We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-o...We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-of-plane negative Poisson's ratio(NPR)phenomenon,originating from its special sawtooth-like structure.The absolute value of the NPR decreases as the number of layers increases.The adsorption of volatile organic compounds(VOCs)including CH_(2)O,C_(2)H_(3)Cl and C_(6)H_(6)by AlO_(2)exhibit small adsorption distance,large adsorption energy,large charge transfer and significant density of states(DOS)changes,indicating the presence of strong interactions.The desorption time of each gas molecule on the AlO_(2)surface is also evaluated,and the results further suggest that the desorption of VOCs can be controlled by changing the temperature to achieve the recycling of AlO_(2).These interesting properties make 2D AlO_(2)a promising material for electronic,mechanical and sensing applications for VOCs.展开更多
The diagnostic efficacy of contemporary bioimaging technologies remains constrained by inherent limitations of conventional imaging agents,including suboptimal sensitivity,off-target biodistribution,and inherent cytot...The diagnostic efficacy of contemporary bioimaging technologies remains constrained by inherent limitations of conventional imaging agents,including suboptimal sensitivity,off-target biodistribution,and inherent cytotoxicity.These limitations have catalyzed the development of intelligent stimuli-responsive block copolymers-based bioimaging agents,which was engineered to dynamically respond to endogenous biochemical cues(e.g.,p H gradients,redox potential,enzyme activity,hypoxia environment) or exogenous physical triggers(e.g.,photoirradiation,thermal gradients,ultrasound(US)/magnetic stimuli).Through spatiotemporally controlled structural transformations,stimuli-responsive block copolymers enable precise contrast targeting,activatable signal amplification,and theranostic integration,thereby substantially enhancing signal-to-noise ratios of bioimaging and diagnostic specificity.Hence,this mini-review systematically examines molecular engineering principles for designing p H-,redox-,enzyme-,light-,thermo-,and US/magnetic-responsive polymers,with emphasis on structure-property relationships governing imaging performance modulation.Furthermore,we critically analyze emerging strategies for optical imaging,US synergies,and magnetic resonance imaging(MRI).Multimodal bioimaging has also been elaborated,which could overcome the inherent trade-offs between resolution,penetration depth,and functional specificity in single-modal approaches.By elucidating mechanistic insights and translational challenges,this mini-review aims to establish a design framework of stimuli-responsive block copolymersbased for high fidelity bioimaging agents and accelerate their clinical translation in precise diagnosis and therapy.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 increase...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
To address the zero-sample challenge in preparation parameter design for newly developed alloys,a novel machine learning strategy that integrates basic dataset construction with Bayesian optimization,was proposed.The ...To address the zero-sample challenge in preparation parameter design for newly developed alloys,a novel machine learning strategy that integrates basic dataset construction with Bayesian optimization,was proposed.The impact of basic sample dataset construction methods,optimization benchmarks and multi-objective utility functions on Bayesian optimization was investigated.It was found that the combination of orthogonal design,linear benchmark,and shifted multiplicative utility function exhibits the best optimization performance.The strategy was then applied to a new Cu-Ni-Co-Si alloy with ultra-low Co content(0.7 wt.%Co),previously designed by our research team.Rapid optimization of six preparation parameters in the two-stage deformation and aging process of the zero-sample alloy was achieved through only 23 experiments.The measured ultimate tensile strength and electrical conductivity of the new alloy were 878 MPa and 44.0%(IACS),respectively,reaching the comprehensive performance level of the Cu-Ni-Co-Si alloy(C70350 alloy)containing 1.0-2.0 wt.%Co.展开更多
As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This stud...As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This study prepared surface polarity-modified ACF using the heteroatom doping method.The modified ACF possessed a richer array of strongly polar oxygen/nitrogen-containing functional groups(primarily phenolic hydroxyl and lactone groups),a larger specific surface are1,and a more developed micropore structure.The adsorption capacities of ethanol for O-ACF and N-ACF were 4.110 mmol/g and 1.698 mmol/g,respectively,which were 11.3 times and 4.7 times those of unmodified ACF.This was a significant improvement over our previous work(0.363 mmol/g).The improvement of adsorption capacity for the N-ACF was mainly due to the higher specific surface are1,greater number of micropores(more adsorption sites)and abundant existence of defects,whereas,for O-ACF,the improvement mainly relied on the abundant presence of oxygen-containing functional groups on the surface.However,water had a negative effect on the adsorption of ethanol for the modified ACF due to competitive adsorption and the disappearance of capillary condensation.It was further revealed that the adsorption process of ethanol and water was quite different.It obeyed the linear driving force(LDF)model for ethanol adsorption,however,the intraparticle diffusion(IPD)model for water adsorption.展开更多
As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term...As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference.To overcome these issues,we design three diketopyrrolopyrrole-based covalent organic frameworks(COFs)via a synergisticπ-extended lock and carboxyl-functionalized anchor molecular engineering strategy.Among them,TPy-DPP-COF features a covalently lockedπ-conjugated structure that enhances planarity,optimizes energy alignment,and minimizes exciton binding energy,thereby promoting charge transfer and suppressing recombination.Concurrently,carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation.These features contribute to the outstanding performance of TPy-DPP-COF,which achieves a high uranium adsorption capacity of 16.33 mg g−1 in natural seawater under irradiation,with only 29.3%capacity loss after 10 cycles,surpassing industrial benchmarks.Density functional theory(DFT)calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway,with DPP units acting as active sites for uranium reduction.This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.展开更多
