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
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
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
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 observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHO...AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHODS:In this prospectively study,130 patients underwent FS-LASIK or FS-LASIK Xtra for high myopia.Their right eyes were selected for inclusion in the study,of which 65 cases of 65 eyes in the FS-LASIK group,65 patients with 65 eyes in the FS-LASIK Xtra group.Patients were evaluated for corneal densitometry at 1,3,and 6mo postoperatively using Pentacam Scheimpflug imaging.RESULTS:Preoperative differences in corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups in different ranges were not statistically significant(P>0.05).Layer-by-layer analysis revealed statistically significant differences in the anterior(120μm),central,and total layer corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups at 1 and 3mo postoperatively(all P<0.05),the FS-LASIK Xtra group is higher than that of the FS-LASIK group.Analysis of different diameter ranges showed statistically significant differences between the FS-LASIK group and the FS-LASIK Xtra group at 1mo postoperatively in the ranges of 0–2,2–6,and 6–10 mm(both P<0.05);At 3mo postoperatively,the FS-LASIK Xtra group is higher than that of the FS-LASIK group in the ranges of 0–2 and 2–6 mm(P<0.05).At 6mo postoperatively,there were no statistically significant differences in corneal densitometry between the FS-LASIK group and the FS-LASIK Xtra group in different diameter ranges(all P>0.05).CONCLUSION:There is an increase in internal corneal densitometry during the early postoperative period after FS-LASIK Xtra for correction of high myopia.However,the densitometry values decreased to the level of conventional FS-LASIK at 6mo after surgery,with the most significant changes observed in the superficial central zone.展开更多
In order to reduce the hazard of coal spontaneous combustion,the cross-linking reaction between O-containing functional groups of coal should be inhibited.So the inhibitory effect of an ionic liquid(IL) on the cross-l...In order to reduce the hazard of coal spontaneous combustion,the cross-linking reaction between O-containing functional groups of coal should be inhibited.So the inhibitory effect of an ionic liquid(IL) on the cross-linking reaction was studied.The O-containing functional groups change the weight loss and H_2O,CO_2,CO yields of bituminous coal before and after[H0Emim][BF_4]and[Amim]Cl pre-treatment and were detected by Fourier Transform Infrared spectroscopy(FT1R) and Thermo Gravimetric(TC) analysis.The results show that | AmimjCI has a weaker ability to inhibit the cross-linking reaction of bituminous coal compared to[HOEmim][BF_4].Besides,based on Quantum Chemistry calculation,it was found that the different inhibiting effects of |H0Emim][BF_4]and[Amim]Cl are greatly related to their anions and the H linked with C2 atom on the imidazole ring.The H-donor ability of coal will be enhanced by[HOEmim][BF_4]leading to a weaker cross-linking reaction of coal.展开更多
Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium ...Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.展开更多
Polyimide(PI)is widely used in high-frequency communication technology due to its exceptional comprehensive properties.However,traditional PI has a relatively elevated dielectric constant and dielectric loss.Herein,th...Polyimide(PI)is widely used in high-frequency communication technology due to its exceptional comprehensive properties.However,traditional PI has a relatively elevated dielectric constant and dielectric loss.Herein,the different cross-linked structures were introduced in PI matrix and conducted a detailed discussion on the influence of cross-linking agent content and cross-linking structure type on the overall performance of PI films.In comparison to the dielectric constant of 2.9 of neat PI,PI with an interchain cross-linking structure containing 2 wt%1,3,5-tris(4-aminophenyl)benzene(TAPB)(interchain-PI-2)exhibited the reduced dielectric constant of 2.55 at 1 MHz.The PI films with intrachain crosslinking structure containing 2 wt%TAPB(intrachain-PI-2)exhibited the lowest dielectric constant of 2.35 and the minimum dielectric loss of0.0075 at 1 MHz.It was due to the more entanglement junctions of intrachain-PI resulting in decreased carrier transport.The thermal expansion coefficients of both interchain-PI and intrachain-PI films were effectively reduced.Moreover,in contrast to interchain-PI films,the intrachain-PI films maintained colorlessness and transparency as the cross-linking agent content increased.This work compared the effects of two different cross-linked structures on the performance of PI films and provided a feasible way to obtain low-k PI films with excellent comprehensive performance for 5G applications.展开更多
