Ti750s titanium alloy,a novel high-temperature titanium alloy designed for short-term service at elevated temperatures(700–750℃),has previously lacked comprehensive understanding of its hot processing behavior.In th...Ti750s titanium alloy,a novel high-temperature titanium alloy designed for short-term service at elevated temperatures(700–750℃),has previously lacked comprehensive understanding of its hot processing behavior.In this study,the high-temperature deformation behavior and microstructural evolution of the Ti750s alloy were systematically investigated through thermal simulation compression tests conducted at temperatures ranging from 900 to 1070℃and strain rates between 0.1 and 10 s⁻1.A hot processing map was constructed using the dynamic material model to optimize the hot processing parameters.The results indicated that the optimal processing window was between 1040 and 1070℃with a strain rate of 0.1 s⁻1.Processing within the instability region resulted in localized plastic deformation,manifesting as pronounced shear bands and a highly heterogeneous strain distribution;this region should be avoided during hot deformation.Within theα+βphase safety zone characterized by low power dissipation rates between 0.32 and 0.4,the primary deformation mechanism in this region was dynamic recovery(DRV),where the lamellarαgrains underwent deformation and rotation.Conversely,in theα+βphase safety zone with high-power dissipation rates between 0.45 and 0.52,dynamic spheroidization of theαphase and dynamic recrystallization(DRX)of theβphase occurred concurrently.In theβphase safety zone with low power dissipation rates between 0.32 and 0.51,the primary deformation mechanism consisted of DRV ofβgrains,accompanied by limited DRX.However,in theβphase safety zone with high-power dissipation rates exceeding 0.56,both DRV and DRX ofβgrains took place,resulted in a significant increase in the size and number of recrystallized grains compared to those observed under low power dissipation conditions.展开更多
Precise high-temperature weather forecasts are essential, as heatwaves are increasing in frequency under the ongoing climate change. Land-surface schemes have been demonstrated to be crucial to numerical weather predi...Precise high-temperature weather forecasts are essential, as heatwaves are increasing in frequency under the ongoing climate change. Land-surface schemes have been demonstrated to be crucial to numerical weather predictions.However, few studies have explored the impact of land surface schemes on short-range high-temperature weather forecasts via operational numerical weather prediction models. To evaluate the impact of the soil thermal process on high-temperature weather forecasts, we coupled the soil thermal process of the state-of-the-art Common Land Model(CoLM) with the South China operational numerical weather prediction model(CMA-TRAMS) and compared the coupled model with the original CMA-TRAMS, which incorporated the Simplified Model for land Surface(SMS). Contrast experiments based on two versions of CMA-TRAMS were conducted for the year 2022 when persistent extreme heatwaves were observed in Central-East China. The results are as follows:(1) Short-range high-temperature weather forecasts were sensitive to soil thermal process schemes. The original CMA-TRAMS clearly underestimated the summertime near-surface air temperature(T2m) over almost all areas of China, whereas the CoLM led to a reduction of the negative biases by approximately 0.5°C.(2) The more accurate initial soil temperatures and the deeper soil structure used in the CoLM test contributed to actual predictions of soil heat flux, soil temperature, and T2m. Nevertheless, the SMS test failed to capture upward heat transport from deeper to shallower soil layers at night due to the shallow soil structure and lower accuracy of the bottom and initial soil temperatures.(3) Higher soil temperatures resulted in increased near-surface moisture and cloud cover in the CoLM test, which led to the warmer soil and further mitigated the cold biases of T2m through reduced longwave and shortwave radiation losses at the land surface.展开更多
To investigate the nucleation behavior during the single-phased metallic solidification process,the commercial ultrapure ferritic stainless steels with no(Initial steel)and various melt treatments(R1,MR1,Y2,MY1,and M1...To investigate the nucleation behavior during the single-phased metallic solidification process,the commercial ultrapure ferritic stainless steels with no(Initial steel)and various melt treatments(R1,MR1,Y2,MY1,and M1 steels)were used to carry out the differential scanning colorimetry(DSC)and high-temperature confocal laser scanning microscope(HT-CLSM)experiments.Based on the results of DSC experiments,the equilibrium solidification process as well as the relationship among the critical undercooling degree(△T_(c)^(DSC)),latent heat of fusion/crystallization(△H_(f)/△H_(c)),equiaxed grain ratio(ER),and average grain size(△_(ave)^(ingot))was revealed.ER is increased with the decreasing△T_(c)^(DSC)and increasing△H_(f)/△H_(c);however,△_(ave)^(ingot)is decreased with them.Referring to the results of HT-CLSM experiments,the average sizes of micro-/macrostructures(d_(ave)/D_(ave)/)are decreased with the increasing cooling rate,as well as the difference between and apparent critical undercooling degree(△T_(c)^(CLSM))was revealed.The heterogeneous nucleation of the crystal nuclei occurs only if△T_(c)^(CLSM)>△T_(c)^(DSC).Combining with the interfacial wetting-lattice mismatch heterogeneous nucleation model,the dynamic mechanism of the metallic solidification was revealed.The as-cast grains of the melt-treated samples were obviously refined,owing to the much higher actual heterogeneous nucleation rates(I_(heter.,i))obtained through melt treatments,and the heterogeneous nucleation rates(I_(heter.,ij))for all samples are increased with the cooling rates,firmly confirming that the as-cast grains of each sample could be refined by the increasing cooling rates.展开更多
This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standar...This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standard system was established for comprehensive quality evaluation of HTD.There were obvious changes in the physicochemical properties,enzyme activities,and volatile flavor components at different storage periods,which affected the sensory evaluation of HTD to a certain extent.The results of high-throughput sequencing revealed significant microbial diversity,and showed that the bacterial community changed significantly more than did the fungal community.During the storage process,the dominant bacterial genera were Kroppenstedtia and Thermoascus.The correlation between dominant microorganisms and quality indicators highlighted their role in HTD quality.Lactococcus,Candida,Pichia,Paecilomyces,and protease activity played a crucial role in the formation of isovaleraldehyde.Acidic protease activity had the greatest impact on the microbial community.Moisture promoted isobutyric acid generation.Furthermore,the comprehensive quality evaluation standard system was established by the entropy weight method combined with multi-factor fuzzy mathematics.Consequently,this study provides innovative insights for comprehensive quality evaluation of HTD during storage and establishes a groundwork for scientific and rational storage of HTD and quality control of sauce-flavor Baijiu.展开更多
