Transition metal chalcogenides,such as cobalt selenide(CoSe_(2)),have high lithium storage capacity.However,their practical application is hindered by severe volume expansion and the dissolution of intermediate polyse...Transition metal chalcogenides,such as cobalt selenide(CoSe_(2)),have high lithium storage capacity.However,their practical application is hindered by severe volume expansion and the dissolution of intermediate polyselenides during repeated cycling.Here,we develop a hollow-embedded architecture in which monodisperse CoSe_(2) nanocrystals"sprout"from the walls of porous carbon nanoboxes(H-CoSe_(2)/C)via tannic acid etching,low-temperature carbonization,and vacuum selenization.This"wall-growth"strategy combines confinement with continuity:the porous carbon walls guide uniform nucleation and provide electrical conductivity,while the internal cavity buffers expansion and relieves stress.The embedded geometry shortens Li^(+)diffusion pathways,suppresses particle aggregation,and establishes robust Co-C coupling to enhance charge transport.As a result,the H-CoSe_(2)/C electrode delivers a high reversible capacity of nearly 950 mAh g^(-1),along with outstanding cycling stability.Remarkably,when paired with a LiCoO_(2) cathode in a quasi-solid-state battery,the device achieves an impressive energy density of 355 Wh kg^(-1) and a power density of 3074 W kg^(-1).This study effectively overcomes the inherent defects of CoSe_(2) based on the hollow structure and interface engineering of metal-organic frameworks,providing an effective design for anode materials of lithium-ion batteries.展开更多
Next-generation fire safety systems demand precise detection and motion recognition of flames.In-sensor computing,which integrates sensing,memory,and processing capabilities,has emerged as a key technology in flame de...Next-generation fire safety systems demand precise detection and motion recognition of flames.In-sensor computing,which integrates sensing,memory,and processing capabilities,has emerged as a key technology in flame detection.However,the implementation of hardware-level functional demonstrations based on artificial vision systems in the solar-blind ultraviolet(UV)band(200-280 nm)is hindered by the weak detection capability.Here,we propose Ga_(2)O_(3)/In_(2)Se_(3) heterojunctions for the ferroelectric(abbreviation:Fe)optoelectronic sensor(abbreviation:OES)array(5×5 pixels),which is capable of ultraweak UV light detection with an ultrahigh detectivity through ferroelectric regulation and features in configurable multimode functionality.The Fe-OES array can directly sense different flame motions and simulate the non-spiking gradient neurons of insect visual system.Moreover,the flame signal can be effectively amplified in combination with leaky integration-and-fire neuron hardware.Using this Fe-OES system and neuromorphic hardware,we successfully demonstrate three flame processing tasks:achieving efficient flame detection across all time periods with terminal and cloud-based alarms;flame motion recognition with a lightweight convolutional neural network achieving 96.47%accuracy;and flame light recognition with 90.51%accuracy by means of a photosensitive artificial neural system.This work provides effective tools and approaches for addressing a variety of complex flame detection tasks.展开更多
The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts rem...The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts remains a primary challenge.In this study,an enhancement in catalytic MOR performance is achieved through the incorporation of Mn atoms with unsaturated t_(2g)orbitals into Ni_(3)Se_(4).Comprehensive experimental analyses and theoretical calculations reveal that substituting Ni with Mn induces strong electron-withdrawing effects,effectively modulating the local coordination environment of the metal centers.The presence of Mn also elongates Ni–Se(O)bonds,which reduces eg orbital occupancy and modifies the spin state of the material.Electrochemical measurements demonstrate that electrodes based on this optimized material exhibit a high spin state and deliver excellent catalytic activity,achieving a MOR current density up to∼190 mA cm^(−2)at 1.6 V.This performance enhancement is attributed to the favorable electronic configuration and reduced reaction energy barriers associated with the high-spin state.展开更多
Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy ...Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination(Se4-Nb2-O2)in N-doped carbon-confined amorphous selenide clusters(a-Nb-Se/O@NC).Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds,eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds,thereby enhancing structural integrity and Na+storage capacity.The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system,where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers.These strengthen d-p orbital hybridization,reduce Na+adsorption energy,and optimize charge transfer pathways and reaction kinetics in the amorphous clusters.Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g^(−1)and exceptional cyclic stability(103%capacity retention)after 5000 cycles at 10.0 A g^(−1).Assembled SIHCs achieve outstanding energy/power densities(207.1 Wh kg^(−1)/18966 W kg^(−1)),surpassing most amorphous and crystalline counterparts.This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.展开更多
Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrent...Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrently construct heterogeneous interfaces,adjust phase structure,and regulate electronic configuration,thereby enhancing OER performance.Thanks to the role of CeO_(2)coupling in reducing the activation-energy and accelerating the reaction kinetics,the heterogeneous NixSey/CeO_(2)catalyst exhibits a low overpotential of 218 mV at 10 mA/cm2and long-term stability(>400 h)in 1.0 mol/L KOH for OER.Moreover,the post-OER characterization reveals that the NixSeymatrix is reconstructed into NiOOH,while the incorporated CeO_(2)nanocrystals self-assemble into larger polycrystalline particles.Theoretical analysis further demonstrates that the optimized electronic states at NiOOH/CeO_(2)interfaces can modulate intermediate chemisorption toward favorable OER kinetics.This study offers fresh perspectives on the synthesis and structure-activity relationship of CeO_(2)-coupled electrocatalysts.展开更多
Flexible tandem solar cells,promising for lightweight power generation,face a hurdle:getting high-quality layers to stick well to rough surfaces like copper indium gallium selenide(CIGS).Scientists have now developed ...Flexible tandem solar cells,promising for lightweight power generation,face a hurdle:getting high-quality layers to stick well to rough surfaces like copper indium gallium selenide(CIGS).Scientists have now developed an innovative strategy to improve this,significantly boosting cell performance and durability.展开更多
Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense...Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas pollutants.Besides the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury resources.This paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium species.Based on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial applications.In addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.展开更多
Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary ba...Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary bandgap copper indium gallium selenide(CIGS)photovoltaic technology has demonstrated a realistic pathway to achieve the industrialization goal of pushing power conversion efficiency(PCE)approaching 30% at low-cost.In this review,we first pinpoint the unique advantage of perovskite/CIGS tandems with respect to the other mainstream photovoltaic technologies and retrospect the research progress of perovskite/CIGS TSCs from both PCE and stability perspective in the last years.Next,we comprehensively discuss the major advancements in absorbers,functional layers of the individual sub-cell,and the interconnection layer between them in the recent decade.Finally,we outline several essential scientific and engineering challenges that are to be solved toward the development of efficient,long-term stable,and large-area perovskite/CIGS TSCs in the future.展开更多
Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SI...Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SIBs).In this study,WSe_(2)/MoSe_(2)nanosheets with a better-matched and stable heterojunction interface were uniformly embedded in carbon nanofiber frameworks(WSe_(2)/MoSe_(2)/CNFs).The ion/electron transfer kinetics were facilitated by heterointerfaces with an enlarged effective utilization range.Meanwhile,the heterointerface directed electron transfer from MoSe_(2)to WSe_(2)and had significant potassium adsorption capability.The ultra-high pseudocapacitance contribution originating from the heterostructure and morphological features of the WSe_(2)/MoSe_(2)nanosheets contributed to enhancing high-rate energy storage.Moreover,in situ X-ray diffraction and ex situ X-ray photoelectron spectroscopy revealed the potassification/depotassification behavior of the WSe_(2)/MoSe_(2)/CNFs during the conversion reaction.Consequently,after 500 cycles at 5 A·g^(-1),the WSe_(2)/MoSe_(2)/CNF anode demonstrated an outstanding long-term cycling performance of 125.6 mAh·g^(-1)for PIBs.While serving as a SIB electrode,it exhibited an exceptional rate capability of 243.5 mAh·g^(-1)at 20 A·g^(-1).With the goal of developing high-performance PIB/SIB electrode materials,the proposed strategy,based on heterointerface adaptation engineering,is promising.展开更多
Wearable photodetectors have come under the limelight of optoelectronic technologies on account of multiple advantages spanning light weight,easy-portability,excellent bendability,outstanding conformability,etc.Among ...Wearable photodetectors have come under the limelight of optoelectronic technologies on account of multiple advantages spanning light weight,easy-portability,excellent bendability,outstanding conformability,etc.Among diverse candidate materials,low-dimensional van der Waals materials(LDvdWMs)have emerged to be preeminent owing to the dangling-bond-free surface,exceptional carrier mobility,nanoscale dimensionality,and excellent light-harvesting capability.However,to date,the majority of flexible LDvdWM photodetectors have been fabricated through exfoliation-,transfer-,or solution-processing methods,which are plagued by limitations such as low production yield,inadequate photosensitivity,and sluggish response rate.Thus far,constructing LDvdWM photodetectors in situ on flexible substrates remains quite challenging due to the irreconcilable contradiction between the weak robustness of flexible polymer substrates against high temperature and the large thermal budget required for crystallization.This study develops scalable preparation of Sb_(2)Se_(3)nanofilm directly on flexible polyimide substrates by exploiting pulsed-laser deposition(PLD),where highly energetic species can be generated to enable overcoming the reaction barrier for crystallization at a relatively low temperature.The corresponding Sb_(2)Se_(3)photodetectors have exhibited high responsivity of 1.15 A/W,exceptional external quantum efficiency of 269%,and impressive specific detectivity reaching 2.4×10^(11)Jones,coupled with swift switching characteristics.Importantly,excellent durability to repeated bending treatments has been confirmed by the consistent photoresponse over 500 convex/concave bending cycles.Furthermore,the device has showcased strong robustness against extrinsic impinging.In the end,by using Sb_(2)Se_(3)photodetectors as sensing components,wide-band imaging beyond human vision and heart rate monitoring have been realized.This study has underscored the high efficacy of PLD for reconciling the long-standing contradiction between the weak robustness of flexible polymer substrates against high temperature and the substantial thermal energy required for crystallization,opening new opportunities towards next-generation wearable optoelectronic industry.展开更多
With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains a...With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains an important challenge.An incipient wetness impregnation method followed by in-situ selenization was used to load copper selenide(CuSe) onto the surface of optimal magnetic biochar (OMBC).The results showed that CuSe significantly enhanced the Hg0removal performance of the OMBC,and CuSe loading ratio of 10%(10CuSe/OMBC) had the best Hg0removal performance.10CuSe/OMBC maintained its Hg0removal efficiency above 95% for 150 min at 30-150℃,and it had a good resistance to SO2.The equilibrium adsorption capacity of 10CuSe/OMBC could reach up to 8.73 mg/g,which was close to the theoretical value 12.99 mg/g,and the adsorption rate was up to 20.33μg/(g·min) Meanwhile,10CuSe/OMBC had strong magnetism that is not permanently magnetized,which could be separated from desulfurization gypsum and recycled many times.Characterization results demonstrated that Se22-,Cu2+and Oβplayed essential roles in the oxidation of Hg0,and Se22-and Se2-can immobilize Hg2+to HgSe.10CuSe/OMBC has important guiding significance for practical application because of its low cost,high performance and low mercury leaching characteristic to form HgSe.展开更多
Transition metal selenides(TMSs),as promising anode materials for sodium ion batteries(SIBs),still face sluggish Na+diffusion kinetics and severe volume change,resulting in undesirable cycling stability and rate capab...Transition metal selenides(TMSs),as promising anode materials for sodium ion batteries(SIBs),still face sluggish Na+diffusion kinetics and severe volume change,resulting in undesirable cycling stability and rate capability.Heterostructure construction is an effective method to improve sodium ion storage in TMSs.Herein,a hierarchical hollow heterostructure of CoSe_(2)@SnSe is precisely designed through a facile coprecipitation process followed by a selenization strategy.The heterostructure constructed by CoSe_(2)and SnSe nanocrystals induces the formation of built-in electric fields and accelerates electron transfer and ion diffusion,thereby improving reaction kinetics significantly.When the as-prepared CoSe_(2)@SnSe composites are employed as anode materials of SIBs,there exhibit ultra-fast electrochemical reaction kinetics and outstanding cycling stability with a high capacity retention of 488.9 mAh g^(-1)at a current density of 2.0 A g^(-1)after 900 cycles.In addition,there still shows an exceptional rate capability of 409.5 mAh g^(-1)at a high current density of 10 A g^(-1).This work provides an effective method for the rational designing of heterostructure anode materials for high-performance SIBs.展开更多
