Low-temperature assembly of MXene nanosheets into three-dimensional(3D) robust aerogels addresses the crucial stability concern of the nano-building blocks during the fabrication process,which is of key importance for...Low-temperature assembly of MXene nanosheets into three-dimensional(3D) robust aerogels addresses the crucial stability concern of the nano-building blocks during the fabrication process,which is of key importance for transforming the fascinating properties at the nanoscale into the macroscopic scale for practical applications.Herein,suitable cross-linking agents(amino-propyltriethoxysilane,Mn^(2+),Fe^(2+),Zn^(2+),and Co^(2+)) as interfacial mediators to engineer the interlayer interactions are reported to realize the graphene oxide(GO)-assisted assembly of Ti_(3)C_(2)T_(x) MXene aerogel at room temperature.This elaborate aerogel construction not only suppresses the oxidation degradation of Ti_(3)C_(2)T_(x) but also generates porous aerogels with a high Ti_(3)C_(2)T_(x) content(87 wt%) and robustness,thereby guaranteeing the functional accessibility of Ti_(3)C_(2)T_(x) nanosheets and operational reliability as integrated functional materials.In combination with a further sulfur modification,the Ti_(3)C_(2)T_(x) aerogel electrode shows promising electrochemical performances as the freestanding anode for sodium-ion storage.Even at an ultrahigh loading mass of 12.3 mg cm^(-2),a pronounced areal capacity of 1.26 mAh cm^(-2) at a current density of 0.1 A g^(-1) has been achieved,which is of practical significance.This work conceptually suggests a new way to exert the utmost surface functionalities of MXenes in 3D monolithic form and can be an inspiring scaffold to promote the application of MXenes in different areas.展开更多
The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious int...The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious interfacial instability,which is a big challenge for design and application of nonflammable GPEs.Here,a nonflammable GPE(SGPE)is developed by in situ polymerizing trifluoroethyl methacrylate(TFMA)monomers with flame-retardant triethyl phosphate(TEP)solvents and LiTFSI–LiDFOB dual lithium salts.TEP is strongly anchored to PTFMA matrix via polarity interaction between-P=O and-CH_(2)CF_(3).It reduces free TEP molecules,which obviously mitigates interfacial reactions,and enhances flame-retardant performance of TEP surprisingly.Anchored TEP molecules are also inhibited in solvation of Li^(+),leading to anion-dominated solvation sheath,which creates inorganic-rich solid electrolyte interface/cathode electrolyte interface layers.Such coordination structure changes Li^(+)transport from sluggish vehicular to fast structural transport,raising ionic conductivity to 1.03 mS cm^(-1) and transfer number to 0.41 at 30℃.The Li|SGPE|Li cell presents highly reversible Li stripping/plating performance for over 1000 h at 0.1 mA cm^(−2),and 4.2 V LiCoO_(2)|SGPE|Li battery delivers high average specific capacity>120 mAh g^(−1) over 200 cycles.This study paves a new way to make nonflammable GPE that is compatible with Li metal anode.展开更多
TiO2 nano powders with Mn concentration of 0 at%-12 at% were synthesized by the sol-gel process, and were annealed at 500 ℃ and 800 ℃ in air for 2 hrs. X-ray diffraction (XRD) measurements indicate that the Mn-TiO...TiO2 nano powders with Mn concentration of 0 at%-12 at% were synthesized by the sol-gel process, and were annealed at 500 ℃ and 800 ℃ in air for 2 hrs. X-ray diffraction (XRD) measurements indicate that the Mn-TiO2 nano powders with Mn concentration of 1 at% and 2 at% annealed at 500 and 800 ℃ are of pure anatase and rutile, respectively. The scanning electron microscope (SEM) observations reveal that the crystal grain size increases with the annealing temperature, and the high resolution transmission electron microscopy (HRTEM) investigations further indicate that the samples are well crystallized, confirming that Mn has doped into the TiO2 crystal lattice effectively. The room temperature ferromagnetism, which could be explained within the scope of the bound magnetic polaron (BMP) theory, is detected in the Mn-TiO2 samples with Mn concentration of 2 at%, and the magnetization of the powders annealed at 500 ℃ is stronger than that of the sample treated at 800 ℃. The UV-VIS diffuse reflectance spectra results demonstrate that the absorption of the TiO2 powders could be enlarged by the enhanced trapped electron absorption caused by Mn doping.展开更多
The presence of endogenous neural stem/progenitor cells in the adult mammalian brain suggests that the central nervous system can be repaired and regenerated after injury.However,whether it is possible to stimulate ne...The presence of endogenous neural stem/progenitor cells in the adult mammalian brain suggests that the central nervous system can be repaired and regenerated after injury.However,whether it is possible to stimulate neurogenesis and reconstruct cortical layers II to VI in non-neurogenic regions,such as the cortex,remains unknown.In this study,we implanted a hyaluronic acid collagen gel loaded with basic fibroblast growth factor into the motor cortex immediately following traumatic injury.Our findings reveal that this gel effectively stimulated the proliferation and migration of endogenous neural stem/progenitor cells,as well as their differentiation into mature and functionally integrated neurons.Importantly,these new neurons reconstructed the architecture of cortical layers II to VI,integrated into the existing neural circuitry,and ultimately led to improved brain function.These findings offer novel insight into potential clinical treatments for traumatic cerebral cortex injuries.展开更多
La0.5Sm0.2Sr0.3MnO3/(Ag2O)x/2 (x = 0.00, 0.04, 0.08, 0.25, 0.30) samples were prepared by the solid-state reaction method, and their transport behaviors, transport mechanism, and magnetoresistance effect were stud...La0.5Sm0.2Sr0.3MnO3/(Ag2O)x/2 (x = 0.00, 0.04, 0.08, 0.25, 0.30) samples were prepared by the solid-state reaction method, and their transport behaviors, transport mechanism, and magnetoresistance effect were studied through the measurement and fitting of p-T curves. The results show that the element Ag takes part in reaction when the doping amount is small. Ag is mainly distributed at the grain boundary of the host material and is in metallic state when the doping amount is relatively large; then the system becomes a two-phase composite. A small amount of Ag doping can apparently increase grain-boundary magnetoresistance induced by the spin-dependent scattering. The resistivity of the sample doped with 30 mol% Ag is one order of magnitude smaller than that of low-doped samples, and its magnetoresistance in the magnetic field of 0.5 T and at 300 K is strengthened apparently reaching 9.4%, which is connected not only with the improvement of the grain-boundary structure of the host material but also with the decrease of material resistivity.展开更多
