NiFe-layered double hydroxides(NiFe-LDHs)are among the most promising earth-abundant electrocatalysts for the oxygen evolution reaction(OER)in alkaline media.However,their practical application is hindered by intrinsi...NiFe-layered double hydroxides(NiFe-LDHs)are among the most promising earth-abundant electrocatalysts for the oxygen evolution reaction(OER)in alkaline media.However,their practical application is hindered by intrinsic activity limitations and poor stability,primarily due to the asymmetric adsorption of oxygen intermediates.To overcome this,the binding strength must be synergistically tuned to a moderate level to optimize catalytic performance.Here,we engineered NiFeCoCr LDH through Co doping to enhance electrical conductivity and controlled Cr leaching to introduce cationic vacancies for modulating intermediate binding strength in NiFe LDH.X-ray absorption near-edge structure and extended X-ray absorption fine structure analyses reveal that NiFe-LDH with Co doping and Cr vacancies modulates the Ni oxidation state and local coordination environment,leading to a balanced electronic structure and enhanced structural complexity around the Ni sites.Additionally,these vacancies can trap OH^(-)/H_(2)O species,which can serve as a reservoir for OH^(-) transfer,facilitating the rapid formation of OER intermediates and enhancing catalytic performance at high current densities.As a result,V_(Cr)-NiFeCo LDH achieves 1.6 A cm^(-2)current density at 1.7 V vs.RHE while maintaining stable operation for over 1000 h at 500 mA cm^(-2).Density functional theory(DFT)calculations validate the synergistic effects of Co doping and Cr-induced vacancies on intermediate binding energies and improved OER kinetics.Overall,this work presents a rational design strategy to simultaneously enhance the activity and durability of NiFe-based OER catalysts for their application in high-performance alkaline water electrolysis.展开更多
The development of synthetic hybrid biological systems integrating photosynthetic organisms with organic-abiotic functional materials holds significant promise for enhancing photosynthetic processes.The artificial reg...The development of synthetic hybrid biological systems integrating photosynthetic organisms with organic-abiotic functional materials holds significant promise for enhancing photosynthetic processes.The artificial regulation of the state transition between photosystem I(PSI)and photosystem II(PSII)represents a strategic and promising approach for improving the efficiency of natural photosynthesis.In this study,we demonstrate that poly(benzimidazolium-phenylthiophene)(CP4)featuring a flexible cationic backbone exhibits superior ultraviolet light-harvesting capability.The polymer CP4 enhanced PSI activity in Chlorella pyrenoidosa(C.pyrenoidosa),subsequently promoting PSII activity and augmenting overall photosynthetic performance.During light-dependent reactions,CP4 significantly accelerated photosynthetic electron transfer,resulting in a 330%increase in the production of oxygen and 93%and 96%increases in the ATP and NADPH contents,respectively.In the context of dark reactions,CP4 facilitated the conversion and utilization of light energy,leading to a 6%increase in both carbohydrate and protein contents.These findings indicate that synthetic light-harvesting polymer materials exhibit considerable application potential in the field of biomass production through enhancement of natural photosynthetic efficiency.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
Dendrite growth represents one of the most significant challenges that impede the development of aqueous zinc-ion batteries.Herein,Gd^(3+)ions are introduced into conventional electrolytes as a microlevelling agent to...Dendrite growth represents one of the most significant challenges that impede the development of aqueous zinc-ion batteries.Herein,Gd^(3+)ions are introduced into conventional electrolytes as a microlevelling agent to achieve dendrite-free zinc electrodeposition.Simulation and experimental results demonstrate that these Gd^(3+)ions are preferentially adsorbed onto the zinc surface,which enables dendritefree zinc anodes by activating the microlevelling effect during electrodeposition.In addition,the Gd^(3+)additives effectively inhibit side reactions and facilitate the desolvation of[Zn(H_(2)O)_(6)]^(2+),leading to highly reversible zinc plating/stripping.Due to these improvements,the zinc anode demonstrates a significantly prolonged cycle life of 2100 h and achieves an exceptional average Coulombic efficiency of 99.72%over 1400 cycles.More importantly,the Zn//NH_(4)V_(4)O_(10)full cell shows a high capacity retention rate of 85.6%after 1000 cycles.This work not only broadens the application of metallic cations in battery electrolytes but also provides fundamental insights into their working mechanisms.展开更多
The rapid advancement of modern science and technology,coupled with the recent surge in new-energy electric vehicles,has significantly boosted the demand for lithium.This has promoted the development and efficient uti...The rapid advancement of modern science and technology,coupled with the recent surge in new-energy electric vehicles,has significantly boosted the demand for lithium.This has promoted the development and efficient utilization of lepidolite as a lithium source.Therefore,the processes for the flotation of lepidolite have been studied in depth,particularly the development and use of lepidolite flotation collectors and the action mechanism of the collectors on the lepidolite surface.Based on the crystal-structure characteristics of lepidolite minerals,this review focuses on the application of anionic collectors,amine cationic collectors(primary amines,quaternary ammonium salts,ether amines,and Gemini amines),and combined collectors to the flotation behavior of lepidolite as well as the adsorption mechanisms.New directions and technologies for the controllable flotation of lepidolite are proposed,including process improvement,reagent synthesis,and mechanistic research.This analysis demonstrates the need for the further study of the complex environment inside lepidolite and pulp.By using modern analytical detection methods and quantum chemical calculations,research on reagents for the flotation of lepidolite has expanded,providing new concepts and references for the efficient flotation recovery and utilization of lepidolite.展开更多
Posaconazole(PCZ)is a broad-spectrum anti-fungal drug approved by FDA and currently used off-label for the treatment of fungal keratitis(FK).Although ocular route serves as the most bioavailable route for treating FK,...Posaconazole(PCZ)is a broad-spectrum anti-fungal drug approved by FDA and currently used off-label for the treatment of fungal keratitis(FK).Although ocular route serves as the most bioavailable route for treating FK,delivery of PCZ to the eye remains a challenge due to poor permeation though the cornea and rapid elimination from the eye.Here we outline a comprehensive formulation development process,beginning with in silico studies,progressing through in vitro evaluations,and ultimately achieving therapeutic benefits in vivo.We report modified niosome-like surfactant vesicles,hereafter termed as NioTherms,formulated using a novel and simple heat-mix method,encapsulating PCZ for ocular administration in the form of an in situ gel.Excipient screening performed using in silico simulations highly correlate with in vitro studies(R^(2)=0.77),guiding optimization by Quality by Design(QbD)approach for encapsulating PCZ in NioTherms resulting in particles with an average size of 180.7±2.3 nm,zeta potential of +27.5±2.2 mV and entrapment efficiency of 87.6%±1.7%.A 2-fold increase in both mucin binding and cellular uptake indicates a functional role of positive surface charge in enhancingmucoadhesive properties of PCZ-NioTherms.In an in vivo murine ocular keratitis model,we demonstrate a 2-fold enhancement in trans-corneal permeability of PCZ-NioTherms and a 3-fold reduction in fungal burden compared to the control standard of care,the PCZ solution.Owing to a facile formulation process,we anticipate that PCZ-NioTherms would serve as a clinically translatable and patient compliant therapeutic intervention for treating FK.展开更多