The polysulfides shuttle effect,sluggish sulfur redox kinetics and the corrosion of the Li anode have become important factors limiting the commercial application of lithium-sulfur batteries(LSBs).Herein,the polyoxome...The polysulfides shuttle effect,sluggish sulfur redox kinetics and the corrosion of the Li anode have become important factors limiting the commercial application of lithium-sulfur batteries(LSBs).Herein,the polyoxometalate(POM)nanoclusters with high catalytic activity and cobalt selenide with strong polarity are initially complemented to construct a PMo_(12)/CoSe_(2)@NC/CNTs multifunctional separator that can simultaneously solve the above problems.A series of experimental and theoretical results demonstrate that the Keggin-type POM,H_(3)PMo_(12)O_(40)nH_(2)O(PMo_(12))nanoclusters could function as catalytic centers for sulfur-involved transformations,with the CoSe_(2)nanoparticles serving as adsorption sites for soluble polysulfides.Accordingly,the assembled battery with the PMo_(12)/CoSe_(2)@NC/CNTs modified separator achieves an initial discharge capacity of 1263.79 mA h g^(-1),maintaining 635.77 mA h g^(-1),with a capacity decay rate of 0.06%per cycle after 500 cycles at 3C.This work provides a strategic approach for incorporating POM nanoclusters with polar periodic nanomaterials in LSB separators,contributing to the development of multifunctional separator materials,thus promoting the advancement of energy storage systems.展开更多
Conversion-alloying anode materials are competitive candidates for high-energy-density sodium-ion batteries(SIBs).However,the sluggish dynamics and severe volume expansion during Na insertion/extraction become the key...Conversion-alloying anode materials are competitive candidates for high-energy-density sodium-ion batteries(SIBs).However,the sluggish dynamics and severe volume expansion during Na insertion/extraction become the key bottlenecks hindering their application in SIBs.Herein,SnTe nanoparticles are anchored on reduced graphene oxide(rGO)and encapsulated by nitrogen-doped carbon(NC)to construct SnTe@rGO@NC composite as anode for SIBs,where hierarchical confinement effect can provide a buffer area to accommodate huge volume expansion as well as enhance electronic conductivity and Na-ion transfer kinetics behavior,confirmed by density functional theory(DFT)calculation and experimental study.Meanwhile,structural stability and interfacial charge transfer of the composite can be further improved by the strong chemical bonds of C-Sn and C-Te.High-angle annular dark field scanning transmission electron microscopy visually at atomic scale declares that SnTe@rGO@NC proceeds conversion-alloying dual-mechanism for Na-ion storage employing Sn as redox center(4SnTe+23Na^(+)+23e^(-)→Na_(15)Sn_(4)+4Na_(2)Te).Thus,SnTe@rGO@NC architecture displays a high reversible specific capacity of 261.5 mAh·g^(-1)at 50 mA·g^(-1),superior rate capability and excellent cycling stability with long-term lifespan over 1000 cycles at 200 mA·g^(-1).The multi-physicochemical encapsulation strategy sheds light on the development of a high-performance conversion-alloying anode for SIBs.展开更多
Lithium-sulfur batteries(LSBs)are a promising candidate for next-generation energy storage solutions.However,challenges such as the shuttling effect and sluggish Li-S reaction kinetics of lithium polysulfides hinder t...Lithium-sulfur batteries(LSBs)are a promising candidate for next-generation energy storage solutions.However,challenges such as the shuttling effect and sluggish Li-S reaction kinetics of lithium polysulfides hinder their practical application.In this work,we present a mixed-phase heterostructure comprising Co_(0.85)Se and MoSe_(2),supported on nitrogen-doped carbon polyhedrons(NCP),as an effective sulfur host in the LSB cathode.Through a combination of theoretical calculations and experimental validation,we demonstrate that the Co_(0.85)Se-MoSe_(2)heterointerface significantly enhances electron transfer efficiency,thereby boosting the overall reaction kinetics of the sulfur cathode.As a result,the Co_(0.85)Se-MoSe_(2)/NCP/S electrodes exhibit initial specific capacities exceeding 1500 mAh g^(-1)at 0.1 C and retain 666 m Ah g^(-1)at 3 C,with a capacity fade rate of 0.044%per cycle over 500 cycles at 1.0 C.Notably,even at a high sulfur loading of 3 mg cm^(-2)and a reduced electrolyte volume of 6.7μL mgS^(-1),the Co_(0.85)SeMoSe_(2)/NCP/S electrodes maintain a capacity of 432 mAh g^(-1)after 100 cycles at 0.2 C.展开更多
Transition metal selenides(TMSs)are effective pre-electrocatalysts and are commonly used in electrochemical processes.During the electrocatalytic oxygen evolution reaction(OER),metal cations in TMSs are in-situ recons...Transition metal selenides(TMSs)are effective pre-electrocatalysts and are commonly used in electrochemical processes.During the electrocatalytic oxygen evolution reaction(OER),metal cations in TMSs are in-situ reconstructed and converted into high-valence metal oxyhydroxides.However,a limited understanding of the effects of electro-oxidation and anion leaching has resulted in insufficient theoretical guidance for the rational design of efficient catalysts.Herein,FeSe@NiSe nanorods were fabricated for the OER using a facile hydrothermal selenization method supported on FeNi foam.In-situ Raman spectroscopy and multiple characterization techniques were employed to elucidate the mechanism of FeSe@NiSe surface evolution.Metal cations on the catalyst surface were reconstructed and converted into OER-active species Fe/NiOOH at low potential.As the applied potential increased,electro-oxidation and leaching of Se occurred,resulting in SeO_(4)^(2−)adsorption on the catalyst surface,which further enhanced catalytic activity.As a result,the reconstructed FeSe@NiSe/iron-nickel foam(INF)exhibited exceptional catalytic activity for OER,achieving an ultralow overpotential of 283 mV at a current density of 100 mA·cm^(−2).Notably,the bifunctional FeSe@NiSe/INF electrode facilitated overall water splitting,affording a current density of 10 mA·cm^(−2) only at 1.53 V,even superior to the noble RuO_(2)(+)||Pt/C(−).This work offers valuable insights into the surface evolution and electrocatalytic mechanisms of TMSs.展开更多
Semiconducting transition-metal dichalcogenides(TMDs)have garnered significant interest due to their unique structures and properties,positioning them as promising candidates for novel electronic and optoelectronic de...Semiconducting transition-metal dichalcogenides(TMDs)have garnered significant interest due to their unique structures and properties,positioning them as promising candidates for novel electronic and optoelectronic devices.However,the performance of TMDs-based devices is hampered by the suboptimal quality of metal electrodes contacting the atomically thin TMDs layers.Understanding the mechanisms that influence contact quality is crucial for advancing TMDs devices.In this study,we investigated the conductive properties of tungsten selenide(WSe_(2))-based devices with different film thicknesses.Using the transmission line method,a negative correlation between contact resistance and film thickness in multi-electrode devices was revealed.Additionally,repeatability tests conducted at varied temperatures indicated enhanced device stability with increasing film thickness.Theoretical analysis,supported by thermionic emission theory and thermal simulations,suggests that the degradation in electrical properties is primarily due to the thermal effect at the contact interface.Furthermore,we found that van der Waals contacts could mitigate the thermal effect through a metal transfer method.Our findings elucidate the critical role of contact resistance in the electronic performance of 2D material-based field-effect transistors(FETs),which further expands their potential in the next generation of electronic and optoelectronic devices.展开更多
