Aqueous zinc-ion batteries(AZIBs)offer a safe,cost-effective,and high-capacity energy storage solution,yet their performance is hindered by interfacial challenges at the Zn anode,including hydrogen evolution,corrosion...Aqueous zinc-ion batteries(AZIBs)offer a safe,cost-effective,and high-capacity energy storage solution,yet their performance is hindered by interfacial challenges at the Zn anode,including hydrogen evolution,corrosion,and dendritic Zn growth.While most studies focus on regulating Zn~(2+)solvation structures in bulk electrolytes,the evolution of interfacial solvation—where Zn~(2+)undergoes desolvation and deposition—remains insufficiently explored.Here,we introduce sulfated nanocellulose(SNC),an anion-rich biopolymer,to tailor the interfacial solvation structure without altering the bulk electrolyte composition.Using in situ attenuated total reflection Fourier transform infrared spectroscopy and fluorescence interface-extended X-ray absorption fine structure,we reveal that SNC facilitates the formation of a low-coordinated Zn~(2+)solvation shell at the interface by weakening H_(2)O coordination.This transformation is driven by electrostatic interactions between Zn~(2+)and anchored sulfate groups,thereby reducing water activity,improving interfacial stability during charge/discharge,and suppressing parasitic reactions.Consequently,a high average coulombic efficiency of 99.6%over 500 cycles in Zn|Ti asymmetric cells and 1.5 Ah pouch cells(13.4 mg cm^(-2)loading,remained stable over 250 cycles)were achieved in SNC-induced AZIBs.This work underscores the importance of interfacial solvation structure engineering—beyond traditional bulk electrolyte design—in enabling practical,high-performance AZIBs.展开更多
Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and hi...Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and high mechanical properties.Inspired by Chinese ramen,we propose a universal fabricating method(printing-P,training-T,cross-linking-C,PTC&PCT)for tough hydrogel scaffolds to fill this gap.First,3D printing fabricates a hydrogel scaffold with desired structures(P).Then,the scaffold could have extraordinarily high mechanical properties and functional surface structure by cycle mechanical training with salting-out assistance(T).Finally,the training results are fixed by photo-cross-linking processing(C).The tough gelatin hydrogel scaffolds exhibit excellent tensile strength of 6.66 MPa(622-fold untreated)and have excellent biocompatibility.Furthermore,this scaffold possesses functional surface structures from nanometer to micron to millimeter,which can efficiently induce directional cell growth.Interestingly,this strategy can produce bionic human tissue with mechanical properties of 10 kPa-10 MPa by changing the type of salt,and many hydrogels,such as gelatin and silk,could be improved with PTC or PCT strategies.Animal experiments show that this scaffold can effectively promote the new generation of muscle fibers,blood vessels,and nerves within 4 weeks,prompting the rapid regeneration of large-volume muscle loss injuries.展开更多
Changes to the microstructure of a hard carbon(HC)and its solid electrolyte interface(SEI)can be effective in improving the electrode kinetics.However,achieving fast charging using a simple and inexpensive strategy wi...Changes to the microstructure of a hard carbon(HC)and its solid electrolyte interface(SEI)can be effective in improving the electrode kinetics.However,achieving fast charging using a simple and inexpensive strategy without sacrificing its initial Coulombic efficiency remains a challenge in sodium ion batteries.A simple liquid-phase coating approach has been used to generate a pitch-derived soft carbon layer on the HC surface,and its effect on the porosity of HC and SEI chemistry has been studied.A variety of structural characterizations show a soft carbon coating can increase the defect and ultra-micropore contents.The increase in ultra-micropore comes from both the soft carbon coatings and the larger pores within the HC that are partially filled by pitch,which provides more Na+storage sites.In-situ FTIR/EIS and ex-situ XPS showed that the soft carbon coating induced the formation of thinner SEI that is richer in NaF from the electrolyte,which stabilized the interface and promoted the charge transfer process.As a result,the anode produced fastcharging(329.8 mAh g^(−1)at 30 mA g^(−1)and 198.6 mAh g^(−1)at 300 mA g^(−1))and had a better cycling performance(a high capacity retention of 81.4%after 100 cycles at 150 mA g^(−1)).This work reveals the critical role of coating layer in changing the pore structure,SEI chemistry and diffusion kinetics of hard carbon,which enables rational design of sodium-ion battery anode with enhanced fast charging capability.展开更多
Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic ch...Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic chlorine.Especially,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC processes.Herein,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the OER.The work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.展开更多
The emerging interfacial polarization strategy exhibits applicative potential in piezoelectric enhancement.However,there is an ongoing effort to address the inherent limitations arising from charge bridging phenomena ...The emerging interfacial polarization strategy exhibits applicative potential in piezoelectric enhancement.However,there is an ongoing effort to address the inherent limitations arising from charge bridging phenomena and stochastic interface disorder that plague the improvement of piezoelectric performance.Here,we report a dual structure reinforced MXene/PVDF-TrFE piezoelectric composite,whose piezoelectricity is enhanced under the coupling effect of interfacial polarization and structural design.Synergistically,molecular dynamics simulations,density functional theory calculations and experimental validation revealed the details of interfacial interactions,which promotes the net spontaneous polarization of PVDF-TrFE from the 0.56 to 31.41 Debye.The oriented MXene distribution and porous structure not only tripled the piezoelectric response but also achieved an eightfold increase in sensitivity within the low-pressure region,along with demonstrating cyclic stability exceeding 20,000 cycles.The properties reinforcement originating from dual structure is elucidated through the finite element simulation and experimental validation.Attributed to the excellent piezoelectric response and deep learning algorithm,the sensor can effectively recognize the signals of artery pulse and finger flexion.Finally,a 3×3 sensor array is fabricated to monitor the pressure distribution wirelessly.This study provides an innovative methodology for reinforcing interfacial polarized piezoelectric materials and insight into structural designs.展开更多