Developing cost-effective single-crystalline Ni-rich Co-poor cathodes operating at high-voltage is one of the most important ways to achieve higher energy Li-ion batteries. However, the Li/O loss and Li/Ni mixing unde...Developing cost-effective single-crystalline Ni-rich Co-poor cathodes operating at high-voltage is one of the most important ways to achieve higher energy Li-ion batteries. However, the Li/O loss and Li/Ni mixing under high-temperature lithiation result in electrochemical kinetic hysteresis and structural instability. Herein, we report a highly-ordered single-crystalline LiNi0.85Co0.05Mn0.10O2(NCM85) cathode by doping K+and F-ions. To be specific, the K-ion as a fluxing agent can remarkably decrease the solid-state lithiation temperature by ~30°C, leading to less Li/Ni mixing and oxygen vacancy. Meanwhile, the strong transitional metal(TM)-F bonds are helpful for enhancing de-/lithiation kinetics and limiting the lattice oxygen escape even at 4.5 V high-voltage. Their advantages synergistically endow the single-crystalline NCM85 cathode with a very high reversible capacity of 222.3 mAh g-1. A superior capacity retention of 91.3% is obtained after 500 times at 1 C in pouch-type full cells, and a prediction value of 75.3% is given after cycling for 5000 h. These findings are reckoned to expedite the exploitation and application of high-voltage single-crystalline Ni-rich cathodes for next-generation Li-ion batteries.展开更多
Living cationic polymerization of 4-acetoxystyrene(STO)was conducted in CH_(2)Cl_(2) at-15℃ using a dicumyl chloride(DCC)/SnCl_(4)/nBu_(4)NBr initiating system.Impurity moisture initiation was inhibited by adding pro...Living cationic polymerization of 4-acetoxystyrene(STO)was conducted in CH_(2)Cl_(2) at-15℃ using a dicumyl chloride(DCC)/SnCl_(4)/nBu_(4)NBr initiating system.Impurity moisture initiation was inhibited by adding proton trap 2,6-di-tert-butylpyridine(DTBP),and the controlled initiation of DCC was confirmed by ^(1)H nuclear magnetic resonance(^(1)H-NMR)spectroscopy and matrix-assisted laser desorption ionization time-offlight mass(MALDI-TOF-MS)spectrometry.The polymerization kinetics were analyzed to for optimizing the polymerization rate.Allyl-telechelic PSTOs(allyl-PSTO-allyl)with molecular weight(Mn)range of 3540–7800 g/mol and narrow molecular weight dispersity(Mw/Mn)about 1.25 were prepared through nucleophilic substitution with allyltrimethylsilane(ATMS)at approximately 40%monomer conversion.The experimental results indicate that the substitution efficiency of ATMS increased with higher ATMS concentration,temperature,and extended reaction time.Nearly unity ally-functionality for allyl-PSTO-allyl was achieved by adding sufficient SnCl_(4) prior to the substitution.展开更多
Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and of...Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and often conflicting requirements of the bulk electrolyte and the electrode-electrolyte interphase.Here,we present a weakly coordinating cationic polymer electrolyte(WCPE)specifically designed to regulate the Li^(+)coordination structure,thereby enabling fast-charging SSLMBs.The WCPE comprises an imidazolium-based polycationic matrix combined with a succinonitrile(SN)-based highconcentration electrolyte.Unlike conventional neutral polymer matrices,the polycationic matrix in the WCPE competes with Li^(+)for interactions with SN,weakening the original coordination between SN and Li^(+).This modulation of SN-Li^(+)interaction improves both Li^(+)conductivity of the WCPE(σ_(Li^(+))=1.29mS cm^(-1))and redox kinetics at the electrode-electrolyte interphase.Consequently,SSLMB cells(comprising LiFePO_(4)cathodes and Li-metal anodes)with the WCPE achieve fast-charging capability(reaching over 80%state of charge within 10 min),outperforming those of previously reported polymer electrolytebased SSLMBs.展开更多
The occurrence,development,and metastasis of tumors often entail abnormal expression of genetic substances.Monitoring and regulating changes in intracellular nucleic acid substances hold promise for achieving accurate...The occurrence,development,and metastasis of tumors often entail abnormal expression of genetic substances.Monitoring and regulating changes in intracellular nucleic acid substances hold promise for achieving accurate tumor diagnosis and effective treatment.However,the effectiveness of integrated tumor diagnosis and treatment based on functional nucleic acids still needs to be improved.In this study,we engineered a multifunctional nucleic acid delivery system grounded in a cationic covalent organic framework carrier.This system not only showcases effective gene silencing but also boasts high sensitivity in detecting miR21 levels within tumor cells,enabling real-time monitoring of tumor gene therapy efficacy.The construction of this integrated functional nucleic acid delivery platform provides new ideas for precise tumor detection and effective tumor treatment.展开更多
Tailoring functional interfacial layers through molecular design of electrolyte additives has emerged as a prevalent strategy to modulate interfacial reactions and stabilize aqueous zinc-ion batteries(AZIBs).In this w...Tailoring functional interfacial layers through molecular design of electrolyte additives has emerged as a prevalent strategy to modulate interfacial reactions and stabilize aqueous zinc-ion batteries(AZIBs).In this work,the effect of alkyl chain-induced conformation evolution in interfacial layers on stabilizing the zinc anode was systematically studied using linear cationic surfactant additives.Based on the electrochemical tests and COMSOL simulations,these additives expanded the electrochemical stability window of electrolytes and formed zincophilic-hydrophobic interfacial layers on the anode surface,thus suppressing side reactions and blocking water erosion.Moreover,the interfacial layers not only increased the nucleation overpotential of zinc ions,thus alleviating the electrolyte concentration polarization,but also restricted the 2D diffusion of zinc ions on the anode surface,thereby inducing uniform deposition of finer zinc particles and inhibiting dendrite growth.Furthermore,theoretical calculations revealed that va rying alkyl chain lengths in cationic surfactants and their adsorption configurations resulted in different interfacial layer thicknesses.Especially the dodecyltrimethylammonium chloride(DTAC),the dodecyl group provided a robust hydrophobic layer,effectively stabilizing the zinc anode.And the Zn‖Zn cell with ZSO-DTAC electrolyte achieved a long lifespan of 2000 h at 1 mA cm^(-2),the Zn‖Cu cell exhibited an excellent Coulombic efficiency of 99.69%at 2 mA cm^(-2).In addition,the Zn‖MnO_(2) full cell delivered an initial capacity of 149.44 mA h g^(-1)at 5 A g^(-1),with 83.02%capacity retention after 2000cycles.This work provided fundamental insights into modulating interfacial conformations and reactions to stabilize zinc anodes by surfactant-type additives,offering practical guidance for electrolyte optimization in high-performance AZIBs.展开更多