Elastomer blends,among which natural rubber(NR)and butadiene rubber(BR),are involved in many components of the automotive/tire industry.A comprehensive understanding of their mechanical behavior requires,among other f...Elastomer blends,among which natural rubber(NR)and butadiene rubber(BR),are involved in many components of the automotive/tire industry.A comprehensive understanding of their mechanical behavior requires,among other features,a detailed description of the crosslink density in these mixtures.In the case of vulcanized immiscible blends,the distribution of the cross-link density within each of the NR-and BR-rich domains is key information,but difficult to determine using the conventional approaches used for one-component crosslinked elastomers.In this study,the vulcanization within NR/BR blends is investigated using a robust^(1)H double-quantum(DQ)MAS recoupling experiment,BaBa-xy16.Two kinds of cross-linked NR/BR blends were considered with two different microstructures for the BR component.The bulk organization of the resulting blends was first probed by analyzing the^(1)H spin-lattice relaxation behavior.In a second step,BaBa-xy16 was used to investigate,in a selective way,the cross-link heterogeneities within NR/BR blends.In particular,for immiscible NR/BR mixtures,the distribution of the cross-link density between both phases was compared and the observed differences were discussed.展开更多
Ionic Liquid Electrospray Thrusters(ILETs)are well suited for micro-nano satellite applications due to their small size,low power consumption,and high specific impulse.However,the limited thrust of a single-emitter IL...Ionic Liquid Electrospray Thrusters(ILETs)are well suited for micro-nano satellite applications due to their small size,low power consumption,and high specific impulse.However,the limited thrust of a single-emitter ILET restricts its use in space missions.To optimize the performance of ILETs and make them suitable for a wider range of space missions,we designed a Circular-emitter ILET(CILET)to convert a one-dimensional(point)emission into a twodimensional(line)emission.The CILET can self-organize multiple Taylor cones simultaneously.The cones were photographed and the axial emission currents were measured under different voltage and pressure difference conditions with a CILET experimental system.The emission can be divided into two stable states and one unstable state based on the flow and current characteristics.The current in Stable state Ⅰ increases non-linearly with the voltage,while that in Stable state Ⅱ is nearly linear with respect to the voltage.The number of cones increases with the voltage in stable states,while the cones become short and crowded under high-voltage conditions.The variation law of the number of cones can be explained with the self-organization theory.The variation in the current exhibits a good correlation with the number of cones.This study demonstrates the feasibility of circular emitters and experimentally indicates that the emission current is improved by approximately two orders of magnitude compared to that of a single capillary.展开更多
The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we desig...The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we designed a cationic hydrogel named PAPTMA to holistically improve the reversibility of ZIBs.The long cationic branch chains in the polymeric matrix construct express pathways for rapid Zn^(2+)transport through an ionic repulsion mechanism,achieving simultaneously high Zn^(2+)transference number(0.79)and high ionic conductivity(28.7 mS cm−1).Additionally,the reactivity of water in the PAPTMA hydrogels is significantly inhibited,thus possessing a strong resistance to parasitic reactions.Mechanical characterization further reveals the superior tensile and adhesion strength of PAPTMA.Leveraging these properties,symmetric batteries employing PAPTMA hydrogel deliver exceeding 6000 h of reversible cycling at 1 mA cm^(−2) and maintain stable operation for 1000 h with a discharge of depth of 71%.When applied in 4×4 cm2 pouch cells with MnO_(2) as the cathode material,the device demonstrates remarkable operational stability and mechanical robustness through 150 cycles.This work presents an eclectic strategy for designing advanced hydrogels that combine high ionic conductivity,enhanced Zn^(2+)mobility,and strong resistance to parasitic reactions,paving the way for long-lasting flexible ZIBs.展开更多
Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storag...Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storage systems.Among the numerous types of SSEs,inorganic oxide garnet-structured superionic conductors Li7La3Zr2O12(LLZO)crystallized with the cubic Iaˉ3d space group have received considerable attention owing to their highly advantageous intrinsic properties encompassing reasonable lithium-ion conductivity,wide electrochemical voltage window,high shear modulus,and excellent chemical stability with electrodes.However,no SSEs possess all the properties necessary for SSLBs,thus both the ionic conductivity at room temperature and stability in ambient air regarding cubic garnet-based electrolytes are still subject to further improvement.Hence,this review comprehensively covers the nine key structural factors affecting the ion conductivity of garnet-based electrolytes comprising Li concentration,Li vacancy concentration,Li carrier concentration and mobility,Li occupancy at available sites,lattice constant,triangle bottleneck size,oxygen vacancy defects,and Li-O bonding interactions.Furthermore,the general illustration of structures and fundamental features being crucial to chemical stability is examined,including Li concentration,Li-site occupation behavior,and Li-O bonding interactions.Insights into the composition-structure-property relations among cubic garnet-based oxide ionic conductors from the perspective of their crystal structures,revealing the potential compatibility conflicts between ionic transportation and chemical stability resulting from Li-O bonding interactions.We believe that this review will lay the foundation for future reasonable structural design of oxide-based or even other types of superionic conductors,thus assisting in promoting the rapid development of alternative green and sustainable technologies.展开更多
Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-...Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes.Herein,we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide)(Pebax) matrix for efficient separation H_(2)S and CO_(2)from CH_(4).Notably,the optimal permeability of H_(2)S reaches up to 4310 Barrer (40C,0.50 bar) in Pebax/ECPIL membranes,along with H_(2)S/CH_(4)and (H_(2)StCO_(2))/CH_(4)selectivity of 97.7 and 112.3,respectively.These values are increased by 1125%,160.8%and 145.9%compared to those in neat Pebax membrane.Additionally,the solubility and diffusion coefficients of the gases were measured,demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H_(2)S and CO_(2),thus elevating the permeability and permselectivity.By using quantum chemical calculations and FT-IR spectroscopy,the highly reversible multi-site hydrogen bonding interaction between ECPILs and H_(2)S was revealed,which is responsible for the fast permeation of H_(2)S and good selectivity.Furthermore,H_(2)S/CO_(2)/CH_(4)(3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h.Overall,this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H_(2)S and CO_(2),but may also provide a novel insight into the design of membrane materials for natural gas upgrading.展开更多
Small-sized Cd_(x) Zn_(1-x) S solid solution nanomaterial is an important candidate for efficient photocatalytic hydrogen evolution(PHE),but it still suffers from easy agglomeration,severe photo corrosion,and fast pho...Small-sized Cd_(x) Zn_(1-x) S solid solution nanomaterial is an important candidate for efficient photocatalytic hydrogen evolution(PHE),but it still suffers from easy agglomeration,severe photo corrosion,and fast photogenerated electron-hole recombination.To tackle these issues,herein,we propose a new strategy to modify Cd_(x) Zn_(1-x) S nanoreactors by the simultaneous utilization of ionic-liquid-assisted morphology engineering and MXene-incorporating method.That is,we designed and synthesized a novel hierarchi-cal Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) Schottky junction composite through the in-situ deposition of ultrathin Cd_(0.8) Zn_(0.2) S nanosheets on unique IL-modified Ti_(3) C_(2) MXenes by a one-pot solvothermal method for efficiently PHE.The unique construction strategy tailors the thickness of ultrathin Cd_(0.8) Zn_(0.2) S nanosheets and prevents them from stacking and agglomeration,and especially,optimizes their charge transfer pathways during the photocatalytic process.Compared with pristine Cd_(0.8) Zn_(0.2) S nanosheets,Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) has abun-dant photogenerated electrons available on the Ti_(3) C_(2) surface for proton reduction reaction,owing to the absence of deep-trapped electrons,suppression of electron-hole recombination in Cd_(0.8) Zn_(0.2) S and high-efficiency charge separation at the Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) Schottky junction interface.Moreover,the hy-drophilicity,electrical conductivity,visible-light absorption capacity,and surficial hydrogen desorption of Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) heterostructure are significantly improved.As a result,the heterostructure exhibits out-standing photocatalytic stability and super high apparent quantum efficiency,being rendered as one of the best noble-metal-free Cd-Zn-S-based photocatalysts.This work illustrates the mechanisms of mor-phology control and heterojunction construction in controlling the catalytic behavior of photocatalysts and highlights the great potential of the IL-assisted route in the synthesis of high-performance MXene-based heterostructures for photocatalytic hydrogen evolution.展开更多
