Separators or electrolyte membranes are recognized as the key components to guarantee ion transport in rechargeable batteries.However,the ever-growing applications of the battery systems for diverse working environmen...Separators or electrolyte membranes are recognized as the key components to guarantee ion transport in rechargeable batteries.However,the ever-growing applications of the battery systems for diverse working environments bring new challenges,which require advanced battery membranes with high thermal stability,excellent mechanical strength,high voltage tolerance,etc.Therefore,it is highly desirable to design novel methods/concepts to solve the current challenges for battery membranes through understanding the mechanism of novel phenomena and electrochemical reactions in battery systems working under unconventional conditions.Recently,the new emerging Janus separators or electrolyte membranes with two or more distinct chemical/physical properties arising from their asymmetric structure and composition,are promising to address the above challenges via rational design of their targeted functionalities.To this end,in this review,we first briefly cover the current challenges of the traditional battery membrane for battery devices working in unconventional conditions.Then,the state-of-art developments of the rational design of Janus membranes to overcome the above challenges for diverse battery applications are summarized.Finally,we outline these latest developments,challenges,and future potential directions of the Janus membrane.Our review is aimed to provide basic guidance for developing functional separators or electrolyte membranes for advanced batteries.展开更多
The current COVID-19 pandemic urges the extremely sensitive and prompt detection of SARS-CoV-2 virus.Here,we present a Human Angiotensin-converting-enzyme 2(ACE2)-functionalized gold“virus traps”nanostructure as an ...The current COVID-19 pandemic urges the extremely sensitive and prompt detection of SARS-CoV-2 virus.Here,we present a Human Angiotensin-converting-enzyme 2(ACE2)-functionalized gold“virus traps”nanostructure as an extremely sensitive SERS biosensor,to selectively capture and rapidly detect S-protein expressed coronavirus,such as the current SARS-CoV-2 in the contaminated water,down to the single-virus level.Such a SERS sensor features extraordinary 106-fold virus enrichment originating from high-affinity of ACE2 with S protein as well as“virus-traps”composed of oblique gold nanoneedles,and 109-fold enhancement of Raman signals originating from multi-component SERS effects.Furthermore,the identification standard of virus signals is established by machine-learning and identification techniques,resulting in an especially low detection limit of 80 copies mL^(−1) for the simulated contaminated water by SARS-CoV-2 virus with complex circumstance as short as 5 min,which is of great significance for achieving real-time monitoring and early warning of coronavirus.Moreover,here-developed method can be used to establish the identification standard for future unknown coronavirus,and immediately enable extremely sensitive and rapid detection of novel virus.展开更多
The positive regulation of bone-forming osteoblast activity and the negative feedback regulation of osteoclastic activity are equally important in strategies to achieve successful alveolar bone regeneration. Here, a m...The positive regulation of bone-forming osteoblast activity and the negative feedback regulation of osteoclastic activity are equally important in strategies to achieve successful alveolar bone regeneration. Here, a molybdenum(Mo)-containing bioactive glass ceramic scaffold with solid-strut-packed structures(Mo-scaffold) was printed, and its ability to regulate pro-osteogenic and antiosteoclastogenic cellular responses was evaluated in vitro and in vivo. We found that extracts derived from Mo-scaffold(Moextracts) strongly stimulated osteogenic differentiation of bone marrow mesenchymal stem cells and inhibited differentiation of osteoclast progenitors. The identified comodulatory effect was further demonstrated to arise from Mo ions in the Mo-extract,wherein Mo ions suppressed osteoclastic differentiation by scavenging reactive oxygen species(ROS) and inhibiting mitochondrial biogenesis in osteoclasts. Consistent with the in vitro findings, the Mo-scaffold was found to significantly promote osteoblastmediated bone formation and inhibit osteoclast-mediated bone resorption throughout the bone healing process, leading to enhanced bone regeneration. In combination with our previous finding that Mo ions participate in material-mediated immunomodulation, this study offers the new insight that Mo ions facilitate bone repair by comodulating the balance between bone formation and resorption. Our findings suggest that Mo ions are multifunctional cellular modulators that can potentially be used in biomaterial design and bone tissue engineering.展开更多
Integrating active Pt clusters into transition-metal oxides with water-dissociation ability is effective to prepare a bifunctional electrocatalyst for water splitting in alkaline.However,the additional utilization of ...Integrating active Pt clusters into transition-metal oxides with water-dissociation ability is effective to prepare a bifunctional electrocatalyst for water splitting in alkaline.However,the additional utilization of a reductant and/or the operation at the elevating temperature causes the over-growth and agglomeration of Pt clusters,thus losing the high catalytic performance.Herein,we report that V dopant not only favors self-reducing Pt clusters on Ni Fe layered double hydroxide(LDH)(Pt/NiFeV)at room temperature,but also regulates interfacial charge redistribution to enhance the water-splitting performance.Experimental and theoretical studies reveal that V dopant into Ni Fe LDH triggers more electrons to transfer to adjacent Fe atoms,thus leading to a higher reducing ability compared to that without V-doping.When used as water-splitting electrocatalyst,V doping promotes electron loss of Pt clusters in Pt/Ni Fe V,optimizing the free energy of hydrogen adsorption and proton recombination kinetics at the cathode.Meanwhile,it also moves the d-band center of Ni away from the Fermi level to optimize the adsorption of*OH intermediates and facilitate the desorption of oxygen molecules at the anode.Thereby,Pt/Ni Fe V exhibits much higher bifunctional performance than V-free Pt/Ni Fe LDH toward both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).This work can spark inspiration of designing other bifunctional electrocatalysts for energy conversion and storage.展开更多