Bacterial infections are becoming the second most common cause of death globally and have contributed significantly to morbidity and mortality.Cationic antibacterial polymers containing quaternary ammonium salts have ...Bacterial infections are becoming the second most common cause of death globally and have contributed significantly to morbidity and mortality.Cationic antibacterial polymers containing quaternary ammonium salts have been explored;however,it remains a key scientific challenge for current research to synergistically optimize the conformational relationships between structural surface features,active sites,and properties.In this study,a novel cationic copolymer microsphere with nano-multiple humps(CPMs-nMHs)was constructed through emulsion polymerization and self-assembly in EtOH/H_2O,with 3-methacrylamido-N,N,N-trimethylpropan-1-aminium chloride(MPAC)as the protruding functional component.Meanwhile,different hydrophilic monomers were adjusted to synthesize polymers with varying forms,which offered a significant research foundation for delving deeper into the impact of their morphology on performance.After being characterized by Fourier transform infrared(FTIR)spectroscopy,scanning electron microscopy(SEM),atomic force microscopy(AFM),X-ray photoelectron spectroscopy(XPS),dynamic light scattering(DLS),and thermogravimetric analysis(TG),the obtained CPMs-nMHs were applied to antibacterial activity against Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus).Surprisingly,the synthesized CPMs-nMHs exhibited excellent antibacterial performance,discovering that the antibacterial rates of up to 100%,while the activities of contrast copolymers were low.We considered that the dual cooperation of cationic structures and nano-multiple humps were responsible for the antibacterial capabilities.Taken together,cationic copolymer microspheres with nano-multiple humps provide a promising strategy for enhancing the antibacterial properties of cationic polymers.展开更多
Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been d...Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been developed to create a cation-accelerating electric field on the surface of the cathode to achieve ultrafast Zn^(2+)diffusion kinetics.By employing electrodeposition to coat MoS_(2)on the surface of BaV_(6)O_(16)·3H_(2)O nanowires,the directional builtin electric field generated at the heterointerface acts as a cation accelerator,continuously accelerating Zn^(2+)diffusion into the active material.The optimized Zn^(2+)diffusion coefficient in CC@BaV-V_(6)O_(16)·3H_(2)@MoS_(2)(7.5×10^(8)cm^(2)s^(-1)) surpasses that of most reported V-based cathodes.Simultaneously,MoS_(2)serving as a cathodic armor extends the cycling life of the Zn-CC@BaV_(6)O_(16)·3H_(2)@MoS_(2)full batteries to over 10000 cycles.This work provides valuable insights into optimizing ion diffusion kinetics for high-performance energy storage devices.展开更多
It is well known that cationic polymers have excellent antimicrobial capacity accompanied with high biotoxicity,to reduce biotoxicity needs to decrease the number of cationic groups on polymers,which will influence an...It is well known that cationic polymers have excellent antimicrobial capacity accompanied with high biotoxicity,to reduce biotoxicity needs to decrease the number of cationic groups on polymers,which will influence antimicrobial activity.It is necessary to design a cationic polymer mimic natural antimicrobial peptide with excellent antibacterial activity and low toxicity to solve the above dilemma.Here,we designed and prepared a series of cationic poly(β-amino ester)s(PBAEs)with different cationic contents,and introducing hydrophobic alkyl chain to adjust the balance between antimicrobial activity and biotoxicity to obtain an ideal antimicrobial polymer.The optimum one of synthesized PBAE(hydrophilic cationic monomer:hydrophobic monomer=5:5)was screened by testing cytotoxicity and minimum inhibitory concentration(MIC),which can effectively kill S.aureus and E.coli with PBAE concentration of15μg/m L by a spread plate bacteriostatic method and dead and alive staining test.The way of PBAE killing bacterial was destroying the membrane like natural antimicrobial peptide observed by scanning electron microscopy(SEM).In addition,PBAE did not exhibit hemolysis and cytotoxicity.In particular,from the result of animal tests,the PBAE was able to promote healing of infected wounds from removing mature S.aureus and E.coli on the surface of infected wound.As a result,our work offers a viable approach for designing antimicrobial materials,highlighting the significant potential of PBAE polymers in the field of biomedical materials.展开更多
Lithium-rich layered oxides (LLOs) are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries (LIBs).However,they suffer from voltage decay and low initial ...Lithium-rich layered oxides (LLOs) are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries (LIBs).However,they suffer from voltage decay and low initial Coulombic efficiency (ICE) due to severe structural degradation caused by irreversible O release.Herein,we introduce a three-in-one strategy of increasing Ni and Mn content,along with Li/Ni disordering and TM–O covalency regulation to boost cationic and anionic redox activity simultaneously and thus enhance the electrochemical activity of LLOs.The target material,Li_(1.2)Ni_(0.168)Mn_(0.558)Co_(0.074)O_(2)(L1),exhibits an improved ICE of 87.2%and specific capacity of 293.2 mA h g^(-1)and minimal voltage decay of less than 0.53 m V cycle-1over 300 cycles at 1C,compared to Li_(1.2)Ni_(0.13)Mn_(0.54)Co_(0.13)O_(2)(Ls)(274.4 mA h g^(-1)for initial capacity,73.8%for ICE and voltage decay of 0.84 mV/cycle over 300 cycles at 1C).Theoretical calculations reveal that the density of states (DOS) area near the Fermi energy level for L1 is larger than that of Ls,indicating higher anionic and cationic redox reactivity than Ls.Moreover,L1 exhibits increased O-vacancy formation energy due to higher Li/Ni disordering of 4.76%(quantified by X-ray diffraction Rietveld refinement) and enhanced TM–O covalency,making lattice O release more difficult and thus improving electrochemical stability.The increased Li/Ni disordering also leads to more Ni^(2+)presence in the Li layer,which acts as a pillar during Li+de-embedding,improving structural stability.This research not only presents a viable approach to designing low-Co LLOs with enhanced capacity and ICE but also contributes significantly to the fundamental understanding of structural regulation in high-performance LIB cathodes.展开更多
Cataract is the leading cause of reversible blindness worldwide,affecting millions,particularly the elderly.Over 65 million people suffer from significant visual impairment due to cataracts,with the burden being highe...Cataract is the leading cause of reversible blindness worldwide,affecting millions,particularly the elderly.Over 65 million people suffer from significant visual impairment due to cataracts,with the burden being highest in low-and middle-income countries where access to surgery is limited.Cataract surgery,one of the most commonly performed and cost-effective procedures,has evolved significantly.Traditional extracapsular cataract extraction(ECCE)has been largely replaced by phacoemulsifi cation,which uses ultrasonic energy through a small incision,reducing recovery time and complications.More recently,femtosecond laser-assisted cataract surgery(FLACS)has emerged,off ering enhanced precision but with ongoing evaluation of its cost-eff ectiveness.Intraocular lenses(IOLs)now allow for customized visual outcomes,addressing distance,near,and intermediate vision.Despite its safety,cataract surgery can still result in complications such as corneal edema and posterior capsular opacifi cation,requiring careful surgical management and patient education.展开更多
