Carbon-based materials have gained significant attention in anticancer treatment because of their exceptional biocompatibility,yet critical challenges persist in establishing definitive correlations between their poro...Carbon-based materials have gained significant attention in anticancer treatment because of their exceptional biocompatibility,yet critical challenges persist in establishing definitive correlations between their porous structures and functional performance.We report the use of a silica template to guide pore formation in the design of mesoporous carbon spheres(mC)with tailored pore structures for improved combined photothermal-chemotherapy.The mesopore size of mC has been adjusted by kinetic control of the resin polymerization and silica hydrolysis.Structural characterization showed that 4.4 nm mesopores enabled an exceptional gemcitabine loading of 228 mg g^(−1) and a sustained pH/thermal dual-responsive release with>70%drug release under near-infrared(NIR)irradiation.Finite element analysis demonstrated pore size-dependent heat transfer dynamics,with the improved mC achieving a superior photothermal conversion efficiency of 62%by a combination of N-doping and defect engineering.In vitro evaluations confirmed outstanding biocompatibility with>95%cell viability at 200μg mL^(−1) and potent tumor suppression in pancreatic and biliary cancer models with an~5%cell viability at 25μg mL^(−1) where combined therapy showed a 3.7-fold increased cytotoxicity over monotherapy.The improved structure of mC facilitated cascade therapeutic effects with enhanced tumor permeability derived from NIR-triggered hyperthermia and prolonged therapeutic exposure due to pH-responsive drug release.This pore engineering strategy establishes a structure-function process for next-generation theranostic platforms,addressing the critical limitations of conventional pancreatic and biliary cancer therapies through spatiotemporal control of multimodal treatment.展开更多
Smart pesticide delivery systems based on stimuli-responsive nanocarriers have attracted considerable attention because of their potential to enhance pesticide efficiency while reducing environmental risks.In this stu...Smart pesticide delivery systems based on stimuli-responsive nanocarriers have attracted considerable attention because of their potential to enhance pesticide efficiency while reducing environmental risks.In this study,a novel p H/glutathione dual-responsive pesticide delivery system was constructed through the synthesis of disulfide-bridged hollow mesoporous organosilica nanospheres(HMONs)via the St??ber method,followed by poly(acrylic acid)(PAA)coating through distillation-precipitation polymerization to form HMONs@PAA nanocomposites.The resulting abamectin-loaded system(Abamectin-HMONs@PAA)demonstrated a 12.73% pesticide loading capacity and significantly improved photostability,retaining twice as much active ingredient as free abamectin after 250 h of UV irradiation(36 W).Release studies revealed p H-and glutathione-dependent characteristics,with cumulative releases in acidic conditions exceeding those in neutral and alkaline environments by 18.66% and 40.98%,respectively,and a 14.2% increase in glutathione-containing solution(0.2 mmol·L^(-1) in 70% ethanol)after 97 h.Bioassays showed superior performance against Plutella xylostella,with a 13.33% reduction in survival rate compared to conventional suspension at equivalent dosage(40 mg·L^(-1)),while maintaining efficacy after extensive rainfall simulation(20 events over 10 days).This study provides a promising approach for developing environmentally responsive nanopesticides with enhanced durability and controlled-release properties,offering significant potential for sustainable crop protection.展开更多
Conversion of ammonia into hydrogen,a crucial pathway for the hydrogen economy,is severely constrained by the intricacy of the required equipment and the low efficiency.Herein,Pd@Pt Ni Co Ru Ir coreshell mesoporous bi...Conversion of ammonia into hydrogen,a crucial pathway for the hydrogen economy,is severely constrained by the intricacy of the required equipment and the low efficiency.Herein,Pd@Pt Ni Co Ru Ir coreshell mesoporous bifunctional electrocatalysts were fabricated via a one-step wet-chemical reduction approach.By utilizing the limiting effect of triblock copolymers,gradient distribution control of six metal elements(Pd core and Pt/Ni/Co/Ru/Ir high-entropy alloys shell) was achieved,where the high-entropy alloy shell forms high-density active sites through lattice distortion effect.With the help of lattice distortion and mesoporous-confinement-enabled interfacial coupling effects,Pd@Pt Ni Co Ru Ir catalyst exhibited exceptional bifunctional performance in alkaline media:A low hydrogen evolution reaction(HER) overpotential of 30.5 m V at 10 m A/cm^(2) and a high ammonia oxidation reaction(AOR) peak current density of 19.6 m A/cm^(2) at 0.7 V vs.RHE,representing a 3.83-fold enhancement over commercial Pt/C.Moreover,a rechargeable Zn-NH_(3) battery system was constructed and achieved 92.3 % Faradaic efficiency(FE) for NH_(3)-to-H_(2) conversion with outstanding stability at 16 m A/cm^(2),thereby providing an innovative solution for efficient ammonia decomposition-based hydrogen production.展开更多
