As a new generation of materials/structures,heterostructure is characterized by heterogeneous zones with dramatically different mechanical,physical or chemical properties.This endows heterostructure with unique interf...As a new generation of materials/structures,heterostructure is characterized by heterogeneous zones with dramatically different mechanical,physical or chemical properties.This endows heterostructure with unique interfaces,robust architectures,and synergistic effects,making it a promising option as advanced biomaterials for the highly variable anatomy and complex functionalities of individual patients.However,the main challenges of developing heterostructure lie in the control of crystal/phase evolution and the distribution/fraction of components and structures.In recent years,additive manufacturing techniques have attracted increasing attention in developing heterostructure due to the unique flexibility in tailored structures and synthetic multimaterials.This review focuses on the additive manufacturing of heterostructure for biomedical applications.The structural features and functional mechanisms of heterostructure are summarized.The typical material systems of heterostructure,mainly including metals,polymers,ceramics,and their composites,are presented.And the resulting synergistic effects on multiple properties are also systematically discussed in terms of mechanical,biocompatible,biodegradable,antibacterial,biosensitive and magnetostrictive properties.Next,this work outlines the research progress of additive manufacturing employed in developing heterostructure from the aspects of advantages,processes,properties,and applications.This review also highlights the prospective utilization of heterostructure in biomedical fields,with particular attention to bioscaffolds,vasculatures,biosensors and biodetections.Finally,future research directions and breakthroughs of heterostructure are prospected with focus on their more prospective applications in infection prevention and drug delivery.展开更多
The d-band states of catalytic materials participate in adsorbing reactive intermediate species and determine the catalytic behaviors in CO_(2)reduction reactions.However,surface d-band states relating to the photocat...The d-band states of catalytic materials participate in adsorbing reactive intermediate species and determine the catalytic behaviors in CO_(2)reduction reactions.However,surface d-band states relating to the photocatalytic CO_(2)reduction reactions behaviors are rarely concerned.Herein,a slightly amount of Cd^(2+)is decorated on the surface of(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material(Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4))to tune the surface d-band states for improved CO_(2)+2reduction reactions.The Cd/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)is fabricated via the facile ions-exchange method to make that slightly Zn2+is substituted by Cd^(2+).The Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)exhibits much enhanced photocatalytic activity in CO_(2)reduction reactions to produce CO and water splitting to produce H_(2).Physical characterizations show that the energy band structure is not changed obviously.Density functional theory reveals that Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)possesses a closer shift of d-band center to Fermi level than(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4),suggesting easier adsorption of CO_(2)reduction reactive intermediates after Cd^(2+)decoration.Further calculations confirm that a relatively reduced adsorption Gibbs energy of reactive intermediates in CO_(2)reduction reaction is required on Zn atoms in Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material,benefiting the photocatalytic CO_(2)reduction reactions.This work engineers surface d-band states by surface Cd^(2+)decoration,which gives an effective strategy to design highly efficient photocatalysts for syngas production.展开更多
The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO...The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO nanocrystals with doping small amount of La^(3+)were used to regulate d-band states for promoting OER activity.Density of states calculations based on density functional theory revealed that La^(3+)doping produced upper shift of d-band center,which would induce stronger electronic interaction between surface Ni atoms and species of oxygen evolution reaction intermediates.Further density functional theory calculation illustrated that La^(3+)doped NiO possessed reduced Gibbs free energy in adsorbing species of OER intermediate.Predicted by theoretical calculations,trace La^(3+)was introduced into crystal lattice of NiO nanoparticles.The La^(3+)doped NiO nanocrystal showed much promoted OER activity than corresponding pristine NiO product.Further electrochemical analysis revealed that La^(3+)doping into NiO increased the intrinsic activity such as improved active sites and reduced charge transfer resistance.The in-situ Raman spectra suggested that NiO phase in La^(3+)doped NiO could be better maintained than pristine NiO during the OER.This work provides an effective strategy to tune the d-band center of NiO for efficient electrocatalytic OER.展开更多
Electrocatalytic conversion of carbon dioxide to high value-added chemicals is a promising method for solving the energy crisis and global warming.Electrochemical active metal-containing conjugated polymers have been ...Electrocatalytic conversion of carbon dioxide to high value-added chemicals is a promising method for solving the energy crisis and global warming.Electrochemical active metal-containing conjugated polymers have been widely studied for heterogeneous carbon dioxide reduction.In the present contribution,we designed and synthesized a stable cobalt phthalocyanine-based conjugated polymer,named CoPPc-TFPPy-CP,and also explored its electro-catalytic application in carbon dioxide reduction to liquid products in an aqueous solution.In the catalyst,cobalt phthalocyanine acts as building blocks connected with 1,3,6,8-tetrakis(4-formyl phenyl)pyrenes via imine-linkages,leading to mesoporous formation polymers with the pore size centered at 4.1nm.And the central co-balt atoms shifted to a higher oxidation state after condensation.With these chemical and structural natures,the catalyst displayed a remarkable electrocatalytic CO_(2) reduction performance with an ethanol Faradaic efficiency of 43.25%at-1.0V vs RHE.While at the same time,the electrochemical reduction process catalyzed by cobalt phthalocyanine produced only carbon monoxide and hydrogen.To the best of our knowledge,CoPPc-TFPPy-CP is the first example among organic polymers and metal-organic frameworks that produces ethanol from CO_(2) with a remarkable selectivity.展开更多
The development of superconducting joining technology for reacted magnesium diboride(MgB_(2))conductors remains a critical challenge for the advancement of cryogen-free MgB_(2)-based magnets for magnetic resonance ima...The development of superconducting joining technology for reacted magnesium diboride(MgB_(2))conductors remains a critical challenge for the advancement of cryogen-free MgB_(2)-based magnets for magnetic resonance imaging(MRI).Herein,the fabrication of superconducting joints using reacted carbon-doped multifilament MgB_(2)wires for MRI magnets is reported.To achieve successful superconducting joints,the powder-in-mold method was employed,which involved tuning the filament protection mechanism,the powder compaction pressure,and the heat treatment condition.The fabricated joints demonstrated clear superconducting-to-normal transitions in self-field,with effective magnetic field screening up to 0.5 T at 20 K.To evaluate the interface between one of the MgB_(2)filaments and the MgB_(2)bulk within the joint,serial sectioning was conducted for the first time in this type of superconducting joint.The serial sectioning revealed space formation at the interface,potentially caused by the volume shrinkage associated with the MgB_(2)formation or the combined effect of the volume shrinkage and the different thermal expansion coefficients of the MgB_(2)bulk,the filament,the mold,and the sealing material.These findings are expected to be pivotal in developing MgB_(2)superconducting joining technology for MRI magnet applications through interface engineering.展开更多
