Aqueous electrochromic battery(ECB)has shown intense potential for achieving energy storage and saving simultaneously.While tungsten oxide(WO_(3))is the most promising EC material for commercialization,the cycling sta...Aqueous electrochromic battery(ECB)has shown intense potential for achieving energy storage and saving simultaneously.While tungsten oxide(WO_(3))is the most promising EC material for commercialization,the cycling stability of WO_(3)-based aqueous ECBs is currently unsatisfactory due to the repeated phase transition during the redox process and the corrosion by acidic electrolytes.Herein,we present a titanium-tungsten oxide alloy(Ti-WO_(3))with controllable morphology and crystal phase synthesized by a facile hot injection method to overcome the challenges.In contrast to conventional monoclinic WO_(3),the Ti-WO_(3)nanorods can stably maintain their cubic crystal phase during the redox reaction in an acidic electrolyte,thus leading to dramatically enhanced response speed and cycling stability,Specifically,when working in a well-matched hybrid Al^(3+)/Zn^(2+)aqueous electrolyte,our phasetransition-free cubic Ti-WO_(3)exhibits an ultra-high cycling stability(>20000 cycles),fast response speed(3,95 s/4,65 s for bleaching/coloring),as well as excellent discharge areal capacity of 214.5 mA h m^(-2),We further fabricate a fully complementa ry aqueous electrochromic device,for the first time,using a Ti-WO_(3)/Prussian blue device architecture.Remarkably,the complementary ECB shows>10000 stable operation cycles,attesting to the feasibility of our Ti-WO_(3)for practical applications.Our work validates the significance of inhibiting the phase transitions of WO_(3)during the electrochromic process for realizing highly cyclable aqueous ECB,which can possibly provide a generalized design guidance for other high-quality metallic oxides for electrochemical applications.展开更多
Perovskite solar cells(PSCs)have been demonstrated to be one of the most promising technologies in the field of renewable energy.However,the presence of the defects in the perovskite films greatly limits the efficienc...Perovskite solar cells(PSCs)have been demonstrated to be one of the most promising technologies in the field of renewable energy.However,the presence of the defects in the perovskite films greatly limits the efficiency and the stability of the PSCs.The additive engineering is one of the most effective approaches to overcome this problem.Most of the successful additives are extracted from the petroleum-based materials,while the research on the biomass-based additives is still lagging behind.In this paper,two ecofriendly hydroxyalkyl cellulose additives,i.e.,hydroxyethyl cellulose(HEC)and hydroxylpropyl cellulose(HPC),are investigated on the performance of the MAPbl_(3)-based inverted PSCs.Due to the strong interaction between the hydroxyl groups of the cellulose and the divalent cations of the perovskite,these additives enhance the crystal grain orientation and significantly repair the defects of the perovskite films.Working as the additives,these two cellulose derivatives show a strong passivation ability,which significantly reduces the trap density and improves the optoelectronic feature of the PSCs.Compared with the average power conversion efficiency(PCE)of the control device(19.19%),an enhancement of~10%is achieved after the addition of HEC.The optimized device(PCE=21.25%)with a long-term stability(10:80 h,PCE=20.93%)is achieved by the incorporation of the HEC additives into the precursor solution.It is the best performance among the PSCs with the cellulose additives up to now.This research provides a novel choice to develop a cost-effective and renewable additive for the PSCs with high efficiency and excellent long-term stability.展开更多
LiBH_(4) has been considered as one of the most promising energy storage materials with its ultrahigh hydrogen capacity,which can supply hydrogen through hydrolysis process or realize hydrogen-to-electricity conversio...LiBH_(4) has been considered as one of the most promising energy storage materials with its ultrahigh hydrogen capacity,which can supply hydrogen through hydrolysis process or realize hydrogen-to-electricity conversion via anodic oxidation reaction of direct borohydride fuel cells(DBFCs).However,the realization of practical hydrogen applications heavily depends on the effective synthesis of high-purity LiBH_(4) and recycling of the spent fuels(LiBO_(2)·xH_(2)O).The present work demonstrates a convenient and high-efficiency solvent-free strategy for regenerating LiBH_(4) with a maximum yield close to 80%,by retrieving its by-products with MgH_(2) as a reducing agent under ambient conditions.Besides,the hydrogen released from the regeneration course can completely compensate the demand for consumed MgH_(2).The isotopic tracer method reveals that the hydrogen stored in LiBH_(4) comes from both MgH_(2) and coordinated water bound to LiBO_(2).Here,the expensive MgH_(2) can be substituted with the readily available and cost-effective MgH_(2)-Mg mixtures to simplify the regeneration route.Notably,LiBH_(4) catalyzed by CoCl_(2) can stably supply hydrogen to proton exchange membrane fuel cell(PEMFC),thus powering a portable prototype vehicle.By combining hydrogen storage,production and utilization in a closed cycle,this work offers new insights into deploying boron-based hydrides for energy applications.展开更多
Layered magnetic materials,such as MnBi_(2)Te_(4),have drawn much attention owing to their potential for realizing twodimensional(2D)magnetism and possible topological states.Recently,FeBi_(2)Te_(4),which is isostruct...Layered magnetic materials,such as MnBi_(2)Te_(4),have drawn much attention owing to their potential for realizing twodimensional(2D)magnetism and possible topological states.Recently,FeBi_(2)Te_(4),which is isostructural to MnBi_(2)Te_(4),has been synthesized in experiments,but its detailed magnetic ordering and band topology have not been clearly understood yet.Here,based on first-principles calculations,we investigate the magnetic and electronic properties of FeBi_(2)Te_(4)in bulk and 2D forms.We show that different from MnBi_(2)Te_(4),the magnetic ground states of bulk,single-layer,and bilayer FeBi_(2)Te_(4)all favor a 120°noncollinear antiferromagnetic ordering,and they are topologically trivial narrow-gap semiconductors.For the bilayer case,we find that a quantum anomalous Hall effect with a unit Chern number is realized in the ferromagnetic state,which may be achieved in experiment by an external magnetic field or by magnetic proximity coupling.Our work clarifies the physical properties of the new material system of FeBi_(2)Te_(4)and reveals it as a potential platform for studying magnetic frustration down to 2D limit as well as quantum anomalous Hall effect.展开更多
Lead-free double perovskite Cs_(2)AgBiBr_(6) has gained increasing attention recently.However,the power conversion efficiency(PCE)of Cs_(2)AgBiBr_(6) perovskite solar cells(PSCs)is still low compared with their lead-b...Lead-free double perovskite Cs_(2)AgBiBr_(6) has gained increasing attention recently.However,the power conversion efficiency(PCE)of Cs_(2)AgBiBr_(6) perovskite solar cells(PSCs)is still low compared with their lead-based counterparts.Here,by using photoluminescence(PL),time-resolved photoluminescence(TRPL),and ultrafast transient absorption(TA)measurements,the unbalance between the electron and hole in diffusion and transfer,which limits the performance of the Cs_(2)AgBiBr_(6) PSCs,was further revealed.Considering this issue,a strategy of using the mesoporous TiO_(2) electron transport layer(ETL)to construct a bulk heterojunction in Cs_(2)AgBiBr_(6) PSCs was proposed.Consequently,the PCE had improved by over 24%comparing with that only used compact TiO_(2) ETL.Moreover,based on mesoporous TiO_(2),the unencapsulated Cs_(2)AgBiBr_(6) PSCs maintained 90%of their initial performance after approximately 1200 h of storage in a desiccator(humidity~30%).This work gives further understanding of Cs_(2)AgBiBr_(6) perovskite and demonstrates that a proper design of balancing the electron and hole diffusion can improve device performance.展开更多
