Lithium-rich manganese-based cathode materials(LMCMs)have garnered significant attention in power lithium-ion batteries(LIBs)and energy storage systems due to their superior energy density and costeffectiveness.Howeve...Lithium-rich manganese-based cathode materials(LMCMs)have garnered significant attention in power lithium-ion batteries(LIBs)and energy storage systems due to their superior energy density and costeffectiveness.However,the commercial application of LMCMs is hindered by challenges such as low initial coulombic efficiency,severe voltage decay,and inferior cycling performance.Surface structure degradation has been confirmed as a critical factor contributing to the electrochemical performance deterioration of LMCMs.Herein,we review the recent progress in surface engineering of LMCMs towards next-generation LIBs.Besides classical surface coating,mechanism and functions of surface oxygen vacancies for greatly boosting the electrochemical performance of LMCMs are also summarized in detail.Finally,we discuss the emerging trends and propose future research directions of surface engineering of LMCMs for achieving more efficient improvements.This work underscores the indispensable potential of surface engineering in enhancing the surface structure stability and electrochemical performance of LMCMs as promising candidates for next-generation high-energy LIBs.Synergistic integration of surface engineering and single-crystal technology will be a promising modification strategy for significantly promoting the commercialization of LMCMs,and the corresponding synergistic mechanisms urgently need to be studied for rationally designing high-performance electrodes.More efforts will be devoted to understand the surface engineering of LMCMs for the large-scale application of high-energy LIBs.展开更多
Precise control of luminescence in carbon quantum dots(CQDs),from single-color to full-color emission,is crucial for advancing their applications in biomedical imaging and display technologies.While CQDs luminescence ...Precise control of luminescence in carbon quantum dots(CQDs),from single-color to full-color emission,is crucial for advancing their applications in biomedical imaging and display technologies.While CQDs luminescence is primarily influenced by conjugated domains and surface states,the underlying interaction mechanisms remain poorly understood.This study explores a graded nitro-engineering approach to simultaneously regulate surface states and sp^(2)conjugated domains through nitro(-NO_(2))modulation,enabling comprehensive color tuning.Using o-phenylenediamine(o-PD)as the carbon source and adjusting nitric acid(HNO_(3))concentrations,we synthesized tricolor-emitting nitro-functionalized CQDs(NO_(2)-CQDs).At lower-NO_(2) concentrations,luminescence is mainly influenced by surface states,where the electron-withdrawing effect of-NO_(2) enhancesπ-electron delocalization and stabilizes sp^(2)conjugation.With increasing-NO_(2) content,the lowest unoccupied molecular orbital(LUMO)energy level decreases(-2.12 eV to-3.39 eV),resulting in a red-shift in fluorescence.At higher-NO_(2) concentrations,luminescence is primarily affected by the sp^(2)conjugated domain,where steric hindrance reduces molecular planarity and conjugation,leading to a blue-shift in fluorescence as the sp^(2)domain size decreases(4.03 nm to 2.83 nm).Combining experimental results with density functional theory(DFT)calculations,we reveal the dual role of-NO2in modulating CQDs luminescence,an approach rarely achieved through surface functionalization.This work presents a novel strategy for precise tuning of CQDs luminescence across the visible spectrum.展开更多
This review provides an insightful and comprehensive exploration of the emerging 2D material borophene,both pristine and modified,emphasizing its unique attributes and potential for sustainable applications.Borophene...This review provides an insightful and comprehensive exploration of the emerging 2D material borophene,both pristine and modified,emphasizing its unique attributes and potential for sustainable applications.Borophene’s distinctive properties include its anisotropic crystal structures that contribute to its exceptional mechanical and electronic properties.The material exhibits superior electrical and thermal conductivity,surpassing many other 2D materials.Borophene’s unique atomic spin arrangements further diversify its potential application for magnetism.Surface and interface engineering,through doping,functionalization,and synthesis of hybridized and nanocomposite borophene-based systems,is crucial for tailoring borophene’s properties to specific applications.This review aims to address this knowledge gap through a comprehensive and critical analysis of different synthetic and functionalisation methods,to enhance surface reactivity by increasing active sites through doping and surface modifications.These approaches optimize diffusion pathways improving accessibility for catalytic reactions,and tailor the electronic density to tune the optical and electronic behavior.Key applications explored include energy systems(batteries,supercapacitors,and hydrogen storage),catalysis for hydrogen and oxygen evolution reactions,sensors,and optoelectronics for advanced photonic devices.The key to all these applications relies on strategies to introduce heteroatoms for tuning electronic and catalytic properties,employ chemical modifications to enhance stability and leverage borophene’s conductivity and reactivity for advanced photonics.Finally,the review addresses challenges and proposes solutions such as encapsulation,functionalization,and integration with composites to mitigate oxidation sensitivity and overcome scalability barriers,enabling sustainable,commercial-scale applications.展开更多
Rechargeable aqueous zinc-ion batteries(AZIBs)exhibit appreciable potential in the domain of electrochemical energy storage.However,there are serious challenges for AZIBs,for instance zinc dendrite growth,hydrogen evo...Rechargeable aqueous zinc-ion batteries(AZIBs)exhibit appreciable potential in the domain of electrochemical energy storage.However,there are serious challenges for AZIBs,for instance zinc dendrite growth,hydrogen evolution reaction(HER),and corrosion side reactions.Herein,we propose a surface engineering modification strategy for coating the montmorillonite(MMT)layer onto the surface of the Zn anode to tackle these issues,thereby achieving high cycling stability for rechargeable AZIBs.The results reveal that the MMT layer on the surface of the Zn anode is able to provide ordered zincophilic channels for zinc ions migration,facilitating the reaction kinetics of zinc ions.Density functional theory(DFT)calculations and water contact angle(CA)tests prove that MMT@Zn anode exhibits superior adsorption capacity for Zn^(2+)and better hydrophobicity than the bare Zn anode,thereby achieving excellent cycling stability.Moreover,the MMT@Zn||MMT@Zn symmetric cell holds the stable cycling over 5600 h at 0.5 mA cm^(-2)and 0.125 m A h cm^(-2),even exceeding 1800 h long cycling under harsh conditions of 5 m A cm^(-2)and 1.25 m A h cm^(-2).The MMT@Zn||V_(2)O_(5)full cell reaches over 3000 cycles at 2 A g^(-1)with excellent rate capability.Therefore,this surface engineering modification strategy for enhancing the electrochemical performance of AZIBs represents a promising application.展开更多
Near-surface geological defects pose a serious threat to human life and infrastructure.Hence,the exploration of geological hazards is essential.Currently,there are various geological hazard exploration methods;however...Near-surface geological defects pose a serious threat to human life and infrastructure.Hence,the exploration of geological hazards is essential.Currently,there are various geological hazard exploration methods;however,those require improvements in terms of economic feasibility,convenience,and lateral resolution.To address this,this study examined an extraction method to determine spatial autocorrelation velocity dispersion curves for application in near-surface exploration.展开更多