We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisti...We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisticated techniques to realize nanoscale preparation of high-quality epitaxial oxide thin films.On the other hand,electrochemistry is a simple,very sensitive,and non-destructive analysis technique for solid-liquid interfaces.To ensure the reproducibility in experiment of the interfaces of such epitaxial oxide films,as well as bulk oxide single-crystals,with IL,we employ a home-built PLD-electrochemical(EC)system with IL as an electrolyte.The system allows one to perform all-in-vacuum experiments during the preparation of well-defined oxide electrode surfaces to their electrochemical analyses.The topics include electrochemical evaluations of the oxide’s own properties,such as carrier density and relative permittivity,and the interfacial properties of oxides in contact with IL,such as flat band potential and electric double layer(EDL)capacitance,ending with future perspectives in all-solid-state electrochemistry.展开更多
A series of multi-hydroxyl bis-(quaternary ammonium)ionic liquids(Ils1‒7)was prepared as bifunctional catalysts for the chemical fixation of CO_(2).All these ionic liquid compounds were efficient for the catalytic syn...A series of multi-hydroxyl bis-(quaternary ammonium)ionic liquids(Ils1‒7)was prepared as bifunctional catalysts for the chemical fixation of CO_(2).All these ionic liquid compounds were efficient for the catalytic synthesis of cyclic carbonates and oxazolidinones via the cycloaddition reactions between CO_(2) and epoxides or aziridines with excellent yield and high selectivity in the absence of co-catalyst,metal and solvent.Due to the synergistic effects of hydroxyl groups and halogen anion,the cycloaddition reactions proceeded smoothly either at atmospheric pressure or room temperature.The selectivity for substituted oxazolidinones at 5-and 4-positions can be tuned via changing the reaction conditions.Finally,possible mechanisms including the activation of both CO_(2) and epoxide or aziridines were proposed based on the literatures and experimental results.展开更多
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 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.
基金Supported by Shandong Province Medical Staff Science and Technology Innovation Program Project(No.SDYWZGKCJH2022021).
文摘AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHODS:In this prospectively study,130 patients underwent FS-LASIK or FS-LASIK Xtra for high myopia.Their right eyes were selected for inclusion in the study,of which 65 cases of 65 eyes in the FS-LASIK group,65 patients with 65 eyes in the FS-LASIK Xtra group.Patients were evaluated for corneal densitometry at 1,3,and 6mo postoperatively using Pentacam Scheimpflug imaging.RESULTS:Preoperative differences in corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups in different ranges were not statistically significant(P>0.05).Layer-by-layer analysis revealed statistically significant differences in the anterior(120μm),central,and total layer corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups at 1 and 3mo postoperatively(all P<0.05),the FS-LASIK Xtra group is higher than that of the FS-LASIK group.Analysis of different diameter ranges showed statistically significant differences between the FS-LASIK group and the FS-LASIK Xtra group at 1mo postoperatively in the ranges of 0–2,2–6,and 6–10 mm(both P<0.05);At 3mo postoperatively,the FS-LASIK Xtra group is higher than that of the FS-LASIK group in the ranges of 0–2 and 2–6 mm(P<0.05).At 6mo postoperatively,there were no statistically significant differences in corneal densitometry between the FS-LASIK group and the FS-LASIK Xtra group in different diameter ranges(all P>0.05).CONCLUSION:There is an increase in internal corneal densitometry during the early postoperative period after FS-LASIK Xtra for correction of high myopia.However,the densitometry values decreased to the level of conventional FS-LASIK at 6mo after surgery,with the most significant changes observed in the superficial central zone.
基金the support from the National Natural Science Foundation of China(Nos.51304073and 51304071)the Educational Commission of Henan Province(Nos.13A440324 and 12B440004)+1 种基金the Open Projects of State Key Laboratory of Coal Resources and Safe Mining,China University of Mining and Technology(No.12KF02)Henan Polytechnic University(Nos.B2012-068 and B2012-085)
文摘In order to reduce the hazard of coal spontaneous combustion,the cross-linking reaction between O-containing functional groups of coal should be inhibited.So the inhibitory effect of an ionic liquid(IL) on the cross-linking reaction was studied.The O-containing functional groups change the weight loss and H_2O,CO_2,CO yields of bituminous coal before and after[H0Emim][BF_4]and[Amim]Cl pre-treatment and were detected by Fourier Transform Infrared spectroscopy(FT1R) and Thermo Gravimetric(TC) analysis.The results show that | AmimjCI has a weaker ability to inhibit the cross-linking reaction of bituminous coal compared to[HOEmim][BF_4].Besides,based on Quantum Chemistry calculation,it was found that the different inhibiting effects of |H0Emim][BF_4]and[Amim]Cl are greatly related to their anions and the H linked with C2 atom on the imidazole ring.The H-donor ability of coal will be enhanced by[HOEmim][BF_4]leading to a weaker cross-linking reaction of coal.