Sodium layered oxides stand out as one of the most promising cathodes for sodium-ion batteries due to their high energy density,elemental abundance,and scalability.However,their practical applications are restricted b...Sodium layered oxides stand out as one of the most promising cathodes for sodium-ion batteries due to their high energy density,elemental abundance,and scalability.However,their practical applications are restricted by interplanar gliding,cation migration,and the formation of intragranular microcracks,which collectively lead to rapid structural degradation and capacity loss.Herein,we rationally design an ultrastable O3-type Na_(0.94)Ca_(0.03)Ni_(1/3)Fe_(1/3)Mn_(1/3)O_(2) cathode,in which Ca^(2+)cations act as pillars within the NaO_(2)slabs,suppressing the irreversible phase transitions and Na/TM cation migration commonly observed in layered oxides.Multiscale in situ and ex situ techniques,combined with post-mortem analysis,reveal that the Ca-pillared pinning effect not only effectively suppresses the interplanar gliding and stress accumulation within the crystal phase but also restrains Na/TM cation migration and surface reconstruction in near-surface regions.Benefiting from the combined effects of structural stabilization,the Ca-pillared cathode exhibits a superior cycling stability,retaining 81.6%of its capacity after 1000 cycles at 2 C within the voltage range of 2.0-4.0 V,along with significantly enhanced wide-temperature(from-40 to 80℃)performance.This work highlights another critical role of Ca pillars in suppressing cation migration and surface structural degradation beyond preventing adverse interplanar gliding,offering valuable insights for designing long-life and wide-temperature layered oxide cathodes.展开更多
Converting CO_(2) into methanol(CH_(3)OH),a high-value-added liquid-phase product,through efficient and highly selective photocatalysis remains a significant challenge.Herein,we present a straightforward cation exchan...Converting CO_(2) into methanol(CH_(3)OH),a high-value-added liquid-phase product,through efficient and highly selective photocatalysis remains a significant challenge.Herein,we present a straightforward cation exchange strategy for the in-situ growth of BiVO_(4) on an InVO_(4) substrate to generate a Z-scheme heterojunction of InVO_(4)/BiVO_(4) .This in-situ partial transformation approach endows the InVO_(4)/BiVO_(4) heterojunction with a tightly connected interface,resulting in a significant improvement in charge separation efficiency between InVO_(4) and BiVO_(4).Moreover,the construction of the heterojunction reduces the formation energy barrier of the ^(*)COOH intermediate during the photoreduction of CO_(2) and increases the desorption energy barrier of the ^(*)CO intermediate,facilitating the deep reduction of ^(*)CO.Consequently,the InVO_(4)/BiVO_(4) heterojunction is capable of photocatalytic CO_(2) reduction to CH_(3)OH with high efficiency and selectivity.Under conditions where water serves as the electron source and a light intensity of 100 m W/cm^(2),the yield of CH_(3)OH reaches 130.5 μmol g^(-1)h^(-1) with a selectivity of 92 %,outperforming photocatalysts reported under similar conditions.展开更多
Background:Home accessibility modifi cations are crucial for promoting independent living and quality of life among persons with disabilities.While developed countries have established comprehensive policy frameworks,...Background:Home accessibility modifi cations are crucial for promoting independent living and quality of life among persons with disabilities.While developed countries have established comprehensive policy frameworks,developing nations like China face unique challenges in program design and implementation.Objective:This study conducts a systematic comparative analysis of home accessibility modification policies across China,Japan,Germany,and Sweden,identifying key policy dimensions and proposing evidence-based recommendations for strengthening China’s policy framework.Methods:We employed a multi-dimensional analytical framework examining legislative foundations,eligibility criteria,funding mechanisms,and service delivery models.Data were collected from primary legislation,governmental regulations,official statistics,and peer-reviewed literature.Results:Significant cross-national variations exist in policy approaches.Japan and Germany utilize social insurance models with standardized assessments,Sweden adopts a universal rights-based approach,while China employs a targeted assistance model focused on economically disadvantaged households.China completed 1.28 million household renovations during its 14th Five-Year Plan,demonstrating strong implementation capacity;future policy refi nement could draw on international experience to strengthen assessment standardization,broaden eff ective coverage,and improve the sustainability of fi nancing.Conclusions:China can benefi t from international experience in developing standardized assessment protocols,diversifying funding mechanisms,and establishing professional service delivery systems,while acknowledging contextual constraints unique to developing country settings.展开更多
The scaling-up of electrochemical CO_(2)reduction requires circumventing the CO_(2)loss as carbonates under alkaline conditions.Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative...The scaling-up of electrochemical CO_(2)reduction requires circumventing the CO_(2)loss as carbonates under alkaline conditions.Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative solution in a pure acidic system,but the catalyst layer in direct contact with the hydrated proton environment usually leads to H_(2)evolution dominating.Herein,we show that polydimethyldiallyl-ammonium-chloride-coated Ag(Ag@PDDA)electrode exhibits outstanding performance with a FE of 86%,a single-pass conversion of 72%,and a stability of 28 h for CO production in pure-acid MEA compared with ammonium poly(N-methyl-piperidine-co-pterphenyl)decorated Ag(Ag/QAPPT)and cetyltrimethylammonium bromide decorated Ag(Ag/CTAB).The in situ ATR-SEIRAS reveal that PDDA creates a positive charge-rich protective outer layer and an N-rich hybrid inner layer,which not only suppresses the migration of H+during the electrolysis process and blocks the direct contact between H2O and Ag catalyst,but also promotes the generation from CO_(2)to*COOH in a pure-acid system.This work highlights the importance of polyelectrolyte engineering in regulating the electrocatalytic interface and accelerates the development of proton exchange membrane CO_(2)electrolysis.展开更多
基金supported by the Natural Science Foundation of China Grant No.52272289 and 5240223,and JSPS(Japan Society for the Promotion of Science)of Grant No.22K19088,23H00313,24H02202,and 24H02205。
文摘NiFe-layered double hydroxides(NiFe-LDHs)are among the most promising earth-abundant electrocatalysts for the oxygen evolution reaction(OER)in alkaline media.However,their practical application is hindered by intrinsic activity limitations and poor stability,primarily due to the asymmetric adsorption of oxygen intermediates.To overcome this,the binding strength must be synergistically tuned to a moderate level to optimize catalytic performance.Here,we engineered NiFeCoCr LDH through Co doping to enhance electrical conductivity and controlled Cr leaching to introduce cationic vacancies for modulating intermediate binding strength in NiFe LDH.X-ray absorption near-edge structure and extended X-ray absorption fine structure analyses reveal that NiFe-LDH with Co doping and Cr vacancies modulates the Ni oxidation state and local coordination environment,leading to a balanced electronic structure and enhanced structural complexity around the Ni sites.Additionally,these vacancies can trap OH^(-)/H_(2)O species,which can serve as a reservoir for OH^(-) transfer,facilitating the rapid formation of OER intermediates and enhancing catalytic performance at high current densities.As a result,V_(Cr)-NiFeCo LDH achieves 1.6 A cm^(-2)current density at 1.7 V vs.RHE while maintaining stable operation for over 1000 h at 500 mA cm^(-2).Density functional theory(DFT)calculations validate the synergistic effects of Co doping and Cr-induced vacancies on intermediate binding energies and improved OER kinetics.Overall,this work presents a rational design strategy to simultaneously enhance the activity and durability of NiFe-based OER catalysts for their application in high-performance alkaline water electrolysis.
