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
Surface/interface engineering plays an important role in improving the performance and economizing the cost and usage of electrocatalysts.In recent years,substantial progress has been achieved in designing and develop...Surface/interface engineering plays an important role in improving the performance and economizing the cost and usage of electrocatalysts.In recent years,substantial progress has been achieved in designing and developing highly active electrocatalysts with the deepening understanding of surface and interface enhanced mechanism.In this review,recent development about optimizing the surface and interfacial structure in promoting the electrocatalytic activity of noble-metals and transition metal compounds is presented and the chemical enhancements are also described in detail.The relationship between the surface/interface structures(both atomic and electronic configuration)and the electrochemical behaviors has been discussed.Finally,personal perspectives have been proposed,highlighting the challenges and opportunities for future development in tuning the surface/interface active sites of electrocatalysts.We believe that this timely review will be beneficial to the construction of highly active and durable electrode materials through optimizing surface atomic arrangement and interfacial interaction,which can largely promote the development of next-generation clean energy conversion technologies.展开更多
Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggis...Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggish CO_(2)reduction reaction(CO_(2)RR)/CO_(2)evolution reaction(CO_(2)ER)kinetics remains a huge challenge.In this work,an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation,which significantly improves the electrocatalytic activity for both CO_(2)RR and CO_(2)ER.Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface,which leads to optimized binding affinity towards reactants and preferred Li_(2)CO_(3)decomposition behavior,enabling excellent catalytic activity during CO_(2)redox.Benefiting from the enhanced charge transfer ability,the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%.This work provides an attractive strategy to construct robust catalysts by interface engineering,which could inspire further design of superior bidirectional catalysts for Li-CO_(2)batteries.展开更多
The high energy density of green synthetic liquid chemicals and fuels makes them ideal for sustainable energy storage and transportation applications.Electroreduction of carbon dioxide(CO_(2))directly into such high v...The high energy density of green synthetic liquid chemicals and fuels makes them ideal for sustainable energy storage and transportation applications.Electroreduction of carbon dioxide(CO_(2))directly into such high value-added chemicals can help us achieve a renewable C cycle.Such electrochemical reduction typically suffers from low faradaic efficiencies(FEs)and generates a mixture of products due to the complexity of controlling the reaction selectivity.This perspective summarizes recent advances in the mechanistic understanding of CO_(2) reduction reaction pathways toward liquid products and the state-of-the-art catalytic materials for conversion of CO_(2) to liquid C1(e.g.,formic acid,methanol)and C2+products(e.g.,acetic acid,ethanol,n-propanol).Many liquid fuels are being produced with FEs between 80%and 100%.We discuss the use of structure-binding energy relationships,computational screening,and machine learning to identify promising candidates for experimental validation.Finally,we classify strategies for controlling catalyst selectivity and summarize breakthroughs,prospects,and challenges in electrocatalytic CO_(2) reduction to guide future developments.展开更多
Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits ...Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water splitting.Here,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of Ru.Benefiting from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performances.The synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water electrolysis.Moreover,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline media.When building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity.展开更多
Atomically precise metal nanocluster and ultrasmall nanoparticle catalysts have garnered significant interest in electrocatalysis applications due to their unique geometric and electronic structures.As an intermediate...Atomically precise metal nanocluster and ultrasmall nanoparticle catalysts have garnered significant interest in electrocatalysis applications due to their unique geometric and electronic structures.As an intermediate state between single-atom catalysts(SACs)and nanoparticles in size,nanoclusters with specific low nuclearity provide designated metallic states with multiple atoms or surface sites for the adsorption and transformation of reactants/intermediates.The unique catalytic properties of nanoclusters offer a novel platform for designing effective and efficient electrocatalysts,potentially surpassing the SACs in certain catalytic reactions.This review summarizes and discusses the latest progress of nanoclusters and ultrasmall nanoparticles for various electrocatalysis applications,including oxygen reduction reaction(ORR),oxygen evolution reaction(OER),CO_(2) reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR),hydrogen evolution reaction(HER),various chemicals oxidation reaction(COR),etc.Specifically,this review highlights surface/interface chemical modification strategies and structure-properties relationships,drawing from the atomic-level insights to determine electrocatalytic performance.Lastly,we present the challenges and opportunities associated with nanocluster or ultrasmall nanoparticle electrocatalysts.展开更多