Synthesis and applications of three-dimensional(3 D)porous graphene frameworks(GFs)have attracted extensive interest owing to their intriguing advantages of high specific surface area,enriched porosity,excellent elect...Synthesis and applications of three-dimensional(3 D)porous graphene frameworks(GFs)have attracted extensive interest owing to their intriguing advantages of high specific surface area,enriched porosity,excellent electrical conductivity,exceptional compressibility and processability.However,it is still challenging for economically viable,fast and scalable assembly of 3 D GFs at room-temperature.Herein,we reported a one-step scalable strategy for fast self-assembly of graphene oxide into 3 D macroscopically porous GFs,with assistance of polyoxometalates(POM)as functional cross-linker and hydrazine hydrate as reductant at room-temperature.The resulting 3 D interconnected macroporous POM-GFs uniformly decorated with ultrasmall POM nanoclusters were directly processed into binder-/additive-free film compact electrodes(1.68 g cm^(-3))with highly aligned,layer-stacked structure and electrically conductivity(622 S m-1)for high-performance supercapacitors,showing an impressive gravimetric capacitance of205 F g-1,volumetric capacitance of 334 F cm^(-3) at 1 mV s^(-1),and remarkable cycling stability with capacitance retention of 83%after 10,000 cycles,outperforming the most reported GFs.Further,the solid-state supercapacitors offered excellent gravimetric capacitance of 157 F g-1 exceptionally volumetric capacitance of 115 F cm^(-3) at 2 mV s^(-1) based on single electrode,and volumetric energy density of2.6 mWh cm^(-3).Therefore,this work will open novel opportunities to room-temperature fast assembly of 3 D porous graphene architectures for high-energy-density supercapacitors.展开更多
Benzoin condensation promoted efficiently in three imidazolium based room tempera- ture ionic liquids [bmim]Br, [bmim]BF4 and [Bnmim]BF4 is reported for the first time. Benzoins were obtained in up to 91% yield within...Benzoin condensation promoted efficiently in three imidazolium based room tempera- ture ionic liquids [bmim]Br, [bmim]BF4 and [Bnmim]BF4 is reported for the first time. Benzoins were obtained in up to 91% yield within less than 30 min under mild conditions.展开更多
This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and ...This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and status are investigated.A sulfur-rich composite with most sulfur dispersed on the surface of a carbon host can realize a high loading ratio(72%S).In contrast,a confined sulfur sample can encapsulate S into the pores of the carbon host with a low loading ratio(44%S).In carbonate ester electrolyte,only the sulfur trapped in porous structures is active via‘solid-solid’behavior during cycling.The S cathode with high surface sulfur shows poor reversible capacity because of the severe side reactions between the surface polysulfides and the carbonate ester solvents.To improve the capacity of the sulfur-rich cathode,ether electrolyte with NaNO_(3) additive is explored to realize a‘solid-liquid’sulfur redox process and confine the shuttle effect of the dissolved polysulfides.As a result,the sulfur-rich cathode achieved high reversible capacity(483 mAh g^(−1)),corresponding to a specific energy of 362 Wh kg^(−1) after 200 cycles,shedding light on the use of ether electrolyte for high-loading sulfur cathode.展开更多
A novel green nanophosphor CaHPO4:Tb3+ was synthesized via a room-temperatureco-precipitation route driven by ethanol solvent. X-ray powder diffraction (XRD), scanningelectron microscopy (SEM) and photoluminesce...A novel green nanophosphor CaHPO4:Tb3+ was synthesized via a room-temperatureco-precipitation route driven by ethanol solvent. X-ray powder diffraction (XRD), scanningelectron microscopy (SEM) and photoluminescence spectroscopy (PL) techniques were utilizedto characterize the structure, morphology and fluorescence performance of the obtained powders.The results demonstrated that the prepared samples were well crystallized with triclinic phaseCaHPO4 structure and particle-like morphology. Photoluminescence measurements indicated thatCaHPOa:Tb3+ had a strong absorption peak at 370 nm and exhibited characteristic emissions withseveral sharp peaks corresponding to the transitions 5D4-7FJ (jr = 6-3) of Tb3+. Moreover, theluminescence optimum concentration for CaHPO4:Tb3+ was determined to be 11 mol%, whichmight be a promising green-emitting ohosohor for display applications.展开更多
The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(>...The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(> 400 ℃) conditions.Herein, a highly active catalytic conversion process of ethane at room temperature(25 ℃) is reported on single iron atoms confined in graphene via the porphyrin-like N4-coordination structures.Combining with the operando time of flight mass spectrometer and density functional theory calculations, the reaction is identified as a radical mechanism, in which the C–H bonds of the same C atom are preferentially and sequentially activated, generating the value-added C2 chemicals, simultaneously avoiding the over-oxidation of the products to CO2.The in-situ formed O–FeN4–O structure at the single iron atom serves as the active center for the reaction and facilitates the formation of ethyl radicals.This work deepens the understanding of alkane C–H activation on the FeN4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane.展开更多
To clarify the contribution of oxygen vacancies to room-temperature ferromagnetism(RTFM)in cobalt doped TiO_(2)(Co-TiO_(2)),and in order to obtain the high level of magnetization suitable for spintronic devices,in thi...To clarify the contribution of oxygen vacancies to room-temperature ferromagnetism(RTFM)in cobalt doped TiO_(2)(Co-TiO_(2)),and in order to obtain the high level of magnetization suitable for spintronic devices,in this work,Co-TiO_(2) nano-particles are prepared via the sol-gel route,followed by vacuum annealing for different durations,and the influence of vacu-um annealing duration on the structure and room-temperature magnetism of the compounds is examined.The results reveal that with an increase in annealing duration,the concentration of oxygen vacancies rises steadily,while the saturation magnetiza-tion(Ms)shows an initial gradual increase,followed by a sharp decline,and even disappearance.The maximum Ms is as high as 1.19 emu/g,which is promising with respect to the development of spintronic devices.Further analysis reveals that oxygen va-cancies,modulated by annealing duration,play a critical role in tuning room-temperature magnetism.An appropriate concentra-tion of oxygen vacancies is beneficial in terms of promoting RTFM in Co-TiO_(2).However,excessive oxygen vacancies will result in a negative impact on RTFM,due to antiferromagnetic superexchange interactions originating from nearest-neighbor Co^(2+)ions.展开更多
