Traditional data-driven fault diagnosis methods depend on expert experience to manually extract effective fault features of signals,which has certain limitations.Conversely,deep learning techniques have gained promine...Traditional data-driven fault diagnosis methods depend on expert experience to manually extract effective fault features of signals,which has certain limitations.Conversely,deep learning techniques have gained prominence as a central focus of research in the field of fault diagnosis by strong fault feature extraction ability and end-to-end fault diagnosis efficiency.Recently,utilizing the respective advantages of convolution neural network(CNN)and Transformer in local and global feature extraction,research on cooperating the two have demonstrated promise in the field of fault diagnosis.However,the cross-channel convolution mechanism in CNN and the self-attention calculations in Transformer contribute to excessive complexity in the cooperative model.This complexity results in high computational costs and limited industrial applicability.To tackle the above challenges,this paper proposes a lightweight CNN-Transformer named as SEFormer for rotating machinery fault diagnosis.First,a separable multiscale depthwise convolution block is designed to extract and integrate multiscale feature information from different channel dimensions of vibration signals.Then,an efficient self-attention block is developed to capture critical fine-grained features of the signal from a global perspective.Finally,experimental results on the planetary gearbox dataset and themotor roller bearing dataset prove that the proposed framework can balance the advantages of robustness,generalization and lightweight compared to recent state-of-the-art fault diagnosis models based on CNN and Transformer.This study presents a feasible strategy for developing a lightweight rotating machinery fault diagnosis framework aimed at economical deployment.展开更多
The numerical dispersion phenomenon in the finite-difference forward modeling simulations of the wave equation significantly affects the imaging accuracy in acoustic reflection logging.This issue is particularly prono...The numerical dispersion phenomenon in the finite-difference forward modeling simulations of the wave equation significantly affects the imaging accuracy in acoustic reflection logging.This issue is particularly pronounced in the reverse time migration(RTM)method used for shear-wave(S-wave)logging imaging.This not only affects imaging accuracy but also introduces ambiguities in the interpretation of logging results.To address this challenge,this study proposes the use of a least-squares difference coefficient optimization algorithm aiming to suppress the numerical dispersion phenomenon in the RTM of S-wave reflection imaging logging.By optimizing the difference coefficients,the high-precision finite-difference algorithm serves as an effective operator for both forward and backward RTM processes.This approach is instrumental in eliminating migration illusions,which are often caused by numerical dispersion.The effectiveness of this optimized algorithm is demonstrated through numerical results,which indicate that it can achieve more accurate forward imaging results across various conditions,including high-and low-velocity strata,and is effective in both large and small spatial grids.The results of processing real data demonstrate that numerical dispersion optimization effectively reduces migration artifacts and diminishes ambiguities in logging interpretations.This optimization offers crucial technical support to the RTM method,enhancing its capability for accurately modeling and imaging S-wave reflections.展开更多
This study explored the application value of iterative decomposition of water and fatwith echo asymmetry and least-squares estimation(IDEAL-IQ)technology in the early diagnosis of ageing osteoporosis(OP).172 participa...This study explored the application value of iterative decomposition of water and fatwith echo asymmetry and least-squares estimation(IDEAL-IQ)technology in the early diagnosis of ageing osteoporosis(OP).172 participants were enrolled and underwentmagnetic resonance imaging(MRI)examinations on a 3.0T scanner.100 cases were included in the normal group(50 males and 50 females;mean age:45 years;age range:20e84 years).33 cases were included in the osteopenia group(17 males and 16 females;mean age:55 years;age range:43e83 years).39 caseswere includedintheOP group(19males and20females;meanage:58years;age range:48 e82 years).Conventional T1WI and T2WI were first obtained,followed by 3D-IDEAL-IQ-acqui-sition.Fat fraction(FF)and apparent transverse relaxation rate(R2*)resultswere automatically calculated from IDEAL-IQ-images on the console.Based on T1Wand T2W-images,300 ROIs for each participantweremanually delineated in L1-L5 vertebral bodies of five middle slices.In each age group of all normal subjects,each parameter was significantly correlated with gender.In male participants from the normal,osteopenia,and OP groups,statistical analysis revealed F values of 11319.292 and 180.130 for comparisons involving FF and R2*values,respectively(all p<0.0001).The sensitivity and specificity of FF values were 0.906 and 0.950,0.994 and 0.997,0.865 and 0.820,respectively.For R2*,they were 0.665 and 0.616,0.563 and 0.519,0.571 and 0.368,respectively.In female participants from the normal,osteopenia,and OP-groups,statis-tical analysis revealed F values of 12461.658 and 548.274 for comparisons involving FF and R2*values,respectively(all p<0.0001).The sensitivity and specificity of FF values were 0.985 and 0.991,0.996 and 0.996,0.581 and 0.678,respectively.For R2*,they were 0.698 and 0.730,0.603 and 0.665,0.622 and 0.525,respectively.Significant differences were indicated in the quanti-tative values among the three groups.FF value had good performance,while R2*value had poor performance indiscriminatingosteopenia andOP-groups.Overall,the IDEAL-IQ techniqueoffers specific reference indices that enable noninvasive and quantitative assessment of lumbar vertebrae bone metabolism,thereby providing diagnostic information for OP.展开更多
The separation of propylene(C_(3)H_(6))and propane(C_(3)H_(8))presents a significant industrial challenge due to their similar molecular dimensions and physicochemical properties.Among various separation methods,molec...The separation of propylene(C_(3)H_(6))and propane(C_(3)H_(8))presents a significant industrial challenge due to their similar molecular dimensions and physicochemical properties.Among various separation methods,molecular sieving emerges as the most promising approach,but it will be significantly compromised at high temperatures due to the significant thermal motion.Here,we report a thermally robust zinc-based metal-organic framework(MOF)that can be synthesized on sub-kilogram scale and achieve exceptional C_(3)H_(6)/C_(3)H_(8) separation performances across a broad temperature range(298–353 K).Unlike conventional MOFs suffering from thermal lattice expansion to give poorer selectivity,this new MOF gives the adsorption capacity of C_(3)H_(6)essentially unchanged and that of C_(3)H_(8) negligible at elevated temperatures,outperforming most state-of-the-art adsorbents,in virtue of multiple hydrogen bonds at the aperture.Column breakthrough experiments confirmed the excellent separation capability,and showed no performance degradation over multi-round adsorption-desorption cycles at 353 K.This study addresses the critical challenge of the trade-off between temperature and selectivity in adsorptive separation,which offers new insights into the design of porous structures for highly effective separation at high temperatures.展开更多
This paper examines a model that combines vortex generators and leading-edge tubercles for controlling the laminar separation bubble(LSB)over an airfoil at low Reynolds numbers(Re).This new concept of passive flow con...This paper examines a model that combines vortex generators and leading-edge tubercles for controlling the laminar separation bubble(LSB)over an airfoil at low Reynolds numbers(Re).This new concept of passive flow control technique utilizing a tubercle and vortex generator(VG)close to the leading edge was analyzed numerically for a NACA0015 airfoil.In this study,the Shear Stress Transport(SST)turbulence model was employed in the numerical modelling.Numerical modelling was completed using the ANSYS-Fluent 18.2 solver.Analyses were conducted to investigate the flow pattern and understand the underlying LSB control phenomena that enabled the new passive flow control method to provide this significant performance benefit.The findings indicated that the new concept of passive flow control technique suppressed the formation of an LSB at the suction surface of the NACA0015 airfoil,resulting in a higher lift coefficient and improved aerodynamic performance.Improvements in LSB dynamics and aerodynamic performance through the passive flow control method lead to increased energy output and enhanced stability.展开更多