Metal sulfides are emerging highly active electrocatalysts for the oxygen evolution reaction(OER),but still suffer from the instability caused by their inevitable reconstruction,especially at industrial-level current ...Metal sulfides are emerging highly active electrocatalysts for the oxygen evolution reaction(OER),but still suffer from the instability caused by their inevitable reconstruction,especially at industrial-level current density.Here,it is discovered that Fe-incorporated Ni3S2 nanowires can deliver extraordinary durability with an ultralow potential degradation rate of 0.006 mV/h in alkaline electrolytes made with fresh water and seawater at a benchmark of 500 mA cm^(-2) while meeting the industrial activity requirement for overpotential less than 300 mV(290 mV).Systematic experiments and theoretical simulations suggest that after forming the S-doped NiFeOOH shell to boost intrinsic activity,Fe incorporation effectivelymitigates the reconstruction of the Ni_(3)S_(2) nanowire core by restraining Ni oxidation and S dissolution,justifying the performance.This work highlights the significance of circumventing reconstruction and provides a strategy to explore practical chalcogenides-based OER electrocatalysts.展开更多
Understanding the luminescence mechanisms and regulating the emission centers of carbon dots(CDs)are important for advancing their related applications.In this work,we systematically investigate the formation processe...Understanding the luminescence mechanisms and regulating the emission centers of carbon dots(CDs)are important for advancing their related applications.In this work,we systematically investigate the formation processes of multi-emission centers in CDs synthesized through a bottom-up approach by controlling the solvothermal reaction temperature.CDs synthesized at a lower temperature(140℃,140-CDs)exhibit smaller particle sizes(3–4 nm)with dominant green–yellow emission,while CDs synthesized at a higher temperature(180℃,180-CDs)exhibit larger particle sizes(8–9 nm)with enhanced red emission and emerging near-infrared(NIR)emission.The green–yellow emission and red emission originate from the core state and the surface-related state,respectively,and the emissions could be regulated by temperature-controlled dehydration and carbonization processes.The clear NIR emission center in 180-CDs is attributable to the increased content of radical defects in the cores during the increased dehydration and carbonization processes during higher-temperature solvothermal treatment.展开更多
We examine the electronic and transport properties of a new phase PdSe monolayer with a puckered structure calculated by first-principles and Boltzmann transport equation.The spin−orbit coupling is found to play a neg...We examine the electronic and transport properties of a new phase PdSe monolayer with a puckered structure calculated by first-principles and Boltzmann transport equation.The spin−orbit coupling is found to play a negligible effect on the electronic properties of PdSe monolayer.The lattice thermal conductivity of PdSe monolayer exhibits remarkable anisotropic characteristic due to anisotropic phonon group velocity along different directions and its intrinsic structure anisotropy.The compromised electronic mobility despite a relatively low thermal conduction results in a moderate ZT value but significantly anisotropic thermoelectric performance in single-layer PdSe.The present work suggests that the remarkable thermal transport anisotropy of PdSe monolayer can be used for thermal management,and enhance the scope of possibilities for heat flow manipulation in PdSe based devices.The sizeable puckered cages and wiggling lattice implies it an ideal platform for ionic and molecular engineering for thermoelectronic applications.展开更多
The stabilization of the formamidinium lead iodide(FAPbI_(3))structure is pivotal for the development of efficient photovoltaic devices.Employing two-dimensional(2D)layers to passivate the threedimensional(3D)perovski...The stabilization of the formamidinium lead iodide(FAPbI_(3))structure is pivotal for the development of efficient photovoltaic devices.Employing two-dimensional(2D)layers to passivate the threedimensional(3D)perovskite is essential for maintaining the a-phase of FAPbI_(3) and enhancing the power conversion efficiency(PCE)of perovskite solar cells(PSCs).However,the role of bulky ligands in the phase management of 2D perovskites,crucial for the stabilization of FAPbI_(3),has not yet been elucidated.In this study,we synthesized nanoscale 2D perovskite capping crusts with<n>=1 and 2 Ruddlesden-Popper(RP)perovskite layers,respectively,which form a type-Ⅱ 2D/3D heterostructure.This heterostructure stabilizes the a-phase of FAPbI_(3),and facilitates ultrafast carrier extraction from the 3D perovskite network to transport contact layer.We introduced tri-fluorinated ligands to mitigate defects caused by the halide vacancies and uncoordinated Pb^(2+)ions,thereby reducing nonradiative carrier recombination and extending carrier lifetime.The films produced were incorporated into PSCs that not only achieved a PCE of 25.39%but also maintained 95%of their initial efficiency after 2000 h of continuous light exposure without encapsulation.These findings underscore the effectiveness of a phase-pure 2D/3D heterostructure-terminated film in inhibiting phase transitions passivating the iodide anion vacancy defects,facilitating the charge carrier extraction,and boosting the performance of optoelectronic devices.展开更多
Aluminum-metal batteries show great potential as next-generation energy storage due to their abundant resources and intrinsic safety.However,the crucial limitations of metallic Al anodes,such as dendrite and corrosion...Aluminum-metal batteries show great potential as next-generation energy storage due to their abundant resources and intrinsic safety.However,the crucial limitations of metallic Al anodes,such as dendrite and corrosion problems in conventional aluminum-metal batteries,remain challenging and elusive.Here,we report a novel electrodeposition strategy to prepare an optimized 3D Al anode on carbon cloth with an uniform deposition morphology,low local current density,and mitigatory volume change.The symmetrical cells with the 3D Al anode show superior stable cycling(>450 h)and low-voltage hysteresis(~170 mV)at 0.5 mA cm^(−2).High reversibility(~99.7%)is achieved for the Al plating/stripping.The graphite||Al‐4/CC full batteries show a long lifespan of 800 cycles with 54 mAh g^(−1) capacity at a high current density of 1000 mA g^(−1),benefiting from the high capacitive-controlled distribution.This study proposes a novel strategy to design 3D Al anodes for metallic-Al-based batteries by eliminating the problems of planar Al anodes and realizing the potential applications of aluminum-graphite batteries.展开更多
All-inorganic metal-halide CsPbBr_(3)perovskite has emerged as an attractive photovoltaic material for its outstanding environmental stability.However,due to the wide bandgap,the performance of CsPbBr_(3)perovskite so...All-inorganic metal-halide CsPbBr_(3)perovskite has emerged as an attractive photovoltaic material for its outstanding environmental stability.However,due to the wide bandgap,the performance of CsPbBr_(3)perovskite solar cells(PSCs)is limited,especially for the short-circuit current density(J_(SC)).In this issue of Energy&Environmental Materials,Guo et al.employed Nb-doped SnO_(2)as electron transporting layers(ETLs),which could greatly improve the J_(SC)of the PSCs based on all-inorganic CsPbBr_(3).展开更多
