a weak oxidizing atmosphere significantly improves the leaching rate of Ce.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 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
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
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 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 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 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financially supported by the National Natural Science Foundation of China(No.22301033)Jiangxi Provincial Natural Science Foundation(No.20232ACB213005 and 20212BAB213001)。
文摘The development of the three-component catalytic system for constructing isoindolinones from simple feedstocks is both significant and challenging.In this study,a unique tartrate-linked dimeric samarium-antimonotungstate[Sm_(2)(H_(2)O)_(6)(tar)(Sb_(2)W_(21)O_(72))]_(2)^(20-)(Sm_(4)tar_(2),H_(4)tar=tartaric acid)was synthesized via a one-step method at room temperature using an acetate buffer solution.The dimeric polyanion of Sm4tar2shows a centrosymmetric structure with a parallelogram-like arrangement and comprises two enantiomeric{Sm_(2)(H_(2)O)_(6)(Sb_(2)W_(21)O_(72))}moieties connected by two enantiomeric tar ligands.Sm_(4)tar_(2)demonstrates efficient catalytic activity in the three-component reaction involving 2-acylbenzoic acids,primary amines,and phosphine oxides to form 3,3-disubstituted isoindolinones.The advantages of this catalytic system include simple feedstocks,green and reusable catalyst,and operational simplicity with water as the sole by-product.This finding enables an effective molecular fragment assembly strategy for synthesizing isoindolinone drug precursor skeletons.
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 by NSFC under Grant No.12272403Beijing Training Program of Innovation under Grant No.S202410019024。
文摘Introducing PT-symmetric generalized Scarf-Ⅱpotentials into the three-coupled nonlinear Gross-Pitaevskii equations offers a new way to seek stable soliton states in quasi-onedimensional spin-1 Bose-Einstein condensates.In scenarios where the spin-independent parameter c_(0)and the spin-dependent parameter c_(2)vary,we use both analytical and numerical methods to investigate the three-coupled nonlinear Gross-Pitaevskii equations with PT-symmetric generalized Scarf-Ⅱpotentials.We obtain analytical soliton states and find that simply modulating c_(2)may change the analytical soliton states from unstable to stable.Additionally,we obtain numerically stable double-hump soliton states propagating in the form of periodic oscillations,exhibiting distinct behavior in energy exchange.For further investigation,we discuss the interaction of numerical double-hump solitons with Gaussian solitons and observe the transfer of energy among the three components.These findings may contribute to a deeper understanding of solitons in Bose-Einstein condensates with PT-symmetric potentials and may hold significance for both theoretical understanding and experimental design in related physics experiments.
文摘We presented the preparation and analysis of La_(1-x)K_(x)CoO_(3)(x=0.1-0.4)catalysts,supported on microwave-absorbing ceramic carriers,using the sol-gel method.We systematically investigated the effects of various reaction conditions under microwave irradiation(0-50 W).These conditions included reaction temperatures(300-600℃),oxygen concentrations(0-6%),and varying K^(+)doping levels on the catalysts'activity.The crystalline phase,microstructure,and the catalytic activity of the catalyst were analyzed by XRD,TEM,H_2-TPR,and O_(2)-TPD.The experimental results reveal that La_(1-x)K_(x)CoO_(3)(x=0.1-0.4)catalysts consistently form homogeneous perovskite nanoparticles across different doping levels.The NO decomposition efficiency on these catalysts initially increases and then decreases with variations in doping amount,temperature,and microwave power.Additionally,an increase in oxygen concentration positively influences NO conversion rates.The optimal performance is observed with La_(0.7)K_(0.3)CoO_(3)catalyst under conditions of x=0.3,400℃,10 W microwave power,and 4%oxygen concentration,achieving a peak NO conversion rate of La_(0.7)K_(0.3)CoO_(3)catalyst is 93.1%.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11974154 and 12304278)the Taishan Scholars Special Funding for Construction Projects(Grant No.tstp20230622)+1 种基金the Natural Science Foundation of Shandong Province(Grant Nos.ZR2022MA004,ZR2023QA127,and ZR2024QA121)the Special Foundation of Yantai for Leading Talents above Provincial Level.
