Hydrogen-bonded framework(HOF) offers an attractive platform to encapsulate enzymes and stabilize their conformation,due to the advantages of mild synthesis conditions,tailorable pore structure,and backbone biocompati...Hydrogen-bonded framework(HOF) offers an attractive platform to encapsulate enzymes and stabilize their conformation,due to the advantages of mild synthesis conditions,tailorable pore structure,and backbone biocompatibility.However,the efficiency of this HOF approach relies on the interfacial interactions between enzyme vip and the ligand precursors,limiting its adaptability to enzymes with varying surface chemistry property.In this study,we report a site-specific surface modification strategy to positively tailor the enzyme surface charge,facilitating the biomimetic encapsulation of enzymes within HOF in situ.Both experimental results and computational simulation reveal that site-specific amination of enzyme surface's acidic residues contributes to the interfacial accumulation of carboxylic ligand precursors in aqueous solutions via synergistic electrostatic and hydrogen bonding interactions.This substantially facilitates the in situ growth of porous HOF surrounding the aminated enzyme biotemplates,with up to 100% enzyme loading efficiency.The resultant hydrogen-bonded biohybrid framework(HBF) retains high biocatalytic functions while exhibiting exceptional stability under harsh conditions.By leveraging the marked catalytic activity of GOx-NH_(2)@HBF-1 and a H_(2)O_(2)-sensitive QD,a highly sensitive glucose fluorescence sensor is fabricated with a wide linear range(5-2000 μmol/L) and a low quantification limit of 5 μmol/L.This work presents a simple yet effective enzyme surface engineering approach for integrating enzyme into HOF,opening new avenues for the construction of multifunctional HOF biocomposites.展开更多
Hydrogen peroxide(H_(2)O_(2))oxidation and reduction reactions(HPOR/HPRR)are pivotal in various innovative electrochemical energy conversion devices.A comprehensive understanding of these mechanisms is critical for ca...Hydrogen peroxide(H_(2)O_(2))oxidation and reduction reactions(HPOR/HPRR)are pivotal in various innovative electrochemical energy conversion devices.A comprehensive understanding of these mechanisms is critical for catalyst design and performance improvement in these applications.In this work,we systematically investigate the HPOR/HPRR mechanisms on low-index Pt surfaces,specifically Pt(111),Pt(100)and Pt(110),through density functional theory(DFT)calculations combined with the computational hydrogen electrode(CHE)model.For HPOR,all the low-index Pt surfaces exhibit a unified potential-determining step(PDS)involving the electrochemical oxidation of hydroperoxyl intermediates(HOO*).The binding free energy of HOO*(Δ_(GHOO*))emerges as an activity descriptor,with Pt(110)exhibiting the highest HPOR activity.The HPRR mechanism follows a chem-electrochemical(C-EC)pathway.The rate-determining step(RDS)of HPRR is either the cleavage of the HO-OH bond(chemical)or the reduction of HO(electrochemical),depending on their respective activation energies.These activation energies are functions of the HO*binding free energy,Δ_(GHO*),establishingΔ_(GHO*)as the descriptor for HPRR activity prediction.Pt(111)and Pt(100)are identified as the most active HPRR catalysts among the studied metal surfaces,although they still experience a significant overpotential.The scaling relationship betweenΔ_(GHOO*)andΔ_(GHO*)reveals a thermodynamic coupling of HPOR and HPRR,explaining their occurrence on Pt surfaces.These findings provide important insights and activity descriptors for both HPOR and HPRR,providing valuable guidance for the design of electrocatalysts in H_(2)O_(2)-related energy applications and fuel cells.展开更多
Photodetectors can convert light energy into electrical signals,so are widely used in photovoltaics,photon counting,monitoring,and imaging.Photodetectors are easy to prepare high-resolution photochips because of their...Photodetectors can convert light energy into electrical signals,so are widely used in photovoltaics,photon counting,monitoring,and imaging.Photodetectors are easy to prepare high-resolution photochips because of their small size unit integration.However,these photodetector units often exhibit poor photoelectric performance due to material defects and inadequate structures,which greatly limit the functions of devices.Designing modification strategies and micro-/nanostructures can compensate for defects,adjust the bandgap,and develop novel quantum structures,which consequently optimize photovoltaic units and revolutionize optoelectronic devices.Here,this paper aims to comprehensively elaborate on the surface/interface engineering scheme of micro-/nano-photodetectors.It starts from the fundamentals of photodetectors,such as principles,types,and parameters,and describes the influence of material selection,manufacturing techniques,and post-processing.Then,we analyse in detail the great influence of surface/interface engineering on the performance of photovoltaic devices,including surface/interface modification and micro-/nanostructural design.Finally,the applications and prospects of optoelectronic devices in various fields such as miniaturization of electronic devices,robotics,and human–computer interaction are shown.展开更多
In this study,polyacrylic acid(PAA)films were employed as a model system,and a series of PAA films with tunable water wettability was systematically prepared by varying molecular weight and curing temperature.Using at...In this study,polyacrylic acid(PAA)films were employed as a model system,and a series of PAA films with tunable water wettability was systematically prepared by varying molecular weight and curing temperature.Using attenuated total reflectance Fourier-transform infrared spectroscopy(ATR-FTIR),the molecular configurations of surface carboxyl groups(COOH),free carboxyl(COOH_(f))and hydrogen-bonded carboxyl(COOH_(HB),were directly correlated with the polar component of surface energy(γ^(s,p)).By decomposing theγ^(s,p)values of the PAA thin films as a sum of the contributions of COOH_(f)and COOH_(H B),the intrinsic polar component of surface energy of COOH_(H B)(γ_(H B)^(s,p*))was quantified for the first time as 8.34 mN/m,significantly lower than that of COOH_(f)(γ_(f)^(s,p*)=34 mN/m).This result highlights that hydrogen bonding markedly reduces theγ^(s,p),providing a rational explanation for the relatively large water contact angle observed on PAA thin films.Furthermore,it establishes a thermodynamic basis for estimating the fraction of surface COOH_(H B)groups(f H B)from wettability measurements.Further extension of the model to carboxyl-terminated self-assembled monolayers(COOH-SAMs)revealed that surface COOH density(ΣCOOH)critically regulates wetting behavior:whenΣCOOH ranges from 4.30 to 5.25 nm^(-2),COOH groups predominantly exist in a free state and facilitate effective hydration layers,thereby promoting superhydrophilicity.Overall,this study not only establishes a unified thermodynamic framework linking surface COOH configurations to macroscopic wettability,but also validates its universality by extending it to COOH-SAMs systems,thereby providing a unified theoretical framework for the controllable design of hydrophilicity in various COOH-functionalized surfaces.展开更多
BACKGROUND Dry eye disease(DED)is a multifactorial ocular surface disorder with rising prevalence.It is closely related to systemic health and psychological factors,such as sleep and mood disorders,which significantly...BACKGROUND Dry eye disease(DED)is a multifactorial ocular surface disorder with rising prevalence.It is closely related to systemic health and psychological factors,such as sleep and mood disorders,which significantly impact the quality of life of patients.AIM To explore the correlations between ocular surface function,sleep quality,and anxiety/depression in patients with DED.METHODS This was a cross-sectional investigative study that included 358 patients with DED between January 2022 and January 2025.Ocular surface was assessed using the ocular surface disease index(OSDI),tear film break-up time,fluorescein staining score,and Schirmer I test.The Pittsburgh Sleep Quality Index(PSQI),Self-Rating Anxiety Scale(SAS),and Self-Rating Depression Scale(SDS)were used to evaluate sleep quality and anxiety/depression levels.Correlation and linear regression analyses were used to explore the relationships.RESULTS The mean PSQI score of the patients was 9.94±2.18;the mean SAS score was 47.30±4.90,and the mean SDS score was 50.08±5.52.These suggested a prevalence of sleep and psychological abnormalities.There was a significant correlation between the indicators of ocular surface function(OSDI,tear film break-up time,fluorescein staining,and Schirmer I test)and PSQI,SAS,and SDS scores(P<0.05).Moreover,multiple regression revealed that age≥50 years(β=1.55,P=0.029),PSQI scores(β=0.58,P<0.001),SAS scores(β=0.17,P=0.017),and SDS scores(β=0.15,P=0.019)were independent predictors of the OSDI scores.CONCLUSION Ocular surface function in patients with DED is closely related to sleep quality and anxiety/depression,emphasizing the need for holistic clinical management.展开更多
