The retrospective study by Edwar et al reinforces the role of therapeutic penetrating keratoplasty(PK)as a vital intervention in severe,treatment-resistant infectious keratitis.In advanced cases—often complicated by ...The retrospective study by Edwar et al reinforces the role of therapeutic penetrating keratoplasty(PK)as a vital intervention in severe,treatment-resistant infectious keratitis.In advanced cases—often complicated by trauma,delayed presentation,and corneal perforation—PK restores globe integrity and provides limited visual recovery.However,its application is constrained by graft-related complications and donor shortages,particularly in low-resource settings.These limitations highlight the need for earlier,globe-sparing strategies to prevent progression and reduce surgical demand.Photoactivated chromophore for infectious keratitis-corneal collagen cross-linking(PACK-CXL)has emerged as a promising adjunct or alternative.With both antimicrobial and tissue-stabilizing effects,PACK-CXL may control infection and preserve corneal structure in earlier stages.A layered treatment framework that incorporates PACK-CXL as an initial intervention and reserves PK for refractory cases may help improve clinical outcomes.Further studies are needed to define their best use in practice.展开更多
Based on the characteristics of laser-induced surface ignition,energetic photosensitive films show promising potential to meet the ignition requirements of various energetic materials(EMs).In this study,DATNBI/ferric ...Based on the characteristics of laser-induced surface ignition,energetic photosensitive films show promising potential to meet the ignition requirements of various energetic materials(EMs).In this study,DATNBI/ferric alginate(DI/FeA),DI/cobalt alginate(DI/CoA),and DI/nickel alginate(DI/Ni A)films are fabricated by employing sodium alginate(SA)with a three-dimensional network structure as the film matrix,via ionic cross-linking of SA with Fe^(3+),Co^(2+),and Ni^(2+)ions.The study demonstrates that the ionic cross-linking enhances the hydrophobic performance of the films,with the water contact angle increasing from 82.1° to 123.5°.Concurrently,the films'near-infrared(NIR)light absorption improved.Furthermore,transition metal ions facilitate accelerated electron transfer,thereby catalyzing the thermal decomposition of DATNBI.Under 1064 nm laser irradiation,the DI/Fe A film exhibits exceptional combustion performance,with an ignition delay time as low as 76 ms.It successfully acts as an NIR laser ignition medium to initiate the self-sustained combustion of CL-20.This study demonstrates the synergistic realization of enhanced hydrophobicity,improved photosensitivity,and promoted catalytic decomposition through microstructural design of the material,providing new insights for the design of additive-free EMs in laser ignition applications.展开更多
Corn starch(CS)is a renewable,biodegradable polysaccharide valued for its film-forming ability,yet native CS films exhibit lowmechanical strength,highwater sensitivity,and limited thermal stability.This study improves...Corn starch(CS)is a renewable,biodegradable polysaccharide valued for its film-forming ability,yet native CS films exhibit lowmechanical strength,highwater sensitivity,and limited thermal stability.This study improves CS-based films by blending with poly(vinyl alcohol)(PVA)or glycerol(GLY)and using citric acid(CA)as a green,non-toxic cross-linker.Composite films were prepared by casting CS–PVA or CS-GLY with CA at 0%-0.20%(w/w of starch).The influence of CA on physicochemical,mechanical,optical,thermal,and water barrier properties was evaluated.CA crosslinking markedly enhanced the tensile strength,water resistance,and thermal stability of CS-PVA films while increasing transparency in CS–GLY films.At 0.20%CA,the composite achieved 34.99MPa tensile strength,reducedwater vapor permeability,andminimized water uptake.FTIR confirmed ester bond formation between CAand hydroxyl groups of CS,PVA,and GLY,whereas thermal analysis showed higher decomposition temperatures and lower weight loss in crosslinked films.Increasing CA levels also decreased opacity and improved light transmittance,indicating greater homogeneity and reduced crystallinity.This dual-polymer matrix combined with a natural crosslinking strategy provides a sustainable route to high-performance,biodegradable CS-based packaging materials.展开更多
LiMnxFe1-xPO_(4) is a promising cathode candidate due to its high security and the availability of a high 4.1 V operating voltage and high energy density.However,the poor electrochemical kinetics and structural instab...LiMnxFe1-xPO_(4) is a promising cathode candidate due to its high security and the availability of a high 4.1 V operating voltage and high energy density.However,the poor electrochemical kinetics and structural instability currently hinder its broader application.Herein,inspired by the hydrogen-bonded cross-linking and steric hindrance effect between short-chain polymer molecules(polyethylene glycol-400,PEG-400),the pomegranate-type LiMn_(0.5)Fe_(0.5)PO_(4)-0.5@C(P-LMFP@C)cathode materials with 3D ion/electron dual-conductive network structure were constructed through ball mill-assisted spray-drying method.The intermolecular effects of PEG-400 promote the spheroidization and uniform PEG coating of LMFP precursor,which prevents agglomeration during sintering.The 3D ion/electron dual-conductive network structure in P-LMFP@C accelerates the Li^(+)transport kinetics,improving the rate performance and cycling stability.As a result,the designed P-LMFP@C has remarkable electrochemical behavior,boasting excellent capacity retention(98%after 100 cycles at the 1C rate)and rate capability(91 mAh·g^(-1)at 20C).Such strategy introduces a novel window for designing high-performance olivine cathodes and offers compatibility with a range of energy storage materials for diverse applications.展开更多
AIM:To compare simultaneous corneal collagen cross-linking(CXL)with intracorneal ring segment(ICRS)implantation versus successive ICRS followed by CXL and detect the impact of the timing of CXL after ICRS implantation...AIM:To compare simultaneous corneal collagen cross-linking(CXL)with intracorneal ring segment(ICRS)implantation versus successive ICRS followed by CXL and detect the impact of the timing of CXL after ICRS implantation in the successive method.METHODS:This is a retrospective study of the records of three groups of patients.Group 1 of 28 patients were operated on with simultaneous ICRS implantation and CXL,group 2 of 32 patients had ICRS implantation followed by CXL after 1mo,and group 3 of 38 patients had ICRS implantation followed by CXL after 3mo.The three groups had follow-up visits after 6,12,and 24mo.RESULTS:The preoperative data,age,and gender differences among 3 groups revealed no significant differences.The postoperative spherical equivalent and best-corrected visual acuity were improved significantly in all groups compared to the baseline,which were more evident in groups 1 and 2.The differences between preoperative and postoperative mean values of mean of K readings(Km)and maximum K reading(Kmax)at 6mo were 4.66 and 4.1 D in group 1,4.43 and 4.64 D in group 2,but 3.2 and 3.4 D in group 3,respectively.The spherical aberrations and the vertical coma showed significant postoperative changes in all groups,and trefoil showed nonsignificant changes.CONCLUSION:Simultaneous and sequential ICRS implantation and CXL at 1mo has similar Km and Kmax better postoperative changes than when both surgeries were done at three-month intervals.展开更多