Machine learning-assisted methods for rapid and accurate prediction of temperature field,mushy zone,and grain size were proposed for the heating−cooling combined mold(HCCM)horizontal continuous casting of C70250 alloy...Machine learning-assisted methods for rapid and accurate prediction of temperature field,mushy zone,and grain size were proposed for the heating−cooling combined mold(HCCM)horizontal continuous casting of C70250 alloy plates.First,finite element simulations of casting processes were carried out with various parameters to build a dataset.Subsequently,different machine learning algorithms were employed to achieve high precision in predicting temperature fields,mushy zone locations,mushy zone inclination angle,and billet grain size.Finally,the process parameters were quickly optimized using a strategy consisting of random generation,prediction,and screening,allowing the mushy zone to be controlled to the desired target.The optimized parameters are 1234℃for heating mold temperature,47 mm/min for casting speed,and 10 L/min for cooling water flow rate.The optimized mushy zone is located in the middle of the second heat insulation section and has an inclination angle of roughly 7°.展开更多
Graphene is a two-dimensional nanomaterial with huge surface area,high carrier mobility and high mechanical strength.Because of its great potential in nanotechnology and environmental protection,it has attracted much ...Graphene is a two-dimensional nanomaterial with huge surface area,high carrier mobility and high mechanical strength.Because of its great potential in nanotechnology and environmental protection,it has attracted much attention in environmental and energy fields since its discovery in 2004.Although graphene is a star material,many reviews have introduced its use in terms of energy,the research progress in the field of environment,especially water pollution control,has been rarely reported.Here,we review exhaustively the research progress of graphene-based materials in environmental pollution remediation in the past ten years.Firstly,the advantages and classification of graphene were introduced.Secondly,the research progress and main achievements of graphene and its composites in the fields of photocatalytic degradation,pollutant adsorption and water treatment were emphatically described,and the mechanism of action in the above fields was summarized.Finally,we discuss the problems existing in the preparation and summarize the application of graphene in the environment.展开更多
This paper expatiates on domestic status of heavy steel casting production, with a special focus on hydraulicturbine castings for Three Gorges Project. In China, there is magnificent demand for heavy castings with the...This paper expatiates on domestic status of heavy steel casting production, with a special focus on hydraulicturbine castings for Three Gorges Project. In China, there is magnificent demand for heavy castings with the rapidgrowth of the national economy in recent years and the expected high growth in the coming 10 to 20 years. Someheavy and large castings such as mill housing and hydraulic turbine runner crown, blade and band for Three GorgesProject have been successfully made. However, the domestic production capability is still far from meeting the giganticrequirements. The domestic capability still lags behind the world class level, and a lot of heavy castings still dependon import. The paper also gives a particular introduction of the key technologies in the manufacturing of heavy steelcastings like metal melting, foundry technology, heat treatment technology and numerical simulation technique, etc.In addition, several case studies on the application of numerical simulation in the production of heavy steel castingsare presented.展开更多
Fiber reinforced lattice composites are lightweight attractive due to their high specific strength and specific stiffness.In the past 10 years,researchers developed three-dimensional（3D） lattice trusses and two-dime...Fiber reinforced lattice composites are lightweight attractive due to their high specific strength and specific stiffness.In the past 10 years,researchers developed three-dimensional（3D） lattice trusses and two-dimensional （2D） lattice grids by various methods including interlacing, weaving,interlocking,filament winding and molding hot- press.The lattice composites have been applied in the fields of radar cross-section reduction,explosive absorption and heat-resistance. In this paper,topologies of the lattice composites, their manufacturing routes,as well as their mechanical and multifunctional applications,were surveyed.展开更多
It has been widely recognized that hole transporting materials(HTMs)play a key role in the rapid progress of perovskite solar cells(PVSCs).However,common organic HTMs such as spiro-OMe TAD not only suffer from high sy...It has been widely recognized that hole transporting materials(HTMs)play a key role in the rapid progress of perovskite solar cells(PVSCs).However,common organic HTMs such as spiro-OMe TAD not only suffer from high synthetic costs,but also usually require the additional chemical doping process to improve their hole transport ability,which unfortunately induces the terrible stability issue.Therefore,it is urgent to develop low-cost dopant-free HTMs for efficient and stable PVSCs.In this work,we have successfully developed a new class of efficient dopant-free fluoranthene-based HTMs(TPF1–5)with quite low lab synthetic costs by combining donor-acceptor and branched structure designs.The detailed structure-property study revealed that tuning the twisted arms at different substitution sites would regulate the intermolecular interactions and film-forming ability,thereby significantly affecting the performance of the HTMs.By applying these HTMs in conventional PVSCs,the dopant-free TPF1-based devices not only achieved the best efficiency of 21.76%,which is comparable to that of the doped spiro-OMeTAD control devices,but also showed much better operational stability,which maintained over 87%of the initial efficiency under maximum power point tracking after 1038 h.展开更多
Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-perform...Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.展开更多
Digital modeling and autonomous control of the die forging process are significant challenges in realizing high-quality intelli-gent forging of components.Using the die forging of AA2014 aluminum alloy as a case study...Digital modeling and autonomous control of the die forging process are significant challenges in realizing high-quality intelli-gent forging of components.Using the die forging of AA2014 aluminum alloy as a case study,a machine-learning-assisted method for di-gital modeling of the forging force and autonomous control in response to forging parameter disturbances was proposed.First,finite ele-ment simulations of the forging processes were conducted under varying friction factors,die temperatures,billet temperatures,and for-ging velocities,and the sample data,including process parameters and forging force under different forging strokes,were gathered.Pre-diction models for the forging force were established using the support vector regression algorithm.The prediction error of F_(f),that is,the forging force required to fill the die cavity fully,was as low as 4.1%.To further improve the prediction accuracy of the model for the ac-tual F_(f),two rounds of iterative forging experiments were conducted using the Bayesian optimization algorithm,and the prediction error of F_(f) in the forging experiments was reduced from 6.0%to 1.5%.Finally,the prediction model of F_(f) combined with a genetic algorithm was used to establish an autonomous optimization strategy for the forging velocity at each stage of the forging stroke,when the billet and die temperatures were disturbed,which realized the autonomous control in response to disturbances.In cases of−20 or−40℃ reductions in the die and billet temperatures,forging experiments conducted with the autonomous optimization strategy maintained the measured F_(f) around the target value of 180 t,with the relative error ranging from−1.3%to+3.1%.This work provides a reference for the study of di-gital modeling and autonomous optimization control of quality factors in the forging process.展开更多
Many strategies have been proposed to produce arenes from lignin as liquid fuel additives.However,the development of these methods is limited by the low yield of products,low atom utilization,and inefficient lignin de...Many strategies have been proposed to produce arenes from lignin as liquid fuel additives.However,the development of these methods is limited by the low yield of products,low atom utilization,and inefficient lignin depolymerization.Herein,we develop an energy-efficient synthetic method for the production of high-carbon-number arenes from sustainable lignin with a total yield of 23.1 wt%.Particularly,high carbon number arenes are obtained by fully utilizing the formaldehyde stabilizing additive and the methoxy group in lignin.The process begins with the reductive depolymerization of formaldehyde-stabilized lignin,followed by transmethylation between lignin monomers over Au/Nb_(2)O_(5) catalyst,and the Ru/Nb2O5-catalyzed hydrodeoxygenation.This work demonstrates the potential of value-added arenes production directly from lignin.展开更多
Solute atoms and precipitates significantly influence the mechanical properties of Mg alloys.Previous studies have mainly focused on the segregation behaviors of Mg alloys after annealing.In this study,we investigated...Solute atoms and precipitates significantly influence the mechanical properties of Mg alloys.Previous studies have mainly focused on the segregation behaviors of Mg alloys after annealing.In this study,we investigated the segregation behaviors of an Mg-RE alloy under deformation.We found that the enrichment of solute atoms occurred in{101^(-)1}compressive twin boundaries under compression at 298 K without any annealing in an Mg-RE alloy by scanning transmission electron microscopy and energy-dispersive X-ray analysis.The segregated solutes and precipitates impeded the twin growth,partially contributing to the formation of small-sized{101^(-)1}compressive twins.This research indicates the twin boundaries can be strengthened by segregated solutes and precipitates formed under deformation at room temperature.展开更多
Controlling surface chemistry is critically important for improving the initial Coulombic efficiency(ICE)and adsorption capacity of hard carbon anode used in Li/Na/K-ion batteries.However,accurately identifying the ty...Controlling surface chemistry is critically important for improving the initial Coulombic efficiency(ICE)and adsorption capacity of hard carbon anode used in Li/Na/K-ion batteries.However,accurately identifying the types and concentrations of hydrogen/oxygen terminated functional groups(HTFG/OTFGs)and distinguishing their functionalities remain challenge.Herein,we quantitatively investigated the surface chemistry on hard carbon via ultra-high temperature programed desorption measurements,and uncovered the role of HTFG/OTFGs in influencing ICE and adsorption capacity in Li/Na/K-ions cells.The C-H group is found to be dominant species on the surface of hard carbon,and presents a positive correlation with ICE values and adsorption capacity.The low reactivity of C-H group with both electrolyte salt and solvent results in the formation of thinner and highly conducive solid electrolyte interphase(SEI)layer,which benefit for the enhanced ICE and improved Li/Na/K-ions diffusion across SEI layer.Additionally,the pimping trapping effect of C-H groups allows the adsorbed Li/Na/K-ions to migrate into graphitic interlayer quickly,enhancing the slope capacity.By fabricating a C-H group-rich surface chemistry on hard carbon,a high ICE value and satisfactory specific capacity have been realized.These findings enrich our understanding of the surface chemistry-induced interfacial reaction,which effectively guides the rational design of high-performance hard carbon.展开更多