Flexible lithium-ion batteries(FLBs)are of critical importance to the seamless power supply of flexible and wearable electronic devices.However,the simultaneous acquirements of mechanical deformability and high energy...Flexible lithium-ion batteries(FLBs)are of critical importance to the seamless power supply of flexible and wearable electronic devices.However,the simultaneous acquirements of mechanical deformability and high energy density remain a major challenge for FLBs.Through billions of years of evolutions,many plants and animals have developed unique compositional and structural characteristics,which enable them to have both high mechanical deformability and robustness to cope with the complex and stressful environment.Inspired by nature,many new materials and designs emerge recently to achieve mechanically flexible and high storage capacity of lithiumion batteries at the same time.Here,we summarize these novel FLBs inspired by natural and biological materials and designs.We first give a brief introduction to the fundamentals and challenges of FLBs.Then,we highlight the latest achievements based on nature inspiration,including fiber-shaped FLBs,origami and kirigami-derived FLBs,and the nature-inspired structural designs in FLBs.Finally,we discuss the current status,remaining challenges,and future opportunities for the development of FLBs.This concise yet focused review highlights current inspirations in FLBs and wishes to broaden our view of FLB materials and designs,which can be directly“borrowed”from nature.展开更多
Thermoelectric power generation provides us the unique capability to explore the deep space and holds promise for harvesting the waste heat and providing a battery-free power supply for IoTs.The past years have witnes...Thermoelectric power generation provides us the unique capability to explore the deep space and holds promise for harvesting the waste heat and providing a battery-free power supply for IoTs.The past years have witnessed massive progress in thermoelectric materials,while the module-level development is still lagged behind.We would like to shine some light on the module-level design and characterization of thermoelectric power generators(TEGs).In the module-level design,we review material selection,thermal management,and the determination of structural parameters.We also look into the module-level characterization,with particular attention on the heat flux measurement.Finally,the challenge in the optimal design and reliable characterization of thermoelectric power generators is discussed,together with a calling to establish a standard test procedure.展开更多
An efficient electrocatalyst is indispensable to significantly reduce energy consumption and accelerate the conversion efficiency of water splitting.In this work,the honeycomb-like porous MoCo alloy on nitrogen-doped ...An efficient electrocatalyst is indispensable to significantly reduce energy consumption and accelerate the conversion efficiency of water splitting.In this work,the honeycomb-like porous MoCo alloy on nitrogen-doped three-dimensional(3D)porous graphene substrate(Mo_(0.3)Co_(0.7)@NPG)has been synthesized from the annealing of layered double hydroxide(MoCo-LDH@NPG).Especially,the Mo_(0.3)Co_(0.7)@NPG exhibits low hydrogen evolution overpotential of 75 mV(10 mA·cm^(-2))and a Tafel slope of 69.9 mV·dec^(-1),which can be attributed to highly conductive NPG substrate,the unique nanostructure and the synergistic effect of Mo and Co.Moreover,the Mo_(0.3)Co_(0.7)@NPG can maintain the original morphology and high catalytic activity after 50-h stability test.This work proposes a general strategy to synthesize a multi-element alloy on conductive substrates with high porosity for electrocatalytic reaction.展开更多
A nanocomposite microneedle(ZCQ/MN)patch containing copper/zinc dual-doped mesoporous silica nanoparticles loaded with quercetin(ZCQ)was developed as a combination therapy for androgenic alopecia(AGA).The degradable m...A nanocomposite microneedle(ZCQ/MN)patch containing copper/zinc dual-doped mesoporous silica nanoparticles loaded with quercetin(ZCQ)was developed as a combination therapy for androgenic alopecia(AGA).The degradable microneedle gradually dissolves after penetration into the skin and releases the ZCQ nanoparticles.ZCQ nanoparticles release quercetin(Qu),copper(Cu^(2+))and zinc ions(Zn^(2+))subcutaneously to synergistically promote hair follicle regeneration.The mechanism of promoting hair follicle regeneration mainly includes the regulation of the main pathophysiological phenomena of AGA such as inhibition of dihydrotestosterone,inhibition of inflammation,promotion of angiogenesis and activation of hair follicle stem cells by the combination of Cu^(2+)and Zn^(2+)ions and Qu.This study demonstrates that the systematic intervention targeting different pathophysiological links of AGA by the combination of organic drug and bioactive metal ions is an effective treatment strategy for hair loss,which provides a theoretical basis for development of biomaterial based anti-hair loss therapy.展开更多
Prussian blue analogues(PBAs)with the 3D open framework are regarded as promising cathode candidates for aqueous Zinc ion batteries(ZIBs).Among various PBAs,nickel hexacyanoferrate(NiHCF)has attracted considerable att...Prussian blue analogues(PBAs)with the 3D open framework are regarded as promising cathode candidates for aqueous Zinc ion batteries(ZIBs).Among various PBAs,nickel hexacyanoferrate(NiHCF)has attracted considerable attention because of its high operating voltage and economic merit.However,the cyclability of NiHCF is unsatisfactory due to poor structural stability during Zn^(2+) ions insertion/deinsertion.Moreover,the ion storage mechanism of NiHCF in aqueous electrolytes has not been fully revealed yet.Herein,high-crystallinity NiHCF(HC-NiHCF)microcubes with improved structural stability and larger crystal plane spacing are synthesized.For the first time,highly reversible Zn2+ions and Na+ions co-insertion/extraction are achieved for the HC-NiHCF microcubes in mixed aqueous electrolyte,as evidenced by various observations including two separated discharge plateaus and sequential changes of Na 1s and Zn 2p signals in ex-situ X-ray photoelectron spectroscopy(XPS).As a result,a high specific capacity of 73.9 mAh g^(−1) is obtained for the HC-NiHCF microcubes at 0.1 A g−1,combined with enhanced cycle stability(75%vs.16.4%)over 1000 cycles at 2 A g^(−1).The reversible Zn^(2+) ions and Na+ions co-insertion in HC-NiHCF microcubes reveals a new ion storage mechanism of Ni-based PBAs in aqueous electrolytes.展开更多
Tendon-bone healing is essential for an effective rotator cuff tendon repair surgery,however,this remains a significant challenge due to the lack of biomaterials with high strength and bioactivity.Inspired by the high...Tendon-bone healing is essential for an effective rotator cuff tendon repair surgery,however,this remains a significant challenge due to the lack of biomaterials with high strength and bioactivity.Inspired by the high-performance exoskeleton of natural organisms,we set out to apply natural fish scale(FS)modified by calcium silicate nanoparticles(CS NPs)as a new biomaterial(CS-FS)to overcome the challenge.Benefit from its“Bouligand”microstructure,such FS-based scaffold maintained excellent tensile strength(125.05 MPa)and toughness(14.16 MJ/m^(3)),which are 1.93 and 2.72 times that of natural tendon respectively,allowing it to well meet the requirements for rotator cuff tendon repair.Additionally,CS-FS showed diverse bioactivities by stimulating the differentiation and phenotypic maintenance of multiple types of cells participated into the composition of tendon-bone junction,(e.g.bone marrow mesenchymal stem cells(BMSCs),chondrocyte,and tendon stem/progenitor cells(TSPCs)).In both rat and rabbit rotator cuff tear(RCT)models,CS-FS played a key role in the tendon-bone interface regeneration and biomechanical function,which may be achieved by activating BMP-2/Smad/Runx2 pathway in BMSCs.Therefore,natural fish scale-based biomaterials are the promising candidate for clinical tendon repair due to their outstanding strength and bioactivity.展开更多
