Due to its low cost and natural abundance of sodium,Na-ion batteries(NIBs)are promising candidates for large-scale energy storage systems.The development of ultralow voltage anode materials is of great significance in...Due to its low cost and natural abundance of sodium,Na-ion batteries(NIBs)are promising candidates for large-scale energy storage systems.The development of ultralow voltage anode materials is of great significance in improving the energy density of NIBs.Low-voltage anode materials,however,are severely lacking in NIBs.Of all the reported insertion oxides anodes,the Na_(2)Ti_(3)O_(7) has the lowest operating voltage(an average potential of 0.3 V vs.Na^(+)/Na)and is less likely to deposit sodium,which has excellent potential for achieving NIBs with high energy densities and high safety.Although significant progress has been made,achieving Na_(2)Ti_(3)O_(7) electrodes with excellent performance remains a severe challenge.This paper systematically summarizes and discusses the physicochemical properties and synthesis methods of Na_(2)Ti_(3)O_(7).Then,the sodium storage mechanisms,key issues and challenges,and the optimization strategies for the electrochemical performance of Na_(2)Ti_(3)O_(7) are classified and further elaborated.Finally,remaining challenges and future research directions on the Na_(2)Ti_(3)O_(7) anode are highlighted.This review offers insights into the design of high-energy and high-safety NIBs.展开更多
La_(4)NiLiO_(8)-coated NCM622 samples were prepared through a sol-gel method,and the electrochemical performance as cathode materials was investigated.It is revealed that part of the introduced La^(3+)ions produce a c...La_(4)NiLiO_(8)-coated NCM622 samples were prepared through a sol-gel method,and the electrochemical performance as cathode materials was investigated.It is revealed that part of the introduced La^(3+)ions produce a coating layer on the surface of NCM622 particles,while the rest occupy the 3b position of the lattice.The optimized sample exhibits a capacity retention of 96.54%after 100 cycles under 1C rate with a discharge specific capacity of 117.54 mAh·g^(-1)under 5C rate,much higher than those of the unmodified sample.The results show that the addition of La^(3+)ion can greatly improve the cyclic stability and the rate performance of NCM622.展开更多
Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utiliz...Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.展开更多
By replacing hexyl chains in poly(3-hexylthiophene)(P3HT)with 2-propoxyethyls,four poly(3-(2-propoxyethyl)thiophene)(P3POET)homopolymers with comparable polydispersity indexes(PDI)and regioregularities were prepared h...By replacing hexyl chains in poly(3-hexylthiophene)(P3HT)with 2-propoxyethyls,four poly(3-(2-propoxyethyl)thiophene)(P3POET)homopolymers with comparable polydispersity indexes(PDI)and regioregularities were prepared herein in addition with step increment of about 7 kDa on numberaverage molecular weight(M_(n))from around 11 to 32 kDa(accordingly denoted as P11k,P18k,P25k,and P32k).When doped in film by FeCl_(3)at the optimized conditions,the maximum power factor(PF_(max))increases greatly from 4.3μW·m^(-1)·K^(-2)for P11k to 8.8μW·m^(-1)·K^(-2)for P18k,and further to 9.7μW·m^(-1)·K^(-2)for P25k,followed by a slight decrease to 9.2μW·m^(-1)·K^(-2)for P32k.The close Seebeck coefficients(S)at PF_(max)are observed in these doped polymer films due to their consistent frontier orbital energy levels and Fermi levels.The main contribution to this PF_(max)evolution thus comes from the corresponding conductivities(σ).Theσvariation of the doped films can be rationally correlated with their microstructure evolution.展开更多
A novel strategy was developed to prepare the methacrylic gelatin-dopamine(GelMA-DA)/Ag nanoparticles(NPs)/graphene oxide(GO) composite hydrogels with good biocompatibility,mechanical properties,and antibacterial acti...A novel strategy was developed to prepare the methacrylic gelatin-dopamine(GelMA-DA)/Ag nanoparticles(NPs)/graphene oxide(GO) composite hydrogels with good biocompatibility,mechanical properties,and antibacterial activity.Mussel-inspired DA was utilized to modify the GelMA molecules,which imparts good adhesive performance to the hydrogels.GO,interfacial enhancer,not only improves mechanical properties of the hydrogels,but also provides anchor sites for loading Ag NPs through numerous oxygencontaining functional groups on the surface.The experimental results show that the GelMA/Ag NPs/GO hydrogels have good biocompatibility,and exhibit a swelling rate of 202±16%,the lap shear strength of 147±17 kPa,and compressive modulus of 136±53 kPa,in the case of the Ag NPs/GO content of 2 mg/mL.Antibacterial activity of the hydrogels against both gram-negative and gram-positive bacteria is dependent on the Ag NPs/GO content derived from the release of Ag^(+).Furthermore,the GelMA/Ag NPs/GO hydrogels possess good adhesive ability,which is resistant to highly twisted state when stuck on the surface of pigskin.These results demonstrate promising potential of the GelMA-DA/Ag NPs/GO hydrogels as wound dressings for biomedical applications in clinical and emergent treatment.展开更多
To achieve high microwave permeability in wide-band for the micron-thick magnetic films,[Fe-Fe_(20)Ni_(80)/Cr]_(n) multilayer structure was proposed by co-sputtering Fe and FeNi to form the magnetic layers and Cr to f...To achieve high microwave permeability in wide-band for the micron-thick magnetic films,[Fe-Fe_(20)Ni_(80)/Cr]_(n) multilayer structure was proposed by co-sputtering Fe and FeNi to form the magnetic layers and Cr to form the interlayers.The multilayer structure contributes to the high permeability by reducing the coercivity and diminishing out-of-plane magnetization.The maximum imaginary permeability of[Fe-Fe_(20)Ni_(80)/Cr]_(n) multilayer film reaches a large value of 800 at 0.52 GHz even though its overall thickness exceeds 1μm.Besides,the magnetic resonance frequency of the multilayer film can be modulated from 0.52 to 1.35 GHz by adjusting the sputtering power of Fe from 0 to 86 W,and its bandwidth for μ’’>200(Δf) is as large as 2.0 GHz.The desirable broad Δf of magnetic permeability,which can be well fitted by the Landau-Lifshitz-Gilbert equations,is due to dual magnetic resonances originated from double magnetic phases of Fe and FeNi that are of different saturation magnetization.The micron-thick multilayer films with high permeability in extended waveband are promising candidate for electromagnetic noise suppression application.展开更多
