Crucial for mediating inflammation and the perception of pain,the ion channel known as transient receptor potential ankyrin 1(TRPA1)holds significant importance.It contributes to the increased production of cytokines ...Crucial for mediating inflammation and the perception of pain,the ion channel known as transient receptor potential ankyrin 1(TRPA1)holds significant importance.It contributes to the increased production of cytokines in the inflammatory cells of cartilage affected by osteoarthritis and represents a promising target for the treatment of this condition.By leveraging the unique advantages of liposomes,a composite microsphere drug delivery system with stable structural properties and high adaptability can be developed,providing a new strategy for osteoarthritis(OA)drug therapy.The liposomes as drug reservoirs for TRPA1 inhibitors were loaded into hyaluronic acid methacrylate(HAMA)hydrogels to make hydrogel microspheres via microfluidic technology.An in vitro inflammatory chondrocyte model was established with interleukin-1β(IL-1β)to demonstrate HAMA@Lipo@HC’s capabilities.A destabilization of the medial meniscus(DMM)mouse model was also created to evaluate the efficacy of intra-articular injections for treating OA.HAMA@Lipo@HC has a uniform particle-size distribution and is injectable.The drug encapsulation rate was 64.29%±2.58%,with a sustained release period of 28 days.Inhibition of TRPA1 via HC-030031 effectively alleviated IL-1β-induced chondrocyte inflammation and matrix degradation.In DMM model OA mice,microspheres showed good long-term sustained drug release properties,improved joint inflammation microenvironment,reduced articular cartilage damage and decreased mechanical nociceptive threshold.This research pioneers the creation of a drug delivery system tailored for delivery into the joint cavity,focusing on TRPA1 as a therapeutic target for osteoarthritis.Additionally,it offers a cutting-edge drug delivery platform aimed at addressing diseases linked to inflammation.展开更多
Incorporation of heteroatoms into the framewo rk of zeolites has become a significant strategy to improve their performance in catalysis and adsorption,because the obtained heteroatom zeolites exhibit quite different ...Incorporation of heteroatoms into the framewo rk of zeolites has become a significant strategy to improve their performance in catalysis and adsorption,because the obtained heteroatom zeolites exhibit quite different properties from the conventional aluminosilicate zeolites in aspects of surface acidity,pore structures,particle size and so on.In this review,the progress on the heteroatom zeolites including their synthesis and application is highlighted.First,the recent advance on the design and synthesis of different heteroatom zeolites is summarized.Special emphasis is placed on the introduction and comparison of three typical methods,including the direct synthesis,post synthesis and improved direct synthesis,for the traditional heteroatom zeolites(such as TS-1,Sn-MFI,Sn-β) and newly-reported heteroatom zeolites(such as W-MFI,Mo-MFI).According to their intrinsic characteristics,the application of heteroatom zeolites in diverse fields,such as production of fine chemicals,air pollution control and biomass conversion is then discussed.Finally,the challenges and perspective on the future development of heteroatom zeolites in low-cost preparation and practical application are proposed.展开更多
A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and cryst...A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and crystal sizes, respectively. The ultrafine Fe_2O_3 nanoparticles in size of 5 nm can be highly dispersed on zeolite Y matrix due to its much better wettability than ZSM-5 and mordenite. By using the obtained Fe_2O_3/zeolite composite as the heterogeneous Fenton-like catalysts, the degradation of phenol as a model reaction was systematically investigated, including the zeolite supports, particle size and dispersion of Fe_2O_3, and reaction conditions of H_2O_2 concentration, temperature, and pH value. The catalyst based on zeolite Y with Fe loading of 9% exhibited the best phenol degradation efficiency (> 90%)in neutral pH within 2 h. Its high catalytic activity in Fenton reaction can be attributed to the bifunctional properties of strong surface BrФnsted acidity and high reactivity of octahedral Fe^(3+) in the highlydispersed ultrafine Fe_2O_3 nanoparticles in size of 5 nm, which were the primary active centers to quickly decompose H_2O_2 into hydroxyl radicals. Since phenol degradation can be performed under mild conditions of ambient temperature (283-323 K) and a wide pH range (4.0-7.0), the catalysts can be easily recovered for recyclable use with stable degradation activity, which own the immense potential in deep treatment of organic pollutants in industrial wastewater.展开更多
Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction bet...Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction between high crystallinity and high surface area,the synthesis of mesoporous SMOs heterojunctions with highly o rdered mesostructures,highly crystallized frameworks,and high surface area remains a huge challenge.In this work,we develop a novel"acid-base pair"adjusted solvent evaporation induced self-assembly(EISA)strategy to prepare highly crystallized ordered mesoporous TiO2/WO3(OM-TiO2/WO3)heterojunctions.The WCl6 and titanium isopropoxide(TIPO)are used as the precursors,respectively,which function as the"acid-base pair",enabling the coassembly with the structure directing agent(PEO-b-PS)into highly ordered meso structures.In addition,PEO-b-PS can be converted to rigid carbon which can protect the meso structures from collapse during the crystallization process.The resultant OM-TiO2/WO3 heterojunctions possess primitive cubic mesostructures,large pore size(~21.1 nm),highly crystalline frameworks and surface area(~98 m2/g).As a sensor for acetone,the obtained OM-TiO2/WO3 show excellent re sponse/recovery perfo rmance(3 s/5 s),good linear dependence,repeatability,selectivity,and long-term stability(35 days).展开更多
Lithium sulfur(Li-S) batteries are regarded as promising candidates for next-generation rechargeable batteries. However, the insulation characteristic of sulfur and severe polysulfide dissolution hindered their develo...Lithium sulfur(Li-S) batteries are regarded as promising candidates for next-generation rechargeable batteries. However, the insulation characteristic of sulfur and severe polysulfide dissolution hindered their development. We presented a facile approach to fabricate Li-S batteries by coating commercial carbon nanotube or graphene slurries on normal sulfur cathode electrode to construct a dual-layer cathode electrode. The conductive CNT or graphene layer could not only improve the conductivity of sulfur cathode, but also suppress the polysulfide diffusion. The CNT@S cathode delivered a high reversible capacity of 740 mAh/g over 300 cycles at 1 C and 870 mAh/g over 100 cycles at 0.2 C. Furthermore, this strategy could be realized on the commercial product line of lithium-ion batteries, which made it possible to large-scale produce Li-S batteries.展开更多