Ultrafine,highly dispersed Pt clusters were immobilized onto the Co nanoparticle surfaces by one-step pyrolysis of the precursor Pt(Ⅱ)-encapsulating Co-MOF-74.Owing to the small size effects of Pt clusters as well as...Ultrafine,highly dispersed Pt clusters were immobilized onto the Co nanoparticle surfaces by one-step pyrolysis of the precursor Pt(Ⅱ)-encapsulating Co-MOF-74.Owing to the small size effects of Pt clusters as well as the strongly enhanced synergistic interactions between Pt and Co atoms,the obtained Pt-on-Co/C400 catalysts exhib-ited excellent catalytic activity toward the hydrolysis of ammonia borane with an extremely high turnover frequency(TOF)value of 3022 min^(-1)at 303 K.Durability test indicated that the obtained Pt-on-Co/C400 catalysts possessed high catalytic stability,and there were no changes in the catalyst structures and catalytic activities after 10 cycles.展开更多
Deep learning has achieved great progress in image recognition,segmentation,semantic recognition and game theory.In this study,a latest deep learning model,a conditional diffusion model was adopted as a surrogate mode...Deep learning has achieved great progress in image recognition,segmentation,semantic recognition and game theory.In this study,a latest deep learning model,a conditional diffusion model was adopted as a surrogate model to predict the heat transfer during the casting process instead of numerical simulation.The conditional diffusion model was established and trained with the geometry shapes,initial temperature fields and temperature fields at t_(i) as the condition and random noise sampled from standard normal distribution as the input.The output was the temperature field at t_(i+1).Therefore,the temperature field at t_(i+1)can be predicted as the temperature field at t_(i) is known,and the continuous temperature fields of all the time steps can be predicted based on the initial temperature field of an arbitrary 2D geometry.A training set with 3022D shapes and their simulated temperature fields at different time steps was established.The accuracy for the temperature field for a single time step reaches 97.7%,and that for continuous time steps reaches 69.1%with the main error actually existing in the sand mold.The effect of geometry shape and initial temperature field on the prediction accuracy was investigated,the former achieves better result than the latter because the former can identify casting,mold and chill by different colors in the input images.The diffusion model has proved the potential as a surrogate model for numerical simulation of the casting process.展开更多
Light-driven artificial molecular machines[1,2]are a class of functional small molecules powered by photochemical reactions,broadly divided into molecular motors and molecular photoswitches.Molecular motors[3,4],owing...Light-driven artificial molecular machines[1,2]are a class of functional small molecules powered by photochemical reactions,broadly divided into molecular motors and molecular photoswitches.Molecular motors[3,4],owing to their intrinsic point chirality and dynamic axial chirality,undergo unidirectional rotation about a carbon–carbon double bond when irradiated with light.In nature,biological molecular motors and pumps are ubiquitous:driving vision,intracellular transport,energy conversion,signal transduction,muscle contraction,and locomotion.展开更多
Developing innovative resource utilization strategies to achieve sustainable recycling of waste-tofuel is highly desirable,yet the design of cost-effective bifunctional catalysts with dual high-efficiency remains unex...Developing innovative resource utilization strategies to achieve sustainable recycling of waste-tofuel is highly desirable,yet the design of cost-effective bifunctional catalysts with dual high-efficiency remains unexplored.While the Fenton-like reaction relies on enhancing peroxymonosulfate(PMS)adsorption and accelerating interfacial electron transfer to improve kinetic rates,CO_(2)reduction is constrained by sluggish kinetics and competing hydrogen evolution reaction.Herein,we construct a bifunctional catalyst(NiFe-BNC)featuring dual-atomic active sites by introducing boron atoms into a biomass-derived chitosan substrate rich in functional groups,which optimizes atomic coordination environments.In situ experiments and density functional theory calculations reveal that B-atom modulation facilitates carbon substrate defect enrichment,while the charge-tuning effect between metal sites and"boron electron bridge"optimizes PMS adsorption configurations.This synergistic effect facilitates the interfacial electron transfer and enhances the CO_(2)adsorption capacity of NiFe-BNC by 6 times that of NiFe-NC.The obtained NiFe-BNC exhibits significantly enhanced catalytic activity and selectivity,realizing 99%efficient degradation of volatile organic pollutants in the flowing phase within 2 h and stable mineralization exceeding 60%,while achieving a large current density of 1000 mA cm^(-2) and CO Faraday efficiency of 98%in the flow electrolytic cell.This work innovatively paves a new way for the rational design of cost-effective functional catalysts to achieve carbon cycle utilization.展开更多
基金financially supported by National Natural Science Foundation of China(No.22275149)Fundamental Research Funds for the Central Universities(No.SWU118105)the Next-Generation Advanced Energy Materials Program of BatteroTech Co.,Ltd.
文摘We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-of-plane negative Poisson's ratio(NPR)phenomenon,originating from its special sawtooth-like structure.The absolute value of the NPR decreases as the number of layers increases.The adsorption of volatile organic compounds(VOCs)including CH_(2)O,C_(2)H_(3)Cl and C_(6)H_(6)by AlO_(2)exhibit small adsorption distance,large adsorption energy,large charge transfer and significant density of states(DOS)changes,indicating the presence of strong interactions.The desorption time of each gas molecule on the AlO_(2)surface is also evaluated,and the results further suggest that the desorption of VOCs can be controlled by changing the temperature to achieve the recycling of AlO_(2).These interesting properties make 2D AlO_(2)a promising material for electronic,mechanical and sensing applications for VOCs.
