Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances ar...Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.展开更多
Flexible energy storage and harvesting devices,as core components of the flexible electronic system,have driven the transformation of electronic system from“external power supply”to“self-powering”and from“fixed f...Flexible energy storage and harvesting devices,as core components of the flexible electronic system,have driven the transformation of electronic system from“external power supply”to“self-powering”and from“fixed forms”to“adaptive configurations”,thus playing an important role in the advancement of wearable technology,the internet of things,and other related fields.MXenes,a class of two-dimensional transition metal carbides,nitrides,and carbonitrides,emerge as promising candidates for flexible energy storage and harvesting devices,attributed to their excellent conductivity,mechanical flexibility,and tunable interfacial characteristics.Specifically,the interfacial characteristics of MXenes,including surface energy,surface terminations,and interlayer spacing,have a decisive influence on the performance of MXene-based energy devices.This review summarizes the influence of microcosmic interfacial characteristics on macroscopic properties,the interfacial regulation strategies,and applications in flexible energy storage and harvesting of MXenes,concluding with current challenges and perspectives to guide the design of high-performance MXene-based energy devices.展开更多
Layered double hydroxides(LDHs)are promising electrocatalysts for the oxygen evolution reaction(OER),yet their practical application remains limited by poor electrical conductivity and sluggish reaction kinetics.In th...Layered double hydroxides(LDHs)are promising electrocatalysts for the oxygen evolution reaction(OER),yet their practical application remains limited by poor electrical conductivity and sluggish reaction kinetics.In this work,we synthesize three high-entropy LDHs(HELDHs)featuring a hierarchical architecture of microspheres assembled from ultrathin nanosheets,via a simple hydrothermal method using a combination of low-cost,catalytically active transition metals(Fe,Co,Ni,Mn,Zn,Cu,and Cr).Among them,the FeCoNiMnZn HELDH exhibits outstanding OER performance,requiring an overpotential of only 306 mV to reach a current density of 100 mA cm^(-2).Notably,during 200 h of continuous operation,the device exhibits a stable and,in some cases,increasing current output.This exceptional activity is attributed to the formation of abundant cation vacancies,induced by Zn leaching,which enhance the intrinsic catalytic properties by optimizing the adsorption energies of key OER intermediates.Density functional theory calculations further validate that these vacancies modulate the electronic structure and lower reaction barriers,underscoring the effectiveness of cation-vacancy engineering in high-entropy systems for efficient and durable water oxidation catalysis.The optimized catalyst was further evaluated as the air cathode in a zinc-air battery,demonstrating practical electrochemical performance.展开更多
Profile of Prof.Ning-Li Wang Academician of the Chinese Academy of Engineering(CAE)Member of the International Academy of Ophthalmology Director,Ophthalmology Center,Beijing Tongren Hospital Dean,School of Ophthalmolo...Profile of Prof.Ning-Li Wang Academician of the Chinese Academy of Engineering(CAE)Member of the International Academy of Ophthalmology Director,Ophthalmology Center,Beijing Tongren Hospital Dean,School of Ophthalmology,Capital Medical University Director,National Engineering Research Center for Ophthalmic Diagnosis and Treatment National Distinguished Physician Member,Academic Advisory Committee.展开更多
4-Bromo-3-methylphenol(BMP)is an important chemical intermediate with wide applications in the fields of medicine and pesticides.The synthesis of BMP from m-cresol via bromination is easy to carry out on an industrial...4-Bromo-3-methylphenol(BMP)is an important chemical intermediate with wide applications in the fields of medicine and pesticides.The synthesis of BMP from m-cresol via bromination is easy to carry out on an industrial scale.However,due to the formation of regioisomeric impurities during bromination and the low melting point of BMP,the separation process is prone to the formation of oily substances,resulting in low yield and purity.In this work,a new cocrystallization engineering approach was proposed to separate and purify BMP.Through design of experiments,the cocrystallization process of BMP and triethylenediamine(DABCO)was optimized using a minimum-run resolution IV screening design combined with response surface methodology.In addition,the obtained 2BMP-DABCO powder was characterized by thermal analysis,powder X-ray diffraction,infrared spectroscopy,and scanning electron microscopy.Single crystals of 2BMP-DABCO were grown from acetone by slow evaporation,and detailed structural information was obtained through single-crystal X-ray diffraction.The self-assembly mechanism was further clarified by density functional theory calculations.This study provides a simple,robust,and scalable method for the production of BMP and offers a reference for the separation and purification of phenolic substances.展开更多