Photo-responsive azobenzene （ABZ） derivatives with different end groups （R） as photoswitchable molecules were employed to construct self-assembled monolayers （SAMs） on silicon substrate by using 3-glycidoxypropy...Photo-responsive azobenzene （ABZ） derivatives with different end groups （R） as photoswitchable molecules were employed to construct self-assembled monolayers （SAMs） on silicon substrate by using 3-glycidoxypropyltrimethoxysilane （GPTS） as the bridging molecules. The assembly process was optimized by changing various parameters, including the type and concentration of ABZ derivatives, reaction time, etc. The obtained SAMs were fully characterized and evaluated using UV spectroscopy, atomic force microscope （AFM）, elllipsometer, static contact angle and X-ray photoelectron spectroscopy （XPS）. It is found that the end group property of azobenzene derivatives is critical to the obtained SAMs＇ photoresponsive properties. Compared with hydrophobic compounds （4-（4＇-aminophenylazo） benzoic acid, ABZ-CF3）, the hydrophilic compounds （4-（4＇-aminophenylazo） benzoic acid, ABZ-COOH） show excellent reversible photoswitching performance with a large contact angle change of 35° under oDtimized process, and the SAMs are removable bv thermal treatment at 240 ℃ in air for onlv 5 min.展开更多
Green and recyclable solid acid catalysts are in urgent demand as a substitute for conventional liquid mineral acids.In this work,a series of novel sulfonic acid-functionalized core-shell Fe_(3)O_(4)@carbon microspher...Green and recyclable solid acid catalysts are in urgent demand as a substitute for conventional liquid mineral acids.In this work,a series of novel sulfonic acid-functionalized core-shell Fe_(3)O_(4)@carbon microspheres(Fe_(3)O_(4)@C-SO_(3)H)have been designed and synthesized as an efficient and recyclable heterogeneous acid catalyst.For the synthesis,core-shell Fe_(3)O_(4)@RF(resorcinol-formaldehyde)microspheres with tunable shell thickness were achieved by interfacial polymerization on magnetic Fe_(3)O_(4)microspheres.After high-temperature carbonization,the microspheres were eventually treated by surface sulfonation,re sulting in Fe_(3)O_(4)@C-x-SO_(3)H(x stands for carbonization temperature)microspheres with abundant surface SO_(3)H groups.The obtained microspheres possess uniform core-shell structure,partially-graphitized carbon skeletons,superparamagnetic property,high magnetization saturation value of 10.6 emu/g,and rich SO_(3)H groups.The surface acid amounts can be adju sted in the range of 0.59-1.04 mmol/g via sulfonation treatment of carbon shells with different graphitization degrees.The magnetic Fe_(3)O_(4)@C-x-SO_(3)H microspheres were utilized as a solid acid catalyst for the acetalization reaction between benzaldehyde and ethylene glycol,demonstrating high selectivity(97%)to benzaldehyde ethylene glycol acetal.More importantly,by applying an external magnetic field,the catalysts can be easily separated from the heterogeneous reaction solutions,which later show well preserved catalytic activity even after 9 cycles,revealing good recyclability and high stability.展开更多
Among various gas sensing materials, metal oxide semiconductors have shown great potential as resistive type sensors. The ordered porous structural metal oxide semiconductors with well-defined meso- or macro-pores che...Among various gas sensing materials, metal oxide semiconductors have shown great potential as resistive type sensors. The ordered porous structural metal oxide semiconductors with well-defined meso- or macro-pores chemically synthesized via soft-templating method and nanocasting strategy have high porosity, highly interconnected pore channels and high surface area with enormous active sites for interacting with gaseous molecules. These features enable them good performance in gas sensing, including high sensitivity, fast response and recovery, good selectivity. This review gives a comprehensive summary about the porous metal oxides with focus on the synthesis methods, structure related properties, as well as the modification strategies for gas sensing improved performances.展开更多
To achieve real-time monitoring of humidity in various applications,we prepared facile and ultra-thin CoAl layered double hydroxide(CoAl LDH)nanosheets to engineer quartz crystal microbalances(QCM).The characteristics...To achieve real-time monitoring of humidity in various applications,we prepared facile and ultra-thin CoAl layered double hydroxide(CoAl LDH)nanosheets to engineer quartz crystal microbalances(QCM).The characteristics of CoAl LDH were investigated by transmission electron microscopy(TEM),X-ray diffraction(XRD),X-ray photoelectric spectroscopy(XPS),Brunauer–Emmett–Telle(BET),atomic force microscopy(AFM)and zeta potential.Due to their large specific surface area and abundant hydroxyl groups,CoAl LDH nanosheets exhibit good humidity sensing performance.In a range of 11.3%and 97.6%relative humidity(RH),the sensor behaved an ultrahigh sensitivity(127.8 Hz/%RH),fast response(9.1 s)and recovery time(3.1 s),low hysteresis(3.1%RH),good linearity(R^(2)=0.9993),stability and selectivity.Besides,the sensor can recover the initial response frequency after being wetted by deionized water,revealing superior self-recovery ability under high humidity.Based on in-situ Fourier transform infrared spectroscopy(FT-IR),the adsorption mechanism of CoAl LDH toward water molecules was explored.The QCM sensor can distinguish different respiratory states of people and wetting degree of fingers,as well as monitor the humidity in vegetable packaging,suggesting excellent properties and a promising application in humidity sensing.展开更多
Acephate pesticide contamination in agricultural production has caused serious human health problems.Metal oxide semiconductor(MOS)gas sensor can be used as a portable and promising alternative tool for efficiently de...Acephate pesticide contamination in agricultural production has caused serious human health problems.Metal oxide semiconductor(MOS)gas sensor can be used as a portable and promising alternative tool for efficiently detection of acephate.In this study,hierarchical assembled SnO_(2)nanosphere,SnO_(2)hollow nanosphere and SnO_2 nanoflower were synthesized respectively as high efficiency sensing materials to build rapid and selective acephate pesticide residues sensors.The morphologies of different SnO_(2)3 D nanostructures were characterized by various material characterization technology.The sensitive performance test results of the 3 D SnO_(2)nanomaterials towards acephate show that hollow nanosphere SnO_(2)based sensor displayed preferable sensitivity,selectivity,and rapid response(9 s)properties toward acephate at the optimal working temperature(300℃).This SnO_(2)hollow nanosphere based gas sensor represents a useful tool for simple and highly effective monitoring of acephate pesticide residues in food and environment.According to the characterization results,particularly Brunauer-Emmett-Teller(BET)and Ultraviolet-Visible Spectroscopy(UV-vis),the obvious and fast response can be attributed to the mesoporous hollow nanosphere structure and appropriate band gap of SnO_2 hollow nanosphere.展开更多
Solid photocatalysts with high specific surface area,superior photoactivity and ease of recycling are highly desired in chemical process,water treatment and so on.In this study,a facile stepwise sol-gel coating approa...Solid photocatalysts with high specific surface area,superior photoactivity and ease of recycling are highly desired in chemical process,water treatment and so on.In this study,a facile stepwise sol-gel coating approach was utilized to synthesize Pt decorated oxygen-deficient mesoporous titania microspheres with core-shell structure and convenient magnetic separability(denoted as Fe3 O4@-SiO2@Pt/mTiO2-x).These photocatalysts consist of magnetic Fe3 O4 cores,nonporous insulating SiO2 middle layer and mesoporous anatase TiO2-x shell decorated by Pt nanoparticles(~3.5 nm)through wet impregnation and H2 reduction.As a result of high activity of oxygen-deficiency of black TiO2-x by H2 reduction and efficient inhibition of electron-hole recombination by Pt nanoparticles,the rationally designed core-shell Fe3 O4@SiO2@Pt/mTiO2-x photocatalysts exhibit superior photocatalytic performance in rhodamine B(RhB)degradation under visible light irradiation,with more than 98%of RhB degraded within 50 min.These core-shell structured photocatalysts show excellent recyclability under the assistance of magnetic separation with well-retained photocatalytic performance even after running five cycles.This stepwise synthesis method paves the way for the rational design of a high-efficiency recyclable heterogeneous catalyst,including photocatalysts,for various applications.展开更多