Precisely tuning the spacing of the active centers on the atomic scale is of great significance to improve the catalytic activity and deepen the understanding of the catalytic mechanism,but still remains a challenge.H...Precisely tuning the spacing of the active centers on the atomic scale is of great significance to improve the catalytic activity and deepen the understanding of the catalytic mechanism,but still remains a challenge.Here,we develop a strategy to dilute catalytically active metal interatomic spacing(d_(M-M))with light atoms and discover the unusual adsorption patterns.For example,by elevating the content of boron as interstitial atoms,the atomic spacing of osmium(d_(Os-Os))gradually increases from 2.73 to 2.96?.More importantly,we find that,with the increase in dOs-Os,the hydrogen adsorption-distance relationship is reversed via downshifting d-band states,which breaks the traditional cognition,thereby optimizing the H adsorption and H_2O dissociation on the electrode surface during the catalytic process;this finally leads to a nearly linear increase in hydrogen evolution reaction activity.Namely,the maximum dOs-Os of 2.96?presents the optimal HER activity(8 mV@10 mA cm^(-2))in alkaline media as well as suppressed O adsorption and thus promoted stability.It is believed that this novel atomic-level distance modulation strategy of catalytic sites and the reversed hydrogen adsorption-distance relationship can shew new insights for optimal design of highly efficient catalysts.展开更多
Cathode materials,nickel doped Cr_(8)O_(21),were synthesized by a solid-state method.The effects of Ni doping on the electrochemical performances of Cr_(8)O_(21) were investigated.The experimental results show that th...Cathode materials,nickel doped Cr_(8)O_(21),were synthesized by a solid-state method.The effects of Ni doping on the electrochemical performances of Cr_(8)O_(21) were investigated.The experimental results show that the discharge capacities of the samples depend on the nickel contents,which increases firstly and then decreases with increasing Ni contents.Optimized Ni_(0.5)Cr_(7.5)O_(21)delivers a first capacity up to 392.6 m Ah·g^(-1)at 0.1C.In addition,Ni doped sample also demonstrates enhanced cycling stability and rate capability compared with that of the bare Cr_(8)O_(21).At 1 C,an initial discharge capacity of 348.7 m Ah·g^(-1)was achieved for Ni_(0.5)Cr_(7.5)O_(21),much higher than 271.4 m Ah·g^(-1)of the un-doped sample,with an increase of more than 28%.Electrochemical impedance spectroscopy results confirm that Ni doping reduces the growth of interface resistance and charge transfer resistance,which is conducive to the electrochemical kinetic behaviors during charge-discharge.展开更多
The mechanical properties,contact angle,thermomechanical and electrochemical properties of PE,PVDF,and ceramic separators were compared.The experimental results show that the PE separator has the largest porosity,the ...The mechanical properties,contact angle,thermomechanical and electrochemical properties of PE,PVDF,and ceramic separators were compared.The experimental results show that the PE separator has the largest porosity,the PVDF separator has the best mechanical properties,wettability,and heat resistance.Three kinds of separators were assembled into lithium-ion batteries for electrochemical tests.Among them,the PE separator has the best rate performance,and the ceramic separator has poor performance in charge-discharge cycles.At the same time,the PE and ceramic separators were tested with different amounts of electrolytes at room temperature and a high temperature,and it is found that the capacity of the PE separator is higher at room temperature,while the performance of the ceramic separator is better at a high temperature.The amount of electrolyte also has a certain influence on its electrochemical performance.展开更多
Catalysts consisting of Zeolite imidazolyl ester skeleton-67(ZIF-67)and graphene oxide(GO)were fabricated through a solvothermal method,followed by etching ZIF-67 with oxygen-rich functional groups on GO in a reductio...Catalysts consisting of Zeolite imidazolyl ester skeleton-67(ZIF-67)and graphene oxide(GO)were fabricated through a solvothermal method,followed by etching ZIF-67 with oxygen-rich functional groups on GO in a reduction atmosphere at 400℃.During this process,an open type of cobalt metal center was formed by the partial vaporization and oxidation of ZIF-67,further reducing to Co and partially combining with oxygen species to amorphous CoOx.Benefiting from the rich functional N,and metal/oxides active centers derived from the calcination process,the synthesized Co/CoOx@NSG-400 showed a low OER overpotential of 10 mA·cm^(-2) at 298 mV,and an ORR half-wave potential of 0.8 V,which demonstrated its excellent bifunctional catalytic activity.Such a controllable calcination strategy with high yields could be expected to pave the way for synthesizing low-cost and efficient bifunctional electrocatalysts.展开更多
