The publisher regrets to inform that in the article of Advanced Powder Materials 4(2025)100261,the published Figs.3 and 5 belong to the initially submitted version,which should be replaced by the final version.The dif...The publisher regrets to inform that in the article of Advanced Powder Materials 4(2025)100261,the published Figs.3 and 5 belong to the initially submitted version,which should be replaced by the final version.The differences between the initial and final versions of these figures are described below.展开更多
The efficiency of perovskite solar cells(PSCs)has progressed rapidly,exceeding 26%for single-junction devices and surpassing 34%in perovskite-silicon tandem configurations,establishing PSCs as a promising alternative ...The efficiency of perovskite solar cells(PSCs)has progressed rapidly,exceeding 26%for single-junction devices and surpassing 34%in perovskite-silicon tandem configurations,establishing PSCs as a promising alternative to traditional photovoltaic technologies.However,their commercialization is constrained by significant stability challenges in outdoor environments.This review critically examines key cell-level issues affecting the long-term performance and reliability of PSCs,focusing on instabilities arising from the intrinsic phases of the perovskite absorber and external stress factors.Mitigation strategies to enhance stability are discussed,alongside recent advancements in charge transport layers,electrodes,and interfaces aimed at reducing environmental degradation and improving energy level alignment for efficient charge extraction.The importance of accelerated aging tests and the establishment of standardized protocols is underscored for accurately predicting device lifetimes and identifying failure mechanisms,thereby ensuring stability under real-world conditions.Furthermore,a comprehensive techno-economic analysis evaluates how advancements in materials and strategic innovations influence efficiency,durability,and cost,which are critical for the commercial adoption of PSCs.This review delineates the essential steps required to transition PSC technology from laboratory-scale research to widespread commercialization within the global photovoltaic industry.展开更多
Intergrowth ferroelectric semiconductors with excellent spontaneous polarization field are highly promising piezo-photocatalytic candidate materials.In addition,developing structural design and revealing polarization ...Intergrowth ferroelectric semiconductors with excellent spontaneous polarization field are highly promising piezo-photocatalytic candidate materials.In addition,developing structural design and revealing polarization enhancement in-depth mechanism are top priorities.Herein,we introduce the intergrowth ferroelectrics Bi_(7)Ti_(4)NbO_(21)thin-layer nanosheets for piezo-photocatalytic CO_(2)reduction.Density functional theory(DFT)calculations indicate that interlayer lattice mismatch leads to increased tilting and rotation angle of Ti/NbO_(6)octahedra on perovskite-like layers,serving as the main reason for increased polarization.Furthermore,the tilting and rotation angle of the interlayer octahedron further increase under stress,suggesting a stronger driving force generated to facilitate charge carrier separation efficiency.Meanwhile,Bi_(7)Ti_(4)NbO_(21)nanosheets provide abundant active sites to effectively adsorb CO_(2)and acquire sensitive stress response,thereby presenting synergistically advanced piezo-photocatalytic CO_(2)reduction activity with a high CO generation rate of 426.97μmol g^(-1)h^(-1).Our work offers new perspectives and directions for initiating and investigating the mechanisms of high-performance intergrowth piezo-photocatalysts.展开更多
Polymer dielectrics possessing excellent electrical insulation and high thermal conductivity are pivotal for dielectric capacitors at elevated temperatures.However,the integration of electrical insulation and thermal ...Polymer dielectrics possessing excellent electrical insulation and high thermal conductivity are pivotal for dielectric capacitors at elevated temperatures.However,the integration of electrical insulation and thermal conductivity in polymers remains a challenge.In this work,we present a feasible strategy to integrate high electrical insulation and high thermal conductivity by bonding carbon quantum dots(CQDs)with the diamine monomer of polyetherimide(PEI).The CQDs with Coulomb blockade effect serve as traps for the migrating of electrons in the dielectrics,while the bonding networks formed by CQDs and PEI further deepen the traps and augment trap density.As a result,the hybrid dielectrics(PEI-NH_(2)-CQDs)exhibit nearly an order of magnitude higher electrical resistivity than that of pure PEI,leading to an 80%increase in discharge energy density with an energy efficiency of 90%at 200℃ compared to pure counterpart.Additionally,this all-organic dielectric achieves a significantly increased thermal conductivity of 0.65 W m^(-1) K^(-1) compared to 0.26 W m^(-1) K^(-1) of PEI,which supports its cyclic stability at elevated temperatures.We also demonstrate the kilogram-scale production of CQDs,synthesizing over 8 kg in a single batch,paving the way for large-scale production of reliable PEI-NH_(2)-CQDs dielectrics.展开更多
The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing area...The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing areas such as displays,lighting,photocatalysis,bio-imaging,and photonics devices and so on.Among the myriad QDs technologies,industrially relevant CuInS_(2)(CIS)QDs have emerged as promising alternatives to traditional Cd-and Pb-based QDs.Their tunable optoelectronic properties,high absorption coefficient,compositional flexibility,remarkable stability as well as Restriction of Hazardous Substances-compliance,with recent trends revealing a renewed interest in this material for various visible and near-infrared technological applications.This review focuses on recent advancements in CIS QDs as multidisciplinary field from its genesis in the mid-1990 to date with an emphasis on key breakthroughs in their synthesis,surface chemistry,post-synthesis modifications,and various applications.First,the comparation of properties of CIS QDs with relevant knowledge from other classes of QDs and from Ⅰ-Ⅱ-Ⅲ semiconductors as well is summarized.Second,recent advances in the synthesis methods,structure-optoelectronic properties,their defects,and passivation strategies as well as CIS-based heterostructures are discussed.Third,the state-of-the-art applications of CIS QDs ranging from solar cells,luminescence solar concentrations,photocatalysis,light emitting diodes,bioimaging and some emerging applications are summarized.Finally,we discuss open challenges and future perspectives for further advancement in this field.展开更多
Two-dimensional(2D)nitride MXenes are predicted to exhibit exceptional metallic properties and high polarity;however,their synthesis remains challenging.Research has relied on traditional molten salt etching,highlight...Two-dimensional(2D)nitride MXenes are predicted to exhibit exceptional metallic properties and high polarity;however,their synthesis remains challenging.Research has relied on traditional molten salt etching,highlighting the need for a scalable,high-purity approach.Here,we present the first solution-based synthesis of Ti_(4)N_(3)T_(x)MXene via a novel saturated salt solution(S^(3))etching technique employing alkali metal salts.By optimizing the sintering process for high-purity Ti_(4)AlN_(3)MAX and refining the S^(3)etching route,we significantly reduced the etch pit density to 1.2×10^(6)cm^(-2)and lowered the etch pit formation rate to 4%,yielding high-quality,phasepure Ti_(4)N_(3)T_(x)MXene.Our study highlights the critical role of alkali metal ions in selective A-layer removal and demonstrates the impressive electrical conductivity and electromagnetic interference shielding performance of 2D nitride MXene,setting a new benchmark for this underexplored material.These findings pave the way for advancing 2D nitride MXenes and their diverse applications.展开更多