Highly luminescent colloidal nanocrystals have wide applications in bioimaging and various optoelectronic devices.Herein we report a facile and mild procedure by combining S2-treatment and binary ligand passivation,wh...Highly luminescent colloidal nanocrystals have wide applications in bioimaging and various optoelectronic devices.Herein we report a facile and mild procedure by combining S2-treatment and binary ligand passivation,which can efficiently enhance the luminescent property of CdSe nanocrystals at room temperature.The photoluminescence quantum yield of as-treated CdSe nanocrystals exhibits drastic enhancement(e.g.,188 times for CdSe nanorods)after this dual-passivation treatment.The methodology proposed here can be applied to various CdSe nanocrystals,regardless of their sizes,shapes,and crystal structures.展开更多
The rapid development of internet and internet of things brings new opportunities for the expansion of intelligent sensors,and acetone as a major disease detection indicator(i.e.,diabetes)making it become extremely im...The rapid development of internet and internet of things brings new opportunities for the expansion of intelligent sensors,and acetone as a major disease detection indicator(i.e.,diabetes)making it become extremely important clinical indicator.Herein,uniform mesoporous ZnO spheres were successfully synthesized via novel formaldehyde-assisted metal-ligand crosslinking strategy.In order to adjust the pore structure of mesoporous ZnO,various mesoporous ZnO spheres were synthesized by changing weight percentage of Zn(NO_(3))_(2)·6 H_(2)O to tannic acid(TA).Moreover,highly active heterojunction mesoporous ZnO/Co_(3)O_(4)has been fabricated based on as-prepared ultra-small Co_(3)O_(4)nanocrystals(ca.3 nm)and mesoporous ZnO spheres by flexible impregnation technique.Profit from nano-size effect and synergistic effect of p-n heterojunction,mesoporous ZnO/Co_(3)O_(4)exhibited excellent acetone sensing performance with high selectivity,superior sensitivity and responsiveness.Typically,5 wt%Co_(3)O_(4)embedded mesoporous ZnO sphere showed prominent acetone response(ca.46 for 50 ppm),which was about 11.5 times higher than that in pure ZnO sensing device,and it was also endowed high cyclic stability.The nanocrystals embedded hybrid material is expected to be used as promising efficient material in the field of catalysis and gas sensing.展开更多
The freshness of seafood can be judged by detecting the concentration of triethylamine(TEA). In this work, 2D Cu O porous nanosheets(Cu O PNs) were prepared by a graphene oxide template method and their particle sizes...The freshness of seafood can be judged by detecting the concentration of triethylamine(TEA). In this work, 2D Cu O porous nanosheets(Cu O PNs) were prepared by a graphene oxide template method and their particle sizes were regulated by changing the calcination temperature. Their structure, morphology and gas sensing performances were investigated by various characterization methods. The response(Rg/Ra) of the gas sensor based on Cu O PNs calcined at 700oC was as high as 440-100 ppm TEA at the operating temperature of 40 ℃. The detection limit was as low as 0.25 ppm. In addition, the gas sensor has good selectivity and stability. The excellent TEA sensitivity is mainly resulted from the appropriate particle size and loose porous framework. This work not only paves the way to explore the novel low temperature TEA gas sensors, but also provides deep insight on improving the structure and properties of gas sensitive materials by controlling the calcination temperature.展开更多
Most catalytic processes are achieved by heating the whole reaction systems including the entire reactor,substrate and solvent,which leads to energy loss and obvious heat transfer limits.In this study,induction heatin...Most catalytic processes are achieved by heating the whole reaction systems including the entire reactor,substrate and solvent,which leads to energy loss and obvious heat transfer limits.In this study,induction heating was employed to boost the catalytic Suzuki-Miyaura cross-coupling reactions by using conductive superparamagnetic microspheres with loaded Pd nanoparticles as heterogeneous catalysts.It was found that,at the same apparent reaction temperatures,the reactions by adopting the induction heating all exhibit better catalytic performance with higher conversion and yield,as compared to the reactions using conventional joule heating.The improvement is mainly attributed to the localized heating effect endowed by high efficiency of the heat transfer from the heat source to catalytic sites,which dissipates the electromagnetic energy through Néel relaxation mechanism.Moreover,it has be found that the reactions have been largely accelerated,resulting in much shorter reaction time required to approach a given value of reactant conversion.These results indicate that the unique heating method based on the superparamagnetic nanomaterials as both the inductive component and catalyst support holds a promising application for fast and efficient heterogeneous catalytic process,and exhibits potential for improving energy transfer efficiency and reducing the side reactions attributed to the uneven temperature profile.展开更多
Plant polyphenol-based coordination polymers(CPs) with ultra-small particle size and tailorable compositions are highly desired in biomedical applicatio ns,but their synthesis is still challenging due to the sophistic...Plant polyphenol-based coordination polymers(CPs) with ultra-small particle size and tailorable compositions are highly desired in biomedical applicatio ns,but their synthesis is still challenging due to the sophisticated coordination assembly process and unavoidable self-oxidation polymerization of polyphenol. He rein,a general ligand covalent-modification mediated coordination assembly strategy is proposed for the synthesis of water-dispersible CPs with tunable metal species(e.g., Gd,Cu,Ni,Zn,Fe)and ultra-small diameter(8.6-37.8 nm) using nontoxic plant polyphenol(e.g..tannic acid,gallic acid) as a polymerizable ligand.Polyphenol molecules react with formaldehyde firstly,which can effectively retard the oxidation induced self-polymerization of polyphenol and lead to the formation of metal ions containing CPs colloidal nanoparticles.These ultrafine nanoparticles with stably chelated metal io ns are highly water dispersible and thus advantageous for bioimaging.As an example,ultra-small Gd contained CPs exhibit higher longitudinal relaxivity(r_(1)=25.5 L mmol^(-1) s^(-1)) value with low r2/r1(1.19) than clinically used Magnevist(Gd-DTPA,r1=3.7 L mmol^(-1) s^(-1)) .Due to the enhanced permeability and retention effect,they can be further used as a positive contrast agent for T1-weighted MR imaging of tumour.展开更多