Oxygen electrocatalysts are of great importance for the air electrode in zinc–air batteries(ZABs).Owing to large surface area,high electrical conductivity and ease of modification,two-dimensional(2D)materials have be...Oxygen electrocatalysts are of great importance for the air electrode in zinc–air batteries(ZABs).Owing to large surface area,high electrical conductivity and ease of modification,two-dimensional(2D)materials have been widely studied as oxygen electrocatalysts for the rechargable ZABs.The elaborately modified 2D materials-based electrocatalysts,usually exhibit excellent performance toward the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),which have attracted extensive interests of worldwide researchers.Given the rapid development of bifunctional electrocatalysts toward ORR and OER,the latest progress of non-noble electrocatalysts based on layered double hydroxides(LDHs),graphene,and MXenes are intensively reviewed.The discussion ranges from fundamental structure,synthesis,electrocatalytic performance of these catalysts,as well as their applications in the rechargeable ZABs.Finally,the challenges and outlook are provided for further advancing the commercialization of rechargeable ZABs.展开更多
High-hardness rock-salt structured transitional metal carbides(TMC)are attracting substantial interest as potential next-generation thermal protection materials.However,the intrinsic brittleness of TMC ceramics impede...High-hardness rock-salt structured transitional metal carbides(TMC)are attracting substantial interest as potential next-generation thermal protection materials.However,the intrinsic brittleness of TMC ceramics impedes their performance in aerodynamically harsh environments.In this work,a promising strategy is proposed to introduce plasticity in TaC–HfC solid solutions by manipulating carbon deficiency.The approach combines density-functional theory(DFT)with experiments and takes Pugh's ratio(k)as the criteria.Depletion of carbon atoms in TaC–HfC solid solutions results in the de-localizing of valence electrons,deviation of spatial modulus along different crystal plane directions,and leading to significant elastic anisotropy.The carbon deficient Ta_(0.8)Hf_(0.2)C_(0.8) is predicted to be a‘softer phase’with reduced modulus and Pugh's ratio(k=0.58).A series of Ta1–xHfxCy(x=0.2 and 0.8,y=0.8,0.9,and 1.0)bulk ceramics are experimentally fabricated by an excessive metal alloying method.Trigonal and hexagonal close-packed structured carbides are derived when the carbon deficiency y decreased to 0.7.The indentation modulus drops from 641.8±14.8 GPa for Ta_(0.8)Hf_(0.2)C_(1.0) to 555.8±9.9 GPa for Ta0.8Hf0.2C0.8.The specific stoichiometric composition of Ta_(0.8)Hf_(0.2)C_(0.8) is experimentally verified to possess both plasticity(k=0.41)and ultra-high nanohardness(41.3±1.3 GPa).展开更多
钠离子电池因其成本低、资源丰富等优点而成为新一代储能设备.在各种正极中,隧道型Na_(0.44)MnO_(2)因其较大的Na^(+)通道,被认为是快速充电电池的合适正极材料,但仍然存在Na^(+)动力学缓慢等问题.本文首次提出了一种Na_(0.44)MnO_(2)...钠离子电池因其成本低、资源丰富等优点而成为新一代储能设备.在各种正极中,隧道型Na_(0.44)MnO_(2)因其较大的Na^(+)通道,被认为是快速充电电池的合适正极材料,但仍然存在Na^(+)动力学缓慢等问题.本文首次提出了一种Na_(0.44)MnO_(2)的新型离子交换方法,通过调节合成条件,可以很好地控制K^(+)残余量和Na_(0.44)MnO_(2)的尺寸.结果表明,Na_(0.44)MnO_(2)结构中的残留K^(+)扩大了Na^(+)的输运通道,小颗粒形貌缩短了Na^(+)的迁移距离,且晶体中的带状缺陷界面进一步加速了Na^(+)的输运.获得的Na_(0.44)MnO_(2)具有本征赝电容特性,在2-4 V和20 C电流下有79.0 mA h g^(-1)的优异倍率性能.长期循环测试表明,20 C下1000次循环的保持率为98.1%,0.5 C下200次循环的保持率为96.3%.本工作为用于快速充电储能装置的高倍率、高稳定性Na_(0.44)MnO_(2)正极的大规模生产提供了一条新途径.展开更多
有机电极具有结构可设计性强、容量大、可容纳大离子等优点.然而,在钠离子电池中,有机电极材料的容量仍然很低,且其在有机电解质中的高溶解度导致其寿命较短.如何通过化合物设计来提高其性能一直是研究人员关注的问题.本研究通过简单方...有机电极具有结构可设计性强、容量大、可容纳大离子等优点.然而,在钠离子电池中,有机电极材料的容量仍然很低,且其在有机电解质中的高溶解度导致其寿命较短.如何通过化合物设计来提高其性能一直是研究人员关注的问题.本研究通过简单方法将氨基酸接枝到有机化合物上,提高了其容量和循环稳定性.首先,氨基酸之间的氢键使其形成更稳定的层状结构;氨基酸基团在有机电极材料和羧甲基纤维素粘合剂之间形成分子间相互作用,降低界面阻力,显著提高循环稳定性,使得钠离子电池循环次数超过2000次.其次,实验和计算结果表明,氨基酸基团提供了Na^(+)转运途径和额外的可逆存储位点,从而提高了比容量(~300 mA h g^(-1)).本策略可以启发未来钠离子电池的有机分子设计.展开更多
The past years has observed a significantly boost of the thermoelectric materials in the scale of thermoelectric figure-of-merit,i.e.ZT,because of its promising application to harvest the widely distributed waste heat...The past years has observed a significantly boost of the thermoelectric materials in the scale of thermoelectric figure-of-merit,i.e.ZT,because of its promising application to harvest the widely distributed waste heat.However,the simplified thermoelectric materials'performance scale also shifted the focus of thermoelectric energy conversion technique from devices-related efforts to materials-level works.As a result,the thermoelectric devices-related works didn't get enough attention.The device-level challenges behind were kept unknown until recent years.However,besides the thermoelectric materials properties,the practical energy conversion efficiency and service life of thermoelectric device is highly determined by assembling process and the contact interface.In this perspective,we are trying to shine some light on the device-level challenge,and give a special focus on the thermoelectric interface materials(TEiM)between the thermoelectric elements and electrode,which is also known as the metallization layer or solder barrier layer.We will go through the technique concerns that determine the scope of the TEiM,including bonding strength,interfacial resistance and stability.Some general working principles are summarized before the discussion of some typical examples of searching proper TEiM for a given thermoelectric conversion material.展开更多
Commercial lithium-ion batteries (LIBs) have been widely used in various energy storage systems. However, many unfavorable factors of LIBs have prompted researchers to turn their attention to the development of emergi...Commercial lithium-ion batteries (LIBs) have been widely used in various energy storage systems. However, many unfavorable factors of LIBs have prompted researchers to turn their attention to the development of emerging secondary batteries. Aqueous zinc ion batteries (AZIBs) present some prominent advantages with environmental friendliness, low cost and convenient operation feature. MnO_(2) electrode is the first to be discovered as promising cathode material. So far, manganese-based oxides have made significant progresses in improving the inherent capacity and energy density. Herein, we summarize comprehensively recent advances of Mn-based compounds as electrode materials for ZIBs. Especially, this review focuses on the design strategies of electrode structures, optimization of the electrochemical performance and the clarification of energy storage mechanisms. Finally, their future research directions and perspective are also proposed.展开更多