Traditionally,the construction of stable interphases relies on solvent structures dominated by aggregated anionic structures(AGG/AGG+).Nonetheless,we find that the construction of stable interphases in hightemperature...Traditionally,the construction of stable interphases relies on solvent structures dominated by aggregated anionic structures(AGG/AGG+).Nonetheless,we find that the construction of stable interphases in hightemperature environments is based on contact ion pairs(CIPs)dominated solvation structure here.In detail,in the long-chain phosphate ester-based electrolyte,the spatial site-blocking effect enables the strong solvation co-solvent ether(diethylene glycol dimethyl ether,G2)to exhibit strong ion-dipole interactions,further multicomponent competitive coordination maintaining the CIP,balancing electrode kinetics,and optimizing the high-temperature interphases.High-temperature in-situ Raman spectroscopy monitors the changes in the stable solvent structure during charge/discharge processes for the first time,and time of flight secondary ion mass spectrometry(TOF-SIMS)reveals the stable solid electrolyte interphase(SEI)with full-depth enrichment of the inorganic component.Benefiting from the high-temperature interfacial chemistry-dependent solvent structure,the advanced electrolyte enables stable cycling of 1.6 Ah 18650 batterie at 100-125℃and discharging with high current pulses(~1.83 A)at 150℃,which has rarely been reported so far.In addition,pin-pricking of 18650 batteries at100%state of charge(SoC)without fire or smoke and the moderate thermal runaway temperature(187℃)tested via the accelerating rate calorimetry(ARC)demonstrate the excellent safety of the optimized electrolyte.展开更多
In mass spectrometry, fragments with a mass higher than the original molecular ion provide valuable insights into the molecular structure and can guide the assembly and disassembly processes for chemical synthesis. He...In mass spectrometry, fragments with a mass higher than the original molecular ion provide valuable insights into the molecular structure and can guide the assembly and disassembly processes for chemical synthesis. Here, we report such an example and following up by modifying the solvothermal reaction conditions (temperature and time) it is possible to isolate the high mass species in crystalline form. [Zn_(4)L_(4)Cl_(4)] (Zn_(4)L_(4), L = N-methylbenzimidazole-2-methanolate) has a boat-like Zn_(4)O_(4) core but electrospray ionization mass spectrometry (ESI-MS) of the solution of its crystals shows higher mass peaks of Zn_(5)L_(5), Zn_(5)L_(6) and Zn_(6)L_(6) species. Thus, both disassembly and reassembly are highly probable processes. Consequently, [Zn(HL)_(2)Cl_(2)] (Zn1, L = N-methylbenzimidazole-2-methanolate), [Zn_(4)L_(6)Cl_(2)] (Zn_(4)L_(6), L = N-methylbenzimidazole-2-methanolate) and [Zn_(6)L_(6)Cl_(4)(CH_(3)O)_(2)] (Zn_(6)L_(6), L = N-methylbenzimidazole-2-methanolate) were prepared. The results of multistage ESI-MS of their dissolved crystals led to a proposed mechanism of their formation in the gas phase as follows: [Zn_(3)L_(4)] through [ZnL] → [ZnL(HL)] → [Zn(HL)_(2)] → [Zn_(2)L] → [Zn_(2)L_(2)] → [Zn_(2)L_(3)]. The mechanism was derived in conjunction with Gibbs free energies calculated using DFT of the fragments observed in the ESI-MS of Zn_(4)L_(4), Zn_(4)L_(6) and Zn_(6)L_(6). This work reveals the complex of chemical reactions, involving fragmentation and unexpected combination, under mass spectrometry condition which allows one to synthesize the observed transients, leading to mechanism of formation by correlation of solid-state/solution structural information.展开更多
A PHE (Process Heat Exchanger) is a key component in transferring high-temperature heat generated from a VHTR (Very High Temperature Reactor) to a chemical reaction for the massive production of hydrogen. Last year, a...A PHE (Process Heat Exchanger) is a key component in transferring high-temperature heat generated from a VHTR (Very High Temperature Reactor) to a chemical reaction for the massive production of hydrogen. Last year, a 10 kW class lab-scale PHE prototype made of Hastelloy-X was manufactured at the Korea Atomic Energy Research Institute (KAERI), and a performance test of the PHE prototype is currently underway in a small-scale nitrogen gas loop at KAERI. The PHE prototype is composed of two kinds of flow plates: grooves 1.0 mm in diameter machined into the flow plate for the primary coolant, and waved channels bent into the flow plate for the secondary coolant. Inside the 10 kW class lab-scale PHE prototype, twenty flow plates for the primary and secondary coolants are stacked in turn. In this study, to understand the macroscopic structural behavior of the PHE prototype under the steady-state operating condition of the gas loop, high-temperature structural analyses on the 10 kW class lab-scale PHE prototype were performed for two extreme cases: in the event of contacting the flow plates together, and when not contacting them. The analysis results for the extreme cases were also compared.展开更多
Processes supported by process-aware information systems are subject to continuous and often subtle changes due to evolving operational,organizational,or regulatory factors.These changes,referred to as incremental con...Processes supported by process-aware information systems are subject to continuous and often subtle changes due to evolving operational,organizational,or regulatory factors.These changes,referred to as incremental concept drift,gradually alter the behavior or structure of processes,making their detection and localization a challenging task.Traditional process mining techniques frequently assume process stationarity and are limited in their ability to detect such drift,particularly from a control-flow perspective.The objective of this research is to develop an interpretable and robust framework capable of detecting and localizing incremental concept drift in event logs,with a specific emphasis on the structural evolution of control-flow semantics in processes.We propose DriftXMiner,a control-flow-aware hybrid framework that combines statistical,machine learning,and process model analysis techniques.The approach comprises three key components:(1)Cumulative Drift Scanner that tracks directional statistical deviations to detect early drift signals;(2)a Temporal Clustering and Drift-Aware Forest Ensemble(DAFE)to capture distributional and classification-level changes in process behavior;and(3)Petri net-based process model reconstruction,which enables the precise localization of structural drift using transition deviation metrics and replay fitness scores.Experimental validation on the BPI Challenge 2017 event log demonstrates that DriftXMiner effectively identifies and localizes gradual and incremental process drift over time.The framework achieves a detection accuracy of 92.5%,a localization precision of 90.3%,and an F1-score of 0.91,outperforming competitive baselines such as CUSUM+Histograms and ADWIN+Alpha Miner.Visual analyses further confirm that identified drift points align with transitions in control-flow models and behavioral cluster structures.DriftXMiner offers a novel and interpretable solution for incremental concept drift detection and localization in dynamic,process-aware systems.By integrating statistical signal accumulation,temporal behavior profiling,and structural process mining,the framework enables finegrained drift explanation and supports adaptive process intelligence in evolving environments.Its modular architecture supports extension to streaming data and real-time monitoring contexts.展开更多