In persulfate-based advanced oxidation process(PS-AOPs),fixing nanosized metal oxide on processable substrates is highly desirable to avoid the aggregation and loss of nanocatalysts during the practical application.Ho...In persulfate-based advanced oxidation process(PS-AOPs),fixing nanosized metal oxide on processable substrates is highly desirable to avoid the aggregation and loss of nanocatalysts during the practical application.However,it is still challenging to develop a versatile strategy for the deposition of metal oxide nanocatalysts on various substrates with different physicochemical properties.Herein,polyphenols are utilized as a“molecular glue”and reductant to mediate the interfacial deposition of MnO_(2) nanocatalysts on different substrates.MnO_(2) nanocatalysts were in-situ grown on macroscope mineral substrates(e.g.,airstone)via an interfacial redox strategy between tannic acid(TA)and oxidized KMnO4,and then employed as a fixed catalyst of peroxymonosulfate(PMS)activation for treating pharmaceutical and personal care products(PPCPs)in water.The fixed MnO_(2) exhibited superior catalytic performance toward different PPCPS via a singlet oxygen(^(1)O_(2))-dominated nonradical oxidation pathway.PPCPs in the secondary effluent of wastewater treatment plants could be effectively removed by a fixed-bed column of the fixed MnO_(2) with long term stability.Redox cycle of Mn^(4+)/Mn^(3+)and surface hydroxyl group of the fixed MnO_(2) was proved to be responsible for the activation of PMS.This work provides a new avenue for developing fixed metal oxides for sustainable water treatment.展开更多
Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment,and thus it is distinctly meaningful to monitor benzene series with quickly,r...Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment,and thus it is distinctly meaningful to monitor benzene series with quickly,real-time and efficient technique.Herein,novel sulfur-doped mesoporous WO_(3)materials were synthesized via classical in-situ solvent evaporation induced co-assembly strategy combined with doping engineering,which possessed highly crystallized frameworks,high specific surface area(40.9–63.8 m^(2)/g)and uniform pore size(~18 nm).Benefitting from abundant oxygen vacancy and defects via S-doping,the tailored mesoporous S/m WO_(3)exhibited excellent benzene sensing performance,including high sensitivity(50 ppm vs.48),low detection limit(ca.500 ppb),outstanding selectivity and favorable stability.In addition,the reduction of band gap resulted from S-doping promotes the carrier migration in the sensing materials and the reaction at the gas–solid sensing interfaces.It provides brand-new approach to design sensitive materials with multiple reaction sites.展开更多
As a key biomarker for noninvasive diagnosis of diabetes,the selective detection of trace acetone in exhaled gas using a portable and low-cost device remains a great challenge.Semiconductor metal oxide(SMO)based gas s...As a key biomarker for noninvasive diagnosis of diabetes,the selective detection of trace acetone in exhaled gas using a portable and low-cost device remains a great challenge.Semiconductor metal oxide(SMO)based gas sensors have drawn signification attention due to their potential in miniaturization,user-friendliness,high cost-effectiveness and selective real-time detection for noninvasive clinical diagnosis.Herein,we propose a one-pot solvent evaporation induced tricomponent co-assembly strategy to design a novel ordered mesoporous SMO of silica-implanted WO_(3)(Si O_(2)/WO_(3))as sensing materials for trace acetone detection.The controlled co-assembly of silicon and tungsten precursors and amphiphilic diblock copolymer poly(ethylene oxide)-block-polystyrene(PEO-b-PS),and the subsequent thermal treatment enable the local lattice disorder of WO_(3)induced by the amorphous silica and the formation of ordered mesoporous Si O_(2)/WO_(3)hybrid walls with a unique metastableε-phase WO_(3)framework.The obtained mesoporous SiO_(2)/WO_(3)composites possess highly crystalline framework with large uniform pore size(12.0-13.3 nm),high surface area(99-113 m^(2)/g)and pore volume(0.17-0.23 cm^(3)/g).Typically,the asfabricated gas sensor based on mesoporous 2.5%Si O_(2)/WO_(3)exhibits rapid response/recovery rate(5/17 s),superior sensitivity(R_(air)/R_(gas)=105 for 50 ppm acetone),as well as high selectivity towards acetone.The limit of detection is as low as 0.25 ppm,which is considerably lower than the thresh value of acetone concentration(>1.1 ppm)in the exhaled breath of diabetic patients,demonstrating its great prospect in real-time monitoring in diabetes diagnosis.Moreover,the mesoporous 2.5%Si O_(2)/WO_(3)sensor is integrated into a wireless sensing module connected to a smart phone,providing a convenient real-time detection of acetone.展开更多
Mesoporous late-transition metal oxides have great potential in applications of energy,catalysis and chemical sensing due to their unique physical and chemical properties.However,their synthesis via the flexible and s...Mesoporous late-transition metal oxides have great potential in applications of energy,catalysis and chemical sensing due to their unique physical and chemical properties.However,their synthesis via the flexible and scalable soft-template method remain a great challenge,due to the weak organic-inorganic interaction between the frequently used surfactants(e.g.,Pluronic-type block copolymers) and metal oxide precursors,and the low crystallization temperature of metal oxides.In this study,ordered mesoporous NiO with dual mesopores,high surface area and well-interconnected crystalline porous frameworks have been successfully synthesized via the facile solvent evaporation-induced co-assembly(EICA) method,by using lab-made amphiphilic diblock copolymer polystyrene-b-poly(4-vinylpyridine)(PS-b-P4 VP) as both the structure-directing agent(the soft template) and macromolecular chelating agents for nickel species,THF as the solvent,and nickel acetylacetonate(Ni(acac)2) as inorganic precursor.Similarly,by using Ni(acac)2 and Fe(acac)3 as the binary precursors,ordered mesoporous Fedoped NiO materials can be obtained,which have bimodal mesopores of large mesopores(32.5 nm) and secondary mesopores(4.0-11.5 nm) in the nanocrystal-assembled walls,high specific surface areas(~74.8 m^2/g) and large pore value(~0.167 cm^3/g).The obtained mesoporous Fe-doped NiO based gas sensor showed superior ethanol sensing performances with good sensitivity,high selectivity and fast response-recovery dynamics.展开更多
基金supported by the National Key Research and Development Program of China(No.82230071)National Natural Science Foundation of China(Nos.82202674,82202334)Wenzhou Science and Technology Project(Nos.Y20220178,Y20220016).
文摘Crucial for mediating inflammation and the perception of pain,the ion channel known as transient receptor potential ankyrin 1(TRPA1)holds significant importance.It contributes to the increased production of cytokines in the inflammatory cells of cartilage affected by osteoarthritis and represents a promising target for the treatment of this condition.By leveraging the unique advantages of liposomes,a composite microsphere drug delivery system with stable structural properties and high adaptability can be developed,providing a new strategy for osteoarthritis(OA)drug therapy.The liposomes as drug reservoirs for TRPA1 inhibitors were loaded into hyaluronic acid methacrylate(HAMA)hydrogels to make hydrogel microspheres via microfluidic technology.An in vitro inflammatory chondrocyte model was established with interleukin-1β(IL-1β)to demonstrate HAMA@Lipo@HC’s capabilities.A destabilization of the medial meniscus(DMM)mouse model was also created to evaluate the efficacy of intra-articular injections for treating OA.HAMA@Lipo@HC has a uniform particle-size distribution and is injectable.The drug encapsulation rate was 64.29%±2.58%,with a sustained release period of 28 days.Inhibition of TRPA1 via HC-030031 effectively alleviated IL-1β-induced chondrocyte inflammation and matrix degradation.In DMM model OA mice,microspheres showed good long-term sustained drug release properties,improved joint inflammation microenvironment,reduced articular cartilage damage and decreased mechanical nociceptive threshold.This research pioneers the creation of a drug delivery system tailored for delivery into the joint cavity,focusing on TRPA1 as a therapeutic target for osteoarthritis.Additionally,it offers a cutting-edge drug delivery platform aimed at addressing diseases linked to inflammation.