Magnesium(Mg)and its alloys,as the lowest density metallic structural alloys,have been widely employed across various industries,including electronic communication,automotive,aircraft,defense,and military.While Mg all...Magnesium(Mg)and its alloys,as the lowest density metallic structural alloys,have been widely employed across various industries,including electronic communication,automotive,aircraft,defense,and military.While Mg alloys are susceptible to issues like pitting or stress corrosion when utilized as key structural components in humid environments,resulting in corrosion fatigue,stress corrosion cracking,or even complete corrosion failure,which impedes their broader applications.To address these disadvantages of Mg alloys,surface selfnanocrystallization(SSNC),involving refining the grain size to create a nanosurface layer,has been proposed to delay or mitigate the initiation and propagation of cracks,thereby significantly enhancing corrosion resistance.The purpose of this paper is to review the effects of various surface self-nanocrystallization techniques,including surface mechanical attrition treatment,high-energy shot peening,ultrasonic surface rolling processing,laser shock peening,and supersonic particle bombardment,on the microstructure and properties of Mg alloys.Additionally,the mechanisms underlying the surface nanocrystallization-induced microstructural evolution in Mg alloys and the factors influencing their corrosion resistance are systematically summarized.Finally,the current challenges and prospects are discussed as well.展开更多
Fe-based superconductors represent a fascinating class of materials,extensively studied for their complex interplay of superconductivity,magnetism,spin density waves,and nematicity,along with the interactions among th...Fe-based superconductors represent a fascinating class of materials,extensively studied for their complex interplay of superconductivity,magnetism,spin density waves,and nematicity,along with the interactions among these orders.An intriguing yet unexplained phenomenon observed in Fe-based superconductors is the emergence of superconductivity below 25K in the non-superconducting parent compound SrFe_(2)As_(2)following exposure to water at its surface.In this study,we employed in situ angle-resolved photoemission spectroscopy and low-energy electron diffraction to meticulously examine the electronic structure evolution of SrFe_(2)As_(2)upon in situ water dosing.Our findings indicate that water dosing markedly attenuates the spin density wave phase and surface Sr reconstruction while preserving the nematic order in SrFe_(2)As_(2).Furthermore,we detected an enhancement in the spectral weight of bands near the Fermi level.Our observations highlight the critical role of the intricate interplay among various orders induced by water dosing,which effectively modifies the band structure and favors the emergence of superconductivity in SrFe_(2)As_(2).展开更多
The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the ...The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the synergistic effects mainly focus on the energetics of key intermediates during the electrocatalysis,while the properties of electrode surface and electric-double-layer(EDL)structure are largely overlooked.Herein,we report the synthesis of Ru nanoparticles integrated with neighboring Ru single atoms on nitrogen doped carbon(Ru1,n/NC)as efficient catalysts toward hydrogen oxidation reaction(HOR)under alkaline electrolytes.Electrochemical data,in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy,and density functional theory calculations reveal that the positively charged Ru single atoms could lead to the dynamically regulated proportion of strongly hydrogen-bonded interfacial water structure with O-down conformation and optimized connectivity of the hydrogen-bond network in the EDL region,which contribute to the accelerated diffusion of hydroxide ions to the electrified interfaces.Consequently,the obtained Ru1,n/NC catalyst displays remarkable HOR performance with the mass activity of 1.15 mAμgPGM^(-1) under alkaline electrolyte.This work demonstrates the promise of single atoms for interfacial water environment adjustment and mass transfer process modulation,providing new insights into rational design of highly-effective SAC-based electrocatalysts.展开更多
Current research on the fabrication of rolled composite plates primarily focuses on processing and bonding mechanisms.Compared with hot-rolling technology,the electrically assisted rolling process has demonstrated exc...Current research on the fabrication of rolled composite plates primarily focuses on processing and bonding mechanisms.Compared with hot-rolling technology,the electrically assisted rolling process has demonstrated excellent performance in interfacial bonding effects.However,the influence of different current loading modes on the interfacial recombination process of composite panels varies significantly.In this study,low-frequency electrically assisted rolling was used in the first pass to pre-bond a composite plate at a low reduction rate of 15%.High-frequency electrically assisted rolling was used during the second pass,and Al/Mg alloy composite plates were obtained.The interfacial microstructure and mechanical properties of the composite plate were coordinated regulation by designing the rolling reduction rate.The results showed the interfacial morphology of the alternating distribution of the melt-diffusion layer,diffusion layer,and the formation of a new Al/Mg bonding interface.At the melt-diffusion interface,the irregular intermetallic compounds(IMCs)and the new Al/Mg bonding interface were alternately distributed,and the IMCs contained theα-Mg,Mg17Al12,and Mg2Al3 phases.In addition,an extremely high shear strength of 78.26 MPa was achieved.Adhesion of the Mg alloy matrix was observed on the fracture surface of the Al alloy side.The high shear strength was mainly attributed to the formation of a unique interfacial structure and the appearance of a melt-diffusion layer.Compared to the diffusion-reduction interface,the regular rectangular IMCs and the new Al/Mg bonding interface were alternately distributed,and the IMCs consisted of the Mg17Al12 and Mg2Al3 phases.The shear test results showed that the shear strength of the interface reached 68.69 MPa,and a regular distribution of the Mg alloy matrix with dimples and the Al alloy matrix with a necking zone was observed on the fracture surface of the Al side.Tensile strength test results revealed a maximum value of 316.86 MPa for the Al/Mg alloy composite plate.The tensile and interfacial bonding strengths can be synchronously enhanced by coordinating the regulation of the interfacial structure.This study proposes a new electrically assisted rolling technology that is useful for the fabrication of composite plates with excellent mechanical properties.展开更多
Enhancing the lubricating properties and antibacterial adhesion resistance of implantable medical materials is critical to prevent soft tissue injury during implantation and the formation of bacterial biofilms.Prior s...Enhancing the lubricating properties and antibacterial adhesion resistance of implantable medical materials is critical to prevent soft tissue injury during implantation and the formation of bacterial biofilms.Prior studies may have exhibited limitations in the preparation methodologies and long-term stability of coatings for implantable medical materials.In this study,we developed a multilayered hybrid hydrogel coating method based on the rate difference of polymerization initiation on the material surface.The acquired coating with persistent lubrication capability retained its functionality after 2×10^(4) cycles of friction and 21 days of PBS immersion.A quaternary ammonium salt coating with antibacterial properties was introduced to further functionalize the coating.Animal experiments demonstrated that this coating exhibited remarkable effects on delaying encrustation and bacterial colonization.These studies indicate that this simple method of introducing lubricating and antibacterial coatings on catheters is likely to enhance the biocompatibility of medical devices and has broad application prospects in this field of medical devices.展开更多