In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of...In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of this development.Inorganic solid-state electrolytes(ISSEs)are the core components of sodium batteries;however,they face significant challenges such as insufficient ionic conductivity,interfacial instability,and dendrite growth,all of which severely hinder practical application.This review critically assesses experimental protocols and theoretical frameworks related to mainstream ISSEs and systematizes optimization strategies aimed at overcoming these challenges.Leveraging integrated insights from both experimental and computational studies,the review first categorizes and summarizes the primary types of ISSEs,namely oxide-,sulfide-,and halide-based electrolytes.It then details interfacial optimization strategies focused on addressing three core interfacial issues:ion transport barriers resulting from mechanical incompatibility,side reactions stemming from electrochemical mismatch,and dendrite formation.Finally,the review advocates prioritizing in-depth research that integrates experimental and theoretical approaches to establish a closed-loop methodology encompassing predictive design,multiscale investigation,mechanistic exploration,and high-throughput automated experimentation,with feedback-driven refinement.This work serves as a comprehensive reference and systematic roadmap for future research on solid-state electrolytes(SSEs).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
Accurate purchase prediction in e-commerce critically depends on the quality of behavioral features.This paper proposes a layered and interpretable feature engineering framework that organizes user signals into three ...Accurate purchase prediction in e-commerce critically depends on the quality of behavioral features.This paper proposes a layered and interpretable feature engineering framework that organizes user signals into three layers:Basic,Conversion&Stability(efficiency and volatility across actions),and Advanced Interactions&Activity(crossbehavior synergies and intensity).Using real Taobao(Alibaba’s primary e-commerce platform)logs(57,976 records for 10,203 users;25 November–03 December 2017),we conducted a hierarchical,layer-wise evaluation that holds data splits and hyperparameters fixed while varying only the feature set to quantify each layer’s marginal contribution.Across logistic regression(LR),decision tree,random forest,XGBoost,and CatBoost models with stratified 5-fold cross-validation,the performance improvedmonotonically fromBasic to Conversion&Stability to Advanced features.With LR,F1 increased from 0.613(Basic)to 0.962(Advanced);boosted models achieved high discrimination(0.995 AUC Score)and an F1 score up to 0.983.Calibration and precision–recall analyses indicated strong ranking quality and acknowledged potential dataset and period biases given the short(9-day)window.By making feature contributions measurable and reproducible,the framework complements model-centric advances and offers a transparent blueprint for production-grade behavioralmodeling.The code and processed artifacts are publicly available,and future work will extend the validation to longer,seasonal datasets and hybrid approaches that combine automated feature learning with domain-driven design.展开更多
Lacto-N-neotetraose(LNn T)is a crucial neutral core human milk oligosaccharide(HMO).In this study,we established a LNn T-producing Saccharomyces cerevisiae cell factory through comprehensive metabolic engineering.Spec...Lacto-N-neotetraose(LNn T)is a crucial neutral core human milk oligosaccharide(HMO).In this study,we established a LNn T-producing Saccharomyces cerevisiae cell factory through comprehensive metabolic engineering.Specifically,the de novo biosynthetic pathway of LNn T was assembled by heterologously expressing the lactose permease(lac12)from Kluyveromyces lactis and the glycosyltransferase from Neisseria meningitidis in S.cerevisiae.Subsequently,carbon source regulation based on the glucose-sensitive GAL regulatory system was employed to optimize the expression time of heterologous genes,achieving a production of 15.61 mg/L of LNn T in shake-flask fermentation.In addition,the key rate-limiting steps involved in LNn T synthesis pathway were identified and the corresponding genes were overexpressed to enhance LNn T production,resulting in an 8-fold increase in LNn T titer compared to that of parental strain.To our knowledge,this is the first report on LNn T biosynthesis in S.cerevisiae,opening up the possibility of green production of LNn T using food-safe microorganisms.展开更多
Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate ...Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate excellent kinetics and structural stability,thanks to the built-in electric field of the carbon heterostructure and its adaptability to volume changes.Yet,the carbon shell imposes a physical barrier to interfacial Na^(+)diffusion,while deep discharge induces the formation of crystalline Na_(2)S,accompanied by severe volumetric expansion and sluggish reversibility—factors that accelerate capacity fading and structural degradation.To address these challenges,a trace-level Ni doping strategy is introduced,enabling precise modulation of the composite's interlayer structure,electronic configuration,and reaction pathway.Ni incorporation expands the MoS_(2) interlayer spacing,reconstructs short-range ordered nanocrystals within a hierarchically porous network,and promotes Na^(+)diffusion by weakening interlayer van der Waals forces.Orbital hybridization between Ni-3d and Mo-4d/S-3p states enhances electronic conductivity and reduces charge transfer resistance.Critically,Ni doping enhances electron transfer from Ni to sulfur,which weakens Na–S bonds and promotes the formation of amorphous Na_(2)S,thereby suppressing crystalline Na_(2)S and enabling a reversible MoS_(2)/Na_(2)S conversion mechanism for improved structural stability and cycling performance.As a result,the optimized MoS_(2)-Ni@C anode delivers a high reversible capacity of 334 mAh g^(-1)at 10 A g^(-1)with 68%retention after 10,000 cycles.When assembled into a SIC device(MoS_(2)-Ni@C//AC),it achieves an energy density of 135 Wh kg^(-1)at a power density of 60.8 kW kg^(-1)(based on anode mass),with 76%retention over 3,000 cycles.展开更多
Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we d...Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we demonstrate that TSP perovskite films exhibit a vertically gradient distribution of residual PbI_(2)clusters,which form Schottky heterojunctions with the perovskite,leading to substantial interfacial energy-level mismatches within NiO_(x)-based TSP p-i-n PSCs.These limitations were effectively addressed via a vertical interfacial engineering enabled by dual-interface modification incorporating tin trifluoromethanesulfonate(Sn(OTF)_(2))and 4-Fluorophenylethylamine chloride(F-PEA)at the NiO_(x)/perovskite and perovskite/C60 interfaces,respectively.The functional Sn(OTF)_(2)not only enhances the conductivity of NiO_(x)films but also suppresses ion migration,while inducing the formation of a Pb-Sn mixed perovskite interlayer that precisely regulates the energy level at the NiO_(x)/perovskite interface.Complementally,F-PEA post-treatment effectively converts surface residual PbI_(2)clusters into a 2D perovskite capping layer,which simultaneously passivates surface defects and enhances energy-level alignment at the perovskite/C60 interface.Consequently,the optimized NiO_(x)-based TSP p-i-n PSCs achieve a notable PCE of 25.6%with superior operational stability.This study elucidates the underlying mechanisms limiting the efficiency of TSP p-i-n PSCs,while establishing design principles for these devices targeting 26%efficiency.展开更多
High-performance alloys are indispensable in modern engineering because of their exceptional strength,ductility,corrosion resistance,fatigue resistance,and thermal stability,which are all significantly influenced by t...High-performance alloys are indispensable in modern engineering because of their exceptional strength,ductility,corrosion resistance,fatigue resistance,and thermal stability,which are all significantly influenced by the alloy interface structures.Despite substantial efforts,a comprehensive overview of interface engineering of high-performance alloys has not been presented so far.In this study,the interfaces in high-performance alloys,particularly grain and phase boundaries,were systematically examined,with emphasis on their crystallographic characteristics and chemical element segregations.The effects of the interfaces on the electrical conductivity,mechanical strength,toughness,hydrogen embrittlement resistance,and thermal stability of the alloys were elucidated.Moreover,correlations among various types of interfaces and advanced experimental and computational techniques were examined using big data analytics,enabling robust design strategies.Challenges currently faced in the field of interface engineering and emerging opportunities in the field are also discussed.The study results would guide the development of next-generation high-performance alloys.展开更多
The osteochondral(OC)interface exhibits a mineral gradient,varying in thickness by several hundred micrometers across different species.Disruptions in this interface damage OC tissues,leading to osteoarthritis.The nat...The osteochondral(OC)interface exhibits a mineral gradient,varying in thickness by several hundred micrometers across different species.Disruptions in this interface damage OC tissues,leading to osteoarthritis.The natural architecture and composition of native OC interfaces can be replicated using biomaterial scaffolds via regenerative engineering approaches.A novel one-step bioextrusion process was employed to fabricate a unitary synthetic graft(USG),which mimics the native OC interface’s mineral concentration gradient.This novel USG is composed of an agarose-based cartilage layer and a bone layer,consisting of agarose enriched with 20%(200 g/L)hydroxyapatite.The USG features a gradient interface with mineral concentrations transitioning from 0%to 20%(mass fraction),mimicking the transition between the cartilage and bone.Thermogravimetric analysis revealed that the gradient transition lengths of the graft and native OC tissue harvested from bovine knees were similar((647±21)vs.