The lattice-oxygen-mediated mechanism is considered as a reasonable mechanism for the electrochemical catalytic oxygen evolution reaction(OER)of NiFe layered double hydroxides(LDHs).A NiFe LDH with distinct lattice co...The lattice-oxygen-mediated mechanism is considered as a reasonable mechanism for the electrochemical catalytic oxygen evolution reaction(OER)of NiFe layered double hydroxides(LDHs).A NiFe LDH with distinct lattice contraction and microcrystallization was synthesized via a simple one-step method using sodium gluconate.The lattice contraction is attributed to the interaction of carbon in sodium gluconate and iron in NiFe LDH.The NiFe LDH with optimized microcrystallization and lattice contraction shows a low overpotential of 217 mV at a current density of 10 mA cm^(−2) and excellent durability of 20 h at a high current density of 100 mA cm^(−2).The results revealed that a contractive metal–oxygen bond could boost the intrinsic activity of active sites and the microcrystallization promotes an increase in the number of active sites in terms of unit area.The chemical environment of oxygen elemental characterization and resistance at different chronopotentiometry times confirm that the lattice oxygen element is indeed involved in the process of OER,supporting the lattice-oxygen-mediated mechanism of NiFe LDH.Density functional theory calculations reveal that contractive metal–oxygen bonds induced a reduction of the adsorption energy barrier of intermediate products,thus improving the intrinsic catalytic activity.The special characteristics of microcrystallization and lattice contraction of NiFe LDH provide a strategy to improve both the number and the intrinsic activity of active sites in a versatile manner.展开更多
To control the power hierarchy design of lithium-ion battery(LIB)builtup sets for electric vehicles(EVs),we offer intensive theoretical and experimental sets of choice anode/cathode architectonics that can be modulate...To control the power hierarchy design of lithium-ion battery(LIB)builtup sets for electric vehicles(EVs),we offer intensive theoretical and experimental sets of choice anode/cathode architectonics that can be modulated in full-scale LIB built-up models.As primary structural tectonics,heterogeneous composite superstructures of full-cell-LIB(anode//cathode)electrodes were designed in closely packed flower agave rosettes TiO2@C(FRTO@C anode)and vertical-star-tower LiFePO4@C(VST@C cathode)building blocks to regulate the electron/ion movement in the three-dimensional axes and orientation pathways.The superpower hierarchy surfaces and multi-directional orientation components may create isosurface potential electrodes with mobile electron movements,in-to-out interplay electron dominances,and electron/charge cloud distributions.This study is the first to evaluate the hotkeys of choice anode/cathode architectonics to assemble different LIB-electrode platforms with high-mobility electron/ion flows and high-performance capacity functionalities.Density functional theory calculation revealed that the FRTO@C anode and VST-(i)@C cathode architectonics are a superior choice for the configuration of full-scale LIB built-up models.The integrated FRTO@C//VST-(i)@C full-scale LIB retains a huge discharge capacity(~94.2%),an average Coulombic efficiency of 99.85%after 2000 cycles at 1 C,and a high energy density of 127 Wh kg?1,thereby satisfying scale-up commercial EV requirements.展开更多
Immobilizing biocomponents on solid surfaces is a critical step in the development of new devices for future biological, medical, and electronic applications. Therefore, numerous integrated films were recently develop...Immobilizing biocomponents on solid surfaces is a critical step in the development of new devices for future biological, medical, and electronic applications. Therefore, numerous integrated films were recently developed by immobilizing different proteins or enzymes on electrode surfaces. In this work, hemeproteins were safely immobilized onto macroporous nickel-based electrodes while maintaining their functionality.Such modified electrodes showed interesting pseudo-capacitive behavior. Among hemeproteins, hemoglobin(Hb) film has a higher electrochemical performance and greater charge/discharge cycling stability than myoglobin(Mb) and cytochrome C(Cyt C). The heme group in an alkaline medium could induce the formation of superoxides on the electrode surface. These capacitive features of hemeprotein-Ni electrode were related to strong binding sites between hemeproteins and porous Ni electrode, the accumulation of superoxide or radicals on the Ni surface, and facile electron transfer and electrolyte diffusion through the three-dimensional macroporous network. Thus, these new protein-based supercapacitors have potential use in free-standing platform technology for the development of implantable energy-storage devices.展开更多
In recent decades,silicon photonics has attracted much attention in telecom and data-com areas.Constituted of high refractive-index contrast waveguides on silicon-on-insulator(SOI),a variety of integrated photonic pas...In recent decades,silicon photonics has attracted much attention in telecom and data-com areas.Constituted of high refractive-index contrast waveguides on silicon-on-insulator(SOI),a variety of integrated photonic passive and active devices have been implemented supported by excellent optical properties of silicon in the mid-infrared spectrum.The main advantage of the silicon photonics is the ability to use complementary metal oxide semiconductor(CMOS)process-compatible fabrication technologies,resulting in high-volume production at low cost.On the other hand,explosively growing traffic in the telecom,data center and high-performance computer demands the data flow to have high speed,wide bandwidth,low cost,and high energy-efficiency,as well as the photonics and electronics to be integrated for ultra-fast data transfer in networks.In practical applications,silicon photonics started with optical interconnect transceivers in the data-com first,and has been now extended to innovative applications such as multi-port optical switches in the telecom network node and integrated optical phased arrays(OPAs)in light detection and ranging(LiDAR).This paper overviews the progresses of silicon photonics from four points reflecting the recent advances mentioned above.CMOS-based silicon photonic platform technologies,applications to optical transceiver in the data-com network,applications to multi-port optical switches in the telecom network and applications to OPA in LiDAR system.展开更多
Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2...Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2)RR)is still challenging owing to the sluggish kinetics or unfavorable thermodynamics for basic chemical processes of CO_(2)RR,such as adsorption,activation,conversion and product desorption.To overcome these shortcomings,recent works have demonstrated that surface engineering of semiconductors,such as introducing surface vacancy,surface doping,and cocatalyst loading,serves as effective or promising strategies for improved photocatalytic CO_(2)RR with high activity and selectivity.The essential reason lies in the activation and reaction pathways can be optimized and regulated through the reconstruction of surface atomic and electronic structures.Herein,in this review,we focus on recent research advances about rational design of semiconductor surface for photocatalytic CO_(2)RR.The surface engineering strategies for improved CO_(2)adsorption,activation,and product selectivity will be reviewed.In addition,theoretical calculations along with in situ characterization techniques will be in the spotlight to clarify the kinetics and thermodynamics of the reaction process.The aim of this review is to provide deep understanding and rational guidance on the design of semiconductors for photocatalytic CO_(2)RR.展开更多