AIM:To investigate the response of the anterior and posterior corneal surface in femtosecond laser-assisted convex stromal lenticule addition keratoplasty(SLAK)combined with cross-linking(CXL)for treating keratoconus ...AIM:To investigate the response of the anterior and posterior corneal surface in femtosecond laser-assisted convex stromal lenticule addition keratoplasty(SLAK)combined with cross-linking(CXL)for treating keratoconus at the first 3mo of follow-up.METHODS:In this prospective observational study,20 eyes of 20 keratoconus patients who underwent SLAK combined with CXL were included.The morphological indices in keratometry and elevation data were recorded from the Sirius at baseline and 1 and 3mo postoperatively.The mean values of maximum keratometry(K_(max)),flat keratometry(K_(1)),and steep keratometry(K_(2))at the central,3-mm,5-mm,and 7-mm areas were measured from the curvature map.The changes in anterior and posterior corneal elevation under the best-fit sphere(BFS)radius at seven points horizontally of the center,3-mm,5-mm,and 7-mm area from the center at both nasal(N)and temporal(T)side were measured from elevation map.RESULTS:For the front corneal curvature,K_(1),and K_(2) at 3-mm,5-mm,and 7-mm of the anterior corneal surface increased significantly 1mo postoperatively(all P<0.05)and remained unchanged until 3mo(P>0.05).For the back corneal curvature,K_(1) and K_(2) along the 3-mm back meridian significantly decreased after month 1(P=0.002,0.077,respectively).Posterior K_(2)-readings along the 5-mm and 7-mm did not change after surgery(P>0.05).Anterior BFS decreased 1mo(P<0.001)postoperatively but remained unchanged until 3mo after SLAK(P>0.05).There was no change in posterior BFS before and after the surgery(P>0.05).Anterior elevation at N5,N3,central,and T5 points and posterior elevation at central and T7 points shifted backward 1mo postoperatively(all P<0.05)and remained stable until 3mo(P>0.05).CONCLUSION:The myopic SLAK combined with CXL is an economical alternative for stabilizing the corneal surface in severe keraoconus.“Pseudoprogression”occurs in the early phase postoperatively,but it is not an indicator of keratoconus progression.展开更多
Aging is a persistent topic of interest,with skin aging as its most visible manifestation,characterized by a reduction in intact collagen and elastic fibers in the dermis.Hyaluronic acid,a vital component of the extra...Aging is a persistent topic of interest,with skin aging as its most visible manifestation,characterized by a reduction in intact collagen and elastic fibers in the dermis.Hyaluronic acid,a vital component of the extracellular matrix present in the skin,has become a mainstream method for skin rejuvenation through injections.However,the rapid degradation of pure hyaluronic acid,combined with insufficient maintenance duration and often limited therapeutic effects,presents significant challenges for injectable treatments.Additionally,low patient compliance due to discomfort from needles penetrating the dermal layer further complicates its use.In this review,we summarize and compare existing interventions for skin aging,focusing on strategies to prolong the degradation cycle of hyaluronic acid,including variations in cross-linking modalities and injection techniques.We conclude that the injection of cross-linked modified hyaluronic acid via microneedles represents a promising approach to extend the degradation cycle,offering valuable insights for current therapeutic strategies.展开更多
Polymer binders possess significant potential in alleviating the volume expansion issues of silicon-based anodes,yet remain challenging due to insufficient interfacial interactions with individual components(Si,C,and ...Polymer binders possess significant potential in alleviating the volume expansion issues of silicon-based anodes,yet remain challenging due to insufficient interfacial interactions with individual components(Si,C,and Cu)of the anode.Herein,we report the synthesis of a stable three-dimensional network structure of the PAA-PEA(polyacrylic acid-polyether amines)polymer binder through intermolecular physicochemical dual cross-linking.By incorporating polar functional groups,the binder molecules not only form strong C-O-Si,N-Si,O=C-O-C,and O=C-O-Cu covalent bonds but also enhance non-covalent interactions with Si,C,and Cu,thereby improving adhesion between the binder and each interface of the anode.Furthermore,weak hydrogen bonds,acting as"sacrificial bonds",dissipate energy and disperse accumulated stress,improving the material flexibility.Due to the high mechanical stability of the framework,which combines both rigidity and flexibility and the coupling effect at the three interfaces,the movement and separation of electrode components are effectively restrained,significantly enhancing the cycling stability of silicon-graphite anodes.The PAA-PEA 2000 electrode exhibits a capacity retention of 78% after 500 cycles at a current density of 0.2 A g^(-1).This work provides insights into the mechanism of binders and guides the design of polymer binders for high-performance Si-based electrodes.展开更多
The active cooling technology of endothermic hydrocarbon fuels is a key way to solve the thermal protection of high-speed aircraft engines,but the condensation coking problem during engine shutdown is a bottleneck tha...The active cooling technology of endothermic hydrocarbon fuels is a key way to solve the thermal protection of high-speed aircraft engines,but the condensation coking problem during engine shutdown is a bottleneck that affects the reusability of aircraft.In this study,a self-designed apparatus was used to separately analyze the condensation coking during the fuel cooling process,and the coking characteristics under different temperature conditions were obtained.The condensation coking mechanism of fuel during cooling process was proposed based on the changes in physical properties of coking precursors obtained by the group contribution method.When the temperature drops to 300℃,not only the gas yield and conversion increase to 71.42% and 89.75% respectively,but the coke mass on the inner surface of the tube also significantly increases from 0.39 to 1.92 mg.Meanwhile,as the temperature further decreases,the morphology of coke gradually transforms into amorphous carbon with a higher degree of graphitization.During the cooling process,due to the liquefaction of coking precursors,their physical properties such as viscosity,density,and saturated vapor pressure undergo sudden changes at 300℃,leading to enhanced intermolecular physical interactions and promoting the physical aggregation of coking precursor molecules,which are deposited on the inner wall of the tube.This work provides a theoretical basis for the subsequent study of condensation coking mechanisms and inhibition methods.展开更多
Microcavity exciton-polaritons,formed by strong light-matter coupling,are essential for realizing Bose-Einstein condensation and low-threshold lasing.Such polaritonic lasing and condensation have been demonstrated in ...Microcavity exciton-polaritons,formed by strong light-matter coupling,are essential for realizing Bose-Einstein condensation and low-threshold lasing.Such polaritonic lasing and condensation have been demonstrated in Ⅲ-Ⅴ semiconductors at liquid helium temperatures.However,the complex fabrication of these microcavities and operating temperatures limit their room-temperature practical application.Here,we experimentally realize room-temperature exciton-polariton condensation and polaritonic lasing in a CsPbBr_(3)perovskite planar microcavity fabricated by the pressing process.Angleresolved photoluminescence spectra demonstrate the strong light-matter coupling and the formation of exciton-polaritons in such a pressed microcavity.Above the critical threshold,mass polaritons accumulating at the bottom of dispersion lead to a narrow emission linewidth and pronounced blueshift,further reinforcing the Bose-Einstein condensation and polaritonic lasing in this system.Our results offer a feasible and effective approach to investigate exciton-polariton condensation and polariton lasing at room temperature.展开更多