We have grown a YCrO_(3)single crystal by the floating-zone method and studied its temperature-dependent crystalline structure and magnetization by x-ray powder diffraction and PPMS DynaCool measurements.All diffracti...We have grown a YCrO_(3)single crystal by the floating-zone method and studied its temperature-dependent crystalline structure and magnetization by x-ray powder diffraction and PPMS DynaCool measurements.All diffraction patterns were well indexed by an orthorhombic structure with space group of Pbnm(No.62).From 36 K to 300 K,no structural phase transition occurs in the pulverized YCrO_(3)single crystal.The antiferromagnetic phase transition temperature was determined as T_(N)=141.58(5)K by the magnetization versus temperature measurements.We found weak ferromagnetic behavior in the magnetic hysteresis loops below TN.Especially,we demonstrated that the antiferromagnetism and weak ferromagnetism appear simultaneously upon cooling.The lattice parameters(a,b,c,and V)deviate downward from the Grüneisen law,displaying an anisotropic magnetostriction effect.We extracted temperature variation of the local distortion parameterΔ.Compared to theΔvalue of Cr ions,Y,O1,and O2 ions show one order of magnitude largerΔvalues indicative of much stronger local lattice distortions.Moreover,the calculated bond valence states of Y and O2 ions have obvious subduction charges.展开更多
Hydrolysis of Mg-based materials is considered as a potential means of safe and convenient real-time control of H_(2)release,enabling efficient loading,discharge and utilization of hydrogen in portable electronic devi...Hydrolysis of Mg-based materials is considered as a potential means of safe and convenient real-time control of H_(2)release,enabling efficient loading,discharge and utilization of hydrogen in portable electronic devices.At present work,the hydrogen generation properties of MgLi-graphite composites were evaluated for the first time.The MgLi-graphite composites with different doping amounts of expanded graphite(abbreviated as EG hereinafter)were synthesized through ball milling and the hydrogen behaviors of the composites were investigated in chloride solutions.Among the above doping systems,the 10 wt.%EG-doped MgLi exhibited the best hydrogen performance in MgCl_(2)solutions.In particular,the 22 h-milled MgLi-10 wt.%EG composites possessed both desirable hydrogen conversion and rapid reaction kinetics,delivering a hydrogen yield of 966 mL H_(2)g^(-1)within merely 2 min and a maximum hydrogen generation rate of 1147 mL H_(2)min^(-1)g^(-1),as opposed to the sluggish kinetics in the EG-free composites.Moreover,the EG-doped MgLi showed superior air-stable ability even under a 75 RH%ambient atmosphere.For example,the 22 h-milled MgLi-10 wt.%EG composites held a fuel conversion of 89%after air exposure for 72 h,rendering it an advantage for Mg-based materials to safely store and transfer in practical applications.The similar favorable hydrogen performance of MgLi-EG composites in(simulate)seawater may shed light on future development of hydrogen generation technologies.展开更多
A versatile sensing platform employing inorganic MoS_(2) nanoflowers and organic poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)has been investigated to develop the resistive and capacitive force-...A versatile sensing platform employing inorganic MoS_(2) nanoflowers and organic poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)has been investigated to develop the resistive and capacitive force-sensitive devices.The microstructure of the sensing layer heightens the sensitivity and response time of the dual-mode pressure sensors by augmenting electron pathways and inner stress in response to mechanical stimuli.Consequently,the capacitive and resistive sensors exhibit sensitivities of 0.37 and 0.12 kPa^(-1),respectively,while demonstrating a remarkable response time of approximately 100 ms.Furthermore,it is noteworthy that the PEDOT:PSS layer exhibits excellent adhesion to polydimethylsiloxane(PDMS)substrates,which contributes to the development of highly robust force-sensitive sensors capable of enduring more than 10000loading/unloading cycles.The combination of MoS_(2)/PEDOT:PSS layers in these dual-mode sensors has shown promising results in detecting human joint movements and subtle physiological signals.Notably,the sensors have achieved a remarkable precision rate of 98%in identifying target objects.These outcomes underscore the significant potential of these sensors for integration into applications such as electronic skin and human-machine interaction.展开更多
Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn ...Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn are prone to react with the hydroxyl ions in alkaline electrolyte upon electrochemical cycling and separates on the surface of spinel to reconstruct into d-MnO_(2) nanosheets irreversibly,thus results in a change of the reaction mechanism with Kþion intercalation.However,the low capacity has greatly limited its practical application.Herein,we found that the tetrahedrally-coordinated Co_(2) þions were leached when MnCo_(2)_(4) was equilibrated in 1 mol L^(-1) HCl solution,leading to the formation of layered CoOOH on MnCo_(2)_(4) surface which is originated from the covalency competition induced selective breakage of the CoT–O bond in CoT–O–CoO and subsequent rearrangement of free Co_(6) octahedra.The as-formed CoOOH is stable upon cycling in alkaline electrolyte,exhibits conversion reaction mechanism with facile proton diffusion and is free of massive structural evolution,thus enables utilization of the bulk electrode material and realizes enhanced specific capacity as well as facilitated charge transfer and ion diffusion.In general,our work not only offers a feasible approach to deliberate modification of MnCo_(2)_(4)'s surface structure,but also provides an in-depth understanding of its charge storage mechanism,which enables rational design of the spinel oxides with promising charge storage properties.展开更多
In the era of smart agriculture,the precise labeling and recording of growth information in plants pose challenges for modern agricultural production.This study introduces strontium aluminate particles coated with H_(...In the era of smart agriculture,the precise labeling and recording of growth information in plants pose challenges for modern agricultural production.This study introduces strontium aluminate particles coated with H_(3)PO_(4)as luminescent labels capable of spatial embedding within plants for information encoding and storage during growth.The encapsulation with H_(3)PO_(4)imparts stability and enhanced luminescence to SrAl_(2)O_(4):Eu^(2+),Dy^(3+)(SAO).Using SAO@H_(3)PO_(4)as a low-damage luminescent label,we implement its delivery into plants through microneedles(MNs)patches.The embedded SAO@H_(3)PO_(4)within plants exhibits sustained and unaltered high signal-to-noise afterglow emission,with luminous intensity remaining at approximately 78%of the original for 27 days.To cater to diverse information recording needs,MNs of various geometric shapes are designed for loading SAO@H3PO4,and the luminescent signals in different shapes can be accurately identified through a designed program,the corresponding information can be conveniently viewed on a computer.Additionally,inspired by binary information concepts,MNs patches with specific arrangements of luminescent and non-luminescent points are created,resulting in varied luminescent MNs arrays on leaves.An advanced camera system with a tailored program accurately identifies and maps the labels to the corresponding recorded information.These findings showcase the potential of low-damage luminescent labels within plants,paving the way for convenient and widespread storage of plant growth information.展开更多
