Mesoporous silica materials with high pore volume were successfully prepared by the chemical precipitation method, with water glass and a biodegradable nonionic surfactant polyethylene glycol (PEG). The obtained mat...Mesoporous silica materials with high pore volume were successfully prepared by the chemical precipitation method, with water glass and a biodegradable nonionic surfactant polyethylene glycol (PEG). The obtained materials were characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), thermo gravimetric analyzer and differential scanning calorimetry (TG-DSC), nitrogen adsorption-desorption measurements, and X-ray diffraction (XRD). The results showed that the changes of the pore parameters depended on both the surfactant content and heat treatment temperature. When the content of PEG was 10wt% and the obtained PEG/SiO2 composite was heated at 600℃, the mesoporous silica with a pore volume of 2.2 cma/g, a BET specific surface area of 361.55 m^2/g, and a diameter of 2-4 μm could be obtained. The obtained mesoporous silica materials have potential applications in the fields of paint and plastic, as thickening, reinforcing, and flatting agents.展开更多
Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the c...Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the charge and discharge process(“shuttle effect”)results in fast capacity fading and inferior electrochemical performance.In this study,Mn_(2)O_(3)with an ordered mesoporous structure(OM-Mn_(2)O_(3))was designed as a cathode host for LSBs via KIT-6 hard templating,to effectively inhibit the polysulfide shuttle effect.OM-Mn_(2)O_(3)offers numerous pores to confine sulfur and tightly anchor the dissolved polysulfides through the combined effects of strong polar-polar interactions,polysulfides,and sulfur chain catenation.The OM-Mn_(2)O_(3)/S composite electrode delivered a discharge capacity of 561 mAh g^(-1) after 250 cycles at 0.5 C owing to the excellent performance of OM-Mn_(2)O_(3).Furthermore,it retained a discharge capacity of 628mA h g^(-1) even at a rate of 2 C,which was significantly higher than that of a pristine sulfur electrode(206mA h g^(-1)).These findings provide a prospective strategy for designing cathode materials for high-performance LSBs.展开更多
The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,th...The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.展开更多
To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environment...To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.展开更多
A novel tetraethylenepentamine(TEPA) functionalized magnetic mesoporous silica adsorbent(FNMs/TEPA) was prepared for the adsorption of Cr(Ⅲ)-ethylenediaminetetraacetic acid(EDTA)from wastewater. The characterization ...A novel tetraethylenepentamine(TEPA) functionalized magnetic mesoporous silica adsorbent(FNMs/TEPA) was prepared for the adsorption of Cr(Ⅲ)-ethylenediaminetetraacetic acid(EDTA)from wastewater. The characterization of the prepared adsorbent certified that TEPA was modified onto the magnetic mesoporous silicon(FNMs), while FNMs/TEPA maintained the ordered mesoporous and pristine magnetic properties. The batch adsorption experiments demonstrated that TEPA significantly enhanced the removal capacity of the adsorbent for Cr(Ⅲ)-EDTA. FNMs/TEPA exhibited an excellent adsorption property(13.84 mg·g-1) at p H 4.0. Even in the presence of high concentrations of coexisting ions and organic acids, the adsorption performance of FNMs/TEPA was stable. Experimental characterization and DFT demonstrated that the adsorption of Cr(Ⅲ)-EDTA was ascribed to the electrostatic interaction, hydrogen bonding, and complexation between Cr(Ⅲ)-EDTA and amino groups on the adsorbent surface. The analysis of the independent gradient model(IGM) shows that electrostatic interaction is the main mode of action in the adsorption process. Moreover, FNMs/TEPA demonstrated remarkable reusability in three regeneration cycles. These findings indicated that FNMs/TEPA possessed excellent application prospects in the disposal of wastewater containing Cr(Ⅲ)-EDTA.展开更多
Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challen...Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.展开更多