The atmospheric surface layer of the tropical coastal ocean is commonly very unstable and experiences weakwind conditions.How the latent(LE)and sensible(H)heat fluxes behave under such conditions are unclear because o...The atmospheric surface layer of the tropical coastal ocean is commonly very unstable and experiences weakwind conditions.How the latent(LE)and sensible(H)heat fluxes behave under such conditions are unclear because of the lack of observation stations in the tropics.Thus,this study aims to analyze LE and H and the microclimate parameters influencing them.The authors deployed an eddy covariance system in a tropical coastal region for seven months.The microclimate parameters investigated were wind speed(U),vapor pressure deficit(Δe),temperature difference(ΔT),wind-vapor pressure deficit(UΔe),wind-temperature difference(UΔT),and atmospheric stability(z/L),where z is height and L is the Monin–Obukhov length.On the daily time scale,the results show that LE was more associated with U thanΔe,while H was more related toΔT than U.Cross-wavelet analysis revealed the strong coherence in the LE-U relationship for periods between one and two days,and for H–ΔT,0.5 to 1 day.Correlation and regression analyses confirmed the time series analyses results,where strong positive correlation coefficients(r)were obtained between LE and U(r=0.494)and H andΔT(r=0.365).Compared to other water bodies,the transfer coefficient of moisture(CE N)was found to be small(=0.40×10^(-3))and independent of stability;conversely,the transfer coefficient of heat(CH N)was closer to literature values(=1.00×10^(-3))and a function of stability.展开更多
Undesired ice accumulation on infrastructure and transportation systems leads to catastrophic events and significant economic losses.Although various anti-icing surfaces with photothermal effects can initially prevent...Undesired ice accumulation on infrastructure and transportation systems leads to catastrophic events and significant economic losses.Although various anti-icing surfaces with photothermal effects can initially prevent icing,any thawy droplets remaining on the horizontal surface can quickly re-freezing once the light diminishes.To address these challenges,we have developed a self-draining slippery surface(SDSS)that enables the thawy droplets to self-remove on the horizontal surface,thereby facilitating real-time anti-icing with the aid of sunlight(100 m W cm^(-2)).This is achieved by sandwiching a thin pyroelectric layer between slippery surface and photothermal film.Due to the synergy between the photothermal and pyroelectric layers,the SDSS not only maintains a high surface temperature of 19.8±2.2℃at the low temperature(-20.0±1.0℃),but also generates amount of charge through thermoelectric coupling.Thus,as cold droplets dropped on the SDSS,electrostatic force pushes the droplets off the charged surface because of the charge transfer mechanism.Even if the surface freezes overnight,the ice can melt and drain off the SDSS within 10 min of exposure to sunlight at-20.0±1.0℃,leaving a clean surface.This work provides a new perspective on the anti-icing system in the real-world environments.展开更多
Global warming induced by increased CO_(2) has caused marked changes in the ocean.Previous estimates of ocean salinity change in response to global warming have considerable ambiguity,largely attributable to the diver...Global warming induced by increased CO_(2) has caused marked changes in the ocean.Previous estimates of ocean salinity change in response to global warming have considerable ambiguity,largely attributable to the diverse sensitivities of surface fluxes.This study utilizes data from the Flux-Anomaly-Forced Model Intercomparison Project to investigate how ocean salinity responds to perturbations of surface fluxes.The findings indicate the emergence of a sea surface salinity(SSS)dipole pattern predominantly in the North Atlantic and Pacific fresh pools,driven by surface flux perturbations.This results in an intensification of the“salty gets saltier and fresh gets fresher”SSS pattern across the global ocean.The spatial pattern amplification(PA)of SSS under global warming is estimated to be approximately 11.5%,with surface water flux perturbations being the most significant contributor to salinity PA,accounting for 8.1% of the change after 70 years in experiments since pre-industrial control(piControl).Notably,the zonal-depth distribution of salinity in the upper ocean exhibits lighter seawater above the denser water,with bowed isopycnals in the upper 400 m.This stable stratification inhibits vertical mixing of salinity and temperature.In response to the flux perturbations,there is a strong positive feedback due to consequent freshening.It is hypothesized that under global warming,an SSS amplification of 7.2%/℃ and a mixed-layer depth amplification of 12.5%/℃ will occur in the global ocean.It suggests that the salinity effect can exert a more stable ocean to hinder the downward transfer of heat,which provides positive feedback to future global warming.展开更多
Human activities have significantly impacted the land surface temperature(LST),endangering human health;however,the relationship between these two factors has not been adequately quantified.This study comprehensively ...Human activities have significantly impacted the land surface temperature(LST),endangering human health;however,the relationship between these two factors has not been adequately quantified.This study comprehensively constructs a Human Activity Intensity(HAI)index and employs the Maximal Information Coefficient,four-quadrant model,and XGBoostSHAP model to investigate the spatiotemporal relationship and influencing factors of HAI-LST in the Yellow River Basin(YRB)from 2000 to 2020.The results indicated that from 2000 to 2020,as HAI and LST increased,the static HAI-LST relationship in the YRB showed a positive correlation that continued to strengthen.This dynamic relationship exhibited conflicting development,with the proportion of coordinated to conflicting regions shifting from 1:4 to 1:2,indicating a reduction in conflict intensity.Notably,only the degree of conflict in the source area decreased significantly,whereas it intensified in the upper and lower reaches.The key factors influencing the HAI-LST relationship include fractional vegetation cover,slope,precipitation,and evapotranspiration,along with region-specific factors such as PM_(2.5),biodiversity,and elevation.Based on these findings,region-specific ecological management strategies have been proposed to mitigate conflict-prone areas and alleviate thermal stress,thereby providing important guidance for promoting harmonious development between humans and nature.展开更多
The Arno River Basin(Central Italy)is affected by a considerable anthropogenic pressure due to the presence of large cities and widespread industrial and agricultural practices.In this work,26 water samples from the A...The Arno River Basin(Central Italy)is affected by a considerable anthropogenic pressure due to the presence of large cities and widespread industrial and agricultural practices.In this work,26 water samples from the Arno River and its main tributaries were analyzed to assess the water pollution status.The geochemical composition of the Arno River changes from the source(dominated by a Ca-HCO_(3) facies)to the mouth(where a Na-Cl(SO4)chemistry prevails)with an increasing quality deterioration,as suggested by the Chemical Water Quality Index,due to anthropogenic contributions and seawater intrusion before flowing into the Ligurian Sea.The Ombrone and Usciana tributaries introduce anthropogenic pollutants into the Arno River,whilst Elsa tributary supplies significant contents of geogenic sulfate.The concentrations of dissolved nitrate and nitrite(up to 63 and 9 mg/L,respectively)and the respective isotopic values of𝛿15N and𝛿18O were also determined to understand origin and fate of the N-species in the Arno River Basin surface waters.The combined application of𝛿15N-NO_(3) and𝛿18O-NO_(3) and N-source apportionment modelling allowed the identification of soil organic nitrogen and sewage and domestic wastes as primary sources for dissolved NO_(3)-.The𝛿15N-NO_(2) and𝛿18O-NO_(2) values suggest that the nitrification process affects the ARB waters,thus controlling the abundances and proportion of the N-species.Our work indicates that additional efforts are needed to improve management strategies to reduce the release of nitrogenated species to the surface waters of the Arno River Basin,since little progress has been made from the early 2000s.展开更多