In the aerospace field,hole burnishing enhancement plays an essential role in improving the service performance of load-bearing holes.To satisfy the assembly accuracy and strength requirements,the structure shape and ...In the aerospace field,hole burnishing enhancement plays an essential role in improving the service performance of load-bearing holes.To satisfy the assembly accuracy and strength requirements,the structure shape and surface integrity must be considered simultaneously during the enhancement process.The current manufacturing process of hole burnishing has a relatively weak balance between the structure shape and surface integrity;therefore,it is necessary to analyze the mechanism and optimize the parameters to improve the strengthening effect of the holes.In this study,a two-dimensional longitudinal simplified model for the hole burnishing process was established,and the reasons for the surface roughness improvement of the hole wall and material accumulation on the upper surface were analyzed.Experiments were conducted to determine the influence of the burnishing parameters on the structure shape(material accumulation,shape contour,and roundness)and surface integrity(surface roughness,residual stress,and surface hardness),based on the opposite requirements of improving the structure shape and surface integrity for the burnishing depth(BD).The results showed that with an increase in the BD,the structure shape deteriorated,whereas the surface integrity improved.Fatigue behavior verification experiments were conducted,and parameter selection schemes for the collaborative improvement of the structure shape and surface integrity were discussed.For the holes of titanium alloy TB6(Ti-10V-2Fe-3Al),the fatigue life can be increased by 162%when the BD,spindle speed,and feed rate were 0.20 mm,200 r/min,and 0.2 mm/r,respectively.展开更多
Iron oxide nanoparticles(IONPs)with intrinsic peroxidase(POD)-mimic activity have gained significant attention as nanozymes.Reducing sizes of IONPs is the mostly applied strategy to boost their enzymatic activity due ...Iron oxide nanoparticles(IONPs)with intrinsic peroxidase(POD)-mimic activity have gained significant attention as nanozymes.Reducing sizes of IONPs is the mostly applied strategy to boost their enzymatic activity due to their high specific surface areas.Herein,we synthesized a series of uniformly sized IONPs ranging from3.17 to 21.2 nm,and found that POD activity of IONPs is not monotone increased by reducing their sizes,with the optimal size of 7.82 nm rather than smaller sized 3.17 nm.The reason for this unnormal phenomenon is that electronic structure also had great influence on POD activity,especially at the ultrasmall size region.Since Fe^(2+)are with higher enzymatic activity than Fe^(3+),3.17 nm IONPs although have the largest specific surface area,are prone to be oxidized,which reduced their iron content and ratio of Fe^(2+)to Fe^(3+),and consequently decreased their POD activity.By intentionally oxidized 7.82 nm IONPs in air,POD activity was obviously reduced,illustrating electronic structure cannot be overlooked.At the larger sized region ranging from 7.82 to 21.2 nm,oxidation degree of IONPs is similar,and surface electronic structure had a negligible effect on POD activity,and therefore,POD activity is predominantly influenced by specific surface area.By using the optimized 7.82 nm IONPs,tumor growth was obviously inhibited,demonstrating their potential in cancer therapeutics.Our results reveal that the designing of nanozymes should comprehensively balance their influence of surface electronic structure and specific surface area.展开更多
As cathode materials for alkali-ion batteries,sodium manganese oxides have been receiving considerable and continuous attention in recent decades.In this work,the structure and environment-dependent stability of NaMn_...As cathode materials for alkali-ion batteries,sodium manganese oxides have been receiving considerable and continuous attention in recent decades.In this work,the structure and environment-dependent stability of NaMn_(2)O_(4) surface were studied based on the first principles calculations.The surface stability diagram of NaMn_(2)O_(4) involving various different terminations of(100),(110)and(111)surfaces was constructed,and the stability of these different terminations could be compared as a function of chemical environment.It is found that the(100)-MnO and(111)-ONa terminations are two more stable terminations under the investigated chemical conditions.And the surface energies of(110)surfaces are negative under the investigated chemical potential,hence,(110)surfaces are unstable.The surface energy of NaMn_(2)O_(4) as a function of O chemical potential is also investigated under constant Na chemical potential.The structure relaxation indicates that the surface rumpling and surface reconstruction can affect the electronic structure of the surface,thereby reducing surface energy and stabilizing the surface.Furthermore,the Wulff shape of NaMn_(2)O_(4) was also constructed based on Gibbs-Wulff theorem.展开更多
Surface/underwater target classification is a key topic in marine information research.However,the complex underwater environment,coupled with the diversity of target types and their variable characteristics,presents ...Surface/underwater target classification is a key topic in marine information research.However,the complex underwater environment,coupled with the diversity of target types and their variable characteristics,presents significant challenges for classifier design.For shallow-water waveguides with a negative thermocline,a residual neural network(ResNet)model based on the sound field elevation structure is constructed.This model demonstrates robust classification performance even when facing low signal-to-noise ratios and environmental mismatches.Meanwhile,to address the reduced generalization ability caused by limited labeled acoustic data,an improved ResNet model based on unsupervised domain adaptation(“proposed UDA-ResNet”)is further constructed.This model incorporates data on simulated elevation structures of the sound field to augment the training process.Adversarial training is employed to extract domain-invariant features from simulated and trial data.These strategies help reduce the negative impact caused by domain differences.Experimental results demonstrate that the proposed method shows strong surface/underwater target classification ability under limited sample sizes,thus confirming its feasibility and effectiveness.展开更多