As a mathematical analysis method,fractal analysis can be used to quantitatively describe irregular shapes with self-similar or self-affine properties.Fractal analysis has been used to characterize the shapes of metal...As a mathematical analysis method,fractal analysis can be used to quantitatively describe irregular shapes with self-similar or self-affine properties.Fractal analysis has been used to characterize the shapes of metal materials at various scales and dimensions.Conventional methods make it difficult to quantitatively describe the relationship between the regular characteristics and properties of metal material surfaces and interfaces.However,fractal analysis can be used to quantitatively describe the shape characteristics of metal materials and to establish the quantitative relationships between the shape characteristics and various properties of metal materials.From the perspective of two-dimensional planes and three-dimensional curved surfaces,this paper reviews the current research status of the fractal analysis of metal precipitate interfaces,metal grain boundary interfaces,metal-deposited film surfaces,metal fracture surfaces,metal machined surfaces,and metal wear surfaces.The relationship between the fractal dimensions and properties of metal material surfaces and interfaces is summarized.Starting from three perspectives of fractal analysis,namely,research scope,image acquisition methods,and calculation methods,this paper identifies the direction of research on fractal analysis of metal material surfaces and interfaces that need to be developed.It is believed that revealing the deep influence mechanism between the fractal dimensions and properties of metal material surfaces and interfaces will be the key research direction of the fractal analysis of metal materials in the future.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
Micron-sized silicon anodes offer significant industrial advantages over nanoscale counterparts due to their cost-effectiveness and scalability.However,their practical applications are significantly hindered by severe...Micron-sized silicon anodes offer significant industrial advantages over nanoscale counterparts due to their cost-effectiveness and scalability.However,their practical applications are significantly hindered by severe stress-induced fragmentation,leading to rapid capacity decay.Addressing this challenge,we introduce a novel dual-conformal encapsulated micron-sized porous Si(μm-pSi)anode by utilizingμm-Si recycled from the photovoltaic industry as the Si precursor.This encapsulation design of the internal conformal SiO_(x)/C layer and external Ti_(3)C_(2)Tx MXene layer forms intergranular and intragranular protective skins onμm-pSi,ensuring simultaneous mechanical and electrochemical stability for efficient Li+storage.As a result,the fabricated WpSi@SiO_(x)/C@MXene anode demonstrates an exceptional cycling performance,delivering 535.1 mA h g^(−1)after 1500 cycles at 5 A g^(−1)with a minimal capacity decay of 0.003%per cycle.Chemo-mechanical modeling and SEI analysis reveal that the dual-conformal coating achieves exceptional mechanical and electrochemical stability through robust mechanical confinement and ultra-fast Li+diffusion kinetics during lithiation,coupled with a Li_(2)CO_(3)/LiF-rich hybrid SEI that facilitates Li+transport,collectively enabling rate-insensitive stress evolution,long-term structural durability,and stable cycling under high-rate conditions.This work provides a compelling design strategy for leveraging sustainableμm-Si to achieve high-rate and long-life lithium-ion batteries.展开更多
Surface passivation with organic ammoniums improves perovskite solar cell performance by forming 2D/quasi-2D structures or adsorbing onto surfaces.However,complexity from mixed phases can trigger phase transitions,com...Surface passivation with organic ammoniums improves perovskite solar cell performance by forming 2D/quasi-2D structures or adsorbing onto surfaces.However,complexity from mixed phases can trigger phase transitions,compromising stability.The control of surface dimensionality after organic ammonium passivation presents significant importance to device stability.In this study,we developed a poly-fluorination strategy for surface treatment in perovskite solar cells,which enabled a high and durable interfacial phase purity after surface passivation.The locked surface dimensionality of perovskite was achieved through robust interaction between the poly-fluorinated ammoniums and the perovskite surface,along with the steric hindrance imparted by fluorine atoms,reducing its reactivity and penetration capabilities.The high hydrophobicity of the poly-fluorinated surface also aids in moisture resistance of the perovskite layer.The champion device achieved a power conversion efficiency(PCE)of 25.2% with certified 24.6%,with 90% of its initial PCE retained after approximately 1200 h under continuous 1-sun illumination,and over 14,400 h storage stability and superior stability under high-temperature operation.展开更多
