Carbon materials are considered as prospective anode candidates for potassium ion batteries(PIBs).However,the low-rate capability is hampered by slow K+diffusion kinetics and obstructed electron transport of carbon-ba...Carbon materials are considered as prospective anode candidates for potassium ion batteries(PIBs).However,the low-rate capability is hampered by slow K+diffusion kinetics and obstructed electron transport of carbon-based anodes.In this work,calcium D-gluconate derived mesoporous carbon nanosheets(CGC)were interpenetrated into the architecture of reduced graphene oxides(RGO)to form the composites of two-dimensional(2D)/2D graphene/mesoporous carbon nanosheets(RGO@CGC).CGC as a rigid skeleton can prevent the graphene layers from restacking and maintain the structural stability of the 2D/2D carbon composites of RGO@CGC.The mesopores in CGC can shorten the path of ion diffusion and facilitate the penetration of electrolytes.RGO possesses the high surface-to-volume ratio and superior electron transport capability in the honeycomb-like 2D network consisting of sp^(2)-hybridized carbon atoms.Especially,theπ-πstacking interaction between CGC and RGO enhances stable composite structure formation,expedites interlayer-electron transfer,and establishes three-dimensional(3D)ion transportation pathways.Owing to these unique structure,RGO@CGC exhibits fast and stable potassium storage capability.Furthermore,the effects of binders and electrolytes on the electrochemical performance of RGO@CGC were investigated.Finally,Prussian blue was synthesized as a positive electrode to explore the possibility of RGO@CGC as a full battery application.展开更多
Obesity has become a global threat to health;however,the available drugs for treating obesity are limited.We investigated the anti-obesity effect of hydroxy-α-sanshool(HAS),an amide derived from the fruit of Zanthoxy...Obesity has become a global threat to health;however,the available drugs for treating obesity are limited.We investigated the anti-obesity effect of hydroxy-α-sanshool(HAS),an amide derived from the fruit of Zanthoxylum bungeanum,which promotes the management of obesity by triggering the browning of white adipose tissue(WAT)targeting the membrane receptor of transient receptor potential vanilloid 1(TRPV1).However,HAS easily undergoes configuration transformation and oxidative degradation.The short peptide CKGGRAKDC or adipose-targeting sequence(ATS)binds specifically to prohibitin on the surface of WAT cells and can be used as recognition assembly to enhance adipocyte targetability.Furthermore,mesoporous silica nanoparticles(MSNs)are widely used in drug delivery systems because of their large specific surface area and pore volume.Therefore,HAS-loaded adipose-targeted MSNs(MSNs-ATS)were developed to enhance the adipocyte targetability,safety,and efficacy of HAS,and tested on mature 3T3-L1 cells and obese mouse models.MSNs-ATS showed higher specificity for adipocyte targetability without obvious toxicity.HAS-loaded MSNs-ATS showed anti-obesity effects superior to those of HAS alone.In conclusion,we successfully developed adipocyte-targeted,HAS-loaded MSNs with good safety and anti-obesity effects.展开更多
Due to the high capacity and moderate volume expansion of silicon protoxide SiO_(x)(160%)compared with that of Si(300%),reducing silicon dioxide SiO_(2)into SiO_(x)while maintaining its special nano-morphology makes i...Due to the high capacity and moderate volume expansion of silicon protoxide SiO_(x)(160%)compared with that of Si(300%),reducing silicon dioxide SiO_(2)into SiO_(x)while maintaining its special nano-morphology makes it attractive as an anode of Li-ion batteries.Herein,through a one-pot facile high-temperature annealing route,using SBA15 as the silicon source,and embedding tin dioxide SnO_(2)particles into carbon coated SiO_(x),the mesoporous SiO_(x)-SnO_(2)@C rod composite was prepared and tested as the anode material.The results revealed that the SnO_(2)particles were distributed uniformly in the wall,which could further improve their volume energy densities.The coated carbon plays a role in maintaining structural integrality during lithiation,and the rich mesopores structure can release the expanded volume and enhance Li-ion transfer.At 0.1 A·g^(-1),the gravimetric and volumetric capacities of the composite were as high as 1271 mAh·g^(-1)and 1573 mAh·cm^(-3),respectively.After 200 cycles,the 95%capacity could be retained compared with that upon the 2nd cycle at 0.5 A·g^(-1).And the rod morphology was well kept,except that the diameter of the rod was 3 times larger than its original size after the cell was discharged into 0.01 V.展开更多
Mesoporous carbon supports mitigate platinum(Pt)sulfonic poisoning through nanopore-confined Pt deposition,yet their morphological impacts on oxygen transport remain unclear.This study integrates carbon support morpho...Mesoporous carbon supports mitigate platinum(Pt)sulfonic poisoning through nanopore-confined Pt deposition,yet their morphological impacts on oxygen transport remain unclear.This study integrates carbon support morphology simulation with an enhanced agglomerate model to establish a mathematical framework elucidating pore evolution,Pt utilization,and oxygen transport in catalyst layers.Results demonstrate dominant local mass transport resistance governed by three factors:(1)active site density dictating oxygen flux;(2)ionomer film thickness defining shortest transport path;(3)ionomer-to-Pt surface area ratio modulating practical pathway length.At low ionomer-to-carbon(I/C)ratios,limited active sites elevate resistance(Factor 1 dominant).Higher I/C ratios improve the ionomer coverage but eventually thicken ionomer films,degrading transport(Factors 2–3 dominant).The results indicate that larger carbon particles result in a net increase in local transport resistance by reducing external surface area and increasing ionomer thickness.As the proportion of Pt situated in nanopores or the Pt mass fraction increases,elevated Pt density inside the nanopores exacerbates pore blockage.This leads to the increased transport resistance by reducing active sites,and increasing ionomer thickness and surface area.Lower Pt loading linearly intensifies oxygen flux resistance.The model underscores the necessity to optimize support morphology,Pt distribution,and ionomer content to prevent pore blockage while balancing catalytic activity and transport efficiency.These insights provide a systematic approach for designing high-performance mesoporous carbon catalysts.展开更多