Nickel selenides have been studied as potential anode materials for sodium-ion batteries due to their high theoretical capacity.However,the low electrical conductivity and the large volumetric variation during the cha...Nickel selenides have been studied as potential anode materials for sodium-ion batteries due to their high theoretical capacity.However,the low electrical conductivity and the large volumetric variation during the charging/discharging process greatly reduce the specific capacity and cycling lifespan of the batteries.In this paper,a simple strategy to fabricate NiSe nanoparticles enclosed in carbon hollow nanofibers(NiSe/C@CNF)is proposed,involving the preparation of Ni-precursor nanofibers by electrospinning,the coating of polydopamine and the formation of NiSe/C@CNF by calcination and selenization.The combination of NiSe nanoparticles and porous carbon hollow nanofibers creates a strong conductive environment,which enhances the dynamic ability of sodium-ion transport and improves charge storage capacity.The fabricated NiSe/C@CNF material exhibits excellent performance.It demonstrates a high rate capability,with specific capacities of 406.8 and 300.1 mAh·g^(-1)at 0.1 and 5.0 A·g^(-1),respectively.These results highlight the potential of NiSe/C@CNF as an anode material for sodium-ion batteries,offering a large capacity and long life.展开更多
Lithium-sulfur batteries(LSBs)are considered as the promising solution to replace conventional lithium-ion batteries due to satisfactory energy density.In recent times,the LSBs field has been found to face some diffic...Lithium-sulfur batteries(LSBs)are considered as the promising solution to replace conventional lithium-ion batteries due to satisfactory energy density.In recent times,the LSBs field has been found to face some difficulties in exploring practical applications in which cycling stability and cycle life are awful owing to the shuttling effect of lithium polysulfides(LiPSs)and low sulfur utilization.In this work,by synthesizing Co_(3)Se_(4) nanoparticles onto N-doped carbon(NC)polyhedra interconnected with carbon nanotubes(CNTs),NC@Co_(3)Se_(4)/CNTs is proposed as a multifunctional sulfur carrier.The Co_(3)Se_(4) nanoparticles fleetly catalyze the conversion of LiPSs and availably immobilize LiPSs.Meanwhile,the NC polyhedral skeleton enhances the electronic conductivity of active sulfur,while the CNTs facilitate Li+diffusion and supply a mass of conductive channels.Density-functional theory(DFT)calculations demonstrate the relevant mechanisms.That is to say,the NC@Co_(3)Se_(4)/CNTs benefit from the synergistic effect of Co_(3)Se_(4) nanoparticles(highly catalytic ability and strong adsorbability for LiPSs)and the special carbonaceous structure,rapidly converting LiPSs and inhibiting the shuttle of LiPSs.Therefore,lithium-sulfur battery assembled with S/NC@Co_(3)Se_(4)/CNTs cathode as well as nitrogen and sulfur co-doped carbon-coated polypropylene(N,S-C/PP)separator possesses a high initial discharge capacity of 1413 mAh·g-1 at 0.12C and persistently circulates for 1000 cycles at 1C with a capacity attenuation rate per cycle of 0.034%.This work provides a realistic idea for the use of transition metal selenide in the field of high-performance LSBs.展开更多
Trimetallic selenides have emerged as a promising electrode for wearable supercapacitors applications,due to their high electrical conductivity,rich redox activity,structural robustness,and porosity.In this report,a t...Trimetallic selenides have emerged as a promising electrode for wearable supercapacitors applications,due to their high electrical conductivity,rich redox activity,structural robustness,and porosity.In this report,a trimetallic nickel–magnesium-manganese selenide(NMMSe)electrode with a well-defined nanosphere morphology was prepared using a low-cost and rapid electrodeposition technique.The electrochemical performance of the NMMSe electrodes was systematically investigated as a positive electrode.The NMMSe electrode prepared with a deposition time of 200 s(denoted as NMMSe-200)revealed a high areal/specific capacity of 439.4μAh cm^(−2)/225.6 mA h g^(−1) at 4 mA cm^(–2),along with excellent cycling stability.To further investigate the effect of deposition time on the nanostructure evaluation and electrochemical behavior,additional NMMSe electrodes were synthesized at the growth times of 100 and 300 s.For the negative electrode,activated carbon derived from pistachio shell waste(i.e.,porous activated carbon(PAC))was employed,demonstrating a high areal capacitance of 913.4 mF cm^(−2) and an excellent surface area of 320.6 m^(2)/g.Finally,a semi-solid-state hybrid capacitor(HC)cell was assembled using NMMSe-200 as the positive(+)electrode and PAC as the negative(-)electrode.The resulting NMMSe//PAC/nickel foam HC cell delivered an impressive areal capacitance of 928.8 mF cm^(−2) at 2 mA cm^(–2),a high energy density of 338.5μWh cm^(–2)(56.4 Wh kg^(−1)),and exceptional cycling stability.These results highlight the strong potential of NMMSe-200 electrodes for high-performance,wearable energy storage systems.展开更多
基金supported by the National Natural Science Foundation of China(No.52377218)。
文摘Transition metal chalcogenides,such as cobalt selenide(CoSe_(2)),have high lithium storage capacity.However,their practical application is hindered by severe volume expansion and the dissolution of intermediate polyselenides during repeated cycling.Here,we develop a hollow-embedded architecture in which monodisperse CoSe_(2) nanocrystals"sprout"from the walls of porous carbon nanoboxes(H-CoSe_(2)/C)via tannic acid etching,low-temperature carbonization,and vacuum selenization.This"wall-growth"strategy combines confinement with continuity:the porous carbon walls guide uniform nucleation and provide electrical conductivity,while the internal cavity buffers expansion and relieves stress.The embedded geometry shortens Li^(+)diffusion pathways,suppresses particle aggregation,and establishes robust Co-C coupling to enhance charge transport.As a result,the H-CoSe_(2)/C electrode delivers a high reversible capacity of nearly 950 mAh g^(-1),along with outstanding cycling stability.Remarkably,when paired with a LiCoO_(2) cathode in a quasi-solid-state battery,the device achieves an impressive energy density of 355 Wh kg^(-1) and a power density of 3074 W kg^(-1).This study effectively overcomes the inherent defects of CoSe_(2) based on the hollow structure and interface engineering of metal-organic frameworks,providing an effective design for anode materials of lithium-ion batteries.
基金supported by the Major Program(JD)of Hubei Province under Grant No.2023BAA009the National Natural Science Foundation of China(Grant No.22105162)+1 种基金the Natural Science Foundation of Hubei Province(Grant No.2023AFB623)the Original Exploration Seed Fund of Hubei University。
文摘Next-generation fire safety systems demand precise detection and motion recognition of flames.In-sensor computing,which integrates sensing,memory,and processing capabilities,has emerged as a key technology in flame detection.However,the implementation of hardware-level functional demonstrations based on artificial vision systems in the solar-blind ultraviolet(UV)band(200-280 nm)is hindered by the weak detection capability.Here,we propose Ga_(2)O_(3)/In_(2)Se_(3) heterojunctions for the ferroelectric(abbreviation:Fe)optoelectronic sensor(abbreviation:OES)array(5×5 pixels),which is capable of ultraweak UV light detection with an ultrahigh detectivity through ferroelectric regulation and features in configurable multimode functionality.The Fe-OES array can directly sense different flame motions and simulate the non-spiking gradient neurons of insect visual system.Moreover,the flame signal can be effectively amplified in combination with leaky integration-and-fire neuron hardware.Using this Fe-OES system and neuromorphic hardware,we successfully demonstrate three flame processing tasks:achieving efficient flame detection across all time periods with terminal and cloud-based alarms;flame motion recognition with a lightweight convolutional neural network achieving 96.47%accuracy;and flame light recognition with 90.51%accuracy by means of a photosensitive artificial neural system.This work provides effective tools and approaches for addressing a variety of complex flame detection tasks.