The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising c...The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising candidates due to their built-in electric fields,ultrafast photocarrier separation,and tunable bandgaps,defect states limit their performance.Therefore,the modulation of the optoelectronic properties in such heterostructures is imperative.Surface charge transfer doping(SCTD)has emerged as a promising strategy for non-destructive modulation of electronic and optoelectronic characteristics in two-dimensional materials.In this work,we demonstrate the construction of high-performance p-i-n vertical heterojunction photodetectors through SCTD of MoTe_(2)/ReS_(2)heterostructure using p-type F_(4)-TCNQ.Systematic characterization reveals that the interfacial doping process effectively amplifies the built-in electric field,enhancing photogenerated carrier separation efficiency.Compared to the pristine heterojunction device,the doped photodetector exhibits remarkable visible to nearinfrared(635-1064 nm)performance.Particularly under 1064 nm illumination at zero bias,the device achieves a responsivity of 2.86 A/W and specific detectivity of 1.41×10^(12)Jones.Notably,the external quantum efficiency reaches an exceptional value of 334%compared to the initial 11.5%,while maintaining ultrafast response characteristics with rise/fall times of 11.6/15.6μs.This work provides new insights into interface engineering through molecular doping for developing high-performance vd W optoelectronic devices.展开更多
As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This stud...As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This study prepared surface polarity-modified ACF using the heteroatom doping method.The modified ACF possessed a richer array of strongly polar oxygen/nitrogen-containing functional groups(primarily phenolic hydroxyl and lactone groups),a larger specific surface are1,and a more developed micropore structure.The adsorption capacities of ethanol for O-ACF and N-ACF were 4.110 mmol/g and 1.698 mmol/g,respectively,which were 11.3 times and 4.7 times those of unmodified ACF.This was a significant improvement over our previous work(0.363 mmol/g).The improvement of adsorption capacity for the N-ACF was mainly due to the higher specific surface are1,greater number of micropores(more adsorption sites)and abundant existence of defects,whereas,for O-ACF,the improvement mainly relied on the abundant presence of oxygen-containing functional groups on the surface.However,water had a negative effect on the adsorption of ethanol for the modified ACF due to competitive adsorption and the disappearance of capillary condensation.It was further revealed that the adsorption process of ethanol and water was quite different.It obeyed the linear driving force(LDF)model for ethanol adsorption,however,the intraparticle diffusion(IPD)model for water adsorption.展开更多
The preparation of immobilized enzyme with excellent performance is one of the difficulties that restrict the application of enzyme catalysis technology.Here,Candida rugosa lipase(CRL)was firstly adsorbed on the surfa...The preparation of immobilized enzyme with excellent performance is one of the difficulties that restrict the application of enzyme catalysis technology.Here,Candida rugosa lipase(CRL)was firstly adsorbed on the surface of magnetic zeolitic imidazolate framework-8(ZIF-8)nanospheres,which was further encapsulated with a mesoporous SiO_(2)nano-membrane formed by tetraethyl orthosilicate(TEOS)polycondensation.Consequently,lipase could be firmly immobilized on carrier surface by physical binding rather than chemical binding,which did not damage the active conformation of enzyme.There were mesopores on the silica nano-membrane,which could improve the accessibility of enzyme and its apparent catalytic activity.Moreover,silica membrane encapsulation could also improve the stability of enzyme,suggesting an effective enzyme immobilization strategy.It showed that TEOS amount and the encapsulation time had significant effects on the thickness of silica membrane and the enzyme activity.The analysis in enzyme activity and protein secondary structure showed that lipase encapsulated in silica membrane retained the active conformation to the greatest extent.Compared with the adsorbed lipase,the encapsulated lipase increased its thermostability by 3 times and resistance to chemical denaturants by 7 times.The relative enzyme activity remained around 80%after 8 repetitions,while the adsorbed lipase only remained at7.3%.展开更多
Superconducting elect rides have attracted growing attention for their potential to achieve high superconducting transition temperatures(T_(C))under pressure.However,many known elect rides are chemically reactive and ...Superconducting elect rides have attracted growing attention for their potential to achieve high superconducting transition temperatures(T_(C))under pressure.However,many known elect rides are chemically reactive and unstable,making high-quality single-crystal growth,characterization,and measurements difficult,and most do not exhibit superconductivity at ambient pressure.In contrast,La_(3) In stands out for its ambient-pressure superconductivity(T_(C)∼9.4 K)and the availability of high-quality single crystals.Here,we investigate its low-energy electronic structure using angle-resolved photoemission spectroscopy and first-principles calculations.The bands near the Fermi energy(E_(F))are mainly derived from La 5d and In 5p orbitals.A saddle point is directly observed at the Brillouin zone(BZ)boundary,while a three-dimensional Van Hove singularity crosses E_(F) at the BZ corner.First-principles calculations further reveal topological Dirac surface states within the bulk energy gap above E_(F).The coexistence of a high density of states and in-gap topological surface states near𝐸F suggests that La3In offers a promising platform for tuning superconductivity and exploring possible topological superconducting phases through doping or external pressure.展开更多
The application of silicon in lithium-ion batteries has been impaired by the low conductivity and large volume expansion.Herein,we develop a facile“surface amination”strategy to successfully encapsulate Si nanoparti...The application of silicon in lithium-ion batteries has been impaired by the low conductivity and large volume expansion.Herein,we develop a facile“surface amination”strategy to successfully encapsulate Si nanoparticles within the ZIF-8-derived N-doped carbon matrix.The amino group-containing organosilica serves as the linking agent between Si nanoparticles and Zn2+and facilitates the coating of the ZIF-8 layer on the Si nanoparticles.This in turn induces the construction of N-doped carbon matrix encapsu-lated Si nanoparticles(NH2-Si@C)during the subsequent carbonization.With buffered volume change and increased conductivity,the rationally designed NH2-Si@C demonstrates a high reversible capacity(1494 mAh g^(-1)at 1 A g^(-1))and satisfactory rate performance(1062 mAh g^(-1)at 5 A g^(-1)).展开更多
Immunoglobulin Y(Ig Y)is an effective orally administered antibody used to protect against various intestinal pathogens,but which cannot tolerate the acidic gastric environment.In this study,Ig Y was microencapsulated...Immunoglobulin Y(Ig Y)is an effective orally administered antibody used to protect against various intestinal pathogens,but which cannot tolerate the acidic gastric environment.In this study,Ig Y was microencapsulated by alginate(ALG)and coated with chitooligosaccharide(COS).A response surface methodology was used to optimize the formulation,and a simulated gastrointestinal(GI)digestion(SGID)system to evaluate the controlled release of microencapsulated Ig Y.The microcapsule formulation was optimized as an ALG concentration of 1.56%(15.6 g/L),COS level of 0.61%(6.1 g/L),and Ig Y/ALG ratio of 62.44%(mass ratio).The microcapsules prepared following this formulation had an encapsulation efficiency of 65.19%,a loading capacity of 33.75%,and an average particle size of 588.75μm.Under this optimum formulation,the coating of COS provided a less porous and more continuous microstructure by filling the cracks on the surface,and thus the GI release rate of encapsulated Ig Y was significantly reduced.The release of encapsulated Ig Y during simulated gastric and intestinal digestion well fitted the zero-order and first-order kinetics functions,respectively.The microcapsule also allowed the Ig Y to retain 84.37%immune-activity after 4 h simulated GI digestion,significantly higher than that for unprotected Ig Y(5.33%).This approach could provide an efficient way to preserve Ig Y and improve its performance in the GI tract.展开更多