基金supported by the National Key Research and Development Program of China(2022YFB4101800)National Natural Science Foundation of China(22278077,22108040)+2 种基金Key Program of Qingyuan Innovation Laboratory(00221004)Research Program of Qingyuan Innovation Laboratory(00523006)Natural Science Foundation of Fujian Province(2022J02019)。
文摘Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.
基金financially supported by the National Natural Science Foundation of China(No.52103029)。
文摘Polyimide(PI)is widely used in high-frequency communication technology due to its exceptional comprehensive properties.However,traditional PI has a relatively elevated dielectric constant and dielectric loss.Herein,the different cross-linked structures were introduced in PI matrix and conducted a detailed discussion on the influence of cross-linking agent content and cross-linking structure type on the overall performance of PI films.In comparison to the dielectric constant of 2.9 of neat PI,PI with an interchain cross-linking structure containing 2 wt%1,3,5-tris(4-aminophenyl)benzene(TAPB)(interchain-PI-2)exhibited the reduced dielectric constant of 2.55 at 1 MHz.The PI films with intrachain crosslinking structure containing 2 wt%TAPB(intrachain-PI-2)exhibited the lowest dielectric constant of 2.35 and the minimum dielectric loss of0.0075 at 1 MHz.It was due to the more entanglement junctions of intrachain-PI resulting in decreased carrier transport.The thermal expansion coefficients of both interchain-PI and intrachain-PI films were effectively reduced.Moreover,in contrast to interchain-PI films,the intrachain-PI films maintained colorlessness and transparency as the cross-linking agent content increased.This work compared the effects of two different cross-linked structures on the performance of PI films and provided a feasible way to obtain low-k PI films with excellent comprehensive performance for 5G applications.
基金financial support from the French National Research Agency(ANR)[grant number ANR-22-CE06-0031]。
文摘Elastomer blends,among which natural rubber(NR)and butadiene rubber(BR),are involved in many components of the automotive/tire industry.A comprehensive understanding of their mechanical behavior requires,among other features,a detailed description of the crosslink density in these mixtures.In the case of vulcanized immiscible blends,the distribution of the cross-link density within each of the NR-and BR-rich domains is key information,but difficult to determine using the conventional approaches used for one-component crosslinked elastomers.In this study,the vulcanization within NR/BR blends is investigated using a robust^(1)H double-quantum(DQ)MAS recoupling experiment,BaBa-xy16.Two kinds of cross-linked NR/BR blends were considered with two different microstructures for the BR component.The bulk organization of the resulting blends was first probed by analyzing the^(1)H spin-lattice relaxation behavior.In a second step,BaBa-xy16 was used to investigate,in a selective way,the cross-link heterogeneities within NR/BR blends.In particular,for immiscible NR/BR mixtures,the distribution of the cross-link density between both phases was compared and the observed differences were discussed.
基金co-supported by the National Key R&D Program of China(No.2020YFC2201001)the Shenzhen Science and Technology Program,China(No.20210623091808026)。
文摘Ionic Liquid Electrospray Thrusters(ILETs)are well suited for micro-nano satellite applications due to their small size,low power consumption,and high specific impulse.However,the limited thrust of a single-emitter ILET restricts its use in space missions.To optimize the performance of ILETs and make them suitable for a wider range of space missions,we designed a Circular-emitter ILET(CILET)to convert a one-dimensional(point)emission into a twodimensional(line)emission.The CILET can self-organize multiple Taylor cones simultaneously.The cones were photographed and the axial emission currents were measured under different voltage and pressure difference conditions with a CILET experimental system.The emission can be divided into two stable states and one unstable state based on the flow and current characteristics.The current in Stable state Ⅰ increases non-linearly with the voltage,while that in Stable state Ⅱ is nearly linear with respect to the voltage.The number of cones increases with the voltage in stable states,while the cones become short and crowded under high-voltage conditions.The variation law of the number of cones can be explained with the self-organization theory.The variation in the current exhibits a good correlation with the number of cones.This study demonstrates the feasibility of circular emitters and experimentally indicates that the emission current is improved by approximately two orders of magnitude compared to that of a single capillary.
基金financially supported by the General Research Fund(CityU 11315622 and CityU 11310123)National Natural Science Foundation(NSFC 52372229 and NSFC 52172241)+3 种基金Green Tech Fund(GTF202220105)Guangdong Basic and Applied Basic Research Foundation(2024A1515011008)City University of Hong Kong(No.9020002)the Shenzhen Research Institute of City University of Hong Kong.