Expanding the specific surface area of substrates and carrying out precise surface engineering of imprinted nanocavities are crucial methods for enhancing the identification efficiency of molecularly imprinted polymer...Expanding the specific surface area of substrates and carrying out precise surface engineering of imprinted nanocavities are crucial methods for enhancing the identification efficiency of molecularly imprinted polymers(MIPs).To implement this synergistic strategy,bioinspired surface engineering was used to incorporate dual covalent receptors via precise post-imprinting modifications(PIMs)onto mesoporous silica nanosheets.The prepared sorbents(denoted as‘‘D-PMIPs”)were utilized to improve the specific identification of adenosine 5-monophosphate(AMP).Significantly,the mesoporous silica nanosheets possess a high surface area of approximately 498.73 m^(2)·g^(-1),which facilitates the formation of abundant specific recognition sites in the D-PMIPs.The dual covalent receptors are valuable for estab-lishing the spatial orientation and arrangement of AMP through multiple cooperative interactions.PIMs enable precise site-specific functionalization within the imprinted cavities,leading to the tailor-made formation of complementary binding sites.The maximum number of high-affinity binding sites(Nmax)of the D-PMIPs is 39.99 lmol·g^(-1),which is significantly higher than that of imprinted sorbents with a sin-gle receptor(i.e.,S-BMIPs or S-PMIPs).The kinetic data of the D-PMIPs can be effectively described by a pseudo-second-order model,indicating that the main binding mechanism involves synergistic chemisorption from boronate affinity and the pyrimidine base.This study suggests that using dual cova-lent receptors and PIMs is a reliable approach for creating imprinted sorbents with high selectivity,allow-ing for the controlled engineering of imprinted sites.展开更多
For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable sur...For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable surface and interfacial properties.Various single crystal types,including metals,semiconductors,ceramics,organics,and nanocrystals,exhibit superior catalytic selectivity and stability in reactions such as water splitting and carbon/nitrogen cycles,benefiting from high electrical conductivity,tunable energy bands,and active sites with high surface energy.Through surface modification,interfacial atomic doping,and heterostructure construction,the distribution of active sites,electronic structure,and mass transport can be precisely regulated,significantly optimizing the catalytic kinetics of single crystal materials.In situ characterizations elucidate catalytic mechanisms at the atomic scale,while emerging methods like AI-assisted synthesis and bio-template directed growth offer pathways to overcome bottlenecks in the precision and cost of single crystal preparation.In addressing stability challenges in complex environments,strategies such as organic-inorganic hybridization and gradient interface design effectively mitigate interfacial instability.Future research should focus on cross-scale structural regulation and multidisciplinary integration to facilitate the transition of single crystal electrocatalysts from fundamental research to industrial applications,enabling efficient energy conversion.展开更多
The present work explored effects of laser surface melting on microstructure and surface topography evolution in AZ31B magnesium alloy.Thermokinetic effects experienced by the material during laser surface melting wer...The present work explored effects of laser surface melting on microstructure and surface topography evolution in AZ31B magnesium alloy.Thermokinetic effects experienced by the material during laser surface melting were simulated using a multiphysics finite element model.Microstructure and phase evolution were examined using scanning electron microscopy,X-ray diffraction,and electron back scatter diffraction.Surface topography was evaluated using white light interferometry.The interaction of surface melted samples with simulated body fluid was monitored by contact angle measurements and immersion studies up to 7 days.Laser surface melting led to formation of a refined microstructure with predominantly basal crystallographic texture.Concurrently,the amount ofβphase(Mg_(17)Al_(12))increased with an increase in the laser fluence.βphase preferentially decorated the cell boundaries.In terms of topography,the surface became progressively rougher with an increase in laser fluence.As a result,upon immersion in simulated body fluid,the laser surface melted samples showed an improved wettability,corrosion resistance,and precipitation of mineral having composition closer to the hydroxyapatite bone mineral compared to the untreated sample.展开更多
Lithium-sulfur(Li-S)batteries have been recognized as one of the most promising candidates for nextgeneration portable electronic devices,owing to their extremely high energy density and low cost.However,the dissoluti...Lithium-sulfur(Li-S)batteries have been recognized as one of the most promising candidates for nextgeneration portable electronic devices,owing to their extremely high energy density and low cost.However,the dissolution of lithium polysulfides(LiPSs)and consequent"shuttle effect"seriously hinder the practical deployment of Li-S batteries.Herein,multi-metal oxide nanorods named attapulgite are proposed as multifunctional ionic sieve to immobilize LiPSs and further promote the regulation of LiPSs.Attapulgite,consisting of Al,Mg,Fe,Si and O ions,possesses more polar sites to immobilize LiPSs in comparison with single metal oxides.In addition,the catalytic nature(Fe ions)of attapulgite avails the LiPSs conversion reaction,which is further confirmed by the linear sweep voltammetry and electrochemical impedance spectroscopy.Benefited from the synergistic effect of multi-metal oxide and conductive carbon,the Li-S battery with the modified separator delivers remarkable discharge capacities of 1059.4 mAh g-1 and 792.5 mAh g-1 for the first and 200th cycle at 0.5 C,respectively.The work presents an effective way to improve the electrochemical performance of Li-S batteries by employing attapulgite nanorods assisted separator surface engineering.展开更多
To date,much efforts have been devoted to the high-efficiency noble metal-free electrocatalysts for hydrogen-and oxygen-involving energy conversion reactions,due to their abundance,low cost and nultifunctionally.Surfa...To date,much efforts have been devoted to the high-efficiency noble metal-free electrocatalysts for hydrogen-and oxygen-involving energy conversion reactions,due to their abundance,low cost and nultifunctionally.Surface/interface engineering is found to be effective in achieving novel physicochemical properties and synergistic effects in nanomaterials for electrocatalysis.Among various engineering strategies,heteroatom-doping has been regarded as a most promising method to improve the electrocatalytic performance via the regulation of electronic structure of catalysts,and numerous works were reported on the synthesis method and mechanism investigation of heteroatom-doping electrocatalysts,though the heteroatom-doping can only provide limited active sites.Engineering of other defects such as vacancies and edge sites and construction of heterostructure have shown to open up a potential avenue for the development of noble metal-free electrocatalysts.In addition,surface functionalization can attach various molecules onto the surface of materials to easily modify their physical or chemical properties,being as a promising complement or substitute for offering materials with catalytic properties.This paper gives the insights into the diverse strategies of surface/interface engineering of the highefficiency noble metal-free electrocatalysts for energy-related electrochemical reactions.The significant advances are summarized.The unique advantages and mechanisms for specific applications are highlighted.The current challenges and outlook of this growing field are also discussed.展开更多
Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2...Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2)RR)is still challenging owing to the sluggish kinetics or unfavorable thermodynamics for basic chemical processes of CO_(2)RR,such as adsorption,activation,conversion and product desorption.To overcome these shortcomings,recent works have demonstrated that surface engineering of semiconductors,such as introducing surface vacancy,surface doping,and cocatalyst loading,serves as effective or promising strategies for improved photocatalytic CO_(2)RR with high activity and selectivity.The essential reason lies in the activation and reaction pathways can be optimized and regulated through the reconstruction of surface atomic and electronic structures.Herein,in this review,we focus on recent research advances about rational design of semiconductor surface for photocatalytic CO_(2)RR.The surface engineering strategies for improved CO_(2)adsorption,activation,and product selectivity will be reviewed.In addition,theoretical calculations along with in situ characterization techniques will be in the spotlight to clarify the kinetics and thermodynamics of the reaction process.The aim of this review is to provide deep understanding and rational guidance on the design of semiconductors for photocatalytic CO_(2)RR.展开更多
The safety and cycle lifespan of zinc metal-based aqueous batteries are greatly restricted by zinc anode.The poor cycling performance of zinc metal anode is often considered to be impacted by the dendrite growth,surfa...The safety and cycle lifespan of zinc metal-based aqueous batteries are greatly restricted by zinc anode.The poor cycling performance of zinc metal anode is often considered to be impacted by the dendrite growth,surface passivation,zinc metal corrosion and hydrogen evolution reaction,while surface roughness is a matter that has often been ignored in past studies.Herein,a roughness gradient is constructed on the zinc anode surface by a simple grinding and pasting method.It has been found the modified zinc anodes with lower surface roughness exhibit the smaller zinc deposition overpotential and longer cycle life.Further,in situ optical microscopy photographs indicate that the zinc anode with an optimized roughness enables more uniform distribution of zinc precipitation and corrosion sites,which will facilitate a stable cycling performance of aqueous zinc ion batteries.The Zn anode dendrite-suppressing mechanism via surface roughness engineering was revealed through finite element computational simulation.These results emphasize the effectiveness of roughness engineering for tuning the surface physics of Zn anode and provide a facile strategy to develop better and safer aqueous zinc ion batteries.展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides a promising way to convert CO_(2)to chemicals.The multicarbon(C_(2+))products,especially ethylene,are of great interest due to their versatile indust...Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides a promising way to convert CO_(2)to chemicals.The multicarbon(C_(2+))products,especially ethylene,are of great interest due to their versatile industrial applications.However,selectively reducing CO_(2)to ethylene is still challenging as the additional energy required for the C–C coupling step results in large overpotential and many competing products.Nonetheless,mechanistic understanding of the key steps and preferred reaction pathways/conditions,as well as rational design of novel catalysts for ethylene production have been regarded as promising approaches to achieving the highly efficient and selective CO_(2)RR.In this review,we first illustrate the key steps for CO_(2)RR to ethylene(e.g.,CO_(2)adsorption/activation,formation of~*CO intermediate,C–C coupling step),offering mechanistic understanding of CO_(2)RR conversion to ethylene.Then the alternative reaction pathways and conditions for the formation of ethylene and competitive products(C_1 and other C_(2+)products)are investigated,guiding the further design and development of preferred conditions for ethylene generation.Engineering strategies of Cu-based catalysts for CO_(2)RR-ethylene are further summarized,and the correlations of reaction mechanism/pathways,engineering strategies and selectivity are elaborated.Finally,major challenges and perspectives in the research area of CO_(2)RR are proposed for future development and practical applications.展开更多
The sluggish kinetics of multiphase sulfur conversion with homogeneous and heterogeneous electrochemical processes,causing the“shuttle effect”of soluble polysulfide species(PSs),is the challenges in terms of lithium...The sluggish kinetics of multiphase sulfur conversion with homogeneous and heterogeneous electrochemical processes,causing the“shuttle effect”of soluble polysulfide species(PSs),is the challenges in terms of lithium-sulfur batteries(LSBs).In this paper,a Mn_(3)O_(4-x) catalyst,which has much higher activity for heterogeneous reactions than for homogeneous reactions(namely,preferentialactivity catalysts),is designed by surface engineering with rational oxygen vacancies.Due to the rational design of the electronic structure,the Mn_(3)O_(4-x) catalyst prefers to accelerate the conversion of Li2S4 into Li_(2)S_(2)/Li_(2)S and optimize Li_(2)S deposition,reducing the accumulation of PSs and thus suppressing the“shuttle effect.”Both density functional theory calculations and in situ X-ray diffraction measurements are used to probe the catalytic mechanism and identify the reaction intermediates of MnS and Li_(y)Mn_(z)O_(4-x) for fundamental understanding.The cell with Mn_(3)O_(4-x) delivers an ultralow attenuation rate of 0.028% per cycle over 2000 cycles at 2.5 C.Even with sulfur loadings of 4.93 and 7.10mg cm^(-2) in a lean electrolyte(8.4μL mg s^(-1)),the cell still shows an initial areal capacity of 7.3mAh cm^(-2).This study may provide a new way to develop preferential-activity heterogeneous-reaction catalysts to suppress the“shuttle effect”of the soluble PSs generated during the redox process of LSBs.展开更多
Amorphous metal-based catalysts(AMCs)have sparked intense research interests in the field of electrocatalysis elicited by their hallmark features such as unlimited volume and morphology,manipulated electronic structur...Amorphous metal-based catalysts(AMCs)have sparked intense research interests in the field of electrocatalysis elicited by their hallmark features such as unlimited volume and morphology,manipulated electronic structures,enriched defects,and unsaturated surface atom coordination.Nevertheless,the manipulation of the amorphous phase in metal-based catalysts is so far impractical,and thus their electrocatalytic mechanism yet remains ambiguous.In this review,the latest advances in AMCs are systematically reviewed,covering amorphous-phase engineering strategy,structure manipulation,and amorphization of various material categories for electrocatalysis.Specifically,a series of applications of AMCs in electrocatalysis for the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),and oxygen evolution reaction(OER)are summarized based on the classification criteria of substances.Finally,we put forward current challenges that have not yet been clarified in the field of AMCs,and propose possible solutions,particularly from the perspective of the evolution of electron microscopy.It is expected to promote the understanding of the amorphization-catalysis relationship and provide a guideline for designing high-performance electrocatalysts.展开更多
Opportunities coexist with challenges for the development of carbon-based cathodes with a high energy density applied for zinc ion hybrid capacitors(ZIHCs).In the present study,a facile and effective surface engineeri...Opportunities coexist with challenges for the development of carbon-based cathodes with a high energy density applied for zinc ion hybrid capacitors(ZIHCs).In the present study,a facile and effective surface engineering approach is demonstrated to greatly improve the energy storage ability of commercial carbon paper(CP)in ZIHC.Benefiting from the introduced oxygen functional groups,larger surface area and improved surface wettability upon air calcination,the assembled aqueous ZIHC with the functionalized carbon paper(FCP)exhibits a much higher areal capacity of 0.22 mAh/cm^(2)at 1 mA/cm^(2),outperforming the counterpart with blank CP by over 5000 times.More importantly,a superior energy density and power density of 130.8μWh/cm^(2)and 7460.5μW/cm^(2),are respectively delivered.Furthermore,more than 90%of the initial capacity is retained over 10000 cycles.This surface engineering strategy to improve the energy storage capability is potentially applicable to developing a wide range of high-energy carbon electrode materials.展开更多