As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 n...As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 nm)severely limits their application in scenarios such as macromolecular mass transfer and so on.In order to overcome this re-striction,mesoporous MOFs(meso-MOFs)with a larger aperture(2-50 nm)have attracted much attention due to their potential applications in biological macromolecular catalysis,energy storage and other fields.To date,how to accurately regulate its mesopore topology and pore ordering still faces important technical challenges.展开更多
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
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
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
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
Organic ultraviolet(UV)filters play a crucial role in reducing sunburn,photoaging,and the risk of skin cancer induced by UV radiation.However,the challenges posed by photodegradation,potential phototoxicity,and poor d...Organic ultraviolet(UV)filters play a crucial role in reducing sunburn,photoaging,and the risk of skin cancer induced by UV radiation.However,the challenges posed by photodegradation,potential phototoxicity,and poor dispersion characteristics of organic UV filters significantly hinder their practical applications.This study aims to encapsulate avobenzone,a widely used UV filter,in mesoporous silica(MPS)to form AB@MPS particles via an in-situ sol-gel process,and to research their sunscreen performance as stabilizers in Pickering emulsion.The UV absorption capability of AB@MPS particles is stronger than free avobenzone.The in vitro skin penetration study reveals a greatly reduced permeability(73.9%)for avobenzone from AB@MPS compared to its free form.Furthermore,the photostability of AB@MPS particles increases 14.3 times compared to that of free avobenzone.In UV protection tests,the Pickering emulsion’s anti-UVA efficacy is 2.28 times greater than that of 20%PG solution,4.41 times greater than Carbomer hydrogel,and 3.59 times greater than the cream formulation.The SPF value of the Pickering emulsion is 2.41 times greater than the 20%PG solution,2 times greater than the Carbomer hydrogel,and 6.77 times greater than the cream formulation.This study presents a promising strategy for the application of Pickering emulsions in the cosmetic and pharmaceutical sectors,providing a safe and efficient formulation for sunscreens.展开更多
To alleviate the quality deterioration and extend the shelf life of crucian carp fillets,a bio-based active composite film integrating eugenol(EG)-loaded mesoporous silica nanoparticles(MSNs)modified with caffeic acid...To alleviate the quality deterioration and extend the shelf life of crucian carp fillets,a bio-based active composite film integrating eugenol(EG)-loaded mesoporous silica nanoparticles(MSNs)modified with caffeic acid(CA)within the zein matrix(EG/CA-MSN/Zein)was developed.This study compared the effects of EG/CA-MSN/Zein,polyethylene(PE),and zein films on the quality of fish fillets during refrigerated storage.The results showed that the EG/CA-MSN/Zein film significantly retarded the increase in pH and microbial growth.Moreover,the film had higher water-holding capacity(WHC),better texture,and color stability,as indicated by low-field nuclear magnetic resonance(LF-NMR),magnetic resonance imaging(MRI),and sensory evaluation.The EG/CA-MSN/Zein composite film extended the shelf life of crucian carp fillets by 3-4 days,highlighting its potential as an environmentally friendly and efficient packaging material for aquatic products.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
The slow kinetics of the cathode CO_(2) reduction reaction and the decomposition reaction of Li2CO3,a widebandwidth insulating product,lead to difficult CO_(2) capture and high charging potential in Li-CO_(2) batterie...The slow kinetics of the cathode CO_(2) reduction reaction and the decomposition reaction of Li2CO3,a widebandwidth insulating product,lead to difficult CO_(2) capture and high charging potential in Li-CO_(2) batteries.To improve the reaction kinetics and decrease the reaction overpotential,we synthesized mesoporous Pt nanosheets with high tensile strain.The presence of many unsaturated coordinated Pt atoms around the pores gives rise to tensile strain in the mesoporous Pt nanosheets.This tensile strain plays a key role in regulating the interactions between the catalytic surface of Pt and the adsorbed intermediates.The two-dimensional structure provides more active sites on the surface for the catalytic reactions.These superiorities enable a low overpotential of 0.36 V at a cutoff capacity of 100μAh·cm^(−2) at a current density of 10μA·cm^(−2) over more than 2000 h.This study opens new possibilities for the rational design of metal-based materials with strain engineering for electrochemical energy storage.展开更多
KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these cat...KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these catalysts and the effect of pore sizes on ethanol catalytic oxidation were investigated.Mn‐40,Mn‐100,and Mn‐150 have triple,double,and single pore systems,respectively.On decreasing the aging temperature of KIT‐6,the pore sizes of KIT‐6 decrease and that of mesoporous MnO2 catalysts increase.The pore sizes and catalytic activities increase in the order:Mn‐40>Mn‐100>Mn‐150.Mn‐40 catalyst has a higher TOF(0.11 s–1 at 120°C)and the best catalytic activity for ethanol oxidation because of a bigger pore size with three pore systems with maximum distribution at 1.9,3.4,and 6.6 nm,decrease in symmetry and degree of order,more surface lattice oxygen species,oxygen vacancies resulting from more Mn3+ions,and better low‐temperature reducibility.展开更多
The efficient storage and application of sustainable solar energy has drawn significant attention from both academic and industrial points of view.However,most developed catalytic materials still suffer from insuffici...The efficient storage and application of sustainable solar energy has drawn significant attention from both academic and industrial points of view.However,most developed catalytic materials still suffer from insufficient mass diffusion and unsatisfactory durability due to the lack of interconnected and regulatable porosity.Developing catalytic architectures with engineered active sites and prominent stability through rational synthesis strategies has become one of the core projects in solar-driven applications.The unique properties of mesoporous silicas render them among the most valuable functional materials for industrial applications,such as high specific surface area,regulatable porosity,adjustable surface properties,tunable particle sizes,and great thermal and mechanical stability.Mesoporous silicas serve as structural templates or catalytic supports to enhance light harvesting via the scattering effect and provide large surface areas for active site generation.These advantages have been widely utilized in solar applications,including hydrogen production,CO_(2)conversion,photovoltaics,biomass utilization,and pollutant degradation.To achieve the specific functionalities and desired activity,various types of mesoporous silicas from different synthesis methods have been customized and synthesized.Moreover,morphology regulation and component modification strategies have also been performed to endow mesoporous silica-based materials with unprecedented efficiency for solar energy storage and utilization.Nevertheless,reviews about synthesis,morphology regulation,and component modification strategies for mesoporous silica-based catalyst design in solar-driven applications are still limited.Herein,the latest progress concerning mesoporous silica-based catalysis in solar-driven applications is comprehensively reviewed.Synthesis principles,formation mechanisms,and rational functionalities of mesoporous silica are systematically summarized.Some typical catalysts with impressive activities in different solar-driven applications are highlighted.Furthermore,challenges and future potential opportunities in this study field are also discussed and proposed.This present review guides the design of mesoporous silica catalysts for efficient solar energy management for solar energy storage and conversion applications.展开更多
1.Introduction Magnesium oxide(MgO)has attracted considerable attention in recent years due to its economic viability,excellent biocompatibil-ity,chemical stability,and non-toxic,odorless nature[1,2].These inherent pr...1.Introduction Magnesium oxide(MgO)has attracted considerable attention in recent years due to its economic viability,excellent biocompatibil-ity,chemical stability,and non-toxic,odorless nature[1,2].These inherent properties position it as a promising candidate for various applications.展开更多