With the legislative development,the organic and inorganic composition separation has become the primary requirement for sewer sediment disposal,however the relevant technology has been rarely reported and the driving...With the legislative development,the organic and inorganic composition separation has become the primary requirement for sewer sediment disposal,however the relevant technology has been rarely reported and the driving mechanism was still unclear.In this study,direct disintegration of biopolymers and indirect broken of connection point were investigated on the hydrolysis and component separation.Three typical sewer sediment treatment approaches,i.e.,alkaline,thermal and cation exchange treatments were proposed,which represented the hydrolysis-driving forces of chemical hydrolysis,physical hydrolysis and innovative cation bridging break-age.The results showed that the organic and inorganic separation rates of sewer sediment driven by alkaline,thermal and cation exchange treatments reached 21.26%,23.80%,and 19.56%-48.0%,respectively,compared to 4.43%in control.The secondary structure of proteins was disrupted,transitioning from𝛼α-helix to𝛽β-turn and random coil.Meanwhile,much biopolymers were released from solid to the liquid phase.From thermody-namic perspective,sewer sediment deposition was controlled by short-range interfacial interactions described by extended Derjaguin-Landau-Verwey-Overbeek theory.Additionally,the separation of organic and inorganic components was positively correlated with the thermodynamic parameters(Corr=0.87),highlighted the robust-ness of various driving forces.And the flocculation energy barriers were 2.40(alkaline),1.60 times(thermal),and 4.02–4.97 times(cation exchange)compared to control group.The findings revealed the contrition differ-ence of direct disintegration of gelatinous biopolymers and indirect breakage of composition connection sites in sediment composition separation,filling the critical gaps in understanding the specific mechanisms of sediment biopolymer disintegration and intermolecular connection breakage.展开更多
Vehicle-induced response separation is a crucial issue in structural health monitoring(SHM).This paper proposes a block-wise sliding recursive wavelet transform algorithm to meet the real-time processing requirements ...Vehicle-induced response separation is a crucial issue in structural health monitoring(SHM).This paper proposes a block-wise sliding recursive wavelet transform algorithm to meet the real-time processing requirements of monitoring data.To extend the separation target from a fixed dataset to a continuously updating data stream,a block-wise sliding framework is first developed.This framework is further optimized considering the characteristics of real-time data streams,and its advantage in computational efficiency is theoretically demonstrated.During the decomposition and reconstruction processes,information from neighboring data blocks is fully utilized to reduce algorithmic complexity.In addition,a delay-setting strategy is introduced for each processing window to mitigate boundary effects,thereby balancing accuracy and efficiency.Simulated signal experiments are conducted to determine the optimal delay configuration and to verify the algorithm’s superior performance,achieving a lower Root Mean Square Error(RMSE)and only 0.0249 times the average computational time compared with the original algorithm.Furthermore,strain signals from the Lieshi River Bridge are employed to validate the method.The proposed algorithm successfully separates the static trend from vehicle-induced responses in real time across different sampling frequencies,demonstrating its effectiveness and applicability in real-time bridge monitoring.展开更多
Lithium-sulfur batteries(LSBs)represent a next-generation energy storage technology,but widespread applications are restricted by the shuttle of lithium polysulfides(LiPSs).The rational design of separators has been d...Lithium-sulfur batteries(LSBs)represent a next-generation energy storage technology,but widespread applications are restricted by the shuttle of lithium polysulfides(LiPSs).The rational design of separators has been demonstrated to be one of the most efficient and cost-effective strategies to curb the shuttle effect,and tremendous research progress has been achieved.The efficiency of a separator depends on its interaction with LiPSs,which is governed by the surface energy and binding strength.Despite several review works that have been reported to advance the separators,most of them primarily focus on active material innovation and construction.The most crucial issues of surface binding energy have not been systematically reviewed,limiting the precise design of efficient separators.In this review,fundamentals related to surface energy and binding interactions with LiPSs are comprehensively analyzed and discussed.With surface binding and energy main lines,the advancements in separator engineering strategies are elaborately summarized and discussed.Moreover,techniques for evaluating affinity to LiPSs are thoroughly analyzed to avoid any ambiguities in measurement.Based on the research context,valuable research directions are suggested to construct efficient separators.This work provides guidelines to regulate the surface binding and energy of separators for high-performance LSBs.展开更多
Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science.Recently,supramolecular polymeric materials(SPMs)have drawn increased ...Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science.Recently,supramolecular polymeric materials(SPMs)have drawn increased attention due to their unique properties and potential applications in self-healing,shape memory,sensors,and flexible electronics.Here,we develop an ionic cluster-optimized microphase separation strategy to enhance the toughening and energy dissipation capabilities of polydisulfide-based supramolecular polymers.The mechanical properties,including Young's modulus and toughness,are significantly improved by integrating the quadruple H-bonding 2-ureido-4-pyrimidone(UPy)induced microphase separation with iron(III)-to-carboxylate ionic clusters.By combining established chemical approaches with adjustable polymer phase ratios,it is revealed that the synergistic effect of these factors expands the interchain spacing,facilitates the formation of microphase domains,and enhances the tolerance of polythioctic acid-based polymers to external mechanical and thermal stimuli,meeting the practical requirements for industrial plastic applications.Moreover,the UPy-functionalized polymers incorporating iron carboxylate clusters exhibit good one-way shape memory behavior with practical applicability at a relatively low recovery temperature.Our work demonstrates a novel strategy for constructing industrially viable shape memory dynamic SPMs and paves the way for future innovations in developing SPMs.展开更多
The removal of trace plutonium(Pu)from uranium products and organic wastes during spent nuclear fuel reprocessing remains a critical challenge,resulting in excessive plutonium content in uranium products and waste org...The removal of trace plutonium(Pu)from uranium products and organic wastes during spent nuclear fuel reprocessing remains a critical challenge,resulting in excessive plutonium content in uranium products and waste organic liquid.Currently,most organic ligands with selective separation functions are lipophilic,while research on water-soluble,highly selective ligands is relatively scarce,and there are also few reports on the single crystal of these ligands coordinating with plutonium.Herein,a hydrophilic multiamide ligand,N,N,N′,N″,N″-hexaethyl-nitrilotriacetamide(NTAamideC2),was synthesized and evaluated for its Pu(Ⅳ)back-extraction efficiency under harsh conditions.Systematic experiments revealed that NTAamideC2 achieved>99%Pu(Ⅳ)back-extraction rate within 15 min across a wide nitric acid concentration range(0-5 M),even with elevated dibutyl phosphate(DBP≤20000 ppm).Remarkably,the separation factor(SFPu/U)reached 767 at 1.5 M HNO_(3),demonstrating exceptional selectivity over uranium(Ⅵ).Spectrophotometric titration and DFT calculations confirmed the formation of 1:1 and 1:2 Pu(Ⅳ)-NTAamideC2 complexes,with log β values of 7.42±0.01 and 13.23±0.02,respectively.Single-crystal X-ray diffraction analysis of{[Pu_(2)(H_(2)O)_(2)(NTAamideC2)_(4)](H_(2)O)_(2)(NO_(3))(ClO_(4))_(7)}revealed a nine-coordinated PuO_(7)N_(2)geometry,where two NTAamideC2 molecules bind via six O and two N atoms.Compared to conventional agents(AHA/HSC),NTAamideC2 exhibited superior acid tolerance and selectivity,aligning with the CHON principle for sustainable nuclear waste management.This work provides a robust strategy for Pu(Ⅳ)removal in uranium purification cycles and advances fundamental insights into Pu coordination chemistry,offering significant potential for industrial nuclear fuel reprocessing.展开更多