The efficient development and utilization of high-phosphorus oolitic hematite is of great strategic significance for the sustainable supply of iron-ore resources in China.In this paper,the mechanism of high-temperatur...The efficient development and utilization of high-phosphorus oolitic hematite is of great strategic significance for the sustainable supply of iron-ore resources in China.In this paper,the mechanism of high-temperature pretreatment for enhancing the effect of iron enrichment and dephosphorization in the magnetization roasting–leaching process was studied by X-ray diffraction(XRD),vibration sample magnetometer(VSM),scanning electron microscopy and energy dispersive spectrometry(SEM–EDS).Compared with the process without high-temperature pretreatment,the iron grade of the magnetic separation concentrate after high-temperature pretreatment had increased by 0.98%,iron recovery rate had increased by 1.33%,and the phosphorus content in the leached residue had decreased by 0.12%.High-temperature pretreatment resulted in the dehydration and decomposition of hydroxyapatite,the dehydration of limonite and the thermal decomposition of siderite,which can produce pores and cracks and weaken the compactness of the ore,improve the magnetization characteristics of roasted ore,and strengthen the iron enrichment and dephosphorization during the magnetization roasting and leaching process.展开更多
To further improve the oxidation-resistance of materials and reduce the cost of grid plates in grate-kiln, a new kind of heat-resistant grid plate was developed. The microstructure of this grid plate with a life more ...To further improve the oxidation-resistance of materials and reduce the cost of grid plates in grate-kiln, a new kind of heat-resistant grid plate was developed. The microstructure of this grid plate with a life more than 18 months was studied by XRD, SEM and EDS techniques. The results show that high hardness, high intensity and good impact property make the new kind of heat-resistant grid plate and its oxide film have a higher resistance to deformation and abrasion at 900-1000℃ Besides, small grain size is beneficial to form a complete protective oxide film. The oxide film composed of SiO2 layer, Cr2O3 layer and Fe2O3 layer is rather thin and bonds closely with the backing. The forming of the chemical stable nickel-rich layer increases the density of Cr2O3 layer.展开更多
This paper introduces techniques in Gaussian process regression model for spatiotemporal data collected from complex systems.This study focuses on extracting local structures and then constructing surrogate models bas...This paper introduces techniques in Gaussian process regression model for spatiotemporal data collected from complex systems.This study focuses on extracting local structures and then constructing surrogate models based on Gaussian process assumptions.The proposed Dynamic Gaussian Process Regression(DGPR)consists of a sequence of local surrogate models related to each other.In DGPR,the time-based spatial clustering is carried out to divide the systems into sub-spatio-temporal parts whose interior has similar variation patterns,where the temporal information is used as the prior information for training the spatial-surrogate model.The DGPR is robust and especially suitable for the loosely coupled model structure,also allowing for parallel computation.The numerical results of the test function show the effectiveness of DGPR.Furthermore,the shock tube problem is successfully approximated under different phenomenon complexity.展开更多
Aiming at the complexity of seismic gestation mechanism and spatial distribution, we hypothesize that the seismic data are composed of background earthquakes and anomaly earthquakes in a certain temporal-spatial scope...Aiming at the complexity of seismic gestation mechanism and spatial distribution, we hypothesize that the seismic data are composed of background earthquakes and anomaly earthquakes in a certain temporal-spatial scope. Also the background earthquakes and anomaly earthquakes both satisfy the 2-D Poisson process of different parameters respectively. In the paper, the concept of N-th order distance is introduced in order to transform 2-D superimposed Poisson process into 1-D mixture density function. On the basis of choosing the distance, mixture density function is decomposed to recognize the anomaly earthquakes through genetic algorithm. Combined with the temporal scanning of C value, the algorithm is applied to the recognition on spatial pattern of foreshock anomalies by exam-ples of Songpan and Longling sequences in the southwest of China.展开更多
This paper establishes 13 evaluation indicators for the competitiveness of agri-food processing industry,uses factor analysis to evaluate the competitiveness of agri-food processing industry in 31 provinces(cities,aut...This paper establishes 13 evaluation indicators for the competitiveness of agri-food processing industry,uses factor analysis to evaluate the competitiveness of agri-food processing industry in 31 provinces(cities,autonomous regions)of China,and does cluster analysis to divide these regions into several categories according to the difference in competitiveness,in order to understand the level of competitiveness of agri-food processing industry in China.展开更多
The dual frequency Heterogeneous Network(HetNet),including sub-6 GHz networks together with Millimeter Wave(mmWave),achieves the high data rates of user in the networks with hotspots.The cache-enabled HetNets with hot...The dual frequency Heterogeneous Network(HetNet),including sub-6 GHz networks together with Millimeter Wave(mmWave),achieves the high data rates of user in the networks with hotspots.The cache-enabled HetNets with hotspots are investigated using an analytical framework in which Macro Base Stations(MBSs)and hotspot centers are treated as two independent homogeneous Poisson Point Processes(PPPs),and locations of Small Base Stations(SBSs)and users are modeled as two Poisson Cluster Processes(PCPs).Under the PCP-based modeling method and the Most Popular Caching(MPC)scheme,we propose a cache-enabled association strategy for HetNets with limited storage capacity.The performance of association probability and coverage probability is explicitly derived,and Monte Carlo simulation is utilized to verify that the results are correct.The outcomes of the simulation present the influence of antenna configuration and cache capacities of MBSs and SBSs on network performance.Numerical optimization of the standard deviation ratio of SBSs and users of association probability is enabled by our analysis.展开更多
The k-Nearest Neighbor method is one of the most popular techniques for both classification and regression purposes.Because of its operation,the application of this classification may be limited to problems with a cer...The k-Nearest Neighbor method is one of the most popular techniques for both classification and regression purposes.Because of its operation,the application of this classification may be limited to problems with a certain number of instances,particularly,when run time is a consideration.However,the classification of large amounts of data has become a fundamental task in many real-world applications.It is logical to scale the k-Nearest Neighbor method to large scale datasets.This paper proposes a new k-Nearest Neighbor classification method(KNN-CCL)which uses a parallel centroid-based and hierarchical clustering algorithm to separate the sample of training dataset into multiple parts.The introduced clustering algorithm uses four stages of successive refinements and generates high quality clusters.The k-Nearest Neighbor approach subsequently makes use of them to predict the test datasets.Finally,sets of experiments are conducted on the UCI datasets.The experimental results confirm that the proposed k-Nearest Neighbor classification method performs well with regard to classification accuracy and performance.展开更多