基金supported by the National Natural Science Foundation of China (Nos.22208218,22078196,and 22278268)the Natural Science Foundation of Shanghai (No.22ZR1460400)Collaborative Innovation Center of Fragrance Flavour and Cosmetics,and Collaborative Innovation Project of Shanghai Institute of Technology (No.XTCX2023-07)。
文摘The diagnostic efficacy of contemporary bioimaging technologies remains constrained by inherent limitations of conventional imaging agents,including suboptimal sensitivity,off-target biodistribution,and inherent cytotoxicity.These limitations have catalyzed the development of intelligent stimuli-responsive block copolymers-based bioimaging agents,which was engineered to dynamically respond to endogenous biochemical cues(e.g.,p H gradients,redox potential,enzyme activity,hypoxia environment) or exogenous physical triggers(e.g.,photoirradiation,thermal gradients,ultrasound(US)/magnetic stimuli).Through spatiotemporally controlled structural transformations,stimuli-responsive block copolymers enable precise contrast targeting,activatable signal amplification,and theranostic integration,thereby substantially enhancing signal-to-noise ratios of bioimaging and diagnostic specificity.Hence,this mini-review systematically examines molecular engineering principles for designing p H-,redox-,enzyme-,light-,thermo-,and US/magnetic-responsive polymers,with emphasis on structure-property relationships governing imaging performance modulation.Furthermore,we critically analyze emerging strategies for optical imaging,US synergies,and magnetic resonance imaging(MRI).Multimodal bioimaging has also been elaborated,which could overcome the inherent trade-offs between resolution,penetration depth,and functional specificity in single-modal approaches.By elucidating mechanistic insights and translational challenges,this mini-review aims to establish a design framework of stimuli-responsive block copolymersbased for high fidelity bioimaging agents and accelerate their clinical translation in precise diagnosis and therapy.
基金supported by the National Natural Science Foundation of China(No.22375063)Science and Technology Commission of Shanghai Municipality(No.23JC1401700)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 National Natural Science Foundation of China(Nos.52404387,52090041,52374379,52425409)Xiaomi Young Scholars Program China,the National Postdoctoral Program for Innovative Talents,China(No.BX20230042)China Postdoctoral Science Foundation(No.2024M750174)。
文摘To address the zero-sample challenge in preparation parameter design for newly developed alloys,a novel machine learning strategy that integrates basic dataset construction with Bayesian optimization,was proposed.The impact of basic sample dataset construction methods,optimization benchmarks and multi-objective utility functions on Bayesian optimization was investigated.It was found that the combination of orthogonal design,linear benchmark,and shifted multiplicative utility function exhibits the best optimization performance.The strategy was then applied to a new Cu-Ni-Co-Si alloy with ultra-low Co content(0.7 wt.%Co),previously designed by our research team.Rapid optimization of six preparation parameters in the two-stage deformation and aging process of the zero-sample alloy was achieved through only 23 experiments.The measured ultimate tensile strength and electrical conductivity of the new alloy were 878 MPa and 44.0%(IACS),respectively,reaching the comprehensive performance level of the Cu-Ni-Co-Si alloy(C70350 alloy)containing 1.0-2.0 wt.%Co.
基金supported by the National Key R&D Program of China(Nos.2022YFB4101500 and 2022YFE0209500)the National Natural Science Foundation of China(Nos.22276191 and 21976177)the Qinghai Province Air Pollution Assessment and Fine Management Support Project,and the University of Chinese Academy of Science.
文摘As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This study prepared surface polarity-modified ACF using the heteroatom doping method.The modified ACF possessed a richer array of strongly polar oxygen/nitrogen-containing functional groups(primarily phenolic hydroxyl and lactone groups),a larger specific surface are1,and a more developed micropore structure.The adsorption capacities of ethanol for O-ACF and N-ACF were 4.110 mmol/g and 1.698 mmol/g,respectively,which were 11.3 times and 4.7 times those of unmodified ACF.This was a significant improvement over our previous work(0.363 mmol/g).The improvement of adsorption capacity for the N-ACF was mainly due to the higher specific surface are1,greater number of micropores(more adsorption sites)and abundant existence of defects,whereas,for O-ACF,the improvement mainly relied on the abundant presence of oxygen-containing functional groups on the surface.However,water had a negative effect on the adsorption of ethanol for the modified ACF due to competitive adsorption and the disappearance of capillary condensation.It was further revealed that the adsorption process of ethanol and water was quite different.It obeyed the linear driving force(LDF)model for ethanol adsorption,however,the intraparticle diffusion(IPD)model for water adsorption.
基金the Young Elite Scientists Sponsorship Program by JXAST(2024QT11)the National Natural Science Foundation of China(22465001,22309003)the Jiangxi Provincial Natural Science Foundation(20232BAB203042,20242BAB22002).