基金supported by the National Key R&D Program of China(Nos.2023YFC3404200,2023YFC34042012023YFC3404202)+1 种基金the National Natural Science Foundation of China(No.22575253)the Beijing Natural Science Foundation(No.Z220025)。
文摘The development of synthetic hybrid biological systems integrating photosynthetic organisms with organic-abiotic functional materials holds significant promise for enhancing photosynthetic processes.The artificial regulation of the state transition between photosystem I(PSI)and photosystem II(PSII)represents a strategic and promising approach for improving the efficiency of natural photosynthesis.In this study,we demonstrate that poly(benzimidazolium-phenylthiophene)(CP4)featuring a flexible cationic backbone exhibits superior ultraviolet light-harvesting capability.The polymer CP4 enhanced PSI activity in Chlorella pyrenoidosa(C.pyrenoidosa),subsequently promoting PSII activity and augmenting overall photosynthetic performance.During light-dependent reactions,CP4 significantly accelerated photosynthetic electron transfer,resulting in a 330%increase in the production of oxygen and 93%and 96%increases in the ATP and NADPH contents,respectively.In the context of dark reactions,CP4 facilitated the conversion and utilization of light energy,leading to a 6%increase in both carbohydrate and protein contents.These findings indicate that synthetic light-harvesting polymer materials exhibit considerable application potential in the field of biomass production through enhancement of natural photosynthetic efficiency.
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 Scientific Research and Technology Development Project of China National Petroleum Corporation(Grant Nos.2024ZG50,2022DQ03-03)the National Natural Science Foundation of China(Grant Nos.52372252)the Science and Technology Innovation Program of Hunan Province(Grant Nos.2024RC1022).
文摘Dendrite growth represents one of the most significant challenges that impede the development of aqueous zinc-ion batteries.Herein,Gd^(3+)ions are introduced into conventional electrolytes as a microlevelling agent to achieve dendrite-free zinc electrodeposition.Simulation and experimental results demonstrate that these Gd^(3+)ions are preferentially adsorbed onto the zinc surface,which enables dendritefree zinc anodes by activating the microlevelling effect during electrodeposition.In addition,the Gd^(3+)additives effectively inhibit side reactions and facilitate the desolvation of[Zn(H_(2)O)_(6)]^(2+),leading to highly reversible zinc plating/stripping.Due to these improvements,the zinc anode demonstrates a significantly prolonged cycle life of 2100 h and achieves an exceptional average Coulombic efficiency of 99.72%over 1400 cycles.More importantly,the Zn//NH_(4)V_(4)O_(10)full cell shows a high capacity retention rate of 85.6%after 1000 cycles.This work not only broadens the application of metallic cations in battery electrolytes but also provides fundamental insights into their working mechanisms.
基金financially supported by the Excellent Youth Scholars Program of State Key Laboratory of Complex Nonferrous Metal Resource Clean Utilization,Kunming University of Science and Technology,China(No.YXQN-2024003)the Central Government-Guided Local Science and Technology Development Fund Project,China(No.202407AB110022)。
文摘The rapid advancement of modern science and technology,coupled with the recent surge in new-energy electric vehicles,has significantly boosted the demand for lithium.This has promoted the development and efficient utilization of lepidolite as a lithium source.Therefore,the processes for the flotation of lepidolite have been studied in depth,particularly the development and use of lepidolite flotation collectors and the action mechanism of the collectors on the lepidolite surface.Based on the crystal-structure characteristics of lepidolite minerals,this review focuses on the application of anionic collectors,amine cationic collectors(primary amines,quaternary ammonium salts,ether amines,and Gemini amines),and combined collectors to the flotation behavior of lepidolite as well as the adsorption mechanisms.New directions and technologies for the controllable flotation of lepidolite are proposed,including process improvement,reagent synthesis,and mechanistic research.This analysis demonstrates the need for the further study of the complex environment inside lepidolite and pulp.By using modern analytical detection methods and quantum chemical calculations,research on reagents for the flotation of lepidolite has expanded,providing new concepts and references for the efficient flotation recovery and utilization of lepidolite.
文摘Posaconazole(PCZ)is a broad-spectrum anti-fungal drug approved by FDA and currently used off-label for the treatment of fungal keratitis(FK).Although ocular route serves as the most bioavailable route for treating FK,delivery of PCZ to the eye remains a challenge due to poor permeation though the cornea and rapid elimination from the eye.Here we outline a comprehensive formulation development process,beginning with in silico studies,progressing through in vitro evaluations,and ultimately achieving therapeutic benefits in vivo.We report modified niosome-like surfactant vesicles,hereafter termed as NioTherms,formulated using a novel and simple heat-mix method,encapsulating PCZ for ocular administration in the form of an in situ gel.Excipient screening performed using in silico simulations highly correlate with in vitro studies(R^(2)=0.77),guiding optimization by Quality by Design(QbD)approach for encapsulating PCZ in NioTherms resulting in particles with an average size of 180.7±2.3 nm,zeta potential of +27.5±2.2 mV and entrapment efficiency of 87.6%±1.7%.A 2-fold increase in both mucin binding and cellular uptake indicates a functional role of positive surface charge in enhancingmucoadhesive properties of PCZ-NioTherms.In an in vivo murine ocular keratitis model,we demonstrate a 2-fold enhancement in trans-corneal permeability of PCZ-NioTherms and a 3-fold reduction in fungal burden compared to the control standard of care,the PCZ solution.Owing to a facile formulation process,we anticipate that PCZ-NioTherms would serve as a clinically translatable and patient compliant therapeutic intervention for treating FK.