Fault fractures usually have large openings and considerable extension. Accordingly, cross-linked gel materials aregenerally considered more suitable plugging agents than water-based gels because the latter often unde...Fault fractures usually have large openings and considerable extension. Accordingly, cross-linked gel materials aregenerally considered more suitable plugging agents than water-based gels because the latter often undergo contaminationvia formation water, which prevents them from being effective over long times. Hence, in this study, aset of oil-based composite gels based on waste grease and epoxy resin has been developed. These materials havebeen observed to possess high compressive strength and resistance to the aforementioned contamination, therebyleading to notable increase in plugging success rate. The compressive strength, thickening time, and resistance toformation water pollution of these gels have been evaluated indoors. The results show that the compressivestrength of the gel can reach 11 MPa;additionally, the related gelation time can be controlled to be more than3 h, thereby providing a safe construction time;Invasion of formation water has a small effect on the gel strengthand does not shorten the thickening time. All considered performance indicators of the oil-based gel confirm itssuitability as a plugging agent for fault fractures.展开更多
Organic materials with room-temperature phosphorescence(RTP)emission have attracted extensive attention owing to their extraordinary properties,including long lifetime,large Stokes shift,and stimuliresponsiveness,and ...Organic materials with room-temperature phosphorescence(RTP)emission have attracted extensive attention owing to their extraordinary properties,including long lifetime,large Stokes shift,and stimuliresponsiveness,and show bright prospects in broad fields.Numerous design strategies,such as creating a rigid environment through crystallization and supramolecular assembly,can be employed to improve the luminescent characteristics of RTP materials by restricting nonradiative transition,enhancing intersystem crossing,and so forth.This review summarizes recent progress with organic room-temperature phosphorescent materials from the perspective of practical applications,including luminescence and display,environmental detection,and bioimaging,and the challenges and prospects will be discussed at the end,which should assist with future research on the application of RTP materials.展开更多
Two-dimensional (2D) ferromagnetic semiconductors have been recognized as the most promising candidates for next-generation low-cost, high-performance and nano-scale spintronic applications such as spin field-effect t...Two-dimensional (2D) ferromagnetic semiconductors have been recognized as the most promising candidates for next-generation low-cost, high-performance and nano-scale spintronic applications such as spin field-effect transistors and quantum computation/communication. However, as one of the 125 important scientific issues raised by Science journal in 2005 that "is it possible to create magnetic semiconductors that work at room temperature?", how to achieve a feasible ferromagnetic semiconductor with high Curie temperature is still a long-standing challenge despite of tremendous efforts have been devoted in this field since 1960s. The recent discovery of 2D ferromagnetic semiconductors Cr2Ge2Te6 and CrI3 has evoked new research interests in 2D intrinsic ferromagnetic semiconductors. But the low Curie temperature (<45 K) of these materials is still badly hindering their industrial applications.展开更多
Attempts have been made to use cell transplantation and biomaterials to promote cell proliferation,differentiation,migration,and survival,as well as angiogenesis,in the context of brain injury.However,whether bioactiv...Attempts have been made to use cell transplantation and biomaterials to promote cell proliferation,differentiation,migration,and survival,as well as angiogenesis,in the context of brain injury.However,whether bioactive materials can repair the damage caused by ischemic stroke by activating endogenous neurogenesis and angiogenesis is still unknown.In this study,we applied chitosan gel loaded with basic fibroblast growth factor to the stroke cavity 7 days after ischemic stroke in rats.The gel slowly released basic fibroblast growth factor,which improved the local microenvironment,activated endogenous neural stem/progenitor cells,and recruited these cells to migrate toward the penumbra and stroke cavity and subsequently differentiate into neurons,while enhancing angiogenesis in the penumbra and stroke cavity and ultimately leading to partial functional recovery.This study revealed the mechanism by which bioactive materials repair ischemic strokes,thus providing a new strategy for the clinical application of bioactive materials in the treatment of ischemic stroke.展开更多
Organic room-temperature phosphorescence(RTP)materials have garnered considerable attention in the fields of biosensing,optoelectronic devices,and anticounterfeiting because of their substantial Stokes shifts,tunable ...Organic room-temperature phosphorescence(RTP)materials have garnered considerable attention in the fields of biosensing,optoelectronic devices,and anticounterfeiting because of their substantial Stokes shifts,tunable emission wavelengths,and prolonged lifetimes.These materials offer remarkable advantages for biological imaging applications by effectively reducing environmental autofluorescence and enhancing imaging resolution.Recently,host-guest systems have been employed as efficient approaches to fabricate pure-organic RTP materials for bioimaging,providing benefits such as controllable preparation and flexible modulation.Consequently,an increasing number of corresponding studies are being reported;however,a comprehensive systematic review is still lacking.Therefore,we summarize recent advances in the development of pureorganic RTP materials using host-guest systems with regard to bioimaging,including rigid matrices and sensitization.The challenge and potential of RTP for biological imaging are also proposed to promote the biomedical applications of organic RTP materials with excellent optical properties.展开更多
Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery...Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery damage or fracture is a critical concern.Water-based(aqueous)electrolytes have been receiving attention as an alternative to organic electrolytes.However,a narrow electrochemicalstability window,water decomposition,and the consequent low battery operating voltage and energy density hinder the practical use of aqueous electrolytes.Therefore,developing novel aqueous electrolytes for sustainable,safe,high-performance LIBs remains challenging.This Review first commences by summarizing the roles and requirements of electrolytes–separators and then delineates the progression of aqueous electrolytes for LIBs,encompassing aqueous liquid and gel electrolyte development trends along with detailed principles of the electrolytes.These aqueous electrolytes are progressed based on strategies using superconcentrated salts,concentrated diluents,polymer additives,polymer networks,and artificial passivation layers,which are used for suppressing water decomposition and widening the electrochemical stability window of water of the electrolytes.In addition,this Review discusses potential strategies for the implementation of aqueous Li-metal batteries with improved electrolyte–electrode interfaces.A comprehensive understanding of each strategy in the aqueous system will assist in the design of an aqueous electrolyte and the development of sustainable and safe high-performance batteries.展开更多
The rapid development of the Internet of Things and artificial intelligence technologies has increased the need for wearable,portable,and self-powered flexible sensing devices.Triboelectric nanogenerators(TENGs)based ...The rapid development of the Internet of Things and artificial intelligence technologies has increased the need for wearable,portable,and self-powered flexible sensing devices.Triboelectric nanogenerators(TENGs)based on gel materials(with excellent conductivity,mechanical tunability,environmental adaptability,and biocompatibility)are considered an advanced approach for developing a new generation of flexible sensors.This review comprehensively summarizes the recent advances in gel-based TENGs for flexible sensors,covering their principles,properties,and applications.Based on the development requirements for flexible sensors,the working mechanism of gel-based TENGs and the characteristic advantages of gels are introduced.Design strategies for the performance optimization of hydrogel-,organogel-,and aerogel-based TENGs are systematically summarized.In addition,the applications of gel-based TENGs in human motion sensing,tactile sensing,health monitoring,environmental monitoring,human-machine interaction,and other related fields are summarized.Finally,the challenges of gel-based TENGs for flexible sensing are discussed,and feasible strategies are proposed to guide future research.展开更多
A Pickering emulsion based on sodium starch octenyl succinate(SSOS)was prepared and its effects on the physicochemical properties of hairtail myofibrillar protein gels(MPGs)subjected to multiple freeze-thaw(F-T)cycles...A Pickering emulsion based on sodium starch octenyl succinate(SSOS)was prepared and its effects on the physicochemical properties of hairtail myofibrillar protein gels(MPGs)subjected to multiple freeze-thaw(F-T)cycles were investigated.The whiteness,water-holding capacity,storage modulus(G')and texture properties of the MPGs were significantly improved by adding 1%-2%Pickering emulsion(P<0.05).Meanwhile,Raman spectral analysis demonstrated that Pickering emulsion promoted the transformation of secondary structure,enhanced hydrogen bonds and hydrophobic interactions,and promoted the transition of disulfide bond conformation from g-g-g to g-g-t and t-g-t.At an emulsion concentration of 2%,theα-helix content decreased by 10.37%,while theβ-sheet content increased by 7.94%,compared to the control.After F-T cycles,the structure of the MPGs was destroyed,with an increase in hardness and a decrease in whiteness and water-holding capacity,however,the quality degradation of MPGs was reduced with 1%-2%Pickering emulsion.These findings demonstrated that SSOS-Pickering emulsions,as potential fat substitutes,can enhance the gel properties and the F-T stability of MPGs.展开更多
基金This work was supported by the National Natural Science Foundation of China(52071137,51977071,51802040,and 21802020)the Science and Technology Innovation Program of Hunan Province(2021RC3066 and 2021RC3067)+1 种基金the Natural Science Foundation of Hunan Province(2020JJ3004 and 2020JJ4192)N.Zhang and X.Xie also acknowledge the financial support of the Fundamental Research Funds for the Central Universities.
文摘Low-temperature assembly of MXene nanosheets into three-dimensional(3D) robust aerogels addresses the crucial stability concern of the nano-building blocks during the fabrication process,which is of key importance for transforming the fascinating properties at the nanoscale into the macroscopic scale for practical applications.Herein,suitable cross-linking agents(amino-propyltriethoxysilane,Mn^(2+),Fe^(2+),Zn^(2+),and Co^(2+)) as interfacial mediators to engineer the interlayer interactions are reported to realize the graphene oxide(GO)-assisted assembly of Ti_(3)C_(2)T_(x) MXene aerogel at room temperature.This elaborate aerogel construction not only suppresses the oxidation degradation of Ti_(3)C_(2)T_(x) but also generates porous aerogels with a high Ti_(3)C_(2)T_(x) content(87 wt%) and robustness,thereby guaranteeing the functional accessibility of Ti_(3)C_(2)T_(x) nanosheets and operational reliability as integrated functional materials.In combination with a further sulfur modification,the Ti_(3)C_(2)T_(x) aerogel electrode shows promising electrochemical performances as the freestanding anode for sodium-ion storage.Even at an ultrahigh loading mass of 12.3 mg cm^(-2),a pronounced areal capacity of 1.26 mAh cm^(-2) at a current density of 0.1 A g^(-1) has been achieved,which is of practical significance.This work conceptually suggests a new way to exert the utmost surface functionalities of MXenes in 3D monolithic form and can be an inspiring scaffold to promote the application of MXenes in different areas.