An effective optimization method for the shape/sizing design of composite wing structures is presented with satisfying weight-cutting results. After decoupling, a kind of two-layer cycled optimization strategy suitabl...An effective optimization method for the shape/sizing design of composite wing structures is presented with satisfying weight-cutting results. After decoupling, a kind of two-layer cycled optimization strategy suitable for these integrated shape/sizing optimization is obtained. The uniform design method is used to provide sample points, and approximation models for shape design variables. And the results of sizing optimization are construct- ed with the quadratic response surface method (QRSM). The complex method based on QRSM is used to opti- mize the shape design variables and the criteria method is adopted to optimize the sizing design variables. Compared with the conventional method, the proposed algorithm is more effective and feasible for solving complex composite optimization problems and has good efficiency in weight cutting.展开更多
The surface and interfacial properties of polymeric bonding agents and nitramine crystal fillers were studied. The surface free energy and adhesion work of polymeric bonding agents and nitramine fillers were calculate...The surface and interfacial properties of polymeric bonding agents and nitramine crystal fillers were studied. The surface free energy and adhesion work of polymeric bonding agents and nitramine fillers were calculated by using Kaeble′s equations. It was observed that the hydroxyl values of neutral polymeric bonding agents (NPBA) correlate well with the polar components of surface free energies. On the basis of the measurements of swelling ratio and initial modulus, the interfacial bonding through highly crosslinked polymeric shell formation around the nitramine particles and generating interfacial reinforcement were rationalized. The application of Tapping Mode AFM (atomic force micro scope) to observing the surface morphology of NPBA reveals that methyl acrylate monomer appears to play a role for aiding the formation of network like structure when nanometer scale images of NPBA are created.展开更多
We assembled approximately 328 seismic records. The data set was from 4 digitally recording long-period and broadband stations of CDSN. We carried out the inversion based on the partitioned waveform inversion (PWI). I...We assembled approximately 328 seismic records. The data set was from 4 digitally recording long-period and broadband stations of CDSN. We carried out the inversion based on the partitioned waveform inversion (PWI). It partitions the large-scale optimization problem into a number of independent small-scale problems. We adopted surface waveform inversion with an equal block (2((2() discretization in order to acquire the images of shear velocity structure at different depths (from surface to 430 km) in the crust and upper-mantle. The resolution of all these anomalies has been established with (check-board( resolution tests. These results show significant difference in velocity, lithosphere and asthenosphere structure between South China Sea and its adjacent regions.展开更多
This paper discusses the coloration process on the stainless steel and the properties of the film. The compositions, morphology and structure of colored films on stainless steel are studied by using SEM,AES,AFM,STM. ...This paper discusses the coloration process on the stainless steel and the properties of the film. The compositions, morphology and structure of colored films on stainless steel are studied by using SEM,AES,AFM,STM. The diffusion controlled mechanisms of films and calculation formula of surface electropotential difference are discussed.展开更多
The production of valuable chemicals using copper(Cu)catalysts via electrochemical CO or CO_(2)reduction reactions(CORR and CO_(2)RR)has shown great potential in the field of sustainable energy conversion[1].Previous ...The production of valuable chemicals using copper(Cu)catalysts via electrochemical CO or CO_(2)reduction reactions(CORR and CO_(2)RR)has shown great potential in the field of sustainable energy conversion[1].Previous research has primarily focused on analyzing the behavior of reaction intermediates or solely on the dynamics within the solution phase,while the synergistic effects between surface species and the solution,particularly the interfacial water and its non-covalent interactions with the Cu surface,have remained partially understood[2].展开更多
Tree plantations are globally significant,and therefore,growth-related challenges cannot be ignored.Canopy structure and light environment influence the growth of plantations,but the precise relationship remains uncle...Tree plantations are globally significant,and therefore,growth-related challenges cannot be ignored.Canopy structure and light environment influence the growth of plantations,but the precise relationship remains unclear.We selected seven-year-old poplar plantations of varying cultivars planted various densities and measured their growth,canopy structure,and light environment.The findings indicate that poplar plantations of different cultivars and at different planting densities showed variations in leaf area index(LAI),average leaf angle(ALA),crown length(CL),length ratio(CLR),roundness(CR)and surface area(CSA),which directly or indirectly affect growth,resulting in disparities in their growing conditions.Crown roundness directly impacted growth,while LAI,CLR and ALA influenced growth indirectly by affecting intercellular carbon dioxide concentration.LAI and CLR had a positive effect;ALA had a negative one.Crown length and surface area directly and indirectly influenced growth by affecting photo synthetically active radiation and net photo synthetic rate,with direct impacts being more pronounced.This research has clarified the regulatory role of canopy structure in plantations growth,providing valuable insights for developing more effective management strategies.展开更多
基金the National Natural Science Foundation of China(No.22379047)Yinzhou R&D Team(X.W.)+2 种基金Guangdong Basic and Applied Basic Research Foundation(2022B1515120019)the Project Funded by the China Scholarship Council(No.202108320278)the support from the Vacuum Interconnected Nanotech Workstation(Nano-X)from Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences(SINANO)。
文摘Aqueous zinc-ion batteries(AZIBs)offer a safe,cost-effective,and high-capacity energy storage solution,yet their performance is hindered by interfacial challenges at the Zn anode,including hydrogen evolution,corrosion,and dendritic Zn growth.While most studies focus on regulating Zn~(2+)solvation structures in bulk electrolytes,the evolution of interfacial solvation—where Zn~(2+)undergoes desolvation and deposition—remains insufficiently explored.Here,we introduce sulfated nanocellulose(SNC),an anion-rich biopolymer,to tailor the interfacial solvation structure without altering the bulk electrolyte composition.Using in situ attenuated total reflection Fourier transform infrared spectroscopy and fluorescence interface-extended X-ray absorption fine structure,we reveal that SNC facilitates the formation of a low-coordinated Zn~(2+)solvation shell at the interface by weakening H_(2)O coordination.This transformation is driven by electrostatic interactions between Zn~(2+)and anchored sulfate groups,thereby reducing water activity,improving interfacial stability during charge/discharge,and suppressing parasitic reactions.Consequently,a high average coulombic efficiency of 99.6%over 500 cycles in Zn|Ti asymmetric cells and 1.5 Ah pouch cells(13.4 mg cm^(-2)loading,remained stable over 250 cycles)were achieved in SNC-induced AZIBs.This work underscores the importance of interfacial solvation structure engineering—beyond traditional bulk electrolyte design—in enabling practical,high-performance AZIBs.