To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li me...To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li metal has low transport kinetics and is easy to causes the growth of lithium dendrites and accumulation of dead Li,which seriously affects the cycle life of batteries and even causes safety problems.Here,by comparing graphite with two types of hard carbon,it was found that hybrid anode formed by hard carbon and lithium metal,possessing more disordered mesoporous structure and lithophilic groups,presents better performance.Results indicate that the mesoporous structure provides abundant active site and storage space for dead lithium.With the synergistic effect of this structure and lithophilic functional groups(–COOH),the reversibility of hard carbon/lithium metal hybrid anode is maintained,promoting uniform deposition of lithium metal and alleviating formation of lithium dendrites.The hybrid anode maintains a 99.5%Coulombic efficiency(CE)after 260 cycles at a specific capacity of 500 m Ah/g.This work provides new insights into the hybrid anodes formed by carbon-based materials and lithium metal with high specific energy and fast charging ability.展开更多
Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile...Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.展开更多
Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially acces...Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar guest species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.展开更多
Due to their low cost,environmental friendliness and high energy density,the lithium-sulfur batteries(LSB)have been regarded as a promising alternative for the next generation of rechargeable battery systems.However,t...Due to their low cost,environmental friendliness and high energy density,the lithium-sulfur batteries(LSB)have been regarded as a promising alternative for the next generation of rechargeable battery systems.However,the practical application of LSB is seriously hampered by its short cycle life and high self-charge owing to the apparent shuttle effect of soluble lithium polysulfides.Using MgSO_(4)@MgO composite as both template and dopant,template-guided S-doped mesoporous graphene(SMG)is prepared via the fluidized-bed chemical vapor deposition method.As the polypropylene(PP)modifier,SMG with high specific surface area,abundant mesoporous structures and moderate S doping content offers a wealth of physical and chemical adsorptive sites and reduced interfacial contact resistance,thereby restraining the serious shuttle effects of lithium polysulfides.Consequently,the LSB configured with mesoporous graphene(MG)as S host material and SMG as a separator modifier exhibits an enhanced electrochemical performance with a high average capacity of 955.64 mA h g^(-1) at 1C and a small capacity decay rate of 0.109%per cycle.Additionally,the density functional theory(DFT)calculation models have been rationally constructed and demonstrated that the doped S atoms in SMG possess higher binding energy to lithium polysulfides than that in MG,indicating that the SMG/PP separator can effectively capture soluble lithium polysulfides via chemical binding forces.This work would provide valuable insight into developing a versatile carbon-based separator modifier for LSB.展开更多
Highly dispersed bimetallic alloy nanoparticle electrocatalysts have been demonstrated to exhibit exceptional performance in driving the nitrate reduction reaction(NO_(3)RR)to generate ammonia(NH_(3)).In this study,we...Highly dispersed bimetallic alloy nanoparticle electrocatalysts have been demonstrated to exhibit exceptional performance in driving the nitrate reduction reaction(NO_(3)RR)to generate ammonia(NH_(3)).In this study,we prepared mesoporous carbon nanofibers(mCNFs)functionalized with ordered PtFe alloys(O-PtFe-mCNFs)by a composite micelle interface-induced co-assembly method using poly(ethylene oxide)-block-polystyrene(PEO-b-PS)as a template.When employed as electrocatalysts,O-PtFe-mCNFs exhibited superior electrocatalytic performance for the NO_(3RR)compared to the mCNFs functionalized with disordered PtFe alloys(D-PtFe-mCNFs).Notably,the NH_(3)production performance was particularly outstanding,with a maximum NH_(3)yield of up to 959.6μmol/(h·cm~2).Furthermore,the Faraday efficiency(FE)was even 88.0%at-0.4 V vs.reversible hydrogen electrode(RHE).This finding provides compelling evidence of the potential of ordered PtFe alloy catalysts for the electrocatalytic NO_(3)RR.展开更多
Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the ...Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the mesoporous characteristics of the template,with cubic symmetry(ia3d).It consists of a β-MnO2 crystalline phase corresponding to pyrolusite,with a rutile structure.Transmission electron microscopy and X-ray photoelectron spectroscopy showed that the 3D-MnO2 catalyst has a large number of exposed Mn4+ ions on the(110)crystal plane surfaces,with a lattice spacing of 0.311 nm; this enhances oxidation of HCHO.Complete conversion of HCHO to CO2 and H2O was achieved at 130 °C on 3D-MnO2; the same conversions on α-MnO2 and β-MnO2 nanorods were obtained at 140 and 180 °C,respectively,under the same conditions.The specific mesoporous structure,high specific surface area,and large number of surface Mn4+ ions are responsible for the catalytic activity of 3D-MnO2 in HCHO oxidation.展开更多