In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment techni...In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment technique known as ultrasonic vibration rapid processing(UVRP),which enables the formation of high-density strong magnetic α-Fe clusters,thereby enhancing the soft magnetic properties of Fe_(78)Si(13)B_(9) amorphous alloy ribbon.展开更多
Using Michael Porter's "diamond model", based on regional development characteristics, we conduct analysis of the competitiveness of processing industry cluster of livestock products in Inner Mongolia fr...Using Michael Porter's "diamond model", based on regional development characteristics, we conduct analysis of the competitiveness of processing industry cluster of livestock products in Inner Mongolia from six aspects (the factor conditions, demand conditions, corporate strategy, structure and competition, related and supporting industries, government and opportunities). And we put forward the following rational recommendations for improving the competitiveness of processing industry cluster of livestock products in Inner Mongolia: (i) The government should increase capital input, focus on supporting processing industry of livestock products, and give play to the guidance and aggregation effect of financial funds; (ii) In terms of enterprises, it is necessary to vigorously develop leading enterprises, to give full play to the cluster effect of the leading enterprises.展开更多
The issue of strong noise has increasingly become a bottleneck restricting the precision and application space of electromagnetic exploration methods.Noise suppression and extraction of effective electromagnetic respo...The issue of strong noise has increasingly become a bottleneck restricting the precision and application space of electromagnetic exploration methods.Noise suppression and extraction of effective electromagnetic response information under a strong noise background is a crucial scientific task to be addressed.To solve the noise suppression problem of the controlled-source electromagnetic method in strong interference areas,we propose an approach based on complex-plane 2D k-means clustering for data processing.Based on the stability of the controlled-source signal response,clustering analysis is applied to classify the spectra of different sources and noises in multiple time segments.By identifying the power spectra with controlled-source characteristics,it helps to improve the quality of the controlled-source response extraction.This paper presents the principle and workflow of the proposed algorithm,and demonstrates feasibility and effectiveness of the new algorithm through synthetic and real data examples.The results show that,compared with the conventional Robust denoising method,the clustering algorithm has a stronger suppression effect on common noise,can identify high-quality signals,and improve the preprocessing data quality of the controlledsource electromagnetic method.展开更多
Text clustering is an important task because of its vital role in NLP-related tasks.However,existing research on clustering is mainly based on the English language,with limited work on low-resource languages,such as U...Text clustering is an important task because of its vital role in NLP-related tasks.However,existing research on clustering is mainly based on the English language,with limited work on low-resource languages,such as Urdu.Low-resource language text clustering has many drawbacks in the form of limited annotated collections and strong linguistic diversity.Theprimary aim of this paper is twofold:(1)By introducing a clustering dataset namedUNC-2025 comprises 100k Urdu news documents,and(2)a detailed empirical standard of Large Language Model(LLM)improved clusteringmethods for Urdu text.We explicitly evaluate the behavior of the 11multilingual and Urdu-specific embeddings on 3 different clustering algorithms.We carefully evaluated our performance based on a set of internal and external measurements of validity.We discover the best configuration of the mBERT embedding with the HDBSCAN algorithm that attains a new state-of-the-art performance with a high score of external validity of 0.95.This new LLM method has created a new strong standard of Urdu text clustering.Importantly,the results confirm the strength and high scalability of the LLM-generated embeddings towards the ability to generalise the fine,subtle semantics needed to discover topics in low-resource settings and open the door to novel NLP applications in underrepresented languages.展开更多
Odd-numbered and high-nuclearity coordination clusters are extremely rare,yet they represent an intriguing subclass lacking regular repeating building blocks and high structural symmetry for understanding self-assembl...Odd-numbered and high-nuclearity coordination clusters are extremely rare,yet they represent an intriguing subclass lacking regular repeating building blocks and high structural symmetry for understanding self-assembled multiatomic systems.Herein,the largest cobalt and polydentate ligand based cluster featuring odd-nuclearity,namely[Co_(19)(HL1)_(8)(L1)_(12)(L′)_(2)(Ac)_(4)]·10CH_(3)CH_(2)OH·6H_(2)O(1,H_(2)L1=1H-benzo[d]imidazole-2-yl)methanol,HL'=1H-benzo[d]imidazole),was obtained with in-situ ligand transformation from H_(2)L1 to L′.It features a hierarchical trilayer and void-cage inside structure,consisting of central disc-shaped[Co_(7)L_(10)]core with two[Co_(6)]rings on both sides.ESI-MS of crystal 1 yields a series of more than sixteen fragments,all featuring an integrated[Co_(19)]core,suggesting stability of the polynuclear cluster in solution.During increased in-source energy from 0 to 100 eV,all MS peaks shifted to a lower m/z range,but the[Co_(19)]core remained intact,excepting for the stepwise elimination of up to three Ac^(−)anions or three L1 linkers.PXRD tracking of the reaction sediments showed the formation of a key precursor of[Co_(4)L_(4)]cubane at 3 h,and its content decreased at 6 h and vanished at 12 h,followed by the appearance of crystals 1 by the generation of a clear solution at 18 h,suggesting an initial cluster assembly-disassembly process.ESI-MS spectra analysis of both reaction sediment and solution further identify the existence of other crucial higher-nuclearity reassembled fragments of[Co_(7)L_(10)]disk and its expansion of[Co_(13)L_(12)(L′)_(2)].A probable tandem assembly-disassembly-reassembly mechanism is put forward as[CoL_(2)]→[Co_(4)L_(4)]→[Co_(7)L_(10)]→[Co_(13)L_(12)(L′)_(2)]→[Co_(19)L_(2)0(L′)_(2)].Their evolution also indicated the ingenious synergy of coexisting organic,inorganic and in-situ generated ligands,along with diverse coordination geometries of metal ions,plays a directional role in forming odd-numbered and high-nuclearity coordination clusters.Magnetism analysis revealed antiferromagnetic coupling plays dominated role in the cluster.展开更多
基金supported by the National basic scientific research projects(JCKY2021204A004)the National Ministries and Commissions Projects(2019-112hbz)the National Natural Science Foundation of China(No.52271113).