Objective:To analyze the impact of maternal-infant separation on the physical and mental state of high-risk pregnancy patients and explore the clinical efficacy of targeted nursing interventions.Methods:A total of 80 ...Objective:To analyze the impact of maternal-infant separation on the physical and mental state of high-risk pregnancy patients and explore the clinical efficacy of targeted nursing interventions.Methods:A total of 80 high-risk pregnancy patients treated in our hospital from January 2023 to January 2024 were selected as the study subjects.These patients were randomly divided into an observation group and a control group(40 cases each)using a random number table.The control group received routine high-risk pregnancy nursing care,while the observation group received specialized maternal-infant separation nursing interventions in addition to routine care.The psychological and physiological states and nursing satisfaction of the two groups were compared before and after the intervention.Results:The SAS scores,SDS scores,and sleep quality scores of the observation group were significantly lower than those of the control group,with statistically significant differences(p<0.05).The incidence of postpartum hemorrhage in the observation group was significantly lower than that in the control group,and the initiation time of lactation was significantly earlier than that in the control group,with both differences being statistically significant(p<0.05).The nursing satisfaction of the observation group was significantly higher than that of the control group(80%vs.32/40),with a statistically significant difference(p<0.05).Conclusion:Maternal-infant separation exacerbates anxiety and depression in high-risk pregnancy patients,reduces sleep quality,increases the risk of postpartum hemorrhage,and delays the initiation of lactation.Specialized nursing interventions for maternal-infant separation can improve the physical and mental state of high-risk pregnancy patients,reduce the incidence of postpartum complications,and enhance nursing satisfaction,making them worthy of clinical application and promotion.展开更多
Zn-I_(2) batteries have emerged as promising next-generation energy storage systems owing to their inherent safety,environmental compatibility,rapid reaction kinetics,and small voltage hysteresis.Nevertheless,two crit...Zn-I_(2) batteries have emerged as promising next-generation energy storage systems owing to their inherent safety,environmental compatibility,rapid reaction kinetics,and small voltage hysteresis.Nevertheless,two critical challenges,i.e.,zinc dendrite growth and polyiodide shuttle effect,severely impede their commercial viability.To conquer these limitations,this study develops a multifunctional separator fabricated from straw-derived carboxylated nanocellulose,with its negative charge density further reinforced by anionic polyacrylamide incorporation.This modification simultaneously improves the separator’s mechanical properties,ionic conductivity,and Zn^(2+)ion transfer number.Remarkably,despite its ultrathin 20μm profile,the engineered separator demonstrates exceptional dendrite suppression and parasitic reaction inhibition,enabling Zn//Zn symmetric cells to achieve impressive cycle life(>1800 h at 2 m A cm^(-2)/2 m Ah cm^(-2))while maintaining robust performance even at ultrahigh areal capacities(25 m Ah cm^(-2)).Additionally,the separator’s anionic characteristic effectively blocks polyiodide migration through electrostatic repulsion,yielding Zn-I_(2) batteries with outstanding rate capability(120.7 m Ah g^(-1)at 5 A g^(-1))and excellent cyclability(94.2%capacity retention after 10,000 cycles).And superior cycling stability can still be achieved under zinc-deficient condition and pouch cell configuration.This work establishes a new paradigm for designing high-performance zinc-based energy storage systems through rational separator engineering.展开更多
Conventional electrolytic methods for separating chemically similar lanthanides(Ln)and actinides(An)are limited by thermodynamics and slow reaction kinetics,restricting their efficiency in rare-earth refining and nucl...Conventional electrolytic methods for separating chemically similar lanthanides(Ln)and actinides(An)are limited by thermodynamics and slow reaction kinetics,restricting their efficiency in rare-earth refining and nuclear fuel recycling.Herein,we report an electroextraction and oxidative back-extraction(EOB)strategy utilizing a LiCl-KCl-KAlCl_(4) molten salt that overcomes these limitations by leveraging divergent interfacial reactivity.The EOB process achieves an exceptional separation factor for Ln/An(>1000),while simultaneously increasing the separation rate by at least one order of magnitude.Through in-situ synchrotron radiation X-ray micro-computed tomography(SR-μCT)and X-ray diffraction(SR-XRD),we capture selective oxidation-induced destabilization of Ln-Al alloys while actinides retain phase stability-directly visualizing the electrochemical alloy transition mechanism.This research redefines the separation of f-block elements in molten salt systems and introduces a multimodal approach to investigating transient interfacial phenomena that are usually inaccessible to conventional metallurgical diagnostics under extreme conditions.展开更多
Biochar has been widely recognized as a promising solid CO_(2)adsorbent with economic and ecological benefits.Industrial CO_(2)emissions originate from diverse sources,while the pore structure and chemical functional ...Biochar has been widely recognized as a promising solid CO_(2)adsorbent with economic and ecological benefits.Industrial CO_(2)emissions originate from diverse sources,while the pore structure and chemical functional groups of biochar exhibit varying degrees of influence on CO_(2)adsorption and separation performance under different adsorption conditions.Therefore,exploring the matching relationship between the physicochemical properties of biochar and its adsorption and separation performance at different adsorption conditions is essential for the development and optimization of carbon-based adsorbents.This study selected the high-performance extreme gradient boosting(XGB)algorithm from various algorithms and utilized it to develop CO_(2),N_(2),CH_(4)adsorption prediction models.Based on this,coupled prediction models were developed for CO_(2)/N_(2)and CO_(2)/CH_(4)adsorption selectivity.Furthermore,feature importance and partial dependence analysis were performed using SHAP values.The results indicate that during CO_(2)adsorption,the influence of the pore structure of biochar outweighs that of its chemical composition.Specifically,the pore structure of 0.4–0.6 nm is the most important property influencing CO_(2)adsorption at low and medium pressure(0–0.6 bar),and the pore structure of 0.6–0.8 nm,as well as the specific surface area contribute the most at high pressure(0.6–1 bar).During CO_(2)selective separation,the CO_(2)/N_(2)mixture is primarily separated through the selective adsorption of CO_(2)by nitrogen functional groups.In contrast,for CO_(2)/CH_(4)mixtures,pore structure<1 nm plays a more critical role in determining adsorption selectivity.In addition,molecular simulation studies further revealed the adsorption filling mechanisms of CO_(2)molecules within different pore sizes and functional groups.Finally,nitrogen-doped biochar was synthesized using de-alkalize lignin as the precursor,KOH as the activating agent,and urea as the nitrogen dopant.CO_(2),N_(2),and CH_(4)isothermal adsorption experiments were conducted,and the experimental results confirmed that the developed prediction models exhibit high accuracy(R^(2)>0.9).展开更多