The electrochemical performance of lithium-ion batteries,i.e.specific capacity and cyclability,is primarily determined by chemical reversibility and structural stability of the electrodes in cycling.Here we have inves...The electrochemical performance of lithium-ion batteries,i.e.specific capacity and cyclability,is primarily determined by chemical reversibility and structural stability of the electrodes in cycling.Here we have investigated the fundamental reaction behaviors of nickel sulfide(NixSy)as lithium-ion battery anodes by in-situ TEM.We find that Ni_(3)S_(2)is the electrochemically stable phase,which appears in the first cycle of the NixSyanode.From the second cycle,conversion between Ni_(3)S_(2)and Li_(2)S/Ni is the dominant electrochemical reaction.In lithiation,the NixSynanoparticles evolve into a mixture of Ni nanocrystals embedded in Li_(2)S matrix,which form a porous structure upon full lithiation,and with the recrystallization of the Ni_(3)S_(2)phase in delithiation,a compact and interconnected network is built.Structural stability in cycles is susceptible to particle size and substrate restraint.Carbon substrate can certainly improve the tolerance for size-dependent pulverization of NixSynanoparticles.When NixSynanoparticle exceeds the critical size value,the morphology of the particle is no longer well maintained even under the constraints of the carbon substrate.This work deepens the understanding of electrochemical reaction behavior of conversiontype materials and helps to rational design of high-energy density battery anodes.展开更多
Nitrogen-doped carbon-coated transition-metal sulfides(TMS@NCs)have been considered as efficient anodes for sodium-ion batteries.However,the uncontrollable morphology and weak core-shell binding forces significantly l...Nitrogen-doped carbon-coated transition-metal sulfides(TMS@NCs)have been considered as efficient anodes for sodium-ion batteries.However,the uncontrollable morphology and weak core-shell binding forces significantly limit the sodium storage performance and life.Herein,based on the reversible ring-opening reaction of the epoxy group of the tertiary amino group-rich epoxide cationic polyacrylamide(ECP)at the beginning of hydrothermal process(acidic environment)and the irreversible ring-opening(cross-linking reactions)at the late hydrothermal period(alkaline environment),47 nm-sized ZnS@NCs were prepared via a one-pot hydrothermal process.During this process,the covalent bonds formed between the ZnS core and elastic carbon shell significantly improved the mechanical and chemical stabilities of ZnS@NC.Benefiting from the nanosize,fast ion/electron transfer,and high stability,ZnS@NC exhibited a high reversible capacity of 421.9 mAh g^(−1) at a current density of 0.1 A g^(−1) after 1000 cycles and a superior rate capability of 273.8 mAh g^(−1) at a current density of 5 A g^(−1).Moreover,via this universal synthesis strategy,a series of TMS@NCs,such as MoS_(2)@NC,NiS@NC,and CuS@NC were developed with excellent capacity and cyclability.展开更多
Here, a new idea was proposed for template-free synthesis of hierarchical m-ZrO_2 nanorods and "their" possible formation mechanism based on a series of chemical reactions by simple hydrothermal method. The ...Here, a new idea was proposed for template-free synthesis of hierarchical m-ZrO_2 nanorods and "their" possible formation mechanism based on a series of chemical reactions by simple hydrothermal method. The traditional preparation methods of hierarchical ZrO_2 nanorods involved inexpensive equipment, complicated process, and high production cost. The as-synthesized products composed of many nanorods with 180-200 nm in diameter and 5-7 μm in length. The fi nal product after annealing involved hierarchical monoclinic ZrO_2(m-ZrO_2) nanorods, namely, the big nanorod was made up of many small nanorods with 40-50 nm in diameter and 500-600 nm in length. The experimental results were useful in understanding the chemical properties of ZrB_2 and ZrO_2 and the design of the derivatives for m-ZrO_2 nanomaterials.展开更多
A series of bulk polycrystalline La 1-xLixMnO3 samples with x ranging from 0.1 to 0.5 was prepared by sol-gel method. X-ray diffraction patterns show that the crystal structures are single rhombohedral perovskite for ...A series of bulk polycrystalline La 1-xLixMnO3 samples with x ranging from 0.1 to 0.5 was prepared by sol-gel method. X-ray diffraction patterns show that the crystal structures are single rhombohedral perovskite for the x≤0.3 sample and the impurity appears when x>0.3. Under the same synthesized conditions, the higher Li content samples display a higher content of liquid phase content and larger mean grain sizes, which leads to the increases of the effect of the grain boundaries. The experimental results show that the change of the ferromagnetic transition temperature and the resistivity can attribute to the effect of the grain boundary and the connectivity of the inter grains as well as the ratio of Mn 3+ to Mn 4+.展开更多
Micro/nanorobots can propel and navigate in many hard-to-reach biological environments,and thus may bring revolutionary changes to biomedical research and applications.However,current MNRs lack the capability to colle...Micro/nanorobots can propel and navigate in many hard-to-reach biological environments,and thus may bring revolutionary changes to biomedical research and applications.However,current MNRs lack the capability to collectively perceive and report physicochemical changes in unknown microenvironments.Here we propose to develop swarming responsive photonic nanorobots that can map local physicochemical conditions on the fly and further guide localized photothermal treatment.The RPNRs consist of a photonic nanochain of periodically-assembled magnetic Fe_(3)O_(4)nanoparticles encapsulated in a responsive hydrogel shell,and show multiple integrated functions,including energetic magnetically-driven swarming motions,bright stimuli-responsive structural colors,and photothermal conversion.Thus,they can actively navigate in complex environments utilizing their controllable swarming motions,then visualize unknown targets(e.g.,tumor lesion)by collectively mapping out local abnormal physicochemical conditions(e.g.,pH,temperature,or glucose concentra-tion)via their responsive structural colors,and further guide external light irradiation to initiate localized photothermal treatment.This work facilitates the development of intelligent motile nanosensors and versatile multifunctional nanotheranostics for cancer and inflam-matory diseases.展开更多