Perovskite oxides(ABO_(3))are thought to be promising electrocatalysts for oxygen evolution reaction(OER),but their specific surface area(SSA)is too low(usually<10 m^(2) g^(−1)).Developing advanced ABO_(3) electroc...Perovskite oxides(ABO_(3))are thought to be promising electrocatalysts for oxygen evolution reaction(OER),but their specific surface area(SSA)is too low(usually<10 m^(2) g^(−1)).Developing advanced ABO_(3) electrocatalysts with high SSA and optimized structure is of great significance but remains a tremendous challenge.Herein,we propose a general strategy for fabrication of mesoporous perovskite oxide nanosheets(MPONs)with controllable atomic doping via self-sacrificial template-induced nanostructure modulation.A variety of MPONs including LaFeO_(3),A-site-doped LaFeO_(3)(A-LaFeO_(3),where A is Pr,Nd,Sm,Eu,or Gd)and B-site-doped LaFeO_(3)(B-LaFeO_(3),where B is Mn,Co,Ni,Cu,or Zn)have been achieved.Interestingly,it is discovered that the catalytic activities of A-LaFeO_(3) MPONs as OER catalysts are overall higher than those of B-LaFeO_(3) ones.Especially,the screened Eu-LaFeO_(3) MPONs only require a low overpotential of 267 mV at 10 mA cm^(−2),outperforming most reported perovskite oxides.The superior catalytic activity of Eu-LaFeO_(3) MPONs is attributed to their favorable porous structure,which increases the density of active sites,and enhanced lattice oxygen participation,which improves the intrinsic activity.This study provides guidance for the design and controlled synthesis of advanced rare-earth-doped MPONs with ultrahigh SSA for enhanced electrocatalysis.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
The preparation of immobilized enzyme with excellent performance is one of the difficulties that restrict the application of enzyme catalysis technology.Here,Candida rugosa lipase(CRL)was firstly adsorbed on the surfa...The preparation of immobilized enzyme with excellent performance is one of the difficulties that restrict the application of enzyme catalysis technology.Here,Candida rugosa lipase(CRL)was firstly adsorbed on the surface of magnetic zeolitic imidazolate framework-8(ZIF-8)nanospheres,which was further encapsulated with a mesoporous SiO_(2)nano-membrane formed by tetraethyl orthosilicate(TEOS)polycondensation.Consequently,lipase could be firmly immobilized on carrier surface by physical binding rather than chemical binding,which did not damage the active conformation of enzyme.There were mesopores on the silica nano-membrane,which could improve the accessibility of enzyme and its apparent catalytic activity.Moreover,silica membrane encapsulation could also improve the stability of enzyme,suggesting an effective enzyme immobilization strategy.It showed that TEOS amount and the encapsulation time had significant effects on the thickness of silica membrane and the enzyme activity.The analysis in enzyme activity and protein secondary structure showed that lipase encapsulated in silica membrane retained the active conformation to the greatest extent.Compared with the adsorbed lipase,the encapsulated lipase increased its thermostability by 3 times and resistance to chemical denaturants by 7 times.The relative enzyme activity remained around 80%after 8 repetitions,while the adsorbed lipase only remained at7.3%.展开更多
文摘Carbon-based materials have gained significant attention in anticancer treatment because of their exceptional biocompatibility,yet critical challenges persist in establishing definitive correlations between their porous structures and functional performance.We report the use of a silica template to guide pore formation in the design of mesoporous carbon spheres(mC)with tailored pore structures for improved combined photothermal-chemotherapy.The mesopore size of mC has been adjusted by kinetic control of the resin polymerization and silica hydrolysis.Structural characterization showed that 4.4 nm mesopores enabled an exceptional gemcitabine loading of 228 mg g^(−1) and a sustained pH/thermal dual-responsive release with>70%drug release under near-infrared(NIR)irradiation.Finite element analysis demonstrated pore size-dependent heat transfer dynamics,with the improved mC achieving a superior photothermal conversion efficiency of 62%by a combination of N-doping and defect engineering.In vitro evaluations confirmed outstanding biocompatibility with>95%cell viability at 200μg mL^(−1) and potent tumor suppression in pancreatic and biliary cancer models with an~5%cell viability at 25μg mL^(−1) where combined therapy showed a 3.7-fold increased cytotoxicity over monotherapy.The improved structure of mC facilitated cascade therapeutic effects with enhanced tumor permeability derived from NIR-triggered hyperthermia and prolonged therapeutic exposure due to pH-responsive drug release.This pore engineering strategy establishes a structure-function process for next-generation theranostic platforms,addressing the critical limitations of conventional pancreatic and biliary cancer therapies through spatiotemporal control of multimodal treatment.