(633±124)μm).The linear viscoelastic properties of the grafts,which were evaluated using strain sweep and frequency sweep tests with oscillatory shear,indicated a dominant storage modulus over loss modulus similar to that of native OC tissues.The compressive and stress relaxation behaviors of the USGs demonstrated that the graft maintained structural integrity under mechanical stress.Viability assays performed after bioextrusion showed that chondrocytes and human fetal osteoblast cells successfully integrated and survived within their designated regions of the graft.The novel USGs exhibit properties similar to native OC tissue and are promising candidates for regenerating OC defects and restoring knee joint functionality.展开更多
All-inorganic lead-free perovskite solar cells have emerged as environmentally benign candidates;however,their device performance is still constrained by pronounced carrier recombination losses in the bulk and at inte...All-inorganic lead-free perovskite solar cells have emerged as environmentally benign candidates;however,their device performance is still constrained by pronounced carrier recombination losses in the bulk and at interfaces.By combining energy band alignment analysis with detailed modeling of recombination mechanisms,a systematic strategy for optimizing hole transport layers is developed.The results reveal that a negative valence band offset produces a cliff-like interface,which facilitates hole extraction while also accounting for the observed variations in open-circuit voltage.Furthermore,short-circuit current losses are quantitatively attributed to different recombination pathways,modeled by incorporating radiative,Shockley–Read–Hall,Auger,and interface recombination processes.This comprehensive approach not only clarifies the correlation between energy level alignment and recombination dynamics but also highlights the competing roles of band offset and interface defects in determining device performance.The optimized device architecture,based on Ge-based lead-free perovskites,achieves a power conversion efficiency of 25.1%,with an open-circuit voltage of 1.29 V,a short-circuit current density of 22.5 mA·cm^(-2),and a fill factor of 86.3%.These findings provide theoretical guidance for designing stable,high-performance,and environmentally friendly lead-free perovskite solar cells.展开更多
This paper introduces a novel nature-inspired metaheuristic algorithm called the Gekko japonicus algorithm.The algo-rithm draws inspiration mainly from the predation strategies and survival behaviors of the Gekko japo...This paper introduces a novel nature-inspired metaheuristic algorithm called the Gekko japonicus algorithm.The algo-rithm draws inspiration mainly from the predation strategies and survival behaviors of the Gekko japonicus.The math-ematical model is developed by simulating various biological behaviors of the Gekko japonicus,such as hybrid loco-motion patterns,directional olfactory guidance,implicit group advantage tendencies,and the tail autotomy mechanism.By integrating multi-stage mutual constraints and dynamically adjusting parameters,GJA maintains an optimal balance between global exploration and local exploitation,thereby effectively solving complex optimization problems.To assess the performance of GJA,comparative analyses were performed against fourteen state-of-the-art metaheuristic algorithms using the CEC2017 and CEC2022 benchmark test sets.Additionally,a Friedman test was performed on the experimen-tal results to assess the statistical significance of differences between various algorithms.And GJA was evaluated using multiple qualitative indicators,further confirming its superiority in exploration and exploitation.Finally,GJA was utilized to solve four engineering optimization problems and further implemented in robotic path planning to verify its practical applicability.Experimental results indicate that,compared to other high-performance algorithms,GJA demonstrates excep-tional performance as a powerful optimization algorithm in complex optimization problems.We make the code publicly available at:https://github.com/zhy1109/Gekko-japonicusalgorithm.展开更多
基金funding support from General Research Fund[Project No.14300525]from the Research Grants Council(RGC)of Hong Kong SAR,Chinafunding support from Natural Science Foundation of China(NSFC)Young Scientists Fund(Project No.22305203)+2 种基金NSFC Projects Nos.22309123,22422303,22303011,22033002,92261112 and U21A20328support from the Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM)at City University of Hong Kongsupport from Young Collaborative Research Grant[Project No.C1003-23Y]support from RGC of Hong Kong SAR,China.
文摘Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.