Due to the relatively sluggish charge carrier separation in metal sulfides,the photocatalytic activity of them is still far lower than expected.Herein,sulfur vacancies and in-plane SnS_(2)/SnO_(2) heterojunction were ...Due to the relatively sluggish charge carrier separation in metal sulfides,the photocatalytic activity of them is still far lower than expected.Herein,sulfur vacancies and in-plane SnS_(2)/SnO_(2) heterojunction were successfully introduced into the SnS_(2) nanosheets through high energy ball-milling.These defective structures were studied by the electron paramagnetic resonance,Raman spectra,X-ray photoelectron spectroscopy,and high-resolution transmission electron microscope analyses.The sulfur vacancies and in-plane heterojunctions strongly accelerate the separation of photoexcited electron-hole pairs,as confirmed by the photo luminesce nce emission spectra and time-resolved photoluminescence decay spectra.The introduction of sulfur vacancies and in-plane heterojunction in SnS_(2) nanosheets results in roughly six times higher photodegrading rate for methyl orange and four times higher photocatalytic reduction rate of Cr6+than those of pure SnS_(2) nanosheets.展开更多
The immune response induced by surface topography crucially determines the implant success.However,how the immune response is mediated by the size of surface topography remains unclear.Hence,various biocompatible Mg-A...The immune response induced by surface topography crucially determines the implant success.However,how the immune response is mediated by the size of surface topography remains unclear.Hence,various biocompatible Mg-Al layered double hydroxides sheet-array films with different sizes(nano,micro and nano/micro mixture)were constructed on the biomedical titanium,and their osteo-immunomodulation effects on the macrophages were explored.The nano-sheet array structures significantly promoted the polarization of M2 macrophages by activating the PI3K-AKT-mTOR signaling pathway with high gene expressions of integrin b2 and FAK.While the micro-sheet array structures enhanced osteogenic differentiation of mouse bone marrow mesenchymal stem cells(mBMSCs)via ROCK-YAP/TAZ-mediated mechanotransduction.Moreover,the nano-sheet array structures promoted the osteogenic differentiation of mBMSCs with a high proportion of M2 macrophages through a shared medium.This study gave further information concerning integrin-induced focal adhesions in cells of different sheet array structures and their role in macrophage polarization and osteogenic differentiation of mBMSCs,which might help to design biomaterial surfaces with optimal geometry for a desired immunemodulation.展开更多
The salt-inclusion materials have drawn significant attention for their manifold structural chemistry and novel physical/chemical properties.Herein,two new salt-inclusion chalcohalides,[Cs_(6)Cl][Ga_(5)GeQ_(12)](Q=S,S...The salt-inclusion materials have drawn significant attention for their manifold structural chemistry and novel physical/chemical properties.Herein,two new salt-inclusion chalcohalides,[Cs_(6)Cl][Ga_(5)GeQ_(12)](Q=S,Se),have been discovered via hightemperature flux methods.The two isostructural compounds are constructed by porous[Ga_(5)GeQ_(12)]^(5−)layers with[ClCs_(6)]^(5+)octahedra filled in the holes.The[Ga_(5)GeQ_(12)]^(5−)layer is composed of the honeycomb-like(Ga/Ge)_(18)Q_(42)rings containing(Ga/Ge)_(3)Q_(9)trimer as basic unit.The band gaps of the two compounds are 3.90 and 2.89 eV,respectively.[Cs_(6)Cl][Ga_(5)GeS_(12)]exhibits interesting two-band emission properties which are related to the intermediate-band electronic structure revealed by density functional theory(DFT)calculations.Owing to the porous layered structure,[Cs_(6)Cl][Ga_(5)GeS_(12)]exhibits topological ion exchange ability towards Cd^(2+)ions with the maximum sorption capacity of 250 mg/g and high distribution coefficient(Kd)near 106 mL/g.This work further enriches the structural diversity of salt-inclusion materials and extends their potential application range to ion exchange adsorption.展开更多
Upon uniaxial compressive loading at 500℃(T/Tm=0.67,where Tm is the absolute melting point),the n-type Skutterudite alloy Yb03Co4Sb12 deforms plastically by creep via a power-law,with a stress exponent~3 consistent w...Upon uniaxial compressive loading at 500℃(T/Tm=0.67,where Tm is the absolute melting point),the n-type Skutterudite alloy Yb03Co4Sb12 deforms plastically by creep via a power-law,with a stress exponent~3 consistent with dislocation viscous glide.An activation energy of 171 kJ/mol is measured over the temperature range of 500-587℃(T/Tm=0.67-0.75)at a stress of 30 MPa.Yb_(0.3)Co_(4)Sb_(12)is ductile at 500℃,exhibiting a compressive strain of 25%when subjected to stresses ranging from 22 to 90 MPa for up to 28 days.Among the thermoelectric materials tested so far for creep,Yb_(0.3)Co_(4)Sb_(12)exhibits a creep resistance intermediate between low-melting(Bi2Te3,TAGS-85)and high-melting thermoelectrics(Mg2Si and ZrNiSn).A relatively modest drop in the figure of merit zT,from 0.67 to 0.52,is displayed by Yb_(0.3)Co_(4)Sb_(12)after accumulating 3.7%compressive creep strain at 500℃,mostly due to a drop in electrical conductivity.展开更多
基金supported by the Science and Technology Development Fund from Macao SAR(FDCT-0057/2019/A1,0092/2019/A2,and 0035/2019/AMJ)Startup grants(SRG2018-00140-IAPME)from the Research and Development Office at University of Macao+1 种基金National Natural Science Foundation of China(Grant no.21875040 and 21905051)Chongqing Key Laboratory fund of Soft-Matter Material Chemistry and Function Manufacturing(No.20200003).
文摘Separators or electrolyte membranes are recognized as the key components to guarantee ion transport in rechargeable batteries.However,the ever-growing applications of the battery systems for diverse working environments bring new challenges,which require advanced battery membranes with high thermal stability,excellent mechanical strength,high voltage tolerance,etc.Therefore,it is highly desirable to design novel methods/concepts to solve the current challenges for battery membranes through understanding the mechanism of novel phenomena and electrochemical reactions in battery systems working under unconventional conditions.Recently,the new emerging Janus separators or electrolyte membranes with two or more distinct chemical/physical properties arising from their asymmetric structure and composition,are promising to address the above challenges via rational design of their targeted functionalities.To this end,in this review,we first briefly cover the current challenges of the traditional battery membrane for battery devices working in unconventional conditions.Then,the state-of-art developments of the rational design of Janus membranes to overcome the above challenges for diverse battery applications are summarized.Finally,we outline these latest developments,challenges,and future potential directions of the Janus membrane.Our review is aimed to provide basic guidance for developing functional separators or electrolyte membranes for advanced batteries.