基金financially supported by the Sichuan Science and Technology Program (Grant No. 2025NSFSC0139)the China Postdoctoral Science Foundation (Grant No.2023MD734228)+10 种基金funding from Generalitat de Catalunya 2021SGR00457supported by MCIN with funding from European Union NextGenerationEU(PRTR-C17.I1)by Generalitat de Catalunya (In-CAEM Project)the support from the project AMaDE(PID2023-149158OB-C43)funded by MCIN/AEI/10.13039/501100011033/by “ERDF A way of making Europe”by the “European Union”supported by the Severo Ochoa program from Spanish MCIN/AEI (Grant No.:CEX2021-001214-S)funded by the CERCA Programme/Generalitat de Catalunyaperformed in the framework of Universitat Autònoma de Barcelona Materials Science PhD programfunding from the CSC-UAB PhD scholarship program. ICN2 is founding member of e-DREAM[87]
文摘The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts remains a primary challenge.In this study,an enhancement in catalytic MOR performance is achieved through the incorporation of Mn atoms with unsaturated t_(2g)orbitals into Ni_(3)Se_(4).Comprehensive experimental analyses and theoretical calculations reveal that substituting Ni with Mn induces strong electron-withdrawing effects,effectively modulating the local coordination environment of the metal centers.The presence of Mn also elongates Ni–Se(O)bonds,which reduces eg orbital occupancy and modifies the spin state of the material.Electrochemical measurements demonstrate that electrodes based on this optimized material exhibit a high spin state and deliver excellent catalytic activity,achieving a MOR current density up to∼190 mA cm^(−2)at 1.6 V.This performance enhancement is attributed to the favorable electronic configuration and reduced reaction energy barriers associated with the high-spin state.
基金supported by the National Natural Science Foundation of China(Grant No.52573299)the Natural Science Foundation of Jiangxi province(No.20242BAB25223,20232BCJ23025,20232BCJ25040,20232BAB214024)the Special Funding Program for Graduate Student Innovation of Jiangxi Province(No.YC2024-S594).
文摘Transition metal selenides as sodium-ion hybrid capacitor(SIHC)anodes still suffer from amorphization difficulties and capacity degradation triggered by polyselenide dissolution.Herein,an atomistic amorphous strategy is proposed to construct adjacent Nb-Nb diatomic pairs with Se/O-coordination(Se4-Nb2-O2)in N-doped carbon-confined amorphous selenide clusters(a-Nb-Se/O@NC).Synergistic carbon confinement and hydrothermal oxygenation induce amorphization of Nb–Se bonds,eliminating crystalline rigidity while creating isotropic dual-ion transport channels and high-density active sites enriched with dangling bonds,thereby enhancing structural integrity and Na+storage capacity.The unique Se/O-coordinated Nb-Nb diatomic configuration establishes an electron-delocalized system,where the low electronegativity of Se counterbalances electron withdrawal from coordinated O at Nb centers.These strengthen d-p orbital hybridization,reduce Na+adsorption energy,and optimize charge transfer pathways and reaction kinetics in the amorphous clusters.Electrochemical tests reveal that the a-Nb-Se/O@NC anode delivers a high reversible capacity of 312.57 mAh g^(−1)and exceptional cyclic stability(103%capacity retention)after 5000 cycles at 10.0 A g^(−1).Assembled SIHCs achieve outstanding energy/power densities(207.1 Wh kg^(−1)/18966 W kg^(−1)),surpassing most amorphous and crystalline counterparts.This work provides methodological insights for the design of electrodes in high-power storage devices through atomic modulation and electronic optimization of amorphous selenides.
基金supported by the grants from the National Natural Science Foundation of China(No.22202098)the Natural Science Foundation of Henan Province(No.242300420199)。
文摘Heterogeneous catalysts have attracted wide attention due to their remarkable oxygen evolution reaction(OER)capabilities.Herein,a one-step strategy involving the coupling of NixSeywith CeO_(2)is proposed to concurrently construct heterogeneous interfaces,adjust phase structure,and regulate electronic configuration,thereby enhancing OER performance.Thanks to the role of CeO_(2)coupling in reducing the activation-energy and accelerating the reaction kinetics,the heterogeneous NixSey/CeO_(2)catalyst exhibits a low overpotential of 218 mV at 10 mA/cm2and long-term stability(>400 h)in 1.0 mol/L KOH for OER.Moreover,the post-OER characterization reveals that the NixSeymatrix is reconstructed into NiOOH,while the incorporated CeO_(2)nanocrystals self-assemble into larger polycrystalline particles.Theoretical analysis further demonstrates that the optimized electronic states at NiOOH/CeO_(2)interfaces can modulate intermediate chemisorption toward favorable OER kinetics.This study offers fresh perspectives on the synthesis and structure-activity relationship of CeO_(2)-coupled electrocatalysts.
文摘Flexible tandem solar cells,promising for lightweight power generation,face a hurdle:getting high-quality layers to stick well to rough surfaces like copper indium gallium selenide(CIGS).Scientists have now developed an innovative strategy to improve this,significantly boosting cell performance and durability.
基金supported by the Basic Research Business Fund Grant Program for University of Science and Technology Beijing (No.06500227)the Fundamental Research Funds for the Central Universities (No.FRF-TP-22-091A1).
文摘Mercury(Hg)pollution has been a global concern in recent decades,posing a significant threat to entire ecosystems and human health due to its cumulative toxicity,persistence,and transport in the atmosphere.The intense interaction between mercury and selenium has opened up a new field for studying mercury removal from industrial flue gas pollutants.Besides the advantages of good Hg^(0) capture performance and lowsecondary pollution of the mineral selenium compounds,the most noteworthy is the relatively low regeneration temperature,allowing adsorbent regeneration with low energy consumption,thus reducing the utilization cost and enabling recovery of mercury resources.This paper reviews the recent progress of mineral selenium compounds in flue gas mercury removal,introduces in detail the different types ofmineral selenium compounds studied in the field ofmercury removal,reviews the adsorption performance of various mineral selenium compounds adsorbents on mercury and the influence of flue gas components,such as reaction temperature,air velocity,and other factors,and summarizes the adsorption mechanism of different fugitive forms of selenium species.Based on the current research progress,future studies should focus on the economic performance and the performance of different carriers and sizes of adsorbents for the removal of Hg^(0) and the correlation between the gas-particle flow characteristics and gas phase mass transfer with the performance of Hg^(0) removal in practical industrial applications.In addition,it remains a challenge to distinguish the oxidation and adsorption of Hg^(0) quantitatively.
基金funding support from the National Key Research and Development Program of China(Grant No.2020YFB0408002)the Beijing Natural Science Foundation(Z240024)+2 种基金the National Natural Science Foundation of China(Grant Nos.22279083,22461160281,W2412076)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2022B1515120006)the Central Guiding Local Science and Technology Development Special Fund Project(Grant No.ZYYD2024JD24)。
文摘Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary bandgap copper indium gallium selenide(CIGS)photovoltaic technology has demonstrated a realistic pathway to achieve the industrialization goal of pushing power conversion efficiency(PCE)approaching 30% at low-cost.In this review,we first pinpoint the unique advantage of perovskite/CIGS tandems with respect to the other mainstream photovoltaic technologies and retrospect the research progress of perovskite/CIGS TSCs from both PCE and stability perspective in the last years.Next,we comprehensively discuss the major advancements in absorbers,functional layers of the individual sub-cell,and the interconnection layer between them in the recent decade.Finally,we outline several essential scientific and engineering challenges that are to be solved toward the development of efficient,long-term stable,and large-area perovskite/CIGS TSCs in the future.