A series of functional,tungsten-containing mesoporous silica materials(W-SiO2) have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and m...A series of functional,tungsten-containing mesoporous silica materials(W-SiO2) have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and metal source respectively.These materials were then characterized through X-ray diffraction(XRD),transmission electron microscopy(TEM),Raman spectroscopy,Fourier transform infrared spectra(FTIR),diffuse reflectance spectra(DRS),and N2 adsorption-desorption,which were found to contain tungsten species that were effectively dispersed throughout the structure.The as-prepared materials W-SiO2 were also found to possess a mesoporous structure.The pore diameters of the respective sample W-SiO2-20 determined from the TEM images ranged from 2 to 4 nm,which was close to the average pore size determined from the nitrogen desorption isotherm(2.9 nm).The materials were evaluated as catalysts for the heterogeneous oxidative desulfurization of dibenzothiophene(DBT),which is able to achieve deep desulfurization within 40 min under the optimal conditions(Catalyst(W-SiO2-20)= 0.01 g,temperature = 60℃,oxidant(H2O2)= 20 μL).For the removal of different organic sulfur compounds within oil,the ability of the catalyst(W-SiO2-20) under the same conditions to remove sulfur compounds decreased in the order:4,6-dimethyldibenzothiophene Dibenzothiophene Benzothiophene 1-dodecanethiol.Additionally,they did not require organic solvents as an extractant in the heterogeneous oxidative desulfurization process.After seven separate catalytic cycles,the desulfurization efficiency was still as high as 90.3%.From the gas chromatography-mass spectrometer analysis,DBT was entirely oxidized to its corresponding sulfone DBTO2 after reaction.A mechanism for the heterogeneous desulfurization reaction was proposed.展开更多
The mesoporous hydroxyapatite (HA) was synthesized by hydrothermal method utilizing cationic surfactant cetyltrimethylammonium bromide (CTAB) as template. The crystalline phase, morphology and porous structure wer...The mesoporous hydroxyapatite (HA) was synthesized by hydrothermal method utilizing cationic surfactant cetyltrimethylammonium bromide (CTAB) as template. The crystalline phase, morphology and porous structure were characterized respectively by different detecting techniques. The results reveal that the particles are highly crystalline hydroxyapatite phase. The surfactant has little influence on the morphology of the crystals, but affects the porous structure obviously. The sample without CTAB has a low surface area not exceeding 33 m^2/g, and no distinct pores can be observed by TEM. While the samples obtained with the surfactant get better parameters. Numerous open-ended pores centered at 2-7 nm spread unequally on the surface of the hydroxyapatite nanorods. The N2 adsorption-desorption experiments show type IV isotherms with distinct hysteresis loops, illustrating the presence of mesoporous structure. When the mole ratio of CTAB to HA is 1:2, the sample has the largest surface area of 97.1 m^2/g and pore volume of 0.466 cm^3/g.展开更多
In this article, we report the preparation of a three-dimensional(3D) interconnected mesoporous anatase TiO2-SiO2 nanocomposite. The nanocomposite was obtained by using an ordered two-dimensional(2D) hexagonal mes...In this article, we report the preparation of a three-dimensional(3D) interconnected mesoporous anatase TiO2-SiO2 nanocomposite. The nanocomposite was obtained by using an ordered two-dimensional(2D) hexagonal mesoporous anatase 70 TiO2-30 SiO2-950 nanocomposite(crystallized at 950 °C for 2 h) as a precursor, NaO H as an etchant of SiO2 via a "creating mesopores in the pore walls" approach. Our strategy adopts mild conditions of creating pores such as diluted NaO H solution, appropriate temperature and solid/liquid ratio, etc. aiming at ensuring the integrities of mesopores architecture and anatase nanocrystals. XRD, TEM and N2 sorption techniques have been used to systematically investigate the physico-chemical properties of the nanocomposites. The results show that the intrawall mesopores are highly dense and uniform(average pore size 3.6 nm), and highly link the initial mesochannels in a 3D manner while retaining mesostructural integrity. There is no significant change to either crystallinity or size of the anatase nanocrystals before and after creating the intrawall mesopores. The photocatalytic degradation rates of rhodamine B(RhB, 0.303 min^–1) and methylene blue(MB, 0.757 min^–1) dyes