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
In the past decade,dry reforming of methane(DRM)has garnered increasing interest as it converts CH_(4)and CO_(2),two typical greenhouse gases,into synthesis gas(H_(2)and CO)for the production of high-value-added chemi...In the past decade,dry reforming of methane(DRM)has garnered increasing interest as it converts CH_(4)and CO_(2),two typical greenhouse gases,into synthesis gas(H_(2)and CO)for the production of high-value-added chemicals and fuels.Nickel-based DRM catalysts,renowned for their high activity and low cost,however,encounter challenges such as severe deactivation from sintering and carbon deposition.Herein,a surrounded NiO@NiAlO precursor derived from Ni(OH)_(2)nanosheets was modified at both the core and shell interfaces with MgO via wet impregnation.The obtained 0.8MgO^(WI)/Ni@NiAlO catalyst achieved a high CH_(4)reaction rate of~177 mmol gNi^(-1)min^(-1)and remained stable for 50 h at 600℃without coke formation.In sharp contrast,other Mg-doped catalysts(MgO modified the core or shell interfaces)and the catalyst without Mg-doping deactivated within 10 h due to coking or Ni particle sintering.The Ni/MgNiO_(2)interfaces and abundant oxygen vacancies(O_(v))generated by Mg-doping contributed to the outstanding resistance to sintering&coking as well as the superior activity and stability of the 0.8MgO^(WI)/Ni@NiAlO catalyst.In-situ investigation further unveiled the reaction mechanism:the activation of CO_(2)via adsorption on O_(v)generates active oxygen species(O^(*)),which reacts with CH_(x)^(*)intermediates formed by the dissociation of CH_(4)on Ni sites,yielding CO and H_(2).This work not only fabricates coke-free and high-stability Ni-based DRM catalysts via interface engineering but also provides insights and a new strategy for the design of high-efficiency and stable catalysts for DRM.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
Understanding frictional anisotropy,which refers to the variation in frictional resistance based on the shear direction,is crucial for optimizing the friction angle between a bio-inspired structure and the surrounding...Understanding frictional anisotropy,which refers to the variation in frictional resistance based on the shear direction,is crucial for optimizing the friction angle between a bio-inspired structure and the surrounding soil.Previous studies focused on estimating the interface frictional anisotropy mobilized by snakeskin-inspired textured surfaces and sand under monotonic shear loading conditions.However,there is a need to estimate interface frictional anisotropy under repetitive shear loads.In this study,a series of repetitive direct shear(DS)tests are performed with snakeskin-inspired textured surfaces under a constant vertical stress and two shear directions(cranial first half→caudal second half or caudal first half→cranial second half).The results show that(1)mobilized shear stress increases with the number of shearing cycles,(2)cranial shearing(shearing against the scales)consistently produces a higher shear resistance and less contractive behavior than caudal shearing(shearing along the scales),and(3)a higher scale height or smaller scale length of the surface yields a higher interface friction angle across all shearing cycles.Further analysis reveals that the gap between the cranial and caudal shear zones of the interface friction angle as a function of L/H(i.e.the ratio of scale length L to scale height H)continues to decrease as the number of shearing cycles approaches asymptotic values.The directional frictional resistance(DFR)decreases as the number of shearing cycles increases.Furthermore,the discussion covers the impact of initial relative density,vertical stress,and the number of shearing cycles on interface frictional anisotropy.展开更多
Coupling with high-voltage oxide cathode is the key to achieve high-energy density sulfide-based all-solid-state lithium batteries.However,the complex interfacial issues including the space charge layer effect and und...Coupling with high-voltage oxide cathode is the key to achieve high-energy density sulfide-based all-solid-state lithium batteries.However,the complex interfacial issues including the space charge layer effect and undesirable side reaction between sulfide solid-state electrolytes and oxide cathode materials are the main constraints on the development of high-performance allsolid-state lithium batteries,which lead to the continuous decay of electrochemical performance.Herein,different from the complicated coating procedure,a LiPO_(2)F_(2)additive engineering was proposed to achieve high-performance all-solid-state lithium batteries.With the introduction of LiPO_(2)F_(2)additive,a protective cathode-electrolyte interphase consisting of LiPxOyFz,LiF,and Li_(3)PO_(4)could be in situ formed to improve the interfacial stability between LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)and Li_(5.5)PS_(4.5)Cl_(1.5)(LPSC).Benefiting from this,the NCM811/LPSC/Li all-solid-state lithium battery exhibited impressive cyclic stability with a capacity retention of 85.5%after 600 cycles(at 0.5 C).Diverse and comprehensive characterization,combined with finite element simulation and density functional theory calculation fully demonstrated the effective component,interfacial stabilization function and enhanced kinetic of LiPO_(2)F_(2)-derived cathode-electrolyte interphase.This work provides not only a feasible and effective method to stabilize the cathodic interface but also worthy insight into interfacial design for high-performance all-solid-state lithium batteries.