基金the National Natural Science Foundation of China(No.51471182)this work is also supported by Shanghai international science and Technology Cooperation Fund(No.17520711700)the National Key Research and Development Project(No.2017YFB0310600).
文摘The current COVID-19 pandemic urges the extremely sensitive and prompt detection of SARS-CoV-2 virus.Here,we present a Human Angiotensin-converting-enzyme 2(ACE2)-functionalized gold“virus traps”nanostructure as an extremely sensitive SERS biosensor,to selectively capture and rapidly detect S-protein expressed coronavirus,such as the current SARS-CoV-2 in the contaminated water,down to the single-virus level.Such a SERS sensor features extraordinary 106-fold virus enrichment originating from high-affinity of ACE2 with S protein as well as“virus-traps”composed of oblique gold nanoneedles,and 109-fold enhancement of Raman signals originating from multi-component SERS effects.Furthermore,the identification standard of virus signals is established by machine-learning and identification techniques,resulting in an especially low detection limit of 80 copies mL^(−1) for the simulated contaminated water by SARS-CoV-2 virus with complex circumstance as short as 5 min,which is of great significance for achieving real-time monitoring and early warning of coronavirus.Moreover,here-developed method can be used to establish the identification standard for future unknown coronavirus,and immediately enable extremely sensitive and rapid detection of novel virus.
基金supported by the National Natural Science Foundation of China(grant nos.82130026,82001102 and 82170958)the Young Elite Scientist Support Program administered by CSA(2021PYRC001)the Natural Science Basic Research Program of Shaanxi(2020JQ-447)。
文摘The positive regulation of bone-forming osteoblast activity and the negative feedback regulation of osteoclastic activity are equally important in strategies to achieve successful alveolar bone regeneration. Here, a molybdenum(Mo)-containing bioactive glass ceramic scaffold with solid-strut-packed structures(Mo-scaffold) was printed, and its ability to regulate pro-osteogenic and antiosteoclastogenic cellular responses was evaluated in vitro and in vivo. We found that extracts derived from Mo-scaffold(Moextracts) strongly stimulated osteogenic differentiation of bone marrow mesenchymal stem cells and inhibited differentiation of osteoclast progenitors. The identified comodulatory effect was further demonstrated to arise from Mo ions in the Mo-extract,wherein Mo ions suppressed osteoclastic differentiation by scavenging reactive oxygen species(ROS) and inhibiting mitochondrial biogenesis in osteoclasts. Consistent with the in vitro findings, the Mo-scaffold was found to significantly promote osteoblastmediated bone formation and inhibit osteoclast-mediated bone resorption throughout the bone healing process, leading to enhanced bone regeneration. In combination with our previous finding that Mo ions participate in material-mediated immunomodulation, this study offers the new insight that Mo ions facilitate bone repair by comodulating the balance between bone formation and resorption. Our findings suggest that Mo ions are multifunctional cellular modulators that can potentially be used in biomaterial design and bone tissue engineering.
基金the financial support from the Science and Technology Commission of Shanghai Municipality(19ZR1479500)the National Natural Science Foundation of China(52072389)the Program of Shanghai Academic Research Leader(20XD1424300)for financial support。
文摘Integrating active Pt clusters into transition-metal oxides with water-dissociation ability is effective to prepare a bifunctional electrocatalyst for water splitting in alkaline.However,the additional utilization of a reductant and/or the operation at the elevating temperature causes the over-growth and agglomeration of Pt clusters,thus losing the high catalytic performance.Herein,we report that V dopant not only favors self-reducing Pt clusters on Ni Fe layered double hydroxide(LDH)(Pt/NiFeV)at room temperature,but also regulates interfacial charge redistribution to enhance the water-splitting performance.Experimental and theoretical studies reveal that V dopant into Ni Fe LDH triggers more electrons to transfer to adjacent Fe atoms,thus leading to a higher reducing ability compared to that without V-doping.When used as water-splitting electrocatalyst,V doping promotes electron loss of Pt clusters in Pt/Ni Fe V,optimizing the free energy of hydrogen adsorption and proton recombination kinetics at the cathode.Meanwhile,it also moves the d-band center of Ni away from the Fermi level to optimize the adsorption of*OH intermediates and facilitate the desorption of oxygen molecules at the anode.Thereby,Pt/Ni Fe V exhibits much higher bifunctional performance than V-free Pt/Ni Fe LDH toward both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).This work can spark inspiration of designing other bifunctional electrocatalysts for energy conversion and storage.
基金National Nature Science Foundation of China,Grant/Award Numbers:21875040,21905051Macao Science and Technology Development Fund,Grant/Award Numbers:FDCT-0035/2019/AMJ,FDCT-0057/2019/A1,FDCT-0092/2019/A2pt>。
文摘Flexible lithium-ion batteries(FLBs)are of critical importance to the seamless power supply of flexible and wearable electronic devices.However,the simultaneous acquirements of mechanical deformability and high energy density remain a major challenge for FLBs.Through billions of years of evolutions,many plants and animals have developed unique compositional and structural characteristics,which enable them to have both high mechanical deformability and robustness to cope with the complex and stressful environment.Inspired by nature,many new materials and designs emerge recently to achieve mechanically flexible and high storage capacity of lithiumion batteries at the same time.Here,we summarize these novel FLBs inspired by natural and biological materials and designs.We first give a brief introduction to the fundamentals and challenges of FLBs.Then,we highlight the latest achievements based on nature inspiration,including fiber-shaped FLBs,origami and kirigami-derived FLBs,and the nature-inspired structural designs in FLBs.Finally,we discuss the current status,remaining challenges,and future opportunities for the development of FLBs.This concise yet focused review highlights current inspirations in FLBs and wishes to broaden our view of FLB materials and designs,which can be directly“borrowed”from nature.
基金supported by Shenzhen DRC project(Grant No.[2018]1433)。
文摘Thermoelectric power generation provides us the unique capability to explore the deep space and holds promise for harvesting the waste heat and providing a battery-free power supply for IoTs.The past years have witnessed massive progress in thermoelectric materials,while the module-level development is still lagged behind.We would like to shine some light on the module-level design and characterization of thermoelectric power generators(TEGs).In the module-level design,we review material selection,thermal management,and the determination of structural parameters.We also look into the module-level characterization,with particular attention on the heat flux measurement.Finally,the challenge in the optimal design and reliable characterization of thermoelectric power generators is discussed,together with a calling to establish a standard test procedure.