The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be mo...The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be more complex,necessitating new theoretical frameworks,though key empirical evidence remains elusive.In this study,we used microdroplets to investigate the crystallization of sodium halides(NaCl,NaBr,and NaI)under homogeneous nucleation conditions across a wide range of supersaturations.In the evaporating droplet,NaCl follows the classical nucleation pathway,whereas NaBr and NaI exhibit the formation of an intermediate phase prior to the nucleation of anhydrous and hydrous single crystals,respectively.Optical and computational analyses indicate that these intermediate phases are liquid crystal phases composed of contact ion pairs.These findings establish a new theoretical framework for crystal nucleation and growth and offer methods to control nucleation pathways,enabling us to achieve desired crystals regardless of specific conditions.展开更多
Photocatalysis is one of the most capable green energy techniques for sustainable solar-to-chemical energy conversion.However,the speedy recombination of photocarriers remains a critical bottleneck in achieving high p...Photocatalysis is one of the most capable green energy techniques for sustainable solar-to-chemical energy conversion.However,the speedy recombination of photocarriers remains a critical bottleneck in achieving high photocatalytic efficiency.Recent advancements have underscored the pivotal role of internal and external electrostatic fields in regulating charge dynamics within semiconductor systems.This review highlights the emerging strategy of employing non-covalent electrostatic interactions to modulate photocatalytic behavior.Internally,spontaneous polarization within polar or ferroelectric semiconductors facilitates efficient charge separation through built-in electric fields.Externally applied mechanical stress and magnetic fields further augment these effects via piezoelectric and magnetoelectric phenomena,offering dynamic control over carrier transport.Beyond macroscopic fields,subtle non-covalent electrostatic forces,such as hydrogen bonds,van der Waals forces,andπ-πstacking,significantly influence surface adsorption,electronic structure modulation,and interfacial charge transfer processes.Combining these external influences with semiconductor properties,we can develop innovative strategies to stabilize the reactive intermediates and reduce the recombination pathways,improving the practical implications of these synergistic effects in energy conversion and environmental remediation.This review systematically elucidates the mechanistic contributions of internal polarization and external fields to the modulation of non-covalent electrostatic forces in photocatalytic systems.Emphasis is placed on material design strategies that integrate structural polarity,field-responsive behavior,and interfacial engineering to achieve superior photocatalytic performance.Finally,the prospects of non-covalent electrostatic interactions in photocatalysis are discussed,providing insights to guide the rational development of more efficient and sustainable photocatalytic systems.展开更多
The growing demand for carbon neutrality has heightened the focus on CO_(2)hydrogenation as a viable strategy for transforming carbon dioxide into valuable chemicals and fuels.Advanced machine learning(ML)approaches i...The growing demand for carbon neutrality has heightened the focus on CO_(2)hydrogenation as a viable strategy for transforming carbon dioxide into valuable chemicals and fuels.Advanced machine learning(ML)approaches integrate materials science with artificial intelligence,enabling scientists to identify hidden patterns in datasets,make informed decisions,and reduce the need for labor-intensive,repetitive experimentation.This review provides a comprehensive overview of ML applications in the thermocatalytic hydrogenation of CO_(2).Following an introduction to ML tools and workflows,various ML algorithms employed in CO_(2)hydrogenation are systematically categorized and reviewed.Next,the application of ML in catalyst discovery is discussed,highlighting its role in identifying optimal compositions and structures.Then,ML-driven strategies for process optimization,particularly in enhancing CO_(2)conversion and product selectivity,are examined.Studies modeling descriptors,spanning catalyst properties and reaction conditions,to predict catalytic performance are analyzed.Consequently,ML-based mechanistic studies are reviewed to elucidate reaction pathways,identify key intermediates,and optimize catalyst performance.Finally,key challenges and future perspectives in leveraging ML for advancing CO_(2)hydrogenation research are presented.展开更多
Ultra-high temperature materials are desirable to withstand the severe aero-thermochemical environments of hypersonic flight,paving the groundworks for flight speeds exceeding Mach 5.Here,we present a novel ultra-high...Ultra-high temperature materials are desirable to withstand the severe aero-thermochemical environments of hypersonic flight,paving the groundworks for flight speeds exceeding Mach 5.Here,we present a novel ultra-high temperature composite with superior ablation resistances up to 3000℃for 900 s,utilizing a tailored ultra-high melting point HfC_(0.76)N_(0.24)matrix reinforced with short carbon fibers.The ablation-resistant capability of this composite is over 14 times greater than that of HfC at 3000℃.Furthermore,this research presents the first comprehensive investigation into the internal mechanisms governing thermal oxidation evolution of HfC_(0.76)N_(0.24)matrix through a combination of experimental results and theoretical simulations.The mechanistic details of these complex oxidation processes are elucidated in terms of chemical bonding and clusters evolutions,along with their relationship to cooperative oxygen atoms and molecules.Notably,nitrogen atoms do not directly generate gas and escape from the composites,rather,they interact with hafnium atoms to form Hf-C-N-O clusters with robust bonding for enhanced viscosity during ablation.These findings provide valuable insights into the transition from micro to macro scales,which will be the paradigm of inspiring and accelerating materials discovery in this field,as well as taking advantage of their full potential in the application of hypersonic aircraft and spacecraft vehicles.展开更多
In recent years,photo-powered energy storage devices have attracted considerable research attention due to their potential applications in smart electronics.In this review,we present a comprehensive summary of recent ...In recent years,photo-powered energy storage devices have attracted considerable research attention due to their potential applications in smart electronics.In this review,we present a comprehensive summary of recent developments in two distinct but highly promising energy storage technologies,photo-assisted metal-air batteries and photo-supercapacitors.The section on metal-air batteries primarily describes the electrochemical performance of Zn-air and Li-air systems,innovative photo-electrode designs,and mechanisms that enhance oxygen evolution and reduction reactions.A brief discussion is also provided of other metal-air systems,including Mg,Fe,and Al.In contrast,the section on photo-supercapacitors explores recent advancements in light-driven charge storage,electrode materials,and device architectures,presenting a comparative performance analysis of materials such as metal oxides,sulfides,and perovskites.Various critical challenges,including material stability,efficiency under varying light conditions,and scalability,are also thoroughly examined.Despite their different working principles,both technologies hold great potential to increase energy efficiency and sustainability through the use of photo-assisted processes.The purpose of this review is to bridge existing knowledge gaps and propose future directions for research in these emerging fields.展开更多