基金supported by the National Natural Science Foundation of China(52422205,52403154)the National Key Research and Development Program of China(2023YFB3811303)+2 种基金the Natural Science Foundation of Sichuan Province(2026NSFSCZY0103,2026NSFSC1406)the Postdoctoral Fellowship Program of China Postdoctoral Science Foundation(GZC20230383)the China Postdoctoral Science Foundation(2025M770159)。
文摘Flexible energy storage and harvesting devices,as core components of the flexible electronic system,have driven the transformation of electronic system from“external power supply”to“self-powering”and from“fixed forms”to“adaptive configurations”,thus playing an important role in the advancement of wearable technology,the internet of things,and other related fields.MXenes,a class of two-dimensional transition metal carbides,nitrides,and carbonitrides,emerge as promising candidates for flexible energy storage and harvesting devices,attributed to their excellent conductivity,mechanical flexibility,and tunable interfacial characteristics.Specifically,the interfacial characteristics of MXenes,including surface energy,surface terminations,and interlayer spacing,have a decisive influence on the performance of MXene-based energy devices.This review summarizes the influence of microcosmic interfacial characteristics on macroscopic properties,the interfacial regulation strategies,and applications in flexible energy storage and harvesting of MXenes,concluding with current challenges and perspectives to guide the design of high-performance MXene-based energy devices.
基金supported by the National Natural Science Foundation of China(NSFC)(22302151,52502312)Natural Science Foundation of Hubei Province(2024AFB755,2024AFB267)+1 种基金Key Project of Hubei Provincial Department of Education Scientific Research Plan(F2023007)Wuhan Institute of Technology Graduate Education Innovation Fund(CX2024285)。
文摘Layered double hydroxides(LDHs)are promising electrocatalysts for the oxygen evolution reaction(OER),yet their practical application remains limited by poor electrical conductivity and sluggish reaction kinetics.In this work,we synthesize three high-entropy LDHs(HELDHs)featuring a hierarchical architecture of microspheres assembled from ultrathin nanosheets,via a simple hydrothermal method using a combination of low-cost,catalytically active transition metals(Fe,Co,Ni,Mn,Zn,Cu,and Cr).Among them,the FeCoNiMnZn HELDH exhibits outstanding OER performance,requiring an overpotential of only 306 mV to reach a current density of 100 mA cm^(-2).Notably,during 200 h of continuous operation,the device exhibits a stable and,in some cases,increasing current output.This exceptional activity is attributed to the formation of abundant cation vacancies,induced by Zn leaching,which enhance the intrinsic catalytic properties by optimizing the adsorption energies of key OER intermediates.Density functional theory calculations further validate that these vacancies modulate the electronic structure and lower reaction barriers,underscoring the effectiveness of cation-vacancy engineering in high-entropy systems for efficient and durable water oxidation catalysis.The optimized catalyst was further evaluated as the air cathode in a zinc-air battery,demonstrating practical electrochemical performance.
文摘Profile of Prof.Ning-Li Wang Academician of the Chinese Academy of Engineering(CAE)Member of the International Academy of Ophthalmology Director,Ophthalmology Center,Beijing Tongren Hospital Dean,School of Ophthalmology,Capital Medical University Director,National Engineering Research Center for Ophthalmic Diagnosis and Treatment National Distinguished Physician Member,Academic Advisory Committee.
基金supported by the National Natural Science Foundation of China(22177011(R.Z.Qiao),21977012(R.Z.Qiao),and 21572018(C.Li))the National High-Level Hospital Clinical Research Funding(2023-NHLHCRF-YXHZ-ZRMS-02)the Joint Project of BRCBC(Biomedical Translational Engineering Research Center of BUCT-CJFH)(XK2020-06).
文摘4-Bromo-3-methylphenol(BMP)is an important chemical intermediate with wide applications in the fields of medicine and pesticides.The synthesis of BMP from m-cresol via bromination is easy to carry out on an industrial scale.However,due to the formation of regioisomeric impurities during bromination and the low melting point of BMP,the separation process is prone to the formation of oily substances,resulting in low yield and purity.In this work,a new cocrystallization engineering approach was proposed to separate and purify BMP.Through design of experiments,the cocrystallization process of BMP and triethylenediamine(DABCO)was optimized using a minimum-run resolution IV screening design combined with response surface methodology.In addition,the obtained 2BMP-DABCO powder was characterized by thermal analysis,powder X-ray diffraction,infrared spectroscopy,and scanning electron microscopy.Single crystals of 2BMP-DABCO were grown from acetone by slow evaporation,and detailed structural information was obtained through single-crystal X-ray diffraction.The self-assembly mechanism was further clarified by density functional theory calculations.This study provides a simple,robust,and scalable method for the production of BMP and offers a reference for the separation and purification of phenolic substances.