Strategy of anchoring alloy nanoparticles made up of the efficient catalytic element(e.g.,Ni,Fe)on dodecyl sulfate(DS^(-))-intercalated NiFe layered double hydroxides(DS^(-)-NiFe LDH)obtained by a convenient one-step ...Strategy of anchoring alloy nanoparticles made up of the efficient catalytic element(e.g.,Ni,Fe)on dodecyl sulfate(DS^(-))-intercalated NiFe layered double hydroxides(DS^(-)-NiFe LDH)obtained by a convenient one-step hydrothermal coprecipitation method for essentially enhancing oxygen evolution reaction(OER)performance was proposed.The results of structural characterization indicate Pt_(2)FeNi alloy nanoparticles evenly distribute on the surface of DS^(-)-NiFe LDH.The sizes of the Pt_(2)FeNi nanoparticles,closely related to their OER performance,could be wellcontrolled by adjusting the amount of H;PtCl;addition.The composite structure of as-prepared product was stable during processes of synthesis,exfoliation,self-assembly,and subsequent electrocatalytic OER.Rigorous electrochemical test proving the contributing catalytic active sites was located at the interface between Pt_(2)FeNi and DS^(-)-NiFe LDH,and the Ni and Fe were the major active elements while O atoms are adsorption sites.The formation of Pt_(2)FeNi nanoparticles could greatly prompt the reduction of Tafel slope.The best-performing Pt_(2)FeNi/DS^(-)-NiFe LDH with a Pt content of 0.98 wt%achieved low overpotential of 204 mV at 10 mA cm^(-2)and 262 mV at 50 mA cm^(-2).This work provides a convenient and effective strategy to create additional active sites for enhancing OER performance of NiFe LDH and make contribution to its wide application.展开更多
The sensing of a flame can be performed by using wide-bandgap semiconductors, which offer a high signal-to-noise ratio since they only response the ultraviolet emission in the flame. Diamond is a robust semiconductor ...The sensing of a flame can be performed by using wide-bandgap semiconductors, which offer a high signal-to-noise ratio since they only response the ultraviolet emission in the flame. Diamond is a robust semiconductor with a wide-bandgap of 5.5 e V, exhibiting an intrinsic solar-blindness for deep-ultraviolet(DUV) detection. In this work, by using a submicron thick boron-doped diamond epilayer grown on a type-Ib diamond substrate, a Schottky photodiode device structure- based flame sensor is demonstrated. The photodiode exhibits extremely low dark current in both forward and reverse modes due to the holes depletion in the epilayer. The photodiode has a photoconductivity gain larger than 100 and a threshold wavelength of 330 nm in the forward bias mode. CO and OH emission bands with wavelengths shorter than 330 nm in a flame light are detected at a forward voltage of-10 V. An alcohol lamp flame in the distance of 250 mm is directly detected without a focusing lens of flame light.展开更多
To effectively alleviate the ever-increasing energy crisis and environmental issues,clean and sustainable energy-related materials as well as the corresponding storage/conversion devices are in urgent demand.Silicon(S...To effectively alleviate the ever-increasing energy crisis and environmental issues,clean and sustainable energy-related materials as well as the corresponding storage/conversion devices are in urgent demand.Silicon(Si) with the second most elemental abundance on the crust in the form of silicate or silica(SiO_(2)) minerals,is an advanced emerging material showing high performance in energy-related fields(e.g.batteries,photocatalytic hydrogen evolution).For the improved performance in industry-scale applications,Si materials with delicate nanostructures and ideal compositions in a massive production are highly cherished.On account of the reserve,low cost and diverse micro-nanostructures,silicate minerals are proposed as promising raw materials.In the article,crystal structures and the reduction approaches for silicate minerals,as well as recent progress on the as-reduced Si products for clean energy storage/conversion,are presented systematically.Moreover,some cutting-edge fields involving Si materials are discussed,which may offer deep insights into the rational design of advanced Si nanostructures for extended energy-related fields.展开更多
For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectu...For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectures,3D networks,or aerogels.The intersupported structure of porous monolithic 3D graphene(3DG)can prevent aggregation or restacking of graphene individuals,and the interconnected sp^(2) network of 3DG not only can provide the highway for the transport of electron/phonon but also can present continual cavities/channels for mass transfer.This review summarizes the synthesis methodology of 3DG porous monoliths and highlights the application for electric double-layer capacitors.Present challenges and future prospects about the manufacture and application of 3DG are also discussed.展开更多
It is demonstrated experimentally and confirmed theoretically that highly defective boron nitride showed outstanding performance for oxidative dehydrogenation of ethylbenzene.The catalyst is derived from carbon-doped ...It is demonstrated experimentally and confirmed theoretically that highly defective boron nitride showed outstanding performance for oxidative dehydrogenation of ethylbenzene.The catalyst is derived from carbon-doped hexagonal boron nitride nanosheets synthesized via a two-step reaction when participating the oxidative dehydrogenation reaction.The first step yields a polymeric precursor with the atomic positions of B,C,N relatively constrained,which is conducive for the formation of carbon atomic clusters uniformly dispersed throughout the BN framework.During the oxidative dehydrogenation of ethylbenzene to styrene,the nanoscale carbon clusters are removed and highly defective boron nitride(D-BN)is obtained,exposing boron-rich zigzag edges of BN that act as the catalytic sites.The catalytic performance of D-BN is therefore remarkably better than un-doped h-BN.Our results indicate that dispersed C-doping in h-BN is highly effective in terms of defect formation and resultant enhanced activity in oxidative dehydrogenation reactions.展开更多
Aprotic lithium–oxygen batteries(LOBs)have been recognized as novel energy storage devices for their outstanding specific energy density,while the large discharge/charge overpotential is a tough barrier to be overcom...Aprotic lithium–oxygen batteries(LOBs)have been recognized as novel energy storage devices for their outstanding specific energy density,while the large discharge/charge overpotential is a tough barrier to be overcome.Here,hetero-structured MoS_(2)/ZnIn_(2)S_(4) nanosheets have been prepared to capture visible light and the generated charge carriers are utilized for promoting both the oxygen reduction reaction and the oxygen evolution reaction.With the light illumination in the discharge process,the abundant photo-inspired electrons serve as the reaction sites to promote the reduction of O_(2) into LiO_(2) which is finally deposited as Li_(2)O_(2).On the contrary,the generated holes in the valence band can contribute to the low oxidization potential of Li_(2)O_(2) during the charge process.It delivers a low charge potential of 3.29 V,with an excellent resulting energy efficiency of 96.7%,much superior to that of 69.2%in the dark condition.It is noted that the involvement of photoelectrons has influenced the growth of Li_(2)O_(2) films on the MoS_(2)/ZnIn_(2)S_(4) nanosheets through the surface-adsorption pathway.The insights from the theoretical calculation confirm that the photoelectrons favor the absorption of LiO_(2) and the formation of the Li_(2)O_(2) film through the surface route.Therefore,this paper provides a deeper understanding of the mechanism of photoinspired charge carriers in LOBs and will enable further exploration of photo-involved energy storage systems.展开更多