Pursuing new two-dimensional(2D)materials has been a hot topic in materials science,driven by their potential for diverse applications.Recent research has unveiled stable planar hypercoordinate motifs with unconventio...Pursuing new two-dimensional(2D)materials has been a hot topic in materials science,driven by their potential for diverse applications.Recent research has unveiled stable planar hypercoordinate motifs with unconventional geometric arrangements and bonding patterns that facilitate the synthesis of new 2D materials with diverse applications.Among these,yet the design of 2D transition metal systems featuring planar pentacoordinate boron(ppB)is particularly intriguing.Here we address this gap by proposing a novel family of transition metal boride monolayers(MBenes)composed of ppB and heptacoordinate M motifs.The novelty of our MBenes stems from their distinct atomic arrangements and bonding configurations,setting them apart from traditional 2D materials.High-throughput calculations identified 10 stable MBenes(with the stoichiometry of MB,M=Cr,Fe,Co,Ni,Cu,Mo,Pd,Ag,Pt,Au)with exceptional thermodynamic,dynamic,thermal,and mechanical stabilities attributed to strong BB covalent bonds and MB ionic interactions.Notably,five of these MBenes(M=Ni,Pd,Pt,Ag,Au)hold high promise as topological superconducting materials with superconducting transition temperatures of 2.4-5.2 K.This discovery not only enriches the family of topological superconducting materials but also opens new avenues for quantum device development.Meanwhile,FeB monolayer exhibits robust ferromagnetic properties with a high Curie temperature of~750 K,which is particularly significant for spintronics applications.In addition,NiB and CuB MBenes demonstrate extremely low sodium diffusion barriers(about 30 and 90 meV)and high sodium storage capacities(788 and 734 mAh g1,respectively),making them promising anode materials for sodium-ion batteries(SIBs).This study expands the selection of electrode materials for SIBs and mitigates some existing limitations in battery technology.Overall,these findings underscore the multifunctional potential of MBenes,positioning them as transformative materials for quantum computing,spintronics,and energy storage applications.展开更多
A seamless combination of mechanical energy-harvesting triboelectric nanogenerators with other technologies is the key to widening their applicability.Combining luminescent and triboelectric materials can develop hybr...A seamless combination of mechanical energy-harvesting triboelectric nanogenerators with other technologies is the key to widening their applicability.Combining luminescent and triboelectric materials can develop hybrid nanogenerators(HNGs)which can be utilized for energy-harvesting,optical thermometry,and lighting applications.In this study,we designed an Er^(3+)and Eu^(3+)co-doped Sr_(1.85)Ca_(0.15)NaNb_(5)O_(15)(SCNNO:EE)green-yellow-emitting phosphor with excellent temperature-sensing capabilities.SCNNO:EE possessed a high dielectric constant and was thus utilized as a filler inside the polydimethylsiloxane polymer to fabricate composite films.The composite films were employed to fabricate various HNG devices and the filler concentration was optimized to attain the highest electrical output of 170 V,5.05μA,and 75μC/m^(2).The piezoelectric-structured energy-harvesting device(PSEHD)was fabricated and further modified to fabricate a self-activated PSEHD(SAPSEHD)for solid-state lighting applications.Different engraved aluminum electrodes were attached to the composite films to obtain different glowing words and patterns.The electrical signals generated by the PSEHD,when the pressure was applied,were fed into the processing unit,which further flowing into the SAPSEHD.The SAPSEHD can generate electrical signals when pressure is applied and automatically produce light by activating the phosphor in the composite film.This type of devices could attract attention at the places where pressure-activated automatic lighting is required.Also,owing to the promising properties of the proposed devices,they can be utilized for various applications on a large scale.展开更多
Ferroelectric materials are gaining increasing attention for the development of advanced catalytic technologies due to their field-responsive polarization states.However,achieving dynamic optimization of catalytic act...Ferroelectric materials are gaining increasing attention for the development of advanced catalytic technologies due to their field-responsive polarization states.However,achieving dynamic optimization of catalytic activity using ferroelectrics remains a fundamental challenge.Inspired by the force-adaptive mechanisms of fish scales,we introduce an intracrystalline force regulation strategy to dynamically control cobalt spin states and enhance peroxymonosulfate(PMS)activation in Fenton-like processes.This approach utilizes BaTi_(0.92)Co_(0.08)O_(3-δ)(BTC-8)nano-ferroelectrics,where ultrasound irradiation generates a built-in electric field that drives electrons towards cobalt sites.This electron transfer is further facilitated by electronegativity differences between cobalt and barium/titanium ions.The resulting piezo-driven electron flow promotes continuous regeneration of high-spin Co^(2+),enhancing PMS adsorption and SO_(4)^(-)-OH bond cleavage,leading to increased production of⋅SO_(4)^(-)and singlet oxygen(^(1)O_(2))for organic pollutant degradation.Consequently,BTC-8 achieves a reaction rate(k=1.7960 min^(-1))28.93 times higher than that of pure barium titanate,surpassing previously reported PMS activation and piezocatalytic systems.This work represents a shift from static electronic structure design to dynamic electronic engineering in the development of advanced catalytic strategies for water remediation.展开更多
Amorphous transition metal compounds(a-TMC)become one of the most promising pre-catalysts toward oxygen evolution reaction(OER)due to their high-entropy nature and flexible self-reconstruction to highly active derivat...Amorphous transition metal compounds(a-TMC)become one of the most promising pre-catalysts toward oxygen evolution reaction(OER)due to their high-entropy nature and flexible self-reconstruction to highly active derivatives.However,the loosen bonds inside the amorphous structure make it an electronic insulator with unstable structure.Here,monodispersed Ni^(2+)-phytate nanospheres implanted by Fe^(3+)ions(NS_(FeNiPA))were firstly prepared and subsequently transferred into homogeneous high-entropy type Fe-Ni-P-O-C amorphous nanospheres(CNS_(FeNiPO)).It is shown that the CNS_(FeNiPO) presents robust structure and remarkable Fe ions migration during potential-driven activation process,which benefits efficient surface reconstruction and spherical morphology preservation.The CNS_(FeNiPO) with low mass loading of 0.1mg/cm^(2)could deliver small overpotential of 270mV at 10mAcm^(−2)and almost 100%retention of the initial current density after 10h test.The improved electrocatalytic activity is attributed to the boosted electron transfer from Ni sites to O-containing intermediates by introduction of Fe and P atoms.Moreover,rechargeable Zn-air battery with CNS_(FeNiPO)+Pt/C could achieve lower charge potential platform and better cycling performance than that with commercial RuO_(2)+Pt/C.This work provides new insights into the design and understanding of high-entropy amorphous pre-catalysts toward OER.展开更多
Simultaneously inducing dual built-in electric fields(EFs)both within a single component and at the heterojunction interface creates a dual-driving force that is crucial for promoting spatial charge separation.This is...Simultaneously inducing dual built-in electric fields(EFs)both within a single component and at the heterojunction interface creates a dual-driving force that is crucial for promoting spatial charge separation.This is particularly significant in challenging coupled systems,such as CO_(2)photoreduction integrated with selective oxidation of toluene to benzaldehyde.However,developing such a system is quite challenging and often requires a precise design and engineering.Herein,we demonstrate a unique Ni-CdS@Ni(OH)_(2)heterojunction synthesized via an in-situ self-assembly method.Comprehensive mechanistic and theoretical investigations reveal that the NiCdS@Ni(OH)_(2)heterojunction induces dual electric fields(EFs):an intrinsic polarized electric-field within the CdS lattice from Ni doping and an interfacial electric-field from the growth of ultrathin nanosheets of Ni(OH)_(2)on NiCdS nanorods,enabling efficient spatial charge separation and enhanced redox potential.As proof of concept,the Ni-CdS@Ni(OH)_(2)heterojunction simultaneously exhibits outstanding bifunctional photocatalytic performance,producing CO at a rate of 427μmol g^(-1)h^(-1)and selectively oxidizing toluene to benzaldehyde at a rate of 1476μmol g^(-1)h^(-1)with a selectivity exceeding 85%.This work offers a promising strategy to optimize the utilization of photogenerated carriers in heterojunction photocatalysts,advancing synergistic photocatalytic redox systems.展开更多