Compared with Pidgeon process,the relative vacuum continuous magnesium smelting process reduces the ratio of material to magnesium by changing raw materials and the direct reduction after calcination of prefabricated ...Compared with Pidgeon process,the relative vacuum continuous magnesium smelting process reduces the ratio of material to magnesium by changing raw materials and the direct reduction after calcination of prefabricated pellets,so that the energy consumption per ton of magnesium produced is reduced by 30∼40%,and the carbon emission is reduced by 43∼52%,breaking through the vacuum conditions to achieve continuous production.However,in the process of industrialization,it was found that the magnesium yield in the condenser was low.Therefore,this paper constructs a condenser model of relative vacuum continuous magnesium refining process,and comprehensively analyzes the condensation mechanism of magnesium vapor through simulation and experiment.It is found that the dynamic characteristics of magnesium vapor condensation is an important index to measure its continuity.Under the condition offlowing argon as the protective gas,when the condensation plate spacing is 10 cm,the surface roughness amplitude variance is 2,and the carrier gasflow rate is 20×10^(-3) m/s,the magnesium vapor has a better condensation effect,and the condensation efficiency formula is derived.展开更多
In this study,a novel cost-effective methodology was developed to enhance the gas barrier properties and permselectivity of unfilled natural rubber(NR)/polybutadiene rubber(BR)composites through the construction of a ...In this study,a novel cost-effective methodology was developed to enhance the gas barrier properties and permselectivity of unfilled natural rubber(NR)/polybutadiene rubber(BR)composites through the construction of a heterogeneous structure using pre-vulcanized powder rubber to replace traditional fillers.The matrix material is composed of a blend of NR and BR,which is widely used in tire manufacturing.By incorporating pre-vulcanized trans-1,4-poly(isoprene-co-butadiene)(TBIR)rubber powder(pVTPR)with different cross-linking densities and contents,significant improvements in the gas barrier properties and CO_(2)permselectivity of the NR/BR/pVTPR composites were observed.The results indicated that compared to NR/BR/TBIR composites prepared through direct blending of NR,BR,and TBIR,the NR/BR/pVTPR composites exhibited markedly superior gas barrier properties.Increasing the cross-linking density of pVTPR resulted in progressive enhancement of the gas barrier properties of the NR/BR/pVTPR composite.For example,the addition of 20 phr pVTPR with a cross-linking density of 346 mol/m^(3)resulted in a 79%improvement in the oxygen barrier property of NR/BR/pVTPR compared to NR/BR,achieving a value of 5.47×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1).Similarly,the nitrogen barrier property improved by 76%compared to NR/BR,reaching 2.4×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1),which is 28%higher than the conventional inner liner material brominated butyl rubber(BIIR,PN2=3.32×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1)).Owing to its low cost,exceptional gas barrier properties,superior adhesion to various tire components,and co-vulcanization capabilities,the NR/BR/pVTPR composite has emerged as a promising alternative to butyl rubber in the inner liner of tires.Furthermore,by fine-tuning the cross-linking density of pVTPR,the high-gas-barrier NR/BR/pVTPR composites also demonstrated remarkable CO_(2)permselectivity,with a CO_(2)/N2 selectivity of 61.4 and a CO_(2)/O_(2)selectivity of 26.12.This innovation provides a novel strategy for CO_(2)capture and separation,with potential applications in future environmental and industrial processes.The multifunctional NR/BR/pVTPR composite,with its superior gas barrier properties and CO_(2)permselectivity,is expected to contribute to the development of safer,greener,and more cost-effective transportation solutions.展开更多
Elastomers are widely used in various fields owing to their excellent tensile properties.Recyclable and self-healing properties are key to extending the service life of elastomers.Accumulating evidence indicates that ...Elastomers are widely used in various fields owing to their excellent tensile properties.Recyclable and self-healing properties are key to extending the service life of elastomers.Accumulating evidence indicates that dynamic covalent chemistry has emerged as a powerful tool for constructing recyclable and self-healing materials.In this work,we demonstrate the preparation of a recyclable and self-healable polydimethylsiloxane(PDMS)elastomer based on the Knoevenagel condensation(KC)reaction.This PDMS elastomer was prepared by the KC reaction catalyzed by 4-dimethylaminopyridine(DMAP).The obtained PDMS elastomer exhibited an elongation at break of 266%,a tensile strength of 0.57 MPa,and a good thermal stability(Td=357℃).In addition,because of the presence of dynamic C=C bonds formed by the KC reaction and low glass transition temperature(Tg=-117℃).This PDMS exhibited good self-healing and recycling properties at room temperature and could be reprocessed by hot pressing.In addition,the PDMS elastomer exhibits good application prospects in the fields of adhesives and flexible electronic devices.展开更多
Utilizing superwettability micro/nanostructures to enhance the condensation heat transfer(CHT)performance of engineering materials has attracted great interest due to its values in basic research and technological inn...Utilizing superwettability micro/nanostructures to enhance the condensation heat transfer(CHT)performance of engineering materials has attracted great interest due to its values in basic research and technological innovations.Currently,exploring facile micro/nanofabrication approaches to create high-efficiency CHT surfaces has been one of research hotspots.In this work,we propose and demonstrate a type of new superwettability hybrid surface for high-efficiency CHT,which consists of superhydrophobic nanoneedle arrays and triangularly-patterned superhydrophilic microdots(SMDs).Such hybrid surface can be fabricated by the facile growth of densely-packed ZnO nanoneedles on the Zn-electroplated copper surface followed by fluorosilane modification and mask-assisted photodegradation.Through regulating the diameters and interspaces of SMDs,we obtain the optimized triangularly-patterned hybrid surface,which shows 42.7%higher CHT coefficient than the squarely-patterned hybrid surface and 58.5%higher CHT coefficient than the superhydrophobic surface.The key of such hybrid surface design is to considerably increase CHT coefficient brought about by SMD-triggered drop sweeping at the cost of slightly reducing heat transfer area of superhydrophobic functional zone for drop jumping.Such new strategy helps develop advanced CHT surfaces for high-efficiency electronic cooling and energy utilization.展开更多
The self-condensation of n-butanal is an important reaction for carbon-chain extension in the commercial production of 2-ethylhexanol.Moreover,aldol condensation is one of the important reactions for the synthesis of ...The self-condensation of n-butanal is an important reaction for carbon-chain extension in the commercial production of 2-ethylhexanol.Moreover,aldol condensation is one of the important reactions for the synthesis of valuable organic chemicals or transportation fuels from biomass-derived platform compounds.So the investigation of the self-condensation of n-butanal is of significance in both academia and industry.This contribution reviewed the catalytic performance of heterogeneous catalysts in the self-condensation of n-butanal and the related reaction mechanism,network,and kinetics.The purpose of this review is to dedicate some help for further development of environmentally friendly catalysts and for a thorough comprehension of aldol condensation.展开更多
This work demonstrates that once a large number of pion is condensed in a high-energy hadron collision, the gamma-ray spectrum from π0decay takes on a typical broken power-law shape, which has been documented in many...This work demonstrates that once a large number of pion is condensed in a high-energy hadron collision, the gamma-ray spectrum from π0decay takes on a typical broken power-law shape, which has been documented in many astronomical observations, but we have not yet recognized it. We show that this pion condensation is caused by a large number of soft gluons condensed in protons.展开更多