基金the National Natural Science Foundation of China (52076076, 52006065)Fundamental Research Funds for Central Universities (2025JC003)Beijing Municipal Natural Science Foundation (3242022)
文摘In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of this development.Inorganic solid-state electrolytes(ISSEs)are the core components of sodium batteries;however,they face significant challenges such as insufficient ionic conductivity,interfacial instability,and dendrite growth,all of which severely hinder practical application.This review critically assesses experimental protocols and theoretical frameworks related to mainstream ISSEs and systematizes optimization strategies aimed at overcoming these challenges.Leveraging integrated insights from both experimental and computational studies,the review first categorizes and summarizes the primary types of ISSEs,namely oxide-,sulfide-,and halide-based electrolytes.It then details interfacial optimization strategies focused on addressing three core interfacial issues:ion transport barriers resulting from mechanical incompatibility,side reactions stemming from electrochemical mismatch,and dendrite formation.Finally,the review advocates prioritizing in-depth research that integrates experimental and theoretical approaches to establish a closed-loop methodology encompassing predictive design,multiscale investigation,mechanistic exploration,and high-throughput automated experimentation,with feedback-driven refinement.This work serves as a comprehensive reference and systematic roadmap for future research on solid-state electrolytes(SSEs).
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 research fund of Hanyang University(HY-202500000001616).
文摘Accurate purchase prediction in e-commerce critically depends on the quality of behavioral features.This paper proposes a layered and interpretable feature engineering framework that organizes user signals into three layers:Basic,Conversion&Stability(efficiency and volatility across actions),and Advanced Interactions&Activity(crossbehavior synergies and intensity).Using real Taobao(Alibaba’s primary e-commerce platform)logs(57,976 records for 10,203 users;25 November–03 December 2017),we conducted a hierarchical,layer-wise evaluation that holds data splits and hyperparameters fixed while varying only the feature set to quantify each layer’s marginal contribution.Across logistic regression(LR),decision tree,random forest,XGBoost,and CatBoost models with stratified 5-fold cross-validation,the performance improvedmonotonically fromBasic to Conversion&Stability to Advanced features.With LR,F1 increased from 0.613(Basic)to 0.962(Advanced);boosted models achieved high discrimination(0.995 AUC Score)and an F1 score up to 0.983.Calibration and precision–recall analyses indicated strong ranking quality and acknowledged potential dataset and period biases given the short(9-day)window.By making feature contributions measurable and reproducible,the framework complements model-centric advances and offers a transparent blueprint for production-grade behavioralmodeling.The code and processed artifacts are publicly available,and future work will extend the validation to longer,seasonal datasets and hybrid approaches that combine automated feature learning with domain-driven design.
基金funded by the National Key Research and Development Program of China(2022YFF1100300)National Natural Science Foundation of China(22108097)+2 种基金Key Research and Development Program of Jiangsu Province(BE2022850)Taihu Innovation-Leading Talent of Wuxi City(1026010241230040)Cross-Integration Innovation Funding of SFST(SFST2023-KY-10).
文摘Lacto-N-neotetraose(LNn T)is a crucial neutral core human milk oligosaccharide(HMO).In this study,we established a LNn T-producing Saccharomyces cerevisiae cell factory through comprehensive metabolic engineering.Specifically,the de novo biosynthetic pathway of LNn T was assembled by heterologously expressing the lactose permease(lac12)from Kluyveromyces lactis and the glycosyltransferase from Neisseria meningitidis in S.cerevisiae.Subsequently,carbon source regulation based on the glucose-sensitive GAL regulatory system was employed to optimize the expression time of heterologous genes,achieving a production of 15.61 mg/L of LNn T in shake-flask fermentation.In addition,the key rate-limiting steps involved in LNn T synthesis pathway were identified and the corresponding genes were overexpressed to enhance LNn T production,resulting in an 8-fold increase in LNn T titer compared to that of parental strain.To our knowledge,this is the first report on LNn T biosynthesis in S.cerevisiae,opening up the possibility of green production of LNn T using food-safe microorganisms.