In Na-ion batteries,O3-type layered oxide cathode materials encounter challenges such as particle cracking,oxygen loss,electrolyte side reactions,and multi-phase transitions during the charge/discharge process.This st...In Na-ion batteries,O3-type layered oxide cathode materials encounter challenges such as particle cracking,oxygen loss,electrolyte side reactions,and multi-phase transitions during the charge/discharge process.This study focuses on surface coating with NiTiO_(3) achieved via secondary heat treatment using a coating precursor and the surface material.Through in-situ x-ray diffraction(XRD)and differential electrochemical mass spectrometry(DEMS),along with crystal structure characterizations of post-cycling materials,it was determined that the NiTiO_(3) coating layer facilitates the formation of a stable lattice structure,effectively inhibiting lattice oxygen loss and reducing side reaction with the electrolyte.This enhancement in cycling stability was evidenced by a capacity retention of approximately 74%over 300 cycles at 1 C,marking a significant 30%improvement over the initial sample.Furthermore,notable advancements in rate performance were observed.Experimental results indicate that a stable and robust surface structure substantially enhances the overall stability of the bulk phase,presenting a novel approach for designing layered oxide cathodes with higher energy density.展开更多
Fe single-atom catalysts(Fe-SACs)have been extensively studied as a highly efficient electrocatalyst toward the oxygen reduction reaction(ORR).Nonetheless,they suffer from stability issue induced by dissolution of Fe ...Fe single-atom catalysts(Fe-SACs)have been extensively studied as a highly efficient electrocatalyst toward the oxygen reduction reaction(ORR).Nonetheless,they suffer from stability issue induced by dissolution of Fe metal center and the OH^(−)blocking.Herein,a surface molecular engineering strategy is developed by usingβ-cyclodextrins(CDs)as a localized molecular encapsulation.The CD-modified Fe-SAC(Fe-SNC-β-CD)shows obviously improved activity toward the ORR with 0.90 V,4.10 and 4.09 mA cm^(-2)for E_(1/2),J_(0)and Jk0.9,respectively.Meanwhile,the Fe-SNC-β-CD shows the excellent long-term stability against aggressive stress and the poisoning.It is confirmed through electrochemical investigation that modification ofβ-CD can,on one hand,regulate the atomic Fe coordination chemistry through the interaction between the CD and FeN_(x) moiety,while on the other mitigate the strong adsorption of OH^(−)and function as protective barrier against the poisoning molecules leading to enhanced ORR activity and stability for the Fe-SACs.The molecular encapsulation strategy demonstrates the uniqueness of post-pyrolysis surface molecular engineering for the design of single-atom catalyst.展开更多
The surface dielectric barrier discharge （SDBD） plasma actuator has shown great promise as an aerodynamic flow control device. In this paper, the encapsulated electrode width of a SDBD actuator is changed to study t...The surface dielectric barrier discharge （SDBD） plasma actuator has shown great promise as an aerodynamic flow control device. In this paper, the encapsulated electrode width of a SDBD actuator is changed to study the airflow acceleration behavior. The effects of encapsulated electrode width on the actuator performance are experimentally investigated by measuring the dielectric layer surface potential, time-averaged ionic wind velocity and thrust force. Experimental results show that the airflow velocity and thrust force increase with the encapsulated electrode width. The results can be attributed to the distinct plasma distribution at different encapsulated electrode widths.展开更多
In this work,the influences of surface layer slurry at different temperatures(10℃,14℃,18℃,22℃)on wax patterns deformation,shrinkage,slurry coating characteristics,and the surface quality of the casting were invest...In this work,the influences of surface layer slurry at different temperatures(10℃,14℃,18℃,22℃)on wax patterns deformation,shrinkage,slurry coating characteristics,and the surface quality of the casting were investigated by using a single factor variable method.The surface morphologies of the shell molds produced by different temperatures of the surface(first)layer slurries were observed via electron microscopy.Furthermore,the microscopic composition of these shell molds was obtained by EDS,and the osmotic effect of the slurry on the wax patterns at different temperatures was also assessed by the PZ-200 Contact Angle detector.The forming reasons for the surface cracks and holes of thick and large ZTC4 titanium alloy by investment casting were analyzed.The experimental results show that the surface of the shell molds prepared by the surface layer slurry with a low temperature exhibits noticeable damage,which is mainly due to the poor coating performance and the serious expansion and contraction of wax pattern at low temperatures.The second layer shell material(SiO_(2),Al_(2)O_(3))immerses into the crack area of the surface layer,contacts and reacts with the molten titanium to form surface cracks and holes in the castings.With the increase of the temperature of surface layer slurry,the damage to the shell surface tends to weaken,and the composition of the shell molds'surface becomes more uniform with less impurities.The results show that the surface layer slurry at 22℃is evenly coated on the surface of the wax patterns with appropriate thickness,and there is no surface shell mold rupture caused by sliding slurry after sand leaching.The surface layer slurry temperature is consistent with the wax pattern temperature and the workshop temperature,so there is no damage of the surface layer shell caused by expansion and contraction.Therefore,the shell mold prepared by the surface layer slurry at this temperature has good integrity,isolating the contact between the low inert shell material and the titanium liquid effectively,and the ZTC4 titanium alloy cylinder casting prepared by this shell mold is smooth,without cracks and holes.展开更多
基金financial support from projects of the National Natural Science Foundation of China(Nos.22104159,22174164)Guangdong Basic and Applied Basic Research Foundation(Nos.2023A1515011632,2024B1515020070)。
文摘Hydrogen-bonded framework(HOF) offers an attractive platform to encapsulate enzymes and stabilize their conformation,due to the advantages of mild synthesis conditions,tailorable pore structure,and backbone biocompatibility.However,the efficiency of this HOF approach relies on the interfacial interactions between enzyme vip and the ligand precursors,limiting its adaptability to enzymes with varying surface chemistry property.In this study,we report a site-specific surface modification strategy to positively tailor the enzyme surface charge,facilitating the biomimetic encapsulation of enzymes within HOF in situ.Both experimental results and computational simulation reveal that site-specific amination of enzyme surface's acidic residues contributes to the interfacial accumulation of carboxylic ligand precursors in aqueous solutions via synergistic electrostatic and hydrogen bonding interactions.This substantially facilitates the in situ growth of porous HOF surrounding the aminated enzyme biotemplates,with up to 100% enzyme loading efficiency.The resultant hydrogen-bonded biohybrid framework(HBF) retains high biocatalytic functions while exhibiting exceptional stability under harsh conditions.By leveraging the marked catalytic activity of GOx-NH_(2)@HBF-1 and a H_(2)O_(2)-sensitive QD,a highly sensitive glucose fluorescence sensor is fabricated with a wide linear range(5-2000 μmol/L) and a low quantification limit of 5 μmol/L.This work presents a simple yet effective enzyme surface engineering approach for integrating enzyme into HOF,opening new avenues for the construction of multifunctional HOF biocomposites.