A novel hole-transport material(HTM)based on an anthradithiophene central bridge named BTPA-7 is developed.In comparison to spiro-OMeTAD(2,2’,7,7’-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9’-spirobifluorene),the sy...A novel hole-transport material(HTM)based on an anthradithiophene central bridge named BTPA-7 is developed.In comparison to spiro-OMeTAD(2,2’,7,7’-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9’-spirobifluorene),the synthetic steps of BTPA-7 are greatly reduced from 6 to 3 and the synthetic cost of BTPA-7 is nearly a half that of spiro-OMeTAD.Moreover,BTPA-7 exhibits a relatively lower conductivity but higher hole mobility and higher glass transition temperature(Tg)than spiro-OMeTAD.Compared with the photovolatic performance for spiro-OMeTAD,FA0.85MA0.15PbI3 and MAPbI3 PSC devices based on BTPA-7 exhibit slightly lower PCEs with the values of 17.58%(18.88%for spiro-OMeTAD)and 11.90%(13.25%for spiro-OMeTAD),respectively.Nevertheless,a dramatically higher JSC of PSC based on BTPA-7is achieved,which arises from the higher hole mobility of BTPA-7.In addition,the relatively hydrophobic character of BTPA-7 eventually enhances the PSC device stability.Lower cost,higher hole mobility,higher Tg,satisfactory photovoltaic performance,and superior device stability of BTPA-7 can be utilized as a substitute for spiro-OMeTAD in PSCs.展开更多
Due to the growing demand for clean and renewable hydrogen fuel,there has been a surge of interest in electrocatalytic water-splitting devices driven by renewable energy sources.However,the feasibility of self-driven ...Due to the growing demand for clean and renewable hydrogen fuel,there has been a surge of interest in electrocatalytic water-splitting devices driven by renewable energy sources.However,the feasibility of self-driven water splitting is limited by inefficient connections between functional modules,lack of highly active and stable electrocatalysts,and intermittent and unpredictable renewable energy supply.Herein,we construct a dualmodulated three-dimensional(3D)NiCo_(2)O_(4)@NiCo_(2)S_(4)(denoted as NCONCS)heterostructure deposited on nickel foam as a multifunctional electrode for electrocatalytic water splitting driven by photovoltaic-powered supercapacitors.Due to a stable 3D architecture configuration,abundant active sites,efficient charge transfer,and tuned interface properties,the NCONCS delivers a high specific capacity and rate performance for supercapacitors.A twoelectrode electrolyzer assembled with the NCONCS as both the anode and the cathode only requires a low cell voltage of 1.47 V to achieve a current density of 10 mA cm^(−2) in alkaline electrolyte,which outperforms the state-of-the-art bifunctional electrocatalysts.Theoretical calculations suggest that the generated heterointerfaces in NCONCS improve the surface binding capability of reaction intermediates while regulating the local electronic structures,which thus accelerates the reaction kinetics of water electrolysis.As a proof of concept,an integrated configuration comprising a two-electrode electrolyzer driven by two series-connected supercapacitors charged by a solar cell delivers a high product yield with superior durability.展开更多
Silicon(Si)is regarded as a promising anode material for next-generation lithium-ion batteries due to its ultrahigh theoretical capacity.However,the drastic volume change and the continuous solid electrolyte interphas...Silicon(Si)is regarded as a promising anode material for next-generation lithium-ion batteries due to its ultrahigh theoretical capacity.However,the drastic volume change and the continuous solid electrolyte interphase(SEI)formation during the lithiation/delithiation process seriously hinder its practical application as commercial anodes.Herein,macrocyclic betacyclodextrin(β-CD)has been designed as the diffusion channel for lithium ions at the molecular scale.The diameter of molecular channel is approximately comparable with the solvated lithium ions,which enables the transport of lithium ions and prevents the penetration of solvent molecules.Moreover,the addition ofβ-CD changes the formation behavior of SEI layer and stabilizes the Si nanoparticles.The enhanced electrochemical performances in terms of fast kinetics and improved stability have been achieved.The Si anode with the particularly selected lithium-ion diffusion channel and stabilized SEI layer exhibits a high reversible capability of 2562 m Ah g-1 after 50 cycles at the current density of 500 m A g-1,1944 m Ah g-1 after 200 cycles at the current density of 1 A g-1,and high rate performance.The novel strategy of molecular channel for lithium-ion diffusion offers new insights into the design of alloy-typed anode electrodes with high capacity for lithium-ion batteries.展开更多
The effect of cold high pressure densification(CHPD)on anisotropy of the critical current density(Jc)in《in situ》single core binary and alloyed MgB2 tapes has been determined as a function of temperatures at 4.2 K,20...The effect of cold high pressure densification(CHPD)on anisotropy of the critical current density(Jc)in《in situ》single core binary and alloyed MgB2 tapes has been determined as a function of temperatures at 4.2 K,20 K and 25 K as well as at applied magnetic fields up to 19 T.The study includes binary and C4H6O5(malic acid)doped MgB2 tapes before and after CHPD.It is remarkable that the CHPD process not only improved the Jc values,in particular at the higher magnetic fields,but also decreased the anisotropy ratio,Г=JC^///JC^⊥In binary MgB2 tapes,the anisotropy factor F increases with higher aspect ratios,even after applying CHPD.In malic acid(C4H6O5)doped tapes,however,the application of CHPD leads only to small enhancements ofГ,even for higher aspect ratios.This is attributed to the higher carbon content in the MgB2 filaments,which in turn is a consequence of the reduced chemical reaction path in the densified filaments.At all applied field values,it was found that CHPD processed C4H6O5 doped tapes exhibit an almost isotropic behavior.This constitutes an advantage in view of industrial magnet applications using wires with square or slightly rectangular configuration.展开更多
基金The Natural Science Foundation of China(51935014,52275395,82072084)Hunan Provincial Natural Science Foundation of China(2020JJ3047)+4 种基金Central South University Innovation-Driven Research Programme(2023CXQD023)JiangXi Provincial Natural Science Foundation of China(20224ACB204013)Technology Innovation Platform Project of Shenzhen Institute of Information Technology 2020(PT2020E002)Guangdong Province Precision Manufacturing and Intelligent Production Education Integration Innovation Platform(2022CJPT019)The Project of State Key Laboratory of Precision Manufacturing for Extreme Service Performance。
文摘As a new generation of materials/structures,heterostructure is characterized by heterogeneous zones with dramatically different mechanical,physical or chemical properties.This endows heterostructure with unique interfaces,robust architectures,and synergistic effects,making it a promising option as advanced biomaterials for the highly variable anatomy and complex functionalities of individual patients.However,the main challenges of developing heterostructure lie in the control of crystal/phase evolution and the distribution/fraction of components and structures.In recent years,additive manufacturing techniques have attracted increasing attention in developing heterostructure due to the unique flexibility in tailored structures and synthetic multimaterials.This review focuses on the additive manufacturing of heterostructure for biomedical applications.The structural features and functional mechanisms of heterostructure are summarized.The typical material systems of heterostructure,mainly including metals,polymers,ceramics,and their composites,are presented.And the resulting synergistic effects on multiple properties are also systematically discussed in terms of mechanical,biocompatible,biodegradable,antibacterial,biosensitive and magnetostrictive properties.Next,this work outlines the research progress of additive manufacturing employed in developing heterostructure from the aspects of advantages,processes,properties,and applications.This review also highlights the prospective utilization of heterostructure in biomedical fields,with particular attention to bioscaffolds,vasculatures,biosensors and biodetections.Finally,future research directions and breakthroughs of heterostructure are prospected with focus on their more prospective applications in infection prevention and drug delivery.