文摘The development of flexible zinc-ion batteries(ZIBs)faces a threeway trade-off among the ionic conductivity,Zn^(2+)mobility,and the electrochemical stability of hydrogel electrolytes.To address this challenge,we designed a cationic hydrogel named PAPTMA to holistically improve the reversibility of ZIBs.The long cationic branch chains in the polymeric matrix construct express pathways for rapid Zn^(2+)transport through an ionic repulsion mechanism,achieving simultaneously high Zn^(2+)transference number(0.79)and high ionic conductivity(28.7 mS cm−1).Additionally,the reactivity of water in the PAPTMA hydrogels is significantly inhibited,thus possessing a strong resistance to parasitic reactions.Mechanical characterization further reveals the superior tensile and adhesion strength of PAPTMA.Leveraging these properties,symmetric batteries employing PAPTMA hydrogel deliver exceeding 6000 h of reversible cycling at 1 mA cm^(−2) and maintain stable operation for 1000 h with a discharge of depth of 71%.When applied in 4×4 cm2 pouch cells with MnO_(2) as the cathode material,the device demonstrates remarkable operational stability and mechanical robustness through 150 cycles.This work presents an eclectic strategy for designing advanced hydrogels that combine high ionic conductivity,enhanced Zn^(2+)mobility,and strong resistance to parasitic reactions,paving the way for long-lasting flexible ZIBs.
基金supported by the National Natural Science Foundation of China(Nos.22171102 and 22090044)the National Key R&D Program of China(Nos.2021YFF0500502 and 2023YFA1506304)+2 种基金the Jilin Province Science and Technology Development Plan(No.20230101024JC)the"Medicine+X"crossinnovation team of Bethune Medical Department of Jilin University"Leading the Charge with Open Competition"construction project(No.2022JBGS04)the Jilin University Graduate Training Office(Nos.2021JGZ08 and 2022YJSJIP20).
文摘Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storage systems.Among the numerous types of SSEs,inorganic oxide garnet-structured superionic conductors Li7La3Zr2O12(LLZO)crystallized with the cubic Iaˉ3d space group have received considerable attention owing to their highly advantageous intrinsic properties encompassing reasonable lithium-ion conductivity,wide electrochemical voltage window,high shear modulus,and excellent chemical stability with electrodes.However,no SSEs possess all the properties necessary for SSLBs,thus both the ionic conductivity at room temperature and stability in ambient air regarding cubic garnet-based electrolytes are still subject to further improvement.Hence,this review comprehensively covers the nine key structural factors affecting the ion conductivity of garnet-based electrolytes comprising Li concentration,Li vacancy concentration,Li carrier concentration and mobility,Li occupancy at available sites,lattice constant,triangle bottleneck size,oxygen vacancy defects,and Li-O bonding interactions.Furthermore,the general illustration of structures and fundamental features being crucial to chemical stability is examined,including Li concentration,Li-site occupation behavior,and Li-O bonding interactions.Insights into the composition-structure-property relations among cubic garnet-based oxide ionic conductors from the perspective of their crystal structures,revealing the potential compatibility conflicts between ionic transportation and chemical stability resulting from Li-O bonding interactions.We believe that this review will lay the foundation for future reasonable structural design of oxide-based or even other types of superionic conductors,thus assisting in promoting the rapid development of alternative green and sustainable technologies.
基金sponsored by the National Natural Science Foundation of China (Nos. 22308145, 22208140, 22178159, 22078145)Natural Science Foundation of Jiangsu Province (BK20230791)Postgraduate Research Innovation Program of Jiangsu Province (KYCX24_0165)。
文摘Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes.Herein,we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide)(Pebax) matrix for efficient separation H_(2)S and CO_(2)from CH_(4).Notably,the optimal permeability of H_(2)S reaches up to 4310 Barrer (40C,0.50 bar) in Pebax/ECPIL membranes,along with H_(2)S/CH_(4)and (H_(2)StCO_(2))/CH_(4)selectivity of 97.7 and 112.3,respectively.These values are increased by 1125%,160.8%and 145.9%compared to those in neat Pebax membrane.Additionally,the solubility and diffusion coefficients of the gases were measured,demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H_(2)S and CO_(2),thus elevating the permeability and permselectivity.By using quantum chemical calculations and FT-IR spectroscopy,the highly reversible multi-site hydrogen bonding interaction between ECPILs and H_(2)S was revealed,which is responsible for the fast permeation of H_(2)S and good selectivity.Furthermore,H_(2)S/CO_(2)/CH_(4)(3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h.Overall,this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H_(2)S and CO_(2),but may also provide a novel insight into the design of membrane materials for natural gas upgrading.