High-efficient rubber antioxidants for enhanced heat resistance without compromising mechanical properties remain an enormous and long-term challenge for the rubber industry.Herein,we employed the in-situ growth of Ce...High-efficient rubber antioxidants for enhanced heat resistance without compromising mechanical properties remain an enormous and long-term challenge for the rubber industry.Herein,we employed the in-situ growth of Ce-doped Co-metal-organic framework(Ce Co-MOF)in dendritic mesoporous organosilica nanoparticles(DMONs@Ce Co-MOF,denoted as DCCM)to prepare a novel antioxidant that exhibit outstanding thermal stability.Dendritic mesoporous organosilica nanoparticles(DMONs)effectively alleviated the incompatibility of Ce Co-MOF in the polymer matrix,and the effective scavenging of free radicals was attributed to the various oxidation states of metal ions in Ce Co-MOF.Surprising,by adding only0.5 phr(parts per hundred of rubber)of DMONs@Ce Co-MOF to silicone rubber,(SR),the retention rate of tensile strength increased from 37.3%to 61.6%after aging 72 h at 250℃,and the retention rate of elongation at break of DCCM/SR1 composites reached 68%,which was 5.43 times of SR.The strategy of anchoring MOFs on the surface of silica also provides a viable method for preparing effective compound functionalized rubber antioxidant.展开更多
Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,...Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn^(2+)as cross-linking and pore-forming agents,followed by KHCO_(3)activation,eliminating the need for toxic phenolic resins and acid treatments for metal removal.Machine learning technology,specifically an Artificial Neural Network(ANN model,was utilized to assist the experimental design and prediction.The ANN model suggested an ideal hierarchical structure and optimized oxygen level,achieved through the adjustment of Zn^(2+)additive concentration,carbonization temperature,and subsequent KHCO_(3)activation to maximize capacitance.The HOMC electrode,with a micropore-to-mesopore ratio(S_(micro)/S_(meso))of 1.01 and an oxygen content of 8.81 at%,acquired a specific capacitance of 362 F·g^(-1)at 0.5 A·g^(-1)in 6 mol·L^(-1)KOH electrolyte.The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg^(-1)with a corresponding specific power density of 300 W·kg^(-1)in TEATFB PC electrolyte.Meanwhile,the long-term cycle stability of 94.33%was achieved after 20,000 cycles.This work provides an ANN assisted strategy for the synthesis of HOMC,highlighting its potential to valorize biomass and agricultural waste in sustainable energy storag solutions.展开更多
To efficiently address the current high cost associated with preparing pseudo-boehmite from organic aluminum,a low-cost alternative,AlCl_(3),is employed as the raw material.The sol-gel method is utilized,and H_(2)O_(2...To efficiently address the current high cost associated with preparing pseudo-boehmite from organic aluminum,a low-cost alternative,AlCl_(3),is employed as the raw material.The sol-gel method is utilized,and H_(2)O_(2)is incorporated for the modification of pseudo-boehmite.The modification mechanism is thoroughly investigated through the use of X-ray powder diffractometer,scanning electron microscope,and BET data analysis,as well as molecular dynamics simulations.Under specific conditions(temperature at 80°C,pH=7,and H_(2)O_(2)volume ratios of 0.5:1,1:1,and 2:1),mesoporous pseudo-boehmite is synthesized with a specific surface area of 227 m^(2)/g,a pore volume of 0.281 cm^(3)/g,a pore size of 6.78 nm,and a peptizing index of 99.47%.A novel and innovative methodology for the cost-effective production of high-performance alumina is offered through the approach.展开更多
Aromatization of light alkanes is a value-added process in both petrochemical and coal chemical industries.Here,single[Ga(OH)]^(2+)ion-exchanged mesoporous hollow-structured ZSM-5(Ga-MH-ZSM-5)material was prepared,and...Aromatization of light alkanes is a value-added process in both petrochemical and coal chemical industries.Here,single[Ga(OH)]^(2+)ion-exchanged mesoporous hollow-structured ZSM-5(Ga-MH-ZSM-5)material was prepared,and it shows unprecedented catalytic performance in light alkane aromatization,considering activity,product selectivity and catalytic stability.The average aromatics yields in ethane aromatization at 600℃and WHSV of 0.8 h^(-1) within 28 h and in propane aromatization at 580℃and WHSV of 1.1 h^(-1) within 20 h reach~18.4%and~70.8%with benzene,toluene and xylenes(BTX)accounting for~96%and~88%of aromatics,respectively.Ga-MH-ZSM-5-0.41 gave a TON for formation of aromatics(TON_(aromatics))from propane as high as 57479,whereas the reported catalysts maximally show a TON_(aromatics) of 5514.This also holds true for ethane aromatization;the TON_(aromatics) obtained on Ga-MH-ZSM-5-0.41 was³3845 in contrast to£392 on reported non-noble metal catalysts.The catalytic activity of Ga-MH-ZSM-5 highly depends on Ga species structures.[Ga(OH)]^(2+)ions are predominant species at Ga loading≤0.3 wt%,while more[Ga(OH)_(2)]^(+)and GaO_(x) oligomers are formed with increasing Ga content.Upon reduction with H_(2),[Ga(OH)]^(2+)and[Ga(OH)_(2)]^(+)are transformed into[GaH]^(2+)and[GaH_(2)]^(+)species,which show a propane dehydrogenation rate of 300 and 15 times of that of Brønsted acid sites respectively.The light alkanes are mainly dehydrogenated into light olefins on[GaH]^(2+)species,and then,oligomerized and cyclized into(alkyl)cycloalkanes on H^(+)sites,which is followed by possible ring expansion on H^(+)and sequential dehydrogenations into aromatics primarily on[GaH]^(2+).展开更多
Confinement effect is an effective method to enhance carbon dioxide(CO_(2))solubility.In this study,a hybrid sorbent of 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([Hmim][NTf_2])/mesoporous titanium ...Confinement effect is an effective method to enhance carbon dioxide(CO_(2))solubility.In this study,a hybrid sorbent of 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([Hmim][NTf_2])/mesoporous titanium dioxide(M-TiO_(2))/water(H_2O)was developed,and its confinement effect was regulated by changing the pore structure of M-TiO_(2).CO_(2) solubility in the hybrid sorbent was measured experimentally,and the thermodynamic properties including Henry's constant and desorption enthalpy were calculated.Furthermore,the confinement effect in the hybrid sorbent was quantified.Additionally,the hybrid sorbent was recycled with a multi-cycle experiment.The results showed that M-TiO_(2) calcined at 773.2 K(MT500)could lead to an efficient confinement effect.CO_(2) solubility in the hybrid sorbent increased by 49.8%compared to that of H_2O when the mass fraction of[Hmim][NTf_2]/MT500 was 5.0%(mass),where the contribution of confinement effect on Gibbs free energy occupied 5.2%.展开更多