Balancing the adsorption of OH⁻and 5-hydroxymethylfurfural(HMF)is crucial in optimizing the competing HMF oxidation reaction and oxygen evolution reaction,especially given the polymerization tendency of HMF in alkalin...Balancing the adsorption of OH⁻and 5-hydroxymethylfurfural(HMF)is crucial in optimizing the competing HMF oxidation reaction and oxygen evolution reaction,especially given the polymerization tendency of HMF in alkaline solutions.Herein,we present an innovative approach for rapidly synthesizing a NiFe bimetallic metalorganic framework(MOF)induced by electron-withdrawing carbon quantum dot(EW-CQD)via electron beam irradiation within 2 min.EW-CQD serve as structural regulators,expanding the NiFe-MOF interlayer spacing,increasing reactive site availability,and more effectively balancing the adsorption of OH6(-) and HMF,thereby significantly boosting the oxidation activity of HMF.The resulting EW-CQD-MOF exhibits a low potential of 1.36 V vs.RHE at 10 mA cm^(-2)and maintains excellent durability over 120 h.Comprehensive in situ characterization elucidates the HMF oxidation reaction pathway,showing high selectivity towards 2,5-furandicarboxylic acid(FDCA)under ambient conditions,with an impressive HMF conversion rate of 94%and FDCA selectivity of 96%within 6 h.These findings underscore the critical role of structural optimization and adsorption balance in catalytic performance enhancement and offer valuable insights for designing high-efficiency catalysts,advancing sustainable catalytic processes.展开更多
Anode-free sodium metal batteries(AFSMBs)have gained attention as next-generation storage systems with high energy density and cost-effectiveness.However,non-uniform sodium(Na)deposition and an unsteady solid electrol...Anode-free sodium metal batteries(AFSMBs)have gained attention as next-generation storage systems with high energy density and cost-effectiveness.However,non-uniform sodium(Na)deposition and an unsteady solid electrolyte interphase(SEI)lead to dendrite-related issues and severe irreversible Na^(+)plating/stripping,greatly aggravating their cycle deterioration.In this study,we effectively modified the 3D current collector's electronic structure by introducing Zn-N_(x)active sites(Zn-CNF),which enhances lateral Na^(+)diffusion and the Na planar growth,enabling uniform deep Na deposition at an exceptionally high capacity of 10 mA h cm^(-2).Furthermore,the Zn-N_(x)bonds enhance the adsorption capacity of PF6and contribute to forming a stable inorganic-rich SEI layer.Consequently,Zn-CNF with the electronic structure regulation endows an ultra-low nucleation overpotential(8 mV)and ultra-high Coulombic efficiency of 99.94%over 1,600 cycles.Symmetric cells demonstrate stable Na^(+)plating/stripping behavior for more than 4,400 h at 1 mA cm^(-2).Moreover,under high cathode loading(7.97 mg cm^(-2)),the AFSMBs achieve a high energy density of 374 W h kg^(-1)and retain a high discharge capacity of 82.49 mA h g^(-1)with a capacity retention of 80.4%after 120 cycles.This work proposes a viable strategy to achieving high-energy-density AFSMBs.展开更多
Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and c...Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and competition against the hydrogen evolution reaction hinder its practical implementation.To address these,the design of highly active catalysts is critical.Single-atom catalysts(SACs)have shown great potential because of their maximized atom utilization,but their limited stability and low metal loading restrict their performances.On the other hand,dual-atom catalysts(DACs)are atomic catalysts with two metal atoms nearby and offer enhanced electrocatalytic performances by aligning with the N≡N bond to enhance N2 reduction efficiency,potentially overcoming the limitations of SAC.This review discusses recent advances in SACs and more importantly DACs for ENRR,highlighting their advantages,limitations,and the need for advanced characterization techniques to better understand catalyst behavior.The review concludes by underscoring the importance of research to optimize these catalysts for efficient and sustainable nitrogen fixation.展开更多
Driven by rapid advancements in smart wearable technologies and perovskite photovoltaics,flexible perovskite solar cells(FPSCs)have emerged as highly promising autonomous power sources,poised to transform the next gen...Driven by rapid advancements in smart wearable technologies and perovskite photovoltaics,flexible perovskite solar cells(FPSCs)have emerged as highly promising autonomous power sources,poised to transform the next generation of mobile energy systems,portable electronics,and integrated wearable devices.For successful deployment in real-world scenarios,FPSCs must exhibit a combination of key attributes,including high power conversion efficiency,lightweight architecture,environmental robustness,and mechanical adaptability-encompassing flexibility,stretchability,and twistability.This review provides a detailed examination of the evolution,current state,and practical deployment of FPSCs,emphasizing their potential as efficient,portable energy solutions.It investigates advanced strategies for improving environmental resilience and mechanical recoverability,including the engineering of flexible substrates,deposition of high-quality perovskite films,and optimization of charge-selective interfaces.Additionally,it offers a systematic analysis of device design,fabrication protocols,scalable printing techniques,and standardized performance evaluation methods tailored for wearable FPSCs.Recent progress in enhancing the optoelectronic properties and mechanical durability of FPSCs is also critically reviewed.Ultimately,this work delivers a comprehensive perspective on FPSCs from both optoelectronic and mechanical viewpoints,identifies key challenges,and outlines future research pathways toward the seamless integration of FPSCs into multifunctional,next-generation wearable systems.展开更多
文摘The publisher regrets to inform that in the article of Advanced Powder Materials 4(2025)100261,the published Figs.3 and 5 belong to the initially submitted version,which should be replaced by the final version.The differences between the initial and final versions of these figures are described below.
基金supported by a National Research Foundation of Korea(NRF)grant(No.2016R1A3B 1908249),funded by the Korean government.
文摘The efficiency of perovskite solar cells(PSCs)has progressed rapidly,exceeding 26%for single-junction devices and surpassing 34%in perovskite-silicon tandem configurations,establishing PSCs as a promising alternative to traditional photovoltaic technologies.However,their commercialization is constrained by significant stability challenges in outdoor environments.This review critically examines key cell-level issues affecting the long-term performance and reliability of PSCs,focusing on instabilities arising from the intrinsic phases of the perovskite absorber and external stress factors.Mitigation strategies to enhance stability are discussed,alongside recent advancements in charge transport layers,electrodes,and interfaces aimed at reducing environmental degradation and improving energy level alignment for efficient charge extraction.The importance of accelerated aging tests and the establishment of standardized protocols is underscored for accurately predicting device lifetimes and identifying failure mechanisms,thereby ensuring stability under real-world conditions.Furthermore,a comprehensive techno-economic analysis evaluates how advancements in materials and strategic innovations influence efficiency,durability,and cost,which are critical for the commercial adoption of PSCs.This review delineates the essential steps required to transition PSC technology from laboratory-scale research to widespread commercialization within the global photovoltaic industry.