基金supported by the National Natural Science Foundation of China(Nos.21875044,21673048)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.17JC1400100)+2 种基金the support by the state key laboratory of Transducer Technology of China(No.SKT1904)Program of Shanghai Academic Research Leader(No.19XD1420300)Research Supporting Project(No.RSP-2019/155)by King Saud University。
文摘Incorporation of heteroatoms into the framewo rk of zeolites has become a significant strategy to improve their performance in catalysis and adsorption,because the obtained heteroatom zeolites exhibit quite different properties from the conventional aluminosilicate zeolites in aspects of surface acidity,pore structures,particle size and so on.In this review,the progress on the heteroatom zeolites including their synthesis and application is highlighted.First,the recent advance on the design and synthesis of different heteroatom zeolites is summarized.Special emphasis is placed on the introduction and comparison of three typical methods,including the direct synthesis,post synthesis and improved direct synthesis,for the traditional heteroatom zeolites(such as TS-1,Sn-MFI,Sn-β) and newly-reported heteroatom zeolites(such as W-MFI,Mo-MFI).According to their intrinsic characteristics,the application of heteroatom zeolites in diverse fields,such as production of fine chemicals,air pollution control and biomass conversion is then discussed.Finally,the challenges and perspective on the future development of heteroatom zeolites in low-cost preparation and practical application are proposed.
基金sponsored by Shanghai Pujiang Program, China (No. 16PJ1401100)the Shanghai Committee of Science and Technology, China (No.15ZR1402000)+3 种基金Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No. 17JC1400100)the NSF of China(No. 21673048)National Youth Top Talent Support Program of National High-Level Personnel of Special Support Program (Youth Top-notch Talent Support Program)the State Key Laboratory of Transducer Technology of China (No. SKT1503)
文摘A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and crystal sizes, respectively. The ultrafine Fe_2O_3 nanoparticles in size of 5 nm can be highly dispersed on zeolite Y matrix due to its much better wettability than ZSM-5 and mordenite. By using the obtained Fe_2O_3/zeolite composite as the heterogeneous Fenton-like catalysts, the degradation of phenol as a model reaction was systematically investigated, including the zeolite supports, particle size and dispersion of Fe_2O_3, and reaction conditions of H_2O_2 concentration, temperature, and pH value. The catalyst based on zeolite Y with Fe loading of 9% exhibited the best phenol degradation efficiency (> 90%)in neutral pH within 2 h. Its high catalytic activity in Fenton reaction can be attributed to the bifunctional properties of strong surface BrФnsted acidity and high reactivity of octahedral Fe^(3+) in the highlydispersed ultrafine Fe_2O_3 nanoparticles in size of 5 nm, which were the primary active centers to quickly decompose H_2O_2 into hydroxyl radicals. Since phenol degradation can be performed under mild conditions of ambient temperature (283-323 K) and a wide pH range (4.0-7.0), the catalysts can be easily recovered for recyclable use with stable degradation activity, which own the immense potential in deep treatment of organic pollutants in industrial wastewater.
基金supported by the National Natural Science Foundation of China(Nos.51822202 and 51772050)China Postdoctoral Science Foundation(No.2019M651342)+2 种基金Shanghai Rising-Star Program(No.18QA1400100)Youth Top-notch Talent Support Program of Shanghai,the Shanghai Committee of Science and Technology,China(No.19520713200)DHU Distinguished Young Professor Program and Fundamental Research Funds for the Central Universities。
文摘Mesoporous semiconducting metal oxides(SMOs)heterojunctions are appealing sensors for gas detecting.However,due to the different hydrolysis and condensation mechanism of every metal precursor and the contradiction between high crystallinity and high surface area,the synthesis of mesoporous SMOs heterojunctions with highly o rdered mesostructures,highly crystallized frameworks,and high surface area remains a huge challenge.In this work,we develop a novel"acid-base pair"adjusted solvent evaporation induced self-assembly(EISA)strategy to prepare highly crystallized ordered mesoporous TiO2/WO3(OM-TiO2/WO3)heterojunctions.The WCl6 and titanium isopropoxide(TIPO)are used as the precursors,respectively,which function as the"acid-base pair",enabling the coassembly with the structure directing agent(PEO-b-PS)into highly ordered meso structures.In addition,PEO-b-PS can be converted to rigid carbon which can protect the meso structures from collapse during the crystallization process.The resultant OM-TiO2/WO3 heterojunctions possess primitive cubic mesostructures,large pore size(~21.1 nm),highly crystalline frameworks and surface area(~98 m2/g).As a sensor for acetone,the obtained OM-TiO2/WO3 show excellent re sponse/recovery perfo rmance(3 s/5 s),good linear dependence,repeatability,selectivity,and long-term stability(35 days).
基金the financial support from the National Natural Science Foundation of China(Nos.51573030,51573028and 51773042)
文摘Lithium sulfur(Li-S) batteries are regarded as promising candidates for next-generation rechargeable batteries. However, the insulation characteristic of sulfur and severe polysulfide dissolution hindered their development. We presented a facile approach to fabricate Li-S batteries by coating commercial carbon nanotube or graphene slurries on normal sulfur cathode electrode to construct a dual-layer cathode electrode. The conductive CNT or graphene layer could not only improve the conductivity of sulfur cathode, but also suppress the polysulfide diffusion. The CNT@S cathode delivered a high reversible capacity of 740 mAh/g over 300 cycles at 1 C and 870 mAh/g over 100 cycles at 0.2 C. Furthermore, this strategy could be realized on the commercial product line of lithium-ion batteries, which made it possible to large-scale produce Li-S batteries.
基金financially supported by The Dow Chemical Company
文摘Photo-responsive azobenzene （ABZ） derivatives with different end groups （R） as photoswitchable molecules were employed to construct self-assembled monolayers （SAMs） on silicon substrate by using 3-glycidoxypropyltrimethoxysilane （GPTS） as the bridging molecules. The assembly process was optimized by changing various parameters, including the type and concentration of ABZ derivatives, reaction time, etc. The obtained SAMs were fully characterized and evaluated using UV spectroscopy, atomic force microscope （AFM）, elllipsometer, static contact angle and X-ray photoelectron spectroscopy （XPS）. It is found that the end group property of azobenzene derivatives is critical to the obtained SAMs＇ photoresponsive properties. Compared with hydrophobic compounds （4-（4＇-aminophenylazo） benzoic acid, ABZ-CF3）, the hydrophilic compounds （4-（4＇-aminophenylazo） benzoic acid, ABZ-COOH） show excellent reversible photoswitching performance with a large contact angle change of 35° under oDtimized process, and the SAMs are removable bv thermal treatment at 240 ℃ in air for onlv 5 min.