Developing a chiral material as versatile and universal chiral stationary phase(CSP) for chiral separation in diverse chromatographic techniques simultaneously is of great significance.In this study,we demonstrated fo...Developing a chiral material as versatile and universal chiral stationary phase(CSP) for chiral separation in diverse chromatographic techniques simultaneously is of great significance.In this study,we demonstrated for the first time that a chiral metal-organic cage(MOC),[Zn_(6)M_(4)],as a universal chiral recognition material for both multi-mode high-performance liquid chromatography(HPLC) and capillary gas chromatography(GC) enantioseparation.Two novel HPLC CSPs with different bonding arms(CSP-A with a cationic imidazolium bonding arm and CSP-B with an alkyl chain bonding arm) were prepared by clicking of functionalized chiral MOC [Zn_(6)M_(4)] onto thiolated silica via thiol-ene click chemistry.Meanwhile,a capillary GC column statically coated with the chiral MOC [Zn_(6)M_(4)] was also fabricated.The results showed that the chiral MOC exhibits excellent enantioselectivity not only in normal phase HPLC(NP-HPLC) and reversed phase(RP-HPLC) but also in GC,and various racemates were well separated,including alcohols,diols,esters,ketones,ethers,amines,and epoxides.Importantly,CSP-A and CSP-B are complementary to commercially available Chiralcel OD-H and Chiralpak AD-H columns in enantioseparation,which can separate some racemates that could not be or could not well be separated by the two widely used commercial columns,suggesting the great potential of the two prepared CSPs in enantioseparation.This work reveals that the chiral MOC is potential versatile chiral recognition materials for both HPLC and GC,and also paves the way to expand the potential applications of MOCs.展开更多
Due to complex ion-ion and ion-membrane interactions, creating innovative membrane structures to acquire favorable ion mixing effect and high separation performance remains a big challenge. Herein, we design covalent ...Due to complex ion-ion and ion-membrane interactions, creating innovative membrane structures to acquire favorable ion mixing effect and high separation performance remains a big challenge. Herein, we design covalent organic framework(COF) scaffold membrane with gate-lane nanostructure for efficient Li^(+)/Mg^(2+) separation. COF nanosheets, serving as the scaffold, are intercalated by polyethyleneimine(PEI) to form the permeating layer. Subsequently, PEI on the surface reacts with 1,4-phenylene diisocyanate to form the polyurea gating layer. The gating layer, bearing tailored smaller pore size,affords high rejection to co-ions(Mg^(2+)) and thus high Li^(+)/Mg^(2+) selectivity. The permeating layer, with asymmetric charge and spatial nanostructure for creating individual lanes of Li^(+) and Cl~-, facilitates Li^(+) transport and thus high Li^(+) permeability. The optimum COF scaffold membrane exhibits the permeance of 11.5 L m^(-2) h^(-1)/bar^(-1) and true selectivity of 231.9 with Li^(+) enrichment of 120.2% at the Mg^(2+)/Li^(+) mass ratio of 50, exceeding the ideal selectivity of 80.5 and outperforming all ever-reported positively charged nanofiltration membranes. Our work may stimulate the further thinking about how to design the hierarchical membrane structure to achieve favorable ion mixing effect and break the membrane permeability-selectivity trade-off in chemical separations.展开更多
Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical proper...Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical properties,leading to uncontrolled zinc(Zn)dendrite formation and undesirable side reactions.To address these limitations and enhance the electrochemical performance of AZIBs,a precisely designed functional separator is developed by incorporating UiO-66-(COOH)_(2)into a poly(vinylidene fluoride)(PVDF)framework(U-PVDF)via a direct in situ growth method.This approach enables uniform distribution of UiO-66-(COOH)_(2)both on the surface and within the PVDF backbone,without increasing separator thickness.Owing to the strong interaction between Zn^(2+)and the abundant carboxyl groups in UiO-66-(COOH)_(2),the U-PVDF separator regulates the Zn^(2+)solvation structure toward a contact ion pair-dominated structure by reducing coordinated water molecules,which effectively mitigates water-induced parasitic reactions and promotes compact Zn deposition.Consequently,a Zn/Zn symmetric cell employing the U-PVDF separator demonstrates superior cycling stability over 1500 cycles without internal short-circuiting at a current density of 6 mA cm^(−2)and an areal capacity of 2 mAh cm^(−2).Moreover,Zn/NaV_(3)O_(8)·xH_(2)O(NVO)cell with the U-PVDF separator exhibits markedly improved cyclability and rate performance compared with those using conventional GF separator.展开更多
The accumulation and circulation of carbon and hydrogen contribute to the chemical evolution of ice giant planets.Species separation and diamond precipitation have been reported in carbon-hydrogen systems and have bee...The accumulation and circulation of carbon and hydrogen contribute to the chemical evolution of ice giant planets.Species separation and diamond precipitation have been reported in carbon-hydrogen systems and have been verified by static and shock compression experiments.Nevertheless,the dynamic formation processes underlying these phenomena remain insufficiently understood.In combination with a deep learning model,we demonstrate that diamonds form through a three-step process involving dissociation,species separation,and nucleation processes.Under shock conditions of 125 GPa and 4590 K,hydrocarbons decompose to give hydrogen and low-molecular-weight alkanes(CH_(4) and C_(2)H_(6)),which escape from the carbon chains,resulting in C/H species separation.The remaining carbon atoms without C-H bonds accumulate and nucleate to form diamond crystals.The process of diamond growth is associated with a critical nucleus size at which the dynamic energy barrier plays a key role.These dynamic processes of diamond formation provide insight into the establishment of a model for the evolution of ice giant planets.展开更多
The effective separation and utilization of photo-generated carriers are of great significance for promoting the development of photocatalysis,especially in the coupled process of photocatalytic H_(2)production and va...The effective separation and utilization of photo-generated carriers are of great significance for promoting the development of photocatalysis,especially in the coupled process of photocatalytic H_(2)production and valueadded chemicals synthesis.To realize this goal,a sandwichstructured MnO_(2)@ZnIn_(2)S_(4)@Ti_(3)C_(2)hollow sphere was designed and synthesized,in which MnO_(2)and Ti_(3)C_(2)were loaded on the inner and outer surfaces of ZnIn_(2)S_(4),respectively.In the photocatalytic system,MnO_(2)as oxidation cocatalyst and Ti_(3)C_(2)as reduction cocatalyst can serve as photo-generated holes and electrons collectors,respectively,which boost the photo-generated carrier separation and create a spatially separated redox reaction.Furthermore,the unique hollow structure integrated into the photocatalytic system further endows a significant enhancement in light-harvesting ability.Remarkably,the optimal MnO_(2)@ZnIn_(2)S_(4)@Ti_(3)C_(2)hollow sphere exhibits an outstanding the photocatalytic activity for coupled H_(2)production(6.29 mmol g^(-1)h^(-1))and selective benzyl alcohol oxidation to benzaldehyde(5.26 mmol g^(-1)h^(-1)),which is significantly superior to that of ZnIn_(2)S_(4),MnO_(2)@ZnIn_(2)S_(4),and ZnIn_(2)S_(4)@Ti_(3)C_(2).By the in situ irradiated X-ray photoelectron spectroscopy,the result reveals that the spatially separated redox dual-cocatalysts can effectively impel the photo-generated carrier separation.Simultaneously,the intermediates during the benzyl alcohol oxidation process have also been confirmed through in situ electron paramagnetic resonance spectroscopy and diffuse reflectance infrared Fourier transform spectroscopy.This work provides a reference and inspiration for constructing efficient photocatalysts that achieve an efficient coupling of photocatalytic H_(2)production and value-added chemicals synthesis.展开更多
Water scarcity,exacerbated by organic micropollutant contamination and climate change,necessitates energy-efficient,eco-friendly purification technologies.Membrane separation has emerged as a transformative solution,o...Water scarcity,exacerbated by organic micropollutant contamination and climate change,necessitates energy-efficient,eco-friendly purification technologies.Membrane separation has emerged as a transformative solution,outperforming energyintensive processes,such as distillation.As highlighted in Nature,traditional chemical separations—dominated by distillation—consume 10%-15%of global energy,whereas advanced membrane technologies can reduce energy use by up to 90%.展开更多
基金supported by the National Natural Science Foundation of China(No.52277055).