基金supported by the Carbon Emission Peak and Neutrality of Jiangsu Province(BE2022031-4)the National Natural Science Foundation of China(Key Program)(52131306,52122209,52403001)+1 种基金the Project on National Key R&D Program of China(2021YFB2400400)the Cultivation Program for The Excellent Doctoral Dissertation of Nanjing Tech University。
文摘Sodium-ion hybrid capacitors(SICs)offer inherent energy-power synergy but are constrained by mismatched kinetics and life spans between the anode and cathode materials.Two-dimensional MoS_(2)@C composites demonstrate excellent kinetics and structural stability,thanks to the built-in electric field of the carbon heterostructure and its adaptability to volume changes.Yet,the carbon shell imposes a physical barrier to interfacial Na^(+)diffusion,while deep discharge induces the formation of crystalline Na_(2)S,accompanied by severe volumetric expansion and sluggish reversibility—factors that accelerate capacity fading and structural degradation.To address these challenges,a trace-level Ni doping strategy is introduced,enabling precise modulation of the composite's interlayer structure,electronic configuration,and reaction pathway.Ni incorporation expands the MoS_(2) interlayer spacing,reconstructs short-range ordered nanocrystals within a hierarchically porous network,and promotes Na^(+)diffusion by weakening interlayer van der Waals forces.Orbital hybridization between Ni-3d and Mo-4d/S-3p states enhances electronic conductivity and reduces charge transfer resistance.Critically,Ni doping enhances electron transfer from Ni to sulfur,which weakens Na–S bonds and promotes the formation of amorphous Na_(2)S,thereby suppressing crystalline Na_(2)S and enabling a reversible MoS_(2)/Na_(2)S conversion mechanism for improved structural stability and cycling performance.As a result,the optimized MoS_(2)-Ni@C anode delivers a high reversible capacity of 334 mAh g^(-1)at 10 A g^(-1)with 68%retention after 10,000 cycles.When assembled into a SIC device(MoS_(2)-Ni@C//AC),it achieves an energy density of 135 Wh kg^(-1)at a power density of 60.8 kW kg^(-1)(based on anode mass),with 76%retention over 3,000 cycles.
基金supported by the National Nature Science Foundation of China(62504130)National Key Research and Development Program of China(2018YFB0704100)+1 种基金the Key university laboratory of highly efficient utilization of solar energy and sustainable development of Guangdong(Y01256331)the Technology Development Project of Henan Province(252102240047).
文摘Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we demonstrate that TSP perovskite films exhibit a vertically gradient distribution of residual PbI_(2)clusters,which form Schottky heterojunctions with the perovskite,leading to substantial interfacial energy-level mismatches within NiO_(x)-based TSP p-i-n PSCs.These limitations were effectively addressed via a vertical interfacial engineering enabled by dual-interface modification incorporating tin trifluoromethanesulfonate(Sn(OTF)_(2))and 4-Fluorophenylethylamine chloride(F-PEA)at the NiO_(x)/perovskite and perovskite/C60 interfaces,respectively.The functional Sn(OTF)_(2)not only enhances the conductivity of NiO_(x)films but also suppresses ion migration,while inducing the formation of a Pb-Sn mixed perovskite interlayer that precisely regulates the energy level at the NiO_(x)/perovskite interface.Complementally,F-PEA post-treatment effectively converts surface residual PbI_(2)clusters into a 2D perovskite capping layer,which simultaneously passivates surface defects and enhances energy-level alignment at the perovskite/C60 interface.Consequently,the optimized NiO_(x)-based TSP p-i-n PSCs achieve a notable PCE of 25.6%with superior operational stability.This study elucidates the underlying mechanisms limiting the efficiency of TSP p-i-n PSCs,while establishing design principles for these devices targeting 26%efficiency.
基金supported by the National Natural Science Foundation of China(Nos.52122408 and 52474397)the High-level Talent Research Start-up Project Funding of Henan Academy of Sciences(No.242017127)+1 种基金the financial support from the Fundamental Research Funds for the Central Universities(University of Science and Technology Beijing(USTB),Nos.FRF-TP-2021-04C1 and 06500135)supported by USTB MatCom of Beijing Advanced Innovation Center for Materials Genome Engineering。
文摘High-performance alloys are indispensable in modern engineering because of their exceptional strength,ductility,corrosion resistance,fatigue resistance,and thermal stability,which are all significantly influenced by the alloy interface structures.Despite substantial efforts,a comprehensive overview of interface engineering of high-performance alloys has not been presented so far.In this study,the interfaces in high-performance alloys,particularly grain and phase boundaries,were systematically examined,with emphasis on their crystallographic characteristics and chemical element segregations.The effects of the interfaces on the electrical conductivity,mechanical strength,toughness,hydrogen embrittlement resistance,and thermal stability of the alloys were elucidated.Moreover,correlations among various types of interfaces and advanced experimental and computational techniques were examined using big data analytics,enabling robust design strategies.Challenges currently faced in the field of interface engineering and emerging opportunities in the field are also discussed.The study results would guide the development of next-generation high-performance alloys.