基金financially supported by the National Natural Science Foundation of China(Nos.21875044,52073064,22005058 and 22005057)National Key R&D Program of China(No.2020YFB2008600)+3 种基金Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.20JC1415300)Program of Shanghai Academic Research Leader(No.19XD1420300)China Post-doctoral Science Foundation(Nos.2020M670973,BX20200085)the State Key Laboratory of Transducer Technology of China(No.SKT1904)。
文摘Green and recyclable solid acid catalysts are in urgent demand as a substitute for conventional liquid mineral acids.In this work,a series of novel sulfonic acid-functionalized core-shell Fe_(3)O_(4)@carbon microspheres(Fe_(3)O_(4)@C-SO_(3)H)have been designed and synthesized as an efficient and recyclable heterogeneous acid catalyst.For the synthesis,core-shell Fe_(3)O_(4)@RF(resorcinol-formaldehyde)microspheres with tunable shell thickness were achieved by interfacial polymerization on magnetic Fe_(3)O_(4)microspheres.After high-temperature carbonization,the microspheres were eventually treated by surface sulfonation,re sulting in Fe_(3)O_(4)@C-x-SO_(3)H(x stands for carbonization temperature)microspheres with abundant surface SO_(3)H groups.The obtained microspheres possess uniform core-shell structure,partially-graphitized carbon skeletons,superparamagnetic property,high magnetization saturation value of 10.6 emu/g,and rich SO_(3)H groups.The surface acid amounts can be adju sted in the range of 0.59-1.04 mmol/g via sulfonation treatment of carbon shells with different graphitization degrees.The magnetic Fe_(3)O_(4)@C-x-SO_(3)H microspheres were utilized as a solid acid catalyst for the acetalization reaction between benzaldehyde and ethylene glycol,demonstrating high selectivity(97%)to benzaldehyde ethylene glycol acetal.More importantly,by applying an external magnetic field,the catalysts can be easily separated from the heterogeneous reaction solutions,which later show well preserved catalytic activity even after 9 cycles,revealing good recyclability and high stability.
基金supported by the National Natural Science Foundation of China(Nos.51372041,51422202, and 21673048)the "Shu Guang" Project(No. 13SG02)supported by Shanghai Municipal Education Commission and Shanghai Education Development Foundation+3 种基金the National Youth Top-notch Talent Support Program in China, China Postdoctoral Science Foundation(No. KLH1615138)Shanghai Nature Science Foundation of China(Nos. 14ZR1416600 and 15ZR1402000)Shanghai Pujiang Program, China(No.16PJ1401100)the International Scientific Partnership Program ISPP at King Saud University for funding this research work through ISPP# 0094
文摘Among various gas sensing materials, metal oxide semiconductors have shown great potential as resistive type sensors. The ordered porous structural metal oxide semiconductors with well-defined meso- or macro-pores chemically synthesized via soft-templating method and nanocasting strategy have high porosity, highly interconnected pore channels and high surface area with enormous active sites for interacting with gaseous molecules. These features enable them good performance in gas sensing, including high sensitivity, fast response and recovery, good selectivity. This review gives a comprehensive summary about the porous metal oxides with focus on the synthesis methods, structure related properties, as well as the modification strategies for gas sensing improved performances.
基金supported by the Shanghai Natural Science Foundation(No.21ZR1427500)the Agricultural Project of Shanghai Science and Technology Innovation Action Plan(No.19391901600).
文摘To achieve real-time monitoring of humidity in various applications,we prepared facile and ultra-thin CoAl layered double hydroxide(CoAl LDH)nanosheets to engineer quartz crystal microbalances(QCM).The characteristics of CoAl LDH were investigated by transmission electron microscopy(TEM),X-ray diffraction(XRD),X-ray photoelectric spectroscopy(XPS),Brunauer–Emmett–Telle(BET),atomic force microscopy(AFM)and zeta potential.Due to their large specific surface area and abundant hydroxyl groups,CoAl LDH nanosheets exhibit good humidity sensing performance.In a range of 11.3%and 97.6%relative humidity(RH),the sensor behaved an ultrahigh sensitivity(127.8 Hz/%RH),fast response(9.1 s)and recovery time(3.1 s),low hysteresis(3.1%RH),good linearity(R^(2)=0.9993),stability and selectivity.Besides,the sensor can recover the initial response frequency after being wetted by deionized water,revealing superior self-recovery ability under high humidity.Based on in-situ Fourier transform infrared spectroscopy(FT-IR),the adsorption mechanism of CoAl LDH toward water molecules was explored.The QCM sensor can distinguish different respiratory states of people and wetting degree of fingers,as well as monitor the humidity in vegetable packaging,suggesting excellent properties and a promising application in humidity sensing.
基金financially funded by the National Natural Science Foundation of China(No.31701678)the Key Project of Shanghai Agriculture Prosperity through Science and Technology(No.2019-02-08-00-15-F01147)+3 种基金the project of Shanghai Science and Technology Committee(No.19391901600)the Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.20JC1415300)the State Key Laborato ry of Transducer Technology of China(No.SKT1904)the Research Support Project number(No.RSP-2020/155),King Saud University,Riyadh,Saudi Arabia。
文摘Acephate pesticide contamination in agricultural production has caused serious human health problems.Metal oxide semiconductor(MOS)gas sensor can be used as a portable and promising alternative tool for efficiently detection of acephate.In this study,hierarchical assembled SnO_(2)nanosphere,SnO_(2)hollow nanosphere and SnO_2 nanoflower were synthesized respectively as high efficiency sensing materials to build rapid and selective acephate pesticide residues sensors.The morphologies of different SnO_(2)3 D nanostructures were characterized by various material characterization technology.The sensitive performance test results of the 3 D SnO_(2)nanomaterials towards acephate show that hollow nanosphere SnO_(2)based sensor displayed preferable sensitivity,selectivity,and rapid response(9 s)properties toward acephate at the optimal working temperature(300℃).This SnO_(2)hollow nanosphere based gas sensor represents a useful tool for simple and highly effective monitoring of acephate pesticide residues in food and environment.According to the characterization results,particularly Brunauer-Emmett-Teller(BET)and Ultraviolet-Visible Spectroscopy(UV-vis),the obvious and fast response can be attributed to the mesoporous hollow nanosphere structure and appropriate band gap of SnO_2 hollow nanosphere.
基金supported by the National Natural Science Foundation of China(Nos.51372041,51422202,21673048,21875044,51822202 and 51772050)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.17JC1400100)+1 种基金Youth Top-notch Talent Support Program of China,Shanghai Rising-Star Program(No.18QA1400100)DHU Distinguished Young Professor Program。
文摘Solid photocatalysts with high specific surface area,superior photoactivity and ease of recycling are highly desired in chemical process,water treatment and so on.In this study,a facile stepwise sol-gel coating approach was utilized to synthesize Pt decorated oxygen-deficient mesoporous titania microspheres with core-shell structure and convenient magnetic separability(denoted as Fe3 O4@-SiO2@Pt/mTiO2-x).These photocatalysts consist of magnetic Fe3 O4 cores,nonporous insulating SiO2 middle layer and mesoporous anatase TiO2-x shell decorated by Pt nanoparticles(~3.5 nm)through wet impregnation and H2 reduction.As a result of high activity of oxygen-deficiency of black TiO2-x by H2 reduction and efficient inhibition of electron-hole recombination by Pt nanoparticles,the rationally designed core-shell Fe3 O4@SiO2@Pt/mTiO2-x photocatalysts exhibit superior photocatalytic performance in rhodamine B(RhB)degradation under visible light irradiation,with more than 98%of RhB degraded within 50 min.These core-shell structured photocatalysts show excellent recyclability under the assistance of magnetic separation with well-retained photocatalytic performance even after running five cycles.This stepwise synthesis method paves the way for the rational design of a high-efficiency recyclable heterogeneous catalyst,including photocatalysts,for various applications.