文摘Traditional data-driven fault diagnosis methods depend on expert experience to manually extract effective fault features of signals,which has certain limitations.Conversely,deep learning techniques have gained prominence as a central focus of research in the field of fault diagnosis by strong fault feature extraction ability and end-to-end fault diagnosis efficiency.Recently,utilizing the respective advantages of convolution neural network(CNN)and Transformer in local and global feature extraction,research on cooperating the two have demonstrated promise in the field of fault diagnosis.However,the cross-channel convolution mechanism in CNN and the self-attention calculations in Transformer contribute to excessive complexity in the cooperative model.This complexity results in high computational costs and limited industrial applicability.To tackle the above challenges,this paper proposes a lightweight CNN-Transformer named as SEFormer for rotating machinery fault diagnosis.First,a separable multiscale depthwise convolution block is designed to extract and integrate multiscale feature information from different channel dimensions of vibration signals.Then,an efficient self-attention block is developed to capture critical fine-grained features of the signal from a global perspective.Finally,experimental results on the planetary gearbox dataset and themotor roller bearing dataset prove that the proposed framework can balance the advantages of robustness,generalization and lightweight compared to recent state-of-the-art fault diagnosis models based on CNN and Transformer.This study presents a feasible strategy for developing a lightweight rotating machinery fault diagnosis framework aimed at economical deployment.
基金supported by Scientific Research and Technology Development Project of CNPC(2021DJ4002,2022DJ3908).
文摘The numerical dispersion phenomenon in the finite-difference forward modeling simulations of the wave equation significantly affects the imaging accuracy in acoustic reflection logging.This issue is particularly pronounced in the reverse time migration(RTM)method used for shear-wave(S-wave)logging imaging.This not only affects imaging accuracy but also introduces ambiguities in the interpretation of logging results.To address this challenge,this study proposes the use of a least-squares difference coefficient optimization algorithm aiming to suppress the numerical dispersion phenomenon in the RTM of S-wave reflection imaging logging.By optimizing the difference coefficients,the high-precision finite-difference algorithm serves as an effective operator for both forward and backward RTM processes.This approach is instrumental in eliminating migration illusions,which are often caused by numerical dispersion.The effectiveness of this optimized algorithm is demonstrated through numerical results,which indicate that it can achieve more accurate forward imaging results across various conditions,including high-and low-velocity strata,and is effective in both large and small spatial grids.The results of processing real data demonstrate that numerical dispersion optimization effectively reduces migration artifacts and diminishes ambiguities in logging interpretations.This optimization offers crucial technical support to the RTM method,enhancing its capability for accurately modeling and imaging S-wave reflections.
基金supported by the Planned Project Grant(Grant No.3502Z20199064)from the Science and Technology Bureau of Xiamen(CN)the training project(Grant No.2020GGB067)of the youth and middle-aged talents of Fujian Provincial Health Commission(CN).
文摘This study explored the application value of iterative decomposition of water and fatwith echo asymmetry and least-squares estimation(IDEAL-IQ)technology in the early diagnosis of ageing osteoporosis(OP).172 participants were enrolled and underwentmagnetic resonance imaging(MRI)examinations on a 3.0T scanner.100 cases were included in the normal group(50 males and 50 females;mean age:45 years;age range:20e84 years).33 cases were included in the osteopenia group(17 males and 16 females;mean age:55 years;age range:43e83 years).39 caseswere includedintheOP group(19males and20females;meanage:58years;age range:48 e82 years).Conventional T1WI and T2WI were first obtained,followed by 3D-IDEAL-IQ-acqui-sition.Fat fraction(FF)and apparent transverse relaxation rate(R2*)resultswere automatically calculated from IDEAL-IQ-images on the console.Based on T1Wand T2W-images,300 ROIs for each participantweremanually delineated in L1-L5 vertebral bodies of five middle slices.In each age group of all normal subjects,each parameter was significantly correlated with gender.In male participants from the normal,osteopenia,and OP groups,statistical analysis revealed F values of 11319.292 and 180.130 for comparisons involving FF and R2*values,respectively(all p<0.0001).The sensitivity and specificity of FF values were 0.906 and 0.950,0.994 and 0.997,0.865 and 0.820,respectively.For R2*,they were 0.665 and 0.616,0.563 and 0.519,0.571 and 0.368,respectively.In female participants from the normal,osteopenia,and OP-groups,statis-tical analysis revealed F values of 12461.658 and 548.274 for comparisons involving FF and R2*values,respectively(all p<0.0001).The sensitivity and specificity of FF values were 0.985 and 0.991,0.996 and 0.996,0.581 and 0.678,respectively.For R2*,they were 0.698 and 0.730,0.603 and 0.665,0.622 and 0.525,respectively.Significant differences were indicated in the quanti-tative values among the three groups.FF value had good performance,while R2*value had poor performance indiscriminatingosteopenia andOP-groups.Overall,the IDEAL-IQ techniqueoffers specific reference indices that enable noninvasive and quantitative assessment of lumbar vertebrae bone metabolism,thereby providing diagnostic information for OP.
基金supported by the National Natural Science Foundation of China(22475240,22090061,22488101)the State Key Laboratory of Catalysis(2024SKL-A-010)。
文摘The separation of propylene(C_(3)H_(6))and propane(C_(3)H_(8))presents a significant industrial challenge due to their similar molecular dimensions and physicochemical properties.Among various separation methods,molecular sieving emerges as the most promising approach,but it will be significantly compromised at high temperatures due to the significant thermal motion.Here,we report a thermally robust zinc-based metal-organic framework(MOF)that can be synthesized on sub-kilogram scale and achieve exceptional C_(3)H_(6)/C_(3)H_(8) separation performances across a broad temperature range(298–353 K).Unlike conventional MOFs suffering from thermal lattice expansion to give poorer selectivity,this new MOF gives the adsorption capacity of C_(3)H_(6)essentially unchanged and that of C_(3)H_(8) negligible at elevated temperatures,outperforming most state-of-the-art adsorbents,in virtue of multiple hydrogen bonds at the aperture.Column breakthrough experiments confirmed the excellent separation capability,and showed no performance degradation over multi-round adsorption-desorption cycles at 353 K.This study addresses the critical challenge of the trade-off between temperature and selectivity in adsorptive separation,which offers new insights into the design of porous structures for highly effective separation at high temperatures.
基金the Scientific Research Projects Unit of Erciyes University under contract no:FDS-2022-11532 and FOA-2025-14773.
文摘This paper examines a model that combines vortex generators and leading-edge tubercles for controlling the laminar separation bubble(LSB)over an airfoil at low Reynolds numbers(Re).This new concept of passive flow control technique utilizing a tubercle and vortex generator(VG)close to the leading edge was analyzed numerically for a NACA0015 airfoil.In this study,the Shear Stress Transport(SST)turbulence model was employed in the numerical modelling.Numerical modelling was completed using the ANSYS-Fluent 18.2 solver.Analyses were conducted to investigate the flow pattern and understand the underlying LSB control phenomena that enabled the new passive flow control method to provide this significant performance benefit.The findings indicated that the new concept of passive flow control technique suppressed the formation of an LSB at the suction surface of the NACA0015 airfoil,resulting in a higher lift coefficient and improved aerodynamic performance.Improvements in LSB dynamics and aerodynamic performance through the passive flow control method lead to increased energy output and enhanced stability.
基金supported by Shaanxi Key Research and Development Program(No.2024SF-YBXM-546)the National Natural Science Foundation of China(No.52470161)the State Key Laboratory of Pollution Control and Resource Reuse Foundation(No.PCRRF21007).