基金supported by the National Natural Science Foundation of China(Nos.52272296 and 51502092)the Fundamental Research Funds for the Central Universities(Nos.JKD01211601 and 1222201718002)the National Overseas High-Level Talent Youth Program in China and the Eastern Scholar Project of Shanghai。
文摘An efficient electrocatalyst is indispensable to significantly reduce energy consumption and accelerate the conversion efficiency of water splitting.In this work,the honeycomb-like porous MoCo alloy on nitrogen-doped three-dimensional(3D)porous graphene substrate(Mo_(0.3)Co_(0.7)@NPG)has been synthesized from the annealing of layered double hydroxide(MoCo-LDH@NPG).Especially,the Mo_(0.3)Co_(0.7)@NPG exhibits low hydrogen evolution overpotential of 75 mV(10 mA·cm^(-2))and a Tafel slope of 69.9 mV·dec^(-1),which can be attributed to highly conductive NPG substrate,the unique nanostructure and the synergistic effect of Mo and Co.Moreover,the Mo_(0.3)Co_(0.7)@NPG can maintain the original morphology and high catalytic activity after 50-h stability test.This work proposes a general strategy to synthesize a multi-element alloy on conductive substrates with high porosity for electrocatalytic reaction.
基金supported by Science and Technology Commission of Shanghai Municipality(No.20S31904500)the National Natural Science Foundation of China(No.81772078 and No.82172200 and No.31900945 and No.82100427)+3 种基金Shanghai 2022"Science and Technology Innovation Action Plan"biomedical science and technology support special project(No.22S31902800)Shanghai Science and Technology Commission INTERNATIONAL COOPERATION Project(No.21520712300)the seed grants from the Wenzhou Institute,University of Chinese Academy of Sciences(WIUCASQD2020013,WIUCASQD2021030)the founding from the First Affiliated Hospital of Wenzhou Medical University.
文摘A nanocomposite microneedle(ZCQ/MN)patch containing copper/zinc dual-doped mesoporous silica nanoparticles loaded with quercetin(ZCQ)was developed as a combination therapy for androgenic alopecia(AGA).The degradable microneedle gradually dissolves after penetration into the skin and releases the ZCQ nanoparticles.ZCQ nanoparticles release quercetin(Qu),copper(Cu^(2+))and zinc ions(Zn^(2+))subcutaneously to synergistically promote hair follicle regeneration.The mechanism of promoting hair follicle regeneration mainly includes the regulation of the main pathophysiological phenomena of AGA such as inhibition of dihydrotestosterone,inhibition of inflammation,promotion of angiogenesis and activation of hair follicle stem cells by the combination of Cu^(2+)and Zn^(2+)ions and Qu.This study demonstrates that the systematic intervention targeting different pathophysiological links of AGA by the combination of organic drug and bioactive metal ions is an effective treatment strategy for hair loss,which provides a theoretical basis for development of biomaterial based anti-hair loss therapy.
基金supported by the Macao Science and Technology Development Fund for funding(File Nos.FDCT-0057/2019/A1,0092/2019/A2,0035/2019/AMJ,0013/2021/AMJ,and 0082/2022/A2)and the Startup grant(No.SRG2018–00140-IAPME)Multi-Year research grant(Nos.MYRG2020–00283-IAPME and MYRG2022–00266-IAPME)from the Research&Development Office at University of Macao.We also acknowledge the fund of the National Nature Science Foundation of China(Grant Nos.52202328,21875040,and。
文摘Prussian blue analogues(PBAs)with the 3D open framework are regarded as promising cathode candidates for aqueous Zinc ion batteries(ZIBs).Among various PBAs,nickel hexacyanoferrate(NiHCF)has attracted considerable attention because of its high operating voltage and economic merit.However,the cyclability of NiHCF is unsatisfactory due to poor structural stability during Zn^(2+) ions insertion/deinsertion.Moreover,the ion storage mechanism of NiHCF in aqueous electrolytes has not been fully revealed yet.Herein,high-crystallinity NiHCF(HC-NiHCF)microcubes with improved structural stability and larger crystal plane spacing are synthesized.For the first time,highly reversible Zn2+ions and Na+ions co-insertion/extraction are achieved for the HC-NiHCF microcubes in mixed aqueous electrolyte,as evidenced by various observations including two separated discharge plateaus and sequential changes of Na 1s and Zn 2p signals in ex-situ X-ray photoelectron spectroscopy(XPS).As a result,a high specific capacity of 73.9 mAh g^(−1) is obtained for the HC-NiHCF microcubes at 0.1 A g−1,combined with enhanced cycle stability(75%vs.16.4%)over 1000 cycles at 2 A g^(−1).The reversible Zn^(2+) ions and Na+ions co-insertion in HC-NiHCF microcubes reveals a new ion storage mechanism of Ni-based PBAs in aqueous electrolytes.
基金supported by the National Basic Research Program of China(grant No.2021YFA0715700)the Natural Science Foundation of China(32130062)+1 种基金Innovation Cross Team of Chinese Academy of Sciences(JCTD-2018-13)Science and Technology Commission of Shanghai Municipality(20442420300,21DZ1205600).
文摘Tendon-bone healing is essential for an effective rotator cuff tendon repair surgery,however,this remains a significant challenge due to the lack of biomaterials with high strength and bioactivity.Inspired by the high-performance exoskeleton of natural organisms,we set out to apply natural fish scale(FS)modified by calcium silicate nanoparticles(CS NPs)as a new biomaterial(CS-FS)to overcome the challenge.Benefit from its“Bouligand”microstructure,such FS-based scaffold maintained excellent tensile strength(125.05 MPa)and toughness(14.16 MJ/m^(3)),which are 1.93 and 2.72 times that of natural tendon respectively,allowing it to well meet the requirements for rotator cuff tendon repair.Additionally,CS-FS showed diverse bioactivities by stimulating the differentiation and phenotypic maintenance of multiple types of cells participated into the composition of tendon-bone junction,(e.g.bone marrow mesenchymal stem cells(BMSCs),chondrocyte,and tendon stem/progenitor cells(TSPCs)).In both rat and rabbit rotator cuff tear(RCT)models,CS-FS played a key role in the tendon-bone interface regeneration and biomechanical function,which may be achieved by activating BMP-2/Smad/Runx2 pathway in BMSCs.Therefore,natural fish scale-based biomaterials are the promising candidate for clinical tendon repair due to their outstanding strength and bioactivity.
基金the Fundamental Research Funds for Central Universities and the National Key R&D Program of China(Grant No.2016YFC1402504)the National Natural Science Foundation of China(No.52172058).