基金financial support from the National Natural Science Foundation of China (NSFC,Nos.21872038 and 21733003)MOST (No.2017YFA0207303)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No.17JC1400100)
文摘Highly luminescent colloidal nanocrystals have wide applications in bioimaging and various optoelectronic devices.Herein we report a facile and mild procedure by combining S2-treatment and binary ligand passivation,which can efficiently enhance the luminescent property of CdSe nanocrystals at room temperature.The photoluminescence quantum yield of as-treated CdSe nanocrystals exhibits drastic enhancement(e.g.,188 times for CdSe nanorods)after this dual-passivation treatment.The methodology proposed here can be applied to various CdSe nanocrystals,regardless of their sizes,shapes,and crystal structures.
基金financially supported by the National Natural Science Foundation of China(Nos.21673048,21875044,52073064,22005058 and 22005057)National Key R&D Program of China(No.2018YFA0209401)+3 种基金Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.20JC1415300)Program of Shanghai Academic Research Leader(No.19XD1420300)the state key laboratory of Transducer Technology of China(No.SKT1904)supporting project number(No.RSP-2020/155)。
文摘The rapid development of internet and internet of things brings new opportunities for the expansion of intelligent sensors,and acetone as a major disease detection indicator(i.e.,diabetes)making it become extremely important clinical indicator.Herein,uniform mesoporous ZnO spheres were successfully synthesized via novel formaldehyde-assisted metal-ligand crosslinking strategy.In order to adjust the pore structure of mesoporous ZnO,various mesoporous ZnO spheres were synthesized by changing weight percentage of Zn(NO_(3))_(2)·6 H_(2)O to tannic acid(TA).Moreover,highly active heterojunction mesoporous ZnO/Co_(3)O_(4)has been fabricated based on as-prepared ultra-small Co_(3)O_(4)nanocrystals(ca.3 nm)and mesoporous ZnO spheres by flexible impregnation technique.Profit from nano-size effect and synergistic effect of p-n heterojunction,mesoporous ZnO/Co_(3)O_(4)exhibited excellent acetone sensing performance with high selectivity,superior sensitivity and responsiveness.Typically,5 wt%Co_(3)O_(4)embedded mesoporous ZnO sphere showed prominent acetone response(ca.46 for 50 ppm),which was about 11.5 times higher than that in pure ZnO sensing device,and it was also endowed high cyclic stability.The nanocrystals embedded hybrid material is expected to be used as promising efficient material in the field of catalysis and gas sensing.
基金financially supported by the National Natural Science Foundation of China (No. 62071300)Science and Technology Commission of Shanghai Municipality (Nos. YDZX20213100003002, 19ZR1435200, 20490761100)+3 种基金Innovation Program of Shanghai Municipal Education Commission (No. 201901-07-00-07-E00015)Program of Shanghai Academic/Technology Research Leader (No. 19XD1422900)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No. 20JC1415300)Foshan Science and Technology Innovation Program (No. 2017IT 100121)。
文摘The freshness of seafood can be judged by detecting the concentration of triethylamine(TEA). In this work, 2D Cu O porous nanosheets(Cu O PNs) were prepared by a graphene oxide template method and their particle sizes were regulated by changing the calcination temperature. Their structure, morphology and gas sensing performances were investigated by various characterization methods. The response(Rg/Ra) of the gas sensor based on Cu O PNs calcined at 700oC was as high as 440-100 ppm TEA at the operating temperature of 40 ℃. The detection limit was as low as 0.25 ppm. In addition, the gas sensor has good selectivity and stability. The excellent TEA sensitivity is mainly resulted from the appropriate particle size and loose porous framework. This work not only paves the way to explore the novel low temperature TEA gas sensors, but also provides deep insight on improving the structure and properties of gas sensitive materials by controlling the calcination temperature.
基金supported by the National Natural Science Foundation of China(Nos.52006032,22001009)the Natural Science Foundation of Anhui Province(No.2008085QB60)。
文摘Most catalytic processes are achieved by heating the whole reaction systems including the entire reactor,substrate and solvent,which leads to energy loss and obvious heat transfer limits.In this study,induction heating was employed to boost the catalytic Suzuki-Miyaura cross-coupling reactions by using conductive superparamagnetic microspheres with loaded Pd nanoparticles as heterogeneous catalysts.It was found that,at the same apparent reaction temperatures,the reactions by adopting the induction heating all exhibit better catalytic performance with higher conversion and yield,as compared to the reactions using conventional joule heating.The improvement is mainly attributed to the localized heating effect endowed by high efficiency of the heat transfer from the heat source to catalytic sites,which dissipates the electromagnetic energy through Néel relaxation mechanism.Moreover,it has be found that the reactions have been largely accelerated,resulting in much shorter reaction time required to approach a given value of reactant conversion.These results indicate that the unique heating method based on the superparamagnetic nanomaterials as both the inductive component and catalyst support holds a promising application for fast and efficient heterogeneous catalytic process,and exhibits potential for improving energy transfer efficiency and reducing the side reactions attributed to the uneven temperature profile.
基金financially supported by the National Natural Science Foundation of China (Nos.21701130 and 311343)the Fundamental Research Funds for the Central Universities+1 种基金“Young Talent Support Plan” of Xi’an Jiaotong UniversityResearch Supporting Project number (No.RSP-2019/155),King Saud University, Riyadh,Saudi Arabia。
文摘Plant polyphenol-based coordination polymers(CPs) with ultra-small particle size and tailorable compositions are highly desired in biomedical applicatio ns,but their synthesis is still challenging due to the sophisticated coordination assembly process and unavoidable self-oxidation polymerization of polyphenol. He rein,a general ligand covalent-modification mediated coordination assembly strategy is proposed for the synthesis of water-dispersible CPs with tunable metal species(e.g., Gd,Cu,Ni,Zn,Fe)and ultra-small diameter(8.6-37.8 nm) using nontoxic plant polyphenol(e.g..tannic acid,gallic acid) as a polymerizable ligand.Polyphenol molecules react with formaldehyde firstly,which can effectively retard the oxidation induced self-polymerization of polyphenol and lead to the formation of metal ions containing CPs colloidal nanoparticles.These ultrafine nanoparticles with stably chelated metal io ns are highly water dispersible and thus advantageous for bioimaging.As an example,ultra-small Gd contained CPs exhibit higher longitudinal relaxivity(r_(1)=25.5 L mmol^(-1) s^(-1)) value with low r2/r1(1.19) than clinically used Magnevist(Gd-DTPA,r1=3.7 L mmol^(-1) s^(-1)) .Due to the enhanced permeability and retention effect,they can be further used as a positive contrast agent for T1-weighted MR imaging of tumour.