Vanadium phosphorus oxide(VPO)catalyst is a promising candidate for the condensation reaction of formaldehyde(FA)and acetic acid(HAc)to produce acrylic acid(AA).However,the complexity of the active phases and their dy...Vanadium phosphorus oxide(VPO)catalyst is a promising candidate for the condensation reaction of formaldehyde(FA)and acetic acid(HAc)to produce acrylic acid(AA).However,the complexity of the active phases and their dynamic interconversion under redox conditions has led to controversies regarding the actual active phase in this reaction.To address this,this study systematically investigates the phase transition and underlying mechanism of VPO catalysts under reaction conditions.X-ray diffraction(XRD)patterns,Raman spectra,transmission electron microscopy images and X-ray photoelectron spectroscopy collectively demonstrated that the V^(4+)phase(VO)_(2)P_(2)O_(7)retained the bulk phase structure throughout the reaction,with only minor surface phase transition observed.In contrast,the V^(5+)phase underwent reduction to other phases in both bulk and surface regions.Specifically,theδ-VOPO_(4)phase rapidly transformed into theαII-VOPO_(4)phase,which could reversibly convert into the R1-VOHPO_(4)phase(V^(4+)).Controlled variable experiments,H_(2)-temperature programmed reduction and in-situ XRD experiments in a hydrogen atmosphere further demonstrated that these phase transitions were primarily attributed to the loss of lattice oxygen.The presence of V^(4+)phase in VPO catalysts enhanced the selectivity of acrylic acid,while the existence of V^(5+)phase promoted the activation of acetic acid.This work elucidates the redox-driven phase evolution of VPO catalysts and offers valuable insights for designing efficient catalysts for FA-HAc cross-condensation by balancing phase stability and activity.展开更多
Accurate descriptions of cloud droplet spectra from aerosol activation to vapor condensation using microphysical parameterization schemes are crucial for numerical simulations of precipitation and climate change in we...Accurate descriptions of cloud droplet spectra from aerosol activation to vapor condensation using microphysical parameterization schemes are crucial for numerical simulations of precipitation and climate change in weather forecasting and climate prediction models.Hence,the latest activation and triple-moment condensation schemes were combined to simulate and analyze the evolution characteristics of a cloud droplet spectrum from activation to condensation and compared with a high-resolution Lagrangian bin model and the current double-moment condensation schemes,in which the spectral shape parameter is fixed or diagnosed by an empirical formula.The results demonstrate that the latest schemes effectively capture the evolution characteristics of the cloud droplet spectrum during activation and condensation,which is in line with the performance of the bin model.The simulation of the latest activation and condensation schemes in a parcel model shows that the cloud droplet spectrum gradually widens and exhibits a multimodal distribution during the activation process,accompanied by a decrease in the spectral shape and slope parameters over time.Conversely,during the condensation process,the cloud droplet spectrum gradually narrows,resulting in increases in the spectral shape and slope parameters.However,these double-moment schemes fail to accurately replicate the evolution of the cloud droplet spectrum and its multimodal distribution characteristics.Furthermore,the latest schemes were coupled into a 1.5D cumulus model,and an observation case was simulated.The simulations confirm that the cloud droplet spectrum appears wider at the supersaturated cloud base and cloud top due to activation,while it becomes narrower at the middle altitudes of the cloud due to condensation growth.展开更多
Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,...Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,composed of N-modified dendritic carbon networks supporting Al_(2)O_(3)nanoparticles,was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate,Al3+and urea.The obtained carbon-supported Al_(2)O_(3)hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state.The introduction of urea enhances the surface N content,the ratio of pyrrolic N,and specific surface area of catalyst,leading to improved adsorption capacity of C=O and the accessibility of active sites.In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor,Al_(2)O_(3)/C-u catalyst achieved a 90%conversion of furfural with 98.0% selectivity to furfuryl alcohol,outperforming that of commercial γ-Al_(2)O_(3).Moreover,Al_(2)O_(3)/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al_(2)O_(3)nanoparticles.This work provides an innovative and facile strategy for fabrication of carbon-supported Al_(2)O_(3)hybrid catalysts with rich AlVspecies,serving as a high selective hydrogenation catalyst through MPV reaction route.展开更多
Oxidation of organic amines(OAs)or aromatic hydrocarbons(AHs)produces carbonyls,which further react with OAs to form carbonyl-amine condensation products,threatening environmental quality and human health.However,ther...Oxidation of organic amines(OAs)or aromatic hydrocarbons(AHs)produces carbonyls,which further react with OAs to form carbonyl-amine condensation products,threatening environmental quality and human health.However,there is still a lack of systematic understanding of the carbonyl-amine condensation reaction processes of OAs or between OAs and AHs,and subsequent environmental health impact.This work systematically investigated the carbonyl-amine condensation coupled ozonolysis kinetics,reaction mechanism,secondary organic aerosol(SOA)formation and cytotoxicity fromthe mixture of dipropylamine(DPA)and styrene(STY)by a combined method of productmass spectrometry identification,particle property analysis and cell exposure evaluation.The results from ozonolysis of DPA and STY mixture revealed that STY inhibited the ozonolysis of DPA to different degrees to accelerate its own decay rate.The barycenter of carbonyl-amine condensation reactionswas shifted from inside of DPA to between DPA and STY,which accelerated STY ozonolysis,but slowed down DPA ozonolysis.For the first time,ozonolysis of DPA and STY mixture to complex carbonyl-amine condensation products through the reactions of DPA with its carbonyl products,DPA with STY’s carbonyl products and DPA’s bond breakage product with STY’s carbonyl products was confirmed.These condensation products significantly contributed to the formation and growth of SOA.The SOA containing particulate carbonyl-amine condensation products showed definite cytotoxicity.These findings are helpful to deeply and comprehensively understand the transformation,fate and environmental health effects of mixed organics in atmospheric environment.展开更多
文摘The retrospective study by Edwar et al reinforces the role of therapeutic penetrating keratoplasty(PK)as a vital intervention in severe,treatment-resistant infectious keratitis.In advanced cases—often complicated by trauma,delayed presentation,and corneal perforation—PK restores globe integrity and provides limited visual recovery.However,its application is constrained by graft-related complications and donor shortages,particularly in low-resource settings.These limitations highlight the need for earlier,globe-sparing strategies to prevent progression and reduce surgical demand.Photoactivated chromophore for infectious keratitis-corneal collagen cross-linking(PACK-CXL)has emerged as a promising adjunct or alternative.With both antimicrobial and tissue-stabilizing effects,PACK-CXL may control infection and preserve corneal structure in earlier stages.A layered treatment framework that incorporates PACK-CXL as an initial intervention and reserves PK for refractory cases may help improve clinical outcomes.Further studies are needed to define their best use in practice.