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
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
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
Organic-inorganic hybrid metal halide perovskite solar cells(PSCs)have attracted much attention due to their high photoelectric conversion efficiency(PCE)and low cost.The certificated PCE of small active area(below 0....Organic-inorganic hybrid metal halide perovskite solar cells(PSCs)have attracted much attention due to their high photoelectric conversion efficiency(PCE)and low cost.The certificated PCE of small active area(below 0.1 cm^(2))device has reached 26.7%[1].However,when considering the scaled-up commercialization of PSCs,an obvious efficiency drop exists for the translation to large-area perovskite submodules(PSMs)with areas more than 200 cm^(2),thus limiting the practical commercialization[2].The major PCE gap between small area cells and large area modules arises the drop of open-circuit voltage(VOC)and fill factor(FF).Formamidinium lead iodide(FAPbI_(3))is now the mostly widely used and highly efficient perovskite composition.However,the photo-active black α-FAPbI_(3) phase will spontaneously transform into photo-inactive yellowδ-FAPbI_(3) phase at room temperature[3].展开更多
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supported financially by the Joint Funds of National Natural Science Foundation of China and Guangdong Province(No.U1601216)the National Natural Science Foundation of China(Nos.51602216 and 51472178)+1 种基金Young Elite Scientists Sponsorship Program by CAST(No.2018QNRC001)Tianjin Natural Science Foundation(No.17JCQNJC02100).
文摘Surface/interface engineering plays an important role in improving the performance and economizing the cost and usage of electrocatalysts.In recent years,substantial progress has been achieved in designing and developing highly active electrocatalysts with the deepening understanding of surface and interface enhanced mechanism.In this review,recent development about optimizing the surface and interfacial structure in promoting the electrocatalytic activity of noble-metals and transition metal compounds is presented and the chemical enhancements are also described in detail.The relationship between the surface/interface structures(both atomic and electronic configuration)and the electrochemical behaviors has been discussed.Finally,personal perspectives have been proposed,highlighting the challenges and opportunities for future development in tuning the surface/interface active sites of electrocatalysts.We believe that this timely review will be beneficial to the construction of highly active and durable electrode materials through optimizing surface atomic arrangement and interfacial interaction,which can largely promote the development of next-generation clean energy conversion technologies.
基金supported by the National Key Research and Development Program of China(2019YFA0705700)Guangdong Innovative and Entrepreneurial Research Team Program(2021ZT09L197)+2 种基金Shenzhen Science and Technology Program(KQTD20210811090112002)Interdisciplinary Research and Innovation Fund of Tsinghua Shenzhen International Graduate School,National Natural Science Foundation of China(No.52373233)the SIAT International Joint Lab Project(No.E3G113).
文摘Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggish CO_(2)reduction reaction(CO_(2)RR)/CO_(2)evolution reaction(CO_(2)ER)kinetics remains a huge challenge.In this work,an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation,which significantly improves the electrocatalytic activity for both CO_(2)RR and CO_(2)ER.Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface,which leads to optimized binding affinity towards reactants and preferred Li_(2)CO_(3)decomposition behavior,enabling excellent catalytic activity during CO_(2)redox.Benefiting from the enhanced charge transfer ability,the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%.This work provides an attractive strategy to construct robust catalysts by interface engineering,which could inspire further design of superior bidirectional catalysts for Li-CO_(2)batteries.
基金supported by the Joint Funds of the National Natural Science Foundation of China(U24B20201)National Natural Science Foundation of China(22372007 and 21972010)+1 种基金the Fundamental Research Funds for the Central Universities(JD2427)the SRC Center for Electron Transfer(2021R1A5A1030054)funded by NRF Korea and AI Graduate School Program(RS-2021-II211343).