Simultaneously enhancing the reaction kinetics,mass transport,and gas release during alkaline hydrogen evolution reaction(HER)is critical to minimizing the reaction polarization resistance,but remains a big challenge....Simultaneously enhancing the reaction kinetics,mass transport,and gas release during alkaline hydrogen evolution reaction(HER)is critical to minimizing the reaction polarization resistance,but remains a big challenge.Through rational design of a hierarchical multiheterogeneous three-dimensionally(3D)ordered macroporous Mo_(2)C-embedded nitrogen-doped carbon with ultrafine Ru nanoclusters anchored on its surface(OMS Mo_(2)C/NC-Ru),we realize both electronic and morphologic engineering of the catalyst to maximize the electrocatalysis performance.The formed Ru-NC heterostructure shows regulative electronic states and optimized adsorption energy with the intermediate H*,and the Mo_(2)C-NC heterostructure accelerates the Volmer reaction due to the strong water dissociation ability as confirmed by theoretical calculations.Consequently,superior HER activity in alkaline solution with an extremely low overpotential of 15.5 mV at 10 mAcm^(−2)with the mass activity more than 17 times higher than that of the benchmark Pt/C,an ultrasmall Tafel slope of 22.7 mV dec−1,and excellent electrocatalytic durability were achieved,attributing to the enhanced mass transport and favorable gas release process endowed from the unique OMS Mo_(2)C/NC-Ru structure.By oxidizing OMS Mo_(2)C/NC-Ru into OMS MoO_(3)-RuO_(2)catalyst,it can also be applied as efficient oxygen evolution electrocatalyst,enabling the construction of a quasi-symmetric electrolyzer for overall water splitting.Such a device's performance surpassed the state-of-the-art Pt/C||RuO2 electrolyzer.This study provides instructive guidance for designing 3D-ordered macroporous multicomponent catalysts for efficient catalytic applications.展开更多
Fluorescent carbon dots(CDs)have recently become a research hotspot in multidisciplinary fields owing to their distinctive advantages,including outstanding photoluminescence properties,high biocompatibility,low toxici...Fluorescent carbon dots(CDs)have recently become a research hotspot in multidisciplinary fields owing to their distinctive advantages,including outstanding photoluminescence properties,high biocompatibility,low toxicity,and abundant raw materials.Among the promising CDs,narrow‐bandwidth emissive CDs with high color purity have emerged as a rising star in recent years because of their significant potential applications in bioimaging,information sensing,and photoelectric displays.In this review,the state-of-the-art advances of narrow-bandwidth emissive CDs are systematically summarized,and the factors influencing the emission bandwidth,preparation methods,and applications of narrow-bandwidth emissive CDs are described in detail.Besides,existing challenges and future perspectives for achieving high-performance narrow-bandwidth emissive CDs are also discussed.This overview paper is expected to generate more interest and promote the rapid development of this significant research area.展开更多
The thermoelectric(TE)materials and corresponding TE devices can achieve direct heat-to-electricity conversion,thus have wide applications in heat energy harvesting(power generator),wearable electronics and local cool...The thermoelectric(TE)materials and corresponding TE devices can achieve direct heat-to-electricity conversion,thus have wide applications in heat energy harvesting(power generator),wearable electronics and local cooling.In recent years,aerogel-based TE materials have received considerable attention and have made remarkable progress because of their unique structural,electrical and thermal properties.In this review,the recent progress in both organic,inorganic,and composite/hybrid TE aerogels is systematically summarized,including the main constituents,preparation method,TE performance,as well as factors affecting the TE performance and the corresponding mechanism.Moreover,two typical aerogel-based TE devices/generators are compared and analyzed in terms of assembly modes and output performance.Finally,the present challenges and some tentative suggestions for future research prospects are provided in conclusion.展开更多
The poor cycling stability of graphite in traditional ester electrolyte limits its applications as anodes for potassium ion batteries(KIBs).Herein,we demonstrate that the introduction of cyclic ether co-solvents into ...The poor cycling stability of graphite in traditional ester electrolyte limits its applications as anodes for potassium ion batteries(KIBs).Herein,we demonstrate that the introduction of cyclic ether co-solvents into ester electrolytes can remarkably enhance the cycling stability of graphite anodes.The graphite anode in ester electrolyte with cyclic ether could achieve a reversible capacity of 196.1 m Ah g^(-1) after 100 cycles at 0.3 C(1 C=280 m A g^(-1)),about three times higher than those in ester electrolytes with or without linear ether.Compared with the SEI formed in ester electrolytes,the addition of tetrahydrofuran promotes the generation of K_(2)CO_(3) and ethylene oxide oligomers(PEO),of which the K_(2)CO_(3) is expected to be more conductive and PEO is mechanically robust.The more uniform,conductive and stable solid electrolyte interphases(SEIs)on graphite in electrolytes with cyclic ethers contribute to the enhancement of the electrochemical performances of graphite.This work provides a novel design of commercialized electrolytes to achieve high-performance anodes for KIBs,which potentially accelerates the development of KIBs.展开更多
基金funded by the Science and Technology Development Fund,Macao SAR(File no.0052/2021/AGJ,0027/2023/AMJ,0083/2023/ITP2 and 0107/2023/AFJ)the Multi-Year Research Grants(MYRG2022-00063-IAPME,MYRG-GRG2023-00230-IAPME-UMDF)from the University of Macao+1 种基金the Guangdong Science and Technology Plan(2022A0505020022)the Major Science and Technology Research and Development Project of Jiangxi Province(20223AAE01003)。
文摘Aqueous electrochromic battery(ECB)has shown intense potential for achieving energy storage and saving simultaneously.While tungsten oxide(WO_(3))is the most promising EC material for commercialization,the cycling stability of WO_(3)-based aqueous ECBs is currently unsatisfactory due to the repeated phase transition during the redox process and the corrosion by acidic electrolytes.Herein,we present a titanium-tungsten oxide alloy(Ti-WO_(3))with controllable morphology and crystal phase synthesized by a facile hot injection method to overcome the challenges.In contrast to conventional monoclinic WO_(3),the Ti-WO_(3)nanorods can stably maintain their cubic crystal phase during the redox reaction in an acidic electrolyte,thus leading to dramatically enhanced response speed and cycling stability,Specifically,when working in a well-matched hybrid Al^(3+)/Zn^(2+)aqueous electrolyte,our phasetransition-free cubic Ti-WO_(3)exhibits an ultra-high cycling stability(>20000 cycles),fast response speed(3,95 s/4,65 s for bleaching/coloring),as well as excellent discharge areal capacity of 214.5 mA h m^(-2),We further fabricate a fully complementa ry aqueous electrochromic device,for the first time,using a Ti-WO_(3)/Prussian blue device architecture.Remarkably,the complementary ECB shows>10000 stable operation cycles,attesting to the feasibility of our Ti-WO_(3)for practical applications.Our work validates the significance of inhibiting the phase transitions of WO_(3)during the electrochromic process for realizing highly cyclable aqueous ECB,which can possibly provide a generalized design guidance for other high-quality metallic oxides for electrochemical applications.
基金the National Natural Science Foundation of China(61935017,62175268,21674123,31700507)Fujian Natural Science Foundation for Distinguished Young Scholars(2020J06039)+4 种基金Project of“100 People Planning in Fujian Province,”Fujian Provincial Department of Finance for the research of organic photovoltaic solar cell(Kle20001A)the Science and Technology Development Fund,Macao SAR(File no.FDCT-0044/2020/A1,0082/2021/A2)UM's research fund(File no.MYRG2020-00151-IAPME)Natural Science Foundation of Guangdong Province,China(2019A1515012186)Shenzhen-Hong Kong-Macao Science and Technology Innovation Project(Category C)(SGDX2020110309360100).