Mesoporous silica nanoparticles(MsNs)are thought to be an attractive drug delivery material because of their advantages including high specific surface area,tunable pore size and morphology,easy sur-face modification ...Mesoporous silica nanoparticles(MsNs)are thought to be an attractive drug delivery material because of their advantages including high specific surface area,tunable pore size and morphology,easy sur-face modification and good biocompatibility.However,as a result of the poor biodegradability of MsNs,their biomedical applications are limited.To break the bottleneck of limited biomedical applications of MSNs,more and more researchers tend to design biodegradable MSNs(b-MSNs)nanosystems to obtain biodegradable as well as safe and reliable drug delivery carriers.In this review,we focused on sum-marizing strategies to improve the degradability of MsNs and innovatively proposed a series of advan-tages of b-MsNs,including controlled cargo release behavior,multifunctional frameworks,nano-catalysis,bio-imaging capabilities and enhanced therapeutic effects.Based on these advantages,we have inno-vatively summarized the applications of b-MsNs for enhanced tumor theranostics,including enhanced chemotherapy,delivery of nanosensitizers,gas molecules and biomacromolecules,initiation of immune response,synergistic therapies and image-guided tumor diagnostics.Finally,the challenges and further clinical translation potential of nanosystems based on b-MsNs are fully discussed and prospected.We believe that such b-MsNs delivery carriers will provide a timely reference for further applications in tu-mor theranostics.展开更多
Herein,we report the self-sacrificial template strategy to design mesoporous layered CeVWO_(x)/TiO_(2)catalysts for the selective catalytic reduction of NO by NH_(3)(NH_(3)-SCR).As-fabricated CeVWO_(x)/TiO_(2)catalyst...Herein,we report the self-sacrificial template strategy to design mesoporous layered CeVWO_(x)/TiO_(2)catalysts for the selective catalytic reduction of NO by NH_(3)(NH_(3)-SCR).As-fabricated CeVWO_(x)/TiO_(2)catalysts with unique mesoporous and layered structure were successfully prepared through the synthesis of Ce,Ti-MOFs by solvothermal method,the impregnation of vanadium and tungsten in Ce,Ti-MOFs and high temperature calcination process.As NH_(3)-SCR catalysts,well-designed CeVWO_(x)/TiO_(2)catalysts exhibit excellent SCR activity with the NO_(x)conversion of over 90%between 210 and 470℃.Meanwhile,CeVWO_(x)/TiO_(2)shows superior tolerance to water vapor and SO_(2).The features of unique mesoporous layered nanostructure,surface acidity,tunable reducibility,active and the strong interaction of active metal oxide and support in CeVWO_(x)/TiO_(2)nanosheets should contribute to the improved SCR performance.In situ diffuse reflection infrared Fourier transform spectroscopy(DRIFTS)analysis indicates that both Langmuir-Hinshelwood(L-H)and Eley-Rideal(E-R)mechanisms are present on the surface of CeVWO_(x)/TiO_(2)at low temperature.This work offers a facile strategy to design and fabricate efficient 2D deNO_x catalyst.展开更多
Rechargeable zinc-air batteries(ZABs)hold significant promise for next-generation energy storage due to their unique advantages in safety,energy and cost.However,their commercial application remains hindered by the sl...Rechargeable zinc-air batteries(ZABs)hold significant promise for next-generation energy storage due to their unique advantages in safety,energy and cost.However,their commercial application remains hindered by the sluggish kinetics of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),necessitating the development of highly efficient and durable electrocatalysts.Herein,we report a hierarchically mesoporous Fe-N-C catalyst(Fe-N/MPC_(S500))synthesized via a template-assisted method,which exhibits exceptional bifunctional ORR/OER performance.The Fe-N/MPC_(S500)catalyst achieves a positive ORR half-wave potential(0.86 V),along with a low OER over-potential of 510 mV at 10 mA cm^(2),surpassing those of most non-precious metal catalysts.Furthermore,in a liquid-state ZAB,Fe-N/MPC_(S500) delivers a high specific capacity of 708 mAh g^(-1),a peak power density of 409 mW cm^(2),and stable charge-discharge cycling over 470 h,outperforming commercial Pt/C+Ir/C catalysts.The outstanding performance is attributed to the hierarchical porosity,optimized Fe-N coordination,and enhanced electron/mass transport.This work presents a scalable and low-cost strategy for developing high-performance single-atom catalysts,paving the way for practical deployment in energy conversion and storage technologies.展开更多
Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NH...Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.展开更多
MXene has attracted great attention due to its high conductivity,large specific surface area and tunable surface functional groups.However,MXene(e.g.,Ti_(3)C_(2))nanosheets tend to stack and mainly offer in-plane site...MXene has attracted great attention due to its high conductivity,large specific surface area and tunable surface functional groups.However,MXene(e.g.,Ti_(3)C_(2))nanosheets tend to stack and mainly offer in-plane sites,showing limited capability in improving the oxygen reduction reaction(ORR)performance of iron phthalocyanine(FePc).In this study,mesoporous Ti_(3)C_(2)(Meso-Ti_(3)C_(2))loaded FePc(FePc/Meso-Ti_(3)C_(2))catalysts were prepared by a simple ultrasonic liquid-phase compounding strategy.Meso-Ti_(3)C_(2)possesses abundant mesopores and edge sites,which optimize the coordination environment and the electronic structure of the FeN4 center in FePc.This optimization improves the mass transfer and the accessibility of the active sites,synergistically enhancing the ORR performance of FePc.As a result,FePc/Meso-Ti_(3)C_(2)shows excellent ORR activity and stability under alkaline conditions with a half-wave potential of 0.914 V against the reversible hydrogen electrode(RHE)and a Tafel slope of 57.2 mV/dec.Furthermore,the zinc-air battery assembled with FePc/Meso-Ti_(3)C_(2)delivers a peak power density of 183.1 mW/cm^(2)and a good long-term discharge stability,exceeding those of FePc/Ti_(3)C_(2)and commercial 20%Pt/C catalysts(20%Pt by mass).展开更多
TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bul...TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bulk structure,the TiNb_(2)O_(7)electrode still suffers from unsatisfactory lithium storage performance.Herein,we demonstrate a spatially confined strategy toward a novel TiNb_(2)O_(7)-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route,where TiNb_(2)O_(7)quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon(NMC)and Ti_(3)C_(2)T_(X)MXene.Impressively,the as-prepared TiNb_(2)O_(7)-NMC/MXene anode exhibits a high reversible capacity(486.2 mAh g^(-1)at 0.1 A g^(-1)after 100 cycles)and long cycle lifespan(363.4 mAh g^(-1)at ss1 A g^(-1)after 500 cycles).Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNb_(2)O_(7)quantum dots,2D Ti_(3)C_(2)T_(X)MXene nanosheets,and N-doped mesoporous carbon.The strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.展开更多
To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environment...To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.展开更多
Due to the limitations of conventional chemotherapy including side effects,poor prognosis,and drug resistance,there is an urgent need for the development of a novel multi-functional combined therapy strategy.Dopamine-...Due to the limitations of conventional chemotherapy including side effects,poor prognosis,and drug resistance,there is an urgent need for the development of a novel multi-functional combined therapy strategy.Dopamine-modified oxaliplatin prodrug(OXA-DA)was successfully synthesized in this study to ameliorate the organ distribution of oxaliplatin for improving the drug efficacy and reducing toxic side effects,and OXA-DA was applied to develop a porous oxaliplatin cross-linked polydopamine nanoparticle for loading siPD-L1 to construct multifunctional nanoplatform.The multifunctional nanoplatform was modified with poly(2-ethyl-2-oxazoline)(PEOz),which occurred charge reversal in the tumor microenvironment,and exerted the lysosomal escape effect in tumor cells to improve the bioavailability of small interfering RNA targeting programmed cell death-ligand 1(siPD-L1).The pH-responsive charge reversal,photothermal,biodegradation,lysosomal escape ability,PD-L1 protein degradation,toxicity properties and multiple antitumor effects were comprehensively evaluated in vitro and in vivo experiments.The findings indicated that OXA-DA-siPD-L1@PDA-PEOz excellently induced tumor cell necrosis and apoptosis as a result of the synergistic effect of chemo-photothermal therapy,and upregulated CD8+T cells produced interferon-γ(IFN-γ)to further attack the tumor cells.In conclusion,the novel nanoplatform-mediated chemo/photothermal/immunotherapy has promising clinical applications in the treatment of malignant tumors.展开更多
Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the c...Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the charge and discharge process(“shuttle effect”)results in fast capacity fading and inferior electrochemical performance.In this study,Mn_(2)O_(3)with an ordered mesoporous structure(OM-Mn_(2)O_(3))was designed as a cathode host for LSBs via KIT-6 hard templating,to effectively inhibit the polysulfide shuttle effect.OM-Mn_(2)O_(3)offers numerous pores to confine sulfur and tightly anchor the dissolved polysulfides through the combined effects of strong polar-polar interactions,polysulfides,and sulfur chain catenation.The OM-Mn_(2)O_(3)/S composite electrode delivered a discharge capacity of 561 mAh g^(-1) after 250 cycles at 0.5 C owing to the excellent performance of OM-Mn_(2)O_(3).Furthermore,it retained a discharge capacity of 628mA h g^(-1) even at a rate of 2 C,which was significantly higher than that of a pristine sulfur electrode(206mA h g^(-1)).These findings provide a prospective strategy for designing cathode materials for high-performance LSBs.展开更多
Microcystins(MCs),a family of cyclic heptapeptide cyanotoxins,exists in aquatic environment where cyanobacterial bloom happens,which will accumulate in aquatic organisms and transfer through the food chain to higher t...Microcystins(MCs),a family of cyclic heptapeptide cyanotoxins,exists in aquatic environment where cyanobacterial bloom happens,which will accumulate in aquatic organisms and transfer through the food chain to higher trophic levels,posing a health risk to both animals and human bodies.Among various MCs,Microcystin-LR(MC-LR)is worthiest studied for its strong toxicity,ubiquity and widespread.Here in this work,iminodiacetic acid(IDA)decorated magnetic mesoporous silica(mSiO_(2))nanocomposites(Fe_(3)O_(4)@mSiO_(2)-IDA)were facilely synthesized which possessed the merits of large surface area(188.21 m^(2)/g),accessible porosity(2.66 nm),excellent hydrophilicity and rapid responsiveness to magnetic field.Then the composites were successfully employed to the removal process of Microcystin-LR in real water samples followed by Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry(MALDI-TOF MS)analysis,achieving the removal efficiency above 92.5%even after ten recycles of the composites.It provided a potential method for removing MC-LR in aqueous environment with high effectiveness,lower costs and less secondary contamination.展开更多
Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challen...Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.展开更多
基金the financial support from the National Natural Science Foundation of China(No.92163124)Foundation for the Sichuan University and Zigong City Joint research project(No.2021CDZG-2)+1 种基金Foundation for the Sichuan University and Yibin City Strategic Cooperation Project(No.2020CDYB-32)Guangxi Key Laboratory of Low Carbon Energy Material(No.2020GKLLCEM02)。
文摘Carbon materials are considered as prospective anode candidates for potassium ion batteries(PIBs).However,the low-rate capability is hampered by slow K+diffusion kinetics and obstructed electron transport of carbon-based anodes.In this work,calcium D-gluconate derived mesoporous carbon nanosheets(CGC)were interpenetrated into the architecture of reduced graphene oxides(RGO)to form the composites of two-dimensional(2D)/2D graphene/mesoporous carbon nanosheets(RGO@CGC).CGC as a rigid skeleton can prevent the graphene layers from restacking and maintain the structural stability of the 2D/2D carbon composites of RGO@CGC.The mesopores in CGC can shorten the path of ion diffusion and facilitate the penetration of electrolytes.RGO possesses the high surface-to-volume ratio and superior electron transport capability in the honeycomb-like 2D network consisting of sp^(2)-hybridized carbon atoms.Especially,theπ-πstacking interaction between CGC and RGO enhances stable composite structure formation,expedites interlayer-electron transfer,and establishes three-dimensional(3D)ion transportation pathways.Owing to these unique structure,RGO@CGC exhibits fast and stable potassium storage capability.Furthermore,the effects of binders and electrolytes on the electrochemical performance of RGO@CGC were investigated.Finally,Prussian blue was synthesized as a positive electrode to explore the possibility of RGO@CGC as a full battery application.