on the resultant nanocomposite are very high, which are 5.1 and 5.3 times that of the precursor; even up to 16.5 and 24.1 times that of Degussa P25 photocatalyst, respectively. These results clearly demonstrate that the 3D interconnected mesopores structure plays an overwhelming role to the increments of activities. The 3D mesoporous anatase TiO2-SiO2 nanocomposite exhibits unexpected-high degradation activities to RhB and MB in the mesoporous metal oxide-based materials reported so far. Additionally, the nanocomposite is considerably stable and reusable. We believe that this method would pave the way for the preparation of other 3D highly interconnected mesoporous metal oxide-based materials with ultra-high performance.展开更多
Mesoporous CeO2 with high specific surface area was synthesized using a modified evaporation-induced self-assembly (EISA) method, and a series of different amounts of Ag were loaded to this mesoporous CeO2 by a modi...Mesoporous CeO2 with high specific surface area was synthesized using a modified evaporation-induced self-assembly (EISA) method, and a series of different amounts of Ag were loaded to this mesoporous CeO2 by a modified ethylene glycol reduction route. The samples were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), energy-dispersive spectrometry (EDS), nitrogen adsorption-desorption, Brunauer-Emmett-Teller (BET) and Barrett-Joyner- Halenda (BJH) methods. The mesoporous CeO2 structure with different proportions of silver nanoparticles and its antibacterial activity were adequately studied, confinnin~ that obtained novel materials show a good antibacterial effect.展开更多
The heterogeneously copper-catalyzed oxidative cleavage of styrene was studied using copper-doped mesoporous KIT-6(CU-KIT-6_x) prepared via pH adjustment(where x is the pH:1.43,2.27,3.78,3.97,4.24 or 6.62).Variat...The heterogeneously copper-catalyzed oxidative cleavage of styrene was studied using copper-doped mesoporous KIT-6(CU-KIT-6_x) prepared via pH adjustment(where x is the pH:1.43,2.27,3.78,3.97,4.24 or 6.62).Variations in the catalyst structure and morphology with pH values were characterized by X-ray power diffraction,nitrogen adsorption-desorption analysis,transmission electron microscopy and X-ray photoelectron spectroscopy.As the pH value applied during the initial synthesis,the resulting Cu-KIT-6_x exhibited different structural,textural and surface characteristics,especially in terms of specific copper species and copper content At a pH value of 3.78,approximately 4.6 wt%copper(Ⅱ) was successfully incorporated into the framework of the initial KIT-6,in the form of-Cu-O-Si- groups.The catalytic performance of each catalyst was evaluated by following the epoxidation of styrene,employing tert-butyl hydroperoxide as the oxidant and CH_3CN as the solvent.A significant styrene conversion of 43.5%with 86.6%selectivity for the desired styrene epoxide was obtained over the Cu-KIT-63.78.A higher Cu content,an ordered cubic laid mesoporous architecture and various specific textural characteristics all combined to endow the Cu-KIT-63.78 with high catalytic activity and good stability.展开更多
Due to the advantages of high surface areas, large pore volumes and pore sizes, abundant nitrogen content that favored the metal-support interactions, N-doped ordered mesoporous carbons are regarded as a kind ...Due to the advantages of high surface areas, large pore volumes and pore sizes, abundant nitrogen content that favored the metal-support interactions, N-doped ordered mesoporous carbons are regarded as a kind of fascinating and potential support for the synthesis of effective supported cat-alysts. Here, a N-doped ordered mesoporous carbon with a high N content (9.58 wt%), high surface area (417 m^2/g), and three-dimensional cubic structure was synthesized successfully and used as an effective support for immobilizing Pt nanoparticles (NPs). The positive effects of nitrogen on the metal particle size enabled ultrasmall Pt NPs (about 1.0 ± 0.5 nm) to be obtained. Moreover, most of the Pt NPs are homogeneously dispersed in the mesoporous channels. However, using the ordered mesoporous carbon without nitrogen as support, the particles were larger (4.4 ± 1.7 nm) and many Pt NPs were distributed on the external surface, demonstrating the important role of the nitrogen species. The obtained N-doped ordered mesoporous material supported catalyst showed excellent catalytic activity (conversion 100%) and selectivity (〉99%) in the hydrogenation of halogenated nitrobenzenes under mild conditions. These values are much higher than those achieved using a commercial Pt/C catalyst (conversion 89% and selectivity 90%). This outstanding catalytic perfor-mance can be attributed to the synergetic effects of the mesoporous structure, N-functionalized support, and stabilized ultrasmall Pt NPs. Moreover, such supported catalyst also showed excellent catalytic performance in the hydrogenation of other halogenated nitrobenzenes and nitroarenes. In addition, the stability of the multifunctional catalyst was excellent and it could be reused more than 10 times without significant losses of activity and selectivity. Our results conclusively show that a N-doped carbon support enable the formation of ultrafine metal NPs and improve the reaction ac-tivity and selectivity.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