文摘Perovskite solar cells(PSCs)have been demonstrated to be one of the most promising technologies in the field of renewable energy.However,the presence of the defects in the perovskite films greatly limits the efficiency and the stability of the PSCs.The additive engineering is one of the most effective approaches to overcome this problem.Most of the successful additives are extracted from the petroleum-based materials,while the research on the biomass-based additives is still lagging behind.In this paper,two ecofriendly hydroxyalkyl cellulose additives,i.e.,hydroxyethyl cellulose(HEC)and hydroxylpropyl cellulose(HPC),are investigated on the performance of the MAPbl_(3)-based inverted PSCs.Due to the strong interaction between the hydroxyl groups of the cellulose and the divalent cations of the perovskite,these additives enhance the crystal grain orientation and significantly repair the defects of the perovskite films.Working as the additives,these two cellulose derivatives show a strong passivation ability,which significantly reduces the trap density and improves the optoelectronic feature of the PSCs.Compared with the average power conversion efficiency(PCE)of the control device(19.19%),an enhancement of~10%is achieved after the addition of HEC.The optimized device(PCE=21.25%)with a long-term stability(10:80 h,PCE=20.93%)is achieved by the incorporation of the HEC additives into the precursor solution.It is the best performance among the PSCs with the cellulose additives up to now.This research provides a novel choice to develop a cost-effective and renewable additive for the PSCs with high efficiency and excellent long-term stability.
基金This work was financially supported by the National Natural Science Foundation of China Projects(Nos.51771075)the National Key R&D Program of China(No.2018YFB1502101)+2 种基金the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(No.NSFC51621001)by the Project Supported by Nat-ural Science Foundation of Guangdong Province of China(2016A030312011)Shao acknowledges support from Macao Science and Technology Development Fund(FDCT)(Project No.:0062/2018/A2 and 0019/2019/AGJ).
文摘LiBH_(4) has been considered as one of the most promising energy storage materials with its ultrahigh hydrogen capacity,which can supply hydrogen through hydrolysis process or realize hydrogen-to-electricity conversion via anodic oxidation reaction of direct borohydride fuel cells(DBFCs).However,the realization of practical hydrogen applications heavily depends on the effective synthesis of high-purity LiBH_(4) and recycling of the spent fuels(LiBO_(2)·xH_(2)O).The present work demonstrates a convenient and high-efficiency solvent-free strategy for regenerating LiBH_(4) with a maximum yield close to 80%,by retrieving its by-products with MgH_(2) as a reducing agent under ambient conditions.Besides,the hydrogen released from the regeneration course can completely compensate the demand for consumed MgH_(2).The isotopic tracer method reveals that the hydrogen stored in LiBH_(4) comes from both MgH_(2) and coordinated water bound to LiBO_(2).Here,the expensive MgH_(2) can be substituted with the readily available and cost-effective MgH_(2)-Mg mixtures to simplify the regeneration route.Notably,LiBH_(4) catalyzed by CoCl_(2) can stably supply hydrogen to proton exchange membrane fuel cell(PEMFC),thus powering a portable prototype vehicle.By combining hydrogen storage,production and utilization in a closed cycle,this work offers new insights into deploying boron-based hydrides for energy applications.
基金funding support from the Singapore MOE Ac RF 308 Tier 2(Grant No.T2EP50220-0026)funding support from Shandong Provincial Natural Science Foundation(Grant No.ZR2023QA012)+3 种基金the Special Fund-ing in the Project of Qilu Young Scholar Program of Shandong Universityfunding support from Australian Research Council Future Fellowship(Grant No.FT220100290)funding support from the AINSE postgraduate awardfunding support from the Research and Development Administration Office at the University of Macao(Grants Nos.MYRG2022-00088-IAPME and SRG2021-00003-IAPME)。
文摘Layered magnetic materials,such as MnBi_(2)Te_(4),have drawn much attention owing to their potential for realizing twodimensional(2D)magnetism and possible topological states.Recently,FeBi_(2)Te_(4),which is isostructural to MnBi_(2)Te_(4),has been synthesized in experiments,but its detailed magnetic ordering and band topology have not been clearly understood yet.Here,based on first-principles calculations,we investigate the magnetic and electronic properties of FeBi_(2)Te_(4)in bulk and 2D forms.We show that different from MnBi_(2)Te_(4),the magnetic ground states of bulk,single-layer,and bilayer FeBi_(2)Te_(4)all favor a 120°noncollinear antiferromagnetic ordering,and they are topologically trivial narrow-gap semiconductors.For the bilayer case,we find that a quantum anomalous Hall effect with a unit Chern number is realized in the ferromagnetic state,which may be achieved in experiment by an external magnetic field or by magnetic proximity coupling.Our work clarifies the physical properties of the new material system of FeBi_(2)Te_(4)and reveals it as a potential platform for studying magnetic frustration down to 2D limit as well as quantum anomalous Hall effect.
基金financial support from Macao Science and Technology Development Fund,China(FDCT-0044/2020/A1,FDCT-091/2017/A2,FDCT-014/2017/AMJ)University of Macao Research Grant,China(MYRG2018-00148-IAPME,MYRG2018-00142-IAPME)from University of Macao+2 种基金the Natural Science Foundation of China,China(91733302,61935017)Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials(2019B121205002)Natural Science Foundation of Guangdong Province,China(2019A1515012186).
文摘Lead-free double perovskite Cs_(2)AgBiBr_(6) has gained increasing attention recently.However,the power conversion efficiency(PCE)of Cs_(2)AgBiBr_(6) perovskite solar cells(PSCs)is still low compared with their lead-based counterparts.Here,by using photoluminescence(PL),time-resolved photoluminescence(TRPL),and ultrafast transient absorption(TA)measurements,the unbalance between the electron and hole in diffusion and transfer,which limits the performance of the Cs_(2)AgBiBr_(6) PSCs,was further revealed.Considering this issue,a strategy of using the mesoporous TiO_(2) electron transport layer(ETL)to construct a bulk heterojunction in Cs_(2)AgBiBr_(6) PSCs was proposed.Consequently,the PCE had improved by over 24%comparing with that only used compact TiO_(2) ETL.Moreover,based on mesoporous TiO_(2),the unencapsulated Cs_(2)AgBiBr_(6) PSCs maintained 90%of their initial performance after approximately 1200 h of storage in a desiccator(humidity~30%).This work gives further understanding of Cs_(2)AgBiBr_(6) perovskite and demonstrates that a proper design of balancing the electron and hole diffusion can improve device performance.
基金the National Key Research and Development Program of China(grant no.2021YFA1501002)National Natural Science Foundation of China(grant nos.22025208,22075300,and 21902162)+1 种基金DNL Cooperation Fund,CAS(grant no.DNL202008)Chinese Academy of Sciences,and Australian Research Council(grant no.DE220100746).