基金supported by the National Natural Science Foundation of China(Nos.52172214,52272221,52171182)the Postdoctoral Innovation Project of Shandong Province(No.202102003)+2 种基金The Key Research and Development Program of Shandong Province(2021ZLGX01)the Qilu Young Scholar ProgramHPC Cloud Platform of Shandong University are also thanked.
文摘The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious interfacial instability,which is a big challenge for design and application of nonflammable GPEs.Here,a nonflammable GPE(SGPE)is developed by in situ polymerizing trifluoroethyl methacrylate(TFMA)monomers with flame-retardant triethyl phosphate(TEP)solvents and LiTFSI–LiDFOB dual lithium salts.TEP is strongly anchored to PTFMA matrix via polarity interaction between-P=O and-CH_(2)CF_(3).It reduces free TEP molecules,which obviously mitigates interfacial reactions,and enhances flame-retardant performance of TEP surprisingly.Anchored TEP molecules are also inhibited in solvation of Li^(+),leading to anion-dominated solvation sheath,which creates inorganic-rich solid electrolyte interface/cathode electrolyte interface layers.Such coordination structure changes Li^(+)transport from sluggish vehicular to fast structural transport,raising ionic conductivity to 1.03 mS cm^(-1) and transfer number to 0.41 at 30℃.The Li|SGPE|Li cell presents highly reversible Li stripping/plating performance for over 1000 h at 0.1 mA cm^(−2),and 4.2 V LiCoO_(2)|SGPE|Li battery delivers high average specific capacity>120 mAh g^(−1) over 200 cycles.This study paves a new way to make nonflammable GPE that is compatible with Li metal anode.
基金Project supported by the Innovation Foundation of BUAA for PhD Graduates (Grant No. 292122)Equipment Research Foundation of China
文摘TiO2 nano powders with Mn concentration of 0 at%-12 at% were synthesized by the sol-gel process, and were annealed at 500 ℃ and 800 ℃ in air for 2 hrs. X-ray diffraction (XRD) measurements indicate that the Mn-TiO2 nano powders with Mn concentration of 1 at% and 2 at% annealed at 500 and 800 ℃ are of pure anatase and rutile, respectively. The scanning electron microscope (SEM) observations reveal that the crystal grain size increases with the annealing temperature, and the high resolution transmission electron microscopy (HRTEM) investigations further indicate that the samples are well crystallized, confirming that Mn has doped into the TiO2 crystal lattice effectively. The room temperature ferromagnetism, which could be explained within the scope of the bound magnetic polaron (BMP) theory, is detected in the Mn-TiO2 samples with Mn concentration of 2 at%, and the magnetization of the powders annealed at 500 ℃ is stronger than that of the sample treated at 800 ℃. The UV-VIS diffuse reflectance spectra results demonstrate that the absorption of the TiO2 powders could be enlarged by the enhanced trapped electron absorption caused by Mn doping.
基金supported by the National Natural Science Foundation of China,Nos.82272171(to ZY),82271403(to XL),81941011(to XL),31971279(to ZY),31730030(to XL)the Natural Science Foundation of Beijing,No.7222004(to HD).
文摘The presence of endogenous neural stem/progenitor cells in the adult mammalian brain suggests that the central nervous system can be repaired and regenerated after injury.However,whether it is possible to stimulate neurogenesis and reconstruct cortical layers II to VI in non-neurogenic regions,such as the cortex,remains unknown.In this study,we implanted a hyaluronic acid collagen gel loaded with basic fibroblast growth factor into the motor cortex immediately following traumatic injury.Our findings reveal that this gel effectively stimulated the proliferation and migration of endogenous neural stem/progenitor cells,as well as their differentiation into mature and functionally integrated neurons.Importantly,these new neurons reconstructed the architecture of cortical layers II to VI,integrated into the existing neural circuitry,and ultimately led to improved brain function.These findings offer novel insight into potential clinical treatments for traumatic cerebral cortex injuries.
基金supported by the Key Program of the National Natural Science Foundation of China (No. 19934003)the Grand Program of Natural Science Research of Anhui Education Department (No. ZD2007003-1)the Natural Science Research Program of Universities and Colleges of Anhui Province, China (Nos. KJ2008A19ZC, KJ2009B281Z, and KJ2009A053Z)
文摘La0.5Sm0.2Sr0.3MnO3/(Ag2O)x/2 (x = 0.00, 0.04, 0.08, 0.25, 0.30) samples were prepared by the solid-state reaction method, and their transport behaviors, transport mechanism, and magnetoresistance effect were studied through the measurement and fitting of p-T curves. The results show that the element Ag takes part in reaction when the doping amount is small. Ag is mainly distributed at the grain boundary of the host material and is in metallic state when the doping amount is relatively large; then the system becomes a two-phase composite. A small amount of Ag doping can apparently increase grain-boundary magnetoresistance induced by the spin-dependent scattering. The resistivity of the sample doped with 30 mol% Ag is one order of magnitude smaller than that of low-doped samples, and its magnetoresistance in the magnetic field of 0.5 T and at 300 K is strengthened apparently reaching 9.4%, which is connected not only with the improvement of the grain-boundary structure of the host material but also with the decrease of material resistivity.