基金Supported by the Shanxi Province Grant(202203021212007,2023SHB003).
文摘Hydrogen peroxide(H_(2)O_(2))oxidation and reduction reactions(HPOR/HPRR)are pivotal in various innovative electrochemical energy conversion devices.A comprehensive understanding of these mechanisms is critical for catalyst design and performance improvement in these applications.In this work,we systematically investigate the HPOR/HPRR mechanisms on low-index Pt surfaces,specifically Pt(111),Pt(100)and Pt(110),through density functional theory(DFT)calculations combined with the computational hydrogen electrode(CHE)model.For HPOR,all the low-index Pt surfaces exhibit a unified potential-determining step(PDS)involving the electrochemical oxidation of hydroperoxyl intermediates(HOO*).The binding free energy of HOO*(Δ_(GHOO*))emerges as an activity descriptor,with Pt(110)exhibiting the highest HPOR activity.The HPRR mechanism follows a chem-electrochemical(C-EC)pathway.The rate-determining step(RDS)of HPRR is either the cleavage of the HO-OH bond(chemical)or the reduction of HO(electrochemical),depending on their respective activation energies.These activation energies are functions of the HO*binding free energy,Δ_(GHO*),establishingΔ_(GHO*)as the descriptor for HPRR activity prediction.Pt(111)and Pt(100)are identified as the most active HPRR catalysts among the studied metal surfaces,although they still experience a significant overpotential.The scaling relationship betweenΔ_(GHOO*)andΔ_(GHO*)reveals a thermodynamic coupling of HPOR and HPRR,explaining their occurrence on Pt surfaces.These findings provide important insights and activity descriptors for both HPOR and HPRR,providing valuable guidance for the design of electrocatalysts in H_(2)O_(2)-related energy applications and fuel cells.
文摘Photodetectors can convert light energy into electrical signals,so are widely used in photovoltaics,photon counting,monitoring,and imaging.Photodetectors are easy to prepare high-resolution photochips because of their small size unit integration.However,these photodetector units often exhibit poor photoelectric performance due to material defects and inadequate structures,which greatly limit the functions of devices.Designing modification strategies and micro-/nanostructures can compensate for defects,adjust the bandgap,and develop novel quantum structures,which consequently optimize photovoltaic units and revolutionize optoelectronic devices.Here,this paper aims to comprehensively elaborate on the surface/interface engineering scheme of micro-/nano-photodetectors.It starts from the fundamentals of photodetectors,such as principles,types,and parameters,and describes the influence of material selection,manufacturing techniques,and post-processing.Then,we analyse in detail the great influence of surface/interface engineering on the performance of photovoltaic devices,including surface/interface modification and micro-/nanostructural design.Finally,the applications and prospects of optoelectronic devices in various fields such as miniaturization of electronic devices,robotics,and human–computer interaction are shown.
文摘In this study,polyacrylic acid(PAA)films were employed as a model system,and a series of PAA films with tunable water wettability was systematically prepared by varying molecular weight and curing temperature.Using attenuated total reflectance Fourier-transform infrared spectroscopy(ATR-FTIR),the molecular configurations of surface carboxyl groups(COOH),free carboxyl(COOH_(f))and hydrogen-bonded carboxyl(COOH_(HB),were directly correlated with the polar component of surface energy(γ^(s,p)).By decomposing theγ^(s,p)values of the PAA thin films as a sum of the contributions of COOH_(f)and COOH_(H B),the intrinsic polar component of surface energy of COOH_(H B)(γ_(H B)^(s,p*))was quantified for the first time as 8.34 mN/m,significantly lower than that of COOH_(f)(γ_(f)^(s,p*)=34 mN/m).This result highlights that hydrogen bonding markedly reduces theγ^(s,p),providing a rational explanation for the relatively large water contact angle observed on PAA thin films.Furthermore,it establishes a thermodynamic basis for estimating the fraction of surface COOH_(H B)groups(f H B)from wettability measurements.Further extension of the model to carboxyl-terminated self-assembled monolayers(COOH-SAMs)revealed that surface COOH density(ΣCOOH)critically regulates wetting behavior:whenΣCOOH ranges from 4.30 to 5.25 nm^(-2),COOH groups predominantly exist in a free state and facilitate effective hydration layers,thereby promoting superhydrophilicity.Overall,this study not only establishes a unified thermodynamic framework linking surface COOH configurations to macroscopic wettability,but also validates its universality by extending it to COOH-SAMs systems,thereby providing a unified theoretical framework for the controllable design of hydrophilicity in various COOH-functionalized surfaces.
文摘BACKGROUND Dry eye disease(DED)is a multifactorial ocular surface disorder with rising prevalence.It is closely related to systemic health and psychological factors,such as sleep and mood disorders,which significantly impact the quality of life of patients.AIM To explore the correlations between ocular surface function,sleep quality,and anxiety/depression in patients with DED.METHODS This was a cross-sectional investigative study that included 358 patients with DED between January 2022 and January 2025.Ocular surface was assessed using the ocular surface disease index(OSDI),tear film break-up time,fluorescein staining score,and Schirmer I test.The Pittsburgh Sleep Quality Index(PSQI),Self-Rating Anxiety Scale(SAS),and Self-Rating Depression Scale(SDS)were used to evaluate sleep quality and anxiety/depression levels.Correlation and linear regression analyses were used to explore the relationships.RESULTS The mean PSQI score of the patients was 9.94±2.18;the mean SAS score was 47.30±4.90,and the mean SDS score was 50.08±5.52.These suggested a prevalence of sleep and psychological abnormalities.There was a significant correlation between the indicators of ocular surface function(OSDI,tear film break-up time,fluorescein staining,and Schirmer I test)and PSQI,SAS,and SDS scores(P<0.05).Moreover,multiple regression revealed that age≥50 years(β=1.55,P=0.029),PSQI scores(β=0.58,P<0.001),SAS scores(β=0.17,P=0.017),and SDS scores(β=0.15,P=0.019)were independent predictors of the OSDI scores.CONCLUSION Ocular surface function in patients with DED is closely related to sleep quality and anxiety/depression,emphasizing the need for holistic clinical management.