Ethylene carbonate(EC)is susceptible to the aggressive chemistry of nickel-rich cathodes,making it undesirable for high-voltage lithium-ion batteries(LIBs).The arbitrary elimination of EC leads to better oxidative tol...Ethylene carbonate(EC)is susceptible to the aggressive chemistry of nickel-rich cathodes,making it undesirable for high-voltage lithium-ion batteries(LIBs).The arbitrary elimination of EC leads to better oxidative tolerance but always incurs interfacial degradation and electrolyte decomposition.Herein,an EC-free electrolyte is deliberately developed based on gradient solvation by pairing solvation-protection agent(1,3,5-trifluorobenzene,F_(3)B)with propylene carbonate(PC)/methyl ethyl carbonate(EMC)formulation.F_(3)B keeps out of inner coordination shell but decomposes preferentially to construct robust interphase,inhibiting solvent decomposition and electrode corrosion.Thereby,the optimized electrolyte(1.1 M)with wide liquid range(-70–77℃)conveys decent interfacial compatibility and high-voltage stability(4.6 V for LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2),NCM622),qualifying reliable operation of practical NCM/graphite pouch cell(81.1%capacity retention over 600 cycles at 0.5 C).The solvation preservation and interface protection from F_(3)B blaze a new avenue for developing high-voltage electrolytes in next-generation LIBs.展开更多
Although advanced anode materials for the lithium-ion battery have been investigated for decades,a reliable,high-capacity,and durable material that can enable a fast charge remains elusive.Herein,we report that a meta...Although advanced anode materials for the lithium-ion battery have been investigated for decades,a reliable,high-capacity,and durable material that can enable a fast charge remains elusive.Herein,we report that a metal phosphorous trichalcogenide of MnPS_(3)(manganese phosphorus trisulfide),endowed with a unique and layered van der Waals structure,is highly beneficial for the fast insertion/extraction of alkali metal ions and can facilitate changes in the buffer volume during cycles with robust structural stability.The few-layered MnPS_(3)anodes displayed the desirable specific capacity and excellent rate chargeability owing to their good electronic and ionic conductivities.When assembled as a half-cell lithium-ion battery,a high reversible capacity of 380 mA h g^(−1)was maintained by the MnPS_(3)after 3000 cycles at a high current density of 4 A g^(−1),with a capacity retention of close to or above 100%.In full-cell testing,a reversible capacity of 450 mA h g^(−1)after 200 cycles was maintained as well.The results of in-situ TEM revealed that MnPS_(3)nanoflakes maintained a high structural integrity without exhibiting any pulverization after undergoing large volumetric expansion for the insertion of a large number of lithium ions.Their kinetics of lithium-ion diffusion,stable structure,and high pseudocapacitance contributed to their comprehensive performance,for example,a high specific capacity,rapid charge-discharge,and long cyclability.MnPS_(3)is thus an efficient anode for the next generation of batteries with a fast charge/discharge capability.展开更多
N-type Si-based typeⅠ clathrates with different Ga content were synthesized by combining the solid-state reaction method,melting method and spark plasma sintering(SPS) method.The effects of Ga composition on high tem...N-type Si-based typeⅠ clathrates with different Ga content were synthesized by combining the solid-state reaction method,melting method and spark plasma sintering(SPS) method.The effects of Ga composition on high temperature thermoelectric transport properties were investigated.The results show that at room temperature,the carrier concentration decreases,while the carrier mobility increases slightly with increasing Ga content.The Seebeck coefficient increases with increasing Ga content.Among all the samples,Ba7.93Ga17.13Si28.72 exhibits higher Seebeck coefficient than the others and reaches 135 μV·K-1 at 1000 K.The sample prepared by this method exhibits very high electrical conductivity,and reaches 1.95×105 S·m-1 for Ba8.01Ga16.61Si28.93 at room temperature.The thermal conductivity of all samples is almost temperature independent in the temperature range of 300-1000 K,indicating the behaviour of a typical metal.The maximum ZT value of 0.75 is obtained at 1000 K for the compound Ba7.93Ga17.13Si28.72.展开更多
The Si_(3)N_(4)/SiC gradient material with a gradient composition structure was prepared by a hot pressing sintering.The sinterability,distribution of residual stress and the effect of residual stress on mechanical pr...The Si_(3)N_(4)/SiC gradient material with a gradient composition structure was prepared by a hot pressing sintering.The sinterability,distribution of residual stress and the effect of residual stress on mechanical properties of Si_(3)N_(4)/SiC gradient materials were studied.The research results show that,at 1750℃,Si_(3)N_(4)/SiC gradient materials with different ratios can achieve co-sintering,and the overall relative density of the sample reaches 98.5%.Interestingly,the flexural strength of Si_(3)N_(4)/SiC gradient material is related to its loading surface.The flexural strength of SiC as the loading surface is about 35%higher than that of Si_(3)N_(4)as the loading surface.The analysis of the residual stress of the material in the gradient structure shows that the gradient stress distribution between the two phases is a vital factor affecting the mechanical properties of the material.With the increase of SiC content in the gradient direction,the fracture toughness of each layer of Si_(3)N_(4)/SiC gradient materials gradually decreases.The surface hardness of the pure SiC side is lower than that reported in other literature.展开更多