基金supported by the Natural Science Foundation of Sichuan Province(No.2022NSFSC0720)Research Center for the Development of the Comprehensive Health Industry and Rural Revitalization of Sichuan TCM(No.DJKYB202306)State Administration of Traditional Chinese Medicine of Sichuan Province of China(No.2020HJZX001).
文摘Obesity has become a global threat to health;however,the available drugs for treating obesity are limited.We investigated the anti-obesity effect of hydroxy-α-sanshool(HAS),an amide derived from the fruit of Zanthoxylum bungeanum,which promotes the management of obesity by triggering the browning of white adipose tissue(WAT)targeting the membrane receptor of transient receptor potential vanilloid 1(TRPV1).However,HAS easily undergoes configuration transformation and oxidative degradation.The short peptide CKGGRAKDC or adipose-targeting sequence(ATS)binds specifically to prohibitin on the surface of WAT cells and can be used as recognition assembly to enhance adipocyte targetability.Furthermore,mesoporous silica nanoparticles(MSNs)are widely used in drug delivery systems because of their large specific surface area and pore volume.Therefore,HAS-loaded adipose-targeted MSNs(MSNs-ATS)were developed to enhance the adipocyte targetability,safety,and efficacy of HAS,and tested on mature 3T3-L1 cells and obese mouse models.MSNs-ATS showed higher specificity for adipocyte targetability without obvious toxicity.HAS-loaded MSNs-ATS showed anti-obesity effects superior to those of HAS alone.In conclusion,we successfully developed adipocyte-targeted,HAS-loaded MSNs with good safety and anti-obesity effects.
文摘Due to the high capacity and moderate volume expansion of silicon protoxide SiO_(x)(160%)compared with that of Si(300%),reducing silicon dioxide SiO_(2)into SiO_(x)while maintaining its special nano-morphology makes it attractive as an anode of Li-ion batteries.Herein,through a one-pot facile high-temperature annealing route,using SBA15 as the silicon source,and embedding tin dioxide SnO_(2)particles into carbon coated SiO_(x),the mesoporous SiO_(x)-SnO_(2)@C rod composite was prepared and tested as the anode material.The results revealed that the SnO_(2)particles were distributed uniformly in the wall,which could further improve their volume energy densities.The coated carbon plays a role in maintaining structural integrality during lithiation,and the rich mesopores structure can release the expanded volume and enhance Li-ion transfer.At 0.1 A·g^(-1),the gravimetric and volumetric capacities of the composite were as high as 1271 mAh·g^(-1)and 1573 mAh·cm^(-3),respectively.After 200 cycles,the 95%capacity could be retained compared with that upon the 2nd cycle at 0.5 A·g^(-1).And the rod morphology was well kept,except that the diameter of the rod was 3 times larger than its original size after the cell was discharged into 0.01 V.
基金supported by the Program of Ministry of Science and Technology of China(No.2023YFB2504200)support of Shanghai Rising-Star Program(Grant No.24QB2703200)the Major Science and Technology Projects of Yunnan Province(No.202302AH360001).
文摘Mesoporous carbon supports mitigate platinum(Pt)sulfonic poisoning through nanopore-confined Pt deposition,yet their morphological impacts on oxygen transport remain unclear.This study integrates carbon support morphology simulation with an enhanced agglomerate model to establish a mathematical framework elucidating pore evolution,Pt utilization,and oxygen transport in catalyst layers.Results demonstrate dominant local mass transport resistance governed by three factors:(1)active site density dictating oxygen flux;(2)ionomer film thickness defining shortest transport path;(3)ionomer-to-Pt surface area ratio modulating practical pathway length.At low ionomer-to-carbon(I/C)ratios,limited active sites elevate resistance(Factor 1 dominant).Higher I/C ratios improve the ionomer coverage but eventually thicken ionomer films,degrading transport(Factors 2–3 dominant).The results indicate that larger carbon particles result in a net increase in local transport resistance by reducing external surface area and increasing ionomer thickness.As the proportion of Pt situated in nanopores or the Pt mass fraction increases,elevated Pt density inside the nanopores exacerbates pore blockage.This leads to the increased transport resistance by reducing active sites,and increasing ionomer thickness and surface area.Lower Pt loading linearly intensifies oxygen flux resistance.The model underscores the necessity to optimize support morphology,Pt distribution,and ionomer content to prevent pore blockage while balancing catalytic activity and transport efficiency.These insights provide a systematic approach for designing high-performance mesoporous carbon catalysts.
基金support from the Beijing Natural Science Foundation(No.JQ23035)。
文摘High-efficient rubber antioxidants for enhanced heat resistance without compromising mechanical properties remain an enormous and long-term challenge for the rubber industry.Herein,we employed the in-situ growth of Ce-doped Co-metal-organic framework(Ce Co-MOF)in dendritic mesoporous organosilica nanoparticles(DMONs@Ce Co-MOF,denoted as DCCM)to prepare a novel antioxidant that exhibit outstanding thermal stability.Dendritic mesoporous organosilica nanoparticles(DMONs)effectively alleviated the incompatibility of Ce Co-MOF in the polymer matrix,and the effective scavenging of free radicals was attributed to the various oxidation states of metal ions in Ce Co-MOF.Surprising,by adding only0.5 phr(parts per hundred of rubber)of DMONs@Ce Co-MOF to silicone rubber,(SR),the retention rate of tensile strength increased from 37.3%to 61.6%after aging 72 h at 250℃,and the retention rate of elongation at break of DCCM/SR1 composites reached 68%,which was 5.43 times of SR.The strategy of anchoring MOFs on the surface of silica also provides a viable method for preparing effective compound functionalized rubber antioxidant.