Surface structural engineering is desirable in modifying the surface performance of carbonyl iron powder(CIP)to enhance microwave absorption(MA)and anti-oxidation performance.Herein,the surface shape-dependent CIP abs...Surface structural engineering is desirable in modifying the surface performance of carbonyl iron powder(CIP)to enhance microwave absorption(MA)and anti-oxidation performance.Herein,the surface shape-dependent CIP absorbers are designed via surface coating with zinc oxide(ZnO)nanoparticles and then a thermal annealing treatment.The morphology of ZnO nanoparticles which can be easily regulated by controlling the annealing temperature ultimately affects the MA performance of CIP coating with ZnO nanoparticles(CIP@ZnO).The core-shell CIP@ZnO particles with cubic cone ZnO nanoparticles exhibit ex-cellent MA performance and thermal stability in comparison to the original CIP.Specifically,the CIP@ZnO annealed at 350 ℃(CIP@ZnO-350)samples which have the cubic cone ZnO nanoparticles exhibit a min-imum reflection loss(RLmin)of-55.35 dB at a thickness of 2.1 mm and a maximum effective absorp-tion bandwidth(EAB)of 7.09 GHz at a thickness of 2.0 mm.In addition,the antioxidant property of the CIP@ZnO composite particles is abruptly enhanced,which breaks the restriction of the application of CIP at high temperatures.The superior MA performance of CIP@ZnO particles with cubic cone ZnO nanoparti-cles comes from the enhancement in surface shape-dependent multiple microwave scattering,interfacial polarization,and electromagnetic-dielectric synergism between ZnO and CIP.展开更多
Although molybdenum disulfide (MoS_(2))-based materials are generally known as active electrocatalysts for the hydrogen evolution reaction (HER), the inert performance for the oxygen evolution reaction (OER) seriously...Although molybdenum disulfide (MoS_(2))-based materials are generally known as active electrocatalysts for the hydrogen evolution reaction (HER), the inert performance for the oxygen evolution reaction (OER) seriously limits their wide applications in alkaline electrolyzers due to there exists too strong metal-sulfur (M−S) bond in MoS_(2). Herein, by means of surface reorganization engineering of bimetal Al, Co-doped MoS_(2) (devoted as AlCo_(3)-MoS_(2)) through in situ substituting partial oxidation, we successfully significantly activate the OER activity of MoS_(2), which affords a considerably low overpotential of 323 mV at −30 mA cm^(−2), far lower than those of MoS_(2), Al-MoS_(2) and Co-MoS_(2) catalysts. Essentially, the AlCo_(3)-MoS_(2) substrate produces lots of M−O (M=Al, Co and Mo) species with oxygen vacancies, which trigger the surface self-reconstruction of pre-catalysts and simultaneously boost the electrocatalytic OER activity. Moreover, benefiting from the moderate M−O species formed on the surface, the redistribution of surface electron states is induced, thus optimizing the adsorption of OH* and OOH* intermediates on metal oxyhydroxides and awakening the OER activity of MoS_(2).展开更多
Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes of...Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes often declines because of capacity fading during cycling. This decline is primarily attributed to anisotropic lattice strain and oxygen release from cathode surfaces. Given notable structural transformations, complex redox reactions, and detrimental interface side reactions in LRMOs, the development of a single modification approach that addresses bulk and surface issues is challenging. Therefore,this study introduces a surface double-coupling engineering strategy that mitigates bulk strain and reduces surface side reactions. The internal spinel-like phase coating layer, featuring threedimensional(3D) lithium-ion diffusion channels, effectively blocks oxygen release from the cathode surface and mitigates lattice strain. In addition, the external Li_(3)PO_(4) coating layer, noted for its superior corrosion resistance, enhances the interfacial lithium transport and inhibits the dissolution of surface transition metals. Notably, the spinel phase, as excellent interlayer, securely anchors Li_(3)PO_(4) to the bulk lattice and suppresses oxygen release from lattices. Consequently, these modifications considerably boost structural stability and durability, achieving an impressive capacity retention of 83.4% and a minimal voltage decay of 1.49 m V per cycle after 150 cycles at 1 C. These findings provide crucial mechanistic insights into the role of surface modifications and guide the development of high-capacity cathodes with enhanced cyclability.展开更多
A new method of extraction of blend surface feature is presented. It contains two steps: segmentation and recovery of parametric representation of the blend. The segmentation separates the points in the blend region f...A new method of extraction of blend surface feature is presented. It contains two steps: segmentation and recovery of parametric representation of the blend. The segmentation separates the points in the blend region from the rest of the input point cloud with the processes of sampling point data, estimation of local surface curvature properties and comparison of maximum curvature values. The recovery of parametric representation generates a set of profile curves by marching throughout the blend and fitting cylinders. Compared with the existing approaches of blend surface feature extraction, the proposed method reduces the requirement of user interaction and is capable of extracting blend surface with either constant radius or variable radius. Application examples are presented to verify the proposed method.展开更多
基金financially supported by the National Natura Science Foundation of China(51108455,52106264)Civil Aviation Safety Capacity Building Fund(ADSA2022026)+2 种基金Liaoning Revitalization Talents Program(XLYC2018013)Liaoning Province AppliedFoundation Research Program Project(2023JH2/101300215)Unveiled the List of Local Service Projects from Education Department of Liaoning Province(JYTMS20230227)。
文摘Lithium-rich manganese-based cathode materials(LMCMs)have garnered significant attention in power lithium-ion batteries(LIBs)and energy storage systems due to their superior energy density and costeffectiveness.However,the commercial application of LMCMs is hindered by challenges such as low initial coulombic efficiency,severe voltage decay,and inferior cycling performance.Surface structure degradation has been confirmed as a critical factor contributing to the electrochemical performance deterioration of LMCMs.Herein,we review the recent progress in surface engineering of LMCMs towards next-generation LIBs.Besides classical surface coating,mechanism and functions of surface oxygen vacancies for greatly boosting the electrochemical performance of LMCMs are also summarized in detail.Finally,we discuss the emerging trends and propose future research directions of surface engineering of LMCMs for achieving more efficient improvements.This work underscores the indispensable potential of surface engineering in enhancing the surface structure stability and electrochemical performance of LMCMs as promising candidates for next-generation high-energy LIBs.Synergistic integration of surface engineering and single-crystal technology will be a promising modification strategy for significantly promoting the commercialization of LMCMs,and the corresponding synergistic mechanisms urgently need to be studied for rationally designing high-performance electrodes.More efforts will be devoted to understand the surface engineering of LMCMs for the large-scale application of high-energy LIBs.