基金financially supported by the Jiangsu Forestry Science and Technology Innovation and Promotion Project(No.LYKJ-Nanjing[2022]02)the Jiangsu Agricultural Science and Technology Innovation Fund(No.CX(23)3090)。
文摘Smart pesticide delivery systems based on stimuli-responsive nanocarriers have attracted considerable attention because of their potential to enhance pesticide efficiency while reducing environmental risks.In this study,a novel p H/glutathione dual-responsive pesticide delivery system was constructed through the synthesis of disulfide-bridged hollow mesoporous organosilica nanospheres(HMONs)via the St??ber method,followed by poly(acrylic acid)(PAA)coating through distillation-precipitation polymerization to form HMONs@PAA nanocomposites.The resulting abamectin-loaded system(Abamectin-HMONs@PAA)demonstrated a 12.73% pesticide loading capacity and significantly improved photostability,retaining twice as much active ingredient as free abamectin after 250 h of UV irradiation(36 W).Release studies revealed p H-and glutathione-dependent characteristics,with cumulative releases in acidic conditions exceeding those in neutral and alkaline environments by 18.66% and 40.98%,respectively,and a 14.2% increase in glutathione-containing solution(0.2 mmol·L^(-1) in 70% ethanol)after 97 h.Bioassays showed superior performance against Plutella xylostella,with a 13.33% reduction in survival rate compared to conventional suspension at equivalent dosage(40 mg·L^(-1)),while maintaining efficacy after extensive rainfall simulation(20 events over 10 days).This study provides a promising approach for developing environmentally responsive nanopesticides with enhanced durability and controlled-release properties,offering significant potential for sustainable crop protection.
基金provided by the National Natural Science Foundation of China (No.52573275)Taishan Scholars Program of Shandong Province (No.tsqn202507205)+4 种基金Youth Innovation Team of Higher Education Institutions in Shandong Province (No.2023KJ105)Collaborative Innovation Center of Yellow River Basin Pharmaceutical Green Manufacturing and Engineering Equipment,University of Jinan,Jinan 250022,ChinaJinan City University Integration Development Strategy Project (No.JNSX2023021)supported by Talents’ plan Foundation of Guangdong Second Provincial General Hospital (No.2024D003)Science and Technology Projects in Guangzhou (No.2025A04J4629)。
文摘Conversion of ammonia into hydrogen,a crucial pathway for the hydrogen economy,is severely constrained by the intricacy of the required equipment and the low efficiency.Herein,Pd@Pt Ni Co Ru Ir coreshell mesoporous bifunctional electrocatalysts were fabricated via a one-step wet-chemical reduction approach.By utilizing the limiting effect of triblock copolymers,gradient distribution control of six metal elements(Pd core and Pt/Ni/Co/Ru/Ir high-entropy alloys shell) was achieved,where the high-entropy alloy shell forms high-density active sites through lattice distortion effect.With the help of lattice distortion and mesoporous-confinement-enabled interfacial coupling effects,Pd@Pt Ni Co Ru Ir catalyst exhibited exceptional bifunctional performance in alkaline media:A low hydrogen evolution reaction(HER) overpotential of 30.5 m V at 10 m A/cm^(2) and a high ammonia oxidation reaction(AOR) peak current density of 19.6 m A/cm^(2) at 0.7 V vs.RHE,representing a 3.83-fold enhancement over commercial Pt/C.Moreover,a rechargeable Zn-NH_(3) battery system was constructed and achieved 92.3 % Faradaic efficiency(FE) for NH_(3)-to-H_(2) conversion with outstanding stability at 16 m A/cm^(2),thereby providing an innovative solution for efficient ammonia decomposition-based hydrogen production.