基金supported by a PETRONAS-Academia Collabora-tion Dialogue 2022 Grant[Grant number PACD 2022]from PETRONAS Research Sdn.Bhd。
文摘The atmospheric surface layer of the tropical coastal ocean is commonly very unstable and experiences weakwind conditions.How the latent(LE)and sensible(H)heat fluxes behave under such conditions are unclear because of the lack of observation stations in the tropics.Thus,this study aims to analyze LE and H and the microclimate parameters influencing them.The authors deployed an eddy covariance system in a tropical coastal region for seven months.The microclimate parameters investigated were wind speed(U),vapor pressure deficit(Δe),temperature difference(ΔT),wind-vapor pressure deficit(UΔe),wind-temperature difference(UΔT),and atmospheric stability(z/L),where z is height and L is the Monin–Obukhov length.On the daily time scale,the results show that LE was more associated with U thanΔe,while H was more related toΔT than U.Cross-wavelet analysis revealed the strong coherence in the LE-U relationship for periods between one and two days,and for H–ΔT,0.5 to 1 day.Correlation and regression analyses confirmed the time series analyses results,where strong positive correlation coefficients(r)were obtained between LE and U(r=0.494)and H andΔT(r=0.365).Compared to other water bodies,the transfer coefficient of moisture(CE N)was found to be small(=0.40×10^(-3))and independent of stability;conversely,the transfer coefficient of heat(CH N)was closer to literature values(=1.00×10^(-3))and a function of stability.
基金supported by the National Natural Science Foundation of China(52273101,51922018,and 21875011)the Fundamental Research Funds for the Central Universities(KG21015201 and KG21020801)China Postdoctoral Science Foundation(2025M77422)。
文摘Undesired ice accumulation on infrastructure and transportation systems leads to catastrophic events and significant economic losses.Although various anti-icing surfaces with photothermal effects can initially prevent icing,any thawy droplets remaining on the horizontal surface can quickly re-freezing once the light diminishes.To address these challenges,we have developed a self-draining slippery surface(SDSS)that enables the thawy droplets to self-remove on the horizontal surface,thereby facilitating real-time anti-icing with the aid of sunlight(100 m W cm^(-2)).This is achieved by sandwiching a thin pyroelectric layer between slippery surface and photothermal film.Due to the synergy between the photothermal and pyroelectric layers,the SDSS not only maintains a high surface temperature of 19.8±2.2℃at the low temperature(-20.0±1.0℃),but also generates amount of charge through thermoelectric coupling.Thus,as cold droplets dropped on the SDSS,electrostatic force pushes the droplets off the charged surface because of the charge transfer mechanism.Even if the surface freezes overnight,the ice can melt and drain off the SDSS within 10 min of exposure to sunlight at-20.0±1.0℃,leaving a clean surface.This work provides a new perspective on the anti-icing system in the real-world environments.
基金supported by the Laoshan Laboratory[grant number LSKJ202202403]the National Natural Science Foundation of China[grant number 42030410]+1 种基金additionally supported by the Startup Foundation for Introducing Talent of NUISTJiangsu Innovation Research Group[grant number JSSCTD202346]。
文摘Global warming induced by increased CO_(2) has caused marked changes in the ocean.Previous estimates of ocean salinity change in response to global warming have considerable ambiguity,largely attributable to the diverse sensitivities of surface fluxes.This study utilizes data from the Flux-Anomaly-Forced Model Intercomparison Project to investigate how ocean salinity responds to perturbations of surface fluxes.The findings indicate the emergence of a sea surface salinity(SSS)dipole pattern predominantly in the North Atlantic and Pacific fresh pools,driven by surface flux perturbations.This results in an intensification of the“salty gets saltier and fresh gets fresher”SSS pattern across the global ocean.The spatial pattern amplification(PA)of SSS under global warming is estimated to be approximately 11.5%,with surface water flux perturbations being the most significant contributor to salinity PA,accounting for 8.1% of the change after 70 years in experiments since pre-industrial control(piControl).Notably,the zonal-depth distribution of salinity in the upper ocean exhibits lighter seawater above the denser water,with bowed isopycnals in the upper 400 m.This stable stratification inhibits vertical mixing of salinity and temperature.In response to the flux perturbations,there is a strong positive feedback due to consequent freshening.It is hypothesized that under global warming,an SSS amplification of 7.2%/℃ and a mixed-layer depth amplification of 12.5%/℃ will occur in the global ocean.It suggests that the salinity effect can exert a more stable ocean to hinder the downward transfer of heat,which provides positive feedback to future global warming.
基金Shanxi Province Graduate Research Practice Innovation Project,No.2023KY465Project on the Reform of Graduate Education and Teaching in Shanxi Province,No.2021YJJG146+1 种基金Research Project of Shanxi Provincial Cultural Relics Bureau,No.22-8-14-1400-119National Key R&D Program of China,No.2021YFB3901300。
文摘Human activities have significantly impacted the land surface temperature(LST),endangering human health;however,the relationship between these two factors has not been adequately quantified.This study comprehensively constructs a Human Activity Intensity(HAI)index and employs the Maximal Information Coefficient,four-quadrant model,and XGBoostSHAP model to investigate the spatiotemporal relationship and influencing factors of HAI-LST in the Yellow River Basin(YRB)from 2000 to 2020.The results indicated that from 2000 to 2020,as HAI and LST increased,the static HAI-LST relationship in the YRB showed a positive correlation that continued to strengthen.This dynamic relationship exhibited conflicting development,with the proportion of coordinated to conflicting regions shifting from 1:4 to 1:2,indicating a reduction in conflict intensity.Notably,only the degree of conflict in the source area decreased significantly,whereas it intensified in the upper and lower reaches.The key factors influencing the HAI-LST relationship include fractional vegetation cover,slope,precipitation,and evapotranspiration,along with region-specific factors such as PM_(2.5),biodiversity,and elevation.Based on these findings,region-specific ecological management strategies have been proposed to mitigate conflict-prone areas and alleviate thermal stress,thereby providing important guidance for promoting harmonious development between humans and nature.
文摘The Arno River Basin(Central Italy)is affected by a considerable anthropogenic pressure due to the presence of large cities and widespread industrial and agricultural practices.In this work,26 water samples from the Arno River and its main tributaries were analyzed to assess the water pollution status.The geochemical composition of the Arno River changes from the source(dominated by a Ca-HCO_(3) facies)to the mouth(where a Na-Cl(SO4)chemistry prevails)with an increasing quality deterioration,as suggested by the Chemical Water Quality Index,due to anthropogenic contributions and seawater intrusion before flowing into the Ligurian Sea.The Ombrone and Usciana tributaries introduce anthropogenic pollutants into the Arno River,whilst Elsa tributary supplies significant contents of geogenic sulfate.The concentrations of dissolved nitrate and nitrite(up to 63 and 9 mg/L,respectively)and the respective isotopic values of𝛿15N and𝛿18O were also determined to understand origin and fate of the N-species in the Arno River Basin surface waters.The combined application of𝛿15N-NO_(3) and𝛿18O-NO_(3) and N-source apportionment modelling allowed the identification of soil organic nitrogen and sewage and domestic wastes as primary sources for dissolved NO_(3)-.The𝛿15N-NO_(2) and𝛿18O-NO_(2) values suggest that the nitrification process affects the ARB waters,thus controlling the abundances and proportion of the N-species.Our work indicates that additional efforts are needed to improve management strategies to reduce the release of nitrogenated species to the surface waters of the Arno River Basin,since little progress has been made from the early 2000s.