基金support from the Natural Science Foundation of Jiangsu Province(BK20220596)Innovative science and technology platform project of cooperation between Yangzhou City and Yangzhou University,China(No.YZ202026305)+1 种基金Natural Science Foundation of China(21922202,21673202 and 22272147)the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Intergrowth ferroelectric semiconductors with excellent spontaneous polarization field are highly promising piezo-photocatalytic candidate materials.In addition,developing structural design and revealing polarization enhancement in-depth mechanism are top priorities.Herein,we introduce the intergrowth ferroelectrics Bi_(7)Ti_(4)NbO_(21)thin-layer nanosheets for piezo-photocatalytic CO_(2)reduction.Density functional theory(DFT)calculations indicate that interlayer lattice mismatch leads to increased tilting and rotation angle of Ti/NbO_(6)octahedra on perovskite-like layers,serving as the main reason for increased polarization.Furthermore,the tilting and rotation angle of the interlayer octahedron further increase under stress,suggesting a stronger driving force generated to facilitate charge carrier separation efficiency.Meanwhile,Bi_(7)Ti_(4)NbO_(21)nanosheets provide abundant active sites to effectively adsorb CO_(2)and acquire sensitive stress response,thereby presenting synergistically advanced piezo-photocatalytic CO_(2)reduction activity with a high CO generation rate of 426.97μmol g^(-1)h^(-1).Our work offers new perspectives and directions for initiating and investigating the mechanisms of high-performance intergrowth piezo-photocatalysts.
基金supported by the National Natural Science Foundation of China(52172265)Excellent Youth Science Foundation of Hunan Province(2022JJ20067)+1 种基金The Science and Technology Innovation Program of Hunan Province(2022RC1074)Central South University Innovation-Driven Research Program(2023CXQD010).
文摘Polymer dielectrics possessing excellent electrical insulation and high thermal conductivity are pivotal for dielectric capacitors at elevated temperatures.However,the integration of electrical insulation and thermal conductivity in polymers remains a challenge.In this work,we present a feasible strategy to integrate high electrical insulation and high thermal conductivity by bonding carbon quantum dots(CQDs)with the diamine monomer of polyetherimide(PEI).The CQDs with Coulomb blockade effect serve as traps for the migrating of electrons in the dielectrics,while the bonding networks formed by CQDs and PEI further deepen the traps and augment trap density.As a result,the hybrid dielectrics(PEI-NH_(2)-CQDs)exhibit nearly an order of magnitude higher electrical resistivity than that of pure PEI,leading to an 80%increase in discharge energy density with an energy efficiency of 90%at 200℃ compared to pure counterpart.Additionally,this all-organic dielectric achieves a significantly increased thermal conductivity of 0.65 W m^(-1) K^(-1) compared to 0.26 W m^(-1) K^(-1) of PEI,which supports its cyclic stability at elevated temperatures.We also demonstrate the kilogram-scale production of CQDs,synthesizing over 8 kg in a single batch,paving the way for large-scale production of reliable PEI-NH_(2)-CQDs dielectrics.
基金X.H.acknowledges the financial support by Australian Research Council(ARC)Future Fellowship(FT190100756)M.P.S.gratefully acknowledges the support by the ARC under Discovery Early Career Researcher Award(DECRA)(DE210101565)and Discovery Project(DP230101676).
文摘The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing areas such as displays,lighting,photocatalysis,bio-imaging,and photonics devices and so on.Among the myriad QDs technologies,industrially relevant CuInS_(2)(CIS)QDs have emerged as promising alternatives to traditional Cd-and Pb-based QDs.Their tunable optoelectronic properties,high absorption coefficient,compositional flexibility,remarkable stability as well as Restriction of Hazardous Substances-compliance,with recent trends revealing a renewed interest in this material for various visible and near-infrared technological applications.This review focuses on recent advancements in CIS QDs as multidisciplinary field from its genesis in the mid-1990 to date with an emphasis on key breakthroughs in their synthesis,surface chemistry,post-synthesis modifications,and various applications.First,the comparation of properties of CIS QDs with relevant knowledge from other classes of QDs and from Ⅰ-Ⅱ-Ⅲ semiconductors as well is summarized.Second,recent advances in the synthesis methods,structure-optoelectronic properties,their defects,and passivation strategies as well as CIS-based heterostructures are discussed.Third,the state-of-the-art applications of CIS QDs ranging from solar cells,luminescence solar concentrations,photocatalysis,light emitting diodes,bioimaging and some emerging applications are summarized.Finally,we discuss open challenges and future perspectives for further advancement in this field.
基金supported by the Nano&Material Technology Development Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(Grant No.RS-2024-00408180)by Institute for Basic Science(No.IBS-R019-G1).
文摘Two-dimensional(2D)nitride MXenes are predicted to exhibit exceptional metallic properties and high polarity;however,their synthesis remains challenging.Research has relied on traditional molten salt etching,highlighting the need for a scalable,high-purity approach.Here,we present the first solution-based synthesis of Ti_(4)N_(3)T_(x)MXene via a novel saturated salt solution(S^(3))etching technique employing alkali metal salts.By optimizing the sintering process for high-purity Ti_(4)AlN_(3)MAX and refining the S^(3)etching route,we significantly reduced the etch pit density to 1.2×10^(6)cm^(-2)and lowered the etch pit formation rate to 4%,yielding high-quality,phasepure Ti_(4)N_(3)T_(x)MXene.Our study highlights the critical role of alkali metal ions in selective A-layer removal and demonstrates the impressive electrical conductivity and electromagnetic interference shielding performance of 2D nitride MXene,setting a new benchmark for this underexplored material.These findings pave the way for advancing 2D nitride MXenes and their diverse applications.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2021R1C1C2006535)supported by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Korea government(MSIT)(No.RS-2024-00403164)supported by the National Research Foundation of Korea grant funded by the Korea government,Ministry of Science and ICT(Development of Nanofiber Yarn Based Compound Sensor as a Comprehensive Wearable Healthcare Solution)(Grant No.RS-2024-00357296).
文摘The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be more complex,necessitating new theoretical frameworks,though key empirical evidence remains elusive.In this study,we used microdroplets to investigate the crystallization of sodium halides(NaCl,NaBr,and NaI)under homogeneous nucleation conditions across a wide range of supersaturations.In the evaporating droplet,NaCl follows the classical nucleation pathway,whereas NaBr and NaI exhibit the formation of an intermediate phase prior to the nucleation of anhydrous and hydrous single crystals,respectively.Optical and computational analyses indicate that these intermediate phases are liquid crystal phases composed of contact ion pairs.These findings establish a new theoretical framework for crystal nucleation and growth and offer methods to control nucleation pathways,enabling us to achieve desired crystals regardless of specific conditions.