To explore ways to improve the accuracy of quantitative analysis of samples in the micrometer to nanometer range of magnitudes,we adopted analytical transmission electron microscopy(AEM/EDS)for qualitative and quantit...To explore ways to improve the accuracy of quantitative analysis of samples in the micrometer to nanometer range of magnitudes,we adopted analytical transmission electron microscopy(AEM/EDS)for qualitative and quantitative analysis of pyrite materials.Additionally,the k factor of pyrite is calculated experimentally.To develop an appropriate non-standard quantitative analysis model for pyrite materials,the experimentally calculated k factor is compared with that estimated from the non-standard quantitative analytical model of the instrument software.The experimental findings demonstrate that the EDS attached to a TEM can be employed for precise quantitative analysis of micro-and nanoscale regions of pyrite materials.Furthermore,it serves as a reference for improving the results of the EDS quantitative analysis of other sulfides.展开更多
基金supported by the National Natural Science Foundation of China (52307239,52102300,52207234)the Natural Science Foundation of Hubei Province (2022CFB1003,2021CFA025)。
文摘Due to its low cost and natural abundance of sodium,Na-ion batteries(NIBs)are promising candidates for large-scale energy storage systems.The development of ultralow voltage anode materials is of great significance in improving the energy density of NIBs.Low-voltage anode materials,however,are severely lacking in NIBs.Of all the reported insertion oxides anodes,the Na_(2)Ti_(3)O_(7) has the lowest operating voltage(an average potential of 0.3 V vs.Na^(+)/Na)and is less likely to deposit sodium,which has excellent potential for achieving NIBs with high energy densities and high safety.Although significant progress has been made,achieving Na_(2)Ti_(3)O_(7) electrodes with excellent performance remains a severe challenge.This paper systematically summarizes and discusses the physicochemical properties and synthesis methods of Na_(2)Ti_(3)O_(7).Then,the sodium storage mechanisms,key issues and challenges,and the optimization strategies for the electrochemical performance of Na_(2)Ti_(3)O_(7) are classified and further elaborated.Finally,remaining challenges and future research directions on the Na_(2)Ti_(3)O_(7) anode are highlighted.This review offers insights into the design of high-energy and high-safety NIBs.
基金Funded by the Guangdong Key R&D Program(Nos.2020B 0909040001 and 2019B090909003)。
文摘La_(4)NiLiO_(8)-coated NCM622 samples were prepared through a sol-gel method,and the electrochemical performance as cathode materials was investigated.It is revealed that part of the introduced La^(3+)ions produce a coating layer on the surface of NCM622 particles,while the rest occupy the 3b position of the lattice.The optimized sample exhibits a capacity retention of 96.54%after 100 cycles under 1C rate with a discharge specific capacity of 117.54 mAh·g^(-1)under 5C rate,much higher than those of the unmodified sample.The results show that the addition of La^(3+)ion can greatly improve the cyclic stability and the rate performance of NCM622.
基金supported by the National Natural Science Foundation of China(22234005,21974070)the Natural Science Foundation of Jiangsu Province(BK20222015)。
文摘Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.
基金Funded by the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan Univesity of Technology。
文摘By replacing hexyl chains in poly(3-hexylthiophene)(P3HT)with 2-propoxyethyls,four poly(3-(2-propoxyethyl)thiophene)(P3POET)homopolymers with comparable polydispersity indexes(PDI)and regioregularities were prepared herein in addition with step increment of about 7 kDa on numberaverage molecular weight(M_(n))from around 11 to 32 kDa(accordingly denoted as P11k,P18k,P25k,and P32k).When doped in film by FeCl_(3)at the optimized conditions,the maximum power factor(PF_(max))increases greatly from 4.3μW·m^(-1)·K^(-2)for P11k to 8.8μW·m^(-1)·K^(-2)for P18k,and further to 9.7μW·m^(-1)·K^(-2)for P25k,followed by a slight decrease to 9.2μW·m^(-1)·K^(-2)for P32k.The close Seebeck coefficients(S)at PF_(max)are observed in these doped polymer films due to their consistent frontier orbital energy levels and Fermi levels.The main contribution to this PF_(max)evolution thus comes from the corresponding conductivities(σ).Theσvariation of the doped films can be rationally correlated with their microstructure evolution.
基金Funded by the National Key Research and Development(R&D) Program of China(No.2018YFB1105702)。
文摘A novel strategy was developed to prepare the methacrylic gelatin-dopamine(GelMA-DA)/Ag nanoparticles(NPs)/graphene oxide(GO) composite hydrogels with good biocompatibility,mechanical properties,and antibacterial activity.Mussel-inspired DA was utilized to modify the GelMA molecules,which imparts good adhesive performance to the hydrogels.GO,interfacial enhancer,not only improves mechanical properties of the hydrogels,but also provides anchor sites for loading Ag NPs through numerous oxygencontaining functional groups on the surface.The experimental results show that the GelMA/Ag NPs/GO hydrogels have good biocompatibility,and exhibit a swelling rate of 202±16%,the lap shear strength of 147±17 kPa,and compressive modulus of 136±53 kPa,in the case of the Ag NPs/GO content of 2 mg/mL.Antibacterial activity of the hydrogels against both gram-negative and gram-positive bacteria is dependent on the Ag NPs/GO content derived from the release of Ag^(+).Furthermore,the GelMA/Ag NPs/GO hydrogels possess good adhesive ability,which is resistant to highly twisted state when stuck on the surface of pigskin.These results demonstrate promising potential of the GelMA-DA/Ag NPs/GO hydrogels as wound dressings for biomedical applications in clinical and emergent treatment.