文摘The high energy density of green synthetic liquid chemicals and fuels makes them ideal for sustainable energy storage and transportation applications.Electroreduction of carbon dioxide(CO_(2))directly into such high value-added chemicals can help us achieve a renewable C cycle.Such electrochemical reduction typically suffers from low faradaic efficiencies(FEs)and generates a mixture of products due to the complexity of controlling the reaction selectivity.This perspective summarizes recent advances in the mechanistic understanding of CO_(2) reduction reaction pathways toward liquid products and the state-of-the-art catalytic materials for conversion of CO_(2) to liquid C1(e.g.,formic acid,methanol)and C2+products(e.g.,acetic acid,ethanol,n-propanol).Many liquid fuels are being produced with FEs between 80%and 100%.We discuss the use of structure-binding energy relationships,computational screening,and machine learning to identify promising candidates for experimental validation.Finally,we classify strategies for controlling catalyst selectivity and summarize breakthroughs,prospects,and challenges in electrocatalytic CO_(2) reduction to guide future developments.
基金sponsored by the National Natural Science Foundation of China(51772162,52072197)the China Postdoctoral Science Foundation(2023M732132)+4 种基金Youth Innovation Team Development Program of Shandong Higher Education Institutions(2022KJ155)Outstanding Youth Foundation of Shandong Province,China(ZR2019JQ14)Taishan Scholar Young Talent Program(tsqn201909114)Major Scientific and Technological Innovation Project(2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant(ZR2020ZD09).
文摘Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water splitting.Here,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of Ru.Benefiting from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performances.The synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water electrolysis.Moreover,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline media.When building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity.
基金financially supported by the National Natural Science Foundation of China(22208331)the Natural Sciences and Engineering Research Council of Canada(NSERC)+2 种基金the Fonds de Recherche du Québec-Nature et Technologies(FRQNT)McGill University,Institut National de la Recherche Scientifique(INRS)andÉcole de Technologie Supérieure(ÉTS).
文摘Atomically precise metal nanocluster and ultrasmall nanoparticle catalysts have garnered significant interest in electrocatalysis applications due to their unique geometric and electronic structures.As an intermediate state between single-atom catalysts(SACs)and nanoparticles in size,nanoclusters with specific low nuclearity provide designated metallic states with multiple atoms or surface sites for the adsorption and transformation of reactants/intermediates.The unique catalytic properties of nanoclusters offer a novel platform for designing effective and efficient electrocatalysts,potentially surpassing the SACs in certain catalytic reactions.This review summarizes and discusses the latest progress of nanoclusters and ultrasmall nanoparticles for various electrocatalysis applications,including oxygen reduction reaction(ORR),oxygen evolution reaction(OER),CO_(2) reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR),hydrogen evolution reaction(HER),various chemicals oxidation reaction(COR),etc.Specifically,this review highlights surface/interface chemical modification strategies and structure-properties relationships,drawing from the atomic-level insights to determine electrocatalytic performance.Lastly,we present the challenges and opportunities associated with nanocluster or ultrasmall nanoparticle electrocatalysts.
基金financially supported by the National Key R&D Program of China(No.2022YFE0121300)the National Natural Science Foundation of China(No.52374376)the Introduction Plan for High-end Foreign Experts(No.G2023105001L)。
文摘As a mathematical analysis method,fractal analysis can be used to quantitatively describe irregular shapes with self-similar or self-affine properties.Fractal analysis has been used to characterize the shapes of metal materials at various scales and dimensions.Conventional methods make it difficult to quantitatively describe the relationship between the regular characteristics and properties of metal material surfaces and interfaces.However,fractal analysis can be used to quantitatively describe the shape characteristics of metal materials and to establish the quantitative relationships between the shape characteristics and various properties of metal materials.From the perspective of two-dimensional planes and three-dimensional curved surfaces,this paper reviews the current research status of the fractal analysis of metal precipitate interfaces,metal grain boundary interfaces,metal-deposited film surfaces,metal fracture surfaces,metal machined surfaces,and metal wear surfaces.The relationship between the fractal dimensions and properties of metal material surfaces and interfaces is summarized.Starting from three perspectives of fractal analysis,namely,research scope,image acquisition methods,and calculation methods,this paper identifies the direction of research on fractal analysis of metal material surfaces and interfaces that need to be developed.It is believed that revealing the deep influence mechanism between the fractal dimensions and properties of metal material surfaces and interfaces will be the key research direction of the fractal analysis of metal materials in the future.
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.