文摘With the legislative development,the organic and inorganic composition separation has become the primary requirement for sewer sediment disposal,however the relevant technology has been rarely reported and the driving mechanism was still unclear.In this study,direct disintegration of biopolymers and indirect broken of connection point were investigated on the hydrolysis and component separation.Three typical sewer sediment treatment approaches,i.e.,alkaline,thermal and cation exchange treatments were proposed,which represented the hydrolysis-driving forces of chemical hydrolysis,physical hydrolysis and innovative cation bridging break-age.The results showed that the organic and inorganic separation rates of sewer sediment driven by alkaline,thermal and cation exchange treatments reached 21.26%,23.80%,and 19.56%-48.0%,respectively,compared to 4.43%in control.The secondary structure of proteins was disrupted,transitioning from𝛼α-helix to𝛽β-turn and random coil.Meanwhile,much biopolymers were released from solid to the liquid phase.From thermody-namic perspective,sewer sediment deposition was controlled by short-range interfacial interactions described by extended Derjaguin-Landau-Verwey-Overbeek theory.Additionally,the separation of organic and inorganic components was positively correlated with the thermodynamic parameters(Corr=0.87),highlighted the robust-ness of various driving forces.And the flocculation energy barriers were 2.40(alkaline),1.60 times(thermal),and 4.02–4.97 times(cation exchange)compared to control group.The findings revealed the contrition differ-ence of direct disintegration of gelatinous biopolymers and indirect breakage of composition connection sites in sediment composition separation,filling the critical gaps in understanding the specific mechanisms of sediment biopolymer disintegration and intermolecular connection breakage.
基金the support of the Major Science and Technology Project of Yunnan Province,China(Grant No.202502AD080007)the National Natural Science Foundation of China(Grant No.52378288)。
文摘Vehicle-induced response separation is a crucial issue in structural health monitoring(SHM).This paper proposes a block-wise sliding recursive wavelet transform algorithm to meet the real-time processing requirements of monitoring data.To extend the separation target from a fixed dataset to a continuously updating data stream,a block-wise sliding framework is first developed.This framework is further optimized considering the characteristics of real-time data streams,and its advantage in computational efficiency is theoretically demonstrated.During the decomposition and reconstruction processes,information from neighboring data blocks is fully utilized to reduce algorithmic complexity.In addition,a delay-setting strategy is introduced for each processing window to mitigate boundary effects,thereby balancing accuracy and efficiency.Simulated signal experiments are conducted to determine the optimal delay configuration and to verify the algorithm’s superior performance,achieving a lower Root Mean Square Error(RMSE)and only 0.0249 times the average computational time compared with the original algorithm.Furthermore,strain signals from the Lieshi River Bridge are employed to validate the method.The proposed algorithm successfully separates the static trend from vehicle-induced responses in real time across different sampling frequencies,demonstrating its effectiveness and applicability in real-time bridge monitoring.
基金supported by the National Natural Science Foundation of China (52172228)the Natural Science Foundation of Fujian Province (2024J01475 and 2023J05127)
文摘Lithium-sulfur batteries(LSBs)represent a next-generation energy storage technology,but widespread applications are restricted by the shuttle of lithium polysulfides(LiPSs).The rational design of separators has been demonstrated to be one of the most efficient and cost-effective strategies to curb the shuttle effect,and tremendous research progress has been achieved.The efficiency of a separator depends on its interaction with LiPSs,which is governed by the surface energy and binding strength.Despite several review works that have been reported to advance the separators,most of them primarily focus on active material innovation and construction.The most crucial issues of surface binding energy have not been systematically reviewed,limiting the precise design of efficient separators.In this review,fundamentals related to surface energy and binding interactions with LiPSs are comprehensively analyzed and discussed.With surface binding and energy main lines,the advancements in separator engineering strategies are elaborately summarized and discussed.Moreover,techniques for evaluating affinity to LiPSs are thoroughly analyzed to avoid any ambiguities in measurement.Based on the research context,valuable research directions are suggested to construct efficient separators.This work provides guidelines to regulate the surface binding and energy of separators for high-performance LSBs.
基金supported by the National Natural Science Foundation of China(No.22375063)Science and Technology Commission of Shanghai Municipality(No.23JC140170O)the Fundamental Research Funds for the Central Universities.
文摘Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science.Recently,supramolecular polymeric materials(SPMs)have drawn increased attention due to their unique properties and potential applications in self-healing,shape memory,sensors,and flexible electronics.Here,we develop an ionic cluster-optimized microphase separation strategy to enhance the toughening and energy dissipation capabilities of polydisulfide-based supramolecular polymers.The mechanical properties,including Young's modulus and toughness,are significantly improved by integrating the quadruple H-bonding 2-ureido-4-pyrimidone(UPy)induced microphase separation with iron(III)-to-carboxylate ionic clusters.By combining established chemical approaches with adjustable polymer phase ratios,it is revealed that the synergistic effect of these factors expands the interchain spacing,facilitates the formation of microphase domains,and enhances the tolerance of polythioctic acid-based polymers to external mechanical and thermal stimuli,meeting the practical requirements for industrial plastic applications.Moreover,the UPy-functionalized polymers incorporating iron carboxylate clusters exhibit good one-way shape memory behavior with practical applicability at a relatively low recovery temperature.Our work demonstrates a novel strategy for constructing industrially viable shape memory dynamic SPMs and paves the way for future innovations in developing SPMs.
基金supported by the China Institute of Atomic Energy。
文摘The removal of trace plutonium(Pu)from uranium products and organic wastes during spent nuclear fuel reprocessing remains a critical challenge,resulting in excessive plutonium content in uranium products and waste organic liquid.Currently,most organic ligands with selective separation functions are lipophilic,while research on water-soluble,highly selective ligands is relatively scarce,and there are also few reports on the single crystal of these ligands coordinating with plutonium.Herein,a hydrophilic multiamide ligand,N,N,N′,N″,N″-hexaethyl-nitrilotriacetamide(NTAamideC2),was synthesized and evaluated for its Pu(Ⅳ)back-extraction efficiency under harsh conditions.Systematic experiments revealed that NTAamideC2 achieved>99%Pu(Ⅳ)back-extraction rate within 15 min across a wide nitric acid concentration range(0-5 M),even with elevated dibutyl phosphate(DBP≤20000 ppm).Remarkably,the separation factor(SFPu/U)reached 767 at 1.5 M HNO_(3),demonstrating exceptional selectivity over uranium(Ⅵ).Spectrophotometric titration and DFT calculations confirmed the formation of 1:1 and 1:2 Pu(Ⅳ)-NTAamideC2 complexes,with log β values of 7.42±0.01 and 13.23±0.02,respectively.Single-crystal X-ray diffraction analysis of{[Pu_(2)(H_(2)O)_(2)(NTAamideC2)_(4)](H_(2)O)_(2)(NO_(3))(ClO_(4))_(7)}revealed a nine-coordinated PuO_(7)N_(2)geometry,where two NTAamideC2 molecules bind via six O and two N atoms.Compared to conventional agents(AHA/HSC),NTAamideC2 exhibited superior acid tolerance and selectivity,aligning with the CHON principle for sustainable nuclear waste management.This work provides a robust strategy for Pu(Ⅳ)removal in uranium purification cycles and advances fundamental insights into Pu coordination chemistry,offering significant potential for industrial nuclear fuel reprocessing.