基金supported by the National Natural Science Foundation of China(No.22201098)the Natural Science Foundation of Shandong Province(Nos.ZR2021QB005 and ZR2021MB008)Jinan City“New University 20”Project(No.202228113).
文摘Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SIBs).In this study,WSe_(2)/MoSe_(2)nanosheets with a better-matched and stable heterojunction interface were uniformly embedded in carbon nanofiber frameworks(WSe_(2)/MoSe_(2)/CNFs).The ion/electron transfer kinetics were facilitated by heterointerfaces with an enlarged effective utilization range.Meanwhile,the heterointerface directed electron transfer from MoSe_(2)to WSe_(2)and had significant potassium adsorption capability.The ultra-high pseudocapacitance contribution originating from the heterostructure and morphological features of the WSe_(2)/MoSe_(2)nanosheets contributed to enhancing high-rate energy storage.Moreover,in situ X-ray diffraction and ex situ X-ray photoelectron spectroscopy revealed the potassification/depotassification behavior of the WSe_(2)/MoSe_(2)/CNFs during the conversion reaction.Consequently,after 500 cycles at 5 A·g^(-1),the WSe_(2)/MoSe_(2)/CNF anode demonstrated an outstanding long-term cycling performance of 125.6 mAh·g^(-1)for PIBs.While serving as a SIB electrode,it exhibited an exceptional rate capability of 243.5 mAh·g^(-1)at 20 A·g^(-1).With the goal of developing high-performance PIB/SIB electrode materials,the proposed strategy,based on heterointerface adaptation engineering,is promising.
基金financially supported by National Natural Science Foundation of China(Nos.U2001215,52272175,12104517)Natural Science Foundation of Guangdong Province(Nos.2022A1515011487,2021A1515110403)+1 种基金Young Top Talents Program(No.2021QN02C068)State Key Laboratory of Optoelectronic Materials and Technologies(Sun Yat-sen University).
文摘Wearable photodetectors have come under the limelight of optoelectronic technologies on account of multiple advantages spanning light weight,easy-portability,excellent bendability,outstanding conformability,etc.Among diverse candidate materials,low-dimensional van der Waals materials(LDvdWMs)have emerged to be preeminent owing to the dangling-bond-free surface,exceptional carrier mobility,nanoscale dimensionality,and excellent light-harvesting capability.However,to date,the majority of flexible LDvdWM photodetectors have been fabricated through exfoliation-,transfer-,or solution-processing methods,which are plagued by limitations such as low production yield,inadequate photosensitivity,and sluggish response rate.Thus far,constructing LDvdWM photodetectors in situ on flexible substrates remains quite challenging due to the irreconcilable contradiction between the weak robustness of flexible polymer substrates against high temperature and the large thermal budget required for crystallization.This study develops scalable preparation of Sb_(2)Se_(3)nanofilm directly on flexible polyimide substrates by exploiting pulsed-laser deposition(PLD),where highly energetic species can be generated to enable overcoming the reaction barrier for crystallization at a relatively low temperature.The corresponding Sb_(2)Se_(3)photodetectors have exhibited high responsivity of 1.15 A/W,exceptional external quantum efficiency of 269%,and impressive specific detectivity reaching 2.4×10^(11)Jones,coupled with swift switching characteristics.Importantly,excellent durability to repeated bending treatments has been confirmed by the consistent photoresponse over 500 convex/concave bending cycles.Furthermore,the device has showcased strong robustness against extrinsic impinging.In the end,by using Sb_(2)Se_(3)photodetectors as sensing components,wide-band imaging beyond human vision and heart rate monitoring have been realized.This study has underscored the high efficacy of PLD for reconciling the long-standing contradiction between the weak robustness of flexible polymer substrates against high temperature and the substantial thermal energy required for crystallization,opening new opportunities towards next-generation wearable optoelectronic industry.
基金supported by the Basic Research Business Fund Grant Program for University of Science and Technology Beijing(No.06500227)the Fundamental Research Funds for the Central Universities(No.FRF-TP-22-091A1)+1 种基金National Natural Science Foundation of China(No.52200121),Chinese Universities Scientific Fund(No.00007713)the Guide special project(No.40103322).
文摘With the rapid development of adsorbents for removal of elemental mercury (Hg0) from coal combustion flue gas,the preparation of adsorbents with superior performance,lower cost and environmental friendliness remains an important challenge.An incipient wetness impregnation method followed by in-situ selenization was used to load copper selenide(CuSe) onto the surface of optimal magnetic biochar (OMBC).The results showed that CuSe significantly enhanced the Hg0removal performance of the OMBC,and CuSe loading ratio of 10%(10CuSe/OMBC) had the best Hg0removal performance.10CuSe/OMBC maintained its Hg0removal efficiency above 95% for 150 min at 30-150℃,and it had a good resistance to SO2.The equilibrium adsorption capacity of 10CuSe/OMBC could reach up to 8.73 mg/g,which was close to the theoretical value 12.99 mg/g,and the adsorption rate was up to 20.33μg/(g·min) Meanwhile,10CuSe/OMBC had strong magnetism that is not permanently magnetized,which could be separated from desulfurization gypsum and recycled many times.Characterization results demonstrated that Se22-,Cu2+and Oβplayed essential roles in the oxidation of Hg0,and Se22-and Se2-can immobilize Hg2+to HgSe.10CuSe/OMBC has important guiding significance for practical application because of its low cost,high performance and low mercury leaching characteristic to form HgSe.
基金the financial support from the LiaoNing Revitalization Talents Program(Grant No.XLYC2403047)the National Natural Science Foundation of China(Grant No.22211530046)+2 种基金the Fundamental Research Funds for the Central Universities(Grant No.DUT23BK022DUT24YG212)the Yingkou Science and Technology Bureau,State Key Laboratory of New Textile Materials and Advanced Processing Technologies(Grant No.FZ2023009)。
文摘Transition metal selenides(TMSs),as promising anode materials for sodium ion batteries(SIBs),still face sluggish Na+diffusion kinetics and severe volume change,resulting in undesirable cycling stability and rate capability.Heterostructure construction is an effective method to improve sodium ion storage in TMSs.Herein,a hierarchical hollow heterostructure of CoSe_(2)@SnSe is precisely designed through a facile coprecipitation process followed by a selenization strategy.The heterostructure constructed by CoSe_(2)and SnSe nanocrystals induces the formation of built-in electric fields and accelerates electron transfer and ion diffusion,thereby improving reaction kinetics significantly.When the as-prepared CoSe_(2)@SnSe composites are employed as anode materials of SIBs,there exhibit ultra-fast electrochemical reaction kinetics and outstanding cycling stability with a high capacity retention of 488.9 mAh g^(-1)at a current density of 2.0 A g^(-1)after 900 cycles.In addition,there still shows an exceptional rate capability of 409.5 mAh g^(-1)at a high current density of 10 A g^(-1).This work provides an effective method for the rational designing of heterostructure anode materials for high-performance SIBs.