基金supported by the Innovative Research Group Project of the National Natural Science Foundation of China(T2121004)Key Programme(52235007)National Outstanding Youth Foundation of China(52325504).
文摘Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and high mechanical properties.Inspired by Chinese ramen,we propose a universal fabricating method(printing-P,training-T,cross-linking-C,PTC&PCT)for tough hydrogel scaffolds to fill this gap.First,3D printing fabricates a hydrogel scaffold with desired structures(P).Then,the scaffold could have extraordinarily high mechanical properties and functional surface structure by cycle mechanical training with salting-out assistance(T).Finally,the training results are fixed by photo-cross-linking processing(C).The tough gelatin hydrogel scaffolds exhibit excellent tensile strength of 6.66 MPa(622-fold untreated)and have excellent biocompatibility.Furthermore,this scaffold possesses functional surface structures from nanometer to micron to millimeter,which can efficiently induce directional cell growth.Interestingly,this strategy can produce bionic human tissue with mechanical properties of 10 kPa-10 MPa by changing the type of salt,and many hydrogels,such as gelatin and silk,could be improved with PTC or PCT strategies.Animal experiments show that this scaffold can effectively promote the new generation of muscle fibers,blood vessels,and nerves within 4 weeks,prompting the rapid regeneration of large-volume muscle loss injuries.
基金National Key Research and Development Program of China(2022YFE0206300)National Natural Science Foundation of China(U21A2081,22075074,22209047)+2 种基金Guangdong Basic and Applied Basic Research Foundation(2024A1515011620)Hunan Provincial Natural Science Foundation of China(2024JJ5068)Foundation of Yuelushan Center for Industrial Innovation(2023YCII0119)。
文摘Changes to the microstructure of a hard carbon(HC)and its solid electrolyte interface(SEI)can be effective in improving the electrode kinetics.However,achieving fast charging using a simple and inexpensive strategy without sacrificing its initial Coulombic efficiency remains a challenge in sodium ion batteries.A simple liquid-phase coating approach has been used to generate a pitch-derived soft carbon layer on the HC surface,and its effect on the porosity of HC and SEI chemistry has been studied.A variety of structural characterizations show a soft carbon coating can increase the defect and ultra-micropore contents.The increase in ultra-micropore comes from both the soft carbon coatings and the larger pores within the HC that are partially filled by pitch,which provides more Na+storage sites.In-situ FTIR/EIS and ex-situ XPS showed that the soft carbon coating induced the formation of thinner SEI that is richer in NaF from the electrolyte,which stabilized the interface and promoted the charge transfer process.As a result,the anode produced fastcharging(329.8 mAh g^(−1)at 30 mA g^(−1)and 198.6 mAh g^(−1)at 300 mA g^(−1))and had a better cycling performance(a high capacity retention of 81.4%after 100 cycles at 150 mA g^(−1)).This work reveals the critical role of coating layer in changing the pore structure,SEI chemistry and diffusion kinetics of hard carbon,which enables rational design of sodium-ion battery anode with enhanced fast charging capability.
文摘Photoelectrocatalytic(PEC)seawater splitting as a green and sustainable route to harvest hydrogen is attractive yet hampered by low activity of photoanodes and unexpected high selectivity to the corrosive and toxic chlorine.Especially,it is full of challenges to unveil the key factors influencing the selectivity of such complex PEC processes.Herein,by regulating the energy band and surface structure of the anatase TiO_(2) nanotube array photoanode via nitrogen-doping,the seawater PEC oxidation shifts from Cl^(-)oxidation reaction(ClOR)dominant on the TiO_(2) photoanode(61.6%)to oxygen evolution reaction(OER)dominant on the N-TiO_(2) photoanode(62.9%).Comprehensive investigations including operando photoelectrochemical FTIR and DFT calculations unveil that the asymmetric hydrogen-bonding water at the N-TiO_(2) electrode/electrolyte interface enriches under illumination,facilitating proton transfer and moderate adsorption strength of oxygen-intermediates,which lowers the energy barrier for the OER yet elevates the energy barrier for the ClOR,resulting to a promoted selectivity towards the OER.The work sheds light on the underlying mechanism of the PEC water oxidation processes,and highlights the crucial role of interfacial water on the PEC selectivity,which could be regulated by controlling the energy band and the surface structure of semiconductors.
基金supported by the National Natural Science Foundation of China(No.52303328)the Postdoctoral Innovation Talents Support Program(No.BX20220257)the Sichuan Science and Technology Program(No.2023NSFSC0313).