文摘Ti750s titanium alloy,a novel high-temperature titanium alloy designed for short-term service at elevated temperatures(700–750℃),has previously lacked comprehensive understanding of its hot processing behavior.In this study,the high-temperature deformation behavior and microstructural evolution of the Ti750s alloy were systematically investigated through thermal simulation compression tests conducted at temperatures ranging from 900 to 1070℃and strain rates between 0.1 and 10 s⁻1.A hot processing map was constructed using the dynamic material model to optimize the hot processing parameters.The results indicated that the optimal processing window was between 1040 and 1070℃with a strain rate of 0.1 s⁻1.Processing within the instability region resulted in localized plastic deformation,manifesting as pronounced shear bands and a highly heterogeneous strain distribution;this region should be avoided during hot deformation.Within theα+βphase safety zone characterized by low power dissipation rates between 0.32 and 0.4,the primary deformation mechanism in this region was dynamic recovery(DRV),where the lamellarαgrains underwent deformation and rotation.Conversely,in theα+βphase safety zone with high-power dissipation rates between 0.45 and 0.52,dynamic spheroidization of theαphase and dynamic recrystallization(DRX)of theβphase occurred concurrently.In theβphase safety zone with low power dissipation rates between 0.32 and 0.51,the primary deformation mechanism consisted of DRV ofβgrains,accompanied by limited DRX.However,in theβphase safety zone with high-power dissipation rates exceeding 0.56,both DRV and DRX ofβgrains took place,resulted in a significant increase in the size and number of recrystallized grains compared to those observed under low power dissipation conditions.
基金National Natural Science Foundation of China(U2242203, 42305164, 42175105)Key Innovation Team of China Meteorological Administration (CMA2023ZD08)Science and Technology Research Project of Guangdong Meteorological Service (GRMC2023M31)。
文摘Precise high-temperature weather forecasts are essential, as heatwaves are increasing in frequency under the ongoing climate change. Land-surface schemes have been demonstrated to be crucial to numerical weather predictions.However, few studies have explored the impact of land surface schemes on short-range high-temperature weather forecasts via operational numerical weather prediction models. To evaluate the impact of the soil thermal process on high-temperature weather forecasts, we coupled the soil thermal process of the state-of-the-art Common Land Model(CoLM) with the South China operational numerical weather prediction model(CMA-TRAMS) and compared the coupled model with the original CMA-TRAMS, which incorporated the Simplified Model for land Surface(SMS). Contrast experiments based on two versions of CMA-TRAMS were conducted for the year 2022 when persistent extreme heatwaves were observed in Central-East China. The results are as follows:(1) Short-range high-temperature weather forecasts were sensitive to soil thermal process schemes. The original CMA-TRAMS clearly underestimated the summertime near-surface air temperature(T2m) over almost all areas of China, whereas the CoLM led to a reduction of the negative biases by approximately 0.5°C.(2) The more accurate initial soil temperatures and the deeper soil structure used in the CoLM test contributed to actual predictions of soil heat flux, soil temperature, and T2m. Nevertheless, the SMS test failed to capture upward heat transport from deeper to shallower soil layers at night due to the shallow soil structure and lower accuracy of the bottom and initial soil temperatures.(3) Higher soil temperatures resulted in increased near-surface moisture and cloud cover in the CoLM test, which led to the warmer soil and further mitigated the cold biases of T2m through reduced longwave and shortwave radiation losses at the land surface.
基金supported by the National Natural Science Foundation of China(Grant Nos.52274339,52174321,52074186,and 52104337)Natural Science Foundation of Jiangsu Province(Grant No.BK20231317)China Baowu Low-Carbon Metallurgy Innovation Fund(Grant No.BWLCF202108).
文摘To investigate the nucleation behavior during the single-phased metallic solidification process,the commercial ultrapure ferritic stainless steels with no(Initial steel)and various melt treatments(R1,MR1,Y2,MY1,and M1 steels)were used to carry out the differential scanning colorimetry(DSC)and high-temperature confocal laser scanning microscope(HT-CLSM)experiments.Based on the results of DSC experiments,the equilibrium solidification process as well as the relationship among the critical undercooling degree(△T_(c)^(DSC)),latent heat of fusion/crystallization(△H_(f)/△H_(c)),equiaxed grain ratio(ER),and average grain size(△_(ave)^(ingot))was revealed.ER is increased with the decreasing△T_(c)^(DSC)and increasing△H_(f)/△H_(c);however,△_(ave)^(ingot)is decreased with them.Referring to the results of HT-CLSM experiments,the average sizes of micro-/macrostructures(d_(ave)/D_(ave)/)are decreased with the increasing cooling rate,as well as the difference between and apparent critical undercooling degree(△T_(c)^(CLSM))was revealed.The heterogeneous nucleation of the crystal nuclei occurs only if△T_(c)^(CLSM)>△T_(c)^(DSC).Combining with the interfacial wetting-lattice mismatch heterogeneous nucleation model,the dynamic mechanism of the metallic solidification was revealed.The as-cast grains of the melt-treated samples were obviously refined,owing to the much higher actual heterogeneous nucleation rates(I_(heter.,i))obtained through melt treatments,and the heterogeneous nucleation rates(I_(heter.,ij))for all samples are increased with the cooling rates,firmly confirming that the as-cast grains of each sample could be refined by the increasing cooling rates.
文摘This study investigated the physicochemical properties,enzyme activities,volatile flavor components,microbial communities,and sensory evaluation of high-temperature Daqu(HTD)during the maturation process,and a standard system was established for comprehensive quality evaluation of HTD.There were obvious changes in the physicochemical properties,enzyme activities,and volatile flavor components at different storage periods,which affected the sensory evaluation of HTD to a certain extent.The results of high-throughput sequencing revealed significant microbial diversity,and showed that the bacterial community changed significantly more than did the fungal community.During the storage process,the dominant bacterial genera were Kroppenstedtia and Thermoascus.The correlation between dominant microorganisms and quality indicators highlighted their role in HTD quality.Lactococcus,Candida,Pichia,Paecilomyces,and protease activity played a crucial role in the formation of isovaleraldehyde.Acidic protease activity had the greatest impact on the microbial community.Moisture promoted isobutyric acid generation.Furthermore,the comprehensive quality evaluation standard system was established by the entropy weight method combined with multi-factor fuzzy mathematics.Consequently,this study provides innovative insights for comprehensive quality evaluation of HTD during storage and establishes a groundwork for scientific and rational storage of HTD and quality control of sauce-flavor Baijiu.