基金financially supported by the National Key R@D Program of China(Grants 2016YFB0100100,2016YFA0200200)the National Natural Science Foundation of China(Grant Nos.51872283,22075279,21805273,22005297,22005298)+7 种基金the Liao Ning Revitalization Talents Program(Grant XLYC1807153)the Natural Science Foundation of Liaoning ProvinceJoint Research Fund Liaoning-Shenyang National Laboratory for Materials Science(Grant 20180510038)Dalian Innovation Support Plan for High Level Talents(2019RT09)the Dalian National Laboratory For Clean Energy(DNL),CASDNL Cooperation Fund,CAS(DNL180310,DNL180308,DNL201912,and DNL201915)DICP(DICP ZZBS201708,DICP ZZBS201802,DICP I2020032)the China Postdoctoral Science Foundation(2019M661141,2020M680995)。
文摘Synthesis and applications of three-dimensional(3 D)porous graphene frameworks(GFs)have attracted extensive interest owing to their intriguing advantages of high specific surface area,enriched porosity,excellent electrical conductivity,exceptional compressibility and processability.However,it is still challenging for economically viable,fast and scalable assembly of 3 D GFs at room-temperature.Herein,we reported a one-step scalable strategy for fast self-assembly of graphene oxide into 3 D macroscopically porous GFs,with assistance of polyoxometalates(POM)as functional cross-linker and hydrazine hydrate as reductant at room-temperature.The resulting 3 D interconnected macroporous POM-GFs uniformly decorated with ultrasmall POM nanoclusters were directly processed into binder-/additive-free film compact electrodes(1.68 g cm^(-3))with highly aligned,layer-stacked structure and electrically conductivity(622 S m-1)for high-performance supercapacitors,showing an impressive gravimetric capacitance of205 F g-1,volumetric capacitance of 334 F cm^(-3) at 1 mV s^(-1),and remarkable cycling stability with capacitance retention of 83%after 10,000 cycles,outperforming the most reported GFs.Further,the solid-state supercapacitors offered excellent gravimetric capacitance of 157 F g-1 exceptionally volumetric capacitance of 115 F cm^(-3) at 2 mV s^(-1) based on single electrode,and volumetric energy density of2.6 mWh cm^(-3).Therefore,this work will open novel opportunities to room-temperature fast assembly of 3 D porous graphene architectures for high-energy-density supercapacitors.
基金We thank the financial support from the National Natural Science Foundation of China.(No.20172038)
文摘Benzoin condensation promoted efficiently in three imidazolium based room tempera- ture ionic liquids [bmim]Br, [bmim]BF4 and [Bnmim]BF4 is reported for the first time. Benzoins were obtained in up to 91% yield within less than 30 min under mild conditions.
基金This research was supported by the Australian Research Council(ARC)(DE170100928,DP170101467)an Australian Renewable Energy Agency(ARENA)Project(G00849).The authors acknowledge the use of the facilities at the UOW Electron Microscopy Center(LE0882813 and LE0237478)and Dr.Tania Silver for critical reading of the manuscript.
文摘This work reports influence of two different electrolytes,carbonate ester and ether electrolytes,on the sulfur redox reactions in room-temperature Na-S batteries.Two sulfur cathodes with different S loading ratio and status are investigated.A sulfur-rich composite with most sulfur dispersed on the surface of a carbon host can realize a high loading ratio(72%S).In contrast,a confined sulfur sample can encapsulate S into the pores of the carbon host with a low loading ratio(44%S).In carbonate ester electrolyte,only the sulfur trapped in porous structures is active via‘solid-solid’behavior during cycling.The S cathode with high surface sulfur shows poor reversible capacity because of the severe side reactions between the surface polysulfides and the carbonate ester solvents.To improve the capacity of the sulfur-rich cathode,ether electrolyte with NaNO_(3) additive is explored to realize a‘solid-liquid’sulfur redox process and confine the shuttle effect of the dissolved polysulfides.As a result,the sulfur-rich cathode achieved high reversible capacity(483 mAh g^(−1)),corresponding to a specific energy of 362 Wh kg^(−1) after 200 cycles,shedding light on the use of ether electrolyte for high-loading sulfur cathode.
基金supported by the National Natural Science Foundation of China(21663021)China Postdoctoral Science Foundation(2015M571977)+1 种基金the Natural Science Foundation of Jiangxi Province(20161BAB213058)the Natural Science Key Project of Jiangxi Province(2017ACB20040)
文摘A novel green nanophosphor CaHPO4:Tb3+ was synthesized via a room-temperatureco-precipitation route driven by ethanol solvent. X-ray powder diffraction (XRD), scanningelectron microscopy (SEM) and photoluminescence spectroscopy (PL) techniques were utilizedto characterize the structure, morphology and fluorescence performance of the obtained powders.The results demonstrated that the prepared samples were well crystallized with triclinic phaseCaHPO4 structure and particle-like morphology. Photoluminescence measurements indicated thatCaHPOa:Tb3+ had a strong absorption peak at 370 nm and exhibited characteristic emissions withseveral sharp peaks corresponding to the transitions 5D4-7FJ (jr = 6-3) of Tb3+. Moreover, theluminescence optimum concentration for CaHPO4:Tb3+ was determined to be 11 mol%, whichmight be a promising green-emitting ohosohor for display applications.