基金supported by National Natural Science Foundation of China(No.51873085)Natural Science Foundation of Liaoning Province-Outstanding Youth Foundation(No.2022-YQ-14)+2 种基金Liaoning Revitalization Talents Program(No.XLYC2007056)China Scholarship Council(CSC Scholarship,No.202006800009)the Shenyang Science and Technology Project(No.RC230707)。
文摘Precise control of luminescence in carbon quantum dots(CQDs),from single-color to full-color emission,is crucial for advancing their applications in biomedical imaging and display technologies.While CQDs luminescence is primarily influenced by conjugated domains and surface states,the underlying interaction mechanisms remain poorly understood.This study explores a graded nitro-engineering approach to simultaneously regulate surface states and sp^(2)conjugated domains through nitro(-NO_(2))modulation,enabling comprehensive color tuning.Using o-phenylenediamine(o-PD)as the carbon source and adjusting nitric acid(HNO_(3))concentrations,we synthesized tricolor-emitting nitro-functionalized CQDs(NO_(2)-CQDs).At lower-NO_(2) concentrations,luminescence is mainly influenced by surface states,where the electron-withdrawing effect of-NO_(2) enhancesπ-electron delocalization and stabilizes sp^(2)conjugation.With increasing-NO_(2) content,the lowest unoccupied molecular orbital(LUMO)energy level decreases(-2.12 eV to-3.39 eV),resulting in a red-shift in fluorescence.At higher-NO_(2) concentrations,luminescence is primarily affected by the sp^(2)conjugated domain,where steric hindrance reduces molecular planarity and conjugation,leading to a blue-shift in fluorescence as the sp^(2)domain size decreases(4.03 nm to 2.83 nm).Combining experimental results with density functional theory(DFT)calculations,we reveal the dual role of-NO2in modulating CQDs luminescence,an approach rarely achieved through surface functionalization.This work presents a novel strategy for precise tuning of CQDs luminescence across the visible spectrum.
基金the Engineering and Physical Sciences Research Council(EPSRC)for funding the researchUK India Education Research Initiative(UKIERI)for funding support.
文摘This review provides an insightful and comprehensive exploration of the emerging 2D material borophene,both pristine and modified,emphasizing its unique attributes and potential for sustainable applications.Borophene’s distinctive properties include its anisotropic crystal structures that contribute to its exceptional mechanical and electronic properties.The material exhibits superior electrical and thermal conductivity,surpassing many other 2D materials.Borophene’s unique atomic spin arrangements further diversify its potential application for magnetism.Surface and interface engineering,through doping,functionalization,and synthesis of hybridized and nanocomposite borophene-based systems,is crucial for tailoring borophene’s properties to specific applications.This review aims to address this knowledge gap through a comprehensive and critical analysis of different synthetic and functionalisation methods,to enhance surface reactivity by increasing active sites through doping and surface modifications.These approaches optimize diffusion pathways improving accessibility for catalytic reactions,and tailor the electronic density to tune the optical and electronic behavior.Key applications explored include energy systems(batteries,supercapacitors,and hydrogen storage),catalysis for hydrogen and oxygen evolution reactions,sensors,and optoelectronics for advanced photonic devices.The key to all these applications relies on strategies to introduce heteroatoms for tuning electronic and catalytic properties,employ chemical modifications to enhance stability and leverage borophene’s conductivity and reactivity for advanced photonics.Finally,the review addresses challenges and proposes solutions such as encapsulation,functionalization,and integration with composites to mitigate oxidation sensitivity and overcome scalability barriers,enabling sustainable,commercial-scale applications.
基金National Natural Science Foundation of China(Grant No.22005318,22379152)Western Young Scholars Foundations of Chinese Academy of Sciences+4 种基金Lanzhou Youth Science and Technology Talent Innovation Project(Grant No.2023-NQ-86,No.2023-QN-96)Lanzhou Chengguan District Science and Technology Plan Project(Grant No.2023-rc-4,2022-rc-4)Collaborative Innovation Alliance Fund for Young Science and Technology Worker(Grant No.HZJJ23-7)National Nature Science Foundations of Gansu Province(Grant No.21JR11RA020)Fundamental Research Funds for the Central Universities(Grant No.31920220073,31920230128)。
文摘Rechargeable aqueous zinc-ion batteries(AZIBs)exhibit appreciable potential in the domain of electrochemical energy storage.However,there are serious challenges for AZIBs,for instance zinc dendrite growth,hydrogen evolution reaction(HER),and corrosion side reactions.Herein,we propose a surface engineering modification strategy for coating the montmorillonite(MMT)layer onto the surface of the Zn anode to tackle these issues,thereby achieving high cycling stability for rechargeable AZIBs.The results reveal that the MMT layer on the surface of the Zn anode is able to provide ordered zincophilic channels for zinc ions migration,facilitating the reaction kinetics of zinc ions.Density functional theory(DFT)calculations and water contact angle(CA)tests prove that MMT@Zn anode exhibits superior adsorption capacity for Zn^(2+)and better hydrophobicity than the bare Zn anode,thereby achieving excellent cycling stability.Moreover,the MMT@Zn||MMT@Zn symmetric cell holds the stable cycling over 5600 h at 0.5 mA cm^(-2)and 0.125 m A h cm^(-2),even exceeding 1800 h long cycling under harsh conditions of 5 m A cm^(-2)and 1.25 m A h cm^(-2).The MMT@Zn||V_(2)O_(5)full cell reaches over 3000 cycles at 2 A g^(-1)with excellent rate capability.Therefore,this surface engineering modification strategy for enhancing the electrochemical performance of AZIBs represents a promising application.
基金supported by the Henan Province science and technology research project(Grant No.242102321031)National Natural Science Foundation of China(grant numbers 42207200).
文摘Near-surface geological defects pose a serious threat to human life and infrastructure.Hence,the exploration of geological hazards is essential.Currently,there are various geological hazard exploration methods;however,those require improvements in terms of economic feasibility,convenience,and lateral resolution.To address this,this study examined an extraction method to determine spatial autocorrelation velocity dispersion curves for application in near-surface exploration.
基金supported by the National Natural Science Foundation of China(22078132,22108103,and U22A20413)the Open Funding Project of the National Key Labora-tory of Biochemical Engineering(2021KF-02)+3 种基金China Postdoctoral Science Foundation(2021M691301)Jiangsu Key Research and Development Program(BE2022356)the Postdoctoral Fellowship Program of China Postdoctoral Science Foundation(CPSF)(GZ20230989)Jiangsu Agricultural Independent Innovation Fund Project(CX(21)3079).