基金supported by the National Natural Science Foundation of China(U22A20429 and 22308103)Shanghai Pilot Program for Basic Research(22TQ1400100-13)+2 种基金Postdoctoral Fellowship Program of CPSF(GZB20230214)China Postdoctoral Science Foundation(2023M731083)the Fundamental Research Funds for the Central Universities.
文摘Developing cost-effective single-crystalline Ni-rich Co-poor cathodes operating at high-voltage is one of the most important ways to achieve higher energy Li-ion batteries. However, the Li/O loss and Li/Ni mixing under high-temperature lithiation result in electrochemical kinetic hysteresis and structural instability. Herein, we report a highly-ordered single-crystalline LiNi0.85Co0.05Mn0.10O2(NCM85) cathode by doping K+and F-ions. To be specific, the K-ion as a fluxing agent can remarkably decrease the solid-state lithiation temperature by ~30°C, leading to less Li/Ni mixing and oxygen vacancy. Meanwhile, the strong transitional metal(TM)-F bonds are helpful for enhancing de-/lithiation kinetics and limiting the lattice oxygen escape even at 4.5 V high-voltage. Their advantages synergistically endow the single-crystalline NCM85 cathode with a very high reversible capacity of 222.3 mAh g-1. A superior capacity retention of 91.3% is obtained after 500 times at 1 C in pouch-type full cells, and a prediction value of 75.3% is given after cycling for 5000 h. These findings are reckoned to expedite the exploitation and application of high-voltage single-crystalline Ni-rich cathodes for next-generation Li-ion batteries.
基金financially supported by the National Natural Science Foundation of China(No.52373011)。
文摘Living cationic polymerization of 4-acetoxystyrene(STO)was conducted in CH_(2)Cl_(2) at-15℃ using a dicumyl chloride(DCC)/SnCl_(4)/nBu_(4)NBr initiating system.Impurity moisture initiation was inhibited by adding proton trap 2,6-di-tert-butylpyridine(DTBP),and the controlled initiation of DCC was confirmed by ^(1)H nuclear magnetic resonance(^(1)H-NMR)spectroscopy and matrix-assisted laser desorption ionization time-offlight mass(MALDI-TOF-MS)spectrometry.The polymerization kinetics were analyzed to for optimizing the polymerization rate.Allyl-telechelic PSTOs(allyl-PSTO-allyl)with molecular weight(Mn)range of 3540–7800 g/mol and narrow molecular weight dispersity(Mw/Mn)about 1.25 were prepared through nucleophilic substitution with allyltrimethylsilane(ATMS)at approximately 40%monomer conversion.The experimental results indicate that the substitution efficiency of ATMS increased with higher ATMS concentration,temperature,and extended reaction time.Nearly unity ally-functionality for allyl-PSTO-allyl was achieved by adding sufficient SnCl_(4) prior to the substitution.
基金supported by the Basic Science Research Program(RS-2024-00344021,RS-2023-00261543,and RS-202300257666)through the National Research Foundation of Korea(NRF),the National Research Council of Science(000)Korea Institute for Advancement of Technology(KIAT)grant funded by the Korea Government(MOTIE)(RS-2024-00420590,HRD Program for Industrial Innovation)The computational resources were provided by KITSI(KSC-2024-CRE-0143)。
文摘Despite the growing interest in fast-cha rging solid-state lithium(Li)-metal batteries(SSLMBs),their practical implementation has yet to be achieved,primarily due to an incomplete understanding of the disparate and often conflicting requirements of the bulk electrolyte and the electrode-electrolyte interphase.Here,we present a weakly coordinating cationic polymer electrolyte(WCPE)specifically designed to regulate the Li^(+)coordination structure,thereby enabling fast-charging SSLMBs.The WCPE comprises an imidazolium-based polycationic matrix combined with a succinonitrile(SN)-based highconcentration electrolyte.Unlike conventional neutral polymer matrices,the polycationic matrix in the WCPE competes with Li^(+)for interactions with SN,weakening the original coordination between SN and Li^(+).This modulation of SN-Li^(+)interaction improves both Li^(+)conductivity of the WCPE(σ_(Li^(+))=1.29mS cm^(-1))and redox kinetics at the electrode-electrolyte interphase.Consequently,SSLMB cells(comprising LiFePO_(4)cathodes and Li-metal anodes)with the WCPE achieve fast-charging capability(reaching over 80%state of charge within 10 min),outperforming those of previously reported polymer electrolytebased SSLMBs.
基金the National Key Research and Development Program of China(No.2021YFB3800900)National Natural Science Foundation of China(No.51925305)the talent cultivation project Funds for the Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(No.HRTP[2022]52)。
文摘The occurrence,development,and metastasis of tumors often entail abnormal expression of genetic substances.Monitoring and regulating changes in intracellular nucleic acid substances hold promise for achieving accurate tumor diagnosis and effective treatment.However,the effectiveness of integrated tumor diagnosis and treatment based on functional nucleic acids still needs to be improved.In this study,we engineered a multifunctional nucleic acid delivery system grounded in a cationic covalent organic framework carrier.This system not only showcases effective gene silencing but also boasts high sensitivity in detecting miR21 levels within tumor cells,enabling real-time monitoring of tumor gene therapy efficacy.The construction of this integrated functional nucleic acid delivery platform provides new ideas for precise tumor detection and effective tumor treatment.
基金funding provided by Cangzhou Institute of Tiangong University(Grant No.TGCYY-F-0301)Hebei Natural Science Foundation,China(Grant No.E2025110039)。
文摘Tailoring functional interfacial layers through molecular design of electrolyte additives has emerged as a prevalent strategy to modulate interfacial reactions and stabilize aqueous zinc-ion batteries(AZIBs).In this work,the effect of alkyl chain-induced conformation evolution in interfacial layers on stabilizing the zinc anode was systematically studied using linear cationic surfactant additives.Based on the electrochemical tests and COMSOL simulations,these additives expanded the electrochemical stability window of electrolytes and formed zincophilic-hydrophobic interfacial layers on the anode surface,thus suppressing side reactions and blocking water erosion.Moreover,the interfacial layers not only increased the nucleation overpotential of zinc ions,thus alleviating the electrolyte concentration polarization,but also restricted the 2D diffusion of zinc ions on the anode surface,thereby inducing uniform deposition of finer zinc particles and inhibiting dendrite growth.Furthermore,theoretical calculations revealed that va rying alkyl chain lengths in cationic surfactants and their adsorption configurations resulted in different interfacial layer thicknesses.Especially the dodecyltrimethylammonium chloride(DTAC),the dodecyl group provided a robust hydrophobic layer,effectively stabilizing the zinc anode.And the Zn‖Zn cell with ZSO-DTAC electrolyte achieved a long lifespan of 2000 h at 1 mA cm^(-2),the Zn‖Cu cell exhibited an excellent Coulombic efficiency of 99.69%at 2 mA cm^(-2).In addition,the Zn‖MnO_(2) full cell delivered an initial capacity of 149.44 mA h g^(-1)at 5 A g^(-1),with 83.02%capacity retention after 2000cycles.This work provided fundamental insights into modulating interfacial conformations and reactions to stabilize zinc anodes by surfactant-type additives,offering practical guidance for electrolyte optimization in high-performance AZIBs.