基金support from the National Natural Science Foundation of China(22088101,21733003,22365021,22305132)the Inner Mongolia Autonomous Region“Grassland Talents”Project(2024098)+3 种基金the Inner Mongolia Natural Science Foundation Youth Fund(2023QN02014)The Local Talent Project of Inner Mongolia(12000-15042222)the Basic Research Expenses Supported under 45 Years Old of Inner Mongolia(10000-23112101/036)the“Young Academic Talents”Program of Inner Mongolia University 23600-5233706.
文摘As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 nm)severely limits their application in scenarios such as macromolecular mass transfer and so on.In order to overcome this re-striction,mesoporous MOFs(meso-MOFs)with a larger aperture(2-50 nm)have attracted much attention due to their potential applications in biological macromolecular catalysis,energy storage and other fields.To date,how to accurately regulate its mesopore topology and pore ordering still faces important technical challenges.
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 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.
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Organic ultraviolet(UV)filters play a crucial role in reducing sunburn,photoaging,and the risk of skin cancer induced by UV radiation.However,the challenges posed by photodegradation,potential phototoxicity,and poor dispersion characteristics of organic UV filters significantly hinder their practical applications.This study aims to encapsulate avobenzone,a widely used UV filter,in mesoporous silica(MPS)to form AB@MPS particles via an in-situ sol-gel process,and to research their sunscreen performance as stabilizers in Pickering emulsion.The UV absorption capability of AB@MPS particles is stronger than free avobenzone.The in vitro skin penetration study reveals a greatly reduced permeability(73.9%)for avobenzone from AB@MPS compared to its free form.Furthermore,the photostability of AB@MPS particles increases 14.3 times compared to that of free avobenzone.In UV protection tests,the Pickering emulsion’s anti-UVA efficacy is 2.28 times greater than that of 20%PG solution,4.41 times greater than Carbomer hydrogel,and 3.59 times greater than the cream formulation.The SPF value of the Pickering emulsion is 2.41 times greater than the 20%PG solution,2 times greater than the Carbomer hydrogel,and 6.77 times greater than the cream formulation.This study presents a promising strategy for the application of Pickering emulsions in the cosmetic and pharmaceutical sectors,providing a safe and efficient formulation for sunscreens.
文摘To alleviate the quality deterioration and extend the shelf life of crucian carp fillets,a bio-based active composite film integrating eugenol(EG)-loaded mesoporous silica nanoparticles(MSNs)modified with caffeic acid(CA)within the zein matrix(EG/CA-MSN/Zein)was developed.This study compared the effects of EG/CA-MSN/Zein,polyethylene(PE),and zein films on the quality of fish fillets during refrigerated storage.The results showed that the EG/CA-MSN/Zein film significantly retarded the increase in pH and microbial growth.Moreover,the film had higher water-holding capacity(WHC),better texture,and color stability,as indicated by low-field nuclear magnetic resonance(LF-NMR),magnetic resonance imaging(MRI),and sensory evaluation.The EG/CA-MSN/Zein composite film extended the shelf life of crucian carp fillets by 3-4 days,highlighting its potential as an environmentally friendly and efficient packaging material for aquatic products.
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supported by the National Natural Science Foundation of China(52002366,22075263,22571288)the Fundamental Research Funds for the Central Universities(WK2060000091,WK2060250115,WK2060000039)the Students’Innovation and Entrepreneurship Foundation of USTC(CY2023C021).