基金the Deputyship for Research and Innovation,“Ministry of Education”in Saudi Arabia for funding this research(IFKSU-HCRA-12-3).
文摘Photocatalysis is one of the most capable green energy techniques for sustainable solar-to-chemical energy conversion.However,the speedy recombination of photocarriers remains a critical bottleneck in achieving high photocatalytic efficiency.Recent advancements have underscored the pivotal role of internal and external electrostatic fields in regulating charge dynamics within semiconductor systems.This review highlights the emerging strategy of employing non-covalent electrostatic interactions to modulate photocatalytic behavior.Internally,spontaneous polarization within polar or ferroelectric semiconductors facilitates efficient charge separation through built-in electric fields.Externally applied mechanical stress and magnetic fields further augment these effects via piezoelectric and magnetoelectric phenomena,offering dynamic control over carrier transport.Beyond macroscopic fields,subtle non-covalent electrostatic forces,such as hydrogen bonds,van der Waals forces,andπ-πstacking,significantly influence surface adsorption,electronic structure modulation,and interfacial charge transfer processes.Combining these external influences with semiconductor properties,we can develop innovative strategies to stabilize the reactive intermediates and reduce the recombination pathways,improving the practical implications of these synergistic effects in energy conversion and environmental remediation.This review systematically elucidates the mechanistic contributions of internal polarization and external fields to the modulation of non-covalent electrostatic forces in photocatalytic systems.Emphasis is placed on material design strategies that integrate structural polarity,field-responsive behavior,and interfacial engineering to achieve superior photocatalytic performance.Finally,the prospects of non-covalent electrostatic interactions in photocatalysis are discussed,providing insights to guide the rational development of more efficient and sustainable photocatalytic systems.
文摘The growing demand for carbon neutrality has heightened the focus on CO_(2)hydrogenation as a viable strategy for transforming carbon dioxide into valuable chemicals and fuels.Advanced machine learning(ML)approaches integrate materials science with artificial intelligence,enabling scientists to identify hidden patterns in datasets,make informed decisions,and reduce the need for labor-intensive,repetitive experimentation.This review provides a comprehensive overview of ML applications in the thermocatalytic hydrogenation of CO_(2).Following an introduction to ML tools and workflows,various ML algorithms employed in CO_(2)hydrogenation are systematically categorized and reviewed.Next,the application of ML in catalyst discovery is discussed,highlighting its role in identifying optimal compositions and structures.Then,ML-driven strategies for process optimization,particularly in enhancing CO_(2)conversion and product selectivity,are examined.Studies modeling descriptors,spanning catalyst properties and reaction conditions,to predict catalytic performance are analyzed.Consequently,ML-based mechanistic studies are reviewed to elucidate reaction pathways,identify key intermediates,and optimize catalyst performance.Finally,key challenges and future perspectives in leveraging ML for advancing CO_(2)hydrogenation research are presented.
基金funding by the National Natural Science Foundation of China(52302128)the Foundation of State Key Laboratory of Science and Technology on Advanced Ceramic Fibers and Composites(No.6142907230303).
文摘Ultra-high temperature materials are desirable to withstand the severe aero-thermochemical environments of hypersonic flight,paving the groundworks for flight speeds exceeding Mach 5.Here,we present a novel ultra-high temperature composite with superior ablation resistances up to 3000℃for 900 s,utilizing a tailored ultra-high melting point HfC_(0.76)N_(0.24)matrix reinforced with short carbon fibers.The ablation-resistant capability of this composite is over 14 times greater than that of HfC at 3000℃.Furthermore,this research presents the first comprehensive investigation into the internal mechanisms governing thermal oxidation evolution of HfC_(0.76)N_(0.24)matrix through a combination of experimental results and theoretical simulations.The mechanistic details of these complex oxidation processes are elucidated in terms of chemical bonding and clusters evolutions,along with their relationship to cooperative oxygen atoms and molecules.Notably,nitrogen atoms do not directly generate gas and escape from the composites,rather,they interact with hafnium atoms to form Hf-C-N-O clusters with robust bonding for enhanced viscosity during ablation.These findings provide valuable insights into the transition from micro to macro scales,which will be the paradigm of inspiring and accelerating materials discovery in this field,as well as taking advantage of their full potential in the application of hypersonic aircraft and spacecraft vehicles.
基金supported by the National Natural Science Foundation of China(Grant No.52263028)Xingdian Talent Funding Project(Year 2022,Yunnan Province,China).
文摘In recent years,photo-powered energy storage devices have attracted considerable research attention due to their potential applications in smart electronics.In this review,we present a comprehensive summary of recent developments in two distinct but highly promising energy storage technologies,photo-assisted metal-air batteries and photo-supercapacitors.The section on metal-air batteries primarily describes the electrochemical performance of Zn-air and Li-air systems,innovative photo-electrode designs,and mechanisms that enhance oxygen evolution and reduction reactions.A brief discussion is also provided of other metal-air systems,including Mg,Fe,and Al.In contrast,the section on photo-supercapacitors explores recent advancements in light-driven charge storage,electrode materials,and device architectures,presenting a comparative performance analysis of materials such as metal oxides,sulfides,and perovskites.Various critical challenges,including material stability,efficiency under varying light conditions,and scalability,are also thoroughly examined.Despite their different working principles,both technologies hold great potential to increase energy efficiency and sustainability through the use of photo-assisted processes.The purpose of this review is to bridge existing knowledge gaps and propose future directions for research in these emerging fields.
基金supported by Research Foundation for Advanced Talents of Inner Mongolia Normal University(2025YJRC005)the National Natural Science Foundation of China(12364038)+5 种基金the“Grassland Talents”project of the Inner Mongolia Autonomous Region(12000-12102613)the Young Science and Technology Talents Cultivation Project of Inner Mongolia University(21200-5223708)the Industrial Technology Innovation Projects of Inner Mongolia Academy of Science and Technology of China(2023JSYD01002)Science and Technology Plan Projects of Inner Mongolia Autonomous Region of China(2023KYPT0012)Key Project Funding from the Inner Mongolia Autonomous Region Natural Science Foundation(2023ZD27)High Level Introduction of Talent Research Start-up Fund(5909002405).