基金financially supported by the National Natural Science Foundation of China(No.22565027)Gansu International Sci&Techn Coop-Base for Water-Retention Functional Materials and Gansu Provincial Outstanding Graduate Students“Innovation Star”Program(Nos.2025CXZX269 and 2025CXZX-281)。
文摘Bacterial infections are becoming the second most common cause of death globally and have contributed significantly to morbidity and mortality.Cationic antibacterial polymers containing quaternary ammonium salts have been explored;however,it remains a key scientific challenge for current research to synergistically optimize the conformational relationships between structural surface features,active sites,and properties.In this study,a novel cationic copolymer microsphere with nano-multiple humps(CPMs-nMHs)was constructed through emulsion polymerization and self-assembly in EtOH/H_2O,with 3-methacrylamido-N,N,N-trimethylpropan-1-aminium chloride(MPAC)as the protruding functional component.Meanwhile,different hydrophilic monomers were adjusted to synthesize polymers with varying forms,which offered a significant research foundation for delving deeper into the impact of their morphology on performance.After being characterized by Fourier transform infrared(FTIR)spectroscopy,scanning electron microscopy(SEM),atomic force microscopy(AFM),X-ray photoelectron spectroscopy(XPS),dynamic light scattering(DLS),and thermogravimetric analysis(TG),the obtained CPMs-nMHs were applied to antibacterial activity against Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus).Surprisingly,the synthesized CPMs-nMHs exhibited excellent antibacterial performance,discovering that the antibacterial rates of up to 100%,while the activities of contrast copolymers were low.We considered that the dual cooperation of cationic structures and nano-multiple humps were responsible for the antibacterial capabilities.Taken together,cationic copolymer microspheres with nano-multiple humps provide a promising strategy for enhancing the antibacterial properties of cationic polymers.
基金National Natural Science Foundation of China (61761047 and 41876055)Program for Innovative Research Team (in Science and Technology) in University of Yunnan Province。
文摘Aqueous zincion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion migration.To address this,a strategy has been developed to create a cation-accelerating electric field on the surface of the cathode to achieve ultrafast Zn^(2+)diffusion kinetics.By employing electrodeposition to coat MoS_(2)on the surface of BaV_(6)O_(16)·3H_(2)O nanowires,the directional builtin electric field generated at the heterointerface acts as a cation accelerator,continuously accelerating Zn^(2+)diffusion into the active material.The optimized Zn^(2+)diffusion coefficient in CC@BaV-V_(6)O_(16)·3H_(2)@MoS_(2)(7.5×10^(8)cm^(2)s^(-1)) surpasses that of most reported V-based cathodes.Simultaneously,MoS_(2)serving as a cathodic armor extends the cycling life of the Zn-CC@BaV_(6)O_(16)·3H_(2)@MoS_(2)full batteries to over 10000 cycles.This work provides valuable insights into optimizing ion diffusion kinetics for high-performance energy storage devices.
基金financially supported by the Natural Science Foundation of Jilin Province Science and Technology Department(No.20230101221JC)the National Natural Science Foundation of China(Nos.52173115,52073278,52203189)the Research Foundation for Advanced Talents of Xiamen University of Technology(Nos.5010423019,YKJ22052R)。
文摘It is well known that cationic polymers have excellent antimicrobial capacity accompanied with high biotoxicity,to reduce biotoxicity needs to decrease the number of cationic groups on polymers,which will influence antimicrobial activity.It is necessary to design a cationic polymer mimic natural antimicrobial peptide with excellent antibacterial activity and low toxicity to solve the above dilemma.Here,we designed and prepared a series of cationic poly(β-amino ester)s(PBAEs)with different cationic contents,and introducing hydrophobic alkyl chain to adjust the balance between antimicrobial activity and biotoxicity to obtain an ideal antimicrobial polymer.The optimum one of synthesized PBAE(hydrophilic cationic monomer:hydrophobic monomer=5:5)was screened by testing cytotoxicity and minimum inhibitory concentration(MIC),which can effectively kill S.aureus and E.coli with PBAE concentration of15μg/m L by a spread plate bacteriostatic method and dead and alive staining test.The way of PBAE killing bacterial was destroying the membrane like natural antimicrobial peptide observed by scanning electron microscopy(SEM).In addition,PBAE did not exhibit hemolysis and cytotoxicity.In particular,from the result of animal tests,the PBAE was able to promote healing of infected wounds from removing mature S.aureus and E.coli on the surface of infected wound.As a result,our work offers a viable approach for designing antimicrobial materials,highlighting the significant potential of PBAE polymers in the field of biomedical materials.
基金National Natural Science Foundation of China (No.52202046)Natural Science Foundation of Shaanxi Province (No.2021JQ-034)。
文摘Lithium-rich layered oxides (LLOs) are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries (LIBs).However,they suffer from voltage decay and low initial Coulombic efficiency (ICE) due to severe structural degradation caused by irreversible O release.Herein,we introduce a three-in-one strategy of increasing Ni and Mn content,along with Li/Ni disordering and TM–O covalency regulation to boost cationic and anionic redox activity simultaneously and thus enhance the electrochemical activity of LLOs.The target material,Li_(1.2)Ni_(0.168)Mn_(0.558)Co_(0.074)O_(2)(L1),exhibits an improved ICE of 87.2%and specific capacity of 293.2 mA h g^(-1)and minimal voltage decay of less than 0.53 m V cycle-1over 300 cycles at 1C,compared to Li_(1.2)Ni_(0.13)Mn_(0.54)Co_(0.13)O_(2)(Ls)(274.4 mA h g^(-1)for initial capacity,73.8%for ICE and voltage decay of 0.84 mV/cycle over 300 cycles at 1C).Theoretical calculations reveal that the density of states (DOS) area near the Fermi energy level for L1 is larger than that of Ls,indicating higher anionic and cationic redox reactivity than Ls.Moreover,L1 exhibits increased O-vacancy formation energy due to higher Li/Ni disordering of 4.76%(quantified by X-ray diffraction Rietveld refinement) and enhanced TM–O covalency,making lattice O release more difficult and thus improving electrochemical stability.The increased Li/Ni disordering also leads to more Ni^(2+)presence in the Li layer,which acts as a pillar during Li+de-embedding,improving structural stability.This research not only presents a viable approach to designing low-Co LLOs with enhanced capacity and ICE but also contributes significantly to the fundamental understanding of structural regulation in high-performance LIB cathodes.