文摘Oxygen electrocatalysts are of great importance for the air electrode in zinc–air batteries(ZABs).Owing to large surface area,high electrical conductivity and ease of modification,two-dimensional(2D)materials have been widely studied as oxygen electrocatalysts for the rechargable ZABs.The elaborately modified 2D materials-based electrocatalysts,usually exhibit excellent performance toward the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),which have attracted extensive interests of worldwide researchers.Given the rapid development of bifunctional electrocatalysts toward ORR and OER,the latest progress of non-noble electrocatalysts based on layered double hydroxides(LDHs),graphene,and MXenes are intensively reviewed.The discussion ranges from fundamental structure,synthesis,electrocatalytic performance of these catalysts,as well as their applications in the rechargeable ZABs.Finally,the challenges and outlook are provided for further advancing the commercialization of rechargeable ZABs.
基金supported by the National Natural Science Foun-dation of China(nos.52073299,51902329)Shanghai Sailing Pro-gram(no.22YF1455700)+4 种基金Natural Science Foundation of Shanghai(no.20ZR1465400)Youth Innovation Promotion Association(CAS,no.2022251)T.Cs.and J.D.acknowledge the financial support of projects:VEGA 2/0174/21T.Cs.was supported by the project Strengthecs(no.H2020-MSCA-IF)of the Slovak Academy of SciencesJ.D.gratefully acknowledge the support of ESET and Alexander von Humboldt Foundations.
文摘High-hardness rock-salt structured transitional metal carbides(TMC)are attracting substantial interest as potential next-generation thermal protection materials.However,the intrinsic brittleness of TMC ceramics impedes their performance in aerodynamically harsh environments.In this work,a promising strategy is proposed to introduce plasticity in TaC–HfC solid solutions by manipulating carbon deficiency.The approach combines density-functional theory(DFT)with experiments and takes Pugh's ratio(k)as the criteria.Depletion of carbon atoms in TaC–HfC solid solutions results in the de-localizing of valence electrons,deviation of spatial modulus along different crystal plane directions,and leading to significant elastic anisotropy.The carbon deficient Ta_(0.8)Hf_(0.2)C_(0.8) is predicted to be a‘softer phase’with reduced modulus and Pugh's ratio(k=0.58).A series of Ta1–xHfxCy(x=0.2 and 0.8,y=0.8,0.9,and 1.0)bulk ceramics are experimentally fabricated by an excessive metal alloying method.Trigonal and hexagonal close-packed structured carbides are derived when the carbon deficiency y decreased to 0.7.The indentation modulus drops from 641.8±14.8 GPa for Ta_(0.8)Hf_(0.2)C_(1.0) to 555.8±9.9 GPa for Ta0.8Hf0.2C0.8.The specific stoichiometric composition of Ta_(0.8)Hf_(0.2)C_(0.8) is experimentally verified to possess both plasticity(k=0.41)and ultra-high nanohardness(41.3±1.3 GPa).
基金supported by the National Natural Science Foundation of China(52202327 and 51972326)the Science and Technology Commission of Shanghai Municipality(22ZR1471300)the Program of Shanghai Academic Research Leader(22XD1424300)。
文摘钠离子电池因其成本低、资源丰富等优点而成为新一代储能设备.在各种正极中,隧道型Na_(0.44)MnO_(2)因其较大的Na^(+)通道,被认为是快速充电电池的合适正极材料,但仍然存在Na^(+)动力学缓慢等问题.本文首次提出了一种Na_(0.44)MnO_(2)的新型离子交换方法,通过调节合成条件,可以很好地控制K^(+)残余量和Na_(0.44)MnO_(2)的尺寸.结果表明,Na_(0.44)MnO_(2)结构中的残留K^(+)扩大了Na^(+)的输运通道,小颗粒形貌缩短了Na^(+)的迁移距离,且晶体中的带状缺陷界面进一步加速了Na^(+)的输运.获得的Na_(0.44)MnO_(2)具有本征赝电容特性,在2-4 V和20 C电流下有79.0 mA h g^(-1)的优异倍率性能.长期循环测试表明,20 C下1000次循环的保持率为98.1%,0.5 C下200次循环的保持率为96.3%.本工作为用于快速充电储能装置的高倍率、高稳定性Na_(0.44)MnO_(2)正极的大规模生产提供了一条新途径.
基金supported by the National Key Research and Development Program of China(2019YFA0210600)the National Natural Science Foundation of China(51922103 and BC0500463)。
文摘有机电极具有结构可设计性强、容量大、可容纳大离子等优点.然而,在钠离子电池中,有机电极材料的容量仍然很低,且其在有机电解质中的高溶解度导致其寿命较短.如何通过化合物设计来提高其性能一直是研究人员关注的问题.本研究通过简单方法将氨基酸接枝到有机化合物上,提高了其容量和循环稳定性.首先,氨基酸之间的氢键使其形成更稳定的层状结构;氨基酸基团在有机电极材料和羧甲基纤维素粘合剂之间形成分子间相互作用,降低界面阻力,显著提高循环稳定性,使得钠离子电池循环次数超过2000次.其次,实验和计算结果表明,氨基酸基团提供了Na^(+)转运途径和额外的可逆存储位点,从而提高了比容量(~300 mA h g^(-1)).本策略可以启发未来钠离子电池的有机分子设计.
基金the support of National Key Project of Research and Development Plan No.2018YFB0703600NSFC program No.51872133 and 51572282Guangdong Innovative and Entrepreneurial Research Team Program,No.2016ZT06G578.
文摘The past years has observed a significantly boost of the thermoelectric materials in the scale of thermoelectric figure-of-merit,i.e.ZT,because of its promising application to harvest the widely distributed waste heat.However,the simplified thermoelectric materials'performance scale also shifted the focus of thermoelectric energy conversion technique from devices-related efforts to materials-level works.As a result,the thermoelectric devices-related works didn't get enough attention.The device-level challenges behind were kept unknown until recent years.However,besides the thermoelectric materials properties,the practical energy conversion efficiency and service life of thermoelectric device is highly determined by assembling process and the contact interface.In this perspective,we are trying to shine some light on the device-level challenge,and give a special focus on the thermoelectric interface materials(TEiM)between the thermoelectric elements and electrode,which is also known as the metallization layer or solder barrier layer.We will go through the technique concerns that determine the scope of the TEiM,including bonding strength,interfacial resistance and stability.Some general working principles are summarized before the discussion of some typical examples of searching proper TEiM for a given thermoelectric conversion material.
基金supported by the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (No. SKL201904SIC)State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology)(No. 2020-KF-12)the Opening Project of State Key Laboratory of Metastable Materials Science and Technology (No. 202007)。
文摘Commercial lithium-ion batteries (LIBs) have been widely used in various energy storage systems. However, many unfavorable factors of LIBs have prompted researchers to turn their attention to the development of emerging secondary batteries. Aqueous zinc ion batteries (AZIBs) present some prominent advantages with environmental friendliness, low cost and convenient operation feature. MnO_(2) electrode is the first to be discovered as promising cathode material. So far, manganese-based oxides have made significant progresses in improving the inherent capacity and energy density. Herein, we summarize comprehensively recent advances of Mn-based compounds as electrode materials for ZIBs. Especially, this review focuses on the design strategies of electrode structures, optimization of the electrochemical performance and the clarification of energy storage mechanisms. Finally, their future research directions and perspective are also proposed.