文摘Expanding the specific surface area of substrates and carrying out precise surface engineering of imprinted nanocavities are crucial methods for enhancing the identification efficiency of molecularly imprinted polymers(MIPs).To implement this synergistic strategy,bioinspired surface engineering was used to incorporate dual covalent receptors via precise post-imprinting modifications(PIMs)onto mesoporous silica nanosheets.The prepared sorbents(denoted as‘‘D-PMIPs”)were utilized to improve the specific identification of adenosine 5-monophosphate(AMP).Significantly,the mesoporous silica nanosheets possess a high surface area of approximately 498.73 m^(2)·g^(-1),which facilitates the formation of abundant specific recognition sites in the D-PMIPs.The dual covalent receptors are valuable for estab-lishing the spatial orientation and arrangement of AMP through multiple cooperative interactions.PIMs enable precise site-specific functionalization within the imprinted cavities,leading to the tailor-made formation of complementary binding sites.The maximum number of high-affinity binding sites(Nmax)of the D-PMIPs is 39.99 lmol·g^(-1),which is significantly higher than that of imprinted sorbents with a sin-gle receptor(i.e.,S-BMIPs or S-PMIPs).The kinetic data of the D-PMIPs can be effectively described by a pseudo-second-order model,indicating that the main binding mechanism involves synergistic chemisorption from boronate affinity and the pyrimidine base.This study suggests that using dual cova-lent receptors and PIMs is a reliable approach for creating imprinted sorbents with high selectivity,allow-ing for the controlled engineering of imprinted sites.
基金supported by National Natural Science Foundation of China(No.52202366)Taishan Scholar Project of Shandong Province(tstp20240515,tsqn202312217)+1 种基金Natural Science Foundation of Shandong Province(China,No.2025HWYQ-050,ZR2021QE011,ZR2022QH072,ZR2021QE284)the King Abdullah University of Science and Technology,the Center of Excellence for Renewable Energy and Storage Technologies.
文摘For emerging renewable and sustainable energy technologies,single crystal materials have become key materials to enhance electrocatalytic performance because of their atomic-level ordered structures and tailorable surface and interfacial properties.Various single crystal types,including metals,semiconductors,ceramics,organics,and nanocrystals,exhibit superior catalytic selectivity and stability in reactions such as water splitting and carbon/nitrogen cycles,benefiting from high electrical conductivity,tunable energy bands,and active sites with high surface energy.Through surface modification,interfacial atomic doping,and heterostructure construction,the distribution of active sites,electronic structure,and mass transport can be precisely regulated,significantly optimizing the catalytic kinetics of single crystal materials.In situ characterizations elucidate catalytic mechanisms at the atomic scale,while emerging methods like AI-assisted synthesis and bio-template directed growth offer pathways to overcome bottlenecks in the precision and cost of single crystal preparation.In addressing stability challenges in complex environments,strategies such as organic-inorganic hybridization and gradient interface design effectively mitigate interfacial instability.Future research should focus on cross-scale structural regulation and multidisciplinary integration to facilitate the transition of single crystal electrocatalysts from fundamental research to industrial applications,enabling efficient energy conversion.
文摘The present work explored effects of laser surface melting on microstructure and surface topography evolution in AZ31B magnesium alloy.Thermokinetic effects experienced by the material during laser surface melting were simulated using a multiphysics finite element model.Microstructure and phase evolution were examined using scanning electron microscopy,X-ray diffraction,and electron back scatter diffraction.Surface topography was evaluated using white light interferometry.The interaction of surface melted samples with simulated body fluid was monitored by contact angle measurements and immersion studies up to 7 days.Laser surface melting led to formation of a refined microstructure with predominantly basal crystallographic texture.Concurrently,the amount ofβphase(Mg_(17)Al_(12))increased with an increase in the laser fluence.βphase preferentially decorated the cell boundaries.In terms of topography,the surface became progressively rougher with an increase in laser fluence.As a result,upon immersion in simulated body fluid,the laser surface melted samples showed an improved wettability,corrosion resistance,and precipitation of mineral having composition closer to the hydroxyapatite bone mineral compared to the untreated sample.
基金supported by the National Natural Science Foundation of China(Nos.51861165101,51822706,51777200)Beijing Natural Science Foundation(No.JQ19012)DNL Cooperation Fund,CAS(DNL201912)。
文摘Lithium-sulfur(Li-S)batteries have been recognized as one of the most promising candidates for nextgeneration portable electronic devices,owing to their extremely high energy density and low cost.However,the dissolution of lithium polysulfides(LiPSs)and consequent"shuttle effect"seriously hinder the practical deployment of Li-S batteries.Herein,multi-metal oxide nanorods named attapulgite are proposed as multifunctional ionic sieve to immobilize LiPSs and further promote the regulation of LiPSs.Attapulgite,consisting of Al,Mg,Fe,Si and O ions,possesses more polar sites to immobilize LiPSs in comparison with single metal oxides.In addition,the catalytic nature(Fe ions)of attapulgite avails the LiPSs conversion reaction,which is further confirmed by the linear sweep voltammetry and electrochemical impedance spectroscopy.Benefited from the synergistic effect of multi-metal oxide and conductive carbon,the Li-S battery with the modified separator delivers remarkable discharge capacities of 1059.4 mAh g-1 and 792.5 mAh g-1 for the first and 200th cycle at 0.5 C,respectively.The work presents an effective way to improve the electrochemical performance of Li-S batteries by employing attapulgite nanorods assisted separator surface engineering.
基金supported by the Natural Science Foundation of Shandong Province(ZR2019PB013)the Natural Science Foundation of Tianjin(19JCZDJC37700)the National Natural Science Foundation of China(21421001 and 21875118)。
文摘To date,much efforts have been devoted to the high-efficiency noble metal-free electrocatalysts for hydrogen-and oxygen-involving energy conversion reactions,due to their abundance,low cost and nultifunctionally.Surface/interface engineering is found to be effective in achieving novel physicochemical properties and synergistic effects in nanomaterials for electrocatalysis.Among various engineering strategies,heteroatom-doping has been regarded as a most promising method to improve the electrocatalytic performance via the regulation of electronic structure of catalysts,and numerous works were reported on the synthesis method and mechanism investigation of heteroatom-doping electrocatalysts,though the heteroatom-doping can only provide limited active sites.Engineering of other defects such as vacancies and edge sites and construction of heterostructure have shown to open up a potential avenue for the development of noble metal-free electrocatalysts.In addition,surface functionalization can attach various molecules onto the surface of materials to easily modify their physical or chemical properties,being as a promising complement or substitute for offering materials with catalytic properties.This paper gives the insights into the diverse strategies of surface/interface engineering of the highefficiency noble metal-free electrocatalysts for energy-related electrochemical reactions.The significant advances are summarized.The unique advantages and mechanisms for specific applications are highlighted.The current challenges and outlook of this growing field are also discussed.