文摘As an independent thermodynamic parameter,pressure significantly influences interatomic distances,leading to an increase in material density.In this work,we employ the CALYPSO structure search and density functional theory calculations to explore the structural phase transitions and electronic properties of calcium-sulfur compounds(Ca_(x)S_(1-x),where x=1/4,1/3,1/2,2/3,3/4,4/5)under 0-1200 GPa.The calculated formation enthalpies suggest that Ca_(x)S_(1-x)compounds undergo multiple phase transitions and eventually decompose into elemental Ca and S,challenging the traditional view that pressure stabilizes and densifies compounds.The analysis of formation enthalpy indicates that an increase in pressure leads to a rise in internal energy and the PV term,resulting in thermodynamic instability.Bader charge analysis reveals that this phenomenon is attributed to a decrease in charge transfer under high pressure.The activation of Ca-3d orbitals is significantly enhanced under pressure,leading to competition with Ca-4s orbitals and S-3p orbitals.This may cause the formation enthalpy minimum on the convex hull to shift sequentially from CaS to CaS_(3),then to Ca_(3)S and Ca_(2)S,and finally back to CaS.These findings provide critical insights into the behavior of alkaline-earth metal sulfides under high pressure,with implications for the synthesis and application of novel materials under extreme conditions and for understanding element distribution in planetary interiors.
基金The Australian Research Council(DP200101197,DP230101107).
文摘Formalizing complex processes and phenomena of a real-world problem may require a large number of variables and constraints,resulting in what is termed a large-scale optimization problem.Nowadays,such large-scale optimization problems are solved using computing machines,leading to an enormous computational time being required,which may delay deriving timely solutions.Decomposition methods,which partition a large-scale optimization problem into lower-dimensional subproblems,represent a key approach to addressing time-efficiency issues.There has been significant progress in both applied mathematics and emerging artificial intelligence approaches on this front.This work aims at providing an overview of the decomposition methods from both the mathematics and computer science points of view.We also remark on the state-of-the-art developments and recent applications of the decomposition methods,and discuss the future research and development perspectives.
基金National Key Research and Development Program of China,Grant/Award Number:2023YFB2903904。
文摘Heterogeneous graphs generally refer to graphs with different types of nodes and edges.A common approach for extracting useful information from heterogeneous graphs is to use meta-graphs,which can be seen as a special kind of directed acyclic graph with same node and edge types as the heterogeneous graph.However,how to design proper metagraphs is challenging.Recently,there have been many works on learning suitable metagraphs from a heterogeneous graph.Existing methods generally introduce continuous weights for edges that are independent of each other,which ignores the topological structures of meta-graphs and can be ineffective.To address this issue,the authors propose a new viewpoint from tensor on learning meta-graphs.Such a viewpoint not only helps interpret the limitation of existing works by CANDECOMP/PARAFAC(CP)decomposition,but also inspires us to propose a topology-aware tensor decomposition,called TENSUS,that reflects the structure of DAGs.The proposed topology-aware tensor decomposition is easy to use and simple to implement,and it can be taken as a plug-in part to upgrade many existing works,including node classification and recommendation on heterogeneous graphs.Experimental results on different tasks demonstrate that the proposed method can significantly improve the state-of-the-arts for all these tasks.
基金supported by the Biological Breeding-National Science and Technology Major Project(2023ZD04076)the Guangxi Key Research and Development Projects of China(GuikeAB21238004)the Agricultural Science and Technology Innovation Program.
文摘When plants respond to drought stress,dynamic cellular changes occur,accompanied by alterations in gene expression,which often act through trans-regulation.However,the detection of trans-acting genetic variants and networks of genes is challenged by the large number of genes and markers.Using a tensor decomposition method,we identify trans-acting expression quantitative trait loci(trans-eQTLs)linked to gene modules,rather than individual genes,which were associated with maize drought response.Module-to-trait association analysis demonstrates that half of the modules are relevant to drought-related traits.Genome-wide association studies of the expression patterns of each module identify 286 trans-eQTLs linked to drought-responsive modules,the majority of which cannot be detected based on individual gene expression.Notably,the trans-eQTLs located in the regions selected during maize improvement tend towards relatively strong selection.We further prioritize the genes that affect the transcriptional regulation of multiple genes in trans,as exemplified by two transcription factor genes.Our analyses highlight that multidimensional reduction could facilitate the identification of trans-acting variations in gene expression in response to dynamic environments and serve as a promising technique for high-order data processing in future crop breeding.