基金financially supported by the National Key Research and Development Program(No.2022YFE0100400)National Natural Science Foundation of China(No.21701130)+2 种基金Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.20JC1415300)State Key Laboratory of Transducer Technology of China(No.SKT2207)Key Research and Development Program of Shaanxi(No.2021GY-225)。
文摘In persulfate-based advanced oxidation process(PS-AOPs),fixing nanosized metal oxide on processable substrates is highly desirable to avoid the aggregation and loss of nanocatalysts during the practical application.However,it is still challenging to develop a versatile strategy for the deposition of metal oxide nanocatalysts on various substrates with different physicochemical properties.Herein,polyphenols are utilized as a“molecular glue”and reductant to mediate the interfacial deposition of MnO_(2) nanocatalysts on different substrates.MnO_(2) nanocatalysts were in-situ grown on macroscope mineral substrates(e.g.,airstone)via an interfacial redox strategy between tannic acid(TA)and oxidized KMnO4,and then employed as a fixed catalyst of peroxymonosulfate(PMS)activation for treating pharmaceutical and personal care products(PPCPs)in water.The fixed MnO_(2) exhibited superior catalytic performance toward different PPCPS via a singlet oxygen(^(1)O_(2))-dominated nonradical oxidation pathway.PPCPs in the secondary effluent of wastewater treatment plants could be effectively removed by a fixed-bed column of the fixed MnO_(2) with long term stability.Redox cycle of Mn^(4+)/Mn^(3+)and surface hydroxyl group of the fixed MnO_(2) was proved to be responsible for the activation of PMS.This work provides a new avenue for developing fixed metal oxides for sustainable water treatment.
基金supported by the National Natural Science Foundation of China(Nos.22125501,U22A20152,22105043,52225204,52173233)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality(No.20JC1415300)+1 种基金the state key laboratory of Transducer Technology of China(No.SKT2207)the Fundamental Research Funds for the Central Universities(No.20720220010)。
文摘Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment,and thus it is distinctly meaningful to monitor benzene series with quickly,real-time and efficient technique.Herein,novel sulfur-doped mesoporous WO_(3)materials were synthesized via classical in-situ solvent evaporation induced co-assembly strategy combined with doping engineering,which possessed highly crystallized frameworks,high specific surface area(40.9–63.8 m^(2)/g)and uniform pore size(~18 nm).Benefitting from abundant oxygen vacancy and defects via S-doping,the tailored mesoporous S/m WO_(3)exhibited excellent benzene sensing performance,including high sensitivity(50 ppm vs.48),low detection limit(ca.500 ppb),outstanding selectivity and favorable stability.In addition,the reduction of band gap resulted from S-doping promotes the carrier migration in the sensing materials and the reaction at the gas–solid sensing interfaces.It provides brand-new approach to design sensitive materials with multiple reaction sites.
基金financially supported by National Natural Science Foundation of China(Nos.62104045,22125501,U22A20152)State Key Laboratory of Transducer Technology of China(No.SKT2207)+1 种基金Medical Engineering Jiont Fund of Fudan University(No.yg2023-10)Fundamental Research Funds for the Central Universities(No.20720220010)。
文摘As a key biomarker for noninvasive diagnosis of diabetes,the selective detection of trace acetone in exhaled gas using a portable and low-cost device remains a great challenge.Semiconductor metal oxide(SMO)based gas sensors have drawn signification attention due to their potential in miniaturization,user-friendliness,high cost-effectiveness and selective real-time detection for noninvasive clinical diagnosis.Herein,we propose a one-pot solvent evaporation induced tricomponent co-assembly strategy to design a novel ordered mesoporous SMO of silica-implanted WO_(3)(Si O_(2)/WO_(3))as sensing materials for trace acetone detection.The controlled co-assembly of silicon and tungsten precursors and amphiphilic diblock copolymer poly(ethylene oxide)-block-polystyrene(PEO-b-PS),and the subsequent thermal treatment enable the local lattice disorder of WO_(3)induced by the amorphous silica and the formation of ordered mesoporous Si O_(2)/WO_(3)hybrid walls with a unique metastableε-phase WO_(3)framework.The obtained mesoporous SiO_(2)/WO_(3)composites possess highly crystalline framework with large uniform pore size(12.0-13.3 nm),high surface area(99-113 m^(2)/g)and pore volume(0.17-0.23 cm^(3)/g).Typically,the asfabricated gas sensor based on mesoporous 2.5%Si O_(2)/WO_(3)exhibits rapid response/recovery rate(5/17 s),superior sensitivity(R_(air)/R_(gas)=105 for 50 ppm acetone),as well as high selectivity towards acetone.The limit of detection is as low as 0.25 ppm,which is considerably lower than the thresh value of acetone concentration(>1.1 ppm)in the exhaled breath of diabetic patients,demonstrating its great prospect in real-time monitoring in diabetes diagnosis.Moreover,the mesoporous 2.5%Si O_(2)/WO_(3)sensor is integrated into a wireless sensing module connected to a smart phone,providing a convenient real-time detection of acetone.
基金supported by the NSF of China(Nos.51372041, 51422202,21673048,21875044,51822202 and 51772050)Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No.17JC1400100)+4 种基金Youth Top-notch Talent Support Program of ChinaShanghai Rising-Star Program(No. 18QA1400100)Youth Top-notch Talent Support Program of ShanghaiDHU distinguished Young Professor Programthe Fundamental Research Funds for the Central Universities
文摘Mesoporous late-transition metal oxides have great potential in applications of energy,catalysis and chemical sensing due to their unique physical and chemical properties.However,their synthesis via the flexible and scalable soft-template method remain a great challenge,due to the weak organic-inorganic interaction between the frequently used surfactants(e.g.,Pluronic-type block copolymers) and metal oxide precursors,and the low crystallization temperature of metal oxides.In this study,ordered mesoporous NiO with dual mesopores,high surface area and well-interconnected crystalline porous frameworks have been successfully synthesized via the facile solvent evaporation-induced co-assembly(EICA) method,by using lab-made amphiphilic diblock copolymer polystyrene-b-poly(4-vinylpyridine)(PS-b-P4 VP) as both the structure-directing agent(the soft template) and macromolecular chelating agents for nickel species,THF as the solvent,and nickel acetylacetonate(Ni(acac)2) as inorganic precursor.Similarly,by using Ni(acac)2 and Fe(acac)3 as the binary precursors,ordered mesoporous Fedoped NiO materials can be obtained,which have bimodal mesopores of large mesopores(32.5 nm) and secondary mesopores(4.0-11.5 nm) in the nanocrystal-assembled walls,high specific surface areas(~74.8 m^2/g) and large pore value(~0.167 cm^3/g).The obtained mesoporous Fe-doped NiO based gas sensor showed superior ethanol sensing performances with good sensitivity,high selectivity and fast response-recovery dynamics.