基金the financial support from the National Natural Science Foundation of China(22072183)the Natural Science Foundation of Hunan Province,China(2022JJ30690)supported in part by the High Performance Computing Center of Central South University。
文摘The d-band states of catalytic materials participate in adsorbing reactive intermediate species and determine the catalytic behaviors in CO_(2)reduction reactions.However,surface d-band states relating to the photocatalytic CO_(2)reduction reactions behaviors are rarely concerned.Herein,a slightly amount of Cd^(2+)is decorated on the surface of(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material(Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4))to tune the surface d-band states for improved CO_(2)+2reduction reactions.The Cd/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)is fabricated via the facile ions-exchange method to make that slightly Zn2+is substituted by Cd^(2+).The Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)exhibits much enhanced photocatalytic activity in CO_(2)reduction reactions to produce CO and water splitting to produce H_(2).Physical characterizations show that the energy band structure is not changed obviously.Density functional theory reveals that Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)possesses a closer shift of d-band center to Fermi level than(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4),suggesting easier adsorption of CO_(2)reduction reactive intermediates after Cd^(2+)decoration.Further calculations confirm that a relatively reduced adsorption Gibbs energy of reactive intermediates in CO_(2)reduction reaction is required on Zn atoms in Cd^(2+)/(CuGa)_(x)Zn_(1-2x)Ga_(2)S_(4)material,benefiting the photocatalytic CO_(2)reduction reactions.This work engineers surface d-band states by surface Cd^(2+)decoration,which gives an effective strategy to design highly efficient photocatalysts for syngas production.
基金financial support from the National Natural Science Foundation of China(No.22072183)the Natural Science Foundation of Hunan Province,China(No.2022JJ30690)。
文摘The d-band state of materials is an important descriptor for activity of oxygen evolution reaction(OER).For NiO materials,there is rarely concern about tuning their d-band states to tailor the OER behaviors.Herein,NiO nanocrystals with doping small amount of La^(3+)were used to regulate d-band states for promoting OER activity.Density of states calculations based on density functional theory revealed that La^(3+)doping produced upper shift of d-band center,which would induce stronger electronic interaction between surface Ni atoms and species of oxygen evolution reaction intermediates.Further density functional theory calculation illustrated that La^(3+)doped NiO possessed reduced Gibbs free energy in adsorbing species of OER intermediate.Predicted by theoretical calculations,trace La^(3+)was introduced into crystal lattice of NiO nanoparticles.The La^(3+)doped NiO nanocrystal showed much promoted OER activity than corresponding pristine NiO product.Further electrochemical analysis revealed that La^(3+)doping into NiO increased the intrinsic activity such as improved active sites and reduced charge transfer resistance.The in-situ Raman spectra suggested that NiO phase in La^(3+)doped NiO could be better maintained than pristine NiO during the OER.This work provides an effective strategy to tune the d-band center of NiO for efficient electrocatalytic OER.
基金the financial support from the National Natural Science Foundation of China(22005099)。
文摘Electrocatalytic conversion of carbon dioxide to high value-added chemicals is a promising method for solving the energy crisis and global warming.Electrochemical active metal-containing conjugated polymers have been widely studied for heterogeneous carbon dioxide reduction.In the present contribution,we designed and synthesized a stable cobalt phthalocyanine-based conjugated polymer,named CoPPc-TFPPy-CP,and also explored its electro-catalytic application in carbon dioxide reduction to liquid products in an aqueous solution.In the catalyst,cobalt phthalocyanine acts as building blocks connected with 1,3,6,8-tetrakis(4-formyl phenyl)pyrenes via imine-linkages,leading to mesoporous formation polymers with the pore size centered at 4.1nm.And the central co-balt atoms shifted to a higher oxidation state after condensation.With these chemical and structural natures,the catalyst displayed a remarkable electrocatalytic CO_(2) reduction performance with an ethanol Faradaic efficiency of 43.25%at-1.0V vs RHE.While at the same time,the electrochemical reduction process catalyzed by cobalt phthalocyanine produced only carbon monoxide and hydrogen.To the best of our knowledge,CoPPc-TFPPy-CP is the first example among organic polymers and metal-organic frameworks that produces ethanol from CO_(2) with a remarkable selectivity.
基金the Japan Society for the Promotion of Science(JSPS)KAKENHI Grant Number JP18F18714Cryogenic Station,Research Network and Facility Services Division,National Institute for Materials Science(NIMS),Japansupported by the ARC Linkage Project(LP200200689)。
文摘The development of superconducting joining technology for reacted magnesium diboride(MgB_(2))conductors remains a critical challenge for the advancement of cryogen-free MgB_(2)-based magnets for magnetic resonance imaging(MRI).Herein,the fabrication of superconducting joints using reacted carbon-doped multifilament MgB_(2)wires for MRI magnets is reported.To achieve successful superconducting joints,the powder-in-mold method was employed,which involved tuning the filament protection mechanism,the powder compaction pressure,and the heat treatment condition.The fabricated joints demonstrated clear superconducting-to-normal transitions in self-field,with effective magnetic field screening up to 0.5 T at 20 K.To evaluate the interface between one of the MgB_(2)filaments and the MgB_(2)bulk within the joint,serial sectioning was conducted for the first time in this type of superconducting joint.The serial sectioning revealed space formation at the interface,potentially caused by the volume shrinkage associated with the MgB_(2)formation or the combined effect of the volume shrinkage and the different thermal expansion coefficients of the MgB_(2)bulk,the filament,the mold,and the sealing material.These findings are expected to be pivotal in developing MgB_(2)superconducting joining technology for MRI magnet applications through interface engineering.