文摘Metal sulfides are emerging highly active electrocatalysts for the oxygen evolution reaction(OER),but still suffer from the instability caused by their inevitable reconstruction,especially at industrial-level current density.Here,it is discovered that Fe-incorporated Ni3S2 nanowires can deliver extraordinary durability with an ultralow potential degradation rate of 0.006 mV/h in alkaline electrolytes made with fresh water and seawater at a benchmark of 500 mA cm^(-2) while meeting the industrial activity requirement for overpotential less than 300 mV(290 mV).Systematic experiments and theoretical simulations suggest that after forming the S-doped NiFeOOH shell to boost intrinsic activity,Fe incorporation effectivelymitigates the reconstruction of the Ni_(3)S_(2) nanowire core by restraining Ni oxidation and S dissolution,justifying the performance.This work highlights the significance of circumventing reconstruction and provides a strategy to explore practical chalcogenides-based OER electrocatalysts.
基金financially supported by the Science and Technology Development Fund of Macao SAR(Nos.0128/2020/A3,0131/2020/A3,0007/2021/AKP,006/2022/ALC and 0139/2022/A3)fund from the University of Macao(No.MYRG2020–00164-IAPME)+1 种基金the Research and Development Grant for Chair Professor Fund from the University of Macao(No.CPG2020–00026-IAPME)the Shenzhen-Hong Kong-Macao Science and Technology Innovation Project(Category C)(Nos.SGDX20210823103803021,EF029/IAPME-QSN/2022/SZSTIC)。
文摘Understanding the luminescence mechanisms and regulating the emission centers of carbon dots(CDs)are important for advancing their related applications.In this work,we systematically investigate the formation processes of multi-emission centers in CDs synthesized through a bottom-up approach by controlling the solvothermal reaction temperature.CDs synthesized at a lower temperature(140℃,140-CDs)exhibit smaller particle sizes(3–4 nm)with dominant green–yellow emission,while CDs synthesized at a higher temperature(180℃,180-CDs)exhibit larger particle sizes(8–9 nm)with enhanced red emission and emerging near-infrared(NIR)emission.The green–yellow emission and red emission originate from the core state and the surface-related state,respectively,and the emissions could be regulated by temperature-controlled dehydration and carbonization processes.The clear NIR emission center in 180-CDs is attributable to the increased content of radical defects in the cores during the increased dehydration and carbonization processes during higher-temperature solvothermal treatment.
基金the National Natural Science Foundation of China(Grant No.22022309)the Natural Science Foundation of Guangdong Province,China(No.2021A1515010024)+1 种基金the University of Macao(Nos.SRG2019-00179-IAPME and MYRG2020-00075-IAPME)the Science and Technology Development Fund from Macao SAR(No.FDCT-0163/2019/A3).
文摘We examine the electronic and transport properties of a new phase PdSe monolayer with a puckered structure calculated by first-principles and Boltzmann transport equation.The spin−orbit coupling is found to play a negligible effect on the electronic properties of PdSe monolayer.The lattice thermal conductivity of PdSe monolayer exhibits remarkable anisotropic characteristic due to anisotropic phonon group velocity along different directions and its intrinsic structure anisotropy.The compromised electronic mobility despite a relatively low thermal conduction results in a moderate ZT value but significantly anisotropic thermoelectric performance in single-layer PdSe.The present work suggests that the remarkable thermal transport anisotropy of PdSe monolayer can be used for thermal management,and enhance the scope of possibilities for heat flow manipulation in PdSe based devices.The sizeable puckered cages and wiggling lattice implies it an ideal platform for ionic and molecular engineering for thermoelectronic applications.
基金the Science and Technology Development Fund,Macao SAR(FDCT-0082/2021/A2,0010/2022/AMJ,0060/2023/RIA1,0136/2022/A3,006/2022/ALC,and EF044/IAPME-HG/2022/MUST)UM’s research fund(MYRG2022-00241IAPME,MYRG-GRG2023-00065-IAPME-UMDF,and MYRGCRG2022-00009-FHS)+8 种基金the research fund from Wuyi University(EF38/IAPME-XGC/2022/WYU)Shaanxi Fundamental Science Research Project for Mathematics and Physics(22JSY015 and 23JSY005)Shaanxi Province science and technology activities for overseas students selected funding project(2023015)the State Key Laboratory for Strength and Vibration of Mechanical Structures(SV2023-KF-18)Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems(2023B1212010003)the China Fundamental Research Funds for the Central Universities,Young Talent Fund of Xi’an Association for Science and Technology(959202313020)the project of Innovative Team of Shaanxi Province(2020TD-001)the Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(NY223053)the National Natural Science Foundation of China(61935017,62105292,62175268,62288102 and 62304111)。
文摘The stabilization of the formamidinium lead iodide(FAPbI_(3))structure is pivotal for the development of efficient photovoltaic devices.Employing two-dimensional(2D)layers to passivate the threedimensional(3D)perovskite is essential for maintaining the a-phase of FAPbI_(3) and enhancing the power conversion efficiency(PCE)of perovskite solar cells(PSCs).However,the role of bulky ligands in the phase management of 2D perovskites,crucial for the stabilization of FAPbI_(3),has not yet been elucidated.In this study,we synthesized nanoscale 2D perovskite capping crusts with<n>=1 and 2 Ruddlesden-Popper(RP)perovskite layers,respectively,which form a type-Ⅱ 2D/3D heterostructure.This heterostructure stabilizes the a-phase of FAPbI_(3),and facilitates ultrafast carrier extraction from the 3D perovskite network to transport contact layer.We introduced tri-fluorinated ligands to mitigate defects caused by the halide vacancies and uncoordinated Pb^(2+)ions,thereby reducing nonradiative carrier recombination and extending carrier lifetime.The films produced were incorporated into PSCs that not only achieved a PCE of 25.39%but also maintained 95%of their initial efficiency after 2000 h of continuous light exposure without encapsulation.These findings underscore the effectiveness of a phase-pure 2D/3D heterostructure-terminated film in inhibiting phase transitions passivating the iodide anion vacancy defects,facilitating the charge carrier extraction,and boosting the performance of optoelectronic devices.
基金This study was funded by the Science and Technology Development Fund,Macao SAR(File no.0191/2017/A3,0041/2019/A1,0046/2019/AFJ,0021/2019/AIR)the University of Macao(File no.MYRG2017-00216-FST and MYRG2018-00192-IAPME)+2 种基金the UEA funding,Science and Technology Program of Guangzhou(2019050001)the National Key Research and Development Program of China(2019YFE0198000)Fuming Chen acknowledges the Pearl River Talent Program(2019QN01L951).
文摘Aluminum-metal batteries show great potential as next-generation energy storage due to their abundant resources and intrinsic safety.However,the crucial limitations of metallic Al anodes,such as dendrite and corrosion problems in conventional aluminum-metal batteries,remain challenging and elusive.Here,we report a novel electrodeposition strategy to prepare an optimized 3D Al anode on carbon cloth with an uniform deposition morphology,low local current density,and mitigatory volume change.The symmetrical cells with the 3D Al anode show superior stable cycling(>450 h)and low-voltage hysteresis(~170 mV)at 0.5 mA cm^(−2).High reversibility(~99.7%)is achieved for the Al plating/stripping.The graphite||Al‐4/CC full batteries show a long lifespan of 800 cycles with 54 mAh g^(−1) capacity at a high current density of 1000 mA g^(−1),benefiting from the high capacitive-controlled distribution.This study proposes a novel strategy to design 3D Al anodes for metallic-Al-based batteries by eliminating the problems of planar Al anodes and realizing the potential applications of aluminum-graphite batteries.