基金supported by the National Natural Science Foundation of China(22201244,22374125,21971221 and 21773203)the Yangzhou University Interdisciplinary Research Foundation for Chemistry Discipline of Targeted Support(yzuxk202010)+2 种基金High-Level Entrepreneurial and Innovative Talents Program of Jiangsu‘Qing Lan Project’in Colleges and Universities of Jiangsu ProvinceLvyangjinfeng Talent Program of Yangzhou,China Postdoctoral Science Foundation(2022M722688)。
文摘The polysulfides shuttle effect,sluggish sulfur redox kinetics and the corrosion of the Li anode have become important factors limiting the commercial application of lithium-sulfur batteries(LSBs).Herein,the polyoxometalate(POM)nanoclusters with high catalytic activity and cobalt selenide with strong polarity are initially complemented to construct a PMo_(12)/CoSe_(2)@NC/CNTs multifunctional separator that can simultaneously solve the above problems.A series of experimental and theoretical results demonstrate that the Keggin-type POM,H_(3)PMo_(12)O_(40)nH_(2)O(PMo_(12))nanoclusters could function as catalytic centers for sulfur-involved transformations,with the CoSe_(2)nanoparticles serving as adsorption sites for soluble polysulfides.Accordingly,the assembled battery with the PMo_(12)/CoSe_(2)@NC/CNTs modified separator achieves an initial discharge capacity of 1263.79 mA h g^(-1),maintaining 635.77 mA h g^(-1),with a capacity decay rate of 0.06%per cycle after 500 cycles at 3C.This work provides a strategic approach for incorporating POM nanoclusters with polar periodic nanomaterials in LSB separators,contributing to the development of multifunctional separator materials,thus promoting the advancement of energy storage systems.
基金supported by Guangdong Basic and Applied Basic Research Foundation(Nos.2021A1515110164 and 2022A1515010208)the National Natural Science Foundation of China(No.52207248)the Open Testing Foundation of Analytical&Testing Center of Northwestern Polytechnical University(No.2022T024).
文摘Conversion-alloying anode materials are competitive candidates for high-energy-density sodium-ion batteries(SIBs).However,the sluggish dynamics and severe volume expansion during Na insertion/extraction become the key bottlenecks hindering their application in SIBs.Herein,SnTe nanoparticles are anchored on reduced graphene oxide(rGO)and encapsulated by nitrogen-doped carbon(NC)to construct SnTe@rGO@NC composite as anode for SIBs,where hierarchical confinement effect can provide a buffer area to accommodate huge volume expansion as well as enhance electronic conductivity and Na-ion transfer kinetics behavior,confirmed by density functional theory(DFT)calculation and experimental study.Meanwhile,structural stability and interfacial charge transfer of the composite can be further improved by the strong chemical bonds of C-Sn and C-Te.High-angle annular dark field scanning transmission electron microscopy visually at atomic scale declares that SnTe@rGO@NC proceeds conversion-alloying dual-mechanism for Na-ion storage employing Sn as redox center(4SnTe+23Na^(+)+23e^(-)→Na_(15)Sn_(4)+4Na_(2)Te).Thus,SnTe@rGO@NC architecture displays a high reversible specific capacity of 261.5 mAh·g^(-1)at 50 mA·g^(-1),superior rate capability and excellent cycling stability with long-term lifespan over 1000 cycles at 200 mA·g^(-1).The multi-physicochemical encapsulation strategy sheds light on the development of a high-performance conversion-alloying anode for SIBs.
基金support from the 2BoSS project of the ERA-MIN3 program with the Spanish grant number PCI2022-132985/AEI/10.13039/501100011033funding from the Generalitat de Catalunya 2021SGR01581 and 2021SGR00457+9 种基金the European Union NextGenerationEU/PRTR,the Natural Science Foundation of Chongqing(No.2023NSCQ-MSX1669)the Science and Technology Research Program of Chongqing Municipal Education Commission(No.KJZDK202401110)support of the Supercomputing Center of Lanzhou University,Chinasupported by MCIN with funding from European Union NextGenerationEU(PRTR-C17.I1)by Generalitat de Catalunya(In-CAEM Project)support from the project AMaDE(PID2023-149158OB-C43)funded by MCIN/AEI/10.13039/501100011033/funding from the CSC-UAB PhD scholarship programfunding from Grant IU16-014206(METCAM-FIB)funded by the European Union through the European Regional Development Fund(ERDF)support of the Ministry of Research and Universities,Generalitat de Catalunya。
文摘Lithium-sulfur batteries(LSBs)are a promising candidate for next-generation energy storage solutions.However,challenges such as the shuttling effect and sluggish Li-S reaction kinetics of lithium polysulfides hinder their practical application.In this work,we present a mixed-phase heterostructure comprising Co_(0.85)Se and MoSe_(2),supported on nitrogen-doped carbon polyhedrons(NCP),as an effective sulfur host in the LSB cathode.Through a combination of theoretical calculations and experimental validation,we demonstrate that the Co_(0.85)Se-MoSe_(2)heterointerface significantly enhances electron transfer efficiency,thereby boosting the overall reaction kinetics of the sulfur cathode.As a result,the Co_(0.85)Se-MoSe_(2)/NCP/S electrodes exhibit initial specific capacities exceeding 1500 mAh g^(-1)at 0.1 C and retain 666 m Ah g^(-1)at 3 C,with a capacity fade rate of 0.044%per cycle over 500 cycles at 1.0 C.Notably,even at a high sulfur loading of 3 mg cm^(-2)and a reduced electrolyte volume of 6.7μL mgS^(-1),the Co_(0.85)SeMoSe_(2)/NCP/S electrodes maintain a capacity of 432 mAh g^(-1)after 100 cycles at 0.2 C.
基金supported by the National Natural Science Foundation of China(No.22469018)the Natural Science Basic Research Program of Department of Science and Technology of Shaanxi Province(Nos.2023-JC-ZD-22 and 2023-JC-YB-404)the Scientific Research Startup Program for Introduced Talents of Shaanxi University of Technology(Nos.SLGRCQD2303 and SLGRCQD2306).
文摘Transition metal selenides(TMSs)are effective pre-electrocatalysts and are commonly used in electrochemical processes.During the electrocatalytic oxygen evolution reaction(OER),metal cations in TMSs are in-situ reconstructed and converted into high-valence metal oxyhydroxides.However,a limited understanding of the effects of electro-oxidation and anion leaching has resulted in insufficient theoretical guidance for the rational design of efficient catalysts.Herein,FeSe@NiSe nanorods were fabricated for the OER using a facile hydrothermal selenization method supported on FeNi foam.In-situ Raman spectroscopy and multiple characterization techniques were employed to elucidate the mechanism of FeSe@NiSe surface evolution.Metal cations on the catalyst surface were reconstructed and converted into OER-active species Fe/NiOOH at low potential.As the applied potential increased,electro-oxidation and leaching of Se occurred,resulting in SeO_(4)^(2−)adsorption on the catalyst surface,which further enhanced catalytic activity.As a result,the reconstructed FeSe@NiSe/iron-nickel foam(INF)exhibited exceptional catalytic activity for OER,achieving an ultralow overpotential of 283 mV at a current density of 100 mA·cm^(−2).Notably,the bifunctional FeSe@NiSe/INF electrode facilitated overall water splitting,affording a current density of 10 mA·cm^(−2) only at 1.53 V,even superior to the noble RuO_(2)(+)||Pt/C(−).This work offers valuable insights into the surface evolution and electrocatalytic mechanisms of TMSs.