文摘As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference.To overcome these issues,we design three diketopyrrolopyrrole-based covalent organic frameworks(COFs)via a synergisticπ-extended lock and carboxyl-functionalized anchor molecular engineering strategy.Among them,TPy-DPP-COF features a covalently lockedπ-conjugated structure that enhances planarity,optimizes energy alignment,and minimizes exciton binding energy,thereby promoting charge transfer and suppressing recombination.Concurrently,carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation.These features contribute to the outstanding performance of TPy-DPP-COF,which achieves a high uranium adsorption capacity of 16.33 mg g−1 in natural seawater under irradiation,with only 29.3%capacity loss after 10 cycles,surpassing industrial benchmarks.Density functional theory(DFT)calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway,with DPP units acting as active sites for uranium reduction.This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.
基金financially supported by the National Key Research and Development Program of China (No. 2023YFB3812601)the National Natural Science Foundation of China (No. 51925401)the Young Elite Scientists Sponsorship Program by CAST, China (No. 2022QNRC001)。
文摘Machine learning-assisted methods for rapid and accurate prediction of temperature field,mushy zone,and grain size were proposed for the heating−cooling combined mold(HCCM)horizontal continuous casting of C70250 alloy plates.First,finite element simulations of casting processes were carried out with various parameters to build a dataset.Subsequently,different machine learning algorithms were employed to achieve high precision in predicting temperature fields,mushy zone locations,mushy zone inclination angle,and billet grain size.Finally,the process parameters were quickly optimized using a strategy consisting of random generation,prediction,and screening,allowing the mushy zone to be controlled to the desired target.The optimized parameters are 1234℃for heating mold temperature,47 mm/min for casting speed,and 10 L/min for cooling water flow rate.The optimized mushy zone is located in the middle of the second heat insulation section and has an inclination angle of roughly 7°.
基金supported by the State Key Research Development Program of China(No.2016YFA0204200)National Natural Science Foundation of China(Nos.21822603,21811540394,5171101651,21677048,21773062,21577036)+1 种基金Shanghai Pujiang Program(No.17PJD011)the Fundamental Research Funds for the Central Universities(No.22A201514021)。
文摘Graphene is a two-dimensional nanomaterial with huge surface area,high carrier mobility and high mechanical strength.Because of its great potential in nanotechnology and environmental protection,it has attracted much attention in environmental and energy fields since its discovery in 2004.Although graphene is a star material,many reviews have introduced its use in terms of energy,the research progress in the field of environment,especially water pollution control,has been rarely reported.Here,we review exhaustively the research progress of graphene-based materials in environmental pollution remediation in the past ten years.Firstly,the advantages and classification of graphene were introduced.Secondly,the research progress and main achievements of graphene and its composites in the fields of photocatalytic degradation,pollutant adsorption and water treatment were emphatically described,and the mechanism of action in the above fields was summarized.Finally,we discuss the problems existing in the preparation and summarize the application of graphene in the environment.
文摘This paper expatiates on domestic status of heavy steel casting production, with a special focus on hydraulicturbine castings for Three Gorges Project. In China, there is magnificent demand for heavy castings with the rapidgrowth of the national economy in recent years and the expected high growth in the coming 10 to 20 years. Someheavy and large castings such as mill housing and hydraulic turbine runner crown, blade and band for Three GorgesProject have been successfully made. However, the domestic production capability is still far from meeting the giganticrequirements. The domestic capability still lags behind the world class level, and a lot of heavy castings still dependon import. The paper also gives a particular introduction of the key technologies in the manufacturing of heavy steelcastings like metal melting, foundry technology, heat treatment technology and numerical simulation technique, etc.In addition, several case studies on the application of numerical simulation in the production of heavy steel castingsare presented.
基金supported by the National High Technology Research and Development Program of China(2007AA03Z547)the National Basic Research Program of China(G2006CB601202)+3 种基金the National Natural Science Foundations of China(10702033,90816025, 10632060 and 10328203)Fund of State Key Laboratory for Modification of Chemical Fibers and Polymer Materials of Donghua University(K0820)Fund of State Key Laboratory of Automotive Safety and Energy of Tsinghua University(KF09132)the Opening Project of Key Laboratory for Advanced Building Materials of Sichuan Province and Funds of State Key Laboratory of Explosion Science and Technology(KFJJ08-15 and KFJJ10-16M).
文摘Fiber reinforced lattice composites are lightweight attractive due to their high specific strength and specific stiffness.In the past 10 years,researchers developed three-dimensional（3D） lattice trusses and two-dimensional （2D） lattice grids by various methods including interlacing, weaving,interlocking,filament winding and molding hot- press.The lattice composites have been applied in the fields of radar cross-section reduction,explosive absorption and heat-resistance. In this paper,topologies of the lattice composites, their manufacturing routes,as well as their mechanical and multifunctional applications,were surveyed.
