查看更多>>摘要：With the fast development of technology for the treatment of tumor and bacteria,photo-therapeutic strate-gies emerge as a kind of highly effective and common treatment,but the low tissue penetration depth of light limits their development.Sonodynamic therapy(SDT),as an efficient and non-invasive treatment,attracts more people's attention due to the inherent property of high tissue penetration.The soft tissue penetration depth of ultrasound(US)can even reach more than 10 cm,which has great advantage over that of light.Therefore,many sonosensitizers are studied and applied to SDT-based therapy.Metal-based inorganic nanocrystals are able to generate more reactive oxygen species(ROS)due to the special composition and band structure.The representative achievements and the specific functions of the nanocrystals sonosensitizers are summarized in this work,and the relationship of structure/composition-SDT performance and the internally regulated composite is revealed.Syner-gistic effects of SDT in combination with other therapeutic modalities are mainly highlighted.At the same time,the critical and potential issues and future perspectives are addressed.
查看更多>>摘要：Solid-state flexible supercapacitors(SCs)have many advantages of high specific capacitance,excellent flexibility,fast charging and discharging,high power density,environmental friendliness,high safety,light weight,ductility,and long cycle stability.They are the ideal choice for the development of flexible energy storage technology in the future,and provide a good prospect for energy storage applications.At present,solid-state flexible SCs are widely used for portable electronic equipment and wearable energy storage equipment,the research of them has become the focus of a growing number of researchers.Electrode material is the key part of SCs and always determines the electrochemical performance of SCs.It has been a hotspot and focus of research.Vanadium-based compounds are considered to be a promising electrode material for SCs because of variable valence,open struc-ture,high theoretical capacity,and low price.Therefore,this study first gives an overview of solid-state flexible SCs,then reviews the current research status of vanadium-based electrode materials in solid-state flexible SCs,and proposes some strategies to solve some problems of vanadium-based electrode materials.
查看更多>>摘要：The high-energy-density and low-cost features endow lithium-sulfur batteries with broad application pro-spects.However,many drawbacks,especially the detri-mental shuttle effect,have hindered the further development of LSBs.In response,a lot of new structures have been applied to suppress the shuttle effect and pro-mote the development of LSBs.Recently,vacancy engi-neering has gained the attention of researchers due to its unique electronic structure.This review aims to analyze the application of vacancy engineering in LSBs.Firstly,the electrochemistry of LSBs has been systematically dis-cussed and the existing challenges as well as improvement tactics of LSBs have also been presented.Subsequently,the preparation methods and characterization technologies of various vacancies are summarized,including oxygen vacancies,sulfur vacancies,selenium vacancies,other anion vacancies,cation vacancies,etc.The latest applications of vacancy engineering in LSBs are also summarized in this review.Finally,some prospects and insights for further investigation and practical application of vacancy engineering in LSBs are put forward.
查看更多>>摘要：To improve the efficiency of oxygen electroly-sis,exploiting bifunctional electrocatalysts with excellent activity and stability is extremely important due to the four-electron transfer dynamics of oxygen evolution reac-tion(OER)and oxygen reduction reaction(ORR).Herein,a series of yolk-shell hollow polyhedrons(YHPs)embed-ded with NiCoFe ternary alloy and metal oxides,which are named YHP-x(x=1,2,3,4),were reported.By controlled etching multi-layered zeolitic imidazolate frameworks and following pyrolytic integration,YHPs are endowed with mass transfer tunnels,accessible inner active sites,and good electrical conductivity.Due to the synergetic effect of the alloy,metal oxides and the yolk-shell structure,YHP-1 exhibits excellent ORR performance with a half-wave potential of 0.79 V and YHP-2 displays superior OER performance with a low overpotential of 257 mV at 10 mA cm-2.The strategy described in this work can be extended to a number of hollow/yolk-shell electrocatalysts for water splitting and metal-air batteries.
查看更多>>摘要：The engineering of the electronic configurations of active sites,together with the production of more accessible active sites through heterostructure design,has been established as a forceful methodology for boosting water electrolysis performance.Herein,a facile approach is developed to fabricate well-dispersed MoO2 and WO2 nanoparticles with abundant heterointerfaces entrapped in N,P-doped carbon nanofibers(referred to as MoO2/WO2@N,P-CNFs hereafter)as hydrogen evolution reaction(HER)electrocatalysts in alkaline and acidic electrolytes.Extensive spectroscopic analyses and theoretical findings manifest that the heterointerface formed by the work function modulation of MoO2/WO2 triggers the sponta-neous electron redistribution from MoO2 to WO2 and a built-in electric field,which is essential to promote water adsorption,optimize the H-intermediate adsorption energy,result in the enhanced charge transfer efficiency,and ulti-mately increase the intrinsic HER activity.Simultaneously,the intimate confinement of MoO2/WO2 heterostructures in the porous carbon substrate can restrain the active sites from unfavorable coarsening and detachment,thus ensur-ing facilitated HER kinetics and outstanding structural robustness.As a result,MoO2/WO2@N,P-CNFs exhibit superior catalytic HER performance in acidic and basic solutions,requiring 118 and 95 mV overpotentials to achieve 10 mA·cm-2,respectively,surpassing a number of reported non-noble metal-based electrocatalysts.This work provides guidelines for the rational design and construction of special metallic heterocomponents with optimized interfacial electronic structure for various electrochemical technologies.