基金supported by National Natural Science Foundation of China(52376104,52201158)Joint Funds of the National Natural Science Foundation of China(U20A20302)+3 种基金Innovative group projects in Hebei Province(E2021202006)the project of Science and Technology in the Universities of Hebei Province(JZX2023006)Natural Science Foundation of Hebei Province(C202202003)Hebei University of Technology Cross-disciplinary(XKJC-2024001)。
文摘Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn^(2+)as cross-linking and pore-forming agents,followed by KHCO_(3)activation,eliminating the need for toxic phenolic resins and acid treatments for metal removal.Machine learning technology,specifically an Artificial Neural Network(ANN model,was utilized to assist the experimental design and prediction.The ANN model suggested an ideal hierarchical structure and optimized oxygen level,achieved through the adjustment of Zn^(2+)additive concentration,carbonization temperature,and subsequent KHCO_(3)activation to maximize capacitance.The HOMC electrode,with a micropore-to-mesopore ratio(S_(micro)/S_(meso))of 1.01 and an oxygen content of 8.81 at%,acquired a specific capacitance of 362 F·g^(-1)at 0.5 A·g^(-1)in 6 mol·L^(-1)KOH electrolyte.The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg^(-1)with a corresponding specific power density of 300 W·kg^(-1)in TEATFB PC electrolyte.Meanwhile,the long-term cycle stability of 94.33%was achieved after 20,000 cycles.This work provides an ANN assisted strategy for the synthesis of HOMC,highlighting its potential to valorize biomass and agricultural waste in sustainable energy storag solutions.
基金Funded by the National Natural Science Foundation of China(Nos.22068021 and 52064030)the Yunnan Young and Middle-aged Academic and Technical Leaders Reserve Talent Program of China(No.202305AC160064)the Yunnan Major Scientific and Technological Program of China(Nos.202402AB080004,202202AG050011,and 202202AG050007)。
文摘To efficiently address the current high cost associated with preparing pseudo-boehmite from organic aluminum,a low-cost alternative,AlCl_(3),is employed as the raw material.The sol-gel method is utilized,and H_(2)O_(2)is incorporated for the modification of pseudo-boehmite.The modification mechanism is thoroughly investigated through the use of X-ray powder diffractometer,scanning electron microscope,and BET data analysis,as well as molecular dynamics simulations.Under specific conditions(temperature at 80°C,pH=7,and H_(2)O_(2)volume ratios of 0.5:1,1:1,and 2:1),mesoporous pseudo-boehmite is synthesized with a specific surface area of 227 m^(2)/g,a pore volume of 0.281 cm^(3)/g,a pore size of 6.78 nm,and a peptizing index of 99.47%.A novel and innovative methodology for the cost-effective production of high-performance alumina is offered through the approach.
文摘Aromatization of light alkanes is a value-added process in both petrochemical and coal chemical industries.Here,single[Ga(OH)]^(2+)ion-exchanged mesoporous hollow-structured ZSM-5(Ga-MH-ZSM-5)material was prepared,and it shows unprecedented catalytic performance in light alkane aromatization,considering activity,product selectivity and catalytic stability.The average aromatics yields in ethane aromatization at 600℃and WHSV of 0.8 h^(-1) within 28 h and in propane aromatization at 580℃and WHSV of 1.1 h^(-1) within 20 h reach~18.4%and~70.8%with benzene,toluene and xylenes(BTX)accounting for~96%and~88%of aromatics,respectively.Ga-MH-ZSM-5-0.41 gave a TON for formation of aromatics(TON_(aromatics))from propane as high as 57479,whereas the reported catalysts maximally show a TON_(aromatics) of 5514.This also holds true for ethane aromatization;the TON_(aromatics) obtained on Ga-MH-ZSM-5-0.41 was³3845 in contrast to£392 on reported non-noble metal catalysts.The catalytic activity of Ga-MH-ZSM-5 highly depends on Ga species structures.[Ga(OH)]^(2+)ions are predominant species at Ga loading≤0.3 wt%,while more[Ga(OH)_(2)]^(+)and GaO_(x) oligomers are formed with increasing Ga content.Upon reduction with H_(2),[Ga(OH)]^(2+)and[Ga(OH)_(2)]^(+)are transformed into[GaH]^(2+)and[GaH_(2)]^(+)species,which show a propane dehydrogenation rate of 300 and 15 times of that of Brønsted acid sites respectively.The light alkanes are mainly dehydrogenated into light olefins on[GaH]^(2+)species,and then,oligomerized and cyclized into(alkyl)cycloalkanes on H^(+)sites,which is followed by possible ring expansion on H^(+)and sequential dehydrogenations into aromatics primarily on[GaH]^(2+).
基金the National Natural Science Foundation of China(22108115,22478415,and 21978134)Natural Science Foundation of Jiangsu Province(BK20241744)。
文摘Confinement effect is an effective method to enhance carbon dioxide(CO_(2))solubility.In this study,a hybrid sorbent of 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([Hmim][NTf_2])/mesoporous titanium dioxide(M-TiO_(2))/water(H_2O)was developed,and its confinement effect was regulated by changing the pore structure of M-TiO_(2).CO_(2) solubility in the hybrid sorbent was measured experimentally,and the thermodynamic properties including Henry's constant and desorption enthalpy were calculated.Furthermore,the confinement effect in the hybrid sorbent was quantified.Additionally,the hybrid sorbent was recycled with a multi-cycle experiment.The results showed that M-TiO_(2) calcined at 773.2 K(MT500)could lead to an efficient confinement effect.CO_(2) solubility in the hybrid sorbent increased by 49.8%compared to that of H_2O when the mass fraction of[Hmim][NTf_2]/MT500 was 5.0%(mass),where the contribution of confinement effect on Gibbs free energy occupied 5.2%.