文摘The emerging interfacial polarization strategy exhibits applicative potential in piezoelectric enhancement.However,there is an ongoing effort to address the inherent limitations arising from charge bridging phenomena and stochastic interface disorder that plague the improvement of piezoelectric performance.Here,we report a dual structure reinforced MXene/PVDF-TrFE piezoelectric composite,whose piezoelectricity is enhanced under the coupling effect of interfacial polarization and structural design.Synergistically,molecular dynamics simulations,density functional theory calculations and experimental validation revealed the details of interfacial interactions,which promotes the net spontaneous polarization of PVDF-TrFE from the 0.56 to 31.41 Debye.The oriented MXene distribution and porous structure not only tripled the piezoelectric response but also achieved an eightfold increase in sensitivity within the low-pressure region,along with demonstrating cyclic stability exceeding 20,000 cycles.The properties reinforcement originating from dual structure is elucidated through the finite element simulation and experimental validation.Attributed to the excellent piezoelectric response and deep learning algorithm,the sensor can effectively recognize the signals of artery pulse and finger flexion.Finally,a 3×3 sensor array is fabricated to monitor the pressure distribution wirelessly.This study provides an innovative methodology for reinforcing interfacial polarized piezoelectric materials and insight into structural designs.
基金funded by the National Key R&D Program of China(No.2024YFB3713703,2023YFB3712700,2021YFB3702101)the Fundamental Research Funds for the Central Universities(2024IAIS-ZD004)+1 种基金State Key Laboratory of Mechanical Transmission for Advanced Equipment Open Fund(SKLMT-ZZKT-2024Z04)the support by the Innovation Group Project of Southern Marine Science and Engineering Guangdong Laboratory(Zhuhai)(311021013).
文摘Magnesium(Mg)and its alloys,as the lowest density metallic structural alloys,have been widely employed across various industries,including electronic communication,automotive,aircraft,defense,and military.While Mg alloys are susceptible to issues like pitting or stress corrosion when utilized as key structural components in humid environments,resulting in corrosion fatigue,stress corrosion cracking,or even complete corrosion failure,which impedes their broader applications.To address these disadvantages of Mg alloys,surface selfnanocrystallization(SSNC),involving refining the grain size to create a nanosurface layer,has been proposed to delay or mitigate the initiation and propagation of cracks,thereby significantly enhancing corrosion resistance.The purpose of this paper is to review the effects of various surface self-nanocrystallization techniques,including surface mechanical attrition treatment,high-energy shot peening,ultrasonic surface rolling processing,laser shock peening,and supersonic particle bombardment,on the microstructure and properties of Mg alloys.Additionally,the mechanisms underlying the surface nanocrystallization-induced microstructural evolution in Mg alloys and the factors influencing their corrosion resistance are systematically summarized.Finally,the current challenges and prospects are discussed as well.
基金supported by the National Nature Science Foundation of China[Grant Nos.92365204 and 12274298(Z.K.Liu)]the National Key R&D program of China[Grant No.2022YFA1604400/03(Z.K.Liu)]Zhangjiang Laboratory(Y.M.Zhang).The authors thank BL02B at the Shanghai Synchrotron Radiation Facility supported by the National Natural Science Foundation of China(Contract No.11227902).
文摘Fe-based superconductors represent a fascinating class of materials,extensively studied for their complex interplay of superconductivity,magnetism,spin density waves,and nematicity,along with the interactions among these orders.An intriguing yet unexplained phenomenon observed in Fe-based superconductors is the emergence of superconductivity below 25K in the non-superconducting parent compound SrFe_(2)As_(2)following exposure to water at its surface.In this study,we employed in situ angle-resolved photoemission spectroscopy and low-energy electron diffraction to meticulously examine the electronic structure evolution of SrFe_(2)As_(2)upon in situ water dosing.Our findings indicate that water dosing markedly attenuates the spin density wave phase and surface Sr reconstruction while preserving the nematic order in SrFe_(2)As_(2).Furthermore,we detected an enhancement in the spectral weight of bands near the Fermi level.Our observations highlight the critical role of the intricate interplay among various orders induced by water dosing,which effectively modifies the band structure and favors the emergence of superconductivity in SrFe_(2)As_(2).
文摘The employment of single atom catalysts(SACs)remarkably increases atomic utilization and catalytic efficiency in various electrochemical processes,especially when coupled with metal clusters/nanoparticles.However,the synergistic effects mainly focus on the energetics of key intermediates during the electrocatalysis,while the properties of electrode surface and electric-double-layer(EDL)structure are largely overlooked.Herein,we report the synthesis of Ru nanoparticles integrated with neighboring Ru single atoms on nitrogen doped carbon(Ru1,n/NC)as efficient catalysts toward hydrogen oxidation reaction(HOR)under alkaline electrolytes.Electrochemical data,in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy,and density functional theory calculations reveal that the positively charged Ru single atoms could lead to the dynamically regulated proportion of strongly hydrogen-bonded interfacial water structure with O-down conformation and optimized connectivity of the hydrogen-bond network in the EDL region,which contribute to the accelerated diffusion of hydroxide ions to the electrified interfaces.Consequently,the obtained Ru1,n/NC catalyst displays remarkable HOR performance with the mass activity of 1.15 mAμgPGM^(-1) under alkaline electrolyte.This work demonstrates the promise of single atoms for interfacial water environment adjustment and mass transfer process modulation,providing new insights into rational design of highly-effective SAC-based electrocatalysts.
基金Supported by National Natural Science Foundation of China(Grant Nos.52075360,52275360,51805359).