基金supported by National Key Research&Development Program of China(No.2023YFE0210900)National Natural Science Foundation of China(No.21975085)+1 种基金Excellent Youth Foundation of Hubei Scientific Committee(No.2021CFA065)open Fund of Hubei Key Laboratory of Material Chemistry and Service Failure(No.2023MCF02)。
文摘It has been widely recognized that hole transporting materials(HTMs)play a key role in the rapid progress of perovskite solar cells(PVSCs).However,common organic HTMs such as spiro-OMe TAD not only suffer from high synthetic costs,but also usually require the additional chemical doping process to improve their hole transport ability,which unfortunately induces the terrible stability issue.Therefore,it is urgent to develop low-cost dopant-free HTMs for efficient and stable PVSCs.In this work,we have successfully developed a new class of efficient dopant-free fluoranthene-based HTMs(TPF1–5)with quite low lab synthetic costs by combining donor-acceptor and branched structure designs.The detailed structure-property study revealed that tuning the twisted arms at different substitution sites would regulate the intermolecular interactions and film-forming ability,thereby significantly affecting the performance of the HTMs.By applying these HTMs in conventional PVSCs,the dopant-free TPF1-based devices not only achieved the best efficiency of 21.76%,which is comparable to that of the doped spiro-OMeTAD control devices,but also showed much better operational stability,which maintained over 87%of the initial efficiency under maximum power point tracking after 1038 h.
基金supported by the National Natural Science Foundation of China(No.21571062)the Program for Professor of Special Appointment(Eastern Scholar)at the Shanghai Institutions of Higher Learning to JGL,and the Fundamental Research Funds for the Central Universities(No.222201717003)。
文摘Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.
基金financially supported by the National Key Research and Development Program of China(No.2022YFB3706901)the National Natural Science Foundation of China(No.52090041)the Young Elite Scientists Sponsorship Program by CAST(No.2022QNRC 001).
文摘Digital modeling and autonomous control of the die forging process are significant challenges in realizing high-quality intelli-gent forging of components.Using the die forging of AA2014 aluminum alloy as a case study,a machine-learning-assisted method for di-gital modeling of the forging force and autonomous control in response to forging parameter disturbances was proposed.First,finite ele-ment simulations of the forging processes were conducted under varying friction factors,die temperatures,billet temperatures,and for-ging velocities,and the sample data,including process parameters and forging force under different forging strokes,were gathered.Pre-diction models for the forging force were established using the support vector regression algorithm.The prediction error of F_(f),that is,the forging force required to fill the die cavity fully,was as low as 4.1%.To further improve the prediction accuracy of the model for the ac-tual F_(f),two rounds of iterative forging experiments were conducted using the Bayesian optimization algorithm,and the prediction error of F_(f) in the forging experiments was reduced from 6.0%to 1.5%.Finally,the prediction model of F_(f) combined with a genetic algorithm was used to establish an autonomous optimization strategy for the forging velocity at each stage of the forging stroke,when the billet and die temperatures were disturbed,which realized the autonomous control in response to disturbances.In cases of−20 or−40℃ reductions in the die and billet temperatures,forging experiments conducted with the autonomous optimization strategy maintained the measured F_(f) around the target value of 180 t,with the relative error ranging from−1.3%to+3.1%.This work provides a reference for the study of di-gital modeling and autonomous optimization control of quality factors in the forging process.
文摘Many strategies have been proposed to produce arenes from lignin as liquid fuel additives.However,the development of these methods is limited by the low yield of products,low atom utilization,and inefficient lignin depolymerization.Herein,we develop an energy-efficient synthetic method for the production of high-carbon-number arenes from sustainable lignin with a total yield of 23.1 wt%.Particularly,high carbon number arenes are obtained by fully utilizing the formaldehyde stabilizing additive and the methoxy group in lignin.The process begins with the reductive depolymerization of formaldehyde-stabilized lignin,followed by transmethylation between lignin monomers over Au/Nb_(2)O_(5) catalyst,and the Ru/Nb2O5-catalyzed hydrodeoxygenation.This work demonstrates the potential of value-added arenes production directly from lignin.
基金support from Interdisciplinary Research Project for Young Teachers of USTB Fundamental Research Funds for the Central Universities(Grant no.FRF-IDRY-23-030).
文摘Solute atoms and precipitates significantly influence the mechanical properties of Mg alloys.Previous studies have mainly focused on the segregation behaviors of Mg alloys after annealing.In this study,we investigated the segregation behaviors of an Mg-RE alloy under deformation.We found that the enrichment of solute atoms occurred in{101^(-)1}compressive twin boundaries under compression at 298 K without any annealing in an Mg-RE alloy by scanning transmission electron microscopy and energy-dispersive X-ray analysis.The segregated solutes and precipitates impeded the twin growth,partially contributing to the formation of small-sized{101^(-)1}compressive twins.This research indicates the twin boundaries can be strengthened by segregated solutes and precipitates formed under deformation at room temperature.