文摘Objective:To analyze the impact of maternal-infant separation on the physical and mental state of high-risk pregnancy patients and explore the clinical efficacy of targeted nursing interventions.Methods:A total of 80 high-risk pregnancy patients treated in our hospital from January 2023 to January 2024 were selected as the study subjects.These patients were randomly divided into an observation group and a control group(40 cases each)using a random number table.The control group received routine high-risk pregnancy nursing care,while the observation group received specialized maternal-infant separation nursing interventions in addition to routine care.The psychological and physiological states and nursing satisfaction of the two groups were compared before and after the intervention.Results:The SAS scores,SDS scores,and sleep quality scores of the observation group were significantly lower than those of the control group,with statistically significant differences(p<0.05).The incidence of postpartum hemorrhage in the observation group was significantly lower than that in the control group,and the initiation time of lactation was significantly earlier than that in the control group,with both differences being statistically significant(p<0.05).The nursing satisfaction of the observation group was significantly higher than that of the control group(80%vs.32/40),with a statistically significant difference(p<0.05).Conclusion:Maternal-infant separation exacerbates anxiety and depression in high-risk pregnancy patients,reduces sleep quality,increases the risk of postpartum hemorrhage,and delays the initiation of lactation.Specialized nursing interventions for maternal-infant separation can improve the physical and mental state of high-risk pregnancy patients,reduce the incidence of postpartum complications,and enhance nursing satisfaction,making them worthy of clinical application and promotion.
基金the financial support from the Natural Science Foundation of Jiangsu Province(BK20231292)the Jiangsu Agricultural Science and Technology Innovation Fund(CX(24)3091)+6 种基金the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX25_1429)the National Key R&D Program of China(2024YFE0109200)the Fundamental Research Funds for the Central Universities(No.2024300440)Guangdong Basic and Applied Basic Research Foundation(2025A1515011098)the National Natural Science Foundation of China(12464032)the Natural Science Foundation of Jiangxi Province(20232BAB201032)Ji'an Science and Technology Plan Project(2024H-100301)。
文摘Zn-I_(2) batteries have emerged as promising next-generation energy storage systems owing to their inherent safety,environmental compatibility,rapid reaction kinetics,and small voltage hysteresis.Nevertheless,two critical challenges,i.e.,zinc dendrite growth and polyiodide shuttle effect,severely impede their commercial viability.To conquer these limitations,this study develops a multifunctional separator fabricated from straw-derived carboxylated nanocellulose,with its negative charge density further reinforced by anionic polyacrylamide incorporation.This modification simultaneously improves the separator’s mechanical properties,ionic conductivity,and Zn^(2+)ion transfer number.Remarkably,despite its ultrathin 20μm profile,the engineered separator demonstrates exceptional dendrite suppression and parasitic reaction inhibition,enabling Zn//Zn symmetric cells to achieve impressive cycle life(>1800 h at 2 m A cm^(-2)/2 m Ah cm^(-2))while maintaining robust performance even at ultrahigh areal capacities(25 m Ah cm^(-2)).Additionally,the separator’s anionic characteristic effectively blocks polyiodide migration through electrostatic repulsion,yielding Zn-I_(2) batteries with outstanding rate capability(120.7 m Ah g^(-1)at 5 A g^(-1))and excellent cyclability(94.2%capacity retention after 10,000 cycles).And superior cycling stability can still be achieved under zinc-deficient condition and pouch cell configuration.This work establishes a new paradigm for designing high-performance zinc-based energy storage systems through rational separator engineering.
基金supported by the National Science Fund for Distinguished Young Scholars(21925603)the National Natural Science Foundation of China(22306185)the China Postdoctoral Science Foundation(2023M732032)。
文摘Conventional electrolytic methods for separating chemically similar lanthanides(Ln)and actinides(An)are limited by thermodynamics and slow reaction kinetics,restricting their efficiency in rare-earth refining and nuclear fuel recycling.Herein,we report an electroextraction and oxidative back-extraction(EOB)strategy utilizing a LiCl-KCl-KAlCl_(4) molten salt that overcomes these limitations by leveraging divergent interfacial reactivity.The EOB process achieves an exceptional separation factor for Ln/An(>1000),while simultaneously increasing the separation rate by at least one order of magnitude.Through in-situ synchrotron radiation X-ray micro-computed tomography(SR-μCT)and X-ray diffraction(SR-XRD),we capture selective oxidation-induced destabilization of Ln-Al alloys while actinides retain phase stability-directly visualizing the electrochemical alloy transition mechanism.This research redefines the separation of f-block elements in molten salt systems and introduces a multimodal approach to investigating transient interfacial phenomena that are usually inaccessible to conventional metallurgical diagnostics under extreme conditions.
基金supported by the Fundamental Research Funds for the Central Universities(No.2025JC008)the National Natural Science Foundation of China(grant number 52176105)+2 种基金the Science and Technology Project of Hebei Education Department-China(BJK2022063)the Hebei Natural Science Foundation-China(grant number E2025502038)the Funding Program for Cultivating Innovative Abilities of Graduate Students in Hebei Province of China(CXZZBS2025184).
文摘Biochar has been widely recognized as a promising solid CO_(2)adsorbent with economic and ecological benefits.Industrial CO_(2)emissions originate from diverse sources,while the pore structure and chemical functional groups of biochar exhibit varying degrees of influence on CO_(2)adsorption and separation performance under different adsorption conditions.Therefore,exploring the matching relationship between the physicochemical properties of biochar and its adsorption and separation performance at different adsorption conditions is essential for the development and optimization of carbon-based adsorbents.This study selected the high-performance extreme gradient boosting(XGB)algorithm from various algorithms and utilized it to develop CO_(2),N_(2),CH_(4)adsorption prediction models.Based on this,coupled prediction models were developed for CO_(2)/N_(2)and CO_(2)/CH_(4)adsorption selectivity.Furthermore,feature importance and partial dependence analysis were performed using SHAP values.The results indicate that during CO_(2)adsorption,the influence of the pore structure of biochar outweighs that of its chemical composition.Specifically,the pore structure of 0.4–0.6 nm is the most important property influencing CO_(2)adsorption at low and medium pressure(0–0.6 bar),and the pore structure of 0.6–0.8 nm,as well as the specific surface area contribute the most at high pressure(0.6–1 bar).During CO_(2)selective separation,the CO_(2)/N_(2)mixture is primarily separated through the selective adsorption of CO_(2)by nitrogen functional groups.In contrast,for CO_(2)/CH_(4)mixtures,pore structure<1 nm plays a more critical role in determining adsorption selectivity.In addition,molecular simulation studies further revealed the adsorption filling mechanisms of CO_(2)molecules within different pore sizes and functional groups.Finally,nitrogen-doped biochar was synthesized using de-alkalize lignin as the precursor,KOH as the activating agent,and urea as the nitrogen dopant.CO_(2),N_(2),and CH_(4)isothermal adsorption experiments were conducted,and the experimental results confirmed that the developed prediction models exhibit high accuracy(R^(2)>0.9).
基金supported by the National Natural Science Foundation of China (Nos.22064020,22364022,and 22174125)the Applied Basic Research Foundation of Yunnan Province (Nos.202101AT070101 and 202201AT070029)。
文摘Developing a chiral material as versatile and universal chiral stationary phase(CSP) for chiral separation in diverse chromatographic techniques simultaneously is of great significance.In this study,we demonstrated for the first time that a chiral metal-organic cage(MOC),[Zn_(6)M_(4)],as a universal chiral recognition material for both multi-mode high-performance liquid chromatography(HPLC) and capillary gas chromatography(GC) enantioseparation.Two novel HPLC CSPs with different bonding arms(CSP-A with a cationic imidazolium bonding arm and CSP-B with an alkyl chain bonding arm) were prepared by clicking of functionalized chiral MOC [Zn_(6)M_(4)] onto thiolated silica via thiol-ene click chemistry.Meanwhile,a capillary GC column statically coated with the chiral MOC [Zn_(6)M_(4)] was also fabricated.The results showed that the chiral MOC exhibits excellent enantioselectivity not only in normal phase HPLC(NP-HPLC) and reversed phase(RP-HPLC) but also in GC,and various racemates were well separated,including alcohols,diols,esters,ketones,ethers,amines,and epoxides.Importantly,CSP-A and CSP-B are complementary to commercially available Chiralcel OD-H and Chiralpak AD-H columns in enantioseparation,which can separate some racemates that could not be or could not well be separated by the two widely used commercial columns,suggesting the great potential of the two prepared CSPs in enantioseparation.This work reveals that the chiral MOC is potential versatile chiral recognition materials for both HPLC and GC,and also paves the way to expand the potential applications of MOCs.