文摘Current research on the fabrication of rolled composite plates primarily focuses on processing and bonding mechanisms.Compared with hot-rolling technology,the electrically assisted rolling process has demonstrated excellent performance in interfacial bonding effects.However,the influence of different current loading modes on the interfacial recombination process of composite panels varies significantly.In this study,low-frequency electrically assisted rolling was used in the first pass to pre-bond a composite plate at a low reduction rate of 15%.High-frequency electrically assisted rolling was used during the second pass,and Al/Mg alloy composite plates were obtained.The interfacial microstructure and mechanical properties of the composite plate were coordinated regulation by designing the rolling reduction rate.The results showed the interfacial morphology of the alternating distribution of the melt-diffusion layer,diffusion layer,and the formation of a new Al/Mg bonding interface.At the melt-diffusion interface,the irregular intermetallic compounds(IMCs)and the new Al/Mg bonding interface were alternately distributed,and the IMCs contained theα-Mg,Mg17Al12,and Mg2Al3 phases.In addition,an extremely high shear strength of 78.26 MPa was achieved.Adhesion of the Mg alloy matrix was observed on the fracture surface of the Al alloy side.The high shear strength was mainly attributed to the formation of a unique interfacial structure and the appearance of a melt-diffusion layer.Compared to the diffusion-reduction interface,the regular rectangular IMCs and the new Al/Mg bonding interface were alternately distributed,and the IMCs consisted of the Mg17Al12 and Mg2Al3 phases.The shear test results showed that the shear strength of the interface reached 68.69 MPa,and a regular distribution of the Mg alloy matrix with dimples and the Al alloy matrix with a necking zone was observed on the fracture surface of the Al side.Tensile strength test results revealed a maximum value of 316.86 MPa for the Al/Mg alloy composite plate.The tensile and interfacial bonding strengths can be synchronously enhanced by coordinating the regulation of the interfacial structure.This study proposes a new electrically assisted rolling technology that is useful for the fabrication of composite plates with excellent mechanical properties.
基金financially supported by the National Natural Science Foundation of China(Nos.52373296 and 52173287)。
文摘Enhancing the lubricating properties and antibacterial adhesion resistance of implantable medical materials is critical to prevent soft tissue injury during implantation and the formation of bacterial biofilms.Prior studies may have exhibited limitations in the preparation methodologies and long-term stability of coatings for implantable medical materials.In this study,we developed a multilayered hybrid hydrogel coating method based on the rate difference of polymerization initiation on the material surface.The acquired coating with persistent lubrication capability retained its functionality after 2×10^(4) cycles of friction and 21 days of PBS immersion.A quaternary ammonium salt coating with antibacterial properties was introduced to further functionalize the coating.Animal experiments demonstrated that this coating exhibited remarkable effects on delaying encrustation and bacterial colonization.These studies indicate that this simple method of introducing lubricating and antibacterial coatings on catheters is likely to enhance the biocompatibility of medical devices and has broad application prospects in this field of medical devices.
文摘In the aerospace field,hole burnishing enhancement plays an essential role in improving the service performance of load-bearing holes.To satisfy the assembly accuracy and strength requirements,the structure shape and surface integrity must be considered simultaneously during the enhancement process.The current manufacturing process of hole burnishing has a relatively weak balance between the structure shape and surface integrity;therefore,it is necessary to analyze the mechanism and optimize the parameters to improve the strengthening effect of the holes.In this study,a two-dimensional longitudinal simplified model for the hole burnishing process was established,and the reasons for the surface roughness improvement of the hole wall and material accumulation on the upper surface were analyzed.Experiments were conducted to determine the influence of the burnishing parameters on the structure shape(material accumulation,shape contour,and roundness)and surface integrity(surface roughness,residual stress,and surface hardness),based on the opposite requirements of improving the structure shape and surface integrity for the burnishing depth(BD).The results showed that with an increase in the BD,the structure shape deteriorated,whereas the surface integrity improved.Fatigue behavior verification experiments were conducted,and parameter selection schemes for the collaborative improvement of the structure shape and surface integrity were discussed.For the holes of titanium alloy TB6(Ti-10V-2Fe-3Al),the fatigue life can be increased by 162%when the BD,spindle speed,and feed rate were 0.20 mm,200 r/min,and 0.2 mm/r,respectively.
基金financially supported by the Natural Science Foundation of Zhejiang Province(No.LR22E010001)the National Natural Science Foundation of China(No.52073258)+1 种基金the Fundamental Research Funds for the Provincial Universities of Zhejiang(No.RF-B2022006)the R&D Program of Zhejiang University of Technology(No.KYY-HX-20190730)
文摘Iron oxide nanoparticles(IONPs)with intrinsic peroxidase(POD)-mimic activity have gained significant attention as nanozymes.Reducing sizes of IONPs is the mostly applied strategy to boost their enzymatic activity due to their high specific surface areas.Herein,we synthesized a series of uniformly sized IONPs ranging from3.17 to 21.2 nm,and found that POD activity of IONPs is not monotone increased by reducing their sizes,with the optimal size of 7.82 nm rather than smaller sized 3.17 nm.The reason for this unnormal phenomenon is that electronic structure also had great influence on POD activity,especially at the ultrasmall size region.Since Fe^(2+)are with higher enzymatic activity than Fe^(3+),3.17 nm IONPs although have the largest specific surface area,are prone to be oxidized,which reduced their iron content and ratio of Fe^(2+)to Fe^(3+),and consequently decreased their POD activity.By intentionally oxidized 7.82 nm IONPs in air,POD activity was obviously reduced,illustrating electronic structure cannot be overlooked.At the larger sized region ranging from 7.82 to 21.2 nm,oxidation degree of IONPs is similar,and surface electronic structure had a negligible effect on POD activity,and therefore,POD activity is predominantly influenced by specific surface area.By using the optimized 7.82 nm IONPs,tumor growth was obviously inhibited,demonstrating their potential in cancer therapeutics.Our results reveal that the designing of nanozymes should comprehensively balance their influence of surface electronic structure and specific surface area.