基金financially supported by the National Key Research and Development Program of China(2022YFE0206300)the National Natural Science Foundation of China(U21A2081,22075074,22209047)+4 种基金the National College Students Innovation and Entrepreneurship Training Program(S202410532594,S202410532357)the Macao Science and Technology Development Fund(File No.0013/2021/AMJ)the Foundation of Yuelushan Center for Industrial Innovation(2023YCII0119)JST SICORP(JPMJSC2112)JST PRESTO(JPMJPR23QA)。
文摘Controlling surface chemistry is critically important for improving the initial Coulombic efficiency(ICE)and adsorption capacity of hard carbon anode used in Li/Na/K-ion batteries.However,accurately identifying the types and concentrations of hydrogen/oxygen terminated functional groups(HTFG/OTFGs)and distinguishing their functionalities remain challenge.Herein,we quantitatively investigated the surface chemistry on hard carbon via ultra-high temperature programed desorption measurements,and uncovered the role of HTFG/OTFGs in influencing ICE and adsorption capacity in Li/Na/K-ions cells.The C-H group is found to be dominant species on the surface of hard carbon,and presents a positive correlation with ICE values and adsorption capacity.The low reactivity of C-H group with both electrolyte salt and solvent results in the formation of thinner and highly conducive solid electrolyte interphase(SEI)layer,which benefit for the enhanced ICE and improved Li/Na/K-ions diffusion across SEI layer.Additionally,the pimping trapping effect of C-H groups allows the adsorbed Li/Na/K-ions to migrate into graphitic interlayer quickly,enhancing the slope capacity.By fabricating a C-H group-rich surface chemistry on hard carbon,a high ICE value and satisfactory specific capacity have been realized.These findings enrich our understanding of the surface chemistry-induced interfacial reaction,which effectively guides the rational design of high-performance hard carbon.
文摘Ultrafine,highly dispersed Pt clusters were immobilized onto the Co nanoparticle surfaces by one-step pyrolysis of the precursor Pt(Ⅱ)-encapsulating Co-MOF-74.Owing to the small size effects of Pt clusters as well as the strongly enhanced synergistic interactions between Pt and Co atoms,the obtained Pt-on-Co/C400 catalysts exhib-ited excellent catalytic activity toward the hydrolysis of ammonia borane with an extremely high turnover frequency(TOF)value of 3022 min^(-1)at 303 K.Durability test indicated that the obtained Pt-on-Co/C400 catalysts possessed high catalytic stability,and there were no changes in the catalyst structures and catalytic activities after 10 cycles.
基金sponsored by Tsinghua-Toyota Joint Research Fund
文摘Deep learning has achieved great progress in image recognition,segmentation,semantic recognition and game theory.In this study,a latest deep learning model,a conditional diffusion model was adopted as a surrogate model to predict the heat transfer during the casting process instead of numerical simulation.The conditional diffusion model was established and trained with the geometry shapes,initial temperature fields and temperature fields at t_(i) as the condition and random noise sampled from standard normal distribution as the input.The output was the temperature field at t_(i+1).Therefore,the temperature field at t_(i+1)can be predicted as the temperature field at t_(i) is known,and the continuous temperature fields of all the time steps can be predicted based on the initial temperature field of an arbitrary 2D geometry.A training set with 3022D shapes and their simulated temperature fields at different time steps was established.The accuracy for the temperature field for a single time step reaches 97.7%,and that for continuous time steps reaches 69.1%with the main error actually existing in the sand mold.The effect of geometry shape and initial temperature field on the prediction accuracy was investigated,the former achieves better result than the latter because the former can identify casting,mold and chill by different colors in the input images.The diffusion model has proved the potential as a surrogate model for numerical simulation of the casting process.
文摘Light-driven artificial molecular machines[1,2]are a class of functional small molecules powered by photochemical reactions,broadly divided into molecular motors and molecular photoswitches.Molecular motors[3,4],owing to their intrinsic point chirality and dynamic axial chirality,undergo unidirectional rotation about a carbon–carbon double bond when irradiated with light.In nature,biological molecular motors and pumps are ubiquitous:driving vision,intracellular transport,energy conversion,signal transduction,muscle contraction,and locomotion.
基金supported by National Natural Science Foundation of China (Grants No. 92266107, 92366207, 52401245)the Shaanxi Fundamental Science Research Project in the fields of Mathematics and Physics (Grant No. 22JSQ008)+1 种基金the China Manned Space Station programQin Chuang Yuan Scientist and Engineer Program (2025QCY-KXJ-094)
文摘Developing innovative resource utilization strategies to achieve sustainable recycling of waste-tofuel is highly desirable,yet the design of cost-effective bifunctional catalysts with dual high-efficiency remains unexplored.While the Fenton-like reaction relies on enhancing peroxymonosulfate(PMS)adsorption and accelerating interfacial electron transfer to improve kinetic rates,CO_(2)reduction is constrained by sluggish kinetics and competing hydrogen evolution reaction.Herein,we construct a bifunctional catalyst(NiFe-BNC)featuring dual-atomic active sites by introducing boron atoms into a biomass-derived chitosan substrate rich in functional groups,which optimizes atomic coordination environments.In situ experiments and density functional theory calculations reveal that B-atom modulation facilitates carbon substrate defect enrichment,while the charge-tuning effect between metal sites and"boron electron bridge"optimizes PMS adsorption configurations.This synergistic effect facilitates the interfacial electron transfer and enhances the CO_(2)adsorption capacity of NiFe-BNC by 6 times that of NiFe-NC.The obtained NiFe-BNC exhibits significantly enhanced catalytic activity and selectivity,realizing 99%efficient degradation of volatile organic pollutants in the flowing phase within 2 h and stable mineralization exceeding 60%,while achieving a large current density of 1000 mA cm^(-2) and CO Faraday efficiency of 98%in the flow electrolytic cell.This work innovatively paves a new way for the rational design of cost-effective functional catalysts to achieve carbon cycle utilization.