查看更多>>摘要：Electrocatalytic oxygen reduction(ORR)via the 2e-pathway to form H2O2 in acidic medium has attracted extensive attention.However,the low activity,insufficient selectivity and high cost of catalysts have been the bottlenecks.Herein,CoSe2 with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe2 phase transition from orthorhombic to cubic phase with more Se deficiency.The cubic phase CoSe2 with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H2O2.The onset potential is as low as 0.73 V vs.reversible hydrogen electrode(RHE),the H2O2 selectivity is 84％(0 V vs.RHE),and the average electron transfer number is about 2.3.Furthermore,the H2O2 yield measured using a flow cell is as high as 115.92 mmol·gcat.-1·h-1 and the Faradaic efficiency is 70％at 0 V vs.RHE,which presents high potential in electrocatalytic acidic ORR to H2O2 and organic pollutant degradation using the electron-Fenton process.
查看更多>>摘要：Herein,a novel single-atomic Pt doping and interface-rich CoS/Co(OH)2(Pt-CoS/Co(OH)2/C)electro-catalyst has been successfully prepared.Benefiting from precise regulation of d-orbital electronic structure modu-lation on Co site,Pt-CoS/Co(OH)2/C exhibited remarkable HER activity and high stability for hydrogen evolution in splitting both water(73 mV@10 mA.cm-2)and seawater(87 mV@10 mA.cm-2).Notably,atomic Pt doping was introduced into CoS/Co(OH)2,which could produce local unbalanced Coulombic force and significantly increased the number of S vacancies,and then expose abundant Co sites.Meantime,Co(OH)2 in Pt-CoS/Co(OH)2/C could act as the adsorption sites for H2O in hydrogen evolution reaction process.Density functional theory results also proved that atomic Pt doping,S vacancies and Co(OH)2 coupling could result in the formation of enriched elec-tronic Co sites and optimize dz2 orbital electronic structure,and then realize the depth upward shift of d-band center and enhance the adsorption of H*on Co sites.
查看更多>>摘要：Developing bifunctional catalysts that can cat-alyze both oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is pivotal to commercializing large-scale water splitting.Herein,a novel hollow nano-triangle composed of NiFe LDH-CoMoSx heterojunction(H-CMSx@NiFe LDH)is proposed as a highly efficient bifunctional electrocatalyst for both OER and HER.To fabricate a heterojunction system,ultra-thin nickel-iron layered double hydroxide(NiFe LDH)nanosheets are uniformly electrodeposited onto a metal-organic frame-work-derived hollow CoMoSx nanotriangle.The strong coupling of CoMoSx and NiFe LDH catalysts forms the intimate heterojunction interfaces to facilitate interfacial charge transfer,which is favorable to enhance the bifunc-tional catalytic activity.Moreover,the large void of CoMoSx nanotriangles and interconnected ultra-thin NiFe LDH nanosheets result in good electrolyte penetration and gas release.Therefore,the as-prepared H-CMSx@NiFe LDH on nickel foam(NF)exhibits an impressive catalytic activity and durability for OER and HER activities,delivering a current density of 100 mA·cm-2 at the small overpotentials of 214 and 299 mV in OER and HER,respectively.Meanwhile,H-CMSx@NiFe LDH/NF proves to be an effective electrode for an alkaline electrolyzer,as a voltage of only 1.99 V is enough to achieve a current density voltage of only 1.99 V is enough to achieve a current density of 400 mA·cm-2 with no degradation in performance over 50 h.
查看更多>>摘要：Constructing a S-scheme heterojunction with tight interface contact and fast charge transfer is beneficial to improving the photocatalytic hydrogen evolution per-formance.Herein,a unique one-dimensional(1D)/two-di-mensional(2D)S-scheme heterojunction containing 1D Sb2S3 nanorods and 2D ZnIn2S4 with affluent sulfur vacancies(denoted as Sv-ZnIn2S4@Sb2S3)was designed.The introduced sulfur vacancy can promote the effective adsorption of H+for the following interfacial hydrogen-evolution reaction.Furthermore,the larger contact area and stronger electron interaction between Sb2S3 and ZnIn2S4 effectively inhibits the recombination of photo-generated electron-hole pairs and abridges the migration distance of charges.As a result,the optimal Sv-ZnIn2S4@Sb2S3 sam-ple achieves H2 evolution activity of 2741.3 mol·h-1·g-1,which is 8.6 times that of pristine ZnIn2S4 and 3.0 times that of the Sv-ZnIn2S4 samples.Based on the experimental result,the photo-reactivity S-scheme mechanism of hydrogen evolution from water splitting with Sv-ZnIn2S4@Sb2S3 is proposed.This work provides an effective method for developing S-scheme heterojunction composites of transition metal sulfide with high hydrogen evolution performance.
查看更多>>摘要：Natural minerals,abundant and easily obtained through simple physical processing,offer a cost-effective and environmentally friendly solution for dyeing wastew-ater disposal and air pollution treatment.This study investigates the photocatalytic removal of NO using natural different types of dyes,loaded on natural sand,under vis-ible light illumination.By examining various coating concentrations of dyes and sand weights,we discovered that sand loaded with Rhodamine B(RhB)exhibits high activity for the photo-oxidation of NO.A combination results of X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),Fourier transform infrared spec-troscopy(FTIR)and thermogravimetric(TG)analyses confirm the presence of SiO2,CaCO3,Al2O3 and iron oxides as the main components of the sand.Furthermore,studying RhB-loaded individual components reveals that CaCO3 plays a crucial role in enhancing the NO removal rate.Experimental results and theoretical calculations demonstrate the establishment of a directional charge transfer channel from CaCO3 to RhB,facilitating the adsorption and activation of molecular NO and O2.This work not only promotes the utilization of natural mineral resources but also enriches the fields of environmental photochemistry and semiconductor photocatalysis.
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