基金supported by the National Natural Science Foundation of China(grant no.52072322,52202235)the Department of Science and Technology of Sichuan Province(CN)(grant no.23GJHZ0147)the Research and Innovation Fund for Graduate Students of Southwest Petroleum University(No.:2022KYCX111)。
文摘Traditionally,the construction of stable interphases relies on solvent structures dominated by aggregated anionic structures(AGG/AGG+).Nonetheless,we find that the construction of stable interphases in hightemperature environments is based on contact ion pairs(CIPs)dominated solvation structure here.In detail,in the long-chain phosphate ester-based electrolyte,the spatial site-blocking effect enables the strong solvation co-solvent ether(diethylene glycol dimethyl ether,G2)to exhibit strong ion-dipole interactions,further multicomponent competitive coordination maintaining the CIP,balancing electrode kinetics,and optimizing the high-temperature interphases.High-temperature in-situ Raman spectroscopy monitors the changes in the stable solvent structure during charge/discharge processes for the first time,and time of flight secondary ion mass spectrometry(TOF-SIMS)reveals the stable solid electrolyte interphase(SEI)with full-depth enrichment of the inorganic component.Benefiting from the high-temperature interfacial chemistry-dependent solvent structure,the advanced electrolyte enables stable cycling of 1.6 Ah 18650 batterie at 100-125℃and discharging with high current pulses(~1.83 A)at 150℃,which has rarely been reported so far.In addition,pin-pricking of 18650 batteries at100%state of charge(SoC)without fire or smoke and the moderate thermal runaway temperature(187℃)tested via the accelerating rate calorimetry(ARC)demonstrate the excellent safety of the optimized electrolyte.
基金supported by the BAGUI Talent Program in Guangxi Province(No.2019AC26001),and the National Natural Science Foundation of China(No.22171075,U23A2080).
文摘In mass spectrometry, fragments with a mass higher than the original molecular ion provide valuable insights into the molecular structure and can guide the assembly and disassembly processes for chemical synthesis. Here, we report such an example and following up by modifying the solvothermal reaction conditions (temperature and time) it is possible to isolate the high mass species in crystalline form. [Zn_(4)L_(4)Cl_(4)] (Zn_(4)L_(4), L = N-methylbenzimidazole-2-methanolate) has a boat-like Zn_(4)O_(4) core but electrospray ionization mass spectrometry (ESI-MS) of the solution of its crystals shows higher mass peaks of Zn_(5)L_(5), Zn_(5)L_(6) and Zn_(6)L_(6) species. Thus, both disassembly and reassembly are highly probable processes. Consequently, [Zn(HL)_(2)Cl_(2)] (Zn1, L = N-methylbenzimidazole-2-methanolate), [Zn_(4)L_(6)Cl_(2)] (Zn_(4)L_(6), L = N-methylbenzimidazole-2-methanolate) and [Zn_(6)L_(6)Cl_(4)(CH_(3)O)_(2)] (Zn_(6)L_(6), L = N-methylbenzimidazole-2-methanolate) were prepared. The results of multistage ESI-MS of their dissolved crystals led to a proposed mechanism of their formation in the gas phase as follows: [Zn_(3)L_(4)] through [ZnL] → [ZnL(HL)] → [Zn(HL)_(2)] → [Zn_(2)L] → [Zn_(2)L_(2)] → [Zn_(2)L_(3)]. The mechanism was derived in conjunction with Gibbs free energies calculated using DFT of the fragments observed in the ESI-MS of Zn_(4)L_(4), Zn_(4)L_(6) and Zn_(6)L_(6). This work reveals the complex of chemical reactions, involving fragmentation and unexpected combination, under mass spectrometry condition which allows one to synthesize the observed transients, leading to mechanism of formation by correlation of solid-state/solution structural information.
文摘A PHE (Process Heat Exchanger) is a key component in transferring high-temperature heat generated from a VHTR (Very High Temperature Reactor) to a chemical reaction for the massive production of hydrogen. Last year, a 10 kW class lab-scale PHE prototype made of Hastelloy-X was manufactured at the Korea Atomic Energy Research Institute (KAERI), and a performance test of the PHE prototype is currently underway in a small-scale nitrogen gas loop at KAERI. The PHE prototype is composed of two kinds of flow plates: grooves 1.0 mm in diameter machined into the flow plate for the primary coolant, and waved channels bent into the flow plate for the secondary coolant. Inside the 10 kW class lab-scale PHE prototype, twenty flow plates for the primary and secondary coolants are stacked in turn. In this study, to understand the macroscopic structural behavior of the PHE prototype under the steady-state operating condition of the gas loop, high-temperature structural analyses on the 10 kW class lab-scale PHE prototype were performed for two extreme cases: in the event of contacting the flow plates together, and when not contacting them. The analysis results for the extreme cases were also compared.
文摘Processes supported by process-aware information systems are subject to continuous and often subtle changes due to evolving operational,organizational,or regulatory factors.These changes,referred to as incremental concept drift,gradually alter the behavior or structure of processes,making their detection and localization a challenging task.Traditional process mining techniques frequently assume process stationarity and are limited in their ability to detect such drift,particularly from a control-flow perspective.The objective of this research is to develop an interpretable and robust framework capable of detecting and localizing incremental concept drift in event logs,with a specific emphasis on the structural evolution of control-flow semantics in processes.We propose DriftXMiner,a control-flow-aware hybrid framework that combines statistical,machine learning,and process model analysis techniques.The approach comprises three key components:(1)Cumulative Drift Scanner that tracks directional statistical deviations to detect early drift signals;(2)a Temporal Clustering and Drift-Aware Forest Ensemble(DAFE)to capture distributional and classification-level changes in process behavior;and(3)Petri net-based process model reconstruction,which enables the precise localization of structural drift using transition deviation metrics and replay fitness scores.Experimental validation on the BPI Challenge 2017 event log demonstrates that DriftXMiner effectively identifies and localizes gradual and incremental process drift over time.The framework achieves a detection accuracy of 92.5%,a localization precision of 90.3%,and an F1-score of 0.91,outperforming competitive baselines such as CUSUM+Histograms and ADWIN+Alpha Miner.Visual analyses further confirm that identified drift points align with transitions in control-flow models and behavioral cluster structures.DriftXMiner offers a novel and interpretable solution for incremental concept drift detection and localization in dynamic,process-aware systems.By integrating statistical signal accumulation,temporal behavior profiling,and structural process mining,the framework enables finegrained drift explanation and supports adaptive process intelligence in evolving environments.Its modular architecture supports extension to streaming data and real-time monitoring contexts.