基金Project(BK20241969)supported by the Natural Science Foundation of Jiangsu Province,ChinaProject(51971249)supported by the National Natural Science Foundation of China。
文摘As cathode materials for alkali-ion batteries,sodium manganese oxides have been receiving considerable and continuous attention in recent decades.In this work,the structure and environment-dependent stability of NaMn_(2)O_(4) surface were studied based on the first principles calculations.The surface stability diagram of NaMn_(2)O_(4) involving various different terminations of(100),(110)and(111)surfaces was constructed,and the stability of these different terminations could be compared as a function of chemical environment.It is found that the(100)-MnO and(111)-ONa terminations are two more stable terminations under the investigated chemical conditions.And the surface energies of(110)surfaces are negative under the investigated chemical potential,hence,(110)surfaces are unstable.The surface energy of NaMn_(2)O_(4) as a function of O chemical potential is also investigated under constant Na chemical potential.The structure relaxation indicates that the surface rumpling and surface reconstruction can affect the electronic structure of the surface,thereby reducing surface energy and stabilizing the surface.Furthermore,the Wulff shape of NaMn_(2)O_(4) was also constructed based on Gibbs-Wulff theorem.
基金supported by the National Natural Science Foundation of China(Grant Nos.62471024 and 62301183)the Open Research Fund of Hanjiang Laboratory(KF2024001).
文摘Surface/underwater target classification is a key topic in marine information research.However,the complex underwater environment,coupled with the diversity of target types and their variable characteristics,presents significant challenges for classifier design.For shallow-water waveguides with a negative thermocline,a residual neural network(ResNet)model based on the sound field elevation structure is constructed.This model demonstrates robust classification performance even when facing low signal-to-noise ratios and environmental mismatches.Meanwhile,to address the reduced generalization ability caused by limited labeled acoustic data,an improved ResNet model based on unsupervised domain adaptation(“proposed UDA-ResNet”)is further constructed.This model incorporates data on simulated elevation structures of the sound field to augment the training process.Adversarial training is employed to extract domain-invariant features from simulated and trial data.These strategies help reduce the negative impact caused by domain differences.Experimental results demonstrate that the proposed method shows strong surface/underwater target classification ability under limited sample sizes,thus confirming its feasibility and effectiveness.
文摘An effective optimization method for the shape/sizing design of composite wing structures is presented with satisfying weight-cutting results. After decoupling, a kind of two-layer cycled optimization strategy suitable for these integrated shape/sizing optimization is obtained. The uniform design method is used to provide sample points, and approximation models for shape design variables. And the results of sizing optimization are construct- ed with the quadratic response surface method (QRSM). The complex method based on QRSM is used to opti- mize the shape design variables and the criteria method is adopted to optimize the sizing design variables. Compared with the conventional method, the proposed algorithm is more effective and feasible for solving complex composite optimization problems and has good efficiency in weight cutting.
文摘The surface and interfacial properties of polymeric bonding agents and nitramine crystal fillers were studied. The surface free energy and adhesion work of polymeric bonding agents and nitramine fillers were calculated by using Kaeble′s equations. It was observed that the hydroxyl values of neutral polymeric bonding agents (NPBA) correlate well with the polar components of surface free energies. On the basis of the measurements of swelling ratio and initial modulus, the interfacial bonding through highly crosslinked polymeric shell formation around the nitramine particles and generating interfacial reinforcement were rationalized. The application of Tapping Mode AFM (atomic force micro scope) to observing the surface morphology of NPBA reveals that methyl acrylate monomer appears to play a role for aiding the formation of network like structure when nanometer scale images of NPBA are created.
基金State Natural Scientific Foundation (49734150) and National High Performance Computation Foundation.
文摘We assembled approximately 328 seismic records. The data set was from 4 digitally recording long-period and broadband stations of CDSN. We carried out the inversion based on the partitioned waveform inversion (PWI). It partitions the large-scale optimization problem into a number of independent small-scale problems. We adopted surface waveform inversion with an equal block (2((2() discretization in order to acquire the images of shear velocity structure at different depths (from surface to 430 km) in the crust and upper-mantle. The resolution of all these anomalies has been established with (check-board( resolution tests. These results show significant difference in velocity, lithosphere and asthenosphere structure between South China Sea and its adjacent regions.
文摘This paper discusses the coloration process on the stainless steel and the properties of the film. The compositions, morphology and structure of colored films on stainless steel are studied by using SEM,AES,AFM,STM. The diffusion controlled mechanisms of films and calculation formula of surface electropotential difference are discussed.
文摘The production of valuable chemicals using copper(Cu)catalysts via electrochemical CO or CO_(2)reduction reactions(CORR and CO_(2)RR)has shown great potential in the field of sustainable energy conversion[1].Previous research has primarily focused on analyzing the behavior of reaction intermediates or solely on the dynamics within the solution phase,while the synergistic effects between surface species and the solution,particularly the interfacial water and its non-covalent interactions with the Cu surface,have remained partially understood[2].
基金supported by the National Key Research and Development Program of China(Grant No.2021YFD2201203)the financial support of the National Natural Science Foundation of China(32001311)。
文摘Tree plantations are globally significant,and therefore,growth-related challenges cannot be ignored.Canopy structure and light environment influence the growth of plantations,but the precise relationship remains unclear.We selected seven-year-old poplar plantations of varying cultivars planted various densities and measured their growth,canopy structure,and light environment.The findings indicate that poplar plantations of different cultivars and at different planting densities showed variations in leaf area index(LAI),average leaf angle(ALA),crown length(CL),length ratio(CLR),roundness(CR)and surface area(CSA),which directly or indirectly affect growth,resulting in disparities in their growing conditions.Crown roundness directly impacted growth,while LAI,CLR and ALA influenced growth indirectly by affecting intercellular carbon dioxide concentration.LAI and CLR had a positive effect;ALA had a negative one.Crown length and surface area directly and indirectly influenced growth by affecting photo synthetically active radiation and net photo synthetic rate,with direct impacts being more pronounced.This research has clarified the regulatory role of canopy structure in plantations growth,providing valuable insights for developing more effective management strategies.