基金the financial support from the Natural Science Foundation of Shanghai(23ZR1423800)Open Research Fund of Shanghai Key Laboratory of Green Chemistry and Chemical Processes(East China Normal University,202503)+1 种基金State Key Laboratory of Advanced Fiber Materials(Donghua University,KF2406)Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University。
文摘Micron-sized silicon anodes offer significant industrial advantages over nanoscale counterparts due to their cost-effectiveness and scalability.However,their practical applications are significantly hindered by severe stress-induced fragmentation,leading to rapid capacity decay.Addressing this challenge,we introduce a novel dual-conformal encapsulated micron-sized porous Si(μm-pSi)anode by utilizingμm-Si recycled from the photovoltaic industry as the Si precursor.This encapsulation design of the internal conformal SiO_(x)/C layer and external Ti_(3)C_(2)Tx MXene layer forms intergranular and intragranular protective skins onμm-pSi,ensuring simultaneous mechanical and electrochemical stability for efficient Li+storage.As a result,the fabricated WpSi@SiO_(x)/C@MXene anode demonstrates an exceptional cycling performance,delivering 535.1 mA h g^(−1)after 1500 cycles at 5 A g^(−1)with a minimal capacity decay of 0.003%per cycle.Chemo-mechanical modeling and SEI analysis reveal that the dual-conformal coating achieves exceptional mechanical and electrochemical stability through robust mechanical confinement and ultra-fast Li+diffusion kinetics during lithiation,coupled with a Li_(2)CO_(3)/LiF-rich hybrid SEI that facilitates Li+transport,collectively enabling rate-insensitive stress evolution,long-term structural durability,and stable cycling under high-rate conditions.This work provides a compelling design strategy for leveraging sustainableμm-Si to achieve high-rate and long-life lithium-ion batteries.
基金grants(grant numbers LR24F040001,LD24E020001 and LD22E020002)from the Natural Science Foundation of Zhejiang Province of Chinathe National Natural Science Foundation of China(grant number 62274146)+1 种基金the support of Key R&D Program of Zhejiang(2024SSYS0061)supported by the Fundamental Research Funds for the Central Universities(226-2022-00200).
文摘Surface passivation with organic ammoniums improves perovskite solar cell performance by forming 2D/quasi-2D structures or adsorbing onto surfaces.However,complexity from mixed phases can trigger phase transitions,compromising stability.The control of surface dimensionality after organic ammonium passivation presents significant importance to device stability.In this study,we developed a poly-fluorination strategy for surface treatment in perovskite solar cells,which enabled a high and durable interfacial phase purity after surface passivation.The locked surface dimensionality of perovskite was achieved through robust interaction between the poly-fluorinated ammoniums and the perovskite surface,along with the steric hindrance imparted by fluorine atoms,reducing its reactivity and penetration capabilities.The high hydrophobicity of the poly-fluorinated surface also aids in moisture resistance of the perovskite layer.The champion device achieved a power conversion efficiency(PCE)of 25.2% with certified 24.6%,with 90% of its initial PCE retained after approximately 1200 h under continuous 1-sun illumination,and over 14,400 h storage stability and superior stability under high-temperature operation.
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.
文摘In the past decade,dry reforming of methane(DRM)has garnered increasing interest as it converts CH_(4)and CO_(2),two typical greenhouse gases,into synthesis gas(H_(2)and CO)for the production of high-value-added chemicals and fuels.Nickel-based DRM catalysts,renowned for their high activity and low cost,however,encounter challenges such as severe deactivation from sintering and carbon deposition.Herein,a surrounded NiO@NiAlO precursor derived from Ni(OH)_(2)nanosheets was modified at both the core and shell interfaces with MgO via wet impregnation.The obtained 0.8MgO^(WI)/Ni@NiAlO catalyst achieved a high CH_(4)reaction rate of~177 mmol gNi^(-1)min^(-1)and remained stable for 50 h at 600℃without coke formation.In sharp contrast,other Mg-doped catalysts(MgO modified the core or shell interfaces)and the catalyst without Mg-doping deactivated within 10 h due to coking or Ni particle sintering.The Ni/MgNiO_(2)interfaces and abundant oxygen vacancies(O_(v))generated by Mg-doping contributed to the outstanding resistance to sintering&coking as well as the superior activity and stability of the 0.8MgO^(WI)/Ni@NiAlO catalyst.In-situ investigation further unveiled the reaction mechanism:the activation of CO_(2)via adsorption on O_(v)generates active oxygen species(O^(*)),which reacts with CH_(x)^(*)intermediates formed by the dissociation of CH_(4)on Ni sites,yielding CO and H_(2).This work not only fabricates coke-free and high-stability Ni-based DRM catalysts via interface engineering but also provides insights and a new strategy for the design of high-efficiency and stable catalysts for DRM.