基金supported by the Science and Technology Innovation Council of Shenzhen(No.KQTD20170810105439418)the National Key R&D Project from Minister of Science and Technology,China(No.2021YFB3200304)+2 种基金National Natural Science Foundation of China(Nos.6237129,52125205,U20A20166,61805015 and 61804011)the Natural Science Foundation of Beijing Municipality(No.Z180011)the Fundamental Research Funds for the Central Universities.
文摘Semiconducting transition-metal dichalcogenides(TMDs)have garnered significant interest due to their unique structures and properties,positioning them as promising candidates for novel electronic and optoelectronic devices.However,the performance of TMDs-based devices is hampered by the suboptimal quality of metal electrodes contacting the atomically thin TMDs layers.Understanding the mechanisms that influence contact quality is crucial for advancing TMDs devices.In this study,we investigated the conductive properties of tungsten selenide(WSe_(2))-based devices with different film thicknesses.Using the transmission line method,a negative correlation between contact resistance and film thickness in multi-electrode devices was revealed.Additionally,repeatability tests conducted at varied temperatures indicated enhanced device stability with increasing film thickness.Theoretical analysis,supported by thermionic emission theory and thermal simulations,suggests that the degradation in electrical properties is primarily due to the thermal effect at the contact interface.Furthermore,we found that van der Waals contacts could mitigate the thermal effect through a metal transfer method.Our findings elucidate the critical role of contact resistance in the electronic performance of 2D material-based field-effect transistors(FETs),which further expands their potential in the next generation of electronic and optoelectronic devices.
基金supported by the National Natural Science Foundation of China(No.22075217)the Key Research and Development Program of Hubei Province(No.2023BAB113)the Natural Science Foundation of Hubei Province of China(Nos.2022CFA001 and 2023CFA088).
文摘Nickel selenides have been studied as potential anode materials for sodium-ion batteries due to their high theoretical capacity.However,the low electrical conductivity and the large volumetric variation during the charging/discharging process greatly reduce the specific capacity and cycling lifespan of the batteries.In this paper,a simple strategy to fabricate NiSe nanoparticles enclosed in carbon hollow nanofibers(NiSe/C@CNF)is proposed,involving the preparation of Ni-precursor nanofibers by electrospinning,the coating of polydopamine and the formation of NiSe/C@CNF by calcination and selenization.The combination of NiSe nanoparticles and porous carbon hollow nanofibers creates a strong conductive environment,which enhances the dynamic ability of sodium-ion transport and improves charge storage capacity.The fabricated NiSe/C@CNF material exhibits excellent performance.It demonstrates a high rate capability,with specific capacities of 406.8 and 300.1 mAh·g^(-1)at 0.1 and 5.0 A·g^(-1),respectively.These results highlight the potential of NiSe/C@CNF as an anode material for sodium-ion batteries,offering a large capacity and long life.
基金supported by the National Natural Science Foundation of China(Nos.52130101 and 52271217)the Project of Science and Technology Development Plan of Jilin Province in China(Nos.20210402058GH,20220201114GX).
文摘Lithium-sulfur batteries(LSBs)are considered as the promising solution to replace conventional lithium-ion batteries due to satisfactory energy density.In recent times,the LSBs field has been found to face some difficulties in exploring practical applications in which cycling stability and cycle life are awful owing to the shuttling effect of lithium polysulfides(LiPSs)and low sulfur utilization.In this work,by synthesizing Co_(3)Se_(4) nanoparticles onto N-doped carbon(NC)polyhedra interconnected with carbon nanotubes(CNTs),NC@Co_(3)Se_(4)/CNTs is proposed as a multifunctional sulfur carrier.The Co_(3)Se_(4) nanoparticles fleetly catalyze the conversion of LiPSs and availably immobilize LiPSs.Meanwhile,the NC polyhedral skeleton enhances the electronic conductivity of active sulfur,while the CNTs facilitate Li+diffusion and supply a mass of conductive channels.Density-functional theory(DFT)calculations demonstrate the relevant mechanisms.That is to say,the NC@Co_(3)Se_(4)/CNTs benefit from the synergistic effect of Co_(3)Se_(4) nanoparticles(highly catalytic ability and strong adsorbability for LiPSs)and the special carbonaceous structure,rapidly converting LiPSs and inhibiting the shuttle of LiPSs.Therefore,lithium-sulfur battery assembled with S/NC@Co_(3)Se_(4)/CNTs cathode as well as nitrogen and sulfur co-doped carbon-coated polypropylene(N,S-C/PP)separator possesses a high initial discharge capacity of 1413 mAh·g-1 at 0.12C and persistently circulates for 1000 cycles at 1C with a capacity attenuation rate per cycle of 0.034%.This work provides a realistic idea for the use of transition metal selenide in the field of high-performance LSBs.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.2018R1A6A1A03025708).
文摘Trimetallic selenides have emerged as a promising electrode for wearable supercapacitors applications,due to their high electrical conductivity,rich redox activity,structural robustness,and porosity.In this report,a trimetallic nickel–magnesium-manganese selenide(NMMSe)electrode with a well-defined nanosphere morphology was prepared using a low-cost and rapid electrodeposition technique.The electrochemical performance of the NMMSe electrodes was systematically investigated as a positive electrode.The NMMSe electrode prepared with a deposition time of 200 s(denoted as NMMSe-200)revealed a high areal/specific capacity of 439.4μAh cm^(−2)/225.6 mA h g^(−1) at 4 mA cm^(–2),along with excellent cycling stability.To further investigate the effect of deposition time on the nanostructure evaluation and electrochemical behavior,additional NMMSe electrodes were synthesized at the growth times of 100 and 300 s.For the negative electrode,activated carbon derived from pistachio shell waste(i.e.,porous activated carbon(PAC))was employed,demonstrating a high areal capacitance of 913.4 mF cm^(−2) and an excellent surface area of 320.6 m^(2)/g.Finally,a semi-solid-state hybrid capacitor(HC)cell was assembled using NMMSe-200 as the positive(+)electrode and PAC as the negative(-)electrode.The resulting NMMSe//PAC/nickel foam HC cell delivered an impressive areal capacitance of 928.8 mF cm^(−2) at 2 mA cm^(–2),a high energy density of 338.5μWh cm^(–2)(56.4 Wh kg^(−1)),and exceptional cycling stability.These results highlight the strong potential of NMMSe-200 electrodes for high-performance,wearable energy storage systems.