基金National Natural Science Foundation of China,Grant/Award Numbers:51874357,51872333,U20A20123。
文摘The lattice-oxygen-mediated mechanism is considered as a reasonable mechanism for the electrochemical catalytic oxygen evolution reaction(OER)of NiFe layered double hydroxides(LDHs).A NiFe LDH with distinct lattice contraction and microcrystallization was synthesized via a simple one-step method using sodium gluconate.The lattice contraction is attributed to the interaction of carbon in sodium gluconate and iron in NiFe LDH.The NiFe LDH with optimized microcrystallization and lattice contraction shows a low overpotential of 217 mV at a current density of 10 mA cm^(−2) and excellent durability of 20 h at a high current density of 100 mA cm^(−2).The results revealed that a contractive metal–oxygen bond could boost the intrinsic activity of active sites and the microcrystallization promotes an increase in the number of active sites in terms of unit area.The chemical environment of oxygen elemental characterization and resistance at different chronopotentiometry times confirm that the lattice oxygen element is indeed involved in the process of OER,supporting the lattice-oxygen-mediated mechanism of NiFe LDH.Density functional theory calculations reveal that contractive metal–oxygen bonds induced a reduction of the adsorption energy barrier of intermediate products,thus improving the intrinsic catalytic activity.The special characteristics of microcrystallization and lattice contraction of NiFe LDH provide a strategy to improve both the number and the intrinsic activity of active sites in a versatile manner.
文摘To control the power hierarchy design of lithium-ion battery(LIB)builtup sets for electric vehicles(EVs),we offer intensive theoretical and experimental sets of choice anode/cathode architectonics that can be modulated in full-scale LIB built-up models.As primary structural tectonics,heterogeneous composite superstructures of full-cell-LIB(anode//cathode)electrodes were designed in closely packed flower agave rosettes TiO2@C(FRTO@C anode)and vertical-star-tower LiFePO4@C(VST@C cathode)building blocks to regulate the electron/ion movement in the three-dimensional axes and orientation pathways.The superpower hierarchy surfaces and multi-directional orientation components may create isosurface potential electrodes with mobile electron movements,in-to-out interplay electron dominances,and electron/charge cloud distributions.This study is the first to evaluate the hotkeys of choice anode/cathode architectonics to assemble different LIB-electrode platforms with high-mobility electron/ion flows and high-performance capacity functionalities.Density functional theory calculation revealed that the FRTO@C anode and VST-(i)@C cathode architectonics are a superior choice for the configuration of full-scale LIB built-up models.The integrated FRTO@C//VST-(i)@C full-scale LIB retains a huge discharge capacity(~94.2%),an average Coulombic efficiency of 99.85%after 2000 cycles at 1 C,and a high energy density of 127 Wh kg?1,thereby satisfying scale-up commercial EV requirements.
文摘Immobilizing biocomponents on solid surfaces is a critical step in the development of new devices for future biological, medical, and electronic applications. Therefore, numerous integrated films were recently developed by immobilizing different proteins or enzymes on electrode surfaces. In this work, hemeproteins were safely immobilized onto macroporous nickel-based electrodes while maintaining their functionality.Such modified electrodes showed interesting pseudo-capacitive behavior. Among hemeproteins, hemoglobin(Hb) film has a higher electrochemical performance and greater charge/discharge cycling stability than myoglobin(Mb) and cytochrome C(Cyt C). The heme group in an alkaline medium could induce the formation of superoxides on the electrode surface. These capacitive features of hemeprotein-Ni electrode were related to strong binding sites between hemeproteins and porous Ni electrode, the accumulation of superoxide or radicals on the Ni surface, and facile electron transfer and electrolyte diffusion through the three-dimensional macroporous network. Thus, these new protein-based supercapacitors have potential use in free-standing platform technology for the development of implantable energy-storage devices.
文摘In recent decades,silicon photonics has attracted much attention in telecom and data-com areas.Constituted of high refractive-index contrast waveguides on silicon-on-insulator(SOI),a variety of integrated photonic passive and active devices have been implemented supported by excellent optical properties of silicon in the mid-infrared spectrum.The main advantage of the silicon photonics is the ability to use complementary metal oxide semiconductor(CMOS)process-compatible fabrication technologies,resulting in high-volume production at low cost.On the other hand,explosively growing traffic in the telecom,data center and high-performance computer demands the data flow to have high speed,wide bandwidth,low cost,and high energy-efficiency,as well as the photonics and electronics to be integrated for ultra-fast data transfer in networks.In practical applications,silicon photonics started with optical interconnect transceivers in the data-com first,and has been now extended to innovative applications such as multi-port optical switches in the telecom network node and integrated optical phased arrays(OPAs)in light detection and ranging(LiDAR).This paper overviews the progresses of silicon photonics from four points reflecting the recent advances mentioned above.CMOS-based silicon photonic platform technologies,applications to optical transceiver in the data-com network,applications to multi-port optical switches in the telecom network and applications to OPA in LiDAR system.
基金financially supported by JSPS KAKENHI(JP18H02065)Photo-excitonic Project in Hokkaido University,National Natural Science Foundation of China(21633004,22002060,and 51872138)+4 种基金Natural Science Foundation of Jiangsu Province(BK20181380)Qing Lan Project,Six Talent Peaks Project in Jiangsu Province(XCL-029)Priority Academic Program Development of the Jiangsu Higher Education Institutions(PAPD)the support provided by the China Scholarships Council(202008320109)China Postdoctoral Science Foundation(2020M681564)。
文摘Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2)RR)is still challenging owing to the sluggish kinetics or unfavorable thermodynamics for basic chemical processes of CO_(2)RR,such as adsorption,activation,conversion and product desorption.To overcome these shortcomings,recent works have demonstrated that surface engineering of semiconductors,such as introducing surface vacancy,surface doping,and cocatalyst loading,serves as effective or promising strategies for improved photocatalytic CO_(2)RR with high activity and selectivity.The essential reason lies in the activation and reaction pathways can be optimized and regulated through the reconstruction of surface atomic and electronic structures.Herein,in this review,we focus on recent research advances about rational design of semiconductor surface for photocatalytic CO_(2)RR.The surface engineering strategies for improved CO_(2)adsorption,activation,and product selectivity will be reviewed.In addition,theoretical calculations along with in situ characterization techniques will be in the spotlight to clarify the kinetics and thermodynamics of the reaction process.The aim of this review is to provide deep understanding and rational guidance on the design of semiconductors for photocatalytic CO_(2)RR.