文摘Pursuing new two-dimensional(2D)materials has been a hot topic in materials science,driven by their potential for diverse applications.Recent research has unveiled stable planar hypercoordinate motifs with unconventional geometric arrangements and bonding patterns that facilitate the synthesis of new 2D materials with diverse applications.Among these,yet the design of 2D transition metal systems featuring planar pentacoordinate boron(ppB)is particularly intriguing.Here we address this gap by proposing a novel family of transition metal boride monolayers(MBenes)composed of ppB and heptacoordinate M motifs.The novelty of our MBenes stems from their distinct atomic arrangements and bonding configurations,setting them apart from traditional 2D materials.High-throughput calculations identified 10 stable MBenes(with the stoichiometry of MB,M=Cr,Fe,Co,Ni,Cu,Mo,Pd,Ag,Pt,Au)with exceptional thermodynamic,dynamic,thermal,and mechanical stabilities attributed to strong BB covalent bonds and MB ionic interactions.Notably,five of these MBenes(M=Ni,Pd,Pt,Ag,Au)hold high promise as topological superconducting materials with superconducting transition temperatures of 2.4-5.2 K.This discovery not only enriches the family of topological superconducting materials but also opens new avenues for quantum device development.Meanwhile,FeB monolayer exhibits robust ferromagnetic properties with a high Curie temperature of~750 K,which is particularly significant for spintronics applications.In addition,NiB and CuB MBenes demonstrate extremely low sodium diffusion barriers(about 30 and 90 meV)and high sodium storage capacities(788 and 734 mAh g1,respectively),making them promising anode materials for sodium-ion batteries(SIBs).This study expands the selection of electrode materials for SIBs and mitigates some existing limitations in battery technology.Overall,these findings underscore the multifunctional potential of MBenes,positioning them as transformative materials for quantum computing,spintronics,and energy storage applications.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean Government(MSIT)(No.2018R1A6A1A03025708).
文摘A seamless combination of mechanical energy-harvesting triboelectric nanogenerators with other technologies is the key to widening their applicability.Combining luminescent and triboelectric materials can develop hybrid nanogenerators(HNGs)which can be utilized for energy-harvesting,optical thermometry,and lighting applications.In this study,we designed an Er^(3+)and Eu^(3+)co-doped Sr_(1.85)Ca_(0.15)NaNb_(5)O_(15)(SCNNO:EE)green-yellow-emitting phosphor with excellent temperature-sensing capabilities.SCNNO:EE possessed a high dielectric constant and was thus utilized as a filler inside the polydimethylsiloxane polymer to fabricate composite films.The composite films were employed to fabricate various HNG devices and the filler concentration was optimized to attain the highest electrical output of 170 V,5.05μA,and 75μC/m^(2).The piezoelectric-structured energy-harvesting device(PSEHD)was fabricated and further modified to fabricate a self-activated PSEHD(SAPSEHD)for solid-state lighting applications.Different engraved aluminum electrodes were attached to the composite films to obtain different glowing words and patterns.The electrical signals generated by the PSEHD,when the pressure was applied,were fed into the processing unit,which further flowing into the SAPSEHD.The SAPSEHD can generate electrical signals when pressure is applied and automatically produce light by activating the phosphor in the composite film.This type of devices could attract attention at the places where pressure-activated automatic lighting is required.Also,owing to the promising properties of the proposed devices,they can be utilized for various applications on a large scale.
基金the National Natural Science Foundation of China(Grant No.U2002217,52102342,52103024 and 12404116)Key Research Program of the Chinese Academy of Sciences(Grant No.ZDRW-CN2021-3-1-18)+5 种基金Chenguang Program of Shanghai Education Development Foundation,Shanghai Municipal Education Commission(Grant No.21CGA40)9th Young Elite Scientists Sponsorship Program by CAST(Grant No.2023QNRC001)10th Young Elite Scientists Sponsorship Program by CAST(Grant No.YESS20240270)the Postdoctoral Fellowship Program of CPSF(Grant No.GZC20232832)Donghua University 2024 Cultivation Project of Discipline Innovation(Grant No.xkcx-202413)Student Training Program for Innovation and Entrepreneurship of Hangzhou Institute for Advanced Study,University of Chinese Academy of Sciences(Grant No.CXCY20230305).
文摘Ferroelectric materials are gaining increasing attention for the development of advanced catalytic technologies due to their field-responsive polarization states.However,achieving dynamic optimization of catalytic activity using ferroelectrics remains a fundamental challenge.Inspired by the force-adaptive mechanisms of fish scales,we introduce an intracrystalline force regulation strategy to dynamically control cobalt spin states and enhance peroxymonosulfate(PMS)activation in Fenton-like processes.This approach utilizes BaTi_(0.92)Co_(0.08)O_(3-δ)(BTC-8)nano-ferroelectrics,where ultrasound irradiation generates a built-in electric field that drives electrons towards cobalt sites.This electron transfer is further facilitated by electronegativity differences between cobalt and barium/titanium ions.The resulting piezo-driven electron flow promotes continuous regeneration of high-spin Co^(2+),enhancing PMS adsorption and SO_(4)^(-)-OH bond cleavage,leading to increased production of⋅SO_(4)^(-)and singlet oxygen(^(1)O_(2))for organic pollutant degradation.Consequently,BTC-8 achieves a reaction rate(k=1.7960 min^(-1))28.93 times higher than that of pure barium titanate,surpassing previously reported PMS activation and piezocatalytic systems.This work represents a shift from static electronic structure design to dynamic electronic engineering in the development of advanced catalytic strategies for water remediation.
基金financially supported by National Natural Science Foundation of China(22278170,52172058)Natural Science Foundation of Anhui Province(2408085QB037)+3 种基金Natural Science Foundation of Anhui Provincial Department of Education(2023AH020042,2024AH051721)financial support from High-Level Talents Introduction and Cultivation Plan of Anhui Province-Young Top Talent,Huainan Innovation and Entrepreneurship Star Team(HNSTD-2024),Huainan Research Center of New Carbon Energy Materials(HNSPT02)New Energy Materials and Technology Research Center of Huainan Normal University.Business Finland,BATCircle2.0 project(Grant No.44612/31/2020)is acknowledged for financial supportU.L.acknowledges Finnish Research Impact Foundation for Tandem Industry Academy Professorship funding in 2023-2025.
文摘Amorphous transition metal compounds(a-TMC)become one of the most promising pre-catalysts toward oxygen evolution reaction(OER)due to their high-entropy nature and flexible self-reconstruction to highly active derivatives.However,the loosen bonds inside the amorphous structure make it an electronic insulator with unstable structure.Here,monodispersed Ni^(2+)-phytate nanospheres implanted by Fe^(3+)ions(NS_(FeNiPA))were firstly prepared and subsequently transferred into homogeneous high-entropy type Fe-Ni-P-O-C amorphous nanospheres(CNS_(FeNiPO)).It is shown that the CNS_(FeNiPO) presents robust structure and remarkable Fe ions migration during potential-driven activation process,which benefits efficient surface reconstruction and spherical morphology preservation.The CNS_(FeNiPO) with low mass loading of 0.1mg/cm^(2)could deliver small overpotential of 270mV at 10mAcm^(−2)and almost 100%retention of the initial current density after 10h test.The improved electrocatalytic activity is attributed to the boosted electron transfer from Ni sites to O-containing intermediates by introduction of Fe and P atoms.Moreover,rechargeable Zn-air battery with CNS_(FeNiPO)+Pt/C could achieve lower charge potential platform and better cycling performance than that with commercial RuO_(2)+Pt/C.This work provides new insights into the design and understanding of high-entropy amorphous pre-catalysts toward OER.
基金The authors sincerely appreciate funding from“Producing Hydrogen in Trentino-H2@TN”(PAT-Trento)through the research grant(SAP 40104237)Researchers Supporting Project number(RSP2025R399)King Saud University,Riyadh,Saudi Arabia.