基金the National Natural Science Foundation of China(Nos.51734005,51874071,and 51604063)the Fok Ying Tung Education Foundation for Young Teachers in the Higher Education Institutions of China(No.161045)+1 种基金the Liao Ning Revitalization Talents Program(No.XLYC1807111)the Fundamental Research Funds for the Central Universities of China(No.N180105030).
文摘The efficient development and utilization of high-phosphorus oolitic hematite is of great strategic significance for the sustainable supply of iron-ore resources in China.In this paper,the mechanism of high-temperature pretreatment for enhancing the effect of iron enrichment and dephosphorization in the magnetization roasting–leaching process was studied by X-ray diffraction(XRD),vibration sample magnetometer(VSM),scanning electron microscopy and energy dispersive spectrometry(SEM–EDS).Compared with the process without high-temperature pretreatment,the iron grade of the magnetic separation concentrate after high-temperature pretreatment had increased by 0.98%,iron recovery rate had increased by 1.33%,and the phosphorus content in the leached residue had decreased by 0.12%.High-temperature pretreatment resulted in the dehydration and decomposition of hydroxyapatite,the dehydration of limonite and the thermal decomposition of siderite,which can produce pores and cracks and weaken the compactness of the ore,improve the magnetization characteristics of roasted ore,and strengthen the iron enrichment and dephosphorization during the magnetization roasting and leaching process.
文摘To further improve the oxidation-resistance of materials and reduce the cost of grid plates in grate-kiln, a new kind of heat-resistant grid plate was developed. The microstructure of this grid plate with a life more than 18 months was studied by XRD, SEM and EDS techniques. The results show that high hardness, high intensity and good impact property make the new kind of heat-resistant grid plate and its oxide film have a higher resistance to deformation and abrasion at 900-1000℃ Besides, small grain size is beneficial to form a complete protective oxide film. The oxide film composed of SiO2 layer, Cr2O3 layer and Fe2O3 layer is rather thin and bonds closely with the backing. The forming of the chemical stable nickel-rich layer increases the density of Cr2O3 layer.
基金co-supported by the National Natural Science Foundation of China(No.12101608)the NSAF(No.U2230208)the Hunan Provincial Innovation Foundation for Postgraduate,China(No.CX20220034).
文摘This paper introduces techniques in Gaussian process regression model for spatiotemporal data collected from complex systems.This study focuses on extracting local structures and then constructing surrogate models based on Gaussian process assumptions.The proposed Dynamic Gaussian Process Regression(DGPR)consists of a sequence of local surrogate models related to each other.In DGPR,the time-based spatial clustering is carried out to divide the systems into sub-spatio-temporal parts whose interior has similar variation patterns,where the temporal information is used as the prior information for training the spatial-surrogate model.The DGPR is robust and especially suitable for the loosely coupled model structure,also allowing for parallel computation.The numerical results of the test function show the effectiveness of DGPR.Furthermore,the shock tube problem is successfully approximated under different phenomenon complexity.
文摘Aiming at the complexity of seismic gestation mechanism and spatial distribution, we hypothesize that the seismic data are composed of background earthquakes and anomaly earthquakes in a certain temporal-spatial scope. Also the background earthquakes and anomaly earthquakes both satisfy the 2-D Poisson process of different parameters respectively. In the paper, the concept of N-th order distance is introduced in order to transform 2-D superimposed Poisson process into 1-D mixture density function. On the basis of choosing the distance, mixture density function is decomposed to recognize the anomaly earthquakes through genetic algorithm. Combined with the temporal scanning of C value, the algorithm is applied to the recognition on spatial pattern of foreshock anomalies by exam-ples of Songpan and Longling sequences in the southwest of China.
基金Supported by Humanities and Social Sciences Project of Hubei Provincial Department of Education(14Q033)
文摘This paper establishes 13 evaluation indicators for the competitiveness of agri-food processing industry,uses factor analysis to evaluate the competitiveness of agri-food processing industry in 31 provinces(cities,autonomous regions)of China,and does cluster analysis to divide these regions into several categories according to the difference in competitiveness,in order to understand the level of competitiveness of agri-food processing industry in China.
基金supported in part by National Key Research and Development Project under Grant 2020YFB1807204in part by the National Natural Science Foundation of China under Grant U2001213 and 61971191+2 种基金in part by the Beijing Natural Science Foundation under Grant L201011in part by the Key project of Natural Science Foundation of Jiangxi Province under Grant 20202ACBL202006in part by the Science and Technology Foundation of Jiangxi Province(20202BCD42010)。
文摘The dual frequency Heterogeneous Network(HetNet),including sub-6 GHz networks together with Millimeter Wave(mmWave),achieves the high data rates of user in the networks with hotspots.The cache-enabled HetNets with hotspots are investigated using an analytical framework in which Macro Base Stations(MBSs)and hotspot centers are treated as two independent homogeneous Poisson Point Processes(PPPs),and locations of Small Base Stations(SBSs)and users are modeled as two Poisson Cluster Processes(PCPs).Under the PCP-based modeling method and the Most Popular Caching(MPC)scheme,we propose a cache-enabled association strategy for HetNets with limited storage capacity.The performance of association probability and coverage probability is explicitly derived,and Monte Carlo simulation is utilized to verify that the results are correct.The outcomes of the simulation present the influence of antenna configuration and cache capacities of MBSs and SBSs on network performance.Numerical optimization of the standard deviation ratio of SBSs and users of association probability is enabled by our analysis.
基金The authors received no specific funding for this work.
文摘The k-Nearest Neighbor method is one of the most popular techniques for both classification and regression purposes.Because of its operation,the application of this classification may be limited to problems with a certain number of instances,particularly,when run time is a consideration.However,the classification of large amounts of data has become a fundamental task in many real-world applications.It is logical to scale the k-Nearest Neighbor method to large scale datasets.This paper proposes a new k-Nearest Neighbor classification method(KNN-CCL)which uses a parallel centroid-based and hierarchical clustering algorithm to separate the sample of training dataset into multiple parts.The introduced clustering algorithm uses four stages of successive refinements and generates high quality clusters.The k-Nearest Neighbor approach subsequently makes use of them to predict the test datasets.Finally,sets of experiments are conducted on the UCI datasets.The experimental results confirm that the proposed k-Nearest Neighbor classification method performs well with regard to classification accuracy and performance.