基金the financial support by the National Natural Science Foundation of China(51874357,51872333,U20A20123)Innovative Research Group of Hunan Provincial Natural Science Foundation of China(2019JJ10006)support from Shenghua Scholar Program of Central South University.R.M.acknowledges support from JSPS KAKENNHI(18H03869)。
文摘Strategy of anchoring alloy nanoparticles made up of the efficient catalytic element(e.g.,Ni,Fe)on dodecyl sulfate(DS^(-))-intercalated NiFe layered double hydroxides(DS^(-)-NiFe LDH)obtained by a convenient one-step hydrothermal coprecipitation method for essentially enhancing oxygen evolution reaction(OER)performance was proposed.The results of structural characterization indicate Pt_(2)FeNi alloy nanoparticles evenly distribute on the surface of DS^(-)-NiFe LDH.The sizes of the Pt_(2)FeNi nanoparticles,closely related to their OER performance,could be wellcontrolled by adjusting the amount of H;PtCl;addition.The composite structure of as-prepared product was stable during processes of synthesis,exfoliation,self-assembly,and subsequent electrocatalytic OER.Rigorous electrochemical test proving the contributing catalytic active sites was located at the interface between Pt_(2)FeNi and DS^(-)-NiFe LDH,and the Ni and Fe were the major active elements while O atoms are adsorption sites.The formation of Pt_(2)FeNi nanoparticles could greatly prompt the reduction of Tafel slope.The best-performing Pt_(2)FeNi/DS^(-)-NiFe LDH with a Pt content of 0.98 wt%achieved low overpotential of 204 mV at 10 mA cm^(-2)and 262 mV at 50 mA cm^(-2).This work provides a convenient and effective strategy to create additional active sites for enhancing OER performance of NiFe LDH and make contribution to its wide application.
基金supported by Grant-in-Aid for Scientific Research in the Ministry of Education,Culture,Sports,Science and Technology of the Japanese Government(No.18360341)
文摘The sensing of a flame can be performed by using wide-bandgap semiconductors, which offer a high signal-to-noise ratio since they only response the ultraviolet emission in the flame. Diamond is a robust semiconductor with a wide-bandgap of 5.5 e V, exhibiting an intrinsic solar-blindness for deep-ultraviolet(DUV) detection. In this work, by using a submicron thick boron-doped diamond epilayer grown on a type-Ib diamond substrate, a Schottky photodiode device structure- based flame sensor is demonstrated. The photodiode exhibits extremely low dark current in both forward and reverse modes due to the holes depletion in the epilayer. The photodiode has a photoconductivity gain larger than 100 and a threshold wavelength of 330 nm in the forward bias mode. CO and OH emission bands with wavelengths shorter than 330 nm in a flame light are detected at a forward voltage of-10 V. An alcohol lamp flame in the distance of 250 mm is directly detected without a focusing lens of flame light.
基金financially supported by National Natural Science Foundation of China(51702291,51874357,U20A20123)the China Postdoctoral Science Foundation(2020M682352)+1 种基金State Key Laboratory of Powder Metallurgy,Central South University,Changsha,Chinasupport from the Youth Talent Program of Zhengzhou University and Henan Provincial Key Technology R&D Program(212102210597)。
文摘To effectively alleviate the ever-increasing energy crisis and environmental issues,clean and sustainable energy-related materials as well as the corresponding storage/conversion devices are in urgent demand.Silicon(Si) with the second most elemental abundance on the crust in the form of silicate or silica(SiO_(2)) minerals,is an advanced emerging material showing high performance in energy-related fields(e.g.batteries,photocatalytic hydrogen evolution).For the improved performance in industry-scale applications,Si materials with delicate nanostructures and ideal compositions in a massive production are highly cherished.On account of the reserve,low cost and diverse micro-nanostructures,silicate minerals are proposed as promising raw materials.In the article,crystal structures and the reduction approaches for silicate minerals,as well as recent progress on the as-reduced Si products for clean energy storage/conversion,are presented systematically.Moreover,some cutting-edge fields involving Si materials are discussed,which may offer deep insights into the rational design of advanced Si nanostructures for extended energy-related fields.
基金The authors acknowledge the support from National Natural Science Foundation of China(51972168,51672124,21603096)Program for Innovative Talents and Entrepreneur in Jiangsu,State Key Laboratory of Catalytic Materials and Reaction Engineering(RIPP,SINOPEC),and Technical Center of Nano Fabrication and Characterization of Nanjing University.
文摘For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3D)porous monoliths,alternatively called as 3D architectures,3D networks,or aerogels.The intersupported structure of porous monolithic 3D graphene(3DG)can prevent aggregation or restacking of graphene individuals,and the interconnected sp^(2) network of 3DG not only can provide the highway for the transport of electron/phonon but also can present continual cavities/channels for mass transfer.This review summarizes the synthesis methodology of 3DG porous monoliths and highlights the application for electric double-layer capacitors.Present challenges and future prospects about the manufacture and application of 3DG are also discussed.
基金support under the Australian Research Council’s Discovery Projects funding scheme(project number DP170101773)support from Alexander von Humboldt Foundation.T.T.+3 种基金financial support from the program of the Ministry of Education,Culture,Sports,Science,and Technology(MEXT,Japan)“Priority Issue on Post-K computer”(Development of new fundamental technologies for high-efficiency energy creation,conversion/storage and use)support from the Ministry of Science and Technology(2016YFA0204100)the National Natural Science Foundation of China(21961160722,91845201,21573254)the Liaoning Revitalization Talents Program XLYC1907055。
文摘It is demonstrated experimentally and confirmed theoretically that highly defective boron nitride showed outstanding performance for oxidative dehydrogenation of ethylbenzene.The catalyst is derived from carbon-doped hexagonal boron nitride nanosheets synthesized via a two-step reaction when participating the oxidative dehydrogenation reaction.The first step yields a polymeric precursor with the atomic positions of B,C,N relatively constrained,which is conducive for the formation of carbon atomic clusters uniformly dispersed throughout the BN framework.During the oxidative dehydrogenation of ethylbenzene to styrene,the nanoscale carbon clusters are removed and highly defective boron nitride(D-BN)is obtained,exposing boron-rich zigzag edges of BN that act as the catalytic sites.The catalytic performance of D-BN is therefore remarkably better than un-doped h-BN.Our results indicate that dispersed C-doping in h-BN is highly effective in terms of defect formation and resultant enhanced activity in oxidative dehydrogenation reactions.
基金China Postdoctoral Science Foundation,Grant/Award Number:2019M661825Natural Science Foundation of Jiangsu Province,Grant/Award Numbers:BK20190413,BK20210616Japan Society。
文摘Aprotic lithium–oxygen batteries(LOBs)have been recognized as novel energy storage devices for their outstanding specific energy density,while the large discharge/charge overpotential is a tough barrier to be overcome.Here,hetero-structured MoS_(2)/ZnIn_(2)S_(4) nanosheets have been prepared to capture visible light and the generated charge carriers are utilized for promoting both the oxygen reduction reaction and the oxygen evolution reaction.With the light illumination in the discharge process,the abundant photo-inspired electrons serve as the reaction sites to promote the reduction of O_(2) into LiO_(2) which is finally deposited as Li_(2)O_(2).On the contrary,the generated holes in the valence band can contribute to the low oxidization potential of Li_(2)O_(2) during the charge process.It delivers a low charge potential of 3.29 V,with an excellent resulting energy efficiency of 96.7%,much superior to that of 69.2%in the dark condition.It is noted that the involvement of photoelectrons has influenced the growth of Li_(2)O_(2) films on the MoS_(2)/ZnIn_(2)S_(4) nanosheets through the surface-adsorption pathway.The insights from the theoretical calculation confirm that the photoelectrons favor the absorption of LiO_(2) and the formation of the Li_(2)O_(2) film through the surface route.Therefore,this paper provides a deeper understanding of the mechanism of photoinspired charge carriers in LOBs and will enable further exploration of photo-involved energy storage systems.