基金financial support from the National Natural Science Foundation of China (22338011, 22378299)Hainan Province Science and Technology Special Fund (ZDYF2025SHFZ025)+1 种基金Ningbo Key Research and Development Project (2022Z121)the China Postdoctoral Science Foundation (2025M771194)。
文摘Due to complex ion-ion and ion-membrane interactions, creating innovative membrane structures to acquire favorable ion mixing effect and high separation performance remains a big challenge. Herein, we design covalent organic framework(COF) scaffold membrane with gate-lane nanostructure for efficient Li^(+)/Mg^(2+) separation. COF nanosheets, serving as the scaffold, are intercalated by polyethyleneimine(PEI) to form the permeating layer. Subsequently, PEI on the surface reacts with 1,4-phenylene diisocyanate to form the polyurea gating layer. The gating layer, bearing tailored smaller pore size,affords high rejection to co-ions(Mg^(2+)) and thus high Li^(+)/Mg^(2+) selectivity. The permeating layer, with asymmetric charge and spatial nanostructure for creating individual lanes of Li^(+) and Cl~-, facilitates Li^(+) transport and thus high Li^(+) permeability. The optimum COF scaffold membrane exhibits the permeance of 11.5 L m^(-2) h^(-1)/bar^(-1) and true selectivity of 231.9 with Li^(+) enrichment of 120.2% at the Mg^(2+)/Li^(+) mass ratio of 50, exceeding the ideal selectivity of 80.5 and outperforming all ever-reported positively charged nanofiltration membranes. Our work may stimulate the further thinking about how to design the hierarchical membrane structure to achieve favorable ion mixing effect and break the membrane permeability-selectivity trade-off in chemical separations.
基金supported by the Basic Science Research Program(RS-2024-00455177)through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT.
文摘Aqueous zinc ion batteries(AZIBs)are considered promising candidates owing to their inherent safety and low cost.However,the conventional glass fiber(GF)separator used in AZIBs suffers from poor physicochemical properties,leading to uncontrolled zinc(Zn)dendrite formation and undesirable side reactions.To address these limitations and enhance the electrochemical performance of AZIBs,a precisely designed functional separator is developed by incorporating UiO-66-(COOH)_(2)into a poly(vinylidene fluoride)(PVDF)framework(U-PVDF)via a direct in situ growth method.This approach enables uniform distribution of UiO-66-(COOH)_(2)both on the surface and within the PVDF backbone,without increasing separator thickness.Owing to the strong interaction between Zn^(2+)and the abundant carboxyl groups in UiO-66-(COOH)_(2),the U-PVDF separator regulates the Zn^(2+)solvation structure toward a contact ion pair-dominated structure by reducing coordinated water molecules,which effectively mitigates water-induced parasitic reactions and promotes compact Zn deposition.Consequently,a Zn/Zn symmetric cell employing the U-PVDF separator demonstrates superior cycling stability over 1500 cycles without internal short-circuiting at a current density of 6 mA cm^(−2)and an areal capacity of 2 mAh cm^(−2).Moreover,Zn/NaV_(3)O_(8)·xH_(2)O(NVO)cell with the U-PVDF separator exhibits markedly improved cyclability and rate performance compared with those using conventional GF separator.
基金supported by the National Natural Science Foundation of China(Grant Nos.12534013,12047561,and 12104507)the Science and Technology Innovation Program of Hunan Province(Grant Nos.2025ZYJ001 and 2021RC4026)the National University of Defense Technology Research Fund Project.
文摘The accumulation and circulation of carbon and hydrogen contribute to the chemical evolution of ice giant planets.Species separation and diamond precipitation have been reported in carbon-hydrogen systems and have been verified by static and shock compression experiments.Nevertheless,the dynamic formation processes underlying these phenomena remain insufficiently understood.In combination with a deep learning model,we demonstrate that diamonds form through a three-step process involving dissociation,species separation,and nucleation processes.Under shock conditions of 125 GPa and 4590 K,hydrocarbons decompose to give hydrogen and low-molecular-weight alkanes(CH_(4) and C_(2)H_(6)),which escape from the carbon chains,resulting in C/H species separation.The remaining carbon atoms without C-H bonds accumulate and nucleate to form diamond crystals.The process of diamond growth is associated with a critical nucleus size at which the dynamic energy barrier plays a key role.These dynamic processes of diamond formation provide insight into the establishment of a model for the evolution of ice giant planets.
基金supported by the National Natural Science Foundation of China(52202102,52472215)Key Innovation Project of the Science-Education-Industry Integration Pilot Engineering of Qilu University of Technology(Shandong Academy of Sciences)(2025ZDZX08)+1 种基金Key Research&Development Project of Shandong Province(2024TSGC0222)Interdisciplinary Innovation Guidance Program from Qilu University of Technology(Shandong Academy of Sciences)(2025XKJC0103)。
文摘The effective separation and utilization of photo-generated carriers are of great significance for promoting the development of photocatalysis,especially in the coupled process of photocatalytic H_(2)production and valueadded chemicals synthesis.To realize this goal,a sandwichstructured MnO_(2)@ZnIn_(2)S_(4)@Ti_(3)C_(2)hollow sphere was designed and synthesized,in which MnO_(2)and Ti_(3)C_(2)were loaded on the inner and outer surfaces of ZnIn_(2)S_(4),respectively.In the photocatalytic system,MnO_(2)as oxidation cocatalyst and Ti_(3)C_(2)as reduction cocatalyst can serve as photo-generated holes and electrons collectors,respectively,which boost the photo-generated carrier separation and create a spatially separated redox reaction.Furthermore,the unique hollow structure integrated into the photocatalytic system further endows a significant enhancement in light-harvesting ability.Remarkably,the optimal MnO_(2)@ZnIn_(2)S_(4)@Ti_(3)C_(2)hollow sphere exhibits an outstanding the photocatalytic activity for coupled H_(2)production(6.29 mmol g^(-1)h^(-1))and selective benzyl alcohol oxidation to benzaldehyde(5.26 mmol g^(-1)h^(-1)),which is significantly superior to that of ZnIn_(2)S_(4),MnO_(2)@ZnIn_(2)S_(4),and ZnIn_(2)S_(4)@Ti_(3)C_(2).By the in situ irradiated X-ray photoelectron spectroscopy,the result reveals that the spatially separated redox dual-cocatalysts can effectively impel the photo-generated carrier separation.Simultaneously,the intermediates during the benzyl alcohol oxidation process have also been confirmed through in situ electron paramagnetic resonance spectroscopy and diffuse reflectance infrared Fourier transform spectroscopy.This work provides a reference and inspiration for constructing efficient photocatalysts that achieve an efficient coupling of photocatalytic H_(2)production and value-added chemicals synthesis.
文摘Water scarcity,exacerbated by organic micropollutant contamination and climate change,necessitates energy-efficient,eco-friendly purification technologies.Membrane separation has emerged as a transformative solution,outperforming energyintensive processes,such as distillation.As highlighted in Nature,traditional chemical separations—dominated by distillation—consume 10%-15%of global energy,whereas advanced membrane technologies can reduce energy use by up to 90%.
