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
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
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
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
Aqueous zinc(Zn)metal batteries(AZMBs)have distinct advantages in terms of safety and cost-effectiveness.However,the industrial application of AZMBs is currently not ready due to challenges of Zn dendrite growth and t...Aqueous zinc(Zn)metal batteries(AZMBs)have distinct advantages in terms of safety and cost-effectiveness.However,the industrial application of AZMBs is currently not ready due to challenges of Zn dendrite growth and the side reactions such as hydrogen evolution reaction(HER)on the Zn anodes.In this review,we discuss how inorganic interfaces impact the Zn^(2+)plating/stripping reaction and overall cell performance.The discussion is categorized based on the types of inorganic materials,including metal oxides,other metal compounds,and inorganic salts.The proposed protection mechanisms for Zn metal anodes are highlighted,with a focus on the dendrite and HER inhibition mechanisms facilitated by various inorganic materials.We also provide our perspective on the rational design of advanced interfaces to enable highly reversible Zn^(2+)plating/stripping reactions toward highly stable AZMBs,paving the way for their practical implementation in energy storage.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
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
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
In the field of organic solar cells(OSCs),side-chain engineering is a key strategy for developing high-performance non-fullerene small molecule acceptors(SMAs),which could adjust the material solubility and modulate t...In the field of organic solar cells(OSCs),side-chain engineering is a key strategy for developing high-performance non-fullerene small molecule acceptors(SMAs),which could adjust the material solubility and modulate the intermolecular stacking properties,profoundly impacting the film morphology and thus acting on the final power conversion efficiency(PCE) of the materials.In this study,two asymmetric acceptor molecules,Qx-Ph Br-BO and Qx-Ph Br-X,were synthesized by migrating the branching site of the outer side chain from the β-site to the γ-site.The branching site located at the γ-site could reduce the steric-hindrance effect and enhance the molecular aggregation behavior,giving rise to redshifted absorption and tight π-π stacking.Morphology analysis shows that the Qx-Ph Br-X-based devices have smoother surfaces and a phase-separated structure,which is more favorable for charge transport and extraction.The Qx-Ph Br-X-based devices exhibit balanced hole-electron mobility,efficient exciton dissociation,and low charge recombination.As a result,Qx-Ph Br-X with γ-site branching exhibits superior photovoltaic performance with a PCE of 17.16 %,which is significantly higher than that of Qx-Ph Br-BO at 16.28 %.These results highlight the importance of side-chain modifications for optimizing OSC efficiency and provide an important reference for precise tuning of side-chain structures in future molecular design.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
Rechargeable alkali metal-sulfur(M-S)batteries,including Li/Na/K-S chemistries,have the potential to utilize abundant and low-cost sulfur cathodes yet offer high theoretical energy densities.However,their practical el...Rechargeable alkali metal-sulfur(M-S)batteries,including Li/Na/K-S chemistries,have the potential to utilize abundant and low-cost sulfur cathodes yet offer high theoretical energy densities.However,their practical electrochemical performance is fundamentally limited by the polysulfide shuttle effect.This challenge is particularly exacerbated in Na-S and K-S systems owing to larger metal-ion radii,weaker solvation energies,slower redox kinetics,and greater electrolyte-electrode incompatibilities compared to Li-S batteries.This review presents a comparative analysis of interface engineering strategies designed to suppress the shuttle effect across these three systems.Following a summary of sulfur cathode properties and reaction mechanisms,we systematically examine the origins of polysulfide shuttling.Our analysis progresses from functional separator design and interlayer enhancements to the implementation of solid-state electrolytes for root-cause inhibition.By evaluating interface engineering research specific to Na-S and K-S batteries,we elucidate both shared principles and unique challenges inherent to alkali M-S systems.Finally,we propose multifaceted solutions to achieve shuttlefree operation and enhance overall battery performance,thereby establishing a foundation for future advancements.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
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
Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challeng...Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challenges such as structural phase transitions,Na^(+)/vacancy ordering,and Jahn–Teller distortion effect,resulting in severe capacity decay and sluggish ion kinetics.We develop a novel Cu/Y dual-doping strategy that leads to the formation of"Na–Y"interlayer aggregates,which act as structural pillars within alkali metal layers,enhancing structural stability and disrupting the ordered arrangement of Na^(+)/vacancies.This disruption leads to a unique coexistence of ordered and disordered Na^(+)/vacancy states with near-zero strain,which significantly improves Na^(+)diffusion kinetics.This structural innovation not only mitigates the unfavorable P2–O2 phase transition but also facilitates rapid ion transport.As a result,the doped material demonstrates exceptional electrochemical performance,including an ultra-long cycle life of 3000 cycles at 10 C and an outstanding high-rate capability of~70 mAh g^(−1)at 50 C.The discovery of this novel interlayer pillar,along with its role in modulating Na^(+)/vacancy arrangements,provides a fresh perspective on engineering layered oxides.It opens up promising new pathways for the structural design of advanced cathode materials toward efficient,stable,and high-rate SIBs.展开更多
Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventi...Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventional carbon anodes that cannot match the fast capacitive anion intercalation behavior of graphite cathodes constraints on improving power density of SDIBs.Herein,we present an ingenious carbon microdomain engineering strategy to fabricate high-performance carbon anode with ion-mediated high-activity nitrogen species and molecular-scale closed-pore architectures.Experimental characterizations and theoretical investigations demonstrate that Zn^(2+)-mediated structural engineering tailors oxidized nitrogen species,which proficiently accelerate the sodium-ion desolvation kinetics;meanwhile the acetate-mediated pore-forming process modulates closed pores,which synergistically afford abundant sodium storage sites for high plateau-region capacity.As a result,the optimized microdomain engineered carbon material(MEC_(3))tailored with the optimal amount of zinc acetate demonstrates an outstanding plateau-region capacity of 253 mAh g^(-1)even at 1 C,among the highest reported values.Consequently,the MEC_(3)||expanded graphite dual-ion battery exhibits an unprecedented cycling stability at high current rate,maintaining 80.6%capacity retention after 10,000 cycles at 10 C,among the best reports.This microdomain engineering strategy provides a new design principle for overcoming kinetic limitations of carbonaceous materials in plateau-dominated sodium storage systems.展开更多
The rapid proliferation of microelectronics,coupled with the advent of the internet ofthings(IoT)era,has created an urgent demand for miniaturized,integrable,and reliable on-chip energystorage systems.All-solid-state ...The rapid proliferation of microelectronics,coupled with the advent of the internet ofthings(IoT)era,has created an urgent demand for miniaturized,integrable,and reliable on-chip energystorage systems.All-solid-state thin-film microbatteries(TFMBs),distinguished by their intrinsicsafety,compact design,and compatibility with microfabrication techniques,have emerged as promisingcandidates to power next-generation IoT devices.Nevertheless,in contrast to the well-establisheddevelopment of conventional lithium-ion batteries,the advancement of TFMBs remains at an earlystage,facing persistent challenges in materials innovation,interface optimization,and scalable manufacturing.This review critically examines the pivotal role of vapor deposition technologies,includingmagnetron sputtering,pulsed laser deposition,thermal/electron-beam evaporation,chemical vapordeposition,and atomic layer deposition,in the fabrication and performance modulation of TFMBs.We systematically summarize recent progress in thin-film electrodes and solid-state electrolytes,withparticular emphasis on how deposition parameters dictate crystallinity,lattice orientation,and ionictransport in functional layers.Furthermore,we highlight strategies for solid-solid interface engineering,three-dimensional structural design,andmultifunctional integration to enhance capacity retention,cycling stability,and interfacial compatibility.Looking ahead,TFMBs are expectedto evolve toward multifunctional platforms,exhibiting mechanical flexibility,optical transparency,and hybrid energy-harvesting compatibility,thereby meeting the heterogeneous energy requirements of future IoT ecosystems.Overall,this review provides a comprehensive perspective onvapor-phase-enabled TFMB technologies,delivering both theoretical insights and technological guidelines for the scalable realization of highperformancemicroscale power sources.展开更多
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(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 National Natural Science Foundation of China(52272183)the Fundamental Research Funds for the Central Universities(buctrc202316)the support of the China Experience Fund and the Stephen Slavens Faculty Scholar Endowment Fund from Oregon State University。
文摘Aqueous zinc(Zn)metal batteries(AZMBs)have distinct advantages in terms of safety and cost-effectiveness.However,the industrial application of AZMBs is currently not ready due to challenges of Zn dendrite growth and the side reactions such as hydrogen evolution reaction(HER)on the Zn anodes.In this review,we discuss how inorganic interfaces impact the Zn^(2+)plating/stripping reaction and overall cell performance.The discussion is categorized based on the types of inorganic materials,including metal oxides,other metal compounds,and inorganic salts.The proposed protection mechanisms for Zn metal anodes are highlighted,with a focus on the dendrite and HER inhibition mechanisms facilitated by various inorganic materials.We also provide our perspective on the rational design of advanced interfaces to enable highly reversible Zn^(2+)plating/stripping reactions toward highly stable AZMBs,paving the way for their practical implementation in energy storage.