基金Funded by the Young Top-notch Talent Cultivation Program of Hubei Provincethe Fundamental Research Funds for the Central Universities(WUT:2021IVA116 and WUT:2021CG015)。
文摘To achieve high microwave permeability in wide-band for the micron-thick magnetic films,[Fe-Fe_(20)Ni_(80)/Cr]_(n) multilayer structure was proposed by co-sputtering Fe and FeNi to form the magnetic layers and Cr to form the interlayers.The multilayer structure contributes to the high permeability by reducing the coercivity and diminishing out-of-plane magnetization.The maximum imaginary permeability of[Fe-Fe_(20)Ni_(80)/Cr]_(n) multilayer film reaches a large value of 800 at 0.52 GHz even though its overall thickness exceeds 1μm.Besides,the magnetic resonance frequency of the multilayer film can be modulated from 0.52 to 1.35 GHz by adjusting the sputtering power of Fe from 0 to 86 W,and its bandwidth for μ’’>200(Δf) is as large as 2.0 GHz.The desirable broad Δf of magnetic permeability,which can be well fitted by the Landau-Lifshitz-Gilbert equations,is due to dual magnetic resonances originated from double magnetic phases of Fe and FeNi that are of different saturation magnetization.The micron-thick multilayer films with high permeability in extended waveband are promising candidate for electromagnetic noise suppression application.
基金financially sponsored by the National Natural Science Foundation of China(Grant Nos.22075223,22179104)the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology)(2022-ZD-4)。
文摘Precisely tuning the spacing of the active centers on the atomic scale is of great significance to improve the catalytic activity and deepen the understanding of the catalytic mechanism,but still remains a challenge.Here,we develop a strategy to dilute catalytically active metal interatomic spacing(d_(M-M))with light atoms and discover the unusual adsorption patterns.For example,by elevating the content of boron as interstitial atoms,the atomic spacing of osmium(d_(Os-Os))gradually increases from 2.73 to 2.96?.More importantly,we find that,with the increase in dOs-Os,the hydrogen adsorption-distance relationship is reversed via downshifting d-band states,which breaks the traditional cognition,thereby optimizing the H adsorption and H_2O dissociation on the electrode surface during the catalytic process;this finally leads to a nearly linear increase in hydrogen evolution reaction activity.Namely,the maximum dOs-Os of 2.96?presents the optimal HER activity(8 mV@10 mA cm^(-2))in alkaline media as well as suppressed O adsorption and thus promoted stability.It is believed that this novel atomic-level distance modulation strategy of catalytic sites and the reversed hydrogen adsorption-distance relationship can shew new insights for optimal design of highly efficient catalysts.
基金National Natural Science Foundation of China(No.51790490)。
文摘Cathode materials,nickel doped Cr_(8)O_(21),were synthesized by a solid-state method.The effects of Ni doping on the electrochemical performances of Cr_(8)O_(21) were investigated.The experimental results show that the discharge capacities of the samples depend on the nickel contents,which increases firstly and then decreases with increasing Ni contents.Optimized Ni_(0.5)Cr_(7.5)O_(21)delivers a first capacity up to 392.6 m Ah·g^(-1)at 0.1C.In addition,Ni doped sample also demonstrates enhanced cycling stability and rate capability compared with that of the bare Cr_(8)O_(21).At 1 C,an initial discharge capacity of 348.7 m Ah·g^(-1)was achieved for Ni_(0.5)Cr_(7.5)O_(21),much higher than 271.4 m Ah·g^(-1)of the un-doped sample,with an increase of more than 28%.Electrochemical impedance spectroscopy results confirm that Ni doping reduces the growth of interface resistance and charge transfer resistance,which is conducive to the electrochemical kinetic behaviors during charge-discharge.
基金National Natural Science Foundation of China(No.51976143)。
文摘The mechanical properties,contact angle,thermomechanical and electrochemical properties of PE,PVDF,and ceramic separators were compared.The experimental results show that the PE separator has the largest porosity,the PVDF separator has the best mechanical properties,wettability,and heat resistance.Three kinds of separators were assembled into lithium-ion batteries for electrochemical tests.Among them,the PE separator has the best rate performance,and the ceramic separator has poor performance in charge-discharge cycles.At the same time,the PE and ceramic separators were tested with different amounts of electrolytes at room temperature and a high temperature,and it is found that the capacity of the PE separator is higher at room temperature,while the performance of the ceramic separator is better at a high temperature.The amount of electrolyte also has a certain influence on its electrochemical performance.
基金Funded in part by the National Natural Science Foundation of China(No.22279096)the Guangdong Basic and Applied Basic Research Foundation(No.2021B1515120072)the Guangdong Key R&D Program(No.2020B0909040001)。
文摘Catalysts consisting of Zeolite imidazolyl ester skeleton-67(ZIF-67)and graphene oxide(GO)were fabricated through a solvothermal method,followed by etching ZIF-67 with oxygen-rich functional groups on GO in a reduction atmosphere at 400℃.During this process,an open type of cobalt metal center was formed by the partial vaporization and oxidation of ZIF-67,further reducing to Co and partially combining with oxygen species to amorphous CoOx.Benefiting from the rich functional N,and metal/oxides active centers derived from the calcination process,the synthesized Co/CoOx@NSG-400 showed a low OER overpotential of 10 mA·cm^(-2) at 298 mV,and an ORR half-wave potential of 0.8 V,which demonstrated its excellent bifunctional catalytic activity.Such a controllable calcination strategy with high yields could be expected to pave the way for synthesizing low-cost and efficient bifunctional electrocatalysts.