基金supported by Research Fund of SWUST for PhD(Grant No.22zx7175)Sichuan Science and Technology Program(Grant No.2024NSFSC1097)。
文摘Based on the characteristics of laser-induced surface ignition,energetic photosensitive films show promising potential to meet the ignition requirements of various energetic materials(EMs).In this study,DATNBI/ferric alginate(DI/FeA),DI/cobalt alginate(DI/CoA),and DI/nickel alginate(DI/Ni A)films are fabricated by employing sodium alginate(SA)with a three-dimensional network structure as the film matrix,via ionic cross-linking of SA with Fe^(3+),Co^(2+),and Ni^(2+)ions.The study demonstrates that the ionic cross-linking enhances the hydrophobic performance of the films,with the water contact angle increasing from 82.1° to 123.5°.Concurrently,the films'near-infrared(NIR)light absorption improved.Furthermore,transition metal ions facilitate accelerated electron transfer,thereby catalyzing the thermal decomposition of DATNBI.Under 1064 nm laser irradiation,the DI/Fe A film exhibits exceptional combustion performance,with an ignition delay time as low as 76 ms.It successfully acts as an NIR laser ignition medium to initiate the self-sustained combustion of CL-20.This study demonstrates the synergistic realization of enhanced hydrophobicity,improved photosensitivity,and promoted catalytic decomposition through microstructural design of the material,providing new insights for the design of additive-free EMs in laser ignition applications.
基金supported through RIIM Competition funding from the Indonesia Endowment Fund for Education Agency,Ministry of Finance of the Republic of Indonesia and National Research and Innovation Agency of Indonesia according to the contract number:61/IV/KS/5/2023 and 2131/UN6.3.1/PT.00/2023.
文摘Corn starch(CS)is a renewable,biodegradable polysaccharide valued for its film-forming ability,yet native CS films exhibit lowmechanical strength,highwater sensitivity,and limited thermal stability.This study improves CS-based films by blending with poly(vinyl alcohol)(PVA)or glycerol(GLY)and using citric acid(CA)as a green,non-toxic cross-linker.Composite films were prepared by casting CS–PVA or CS-GLY with CA at 0%-0.20%(w/w of starch).The influence of CA on physicochemical,mechanical,optical,thermal,and water barrier properties was evaluated.CA crosslinking markedly enhanced the tensile strength,water resistance,and thermal stability of CS-PVA films while increasing transparency in CS–GLY films.At 0.20%CA,the composite achieved 34.99MPa tensile strength,reducedwater vapor permeability,andminimized water uptake.FTIR confirmed ester bond formation between CAand hydroxyl groups of CS,PVA,and GLY,whereas thermal analysis showed higher decomposition temperatures and lower weight loss in crosslinked films.Increasing CA levels also decreased opacity and improved light transmittance,indicating greater homogeneity and reduced crystallinity.This dual-polymer matrix combined with a natural crosslinking strategy provides a sustainable route to high-performance,biodegradable CS-based packaging materials.
基金supported by the Key Technologies R&D Program of Xiamen(No.3502Z20231057)Industry Leading Key Projects of Fujian Province(No.2022H0057)+2 种基金the National Natural Science Foundation of China(No.21975212)High-Level Talent Start-Up Foundation of Xiamen Institute of Technology for financial support(No.YKJ23017R)Graduate Science and Technology Innovation Program of Xiamen University of Technology(No.YKJCX2023194).
文摘LiMnxFe1-xPO_(4) is a promising cathode candidate due to its high security and the availability of a high 4.1 V operating voltage and high energy density.However,the poor electrochemical kinetics and structural instability currently hinder its broader application.Herein,inspired by the hydrogen-bonded cross-linking and steric hindrance effect between short-chain polymer molecules(polyethylene glycol-400,PEG-400),the pomegranate-type LiMn_(0.5)Fe_(0.5)PO_(4)-0.5@C(P-LMFP@C)cathode materials with 3D ion/electron dual-conductive network structure were constructed through ball mill-assisted spray-drying method.The intermolecular effects of PEG-400 promote the spheroidization and uniform PEG coating of LMFP precursor,which prevents agglomeration during sintering.The 3D ion/electron dual-conductive network structure in P-LMFP@C accelerates the Li^(+)transport kinetics,improving the rate performance and cycling stability.As a result,the designed P-LMFP@C has remarkable electrochemical behavior,boasting excellent capacity retention(98%after 100 cycles at the 1C rate)and rate capability(91 mAh·g^(-1)at 20C).Such strategy introduces a novel window for designing high-performance olivine cathodes and offers compatibility with a range of energy storage materials for diverse applications.
文摘AIM:To compare simultaneous corneal collagen cross-linking(CXL)with intracorneal ring segment(ICRS)implantation versus successive ICRS followed by CXL and detect the impact of the timing of CXL after ICRS implantation in the successive method.METHODS:This is a retrospective study of the records of three groups of patients.Group 1 of 28 patients were operated on with simultaneous ICRS implantation and CXL,group 2 of 32 patients had ICRS implantation followed by CXL after 1mo,and group 3 of 38 patients had ICRS implantation followed by CXL after 3mo.The three groups had follow-up visits after 6,12,and 24mo.RESULTS:The preoperative data,age,and gender differences among 3 groups revealed no significant differences.The postoperative spherical equivalent and best-corrected visual acuity were improved significantly in all groups compared to the baseline,which were more evident in groups 1 and 2.The differences between preoperative and postoperative mean values of mean of K readings(Km)and maximum K reading(Kmax)at 6mo were 4.66 and 4.1 D in group 1,4.43 and 4.64 D in group 2,but 3.2 and 3.4 D in group 3,respectively.The spherical aberrations and the vertical coma showed significant postoperative changes in all groups,and trefoil showed nonsignificant changes.CONCLUSION:Simultaneous and sequential ICRS implantation and CXL at 1mo has similar Km and Kmax better postoperative changes than when both surgeries were done at three-month intervals.
基金Supported by the Social Development Grant of Shaanxi Province(No.2022SF-404)the Science and Technology Program of Xi’an,China(No.23YXYJ0010,No.23YXYJ0037)+1 种基金the Research Project of Xi’an Health Commission(No.2024ms05)the Technology Innovation Supporting Program of Shaanxi(No.2024RS-CXTD-11).