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 (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 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the financial support by the Beijing Natural Science Foundation (No.Z230018)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB0520102)CAS Project for Young Scientists in Basic Research (No.YSBR-102)。
文摘In the field of organic solar cells(OSCs),side-chain engineering is a key strategy for developing high-performance non-fullerene small molecule acceptors(SMAs),which could adjust the material solubility and modulate the intermolecular stacking properties,profoundly impacting the film morphology and thus acting on the final power conversion efficiency(PCE) of the materials.In this study,two asymmetric acceptor molecules,Qx-Ph Br-BO and Qx-Ph Br-X,were synthesized by migrating the branching site of the outer side chain from the β-site to the γ-site.The branching site located at the γ-site could reduce the steric-hindrance effect and enhance the molecular aggregation behavior,giving rise to redshifted absorption and tight π-π stacking.Morphology analysis shows that the Qx-Ph Br-X-based devices have smoother surfaces and a phase-separated structure,which is more favorable for charge transport and extraction.The Qx-Ph Br-X-based devices exhibit balanced hole-electron mobility,efficient exciton dissociation,and low charge recombination.As a result,Qx-Ph Br-X with γ-site branching exhibits superior photovoltaic performance with a PCE of 17.16 %,which is significantly higher than that of Qx-Ph Br-BO at 16.28 %.These results highlight the importance of side-chain modifications for optimizing OSC efficiency and provide an important reference for precise tuning of side-chain structures in future molecular design.
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(52371131)the 10th Youth Talent Lifting Project of the China Association for Science and Technology.
文摘Rechargeable alkali metal-sulfur(M-S)batteries,including Li/Na/K-S chemistries,have the potential to utilize abundant and low-cost sulfur cathodes yet offer high theoretical energy densities.However,their practical electrochemical performance is fundamentally limited by the polysulfide shuttle effect.This challenge is particularly exacerbated in Na-S and K-S systems owing to larger metal-ion radii,weaker solvation energies,slower redox kinetics,and greater electrolyte-electrode incompatibilities compared to Li-S batteries.This review presents a comparative analysis of interface engineering strategies designed to suppress the shuttle effect across these three systems.Following a summary of sulfur cathode properties and reaction mechanisms,we systematically examine the origins of polysulfide shuttling.Our analysis progresses from functional separator design and interlayer enhancements to the implementation of solid-state electrolytes for root-cause inhibition.By evaluating interface engineering research specific to Na-S and K-S batteries,we elucidate both shared principles and unique challenges inherent to alkali M-S systems.Finally,we propose multifaceted solutions to achieve shuttlefree operation and enhance overall battery performance,thereby establishing a foundation for future advancements.
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.
基金supported by the “Pioneer” and “Leading Goose” R&D Program of Zhejiang Province of China (No. 2024C01056)the support from London South Bank University
文摘Layered oxides have attracted significant attention as cathodes for sodium-ion batteries(SIBs)due to their compositional versatility and tuneable electrochemical performance.However,these materials still face challenges such as structural phase transitions,Na^(+)/vacancy ordering,and Jahn–Teller distortion effect,resulting in severe capacity decay and sluggish ion kinetics.We develop a novel Cu/Y dual-doping strategy that leads to the formation of"Na–Y"interlayer aggregates,which act as structural pillars within alkali metal layers,enhancing structural stability and disrupting the ordered arrangement of Na^(+)/vacancies.This disruption leads to a unique coexistence of ordered and disordered Na^(+)/vacancy states with near-zero strain,which significantly improves Na^(+)diffusion kinetics.This structural innovation not only mitigates the unfavorable P2–O2 phase transition but also facilitates rapid ion transport.As a result,the doped material demonstrates exceptional electrochemical performance,including an ultra-long cycle life of 3000 cycles at 10 C and an outstanding high-rate capability of~70 mAh g^(−1)at 50 C.The discovery of this novel interlayer pillar,along with its role in modulating Na^(+)/vacancy arrangements,provides a fresh perspective on engineering layered oxides.It opens up promising new pathways for the structural design of advanced cathode materials toward efficient,stable,and high-rate SIBs.