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the funding supported from the National Research Foundation of Korea(NRF)grant funded by the Korea Government MSIT(No.2021R1C1C1006003).
文摘Understanding frictional anisotropy,which refers to the variation in frictional resistance based on the shear direction,is crucial for optimizing the friction angle between a bio-inspired structure and the surrounding soil.Previous studies focused on estimating the interface frictional anisotropy mobilized by snakeskin-inspired textured surfaces and sand under monotonic shear loading conditions.However,there is a need to estimate interface frictional anisotropy under repetitive shear loads.In this study,a series of repetitive direct shear(DS)tests are performed with snakeskin-inspired textured surfaces under a constant vertical stress and two shear directions(cranial first half→caudal second half or caudal first half→cranial second half).The results show that(1)mobilized shear stress increases with the number of shearing cycles,(2)cranial shearing(shearing against the scales)consistently produces a higher shear resistance and less contractive behavior than caudal shearing(shearing along the scales),and(3)a higher scale height or smaller scale length of the surface yields a higher interface friction angle across all shearing cycles.Further analysis reveals that the gap between the cranial and caudal shear zones of the interface friction angle as a function of L/H(i.e.the ratio of scale length L to scale height H)continues to decrease as the number of shearing cycles approaches asymptotic values.The directional frictional resistance(DFR)decreases as the number of shearing cycles increases.Furthermore,the discussion covers the impact of initial relative density,vertical stress,and the number of shearing cycles on interface frictional anisotropy.
基金support by the Department of Science&Technology of Zhejiang Province under grant no.2024C01095Zhejiang Provincial Natural Science Foundation of China under grant nos.LD22E020006 and LBMHD24E020001the National Natural Science Foundation of China(NSFC)under grant nos.21972127,U20A20253,and 22279116.
文摘Coupling with high-voltage oxide cathode is the key to achieve high-energy density sulfide-based all-solid-state lithium batteries.However,the complex interfacial issues including the space charge layer effect and undesirable side reaction between sulfide solid-state electrolytes and oxide cathode materials are the main constraints on the development of high-performance allsolid-state lithium batteries,which lead to the continuous decay of electrochemical performance.Herein,different from the complicated coating procedure,a LiPO_(2)F_(2)additive engineering was proposed to achieve high-performance all-solid-state lithium batteries.With the introduction of LiPO_(2)F_(2)additive,a protective cathode-electrolyte interphase consisting of LiPxOyFz,LiF,and Li_(3)PO_(4)could be in situ formed to improve the interfacial stability between LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)and Li_(5.5)PS_(4.5)Cl_(1.5)(LPSC).Benefiting from this,the NCM811/LPSC/Li all-solid-state lithium battery exhibited impressive cyclic stability with a capacity retention of 85.5%after 600 cycles(at 0.5 C).Diverse and comprehensive characterization,combined with finite element simulation and density functional theory calculation fully demonstrated the effective component,interfacial stabilization function and enhanced kinetic of LiPO_(2)F_(2)-derived cathode-electrolyte interphase.This work provides not only a feasible and effective method to stabilize the cathodic interface but also worthy insight into interfacial design for high-performance all-solid-state lithium batteries.
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 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 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support from open fund of Fujian Provincial Key Laboratory of Functional Materials and Applications(Xiamen University of Technology,fma2024003)the National Key R&D Program of China(No.2021YFB3500400)the National Natural Science Foundation of China(Nos.52073286 and 22275185).
文摘Organic-inorganic hybrid metal halide perovskite solar cells(PSCs)have attracted much attention due to their high photoelectric conversion efficiency(PCE)and low cost.The certificated PCE of small active area(below 0.1 cm^(2))device has reached 26.7%[1].However,when considering the scaled-up commercialization of PSCs,an obvious efficiency drop exists for the translation to large-area perovskite submodules(PSMs)with areas more than 200 cm^(2),thus limiting the practical commercialization[2].The major PCE gap between small area cells and large area modules arises the drop of open-circuit voltage(VOC)and fill factor(FF).Formamidinium lead iodide(FAPbI_(3))is now the mostly widely used and highly efficient perovskite composition.However,the photo-active black α-FAPbI_(3) phase will spontaneously transform into photo-inactive yellowδ-FAPbI_(3) phase at room temperature[3].