文摘AIM:To investigate the response of the anterior and posterior corneal surface in femtosecond laser-assisted convex stromal lenticule addition keratoplasty(SLAK)combined with cross-linking(CXL)for treating keratoconus at the first 3mo of follow-up.METHODS:In this prospective observational study,20 eyes of 20 keratoconus patients who underwent SLAK combined with CXL were included.The morphological indices in keratometry and elevation data were recorded from the Sirius at baseline and 1 and 3mo postoperatively.The mean values of maximum keratometry(K_(max)),flat keratometry(K_(1)),and steep keratometry(K_(2))at the central,3-mm,5-mm,and 7-mm areas were measured from the curvature map.The changes in anterior and posterior corneal elevation under the best-fit sphere(BFS)radius at seven points horizontally of the center,3-mm,5-mm,and 7-mm area from the center at both nasal(N)and temporal(T)side were measured from elevation map.RESULTS:For the front corneal curvature,K_(1),and K_(2) at 3-mm,5-mm,and 7-mm of the anterior corneal surface increased significantly 1mo postoperatively(all P<0.05)and remained unchanged until 3mo(P>0.05).For the back corneal curvature,K_(1) and K_(2) along the 3-mm back meridian significantly decreased after month 1(P=0.002,0.077,respectively).Posterior K_(2)-readings along the 5-mm and 7-mm did not change after surgery(P>0.05).Anterior BFS decreased 1mo(P<0.001)postoperatively but remained unchanged until 3mo after SLAK(P>0.05).There was no change in posterior BFS before and after the surgery(P>0.05).Anterior elevation at N5,N3,central,and T5 points and posterior elevation at central and T7 points shifted backward 1mo postoperatively(all P<0.05)and remained stable until 3mo(P>0.05).CONCLUSION:The myopic SLAK combined with CXL is an economical alternative for stabilizing the corneal surface in severe keraoconus.“Pseudoprogression”occurs in the early phase postoperatively,but it is not an indicator of keratoconus progression.
基金financial support from several corporate sponsors.Contributions were made by the National Natural Science Foundation of China(Grant No.32071332)Shenzhen Science and Technology Innovation Project(Grant No.JCYJ20210324095802006)+2 种基金Ningbo Bureau of Science and Technology(Grant No.2023Z187)TransEasy Medical Tech.Co.,Ltd.(Grant No.2021114)Shenzhen University MedTech Innovation Fund(2023YG027).
文摘Aging is a persistent topic of interest,with skin aging as its most visible manifestation,characterized by a reduction in intact collagen and elastic fibers in the dermis.Hyaluronic acid,a vital component of the extracellular matrix present in the skin,has become a mainstream method for skin rejuvenation through injections.However,the rapid degradation of pure hyaluronic acid,combined with insufficient maintenance duration and often limited therapeutic effects,presents significant challenges for injectable treatments.Additionally,low patient compliance due to discomfort from needles penetrating the dermal layer further complicates its use.In this review,we summarize and compare existing interventions for skin aging,focusing on strategies to prolong the degradation cycle of hyaluronic acid,including variations in cross-linking modalities and injection techniques.We conclude that the injection of cross-linked modified hyaluronic acid via microneedles represents a promising approach to extend the degradation cycle,offering valuable insights for current therapeutic strategies.
基金financial support from the National Natural Science Foundation of China[grant number 21878299]。
文摘Polymer binders possess significant potential in alleviating the volume expansion issues of silicon-based anodes,yet remain challenging due to insufficient interfacial interactions with individual components(Si,C,and Cu)of the anode.Herein,we report the synthesis of a stable three-dimensional network structure of the PAA-PEA(polyacrylic acid-polyether amines)polymer binder through intermolecular physicochemical dual cross-linking.By incorporating polar functional groups,the binder molecules not only form strong C-O-Si,N-Si,O=C-O-C,and O=C-O-Cu covalent bonds but also enhance non-covalent interactions with Si,C,and Cu,thereby improving adhesion between the binder and each interface of the anode.Furthermore,weak hydrogen bonds,acting as"sacrificial bonds",dissipate energy and disperse accumulated stress,improving the material flexibility.Due to the high mechanical stability of the framework,which combines both rigidity and flexibility and the coupling effect at the three interfaces,the movement and separation of electrode components are effectively restrained,significantly enhancing the cycling stability of silicon-graphite anodes.The PAA-PEA 2000 electrode exhibits a capacity retention of 78% after 500 cycles at a current density of 0.2 A g^(-1).This work provides insights into the mechanism of binders and guides the design of polymer binders for high-performance Si-based electrodes.
基金support from the National Natural Science Foundation of China (22308233,92060101)the Natural Science Foundation of Sichuan Province of China (2024NSFSC1162)+1 种基金the Source of Origin Project of Beijing Power Machinery Research Institutethe Sichuan Province Science Fund for Distinguished Young Scholars (2021JDJQ0011)。
文摘The active cooling technology of endothermic hydrocarbon fuels is a key way to solve the thermal protection of high-speed aircraft engines,but the condensation coking problem during engine shutdown is a bottleneck that affects the reusability of aircraft.In this study,a self-designed apparatus was used to separately analyze the condensation coking during the fuel cooling process,and the coking characteristics under different temperature conditions were obtained.The condensation coking mechanism of fuel during cooling process was proposed based on the changes in physical properties of coking precursors obtained by the group contribution method.When the temperature drops to 300℃,not only the gas yield and conversion increase to 71.42% and 89.75% respectively,but the coke mass on the inner surface of the tube also significantly increases from 0.39 to 1.92 mg.Meanwhile,as the temperature further decreases,the morphology of coke gradually transforms into amorphous carbon with a higher degree of graphitization.During the cooling process,due to the liquefaction of coking precursors,their physical properties such as viscosity,density,and saturated vapor pressure undergo sudden changes at 300℃,leading to enhanced intermolecular physical interactions and promoting the physical aggregation of coking precursor molecules,which are deposited on the inner wall of the tube.This work provides a theoretical basis for the subsequent study of condensation coking mechanisms and inhibition methods.
基金support from theNational Natural Science Foundation(Grant No.12204111)the National Key Research and Development Program ofChina(Grant No.2023YFA1407100)Shanghai Pilot Pro-gram for Basic Research(Grant No.22JC1403202)。
文摘Microcavity exciton-polaritons,formed by strong light-matter coupling,are essential for realizing Bose-Einstein condensation and low-threshold lasing.Such polaritonic lasing and condensation have been demonstrated in Ⅲ-Ⅴ semiconductors at liquid helium temperatures.However,the complex fabrication of these microcavities and operating temperatures limit their room-temperature practical application.Here,we experimentally realize room-temperature exciton-polariton condensation and polaritonic lasing in a CsPbBr_(3)perovskite planar microcavity fabricated by the pressing process.Angleresolved photoluminescence spectra demonstrate the strong light-matter coupling and the formation of exciton-polaritons in such a pressed microcavity.Above the critical threshold,mass polaritons accumulating at the bottom of dispersion lead to a narrow emission linewidth and pronounced blueshift,further reinforcing the Bose-Einstein condensation and polaritonic lasing in this system.Our results offer a feasible and effective approach to investigate exciton-polariton condensation and polariton lasing at room temperature.