基金the financial support from the Ministry of Science and Technology of China (Nos.2016YFA0204100 and 2016YFA0200200)the National Natural Science Foundation of China (Nos.21890753, 21573220 and 21802124)+2 种基金the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (No.QYZDB-SSW-JSC020)the DNL Cooperation Fund, CAS (No.DNL180201)the financial and technique supports from the Westlake Education Foundation, Supercomputing Systems in the Information Technology Center of Westlake University
文摘The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources.However, it is a great challenge due to the typically required high temperature(> 400 ℃) conditions.Herein, a highly active catalytic conversion process of ethane at room temperature(25 ℃) is reported on single iron atoms confined in graphene via the porphyrin-like N4-coordination structures.Combining with the operando time of flight mass spectrometer and density functional theory calculations, the reaction is identified as a radical mechanism, in which the C–H bonds of the same C atom are preferentially and sequentially activated, generating the value-added C2 chemicals, simultaneously avoiding the over-oxidation of the products to CO2.The in-situ formed O–FeN4–O structure at the single iron atom serves as the active center for the reaction and facilitates the formation of ethyl radicals.This work deepens the understanding of alkane C–H activation on the FeN4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane.
基金supported by the National Training Program of Innovation and Entrepreneurship for Undergraduates(No.201910389022).
文摘To clarify the contribution of oxygen vacancies to room-temperature ferromagnetism(RTFM)in cobalt doped TiO_(2)(Co-TiO_(2)),and in order to obtain the high level of magnetization suitable for spintronic devices,in this work,Co-TiO_(2) nano-particles are prepared via the sol-gel route,followed by vacuum annealing for different durations,and the influence of vacu-um annealing duration on the structure and room-temperature magnetism of the compounds is examined.The results reveal that with an increase in annealing duration,the concentration of oxygen vacancies rises steadily,while the saturation magnetiza-tion(Ms)shows an initial gradual increase,followed by a sharp decline,and even disappearance.The maximum Ms is as high as 1.19 emu/g,which is promising with respect to the development of spintronic devices.Further analysis reveals that oxygen va-cancies,modulated by annealing duration,play a critical role in tuning room-temperature magnetism.An appropriate concentra-tion of oxygen vacancies is beneficial in terms of promoting RTFM in Co-TiO_(2).However,excessive oxygen vacancies will result in a negative impact on RTFM,due to antiferromagnetic superexchange interactions originating from nearest-neighbor Co^(2+)ions.
基金“Research and Application of Key Techniques for Drilling and Completion of Bozhong 19-6 Condensate Gas Field Development-Phase I”sub topic 4“Research on Leakage Prevention and Plugging Techniques for Fault and Buried Hill Reservoirs”,a Project of China National Offshore Oil (China)Co.,Ltd. (Project No.YXKY-2020-TJ-03).
文摘Fault fractures usually have large openings and considerable extension. Accordingly, cross-linked gel materials aregenerally considered more suitable plugging agents than water-based gels because the latter often undergo contaminationvia formation water, which prevents them from being effective over long times. Hence, in this study, aset of oil-based composite gels based on waste grease and epoxy resin has been developed. These materials havebeen observed to possess high compressive strength and resistance to the aforementioned contamination, therebyleading to notable increase in plugging success rate. The compressive strength, thickening time, and resistance toformation water pollution of these gels have been evaluated indoors. The results show that the compressivestrength of the gel can reach 11 MPa;additionally, the related gelation time can be controlled to be more than3 h, thereby providing a safe construction time;Invasion of formation water has a small effect on the gel strengthand does not shorten the thickening time. All considered performance indicators of the oil-based gel confirm itssuitability as a plugging agent for fault fractures.
基金We gratefully acknowledge the financial support from the National Key Research and Development Program of China(2022YFB3203500)the National Natural Science Foundation of China(21788102,22125803,and 22020102006)+2 种基金project support by the Shanghai Municipal Science and Technology Major Project(Grant No.2018SHZDZX03)Program of Shanghai Academic/Technology Research Leader(20XD1421300)the Fundamental Research Funds for the Central Universities.
文摘Organic materials with room-temperature phosphorescence(RTP)emission have attracted extensive attention owing to their extraordinary properties,including long lifetime,large Stokes shift,and stimuliresponsiveness,and show bright prospects in broad fields.Numerous design strategies,such as creating a rigid environment through crystallization and supramolecular assembly,can be employed to improve the luminescent characteristics of RTP materials by restricting nonradiative transition,enhancing intersystem crossing,and so forth.This review summarizes recent progress with organic room-temperature phosphorescent materials from the perspective of practical applications,including luminescence and display,environmental detection,and bioimaging,and the challenges and prospects will be discussed at the end,which should assist with future research on the application of RTP materials.
文摘Two-dimensional (2D) ferromagnetic semiconductors have been recognized as the most promising candidates for next-generation low-cost, high-performance and nano-scale spintronic applications such as spin field-effect transistors and quantum computation/communication. However, as one of the 125 important scientific issues raised by Science journal in 2005 that "is it possible to create magnetic semiconductors that work at room temperature?", how to achieve a feasible ferromagnetic semiconductor with high Curie temperature is still a long-standing challenge despite of tremendous efforts have been devoted in this field since 1960s. The recent discovery of 2D ferromagnetic semiconductors Cr2Ge2Te6 and CrI3 has evoked new research interests in 2D intrinsic ferromagnetic semiconductors. But the low Curie temperature (<45 K) of these materials is still badly hindering their industrial applications.