基金from"XingLiao Talent Program"of Liaoning Province(No.XLYC2203156)Shenyang Young and Middle-aged Science and Technology Innovation Talent Support Program(No.RC220397)are greatly acknowledged。
文摘Mesoporous silica nanoparticles(MsNs)are thought to be an attractive drug delivery material because of their advantages including high specific surface area,tunable pore size and morphology,easy sur-face modification and good biocompatibility.However,as a result of the poor biodegradability of MsNs,their biomedical applications are limited.To break the bottleneck of limited biomedical applications of MSNs,more and more researchers tend to design biodegradable MSNs(b-MSNs)nanosystems to obtain biodegradable as well as safe and reliable drug delivery carriers.In this review,we focused on sum-marizing strategies to improve the degradability of MsNs and innovatively proposed a series of advan-tages of b-MsNs,including controlled cargo release behavior,multifunctional frameworks,nano-catalysis,bio-imaging capabilities and enhanced therapeutic effects.Based on these advantages,we have inno-vatively summarized the applications of b-MsNs for enhanced tumor theranostics,including enhanced chemotherapy,delivery of nanosensitizers,gas molecules and biomacromolecules,initiation of immune response,synergistic therapies and image-guided tumor diagnostics.Finally,the challenges and further clinical translation potential of nanosystems based on b-MsNs are fully discussed and prospected.We believe that such b-MsNs delivery carriers will provide a timely reference for further applications in tu-mor theranostics.
基金Project supported by National Key Research and Development Plan of China(2021YFB3802003,2022YFB3504102)the Key Research and Development Plan of Jiangsu Province(Social Development,BE2021713)+1 种基金the Six Talent Peaks Project of Jiangsu Province(JNHB-044)the Natural Science Foundation of Jiangsu Province of China(BK20160982)。
文摘Herein,we report the self-sacrificial template strategy to design mesoporous layered CeVWO_(x)/TiO_(2)catalysts for the selective catalytic reduction of NO by NH_(3)(NH_(3)-SCR).As-fabricated CeVWO_(x)/TiO_(2)catalysts with unique mesoporous and layered structure were successfully prepared through the synthesis of Ce,Ti-MOFs by solvothermal method,the impregnation of vanadium and tungsten in Ce,Ti-MOFs and high temperature calcination process.As NH_(3)-SCR catalysts,well-designed CeVWO_(x)/TiO_(2)catalysts exhibit excellent SCR activity with the NO_(x)conversion of over 90%between 210 and 470℃.Meanwhile,CeVWO_(x)/TiO_(2)shows superior tolerance to water vapor and SO_(2).The features of unique mesoporous layered nanostructure,surface acidity,tunable reducibility,active and the strong interaction of active metal oxide and support in CeVWO_(x)/TiO_(2)nanosheets should contribute to the improved SCR performance.In situ diffuse reflection infrared Fourier transform spectroscopy(DRIFTS)analysis indicates that both Langmuir-Hinshelwood(L-H)and Eley-Rideal(E-R)mechanisms are present on the surface of CeVWO_(x)/TiO_(2)at low temperature.This work offers a facile strategy to design and fabricate efficient 2D deNO_x catalyst.
基金supported by the Shanghai Sailing Program(22YF1400700)the Chenguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission(22CGA37)+3 种基金the Fundamental Research Funds for the Central Universities(2232022D-18)the National Natural Science Foundation of China(52302084)the Natural Science Foundation of Yancheng(YCBK2024004)the Jiaxing Science and Technology Project for Youth Talent(2024AY40016).
文摘Rechargeable zinc-air batteries(ZABs)hold significant promise for next-generation energy storage due to their unique advantages in safety,energy and cost.However,their commercial application remains hindered by the sluggish kinetics of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),necessitating the development of highly efficient and durable electrocatalysts.Herein,we report a hierarchically mesoporous Fe-N-C catalyst(Fe-N/MPC_(S500))synthesized via a template-assisted method,which exhibits exceptional bifunctional ORR/OER performance.The Fe-N/MPC_(S500)catalyst achieves a positive ORR half-wave potential(0.86 V),along with a low OER over-potential of 510 mV at 10 mA cm^(2),surpassing those of most non-precious metal catalysts.Furthermore,in a liquid-state ZAB,Fe-N/MPC_(S500) delivers a high specific capacity of 708 mAh g^(-1),a peak power density of 409 mW cm^(2),and stable charge-discharge cycling over 470 h,outperforming commercial Pt/C+Ir/C catalysts.The outstanding performance is attributed to the hierarchical porosity,optimized Fe-N coordination,and enhanced electron/mass transport.This work presents a scalable and low-cost strategy for developing high-performance single-atom catalysts,paving the way for practical deployment in energy conversion and storage technologies.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22278092,22078116 and 22222805)Guangdong Provincial Key Research and Development Program(No.2020B1111380002)+2 种基金Science and Technology Research Project of Guangzhou(Nos.2023A03J0034,2023A04J0077 and 202102020467)State Key Laboratory of Pulp and Paper Engineering(No.202313)Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.202255464).
文摘Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.
文摘MXene has attracted great attention due to its high conductivity,large specific surface area and tunable surface functional groups.However,MXene(e.g.,Ti_(3)C_(2))nanosheets tend to stack and mainly offer in-plane sites,showing limited capability in improving the oxygen reduction reaction(ORR)performance of iron phthalocyanine(FePc).In this study,mesoporous Ti_(3)C_(2)(Meso-Ti_(3)C_(2))loaded FePc(FePc/Meso-Ti_(3)C_(2))catalysts were prepared by a simple ultrasonic liquid-phase compounding strategy.Meso-Ti_(3)C_(2)possesses abundant mesopores and edge sites,which optimize the coordination environment and the electronic structure of the FeN4 center in FePc.This optimization improves the mass transfer and the accessibility of the active sites,synergistically enhancing the ORR performance of FePc.As a result,FePc/Meso-Ti_(3)C_(2)shows excellent ORR activity and stability under alkaline conditions with a half-wave potential of 0.914 V against the reversible hydrogen electrode(RHE)and a Tafel slope of 57.2 mV/dec.Furthermore,the zinc-air battery assembled with FePc/Meso-Ti_(3)C_(2)delivers a peak power density of 183.1 mW/cm^(2)and a good long-term discharge stability,exceeding those of FePc/Ti_(3)C_(2)and commercial 20%Pt/C catalysts(20%Pt by mass).