文摘Simultaneously inducing dual built-in electric fields(EFs)both within a single component and at the heterojunction interface creates a dual-driving force that is crucial for promoting spatial charge separation.This is particularly significant in challenging coupled systems,such as CO_(2)photoreduction integrated with selective oxidation of toluene to benzaldehyde.However,developing such a system is quite challenging and often requires a precise design and engineering.Herein,we demonstrate a unique Ni-CdS@Ni(OH)_(2)heterojunction synthesized via an in-situ self-assembly method.Comprehensive mechanistic and theoretical investigations reveal that the NiCdS@Ni(OH)_(2)heterojunction induces dual electric fields(EFs):an intrinsic polarized electric-field within the CdS lattice from Ni doping and an interfacial electric-field from the growth of ultrathin nanosheets of Ni(OH)_(2)on NiCdS nanorods,enabling efficient spatial charge separation and enhanced redox potential.As proof of concept,the Ni-CdS@Ni(OH)_(2)heterojunction simultaneously exhibits outstanding bifunctional photocatalytic performance,producing CO at a rate of 427μmol g^(-1)h^(-1)and selectively oxidizing toluene to benzaldehyde at a rate of 1476μmol g^(-1)h^(-1)with a selectivity exceeding 85%.This work offers a promising strategy to optimize the utilization of photogenerated carriers in heterojunction photocatalysts,advancing synergistic photocatalytic redox systems.
基金funded by Shanghai Pujiang Program(21PJD022)Hunan Provincial Natural Science Foundation(2023JJ60522).
文摘Balancing the adsorption of OH⁻and 5-hydroxymethylfurfural(HMF)is crucial in optimizing the competing HMF oxidation reaction and oxygen evolution reaction,especially given the polymerization tendency of HMF in alkaline solutions.Herein,we present an innovative approach for rapidly synthesizing a NiFe bimetallic metalorganic framework(MOF)induced by electron-withdrawing carbon quantum dot(EW-CQD)via electron beam irradiation within 2 min.EW-CQD serve as structural regulators,expanding the NiFe-MOF interlayer spacing,increasing reactive site availability,and more effectively balancing the adsorption of OH6(-) and HMF,thereby significantly boosting the oxidation activity of HMF.The resulting EW-CQD-MOF exhibits a low potential of 1.36 V vs.RHE at 10 mA cm^(-2)and maintains excellent durability over 120 h.Comprehensive in situ characterization elucidates the HMF oxidation reaction pathway,showing high selectivity towards 2,5-furandicarboxylic acid(FDCA)under ambient conditions,with an impressive HMF conversion rate of 94%and FDCA selectivity of 96%within 6 h.These findings underscore the critical role of structural optimization and adsorption balance in catalytic performance enhancement and offer valuable insights for designing high-efficiency catalysts,advancing sustainable catalytic processes.
基金supports by Central South University Innovation-Driven Research Programme(2023CXQD038)the Fundamental Research Funds for the Central Universities of Central South University(2025ZZTS0089)supported by the High Performance Computing Center of Central South University.
文摘Anode-free sodium metal batteries(AFSMBs)have gained attention as next-generation storage systems with high energy density and cost-effectiveness.However,non-uniform sodium(Na)deposition and an unsteady solid electrolyte interphase(SEI)lead to dendrite-related issues and severe irreversible Na^(+)plating/stripping,greatly aggravating their cycle deterioration.In this study,we effectively modified the 3D current collector's electronic structure by introducing Zn-N_(x)active sites(Zn-CNF),which enhances lateral Na^(+)diffusion and the Na planar growth,enabling uniform deep Na deposition at an exceptionally high capacity of 10 mA h cm^(-2).Furthermore,the Zn-N_(x)bonds enhance the adsorption capacity of PF6and contribute to forming a stable inorganic-rich SEI layer.Consequently,Zn-CNF with the electronic structure regulation endows an ultra-low nucleation overpotential(8 mV)and ultra-high Coulombic efficiency of 99.94%over 1,600 cycles.Symmetric cells demonstrate stable Na^(+)plating/stripping behavior for more than 4,400 h at 1 mA cm^(-2).Moreover,under high cathode loading(7.97 mg cm^(-2)),the AFSMBs achieve a high energy density of 374 W h kg^(-1)and retain a high discharge capacity of 82.49 mA h g^(-1)with a capacity retention of 80.4%after 120 cycles.This work proposes a viable strategy to achieving high-energy-density AFSMBs.
基金supported by the National Research Foundation of Korea(2022R1C1C2005786,RS-2023-00256106,RS-2023-00207831,RS-2024-00346153).
文摘Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and competition against the hydrogen evolution reaction hinder its practical implementation.To address these,the design of highly active catalysts is critical.Single-atom catalysts(SACs)have shown great potential because of their maximized atom utilization,but their limited stability and low metal loading restrict their performances.On the other hand,dual-atom catalysts(DACs)are atomic catalysts with two metal atoms nearby and offer enhanced electrocatalytic performances by aligning with the N≡N bond to enhance N2 reduction efficiency,potentially overcoming the limitations of SAC.This review discusses recent advances in SACs and more importantly DACs for ENRR,highlighting their advantages,limitations,and the need for advanced characterization techniques to better understand catalyst behavior.The review concludes by underscoring the importance of research to optimize these catalysts for efficient and sustainable nitrogen fixation.
基金supported by the Commercialization Promotion Agency for R&D Outcomes(COMPA)grant funded by the Korea government(Ministry of Science and ICT)(RS-2025-02311658)supported by the Ministry of Education of the Republic of Korea and the National Research Foundation of Korea(NRF-2023R1A2C2008017)Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(NRF-2020R1A6A1A03043435).
文摘Driven by rapid advancements in smart wearable technologies and perovskite photovoltaics,flexible perovskite solar cells(FPSCs)have emerged as highly promising autonomous power sources,poised to transform the next generation of mobile energy systems,portable electronics,and integrated wearable devices.For successful deployment in real-world scenarios,FPSCs must exhibit a combination of key attributes,including high power conversion efficiency,lightweight architecture,environmental robustness,and mechanical adaptability-encompassing flexibility,stretchability,and twistability.This review provides a detailed examination of the evolution,current state,and practical deployment of FPSCs,emphasizing their potential as efficient,portable energy solutions.It investigates advanced strategies for improving environmental resilience and mechanical recoverability,including the engineering of flexible substrates,deposition of high-quality perovskite films,and optimization of charge-selective interfaces.Additionally,it offers a systematic analysis of device design,fabrication protocols,scalable printing techniques,and standardized performance evaluation methods tailored for wearable FPSCs.Recent progress in enhancing the optoelectronic properties and mechanical durability of FPSCs is also critically reviewed.Ultimately,this work delivers a comprehensive perspective on FPSCs from both optoelectronic and mechanical viewpoints,identifies key challenges,and outlines future research pathways toward the seamless integration of FPSCs into multifunctional,next-generation wearable systems.