基金the support by the National Natural Science Foundation of China(11972219 and 11902185)the support of Shanghai Sailing Program(19YF1415100)+2 种基金the Young Elite Scientist Sponsorship Program by CAST(2019QNRC001)the support of the National Natural Science Foundation of China(52090022)the Natural Science Foundation for Distinguished Young Scholars of Hebei Province(E2020203085)。
文摘The electrochemical performance of lithium-ion batteries,i.e.specific capacity and cyclability,is primarily determined by chemical reversibility and structural stability of the electrodes in cycling.Here we have investigated the fundamental reaction behaviors of nickel sulfide(NixSy)as lithium-ion battery anodes by in-situ TEM.We find that Ni_(3)S_(2)is the electrochemically stable phase,which appears in the first cycle of the NixSyanode.From the second cycle,conversion between Ni_(3)S_(2)and Li_(2)S/Ni is the dominant electrochemical reaction.In lithiation,the NixSynanoparticles evolve into a mixture of Ni nanocrystals embedded in Li_(2)S matrix,which form a porous structure upon full lithiation,and with the recrystallization of the Ni_(3)S_(2)phase in delithiation,a compact and interconnected network is built.Structural stability in cycles is susceptible to particle size and substrate restraint.Carbon substrate can certainly improve the tolerance for size-dependent pulverization of NixSynanoparticles.When NixSynanoparticle exceeds the critical size value,the morphology of the particle is no longer well maintained even under the constraints of the carbon substrate.This work deepens the understanding of electrochemical reaction behavior of conversiontype materials and helps to rational design of high-energy density battery anodes.
基金supported by research grants from the National Research Foundation of Korea(Nos.2020R1I1A1A01072996,2021K2A9A2A06044652,and 2019H1D3A1A01069779)KIST Institutional Program(2E331863)funded by the government of the Republic of Korea.
文摘Nitrogen-doped carbon-coated transition-metal sulfides(TMS@NCs)have been considered as efficient anodes for sodium-ion batteries.However,the uncontrollable morphology and weak core-shell binding forces significantly limit the sodium storage performance and life.Herein,based on the reversible ring-opening reaction of the epoxy group of the tertiary amino group-rich epoxide cationic polyacrylamide(ECP)at the beginning of hydrothermal process(acidic environment)and the irreversible ring-opening(cross-linking reactions)at the late hydrothermal period(alkaline environment),47 nm-sized ZnS@NCs were prepared via a one-pot hydrothermal process.During this process,the covalent bonds formed between the ZnS core and elastic carbon shell significantly improved the mechanical and chemical stabilities of ZnS@NC.Benefiting from the nanosize,fast ion/electron transfer,and high stability,ZnS@NC exhibited a high reversible capacity of 421.9 mAh g^(−1) at a current density of 0.1 A g^(−1) after 1000 cycles and a superior rate capability of 273.8 mAh g^(−1) at a current density of 5 A g^(−1).Moreover,via this universal synthesis strategy,a series of TMS@NCs,such as MoS_(2)@NC,NiS@NC,and CuS@NC were developed with excellent capacity and cyclability.
基金Funded by the Ministry of Science and Technology of China(S2010GR0771)the National Natural Science Foundation of China(51161140399)
文摘Here, a new idea was proposed for template-free synthesis of hierarchical m-ZrO_2 nanorods and "their" possible formation mechanism based on a series of chemical reactions by simple hydrothermal method. The traditional preparation methods of hierarchical ZrO_2 nanorods involved inexpensive equipment, complicated process, and high production cost. The as-synthesized products composed of many nanorods with 180-200 nm in diameter and 5-7 μm in length. The fi nal product after annealing involved hierarchical monoclinic ZrO_2(m-ZrO_2) nanorods, namely, the big nanorod was made up of many small nanorods with 40-50 nm in diameter and 500-600 nm in length. The experimental results were useful in understanding the chemical properties of ZrB_2 and ZrO_2 and the design of the derivatives for m-ZrO_2 nanomaterials.
文摘A series of bulk polycrystalline La 1-xLixMnO3 samples with x ranging from 0.1 to 0.5 was prepared by sol-gel method. X-ray diffraction patterns show that the crystal structures are single rhombohedral perovskite for the x≤0.3 sample and the impurity appears when x>0.3. Under the same synthesized conditions, the higher Li content samples display a higher content of liquid phase content and larger mean grain sizes, which leads to the increases of the effect of the grain boundaries. The experimental results show that the change of the ferromagnetic transition temperature and the resistivity can attribute to the effect of the grain boundary and the connectivity of the inter grains as well as the ratio of Mn 3+ to Mn 4+.
基金supported by the National Key Research and Development Project(No.2021YFA1201400)National Natural Science Foundation of China(Nos.52073222,51573144 and 21474078)the Fundamental Research Funds for the Central Universities(WUT:2021IVA118 and 2022IVA201).
文摘Micro/nanorobots can propel and navigate in many hard-to-reach biological environments,and thus may bring revolutionary changes to biomedical research and applications.However,current MNRs lack the capability to collectively perceive and report physicochemical changes in unknown microenvironments.Here we propose to develop swarming responsive photonic nanorobots that can map local physicochemical conditions on the fly and further guide localized photothermal treatment.The RPNRs consist of a photonic nanochain of periodically-assembled magnetic Fe_(3)O_(4)nanoparticles encapsulated in a responsive hydrogel shell,and show multiple integrated functions,including energetic magnetically-driven swarming motions,bright stimuli-responsive structural colors,and photothermal conversion.Thus,they can actively navigate in complex environments utilizing their controllable swarming motions,then visualize unknown targets(e.g.,tumor lesion)by collectively mapping out local abnormal physicochemical conditions(e.g.,pH,temperature,or glucose concentra-tion)via their responsive structural colors,and further guide external light irradiation to initiate localized photothermal treatment.This work facilitates the development of intelligent motile nanosensors and versatile multifunctional nanotheranostics for cancer and inflam-matory diseases.