基金supported by the Major Science and Technology Project of Zhongshan City(No.2022AJ004)the Key Basic and Applied Research Program of Guangdong Province(Nos.2019B030302010 and 2022B1515120082)Guangdong Science and Technology Innovation Project(No.2021TX06C111).
文摘In general,the rapid growth of α-Fe clusters is a challenge in high Fe-content Fe-based amorphous alloys,negatively affecting their physical properties.Herein,we introduce an efficient and rapid post-treatment technique known as ultrasonic vibration rapid processing(UVRP),which enables the formation of high-density strong magnetic α-Fe clusters,thereby enhancing the soft magnetic properties of Fe_(78)Si(13)B_(9) amorphous alloy ribbon.
基金Supported by National Natural Science Foundation(70963014,71210107012)
文摘Using Michael Porter's "diamond model", based on regional development characteristics, we conduct analysis of the competitiveness of processing industry cluster of livestock products in Inner Mongolia from six aspects (the factor conditions, demand conditions, corporate strategy, structure and competition, related and supporting industries, government and opportunities). And we put forward the following rational recommendations for improving the competitiveness of processing industry cluster of livestock products in Inner Mongolia: (i) The government should increase capital input, focus on supporting processing industry of livestock products, and give play to the guidance and aggregation effect of financial funds; (ii) In terms of enterprises, it is necessary to vigorously develop leading enterprises, to give full play to the cluster effect of the leading enterprises.
基金supported by the National Key Research and Development Program Project of China(Grant No.2023YFF0718003)the key research and development plan project of Yunnan Province(Grant No.202303AA080006).
文摘The issue of strong noise has increasingly become a bottleneck restricting the precision and application space of electromagnetic exploration methods.Noise suppression and extraction of effective electromagnetic response information under a strong noise background is a crucial scientific task to be addressed.To solve the noise suppression problem of the controlled-source electromagnetic method in strong interference areas,we propose an approach based on complex-plane 2D k-means clustering for data processing.Based on the stability of the controlled-source signal response,clustering analysis is applied to classify the spectra of different sources and noises in multiple time segments.By identifying the power spectra with controlled-source characteristics,it helps to improve the quality of the controlled-source response extraction.This paper presents the principle and workflow of the proposed algorithm,and demonstrates feasibility and effectiveness of the new algorithm through synthetic and real data examples.The results show that,compared with the conventional Robust denoising method,the clustering algorithm has a stronger suppression effect on common noise,can identify high-quality signals,and improve the preprocessing data quality of the controlledsource electromagnetic method.
基金Chang Gung University and Chang Gung Memorial Hospital under project number NERPD4Q0021.
文摘Text clustering is an important task because of its vital role in NLP-related tasks.However,existing research on clustering is mainly based on the English language,with limited work on low-resource languages,such as Urdu.Low-resource language text clustering has many drawbacks in the form of limited annotated collections and strong linguistic diversity.Theprimary aim of this paper is twofold:(1)By introducing a clustering dataset namedUNC-2025 comprises 100k Urdu news documents,and(2)a detailed empirical standard of Large Language Model(LLM)improved clusteringmethods for Urdu text.We explicitly evaluate the behavior of the 11multilingual and Urdu-specific embeddings on 3 different clustering algorithms.We carefully evaluated our performance based on a set of internal and external measurements of validity.We discover the best configuration of the mBERT embedding with the HDBSCAN algorithm that attains a new state-of-the-art performance with a high score of external validity of 0.95.This new LLM method has created a new strong standard of Urdu text clustering.Importantly,the results confirm the strength and high scalability of the LLM-generated embeddings towards the ability to generalise the fine,subtle semantics needed to discover topics in low-resource settings and open the door to novel NLP applications in underrepresented languages.
基金supported by the BAGUI Talent Program in Guangxi Province(No.2019AC26001)the National Natural Science Foundation of China(Nos.22171075,U23A2080,22371173).
文摘Odd-numbered and high-nuclearity coordination clusters are extremely rare,yet they represent an intriguing subclass lacking regular repeating building blocks and high structural symmetry for understanding self-assembled multiatomic systems.Herein,the largest cobalt and polydentate ligand based cluster featuring odd-nuclearity,namely[Co_(19)(HL1)_(8)(L1)_(12)(L′)_(2)(Ac)_(4)]·10CH_(3)CH_(2)OH·6H_(2)O(1,H_(2)L1=1H-benzo[d]imidazole-2-yl)methanol,HL'=1H-benzo[d]imidazole),was obtained with in-situ ligand transformation from H_(2)L1 to L′.It features a hierarchical trilayer and void-cage inside structure,consisting of central disc-shaped[Co_(7)L_(10)]core with two[Co_(6)]rings on both sides.ESI-MS of crystal 1 yields a series of more than sixteen fragments,all featuring an integrated[Co_(19)]core,suggesting stability of the polynuclear cluster in solution.During increased in-source energy from 0 to 100 eV,all MS peaks shifted to a lower m/z range,but the[Co_(19)]core remained intact,excepting for the stepwise elimination of up to three Ac^(−)anions or three L1 linkers.PXRD tracking of the reaction sediments showed the formation of a key precursor of[Co_(4)L_(4)]cubane at 3 h,and its content decreased at 6 h and vanished at 12 h,followed by the appearance of crystals 1 by the generation of a clear solution at 18 h,suggesting an initial cluster assembly-disassembly process.ESI-MS spectra analysis of both reaction sediment and solution further identify the existence of other crucial higher-nuclearity reassembled fragments of[Co_(7)L_(10)]disk and its expansion of[Co_(13)L_(12)(L′)_(2)].A probable tandem assembly-disassembly-reassembly mechanism is put forward as[CoL_(2)]→[Co_(4)L_(4)]→[Co_(7)L_(10)]→[Co_(13)L_(12)(L′)_(2)]→[Co_(19)L_(2)0(L′)_(2)].Their evolution also indicated the ingenious synergy of coexisting organic,inorganic and in-situ generated ligands,along with diverse coordination geometries of metal ions,plays a directional role in forming odd-numbered and high-nuclearity coordination clusters.Magnetism analysis revealed antiferromagnetic coupling plays dominated role in the cluster.