基金financially supported by JSPS KAKENHI(JP18H02065)Photo-excitonic Project in Hokkaido University,National Natural Science Foundation of China(21633004,22002060,and 51872138)+4 种基金Natural Science Foundation of Jiangsu Province(BK20181380)Qing Lan Project,Six Talent Peaks Project in Jiangsu Province(XCL-029)Priority Academic Program Development of the Jiangsu Higher Education Institutions(PAPD)the support provided by the China Scholarships Council(202008320109)China Postdoctoral Science Foundation(2020M681564)。
文摘Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2)RR)is still challenging owing to the sluggish kinetics or unfavorable thermodynamics for basic chemical processes of CO_(2)RR,such as adsorption,activation,conversion and product desorption.To overcome these shortcomings,recent works have demonstrated that surface engineering of semiconductors,such as introducing surface vacancy,surface doping,and cocatalyst loading,serves as effective or promising strategies for improved photocatalytic CO_(2)RR with high activity and selectivity.The essential reason lies in the activation and reaction pathways can be optimized and regulated through the reconstruction of surface atomic and electronic structures.Herein,in this review,we focus on recent research advances about rational design of semiconductor surface for photocatalytic CO_(2)RR.The surface engineering strategies for improved CO_(2)adsorption,activation,and product selectivity will be reviewed.In addition,theoretical calculations along with in situ characterization techniques will be in the spotlight to clarify the kinetics and thermodynamics of the reaction process.The aim of this review is to provide deep understanding and rational guidance on the design of semiconductors for photocatalytic CO_(2)RR.
基金supported by the National Natural Science Foundation of China (51904216)the National Innovation and Entrepreneurship Training Program for College Students (202010497002, 202010497004)。
文摘The safety and cycle lifespan of zinc metal-based aqueous batteries are greatly restricted by zinc anode.The poor cycling performance of zinc metal anode is often considered to be impacted by the dendrite growth,surface passivation,zinc metal corrosion and hydrogen evolution reaction,while surface roughness is a matter that has often been ignored in past studies.Herein,a roughness gradient is constructed on the zinc anode surface by a simple grinding and pasting method.It has been found the modified zinc anodes with lower surface roughness exhibit the smaller zinc deposition overpotential and longer cycle life.Further,in situ optical microscopy photographs indicate that the zinc anode with an optimized roughness enables more uniform distribution of zinc precipitation and corrosion sites,which will facilitate a stable cycling performance of aqueous zinc ion batteries.The Zn anode dendrite-suppressing mechanism via surface roughness engineering was revealed through finite element computational simulation.These results emphasize the effectiveness of roughness engineering for tuning the surface physics of Zn anode and provide a facile strategy to develop better and safer aqueous zinc ion batteries.
基金financially supported via Australian Research Council(FT180100705)the support by the National Natural Science Foundation of China(22209103)+3 种基金the support from UTS Chancellor's Research Fellowshipsthe support from Open Project of State Key Laboratory of Advanced Special Steel,the Shanghai Key Laboratory of Advanced Ferrometallurgy,Shanghai University(SKLASS 2021-**)Joint International Laboratory on Environmental and Energy Frontier MaterialsInnovation Research Team of High-Level Local Universities in Shanghai。
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides a promising way to convert CO_(2)to chemicals.The multicarbon(C_(2+))products,especially ethylene,are of great interest due to their versatile industrial applications.However,selectively reducing CO_(2)to ethylene is still challenging as the additional energy required for the C–C coupling step results in large overpotential and many competing products.Nonetheless,mechanistic understanding of the key steps and preferred reaction pathways/conditions,as well as rational design of novel catalysts for ethylene production have been regarded as promising approaches to achieving the highly efficient and selective CO_(2)RR.In this review,we first illustrate the key steps for CO_(2)RR to ethylene(e.g.,CO_(2)adsorption/activation,formation of~*CO intermediate,C–C coupling step),offering mechanistic understanding of CO_(2)RR conversion to ethylene.Then the alternative reaction pathways and conditions for the formation of ethylene and competitive products(C_1 and other C_(2+)products)are investigated,guiding the further design and development of preferred conditions for ethylene generation.Engineering strategies of Cu-based catalysts for CO_(2)RR-ethylene are further summarized,and the correlations of reaction mechanism/pathways,engineering strategies and selectivity are elaborated.Finally,major challenges and perspectives in the research area of CO_(2)RR are proposed for future development and practical applications.
基金National Nature Science Foundation of China,Grant/Award Number:21908124。
文摘The sluggish kinetics of multiphase sulfur conversion with homogeneous and heterogeneous electrochemical processes,causing the“shuttle effect”of soluble polysulfide species(PSs),is the challenges in terms of lithium-sulfur batteries(LSBs).In this paper,a Mn_(3)O_(4-x) catalyst,which has much higher activity for heterogeneous reactions than for homogeneous reactions(namely,preferentialactivity catalysts),is designed by surface engineering with rational oxygen vacancies.Due to the rational design of the electronic structure,the Mn_(3)O_(4-x) catalyst prefers to accelerate the conversion of Li2S4 into Li_(2)S_(2)/Li_(2)S and optimize Li_(2)S deposition,reducing the accumulation of PSs and thus suppressing the“shuttle effect.”Both density functional theory calculations and in situ X-ray diffraction measurements are used to probe the catalytic mechanism and identify the reaction intermediates of MnS and Li_(y)Mn_(z)O_(4-x) for fundamental understanding.The cell with Mn_(3)O_(4-x) delivers an ultralow attenuation rate of 0.028% per cycle over 2000 cycles at 2.5 C.Even with sulfur loadings of 4.93 and 7.10mg cm^(-2) in a lean electrolyte(8.4μL mg s^(-1)),the cell still shows an initial areal capacity of 7.3mAh cm^(-2).This study may provide a new way to develop preferential-activity heterogeneous-reaction catalysts to suppress the“shuttle effect”of the soluble PSs generated during the redox process of LSBs.
基金the National Natural Science Foundation of China(Nos.52001222,52075361,and U21A20174)the Key National Scientific and Technological Cooperation Projects of Shanxi Province(No.202104041101008)+5 种基金the Major Science and Technology Project of Shanxi Province(No.20201102003)the Key Research and Development Projects in Shanxi Province(No.201903D421030)the Natural Science Foundation of Shanxi Province(Nos.201701D221073 and 201901D111107)the Program for the Innovative Talents of Higher Education Institutions of Shanxi(PTIT)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(STIP,No.2019L025)the Special Foundation for Youth San Jin scholars。
文摘Amorphous metal-based catalysts(AMCs)have sparked intense research interests in the field of electrocatalysis elicited by their hallmark features such as unlimited volume and morphology,manipulated electronic structures,enriched defects,and unsaturated surface atom coordination.Nevertheless,the manipulation of the amorphous phase in metal-based catalysts is so far impractical,and thus their electrocatalytic mechanism yet remains ambiguous.In this review,the latest advances in AMCs are systematically reviewed,covering amorphous-phase engineering strategy,structure manipulation,and amorphization of various material categories for electrocatalysis.Specifically,a series of applications of AMCs in electrocatalysis for the oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),and oxygen evolution reaction(OER)are summarized based on the classification criteria of substances.Finally,we put forward current challenges that have not yet been clarified in the field of AMCs,and propose possible solutions,particularly from the perspective of the evolution of electron microscopy.It is expected to promote the understanding of the amorphization-catalysis relationship and provide a guideline for designing high-performance electrocatalysts.