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financially supported by the National Key Research and Development Program of China(Grant No.2021YFA1600701)the Guangdong Basic and Applied Basic Research Foundation,China(Project No.2021B1515140028)the National Natural Science Foundation of China(Grant No.12275154)。
文摘High entropy alloys(HEAs)constituted of single solid solution phase,but remains chemical inhomogeneity in nature due to its multi-principal composition.Currently,existence of nanoscale spinodal decomposition(SD)phase in matrix was found to have significant impact on the properties of HEAs.Nevertheless,the morphology evolution and the kinetics of SD is not clear,which hinders in-depth understanding of the structure-property relationship.In this study,we examine the spinodal structures in(FeCoCrNi)85(AlCu)15 HEAs at different states using in-situ small-angle neutron scattering(SANS),in conjunction with transmission electron microscopy technique.The result demonstrates that SD occurred when aging the HEA samples at temperatures ranging from 500 to 800℃,which leads to the phase constitution of NiAlCu-rich and FeCoCr-rich spinodal phases,L1_(2)ordered phases,and FCC matrix.The characteristic wavelength of SD(λ_(SD))grows from 5.31 to 51.26 nm when aging temperature rises from 500 to 800℃,which explains the enhancement of the alloy’s microhardness.The SD kinetics was unraveled by fitting the time-dependentλ_(SD)through in-situ SANS measurement at 700℃.During isothermal treatment at 700℃,theλ_(SD)increases from 10.42 to 17.43 nm with prolonged time,and SD is in the late stage from the exponential trend of theλ_(SD)over time.Moreover,comparing with aging temperature,the aging time has a relatively minor impact on the coarsening of SD.
基金the National Natural Science Foundation of China[Grant No.52270183].
文摘Exploring the factors driving the decoupling of China’s sulfur dioxide(SO_(2))emissions from economic growth(DEI)is crucial for achieving sustainable development.By analyzing the decoupling indicators and driving factors at both the generation and treatment stages of SO_(2),more effective targeted mitigation strategies can be developed.We employ the Tapio decoupling model and propose a two-stage method to examine the decoupling issues related to SO_(2).Our findings indicate that:①DEI shows a steady and significant improvement,with SO_(2)emission intensity identified as the primary driver.②for the decoupling of economic growth and SO_(2)generation,energy scale serves as the largest stimulator,while the effect of energy intensity changes from negative to positive,and pollution intensity is first positive and then negative.③For the decoupling of SO_(2)generation and SO_(2)removal,treatment efficiency leads as the largest promoter,followed by treatment intensity.Based on these results,this study recommends that China focuses more on enhancing clean energy utilization and the effectiveness of treatment processes.
基金supported by the National Key Research and Development Program of China(2020YFC1909104)National Natural Science Foundation of China(52274355)Major Science and Technology Project of Inner Mongolia Autonomous Region(2021ZD0016)。
文摘The Mountain Pass mine is recognized as one of the world's primary sources of rare earth minerals.These rare earth minerals mainly consist of bastnaesite and a small amount of monazite phosphate,which cannot be decomposed and recovered through conventional oxidative roasting and hydrochloric acid leaching process.An efficient,clean,and economical process called the"combined method"was proposed for the utilization of the Mountain Pass mine to extract rare earths from Mountain Pass rare earth concentrate(MPREC).The main steps of this process include weak oxidation atmosphere roasting,step leaching of hydrochloric acid,solid-liquid separation,the monazite slag with sulfuric acid roasting water leaching,etc.In this paper,the roasting process of MPREC under a weak oxidation atmosphere was investigated.The study examines the thermal decomposition kinetics,phase transition process,and leaching behavior of MPREC in air/CO_(2)atmosphere.Results show that,the activation energy(Ea)for MPREC thermal decomposition in air and CO_(2)atmosphere are 146 and 320 kJ/mol,respectively.At temperature above 500℃in air or above 700℃in CO_(2)atmosphere,REOF are generated from bastnaesite through an in-situ reaction with CaO,which is decomposed from CaCO_(3),to form CaF_(2)and rare earth oxide(REO).Thus,F is regulated into solid phase.In an oxidizing atmosphere,the thermal decomposition of bastnaesite is accompanied by the rapid oxidation of Ce(Ⅲ).In co ntrast,the oxidation of Ce(Ⅲ)in a CO_(2)atmosphere is significantly inhibited.At 700℃,the oxidation rate of Ce in air is 74.09%,while in a CO_(2)atmosphere,it is only 33.83%.The hydrochloric acid leaching experiment shows that,the leaching rate of rare earth after roasting at 600℃under an air atmosphere reaches to 82.9%,and it reaches 87%after roasting at 800℃under a CO_(2)atmosphere.The reduction of Ce oxidation in a weak oxidizing atmosphere significantly improves the leaching rate of Ce.
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 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.
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.