基金the Science and Technology Development Fund,Macao SAR(File no.FDCT-0044/2020/A1,FDCT-091/2017/A2,FDCT-014/2017/AMJ)UM’s research fund(File no.MYRG2018-00148-IAPME)+2 种基金the Natural Science Foundation of China(61935017)Natural Science Foundation of Guangdong Province,China(2019A1515012186)Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials(2019B121205002)
文摘All-inorganic metal-halide CsPbBr_(3)perovskite has emerged as an attractive photovoltaic material for its outstanding environmental stability.However,due to the wide bandgap,the performance of CsPbBr_(3)perovskite solar cells(PSCs)is limited,especially for the short-circuit current density(J_(SC)).In this issue of Energy&Environmental Materials,Guo et al.employed Nb-doped SnO_(2)as electron transporting layers(ETLs),which could greatly improve the J_(SC)of the PSCs based on all-inorganic CsPbBr_(3).
基金the opening project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure(Grant No.SKL201907SIC)Science and Technology Development Fund,Macao SAR,China(File Nos.0090/2021/A2 and 0051/2019/AFJ)+2 种基金Guangdong Basic and Applied Basic Research Foundation,China(GuangdongDongguan Joint Fund No.2020B1515120025)University of Macao(MYRG2020-00278-IAPME and EF030/IAPMELHF/2021/GDSTIC)Guangdong-Hong Kong-Macao Joint Laboratory for Neutron Scattering Science and Technology(Grant No.2019B121205003)。
文摘We have grown a YCrO_(3)single crystal by the floating-zone method and studied its temperature-dependent crystalline structure and magnetization by x-ray powder diffraction and PPMS DynaCool measurements.All diffraction patterns were well indexed by an orthorhombic structure with space group of Pbnm(No.62).From 36 K to 300 K,no structural phase transition occurs in the pulverized YCrO_(3)single crystal.The antiferromagnetic phase transition temperature was determined as T_(N)=141.58(5)K by the magnetization versus temperature measurements.We found weak ferromagnetic behavior in the magnetic hysteresis loops below TN.Especially,we demonstrated that the antiferromagnetism and weak ferromagnetism appear simultaneously upon cooling.The lattice parameters(a,b,c,and V)deviate downward from the Grüneisen law,displaying an anisotropic magnetostriction effect.We extracted temperature variation of the local distortion parameterΔ.Compared to theΔvalue of Cr ions,Y,O1,and O2 ions show one order of magnitude largerΔvalues indicative of much stronger local lattice distortions.Moreover,the calculated bond valence states of Y and O2 ions have obvious subduction charges.
基金financially supported by the National Natural Science Foundation of China Projects(Nos.51771075)the National Key R&D Program of China(No.2018YFB1502101)+1 种基金the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(No.NSFC51621001)the Project Supported by Natural Science Foundation of Guangdong Province of China(2016A030312011)
文摘Hydrolysis of Mg-based materials is considered as a potential means of safe and convenient real-time control of H_(2)release,enabling efficient loading,discharge and utilization of hydrogen in portable electronic devices.At present work,the hydrogen generation properties of MgLi-graphite composites were evaluated for the first time.The MgLi-graphite composites with different doping amounts of expanded graphite(abbreviated as EG hereinafter)were synthesized through ball milling and the hydrogen behaviors of the composites were investigated in chloride solutions.Among the above doping systems,the 10 wt.%EG-doped MgLi exhibited the best hydrogen performance in MgCl_(2)solutions.In particular,the 22 h-milled MgLi-10 wt.%EG composites possessed both desirable hydrogen conversion and rapid reaction kinetics,delivering a hydrogen yield of 966 mL H_(2)g^(-1)within merely 2 min and a maximum hydrogen generation rate of 1147 mL H_(2)min^(-1)g^(-1),as opposed to the sluggish kinetics in the EG-free composites.Moreover,the EG-doped MgLi showed superior air-stable ability even under a 75 RH%ambient atmosphere.For example,the 22 h-milled MgLi-10 wt.%EG composites held a fuel conversion of 89%after air exposure for 72 h,rendering it an advantage for Mg-based materials to safely store and transfer in practical applications.The similar favorable hydrogen performance of MgLi-EG composites in(simulate)seawater may shed light on future development of hydrogen generation technologies.
基金supported by the Natural Science Foundation of Guangdong Province(Grant No.2021A1515010691)the College Innovation Team Project of Guangdong Province(Grant No.2021KCXTD042)Wuyi University-Hong Kong-Macao Joint Research and Development Fund(Grant No.2019WGALH06)。
文摘A versatile sensing platform employing inorganic MoS_(2) nanoflowers and organic poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)has been investigated to develop the resistive and capacitive force-sensitive devices.The microstructure of the sensing layer heightens the sensitivity and response time of the dual-mode pressure sensors by augmenting electron pathways and inner stress in response to mechanical stimuli.Consequently,the capacitive and resistive sensors exhibit sensitivities of 0.37 and 0.12 kPa^(-1),respectively,while demonstrating a remarkable response time of approximately 100 ms.Furthermore,it is noteworthy that the PEDOT:PSS layer exhibits excellent adhesion to polydimethylsiloxane(PDMS)substrates,which contributes to the development of highly robust force-sensitive sensors capable of enduring more than 10000loading/unloading cycles.The combination of MoS_(2)/PEDOT:PSS layers in these dual-mode sensors has shown promising results in detecting human joint movements and subtle physiological signals.Notably,the sensors have achieved a remarkable precision rate of 98%in identifying target objects.These outcomes underscore the significant potential of these sensors for integration into applications such as electronic skin and human-machine interaction.
基金supported by the National Key Research and Development Program of China(2022YFE0206300)the National Natural Science Foundation of China(22209047,U21A2081,22075074)+2 种基金Natural Science Foundation of Hunan Province(2020JJ5035)Hunan Provincial Department of Education Outstanding Youth Project(23B0037)Macao Science and Technology Development Fund(Macao SAR,FDCT-0096/2020/A2).
文摘Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn are prone to react with the hydroxyl ions in alkaline electrolyte upon electrochemical cycling and separates on the surface of spinel to reconstruct into d-MnO_(2) nanosheets irreversibly,thus results in a change of the reaction mechanism with Kþion intercalation.However,the low capacity has greatly limited its practical application.Herein,we found that the tetrahedrally-coordinated Co_(2) þions were leached when MnCo_(2)_(4) was equilibrated in 1 mol L^(-1) HCl solution,leading to the formation of layered CoOOH on MnCo_(2)_(4) surface which is originated from the covalency competition induced selective breakage of the CoT–O bond in CoT–O–CoO and subsequent rearrangement of free Co_(6) octahedra.The as-formed CoOOH is stable upon cycling in alkaline electrolyte,exhibits conversion reaction mechanism with facile proton diffusion and is free of massive structural evolution,thus enables utilization of the bulk electrode material and realizes enhanced specific capacity as well as facilitated charge transfer and ion diffusion.In general,our work not only offers a feasible approach to deliberate modification of MnCo_(2)_(4)'s surface structure,but also provides an in-depth understanding of its charge storage mechanism,which enables rational design of the spinel oxides with promising charge storage properties.