基金supported by the National Natural Science Foundation of China,Nos.81941011(to XL),31771053(to HD),31730030(to XL),31971279(to ZY),31900749(to PH),31650001(to XL),31320103903(to XL),31670988(to ZY)the Natural Science Foundation of Beijing,Nos.7222004(to HD)+1 种基金a grant from Ministry of Science and Technology of China,Nos.2017YFC1104002(to ZY),2017YFC1104001(to XL)a grant from Beihang University,No.JKF-YG-22-B001(to FH)。
文摘Attempts have been made to use cell transplantation and biomaterials to promote cell proliferation,differentiation,migration,and survival,as well as angiogenesis,in the context of brain injury.However,whether bioactive materials can repair the damage caused by ischemic stroke by activating endogenous neurogenesis and angiogenesis is still unknown.In this study,we applied chitosan gel loaded with basic fibroblast growth factor to the stroke cavity 7 days after ischemic stroke in rats.The gel slowly released basic fibroblast growth factor,which improved the local microenvironment,activated endogenous neural stem/progenitor cells,and recruited these cells to migrate toward the penumbra and stroke cavity and subsequently differentiate into neurons,while enhancing angiogenesis in the penumbra and stroke cavity and ultimately leading to partial functional recovery.This study revealed the mechanism by which bioactive materials repair ischemic strokes,thus providing a new strategy for the clinical application of bioactive materials in the treatment of ischemic stroke.
基金the financial support from the National Natural Science Foundation of China (Nos. 22125803, 22020102006 and 22307036)a project supported by the Shanghai Municipal Science and Technology Major Project (No. 2018SHZDZX03)+2 种基金the Program of Shanghai Academic/Technology Research Leader (No. 20XD1421300)China Postdoctoral Science Foundation (No. 2023M731079)the Fundamental Research Funds for the Central Universities
文摘Organic room-temperature phosphorescence(RTP)materials have garnered considerable attention in the fields of biosensing,optoelectronic devices,and anticounterfeiting because of their substantial Stokes shifts,tunable emission wavelengths,and prolonged lifetimes.These materials offer remarkable advantages for biological imaging applications by effectively reducing environmental autofluorescence and enhancing imaging resolution.Recently,host-guest systems have been employed as efficient approaches to fabricate pure-organic RTP materials for bioimaging,providing benefits such as controllable preparation and flexible modulation.Consequently,an increasing number of corresponding studies are being reported;however,a comprehensive systematic review is still lacking.Therefore,we summarize recent advances in the development of pureorganic RTP materials using host-guest systems with regard to bioimaging,including rigid matrices and sensitization.The challenge and potential of RTP for biological imaging are also proposed to promote the biomedical applications of organic RTP materials with excellent optical properties.
基金the National Research Foundation(NRF)of Korea(No.2022R1A2B5B02002097),funded by the Korea government(MSIT).
文摘Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery damage or fracture is a critical concern.Water-based(aqueous)electrolytes have been receiving attention as an alternative to organic electrolytes.However,a narrow electrochemicalstability window,water decomposition,and the consequent low battery operating voltage and energy density hinder the practical use of aqueous electrolytes.Therefore,developing novel aqueous electrolytes for sustainable,safe,high-performance LIBs remains challenging.This Review first commences by summarizing the roles and requirements of electrolytes–separators and then delineates the progression of aqueous electrolytes for LIBs,encompassing aqueous liquid and gel electrolyte development trends along with detailed principles of the electrolytes.These aqueous electrolytes are progressed based on strategies using superconcentrated salts,concentrated diluents,polymer additives,polymer networks,and artificial passivation layers,which are used for suppressing water decomposition and widening the electrochemical stability window of water of the electrolytes.In addition,this Review discusses potential strategies for the implementation of aqueous Li-metal batteries with improved electrolyte–electrode interfaces.A comprehensive understanding of each strategy in the aqueous system will assist in the design of an aqueous electrolyte and the development of sustainable and safe high-performance batteries.
基金supported by the National Natural Science Foundation of China(22068005,22278091)the Training Program for 1000 Backbone Teachers in Guangxi(2022).
文摘The rapid development of the Internet of Things and artificial intelligence technologies has increased the need for wearable,portable,and self-powered flexible sensing devices.Triboelectric nanogenerators(TENGs)based on gel materials(with excellent conductivity,mechanical tunability,environmental adaptability,and biocompatibility)are considered an advanced approach for developing a new generation of flexible sensors.This review comprehensively summarizes the recent advances in gel-based TENGs for flexible sensors,covering their principles,properties,and applications.Based on the development requirements for flexible sensors,the working mechanism of gel-based TENGs and the characteristic advantages of gels are introduced.Design strategies for the performance optimization of hydrogel-,organogel-,and aerogel-based TENGs are systematically summarized.In addition,the applications of gel-based TENGs in human motion sensing,tactile sensing,health monitoring,environmental monitoring,human-machine interaction,and other related fields are summarized.Finally,the challenges of gel-based TENGs for flexible sensing are discussed,and feasible strategies are proposed to guide future research.
基金supported by the National Natural Science Foundation of China(U20A2067,32272360)。
文摘A Pickering emulsion based on sodium starch octenyl succinate(SSOS)was prepared and its effects on the physicochemical properties of hairtail myofibrillar protein gels(MPGs)subjected to multiple freeze-thaw(F-T)cycles were investigated.The whiteness,water-holding capacity,storage modulus(G')and texture properties of the MPGs were significantly improved by adding 1%-2%Pickering emulsion(P<0.05).Meanwhile,Raman spectral analysis demonstrated that Pickering emulsion promoted the transformation of secondary structure,enhanced hydrogen bonds and hydrophobic interactions,and promoted the transition of disulfide bond conformation from g-g-g to g-g-t and t-g-t.At an emulsion concentration of 2%,theα-helix content decreased by 10.37%,while theβ-sheet content increased by 7.94%,compared to the control.After F-T cycles,the structure of the MPGs was destroyed,with an increase in hardness and a decrease in whiteness and water-holding capacity,however,the quality degradation of MPGs was reduced with 1%-2%Pickering emulsion.These findings demonstrated that SSOS-Pickering emulsions,as potential fat substitutes,can enhance the gel properties and the F-T stability of MPGs.