基金support from the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(52125105,52572282,52472269,52273312,22309200)+3 种基金Guangdong Basic and Applied Basic Research Foundation(2024A1515010201,2024A1515012379,2024A1515011670,2023A1515011519)Guangdong Special Support Program Outstanding Young Talents in Science and Technology Innovation(2021TQ05L894)Shenzhen Science and Technology Planning Project(JSGG20220831104004008,SGDX20230116092055008,KCXST20221021111606016)the NSRF via the Program Management Unit for Human Resources&Institutional Development,Research and Innovation(B49G680115).
文摘Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventional carbon anodes that cannot match the fast capacitive anion intercalation behavior of graphite cathodes constraints on improving power density of SDIBs.Herein,we present an ingenious carbon microdomain engineering strategy to fabricate high-performance carbon anode with ion-mediated high-activity nitrogen species and molecular-scale closed-pore architectures.Experimental characterizations and theoretical investigations demonstrate that Zn^(2+)-mediated structural engineering tailors oxidized nitrogen species,which proficiently accelerate the sodium-ion desolvation kinetics;meanwhile the acetate-mediated pore-forming process modulates closed pores,which synergistically afford abundant sodium storage sites for high plateau-region capacity.As a result,the optimized microdomain engineered carbon material(MEC_(3))tailored with the optimal amount of zinc acetate demonstrates an outstanding plateau-region capacity of 253 mAh g^(-1)even at 1 C,among the highest reported values.Consequently,the MEC_(3)||expanded graphite dual-ion battery exhibits an unprecedented cycling stability at high current rate,maintaining 80.6%capacity retention after 10,000 cycles at 10 C,among the best reports.This microdomain engineering strategy provides a new design principle for overcoming kinetic limitations of carbonaceous materials in plateau-dominated sodium storage systems.
基金supported by the National Key Research and Development Program of China(2023YFA1608800)Guangdong Basic and Applied Basic Research Foundation(2024A1515012385,2024B1515120042)+5 种基金Shenzhen Foundation Research Fund(JCYJ20240813095004006)the National Natural Science Foundation of China(12426301,12275119,52227802)Shenzhen Science and Technology Program(KQTD20200820113047086)Shenzhen Key Laboratory of Solid State Batteries(SYSPG20241211173726011)Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices(2019B121205001)Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(2018B030322001)。
文摘The rapid proliferation of microelectronics,coupled with the advent of the internet ofthings(IoT)era,has created an urgent demand for miniaturized,integrable,and reliable on-chip energystorage systems.All-solid-state thin-film microbatteries(TFMBs),distinguished by their intrinsicsafety,compact design,and compatibility with microfabrication techniques,have emerged as promisingcandidates to power next-generation IoT devices.Nevertheless,in contrast to the well-establisheddevelopment of conventional lithium-ion batteries,the advancement of TFMBs remains at an earlystage,facing persistent challenges in materials innovation,interface optimization,and scalable manufacturing.This review critically examines the pivotal role of vapor deposition technologies,includingmagnetron sputtering,pulsed laser deposition,thermal/electron-beam evaporation,chemical vapordeposition,and atomic layer deposition,in the fabrication and performance modulation of TFMBs.We systematically summarize recent progress in thin-film electrodes and solid-state electrolytes,withparticular emphasis on how deposition parameters dictate crystallinity,lattice orientation,and ionictransport in functional layers.Furthermore,we highlight strategies for solid-solid interface engineering,three-dimensional structural design,andmultifunctional integration to enhance capacity retention,cycling stability,and interfacial compatibility.Looking ahead,TFMBs are expectedto evolve toward multifunctional platforms,exhibiting mechanical flexibility,optical transparency,and hybrid energy-harvesting compatibility,thereby meeting the heterogeneous energy requirements of future IoT ecosystems.Overall,this review provides a comprehensive perspective onvapor-phase-enabled TFMB technologies,delivering both theoretical insights and technological guidelines for the scalable realization of highperformancemicroscale power sources.