基金This research was funded by Key Scientific Research Projects of General Universities in Guangdong Province,China(No.2021KCXTD086)Guangzhou Basic and Applied Basic Research Project in China(No.202102020134)Youth Innovation Talents Project of Guangdong Universities(natural science)in China(No.2019KQNCX098).
文摘Opportunities coexist with challenges for the development of carbon-based cathodes with a high energy density applied for zinc ion hybrid capacitors(ZIHCs).In the present study,a facile and effective surface engineering approach is demonstrated to greatly improve the energy storage ability of commercial carbon paper(CP)in ZIHC.Benefiting from the introduced oxygen functional groups,larger surface area and improved surface wettability upon air calcination,the assembled aqueous ZIHC with the functionalized carbon paper(FCP)exhibits a much higher areal capacity of 0.22 mAh/cm^(2)at 1 mA/cm^(2),outperforming the counterpart with blank CP by over 5000 times.More importantly,a superior energy density and power density of 130.8μWh/cm^(2)and 7460.5μW/cm^(2),are respectively delivered.Furthermore,more than 90%of the initial capacity is retained over 10000 cycles.This surface engineering strategy to improve the energy storage capability is potentially applicable to developing a wide range of high-energy carbon electrode materials.
基金National Natural Science Foundation of China(No.52173264).
文摘Surface structural engineering is desirable in modifying the surface performance of carbonyl iron powder(CIP)to enhance microwave absorption(MA)and anti-oxidation performance.Herein,the surface shape-dependent CIP absorbers are designed via surface coating with zinc oxide(ZnO)nanoparticles and then a thermal annealing treatment.The morphology of ZnO nanoparticles which can be easily regulated by controlling the annealing temperature ultimately affects the MA performance of CIP coating with ZnO nanoparticles(CIP@ZnO).The core-shell CIP@ZnO particles with cubic cone ZnO nanoparticles exhibit ex-cellent MA performance and thermal stability in comparison to the original CIP.Specifically,the CIP@ZnO annealed at 350 ℃(CIP@ZnO-350)samples which have the cubic cone ZnO nanoparticles exhibit a min-imum reflection loss(RLmin)of-55.35 dB at a thickness of 2.1 mm and a maximum effective absorp-tion bandwidth(EAB)of 7.09 GHz at a thickness of 2.0 mm.In addition,the antioxidant property of the CIP@ZnO composite particles is abruptly enhanced,which breaks the restriction of the application of CIP at high temperatures.The superior MA performance of CIP@ZnO particles with cubic cone ZnO nanoparti-cles comes from the enhancement in surface shape-dependent multiple microwave scattering,interfacial polarization,and electromagnetic-dielectric synergism between ZnO and CIP.
基金This work was supported by the NSFC(21501096,22075223)Natural Science Foundation of Jiangsu(BK20150086,BK20201120)+1 种基金the Foundation of the Jiangsu Education Committee(15KJB150020)the Six Talent Peaks Project in Jiangsu Province(JY-087)and the Innovation Project of Jiangsu Province.
文摘Although molybdenum disulfide (MoS_(2))-based materials are generally known as active electrocatalysts for the hydrogen evolution reaction (HER), the inert performance for the oxygen evolution reaction (OER) seriously limits their wide applications in alkaline electrolyzers due to there exists too strong metal-sulfur (M−S) bond in MoS_(2). Herein, by means of surface reorganization engineering of bimetal Al, Co-doped MoS_(2) (devoted as AlCo_(3)-MoS_(2)) through in situ substituting partial oxidation, we successfully significantly activate the OER activity of MoS_(2), which affords a considerably low overpotential of 323 mV at −30 mA cm^(−2), far lower than those of MoS_(2), Al-MoS_(2) and Co-MoS_(2) catalysts. Essentially, the AlCo_(3)-MoS_(2) substrate produces lots of M−O (M=Al, Co and Mo) species with oxygen vacancies, which trigger the surface self-reconstruction of pre-catalysts and simultaneously boost the electrocatalytic OER activity. Moreover, benefiting from the moderate M−O species formed on the surface, the redistribution of surface electron states is induced, thus optimizing the adsorption of OH* and OOH* intermediates on metal oxyhydroxides and awakening the OER activity of MoS_(2).
基金National Natural Science Foundation of China (22179008, 21875022)Yibin ‘Jie Bang Gua Shuai’ (2022JB004)+3 种基金support from the Beijing Nova Program (20230484241)support from the Postdoctoral Fellowship Program of CPSF (GZB20230931)Special Support of the Chongqing Postdoctoral Research Project (2023CQBSHTB2041)Initial Energy Science & Technology Co., Ltd (IEST)。
文摘Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes often declines because of capacity fading during cycling. This decline is primarily attributed to anisotropic lattice strain and oxygen release from cathode surfaces. Given notable structural transformations, complex redox reactions, and detrimental interface side reactions in LRMOs, the development of a single modification approach that addresses bulk and surface issues is challenging. Therefore,this study introduces a surface double-coupling engineering strategy that mitigates bulk strain and reduces surface side reactions. The internal spinel-like phase coating layer, featuring threedimensional(3D) lithium-ion diffusion channels, effectively blocks oxygen release from the cathode surface and mitigates lattice strain. In addition, the external Li_(3)PO_(4) coating layer, noted for its superior corrosion resistance, enhances the interfacial lithium transport and inhibits the dissolution of surface transition metals. Notably, the spinel phase, as excellent interlayer, securely anchors Li_(3)PO_(4) to the bulk lattice and suppresses oxygen release from lattices. Consequently, these modifications considerably boost structural stability and durability, achieving an impressive capacity retention of 83.4% and a minimal voltage decay of 1.49 m V per cycle after 150 cycles at 1 C. These findings provide crucial mechanistic insights into the role of surface modifications and guide the development of high-capacity cathodes with enhanced cyclability.
基金This project is supported by General Electric Corporate ResearchDevelopment and National Advanced Technology Project of China (No.863-511-942-018).
文摘A new method of extraction of blend surface feature is presented. It contains two steps: segmentation and recovery of parametric representation of the blend. The segmentation separates the points in the blend region from the rest of the input point cloud with the processes of sampling point data, estimation of local surface curvature properties and comparison of maximum curvature values. The recovery of parametric representation generates a set of profile curves by marching throughout the blend and fitting cylinders. Compared with the existing approaches of blend surface feature extraction, the proposed method reduces the requirement of user interaction and is capable of extracting blend surface with either constant radius or variable radius. Application examples are presented to verify the proposed method.