基金financial support from 2024 Domestic Visiting Scholar Program for Teachers'Professional Development in Universities(Grant No.FX2024022)National Natural Science Foundation of China(Grant No.61904043)。
文摘The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising candidates due to their built-in electric fields,ultrafast photocarrier separation,and tunable bandgaps,defect states limit their performance.Therefore,the modulation of the optoelectronic properties in such heterostructures is imperative.Surface charge transfer doping(SCTD)has emerged as a promising strategy for non-destructive modulation of electronic and optoelectronic characteristics in two-dimensional materials.In this work,we demonstrate the construction of high-performance p-i-n vertical heterojunction photodetectors through SCTD of MoTe_(2)/ReS_(2)heterostructure using p-type F_(4)-TCNQ.Systematic characterization reveals that the interfacial doping process effectively amplifies the built-in electric field,enhancing photogenerated carrier separation efficiency.Compared to the pristine heterojunction device,the doped photodetector exhibits remarkable visible to nearinfrared(635-1064 nm)performance.Particularly under 1064 nm illumination at zero bias,the device achieves a responsivity of 2.86 A/W and specific detectivity of 1.41×10^(12)Jones.Notably,the external quantum efficiency reaches an exceptional value of 334%compared to the initial 11.5%,while maintaining ultrafast response characteristics with rise/fall times of 11.6/15.6μs.This work provides new insights into interface engineering through molecular doping for developing high-performance vd W optoelectronic devices.
基金supported by the National Key R&D Program of China(Nos.2022YFB4101500 and 2022YFE0209500)the National Natural Science Foundation of China(Nos.22276191 and 21976177)the Qinghai Province Air Pollution Assessment and Fine Management Support Project,and the University of Chinese Academy of Science.
文摘As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This study prepared surface polarity-modified ACF using the heteroatom doping method.The modified ACF possessed a richer array of strongly polar oxygen/nitrogen-containing functional groups(primarily phenolic hydroxyl and lactone groups),a larger specific surface are1,and a more developed micropore structure.The adsorption capacities of ethanol for O-ACF and N-ACF were 4.110 mmol/g and 1.698 mmol/g,respectively,which were 11.3 times and 4.7 times those of unmodified ACF.This was a significant improvement over our previous work(0.363 mmol/g).The improvement of adsorption capacity for the N-ACF was mainly due to the higher specific surface are1,greater number of micropores(more adsorption sites)and abundant existence of defects,whereas,for O-ACF,the improvement mainly relied on the abundant presence of oxygen-containing functional groups on the surface.However,water had a negative effect on the adsorption of ethanol for the modified ACF due to competitive adsorption and the disappearance of capillary condensation.It was further revealed that the adsorption process of ethanol and water was quite different.It obeyed the linear driving force(LDF)model for ethanol adsorption,however,the intraparticle diffusion(IPD)model for water adsorption.
基金the financial supports from the National Natural Science Foundation of China(Nos.22378093,21878065)Natural Science Foundation of Hebei Province,China(No.E2022201100)+2 种基金the Science and Technology Support Plan of Baoding City(No.2241ZF111)the Medical Science Foundation of Hebei University(No.2021A09)the Foundation of Affiliated Hospital of Hebei University(No.2021Z003)。
文摘The preparation of immobilized enzyme with excellent performance is one of the difficulties that restrict the application of enzyme catalysis technology.Here,Candida rugosa lipase(CRL)was firstly adsorbed on the surface of magnetic zeolitic imidazolate framework-8(ZIF-8)nanospheres,which was further encapsulated with a mesoporous SiO_(2)nano-membrane formed by tetraethyl orthosilicate(TEOS)polycondensation.Consequently,lipase could be firmly immobilized on carrier surface by physical binding rather than chemical binding,which did not damage the active conformation of enzyme.There were mesopores on the silica nano-membrane,which could improve the accessibility of enzyme and its apparent catalytic activity.Moreover,silica membrane encapsulation could also improve the stability of enzyme,suggesting an effective enzyme immobilization strategy.It showed that TEOS amount and the encapsulation time had significant effects on the thickness of silica membrane and the enzyme activity.The analysis in enzyme activity and protein secondary structure showed that lipase encapsulated in silica membrane retained the active conformation to the greatest extent.Compared with the adsorbed lipase,the encapsulated lipase increased its thermostability by 3 times and resistance to chemical denaturants by 7 times.The relative enzyme activity remained around 80%after 8 repetitions,while the adsorbed lipase only remained at7.3%.
基金supported by the National Natural Science Foundation of China(Grant Nos.12222413,12174443,12274459,and 12404266)the National Key R&D Program of China(Grant Nos.2023YFA1406500,2022YFA1403800,and 2022YFA1403103)+3 种基金the Natural Science Foundation of Shanghai (Grant No.23ZR1482200)the Natural Science Foundation of Ningbo (Grant No.2024J019)the Science Research Project of Hebei Education Department (Grant No.BJ2025060)the funding of Ningbo Yongjiang Talent Program。
文摘Superconducting elect rides have attracted growing attention for their potential to achieve high superconducting transition temperatures(T_(C))under pressure.However,many known elect rides are chemically reactive and unstable,making high-quality single-crystal growth,characterization,and measurements difficult,and most do not exhibit superconductivity at ambient pressure.In contrast,La_(3) In stands out for its ambient-pressure superconductivity(T_(C)∼9.4 K)and the availability of high-quality single crystals.Here,we investigate its low-energy electronic structure using angle-resolved photoemission spectroscopy and first-principles calculations.The bands near the Fermi energy(E_(F))are mainly derived from La 5d and In 5p orbitals.A saddle point is directly observed at the Brillouin zone(BZ)boundary,while a three-dimensional Van Hove singularity crosses E_(F) at the BZ corner.First-principles calculations further reveal topological Dirac surface states within the bulk energy gap above E_(F).The coexistence of a high density of states and in-gap topological surface states near𝐸F suggests that La3In offers a promising platform for tuning superconductivity and exploring possible topological superconducting phases through doping or external pressure.
基金supported by the Hainan Provincial Joint Project of Sanya Yazhou Bay Science and Technology City(No.2021JJLH0069)the Project of Sanya Yazhou Bay Science and Technology City(grant No SCKJ-JYRC-2023-55)the Hainan Provincial Natural Science Foundation of China(No.522CXTD516).