基金supported by the National Key Research and Development Program of China(No.2022YFB2404800)。
文摘Ethylene carbonate(EC)is susceptible to the aggressive chemistry of nickel-rich cathodes,making it undesirable for high-voltage lithium-ion batteries(LIBs).The arbitrary elimination of EC leads to better oxidative tolerance but always incurs interfacial degradation and electrolyte decomposition.Herein,an EC-free electrolyte is deliberately developed based on gradient solvation by pairing solvation-protection agent(1,3,5-trifluorobenzene,F_(3)B)with propylene carbonate(PC)/methyl ethyl carbonate(EMC)formulation.F_(3)B keeps out of inner coordination shell but decomposes preferentially to construct robust interphase,inhibiting solvent decomposition and electrode corrosion.Thereby,the optimized electrolyte(1.1 M)with wide liquid range(-70–77℃)conveys decent interfacial compatibility and high-voltage stability(4.6 V for LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2),NCM622),qualifying reliable operation of practical NCM/graphite pouch cell(81.1%capacity retention over 600 cycles at 0.5 C).The solvation preservation and interface protection from F_(3)B blaze a new avenue for developing high-voltage electrolytes in next-generation LIBs.
基金National Natural Science Foundation of China,Grant/Award Numbers:11902185,11972219,U21A2086National Key Research and Development Program of China,Grant/Award Number:2020YFB0704503+1 种基金Young Elite Scientist Sponsorship Program by CAST,Grant/Award Number:2019QNRC001Shanghai Sailing Program,Grant/Award Number:19YF1415100。
文摘Although advanced anode materials for the lithium-ion battery have been investigated for decades,a reliable,high-capacity,and durable material that can enable a fast charge remains elusive.Herein,we report that a metal phosphorous trichalcogenide of MnPS_(3)(manganese phosphorus trisulfide),endowed with a unique and layered van der Waals structure,is highly beneficial for the fast insertion/extraction of alkali metal ions and can facilitate changes in the buffer volume during cycles with robust structural stability.The few-layered MnPS_(3)anodes displayed the desirable specific capacity and excellent rate chargeability owing to their good electronic and ionic conductivities.When assembled as a half-cell lithium-ion battery,a high reversible capacity of 380 mA h g^(−1)was maintained by the MnPS_(3)after 3000 cycles at a high current density of 4 A g^(−1),with a capacity retention of close to or above 100%.In full-cell testing,a reversible capacity of 450 mA h g^(−1)after 200 cycles was maintained as well.The results of in-situ TEM revealed that MnPS_(3)nanoflakes maintained a high structural integrity without exhibiting any pulverization after undergoing large volumetric expansion for the insertion of a large number of lithium ions.Their kinetics of lithium-ion diffusion,stable structure,and high pseudocapacitance contributed to their comprehensive performance,for example,a high specific capacity,rapid charge-discharge,and long cyclability.MnPS_(3)is thus an efficient anode for the next generation of batteries with a fast charge/discharge capability.
基金Project supported by the National Basic Research Program of China (Grant Nos 2007CB607501 and 2007CB607503)Yunnan Natural Science Fund (Grant No 2008CD114)
文摘N-type Si-based typeⅠ clathrates with different Ga content were synthesized by combining the solid-state reaction method,melting method and spark plasma sintering(SPS) method.The effects of Ga composition on high temperature thermoelectric transport properties were investigated.The results show that at room temperature,the carrier concentration decreases,while the carrier mobility increases slightly with increasing Ga content.The Seebeck coefficient increases with increasing Ga content.Among all the samples,Ba7.93Ga17.13Si28.72 exhibits higher Seebeck coefficient than the others and reaches 135 μV·K-1 at 1000 K.The sample prepared by this method exhibits very high electrical conductivity,and reaches 1.95×105 S·m-1 for Ba8.01Ga16.61Si28.93 at room temperature.The thermal conductivity of all samples is almost temperature independent in the temperature range of 300-1000 K,indicating the behaviour of a typical metal.The maximum ZT value of 0.75 is obtained at 1000 K for the compound Ba7.93Ga17.13Si28.72.
基金Funded by the National Natural Science Foundation of China(Nos.43190311,43200301 and 631800611)。
文摘The Si_(3)N_(4)/SiC gradient material with a gradient composition structure was prepared by a hot pressing sintering.The sinterability,distribution of residual stress and the effect of residual stress on mechanical properties of Si_(3)N_(4)/SiC gradient materials were studied.The research results show that,at 1750℃,Si_(3)N_(4)/SiC gradient materials with different ratios can achieve co-sintering,and the overall relative density of the sample reaches 98.5%.Interestingly,the flexural strength of Si_(3)N_(4)/SiC gradient material is related to its loading surface.The flexural strength of SiC as the loading surface is about 35%higher than that of Si_(3)N_(4)as the loading surface.The analysis of the residual stress of the material in the gradient structure shows that the gradient stress distribution between the two phases is a vital factor affecting the mechanical properties of the material.With the increase of SiC content in the gradient direction,the fracture toughness of each layer of Si_(3)N_(4)/SiC gradient materials gradually decreases.The surface hardness of the pure SiC side is lower than that reported in other literature.
基金Funded by the International Science&Technology Cooperation Program of Hubei Province of China(No.2022EHB024)。
文摘To explore ways to improve the accuracy of quantitative analysis of samples in the micrometer to nanometer range of magnitudes,we adopted analytical transmission electron microscopy(AEM/EDS)for qualitative and quantitative analysis of pyrite materials.Additionally,the k factor of pyrite is calculated experimentally.To develop an appropriate non-standard quantitative analysis model for pyrite materials,the experimentally calculated k factor is compared with that estimated from the non-standard quantitative analytical model of the instrument software.The experimental findings demonstrate that the EDS attached to a TEM can be employed for precise quantitative analysis of micro-and nanoscale regions of pyrite materials.Furthermore,it serves as a reference for improving the results of the EDS quantitative analysis of other sulfides.