基金support from the Natural Science Foundation of Shanghai(23ZR1423800),Shuguang Program supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(18SG35)Open Research Fund of Shanghai Key Laboratory of Green Chemistry and Chemical Processes(East China Normal University)Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University.
文摘TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bulk structure,the TiNb_(2)O_(7)electrode still suffers from unsatisfactory lithium storage performance.Herein,we demonstrate a spatially confined strategy toward a novel TiNb_(2)O_(7)-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route,where TiNb_(2)O_(7)quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon(NMC)and Ti_(3)C_(2)T_(X)MXene.Impressively,the as-prepared TiNb_(2)O_(7)-NMC/MXene anode exhibits a high reversible capacity(486.2 mAh g^(-1)at 0.1 A g^(-1)after 100 cycles)and long cycle lifespan(363.4 mAh g^(-1)at ss1 A g^(-1)after 500 cycles).Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNb_(2)O_(7)quantum dots,2D Ti_(3)C_(2)T_(X)MXene nanosheets,and N-doped mesoporous carbon.The strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.
基金supported by the National Natural Science Foundation of China(52370041)National Natural Science Foundation of China(21976134 and 21707104)State Key Laboratory of Pollution treatment and Resource Reuse Foundation(NO.PCRRK21001).
文摘To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.
基金the National Natural Science Foundation of China(Nos.32071342 and 32101065)the Natural Science Foundation of Guangdong Province(Nos.2023A1515012015,2022A1515110271 and 2020A1515011353).
文摘Due to the limitations of conventional chemotherapy including side effects,poor prognosis,and drug resistance,there is an urgent need for the development of a novel multi-functional combined therapy strategy.Dopamine-modified oxaliplatin prodrug(OXA-DA)was successfully synthesized in this study to ameliorate the organ distribution of oxaliplatin for improving the drug efficacy and reducing toxic side effects,and OXA-DA was applied to develop a porous oxaliplatin cross-linked polydopamine nanoparticle for loading siPD-L1 to construct multifunctional nanoplatform.The multifunctional nanoplatform was modified with poly(2-ethyl-2-oxazoline)(PEOz),which occurred charge reversal in the tumor microenvironment,and exerted the lysosomal escape effect in tumor cells to improve the bioavailability of small interfering RNA targeting programmed cell death-ligand 1(siPD-L1).The pH-responsive charge reversal,photothermal,biodegradation,lysosomal escape ability,PD-L1 protein degradation,toxicity properties and multiple antitumor effects were comprehensively evaluated in vitro and in vivo experiments.The findings indicated that OXA-DA-siPD-L1@PDA-PEOz excellently induced tumor cell necrosis and apoptosis as a result of the synergistic effect of chemo-photothermal therapy,and upregulated CD8+T cells produced interferon-γ(IFN-γ)to further attack the tumor cells.In conclusion,the novel nanoplatform-mediated chemo/photothermal/immunotherapy has promising clinical applications in the treatment of malignant tumors.
基金Ministry of Trade,Industry and Energy,Grant/Award Number:20010095Korea Evaluation Institute of Industrial Technology,Grant/Award Number:20012341。
文摘Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the charge and discharge process(“shuttle effect”)results in fast capacity fading and inferior electrochemical performance.In this study,Mn_(2)O_(3)with an ordered mesoporous structure(OM-Mn_(2)O_(3))was designed as a cathode host for LSBs via KIT-6 hard templating,to effectively inhibit the polysulfide shuttle effect.OM-Mn_(2)O_(3)offers numerous pores to confine sulfur and tightly anchor the dissolved polysulfides through the combined effects of strong polar-polar interactions,polysulfides,and sulfur chain catenation.The OM-Mn_(2)O_(3)/S composite electrode delivered a discharge capacity of 561 mAh g^(-1) after 250 cycles at 0.5 C owing to the excellent performance of OM-Mn_(2)O_(3).Furthermore,it retained a discharge capacity of 628mA h g^(-1) even at a rate of 2 C,which was significantly higher than that of a pristine sulfur electrode(206mA h g^(-1)).These findings provide a prospective strategy for designing cathode materials for high-performance LSBs.
基金financially supported by National Key R&D Program of China(No.2018YFA0507501)the National Natural Science Foundation of China(Nos.22074019,21425518,22004017,22205085,and 32160305)+2 种基金Key Science and Technology Project of Jiangxi Province(Nos.20213AAG01012 and 2022KSG01004)Water Science and Technology Project of Jiangxi Province(Nos.202124ZDKT19 and 202223YBKT07)Shanghai Sailing Program(No.20YF1405300).
文摘Microcystins(MCs),a family of cyclic heptapeptide cyanotoxins,exists in aquatic environment where cyanobacterial bloom happens,which will accumulate in aquatic organisms and transfer through the food chain to higher trophic levels,posing a health risk to both animals and human bodies.Among various MCs,Microcystin-LR(MC-LR)is worthiest studied for its strong toxicity,ubiquity and widespread.Here in this work,iminodiacetic acid(IDA)decorated magnetic mesoporous silica(mSiO_(2))nanocomposites(Fe_(3)O_(4)@mSiO_(2)-IDA)were facilely synthesized which possessed the merits of large surface area(188.21 m^(2)/g),accessible porosity(2.66 nm),excellent hydrophilicity and rapid responsiveness to magnetic field.Then the composites were successfully employed to the removal process of Microcystin-LR in real water samples followed by Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry(MALDI-TOF MS)analysis,achieving the removal efficiency above 92.5%even after ten recycles of the composites.It provided a potential method for removing MC-LR in aqueous environment with high effectiveness,lower costs and less secondary contamination.
基金supported by the National Natural Science Foundation of China(No.52374350)China Postdoctoral Science Foundation(Nos.2020M680347 and 2021T140051)the Fundamental Research Funds for the Central Universities(No.FRF-TP-20-045A1)。
文摘Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.