基金supported by the National Natural Science Foundations of China(Grant Nos.12274144 and 52102042)the Project of GDUPS(2018)for Prof.Bingfu LEI,the Guangdong Provincial Special Fund for Modern Agriculture Industry Technology Innovation Teams(Nos.2022KJ22,2023KJ122)+1 种基金Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515010452 and 2022A1515010229)the Guangdong Provincial Science&Technology Project(No.2020A1414010049).
文摘In the era of smart agriculture,the precise labeling and recording of growth information in plants pose challenges for modern agricultural production.This study introduces strontium aluminate particles coated with H_(3)PO_(4)as luminescent labels capable of spatial embedding within plants for information encoding and storage during growth.The encapsulation with H_(3)PO_(4)imparts stability and enhanced luminescence to SrAl_(2)O_(4):Eu^(2+),Dy^(3+)(SAO).Using SAO@H_(3)PO_(4)as a low-damage luminescent label,we implement its delivery into plants through microneedles(MNs)patches.The embedded SAO@H_(3)PO_(4)within plants exhibits sustained and unaltered high signal-to-noise afterglow emission,with luminous intensity remaining at approximately 78%of the original for 27 days.To cater to diverse information recording needs,MNs of various geometric shapes are designed for loading SAO@H3PO4,and the luminescent signals in different shapes can be accurately identified through a designed program,the corresponding information can be conveniently viewed on a computer.Additionally,inspired by binary information concepts,MNs patches with specific arrangements of luminescent and non-luminescent points are created,resulting in varied luminescent MNs arrays on leaves.An advanced camera system with a tailored program accurately identifies and maps the labels to the corresponding recorded information.These findings showcase the potential of low-damage luminescent labels within plants,paving the way for convenient and widespread storage of plant growth information.
基金University of Macao,Grant/Award Numbers:MYRG2018-00192-IAPME,MYRG2020-00187-IAPMEScience and Technology Development Fund,Macao SAR,Grant/Award Numbers:0021/2019/AIR,0041/2019/A1,0046/2019/AFJ,0191/2017/A3UEA funding。
文摘Simultaneously enhancing the reaction kinetics,mass transport,and gas release during alkaline hydrogen evolution reaction(HER)is critical to minimizing the reaction polarization resistance,but remains a big challenge.Through rational design of a hierarchical multiheterogeneous three-dimensionally(3D)ordered macroporous Mo_(2)C-embedded nitrogen-doped carbon with ultrafine Ru nanoclusters anchored on its surface(OMS Mo_(2)C/NC-Ru),we realize both electronic and morphologic engineering of the catalyst to maximize the electrocatalysis performance.The formed Ru-NC heterostructure shows regulative electronic states and optimized adsorption energy with the intermediate H*,and the Mo_(2)C-NC heterostructure accelerates the Volmer reaction due to the strong water dissociation ability as confirmed by theoretical calculations.Consequently,superior HER activity in alkaline solution with an extremely low overpotential of 15.5 mV at 10 mAcm^(−2)with the mass activity more than 17 times higher than that of the benchmark Pt/C,an ultrasmall Tafel slope of 22.7 mV dec−1,and excellent electrocatalytic durability were achieved,attributing to the enhanced mass transport and favorable gas release process endowed from the unique OMS Mo_(2)C/NC-Ru structure.By oxidizing OMS Mo_(2)C/NC-Ru into OMS MoO_(3)-RuO_(2)catalyst,it can also be applied as efficient oxygen evolution electrocatalyst,enabling the construction of a quasi-symmetric electrolyzer for overall water splitting.Such a device's performance surpassed the state-of-the-art Pt/C||RuO2 electrolyzer.This study provides instructive guidance for designing 3D-ordered macroporous multicomponent catalysts for efficient catalytic applications.
基金This study was supported by the National Key Research and Development Program of China(2019YFE0112200)the Science and Technology Development Fund of Macao SAR,China(0073/2019/AMJ)+2 种基金the National Natural Science Foundation of China(51873007,21835006,51961165102,and 52003022)the Fundamental Research Funds for the Central Universities of China(PT2021-02,buctrc202009)the high-performance computing platform of BUCT.
文摘Fluorescent carbon dots(CDs)have recently become a research hotspot in multidisciplinary fields owing to their distinctive advantages,including outstanding photoluminescence properties,high biocompatibility,low toxicity,and abundant raw materials.Among the promising CDs,narrow‐bandwidth emissive CDs with high color purity have emerged as a rising star in recent years because of their significant potential applications in bioimaging,information sensing,and photoelectric displays.In this review,the state-of-the-art advances of narrow-bandwidth emissive CDs are systematically summarized,and the factors influencing the emission bandwidth,preparation methods,and applications of narrow-bandwidth emissive CDs are described in detail.Besides,existing challenges and future perspectives for achieving high-performance narrow-bandwidth emissive CDs are also discussed.This overview paper is expected to generate more interest and promote the rapid development of this significant research area.
基金supported by Shenzhen Fundamental Research Program(Grant No.JCYJ20200109105604088)Distinguished Young Talents in Higher Education of Guangdong,China(Project No.2020KQNCX061)。
文摘The thermoelectric(TE)materials and corresponding TE devices can achieve direct heat-to-electricity conversion,thus have wide applications in heat energy harvesting(power generator),wearable electronics and local cooling.In recent years,aerogel-based TE materials have received considerable attention and have made remarkable progress because of their unique structural,electrical and thermal properties.In this review,the recent progress in both organic,inorganic,and composite/hybrid TE aerogels is systematically summarized,including the main constituents,preparation method,TE performance,as well as factors affecting the TE performance and the corresponding mechanism.Moreover,two typical aerogel-based TE devices/generators are compared and analyzed in terms of assembly modes and output performance.Finally,the present challenges and some tentative suggestions for future research prospects are provided in conclusion.
基金financially supported by the National Natural Science Foundation of China(U21A2081,22075074,22179014)the Outstanding Young Scientists Research Funds from Hunan Province(2020JJ2004)+2 种基金the Major Science and Technology Program of Hunan Province(2020WK2013)the Natural Science Foundation of Hunan Province(2021JJ40047)the State Key Laboratory of Materials Processing and Die&Mould Technology,Huazhong University of Science and Technology(P2022-020)。
文摘The poor cycling stability of graphite in traditional ester electrolyte limits its applications as anodes for potassium ion batteries(KIBs).Herein,we demonstrate that the introduction of cyclic ether co-solvents into ester electrolytes can remarkably enhance the cycling stability of graphite anodes.The graphite anode in ester electrolyte with cyclic ether could achieve a reversible capacity of 196.1 m Ah g^(-1) after 100 cycles at 0.3 C(1 C=280 m A g^(-1)),about three times higher than those in ester electrolytes with or without linear ether.Compared with the SEI formed in ester electrolytes,the addition of tetrahydrofuran promotes the generation of K_(2)CO_(3) and ethylene oxide oligomers(PEO),of which the K_(2)CO_(3) is expected to be more conductive and PEO is mechanically robust.The more uniform,conductive and stable solid electrolyte interphases(SEIs)on graphite in electrolytes with cyclic ethers contribute to the enhancement of the electrochemical performances of graphite.This work provides a novel design of commercialized electrolytes to achieve high-performance anodes for KIBs,which potentially accelerates the development of KIBs.