基金the National Natural Science Foundation of China(U1908225,U1702253)the Special Funds for Ba-sic Research Operations of Central Universities(N182515007,N170908001,N2025004).
文摘Compared with Pidgeon process,the relative vacuum continuous magnesium smelting process reduces the ratio of material to magnesium by changing raw materials and the direct reduction after calcination of prefabricated pellets,so that the energy consumption per ton of magnesium produced is reduced by 30∼40%,and the carbon emission is reduced by 43∼52%,breaking through the vacuum conditions to achieve continuous production.However,in the process of industrialization,it was found that the magnesium yield in the condenser was low.Therefore,this paper constructs a condenser model of relative vacuum continuous magnesium refining process,and comprehensively analyzes the condensation mechanism of magnesium vapor through simulation and experiment.It is found that the dynamic characteristics of magnesium vapor condensation is an important index to measure its continuity.Under the condition offlowing argon as the protective gas,when the condensation plate spacing is 10 cm,the surface roughness amplitude variance is 2,and the carrier gasflow rate is 20×10^(-3) m/s,the magnesium vapor has a better condensation effect,and the condensation efficiency formula is derived.
基金supported by the National Key Research and Development Program of China (No. 2022YFB3704700(2022YFB3704702))the National Natural Science Foundation of China (No. 52473096)+1 种基金Major Scientific and Technological Innovation Project of Shandong Province (No. 2021CXGC010901)Taishan Scholar Program
文摘In this study,a novel cost-effective methodology was developed to enhance the gas barrier properties and permselectivity of unfilled natural rubber(NR)/polybutadiene rubber(BR)composites through the construction of a heterogeneous structure using pre-vulcanized powder rubber to replace traditional fillers.The matrix material is composed of a blend of NR and BR,which is widely used in tire manufacturing.By incorporating pre-vulcanized trans-1,4-poly(isoprene-co-butadiene)(TBIR)rubber powder(pVTPR)with different cross-linking densities and contents,significant improvements in the gas barrier properties and CO_(2)permselectivity of the NR/BR/pVTPR composites were observed.The results indicated that compared to NR/BR/TBIR composites prepared through direct blending of NR,BR,and TBIR,the NR/BR/pVTPR composites exhibited markedly superior gas barrier properties.Increasing the cross-linking density of pVTPR resulted in progressive enhancement of the gas barrier properties of the NR/BR/pVTPR composite.For example,the addition of 20 phr pVTPR with a cross-linking density of 346 mol/m^(3)resulted in a 79%improvement in the oxygen barrier property of NR/BR/pVTPR compared to NR/BR,achieving a value of 5.47×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1).Similarly,the nitrogen barrier property improved by 76%compared to NR/BR,reaching 2.4×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1),which is 28%higher than the conventional inner liner material brominated butyl rubber(BIIR,PN2=3.32×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1)).Owing to its low cost,exceptional gas barrier properties,superior adhesion to various tire components,and co-vulcanization capabilities,the NR/BR/pVTPR composite has emerged as a promising alternative to butyl rubber in the inner liner of tires.Furthermore,by fine-tuning the cross-linking density of pVTPR,the high-gas-barrier NR/BR/pVTPR composites also demonstrated remarkable CO_(2)permselectivity,with a CO_(2)/N2 selectivity of 61.4 and a CO_(2)/O_(2)selectivity of 26.12.This innovation provides a novel strategy for CO_(2)capture and separation,with potential applications in future environmental and industrial processes.The multifunctional NR/BR/pVTPR composite,with its superior gas barrier properties and CO_(2)permselectivity,is expected to contribute to the development of safer,greener,and more cost-effective transportation solutions.
基金supported by the National Natural Science Foundation of China(Nos.51973025 and 52222307)Jilin Science and Technology Bureau(Nos.20220204107YY and 20230204086YY)+1 种基金Changchun Science and Technology Bureau(No.21ZGY06)Jilin Province Development and Reform Commission(No.2023C028-4).
文摘Elastomers are widely used in various fields owing to their excellent tensile properties.Recyclable and self-healing properties are key to extending the service life of elastomers.Accumulating evidence indicates that dynamic covalent chemistry has emerged as a powerful tool for constructing recyclable and self-healing materials.In this work,we demonstrate the preparation of a recyclable and self-healable polydimethylsiloxane(PDMS)elastomer based on the Knoevenagel condensation(KC)reaction.This PDMS elastomer was prepared by the KC reaction catalyzed by 4-dimethylaminopyridine(DMAP).The obtained PDMS elastomer exhibited an elongation at break of 266%,a tensile strength of 0.57 MPa,and a good thermal stability(Td=357℃).In addition,because of the presence of dynamic C=C bonds formed by the KC reaction and low glass transition temperature(Tg=-117℃).This PDMS exhibited good self-healing and recycling properties at room temperature and could be reprocessed by hot pressing.In addition,the PDMS elastomer exhibits good application prospects in the fields of adhesives and flexible electronic devices.
基金supported by National Natural Science Foundation of China(No.21573276)Natural Science Foundation of Jiangsu Province(No.BK20170007)Jiangsu Funding Program for Excellent Postdoctoral Talent(No.2022ZB846).
文摘Utilizing superwettability micro/nanostructures to enhance the condensation heat transfer(CHT)performance of engineering materials has attracted great interest due to its values in basic research and technological innovations.Currently,exploring facile micro/nanofabrication approaches to create high-efficiency CHT surfaces has been one of research hotspots.In this work,we propose and demonstrate a type of new superwettability hybrid surface for high-efficiency CHT,which consists of superhydrophobic nanoneedle arrays and triangularly-patterned superhydrophilic microdots(SMDs).Such hybrid surface can be fabricated by the facile growth of densely-packed ZnO nanoneedles on the Zn-electroplated copper surface followed by fluorosilane modification and mask-assisted photodegradation.Through regulating the diameters and interspaces of SMDs,we obtain the optimized triangularly-patterned hybrid surface,which shows 42.7%higher CHT coefficient than the squarely-patterned hybrid surface and 58.5%higher CHT coefficient than the superhydrophobic surface.The key of such hybrid surface design is to considerably increase CHT coefficient brought about by SMD-triggered drop sweeping at the cost of slightly reducing heat transfer area of superhydrophobic functional zone for drop jumping.Such new strategy helps develop advanced CHT surfaces for high-efficiency electronic cooling and energy utilization.
基金supported by the National Natural Science Foundation of China(21476058,U21A20306,21506046 and 21978066)。
文摘The self-condensation of n-butanal is an important reaction for carbon-chain extension in the commercial production of 2-ethylhexanol.Moreover,aldol condensation is one of the important reactions for the synthesis of valuable organic chemicals or transportation fuels from biomass-derived platform compounds.So the investigation of the self-condensation of n-butanal is of significance in both academia and industry.This contribution reviewed the catalytic performance of heterogeneous catalysts in the self-condensation of n-butanal and the related reaction mechanism,network,and kinetics.The purpose of this review is to dedicate some help for further development of environmentally friendly catalysts and for a thorough comprehension of aldol condensation.