文摘The slow kinetics of the cathode CO_(2) reduction reaction and the decomposition reaction of Li2CO3,a widebandwidth insulating product,lead to difficult CO_(2) capture and high charging potential in Li-CO_(2) batteries.To improve the reaction kinetics and decrease the reaction overpotential,we synthesized mesoporous Pt nanosheets with high tensile strain.The presence of many unsaturated coordinated Pt atoms around the pores gives rise to tensile strain in the mesoporous Pt nanosheets.This tensile strain plays a key role in regulating the interactions between the catalytic surface of Pt and the adsorbed intermediates.The two-dimensional structure provides more active sites on the surface for the catalytic reactions.These superiorities enable a low overpotential of 0.36 V at a cutoff capacity of 100μAh·cm^(−2) at a current density of 10μA·cm^(−2) over more than 2000 h.This study opens new possibilities for the rational design of metal-based materials with strain engineering for electrochemical energy storage.
基金supported by the National Key Research and Development Program Foundation of China(2016YFC0209203)the National Natural Science Foundation of China(21707130,21325731)~~
文摘KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these catalysts and the effect of pore sizes on ethanol catalytic oxidation were investigated.Mn‐40,Mn‐100,and Mn‐150 have triple,double,and single pore systems,respectively.On decreasing the aging temperature of KIT‐6,the pore sizes of KIT‐6 decrease and that of mesoporous MnO2 catalysts increase.The pore sizes and catalytic activities increase in the order:Mn‐40>Mn‐100>Mn‐150.Mn‐40 catalyst has a higher TOF(0.11 s–1 at 120°C)and the best catalytic activity for ethanol oxidation because of a bigger pore size with three pore systems with maximum distribution at 1.9,3.4,and 6.6 nm,decrease in symmetry and degree of order,more surface lattice oxygen species,oxygen vacancies resulting from more Mn3+ions,and better low‐temperature reducibility.
基金financially supported by the Ningbo Institute of Digital Twin,Eastern Institute of Technology,Ningbo.We also acknowledge supportfrom the Young Innovative Talent of Yongjiang Talent Project(2023A‐387‐G).
文摘The efficient storage and application of sustainable solar energy has drawn significant attention from both academic and industrial points of view.However,most developed catalytic materials still suffer from insufficient mass diffusion and unsatisfactory durability due to the lack of interconnected and regulatable porosity.Developing catalytic architectures with engineered active sites and prominent stability through rational synthesis strategies has become one of the core projects in solar-driven applications.The unique properties of mesoporous silicas render them among the most valuable functional materials for industrial applications,such as high specific surface area,regulatable porosity,adjustable surface properties,tunable particle sizes,and great thermal and mechanical stability.Mesoporous silicas serve as structural templates or catalytic supports to enhance light harvesting via the scattering effect and provide large surface areas for active site generation.These advantages have been widely utilized in solar applications,including hydrogen production,CO_(2)conversion,photovoltaics,biomass utilization,and pollutant degradation.To achieve the specific functionalities and desired activity,various types of mesoporous silicas from different synthesis methods have been customized and synthesized.Moreover,morphology regulation and component modification strategies have also been performed to endow mesoporous silica-based materials with unprecedented efficiency for solar energy storage and utilization.Nevertheless,reviews about synthesis,morphology regulation,and component modification strategies for mesoporous silica-based catalyst design in solar-driven applications are still limited.Herein,the latest progress concerning mesoporous silica-based catalysis in solar-driven applications is comprehensively reviewed.Synthesis principles,formation mechanisms,and rational functionalities of mesoporous silica are systematically summarized.Some typical catalysts with impressive activities in different solar-driven applications are highlighted.Furthermore,challenges and future potential opportunities in this study field are also discussed and proposed.This present review guides the design of mesoporous silica catalysts for efficient solar energy management for solar energy storage and conversion applications.
基金financially supported by the National Natural Science Foundation of China(11475041,U21A20323)Kunlun Talent Program of Qinghai Province,Qinghai Provincial Science and Technology Project(2024-QY-203)Sci-Tech Project of Qinghai Salt Lake Industry Co.,Ltd.(E141GH01).