基金National Key Research And Development Program(No.2016YFB0901600)CAS Center for Excellence in Superconducting Electronics+3 种基金the Key Research Program of Chinese Academy of Sciences(Nos.QYZDJ-SSWJSC013 and KGZD-EW-T06)National Natural Science Foundation of China(Nos.21871008 and 21801247)Jingdezhen Science and Technology Bureau(No.20192GYZD008-21)Science Foundation for Youth Scholar of State Key Laboratory of High Performance Ceramics and Superfine Microstructures(No.SKL 201804)。
文摘Due to the relatively sluggish charge carrier separation in metal sulfides,the photocatalytic activity of them is still far lower than expected.Herein,sulfur vacancies and in-plane SnS_(2)/SnO_(2) heterojunction were successfully introduced into the SnS_(2) nanosheets through high energy ball-milling.These defective structures were studied by the electron paramagnetic resonance,Raman spectra,X-ray photoelectron spectroscopy,and high-resolution transmission electron microscope analyses.The sulfur vacancies and in-plane heterojunctions strongly accelerate the separation of photoexcited electron-hole pairs,as confirmed by the photo luminesce nce emission spectra and time-resolved photoluminescence decay spectra.The introduction of sulfur vacancies and in-plane heterojunction in SnS_(2) nanosheets results in roughly six times higher photodegrading rate for methyl orange and four times higher photocatalytic reduction rate of Cr6+than those of pure SnS_(2) nanosheets.
基金financially supported by the National Natural Science Foundation of China(51831011,31870944)Medical discipline Construction Project of Pudong Health Committee of Shanghai(PWYts2021-05)Postdoctoral Science Foundation of China(2021 M693260).
文摘The immune response induced by surface topography crucially determines the implant success.However,how the immune response is mediated by the size of surface topography remains unclear.Hence,various biocompatible Mg-Al layered double hydroxides sheet-array films with different sizes(nano,micro and nano/micro mixture)were constructed on the biomedical titanium,and their osteo-immunomodulation effects on the macrophages were explored.The nano-sheet array structures significantly promoted the polarization of M2 macrophages by activating the PI3K-AKT-mTOR signaling pathway with high gene expressions of integrin b2 and FAK.While the micro-sheet array structures enhanced osteogenic differentiation of mouse bone marrow mesenchymal stem cells(mBMSCs)via ROCK-YAP/TAZ-mediated mechanotransduction.Moreover,the nano-sheet array structures promoted the osteogenic differentiation of mBMSCs with a high proportion of M2 macrophages through a shared medium.This study gave further information concerning integrin-induced focal adhesions in cells of different sheet array structures and their role in macrophage polarization and osteogenic differentiation of mBMSCs,which might help to design biomaterial surfaces with optimal geometry for a desired immunemodulation.
基金supported by the National Natural Science Foundation of China (22005006,21871008,22001263)the China Postdoctoral Science Foundation (2019M660298,2020T130009)
文摘The salt-inclusion materials have drawn significant attention for their manifold structural chemistry and novel physical/chemical properties.Herein,two new salt-inclusion chalcohalides,[Cs_(6)Cl][Ga_(5)GeQ_(12)](Q=S,Se),have been discovered via hightemperature flux methods.The two isostructural compounds are constructed by porous[Ga_(5)GeQ_(12)]^(5−)layers with[ClCs_(6)]^(5+)octahedra filled in the holes.The[Ga_(5)GeQ_(12)]^(5−)layer is composed of the honeycomb-like(Ga/Ge)_(18)Q_(42)rings containing(Ga/Ge)_(3)Q_(9)trimer as basic unit.The band gaps of the two compounds are 3.90 and 2.89 eV,respectively.[Cs_(6)Cl][Ga_(5)GeS_(12)]exhibits interesting two-band emission properties which are related to the intermediate-band electronic structure revealed by density functional theory(DFT)calculations.Owing to the porous layered structure,[Cs_(6)Cl][Ga_(5)GeS_(12)]exhibits topological ion exchange ability towards Cd^(2+)ions with the maximum sorption capacity of 250 mg/g and high distribution coefficient(Kd)near 106 mL/g.This work further enriches the structural diversity of salt-inclusion materials and extends their potential application range to ion exchange adsorption.
基金supported by the NASA Science Missions Directorate’s Radioisotope Power Systems Technology Advancement Program.This work made use of the MatCI Facility which receives support from the MRSEC Program(NSF DMR-1720139)of the Materials Research Center at Northwestern University.This work made use,as well,of the EPIC facility of Northwestern University’s NUANCE Center,which has received support from the Soft and Hybrid Nanotechnology Experimental(SHyNE)Resource(NSF ECCS-1542205)the MRSEC program(NSF DMR-1720139)at the Materials Research Center+3 种基金the International Institute for Nanotechnology(IIN)the Keck Foundationthe State of Illinois,through the IIN.This work also made use of the IMSERC at Northwestern University,which has received support from the Soft and Hybrid Nanotechnology Experimental(SHyNE)Resource(NSF ECCS-1542205)the State of Illinois and International Institute for Nanotechnology(IIN).GJS Acknowledges support from the NASA Science Mission Directorate’s Radioisotope Power Systems Thermoelectric Technology Development program.
文摘Upon uniaxial compressive loading at 500℃(T/Tm=0.67,where Tm is the absolute melting point),the n-type Skutterudite alloy Yb03Co4Sb12 deforms plastically by creep via a power-law,with a stress exponent~3 consistent with dislocation viscous glide.An activation energy of 171 kJ/mol is measured over the temperature range of 500-587℃(T/Tm=0.67-0.75)at a stress of 30 MPa.Yb_(0.3)Co_(4)Sb_(12)is ductile at 500℃,exhibiting a compressive strain of 25%when subjected to stresses ranging from 22 to 90 MPa for up to 28 days.Among the thermoelectric materials tested so far for creep,Yb_(0.3)Co_(4)Sb_(12)exhibits a creep resistance intermediate between low-melting(Bi2Te3,TAGS-85)and high-melting thermoelectrics(Mg2Si and ZrNiSn).A relatively modest drop in the figure of merit zT,from 0.67 to 0.52,is displayed by Yb_(0.3)Co_(4)Sb_(12)after accumulating 3.7%compressive creep strain at 500℃,mostly due to a drop in electrical conductivity.