文摘The application of silicon in lithium-ion batteries has been impaired by the low conductivity and large volume expansion.Herein,we develop a facile“surface amination”strategy to successfully encapsulate Si nanoparticles within the ZIF-8-derived N-doped carbon matrix.The amino group-containing organosilica serves as the linking agent between Si nanoparticles and Zn2+and facilitates the coating of the ZIF-8 layer on the Si nanoparticles.This in turn induces the construction of N-doped carbon matrix encapsu-lated Si nanoparticles(NH2-Si@C)during the subsequent carbonization.With buffered volume change and increased conductivity,the rationally designed NH2-Si@C demonstrates a high reversible capacity(1494 mAh g^(-1)at 1 A g^(-1))and satisfactory rate performance(1062 mAh g^(-1)at 5 A g^(-1)).
基金Project supported by the National Key Research and Development Program of China(No.2018YFD0400305)the Modern Agro-industry Technology Research System of China(No.CARS-40-K26)the“One Belt and One Road”International Science and Technology Cooperation Program of Zhejiang,China(No.2019C04022)。
文摘Immunoglobulin Y(Ig Y)is an effective orally administered antibody used to protect against various intestinal pathogens,but which cannot tolerate the acidic gastric environment.In this study,Ig Y was microencapsulated by alginate(ALG)and coated with chitooligosaccharide(COS).A response surface methodology was used to optimize the formulation,and a simulated gastrointestinal(GI)digestion(SGID)system to evaluate the controlled release of microencapsulated Ig Y.The microcapsule formulation was optimized as an ALG concentration of 1.56%(15.6 g/L),COS level of 0.61%(6.1 g/L),and Ig Y/ALG ratio of 62.44%(mass ratio).The microcapsules prepared following this formulation had an encapsulation efficiency of 65.19%,a loading capacity of 33.75%,and an average particle size of 588.75μm.Under this optimum formulation,the coating of COS provided a less porous and more continuous microstructure by filling the cracks on the surface,and thus the GI release rate of encapsulated Ig Y was significantly reduced.The release of encapsulated Ig Y during simulated gastric and intestinal digestion well fitted the zero-order and first-order kinetics functions,respectively.The microcapsule also allowed the Ig Y to retain 84.37%immune-activity after 4 h simulated GI digestion,significantly higher than that for unprotected Ig Y(5.33%).This approach could provide an efficient way to preserve Ig Y and improve its performance in the GI tract.
基金Project supported by the National Key R&D Program of China (Grant No.2022YFB2402500)the National Natural Science Foundation of China (Grant Nos.52122214,92372116,and 52394174)+2 种基金Youth Innovation Promotion Association of the Chinese Academy of Sciences (Grant No.2020006)Jiangsu Province Carbon Peak and Neutrality Innovation Program (Industry tackling on prospect and key technology BE2022002-5)Guangxi Power Grid Project (Grant No.GXKJXM20210260)。
文摘In Na-ion batteries,O3-type layered oxide cathode materials encounter challenges such as particle cracking,oxygen loss,electrolyte side reactions,and multi-phase transitions during the charge/discharge process.This study focuses on surface coating with NiTiO_(3) achieved via secondary heat treatment using a coating precursor and the surface material.Through in-situ x-ray diffraction(XRD)and differential electrochemical mass spectrometry(DEMS),along with crystal structure characterizations of post-cycling materials,it was determined that the NiTiO_(3) coating layer facilitates the formation of a stable lattice structure,effectively inhibiting lattice oxygen loss and reducing side reaction with the electrolyte.This enhancement in cycling stability was evidenced by a capacity retention of approximately 74%over 300 cycles at 1 C,marking a significant 30%improvement over the initial sample.Furthermore,notable advancements in rate performance were observed.Experimental results indicate that a stable and robust surface structure substantially enhances the overall stability of the bulk phase,presenting a novel approach for designing layered oxide cathodes with higher energy density.
基金the National Natural Science Foundation of China(52171199)for the financial support.
文摘Fe single-atom catalysts(Fe-SACs)have been extensively studied as a highly efficient electrocatalyst toward the oxygen reduction reaction(ORR).Nonetheless,they suffer from stability issue induced by dissolution of Fe metal center and the OH^(−)blocking.Herein,a surface molecular engineering strategy is developed by usingβ-cyclodextrins(CDs)as a localized molecular encapsulation.The CD-modified Fe-SAC(Fe-SNC-β-CD)shows obviously improved activity toward the ORR with 0.90 V,4.10 and 4.09 mA cm^(-2)for E_(1/2),J_(0)and Jk0.9,respectively.Meanwhile,the Fe-SNC-β-CD shows the excellent long-term stability against aggressive stress and the poisoning.It is confirmed through electrochemical investigation that modification ofβ-CD can,on one hand,regulate the atomic Fe coordination chemistry through the interaction between the CD and FeN_(x) moiety,while on the other mitigate the strong adsorption of OH^(−)and function as protective barrier against the poisoning molecules leading to enhanced ORR activity and stability for the Fe-SACs.The molecular encapsulation strategy demonstrates the uniqueness of post-pyrolysis surface molecular engineering for the design of single-atom catalyst.
基金supported by National Natural Science Foundation of China(No.11175037)National Natural Science Foundation for Young Scientists of China(No.11305017)Special Fund for Theoretical Physics(No.11247239)
文摘The surface dielectric barrier discharge （SDBD） plasma actuator has shown great promise as an aerodynamic flow control device. In this paper, the encapsulated electrode width of a SDBD actuator is changed to study the airflow acceleration behavior. The effects of encapsulated electrode width on the actuator performance are experimentally investigated by measuring the dielectric layer surface potential, time-averaged ionic wind velocity and thrust force. Experimental results show that the airflow velocity and thrust force increase with the encapsulated electrode width. The results can be attributed to the distinct plasma distribution at different encapsulated electrode widths.
文摘In this work,the influences of surface layer slurry at different temperatures(10℃,14℃,18℃,22℃)on wax patterns deformation,shrinkage,slurry coating characteristics,and the surface quality of the casting were investigated by using a single factor variable method.The surface morphologies of the shell molds produced by different temperatures of the surface(first)layer slurries were observed via electron microscopy.Furthermore,the microscopic composition of these shell molds was obtained by EDS,and the osmotic effect of the slurry on the wax patterns at different temperatures was also assessed by the PZ-200 Contact Angle detector.The forming reasons for the surface cracks and holes of thick and large ZTC4 titanium alloy by investment casting were analyzed.The experimental results show that the surface of the shell molds prepared by the surface layer slurry with a low temperature exhibits noticeable damage,which is mainly due to the poor coating performance and the serious expansion and contraction of wax pattern at low temperatures.The second layer shell material(SiO_(2),Al_(2)O_(3))immerses into the crack area of the surface layer,contacts and reacts with the molten titanium to form surface cracks and holes in the castings.With the increase of the temperature of surface layer slurry,the damage to the shell surface tends to weaken,and the composition of the shell molds'surface becomes more uniform with less impurities.The results show that the surface layer slurry at 22℃is evenly coated on the surface of the wax patterns with appropriate thickness,and there is no surface shell mold rupture caused by sliding slurry after sand leaching.The surface layer slurry temperature is consistent with the wax pattern temperature and the workshop temperature,so there is no damage of the surface layer shell caused by expansion and contraction.Therefore,the shell mold prepared by the surface layer slurry at this temperature has good integrity,isolating the contact between the low inert shell material and the titanium liquid effectively,and the ZTC4 titanium alloy cylinder casting prepared by this shell mold is smooth,without cracks and holes.