基金partly supported by the National Key R&D Program of China (Grant No. 2023YFB3001502)the National Natural Science of China (Grant No. 12373002)。
文摘This work demonstrates that once a large number of pion is condensed in a high-energy hadron collision, the gamma-ray spectrum from π0decay takes on a typical broken power-law shape, which has been documented in many astronomical observations, but we have not yet recognized it. We show that this pion condensation is caused by a large number of soft gluons condensed in protons.
文摘Vanadium phosphorus oxide(VPO)catalyst is a promising candidate for the condensation reaction of formaldehyde(FA)and acetic acid(HAc)to produce acrylic acid(AA).However,the complexity of the active phases and their dynamic interconversion under redox conditions has led to controversies regarding the actual active phase in this reaction.To address this,this study systematically investigates the phase transition and underlying mechanism of VPO catalysts under reaction conditions.X-ray diffraction(XRD)patterns,Raman spectra,transmission electron microscopy images and X-ray photoelectron spectroscopy collectively demonstrated that the V^(4+)phase(VO)_(2)P_(2)O_(7)retained the bulk phase structure throughout the reaction,with only minor surface phase transition observed.In contrast,the V^(5+)phase underwent reduction to other phases in both bulk and surface regions.Specifically,theδ-VOPO_(4)phase rapidly transformed into theαII-VOPO_(4)phase,which could reversibly convert into the R1-VOHPO_(4)phase(V^(4+)).Controlled variable experiments,H_(2)-temperature programmed reduction and in-situ XRD experiments in a hydrogen atmosphere further demonstrated that these phase transitions were primarily attributed to the loss of lattice oxygen.The presence of V^(4+)phase in VPO catalysts enhanced the selectivity of acrylic acid,while the existence of V^(5+)phase promoted the activation of acetic acid.This work elucidates the redox-driven phase evolution of VPO catalysts and offers valuable insights for designing efficient catalysts for FA-HAc cross-condensation by balancing phase stability and activity.
基金supported by the National Natural Science Foundations of China(Grant Nos.42305163 and U22A20577)the Construction Project of Weather Modification Ability in Central China(Grant No.ZQC-H22256)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0760300)the Projects of the Earth System Numerical Simulation Facility(Grant Nos.2024-EL-PT-000707,2023-ELPT-000482,2023-EL-ZD-00026,and 2022-EL-PT-00083)the STS Program of the Inner Mongolia Meteorological Service,Chongqing Institute of Green and Intelligent Technology,Chinese Academy of Sciences,and Institute of Atmospheric Physics,Chinese Academy of Sciences(Grant No.2021CG0047)。
文摘Accurate descriptions of cloud droplet spectra from aerosol activation to vapor condensation using microphysical parameterization schemes are crucial for numerical simulations of precipitation and climate change in weather forecasting and climate prediction models.Hence,the latest activation and triple-moment condensation schemes were combined to simulate and analyze the evolution characteristics of a cloud droplet spectrum from activation to condensation and compared with a high-resolution Lagrangian bin model and the current double-moment condensation schemes,in which the spectral shape parameter is fixed or diagnosed by an empirical formula.The results demonstrate that the latest schemes effectively capture the evolution characteristics of the cloud droplet spectrum during activation and condensation,which is in line with the performance of the bin model.The simulation of the latest activation and condensation schemes in a parcel model shows that the cloud droplet spectrum gradually widens and exhibits a multimodal distribution during the activation process,accompanied by a decrease in the spectral shape and slope parameters over time.Conversely,during the condensation process,the cloud droplet spectrum gradually narrows,resulting in increases in the spectral shape and slope parameters.However,these double-moment schemes fail to accurately replicate the evolution of the cloud droplet spectrum and its multimodal distribution characteristics.Furthermore,the latest schemes were coupled into a 1.5D cumulus model,and an observation case was simulated.The simulations confirm that the cloud droplet spectrum appears wider at the supersaturated cloud base and cloud top due to activation,while it becomes narrower at the middle altitudes of the cloud due to condensation growth.
基金China Postdoctoral Science Foundation (2023M733451)Dalian Innovation Team in Key Areas(2020RT06)Engineering Research Center for Key Aromatic Compounds and LiaoNing Key Laboratory,Liaoning Provincial Natural Science Foundation (Doctoral Research Start-up Fund 2024-BSBA-37)。
文摘Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,composed of N-modified dendritic carbon networks supporting Al_(2)O_(3)nanoparticles,was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate,Al3+and urea.The obtained carbon-supported Al_(2)O_(3)hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state.The introduction of urea enhances the surface N content,the ratio of pyrrolic N,and specific surface area of catalyst,leading to improved adsorption capacity of C=O and the accessibility of active sites.In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor,Al_(2)O_(3)/C-u catalyst achieved a 90%conversion of furfural with 98.0% selectivity to furfuryl alcohol,outperforming that of commercial γ-Al_(2)O_(3).Moreover,Al_(2)O_(3)/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al_(2)O_(3)nanoparticles.This work provides an innovative and facile strategy for fabrication of carbon-supported Al_(2)O_(3)hybrid catalysts with rich AlVspecies,serving as a high selective hydrogenation catalyst through MPV reaction route.
基金supported by the National Natural Science Foundation of China(Nos.42177354 and 42020104001)the National Key R&D Program of China(No.2019YFC0214402)+1 种基金the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)Guangdong Basic and Applied Basic Research Foundation(No.2019B151502064).
文摘Oxidation of organic amines(OAs)or aromatic hydrocarbons(AHs)produces carbonyls,which further react with OAs to form carbonyl-amine condensation products,threatening environmental quality and human health.However,there is still a lack of systematic understanding of the carbonyl-amine condensation reaction processes of OAs or between OAs and AHs,and subsequent environmental health impact.This work systematically investigated the carbonyl-amine condensation coupled ozonolysis kinetics,reaction mechanism,secondary organic aerosol(SOA)formation and cytotoxicity fromthe mixture of dipropylamine(DPA)and styrene(STY)by a combined method of productmass spectrometry identification,particle property analysis and cell exposure evaluation.The results from ozonolysis of DPA and STY mixture revealed that STY inhibited the ozonolysis of DPA to different degrees to accelerate its own decay rate.The barycenter of carbonyl-amine condensation reactionswas shifted from inside of DPA to between DPA and STY,which accelerated STY ozonolysis,but slowed down DPA ozonolysis.For the first time,ozonolysis of DPA and STY mixture to complex carbonyl-amine condensation products through the reactions of DPA with its carbonyl products,DPA with STY’s carbonyl products and DPA’s bond breakage product with STY’s carbonyl products was confirmed.These condensation products significantly contributed to the formation and growth of SOA.The SOA containing particulate carbonyl-amine condensation products showed definite cytotoxicity.These findings are helpful to deeply and comprehensively understand the transformation,fate and environmental health effects of mixed organics in atmospheric environment.