文摘Cataract is the leading cause of reversible blindness worldwide,affecting millions,particularly the elderly.Over 65 million people suffer from significant visual impairment due to cataracts,with the burden being highest in low-and middle-income countries where access to surgery is limited.Cataract surgery,one of the most commonly performed and cost-effective procedures,has evolved significantly.Traditional extracapsular cataract extraction(ECCE)has been largely replaced by phacoemulsifi cation,which uses ultrasonic energy through a small incision,reducing recovery time and complications.More recently,femtosecond laser-assisted cataract surgery(FLACS)has emerged,off ering enhanced precision but with ongoing evaluation of its cost-eff ectiveness.Intraocular lenses(IOLs)now allow for customized visual outcomes,addressing distance,near,and intermediate vision.Despite its safety,cataract surgery can still result in complications such as corneal edema and posterior capsular opacifi cation,requiring careful surgical management and patient education.
基金supported by the National Key R&D Program of China(2023YFB2406000)the National Natural Science Foundation of China(22479057,52172201,51732005)。
文摘Sodium layered oxides stand out as one of the most promising cathodes for sodium-ion batteries due to their high energy density,elemental abundance,and scalability.However,their practical applications are restricted by interplanar gliding,cation migration,and the formation of intragranular microcracks,which collectively lead to rapid structural degradation and capacity loss.Herein,we rationally design an ultrastable O3-type Na_(0.94)Ca_(0.03)Ni_(1/3)Fe_(1/3)Mn_(1/3)O_(2) cathode,in which Ca^(2+)cations act as pillars within the NaO_(2)slabs,suppressing the irreversible phase transitions and Na/TM cation migration commonly observed in layered oxides.Multiscale in situ and ex situ techniques,combined with post-mortem analysis,reveal that the Ca-pillared pinning effect not only effectively suppresses the interplanar gliding and stress accumulation within the crystal phase but also restrains Na/TM cation migration and surface reconstruction in near-surface regions.Benefiting from the combined effects of structural stabilization,the Ca-pillared cathode exhibits a superior cycling stability,retaining 81.6%of its capacity after 1000 cycles at 2 C within the voltage range of 2.0-4.0 V,along with significantly enhanced wide-temperature(from-40 to 80℃)performance.This work highlights another critical role of Ca pillars in suppressing cation migration and surface structural degradation beyond preventing adverse interplanar gliding,offering valuable insights for designing long-life and wide-temperature layered oxide cathodes.
基金financially supported the National Key R&D Program of China (No.2022YFA1502902)the National Natural Science Foundation of China (NSFC,Nos.22475152 and U21A20286)the 111 Project of China (No.D17003)。
文摘Converting CO_(2) into methanol(CH_(3)OH),a high-value-added liquid-phase product,through efficient and highly selective photocatalysis remains a significant challenge.Herein,we present a straightforward cation exchange strategy for the in-situ growth of BiVO_(4) on an InVO_(4) substrate to generate a Z-scheme heterojunction of InVO_(4)/BiVO_(4) .This in-situ partial transformation approach endows the InVO_(4)/BiVO_(4) heterojunction with a tightly connected interface,resulting in a significant improvement in charge separation efficiency between InVO_(4) and BiVO_(4).Moreover,the construction of the heterojunction reduces the formation energy barrier of the ^(*)COOH intermediate during the photoreduction of CO_(2) and increases the desorption energy barrier of the ^(*)CO intermediate,facilitating the deep reduction of ^(*)CO.Consequently,the InVO_(4)/BiVO_(4) heterojunction is capable of photocatalytic CO_(2) reduction to CH_(3)OH with high efficiency and selectivity.Under conditions where water serves as the electron source and a light intensity of 100 m W/cm^(2),the yield of CH_(3)OH reaches 130.5 μmol g^(-1)h^(-1) with a selectivity of 92 %,outperforming photocatalysts reported under similar conditions.
基金funded by the China Disabled Persons’Federation under its 2024 research project(Grant No.2024CDPFAT-47)the Yancheng Social Science Foundation(Grant No.25skB252).
文摘Background:Home accessibility modifi cations are crucial for promoting independent living and quality of life among persons with disabilities.While developed countries have established comprehensive policy frameworks,developing nations like China face unique challenges in program design and implementation.Objective:This study conducts a systematic comparative analysis of home accessibility modification policies across China,Japan,Germany,and Sweden,identifying key policy dimensions and proposing evidence-based recommendations for strengthening China’s policy framework.Methods:We employed a multi-dimensional analytical framework examining legislative foundations,eligibility criteria,funding mechanisms,and service delivery models.Data were collected from primary legislation,governmental regulations,official statistics,and peer-reviewed literature.Results:Significant cross-national variations exist in policy approaches.Japan and Germany utilize social insurance models with standardized assessments,Sweden adopts a universal rights-based approach,while China employs a targeted assistance model focused on economically disadvantaged households.China completed 1.28 million household renovations during its 14th Five-Year Plan,demonstrating strong implementation capacity;future policy refi nement could draw on international experience to strengthen assessment standardization,broaden eff ective coverage,and improve the sustainability of fi nancing.Conclusions:China can benefi t from international experience in developing standardized assessment protocols,diversifying funding mechanisms,and establishing professional service delivery systems,while acknowledging contextual constraints unique to developing country settings.
基金financial support of the National Natural Science Foundation of China(NSFC)(52394202,52021004,52301232,and 52476056)the Natural Science Foundation of Chongqing Province(2024NSCQ-MSX1109).
文摘The scaling-up of electrochemical CO_(2)reduction requires circumventing the CO_(2)loss as carbonates under alkaline conditions.Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative solution in a pure acidic system,but the catalyst layer in direct contact with the hydrated proton environment usually leads to H_(2)evolution dominating.Herein,we show that polydimethyldiallyl-ammonium-chloride-coated Ag(Ag@PDDA)electrode exhibits outstanding performance with a FE of 86%,a single-pass conversion of 72%,and a stability of 28 h for CO production in pure-acid MEA compared with ammonium poly(N-methyl-piperidine-co-pterphenyl)decorated Ag(Ag/QAPPT)and cetyltrimethylammonium bromide decorated Ag(Ag/CTAB).The in situ ATR-SEIRAS reveal that PDDA creates a positive charge-rich protective outer layer and an N-rich hybrid inner layer,which not only suppresses the migration of H+during the electrolysis process and blocks the direct contact between H2O and Ag catalyst,but also promotes the generation from CO_(2)to*COOH in a pure-acid system.This work highlights the importance of polyelectrolyte engineering in regulating the electrocatalytic interface and accelerates the development of proton exchange membrane CO_(2)electrolysis.