基金financial supports pro-vided by the National Natural Science Foundation of China(No.21905279)the Natural Science Foundation of Fujian Province(No.2020J05086).
文摘Small-sized Cd_(x) Zn_(1-x) S solid solution nanomaterial is an important candidate for efficient photocatalytic hydrogen evolution(PHE),but it still suffers from easy agglomeration,severe photo corrosion,and fast photogenerated electron-hole recombination.To tackle these issues,herein,we propose a new strategy to modify Cd_(x) Zn_(1-x) S nanoreactors by the simultaneous utilization of ionic-liquid-assisted morphology engineering and MXene-incorporating method.That is,we designed and synthesized a novel hierarchi-cal Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) Schottky junction composite through the in-situ deposition of ultrathin Cd_(0.8) Zn_(0.2) S nanosheets on unique IL-modified Ti_(3) C_(2) MXenes by a one-pot solvothermal method for efficiently PHE.The unique construction strategy tailors the thickness of ultrathin Cd_(0.8) Zn_(0.2) S nanosheets and prevents them from stacking and agglomeration,and especially,optimizes their charge transfer pathways during the photocatalytic process.Compared with pristine Cd_(0.8) Zn_(0.2) S nanosheets,Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) has abun-dant photogenerated electrons available on the Ti_(3) C_(2) surface for proton reduction reaction,owing to the absence of deep-trapped electrons,suppression of electron-hole recombination in Cd_(0.8) Zn_(0.2) S and high-efficiency charge separation at the Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) Schottky junction interface.Moreover,the hy-drophilicity,electrical conductivity,visible-light absorption capacity,and surficial hydrogen desorption of Cd_(0.8) Zn_(0.2) S/Ti_(3) C_(2) heterostructure are significantly improved.As a result,the heterostructure exhibits out-standing photocatalytic stability and super high apparent quantum efficiency,being rendered as one of the best noble-metal-free Cd-Zn-S-based photocatalysts.This work illustrates the mechanisms of mor-phology control and heterojunction construction in controlling the catalytic behavior of photocatalysts and highlights the great potential of the IL-assisted route in the synthesis of high-performance MXene-based heterostructures for photocatalytic hydrogen evolution.
文摘We introduce our state-of-the art of“vacuum consistent electrochemistry”to an investigation of the interfaces between oxides and ionic liquid(IL).Pulsed laser deposition(PLD)has been one of the powerful and sophisticated techniques to realize nanoscale preparation of high-quality epitaxial oxide thin films.On the other hand,electrochemistry is a simple,very sensitive,and non-destructive analysis technique for solid-liquid interfaces.To ensure the reproducibility in experiment of the interfaces of such epitaxial oxide films,as well as bulk oxide single-crystals,with IL,we employ a home-built PLD-electrochemical(EC)system with IL as an electrolyte.The system allows one to perform all-in-vacuum experiments during the preparation of well-defined oxide electrode surfaces to their electrochemical analyses.The topics include electrochemical evaluations of the oxide’s own properties,such as carrier density and relative permittivity,and the interfacial properties of oxides in contact with IL,such as flat band potential and electric double layer(EDL)capacitance,ending with future perspectives in all-solid-state electrochemistry.
文摘A series of multi-hydroxyl bis-(quaternary ammonium)ionic liquids(Ils1‒7)was prepared as bifunctional catalysts for the chemical fixation of CO_(2).All these ionic liquid compounds were efficient for the catalytic synthesis of cyclic carbonates and oxazolidinones via the cycloaddition reactions between CO_(2) and epoxides or aziridines with excellent yield and high selectivity in the absence of co-catalyst,metal and solvent.Due to the synergistic effects of hydroxyl groups and halogen anion,the cycloaddition reactions proceeded smoothly either at atmospheric pressure or room temperature.The selectivity for substituted oxazolidinones at 5-and 4-positions can be tuned via changing the reaction conditions.Finally,possible mechanisms including the activation of both CO_(2) and epoxide or aziridines were proposed based on the literatures and experimental results.