文摘1.Introduction Magnesium oxide(MgO)has attracted considerable attention in recent years due to its economic viability,excellent biocompatibil-ity,chemical stability,and non-toxic,odorless nature[1,2].These inherent properties position it as a promising candidate for various applications.
基金financially supported by the National Key Research and Development Program(Nos.2022YFB2502104 and 2022YFA1602700)the Key Research and Development Program of Jiangsu Provincial Department of Science and Technology of China(No.BE2022332)+4 种基金the Jiangsu Carbon Peak Carbon Neutralization Science and Technology Innovation Special Fund(No.BE2022605)the National Natural Science Foundation of China(Nos.22109073,22379071)the DECRA program of Australian Research Council(No.DE230100357)the JSPS KAKENHI(No.JP23K13703)the Center for Computational Materials Science,Institute for Materials Research,Tohoku University for the use of MASAMUNE-IMR(202312-SCKXX-0203)。
文摘Perovskite oxides(ABO_(3))are thought to be promising electrocatalysts for oxygen evolution reaction(OER),but their specific surface area(SSA)is too low(usually<10 m^(2) g^(−1)).Developing advanced ABO_(3) electrocatalysts with high SSA and optimized structure is of great significance but remains a tremendous challenge.Herein,we propose a general strategy for fabrication of mesoporous perovskite oxide nanosheets(MPONs)with controllable atomic doping via self-sacrificial template-induced nanostructure modulation.A variety of MPONs including LaFeO_(3),A-site-doped LaFeO_(3)(A-LaFeO_(3),where A is Pr,Nd,Sm,Eu,or Gd)and B-site-doped LaFeO_(3)(B-LaFeO_(3),where B is Mn,Co,Ni,Cu,or Zn)have been achieved.Interestingly,it is discovered that the catalytic activities of A-LaFeO_(3) MPONs as OER catalysts are overall higher than those of B-LaFeO_(3) ones.Especially,the screened Eu-LaFeO_(3) MPONs only require a low overpotential of 267 mV at 10 mA cm^(−2),outperforming most reported perovskite oxides.The superior catalytic activity of Eu-LaFeO_(3) MPONs is attributed to their favorable porous structure,which increases the density of active sites,and enhanced lattice oxygen participation,which improves the intrinsic activity.This study provides guidance for the design and controlled synthesis of advanced rare-earth-doped MPONs with ultrahigh SSA for enhanced electrocatalysis.
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the financial supports from the National Natural Science Foundation of China(Nos.22378093,21878065)Natural Science Foundation of Hebei Province,China(No.E2022201100)+2 种基金the Science and Technology Support Plan of Baoding City(No.2241ZF111)the Medical Science Foundation of Hebei University(No.2021A09)the Foundation of Affiliated Hospital of Hebei University(No.2021Z003)。
文摘The preparation of immobilized enzyme with excellent performance is one of the difficulties that restrict the application of enzyme catalysis technology.Here,Candida rugosa lipase(CRL)was firstly adsorbed on the surface of magnetic zeolitic imidazolate framework-8(ZIF-8)nanospheres,which was further encapsulated with a mesoporous SiO_(2)nano-membrane formed by tetraethyl orthosilicate(TEOS)polycondensation.Consequently,lipase could be firmly immobilized on carrier surface by physical binding rather than chemical binding,which did not damage the active conformation of enzyme.There were mesopores on the silica nano-membrane,which could improve the accessibility of enzyme and its apparent catalytic activity.Moreover,silica membrane encapsulation could also improve the stability of enzyme,suggesting an effective enzyme immobilization strategy.It showed that TEOS amount and the encapsulation time had significant effects on the thickness of silica membrane and the enzyme activity.The analysis in enzyme activity and protein secondary structure showed that lipase encapsulated in silica membrane retained the active conformation to the greatest extent.Compared with the adsorbed lipase,the encapsulated lipase increased its thermostability by 3 times and resistance to chemical denaturants by 7 times.The relative enzyme activity remained around 80%after 8 repetitions,while the adsorbed lipase only remained at7.3%.