基金financially supported by the National Key Research and Development Program of China(2016YFA0202403)the National University Research Fund(GK261001009)+7 种基金the Changjiang Scholar and Innovative Research Team(IRT_14R33)the Overseas Talent Recruitment Project(B14041)the Chinese National 1000talent plan program(Grant No.111001034)the JSPS Kakenhi grants(No.26288113 and 15K05486)support from the Strategic Research Foundation at Private Universities(Nihon University and the MEXT,Japan)the Natural Science Foundation of Shaanxi Province(2019JQ-423)the Fundamental Research Funds for the Central Universities(GK201903053)Key Lab of photovoltaic and Energy Conservation Materials,Chinese Academy of Sciences(No.PECL2019KF019)。
文摘A novel hole-transport material(HTM)based on an anthradithiophene central bridge named BTPA-7 is developed.In comparison to spiro-OMeTAD(2,2’,7,7’-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9’-spirobifluorene),the synthetic steps of BTPA-7 are greatly reduced from 6 to 3 and the synthetic cost of BTPA-7 is nearly a half that of spiro-OMeTAD.Moreover,BTPA-7 exhibits a relatively lower conductivity but higher hole mobility and higher glass transition temperature(Tg)than spiro-OMeTAD.Compared with the photovolatic performance for spiro-OMeTAD,FA0.85MA0.15PbI3 and MAPbI3 PSC devices based on BTPA-7 exhibit slightly lower PCEs with the values of 17.58%(18.88%for spiro-OMeTAD)and 11.90%(13.25%for spiro-OMeTAD),respectively.Nevertheless,a dramatically higher JSC of PSC based on BTPA-7is achieved,which arises from the higher hole mobility of BTPA-7.In addition,the relatively hydrophobic character of BTPA-7 eventually enhances the PSC device stability.Lower cost,higher hole mobility,higher Tg,satisfactory photovoltaic performance,and superior device stability of BTPA-7 can be utilized as a substitute for spiro-OMeTAD in PSCs.
文摘Due to the growing demand for clean and renewable hydrogen fuel,there has been a surge of interest in electrocatalytic water-splitting devices driven by renewable energy sources.However,the feasibility of self-driven water splitting is limited by inefficient connections between functional modules,lack of highly active and stable electrocatalysts,and intermittent and unpredictable renewable energy supply.Herein,we construct a dualmodulated three-dimensional(3D)NiCo_(2)O_(4)@NiCo_(2)S_(4)(denoted as NCONCS)heterostructure deposited on nickel foam as a multifunctional electrode for electrocatalytic water splitting driven by photovoltaic-powered supercapacitors.Due to a stable 3D architecture configuration,abundant active sites,efficient charge transfer,and tuned interface properties,the NCONCS delivers a high specific capacity and rate performance for supercapacitors.A twoelectrode electrolyzer assembled with the NCONCS as both the anode and the cathode only requires a low cell voltage of 1.47 V to achieve a current density of 10 mA cm^(−2) in alkaline electrolyte,which outperforms the state-of-the-art bifunctional electrocatalysts.Theoretical calculations suggest that the generated heterointerfaces in NCONCS improve the surface binding capability of reaction intermediates while regulating the local electronic structures,which thus accelerates the reaction kinetics of water electrolysis.As a proof of concept,an integrated configuration comprising a two-electrode electrolyzer driven by two series-connected supercapacitors charged by a solar cell delivers a high product yield with superior durability.
基金financial support by the National Natural Science Foundation of China(51874357,51872333)Innovative Research Group of Hunan Provincial Natural Science Foundation of China(2019JJ10006)+3 种基金the support from the 100 Talented Program of Hunan Province“Huxiang high-level talents”program(2019RS1007)support from Shenghua Scholar Program of Central South Universitysupport from JSPS KAKENNHI(18H03869)
文摘Silicon(Si)is regarded as a promising anode material for next-generation lithium-ion batteries due to its ultrahigh theoretical capacity.However,the drastic volume change and the continuous solid electrolyte interphase(SEI)formation during the lithiation/delithiation process seriously hinder its practical application as commercial anodes.Herein,macrocyclic betacyclodextrin(β-CD)has been designed as the diffusion channel for lithium ions at the molecular scale.The diameter of molecular channel is approximately comparable with the solvated lithium ions,which enables the transport of lithium ions and prevents the penetration of solvent molecules.Moreover,the addition ofβ-CD changes the formation behavior of SEI layer and stabilizes the Si nanoparticles.The enhanced electrochemical performances in terms of fast kinetics and improved stability have been achieved.The Si anode with the particularly selected lithium-ion diffusion channel and stabilized SEI layer exhibits a high reversible capability of 2562 m Ah g-1 after 50 cycles at the current density of 500 m A g-1,1944 m Ah g-1 after 200 cycles at the current density of 1 A g-1,and high rate performance.The novel strategy of molecular channel for lithium-ion diffusion offers new insights into the design of alloy-typed anode electrodes with high capacity for lithium-ion batteries.
基金This work was supported by the Australian Research Council(Grant No.LP160101784)A.K.thanks the Researchers Supporting Project(RSP-2019/127)King Saud University,Riyadh,Saudi Arabia for the support.This work was performed in part at the Queensland node of the Australian National Fabrication Facility,a company established under the National Collaborative Research Infrastructure Strategy to provide nano-and microfabrication facilities for Australia's researchers.M.M.acknowledges an internal funding project of the University of Osijek(ZUP-2018).
文摘The effect of cold high pressure densification(CHPD)on anisotropy of the critical current density(Jc)in《in situ》single core binary and alloyed MgB2 tapes has been determined as a function of temperatures at 4.2 K,20 K and 25 K as well as at applied magnetic fields up to 19 T.The study includes binary and C4H6O5(malic acid)doped MgB2 tapes before and after CHPD.It is remarkable that the CHPD process not only improved the Jc values,in particular at the higher magnetic fields,but also decreased the anisotropy ratio,Г=JC^///JC^⊥In binary MgB2 tapes,the anisotropy factor F increases with higher aspect ratios,even after applying CHPD.In malic acid(C4H6O5)doped tapes,however,the application of CHPD leads only to small enhancements ofГ,even for higher aspect ratios.This is attributed to the higher carbon content in the MgB2 filaments,which in turn is a consequence of the reduced chemical reaction path in the densified filaments.At all applied field values,it was found that CHPD processed C4H6O5 doped tapes exhibit an almost isotropic behavior.This constitutes an advantage in view of industrial magnet applications using wires with square or slightly rectangular configuration.