基金supported by the School of Engineering and Digital Sciences of Nazarbayev University,Astana,Kazakhstan(to CE)。
文摘The osteochondral(OC)interface exhibits a mineral gradient,varying in thickness by several hundred micrometers across different species.Disruptions in this interface damage OC tissues,leading to osteoarthritis.The natural architecture and composition of native OC interfaces can be replicated using biomaterial scaffolds via regenerative engineering approaches.A novel one-step bioextrusion process was employed to fabricate a unitary synthetic graft(USG),which mimics the native OC interface’s mineral concentration gradient.This novel USG is composed of an agarose-based cartilage layer and a bone layer,consisting of agarose enriched with 20%(200 g/L)hydroxyapatite.The USG features a gradient interface with mineral concentrations transitioning from 0%to 20%(mass fraction),mimicking the transition between the cartilage and bone.Thermogravimetric analysis revealed that the gradient transition lengths of the graft and native OC tissue harvested from bovine knees were similar((647±21)vs.(633±124)μm).The linear viscoelastic properties of the grafts,which were evaluated using strain sweep and frequency sweep tests with oscillatory shear,indicated a dominant storage modulus over loss modulus similar to that of native OC tissues.The compressive and stress relaxation behaviors of the USGs demonstrated that the graft maintained structural integrity under mechanical stress.Viability assays performed after bioextrusion showed that chondrocytes and human fetal osteoblast cells successfully integrated and survived within their designated regions of the graft.The novel USGs exhibit properties similar to native OC tissue and are promising candidates for regenerating OC defects and restoring knee joint functionality.
基金supported by the National Natural Science Foundation of China(Grant Nos.52102165 and 62474056)the Natural Science Foundation of Nanjing University of Posts and Telecommunications(Grant Nos.NY221029 and NY222165)。
文摘All-inorganic lead-free perovskite solar cells have emerged as environmentally benign candidates;however,their device performance is still constrained by pronounced carrier recombination losses in the bulk and at interfaces.By combining energy band alignment analysis with detailed modeling of recombination mechanisms,a systematic strategy for optimizing hole transport layers is developed.The results reveal that a negative valence band offset produces a cliff-like interface,which facilitates hole extraction while also accounting for the observed variations in open-circuit voltage.Furthermore,short-circuit current losses are quantitatively attributed to different recombination pathways,modeled by incorporating radiative,Shockley–Read–Hall,Auger,and interface recombination processes.This comprehensive approach not only clarifies the correlation between energy level alignment and recombination dynamics but also highlights the competing roles of band offset and interface defects in determining device performance.The optimized device architecture,based on Ge-based lead-free perovskites,achieves a power conversion efficiency of 25.1%,with an open-circuit voltage of 1.29 V,a short-circuit current density of 22.5 mA·cm^(-2),and a fill factor of 86.3%.These findings provide theoretical guidance for designing stable,high-performance,and environmentally friendly lead-free perovskite solar cells.
基金CHINA POSTDOCTORAL SCIENCE FOUNDATION(Grant No.2025M771925)Young Scientists Fund(C Class)(Grant No.32501636)Special Fund of Fundamental Scientific Research Business Expense for Higher School of Central Government(Grant No.2572025JT04).
文摘This paper introduces a novel nature-inspired metaheuristic algorithm called the Gekko japonicus algorithm.The algo-rithm draws inspiration mainly from the predation strategies and survival behaviors of the Gekko japonicus.The math-ematical model is developed by simulating various biological behaviors of the Gekko japonicus,such as hybrid loco-motion patterns,directional olfactory guidance,implicit group advantage tendencies,and the tail autotomy mechanism.By integrating multi-stage mutual constraints and dynamically adjusting parameters,GJA maintains an optimal balance between global exploration and local exploitation,thereby effectively solving complex optimization problems.To assess the performance of GJA,comparative analyses were performed against fourteen state-of-the-art metaheuristic algorithms using the CEC2017 and CEC2022 benchmark test sets.Additionally,a Friedman test was performed on the experimen-tal results to assess the statistical significance of differences between various algorithms.And GJA was evaluated using multiple qualitative indicators,further confirming its superiority in exploration and exploitation.Finally,GJA was utilized to solve four engineering optimization problems and further implemented in robotic path planning to verify its practical applicability.Experimental results indicate that,compared to other high-performance algorithms,GJA demonstrates excep-tional performance as a powerful optimization algorithm in complex optimization problems.We make the code publicly available at:https://github.com/zhy1109/Gekko-japonicusalgorithm.