Li3V2(PO4)3 precursor was obtained with V2Os.nH2O , LiOH'H2O, NH4H2PO4 and sucrose as starting materials by grinding-sol-gel method, and then the monoclinic-typed Li3Vz(PO4)3 cathode material was prepared by sint...Li3V2(PO4)3 precursor was obtained with V2Os.nH2O , LiOH'H2O, NH4H2PO4 and sucrose as starting materials by grinding-sol-gel method, and then the monoclinic-typed Li3Vz(PO4)3 cathode material was prepared by sintering the amorphous Li3V2(PO4)3. The as-sintered samples were investigated by X-ray diffraction (XRD), transmission electron microscopy (TEM), N2 adsorption-desorption and electrochemical measurement. It is found that Li3Vz(PO4)3 sintered at 700 ℃ possesses good wormhole-like mesoporous structure with the largest specific surface area of 188 cmZ/g, and the smallest pore size of 9.3 nm. Electrochemical test reveals that the initial discharge capacity of the 700 ℃ sintered sample is 155.9 mA.h/g at the rate of 0.2C, and the capacity retains 154 mA.h/g after 50 cycles, exhibiting a stable discharge capacity at room temperature.展开更多
基金the National Natural Science Foundation of China (No.20671010, 20236020, 20325621, 50642042).
文摘Mesoporous silica materials with high pore volume were successfully prepared by the chemical precipitation method, with water glass and a biodegradable nonionic surfactant polyethylene glycol (PEG). The obtained materials were characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), thermo gravimetric analyzer and differential scanning calorimetry (TG-DSC), nitrogen adsorption-desorption measurements, and X-ray diffraction (XRD). The results showed that the changes of the pore parameters depended on both the surfactant content and heat treatment temperature. When the content of PEG was 10wt% and the obtained PEG/SiO2 composite was heated at 600℃, the mesoporous silica with a pore volume of 2.2 cma/g, a BET specific surface area of 361.55 m^2/g, and a diameter of 2-4 μm could be obtained. The obtained mesoporous silica materials have potential applications in the fields of paint and plastic, as thickening, reinforcing, and flatting agents.
基金Ministry of Trade,Industry and Energy,Grant/Award Number:20010095Korea Evaluation Institute of Industrial Technology,Grant/Award Number:20012341。
文摘Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the charge and discharge process(“shuttle effect”)results in fast capacity fading and inferior electrochemical performance.In this study,Mn_(2)O_(3)with an ordered mesoporous structure(OM-Mn_(2)O_(3))was designed as a cathode host for LSBs via KIT-6 hard templating,to effectively inhibit the polysulfide shuttle effect.OM-Mn_(2)O_(3)offers numerous pores to confine sulfur and tightly anchor the dissolved polysulfides through the combined effects of strong polar-polar interactions,polysulfides,and sulfur chain catenation.The OM-Mn_(2)O_(3)/S composite electrode delivered a discharge capacity of 561 mAh g^(-1) after 250 cycles at 0.5 C owing to the excellent performance of OM-Mn_(2)O_(3).Furthermore,it retained a discharge capacity of 628mA h g^(-1) even at a rate of 2 C,which was significantly higher than that of a pristine sulfur electrode(206mA h g^(-1)).These findings provide a prospective strategy for designing cathode materials for high-performance LSBs.
基金gratefully acknowledge the financial support of the National Natural Science Foundation of China(22108145 and 21978143)the Shandong Province Natural Science Foundation(ZR2020QB189)+1 种基金State Key Laboratory of Heavy Oil Processing(SKLHOP202203008)the Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering(STHGYX2201).
文摘The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.
基金supported by the National Natural Science Foundation of China(52370041)National Natural Science Foundation of China(21976134 and 21707104)State Key Laboratory of Pollution treatment and Resource Reuse Foundation(NO.PCRRK21001).
文摘To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.
基金supported by the National Natural Science Foundation of China(22076111)Key Research and Development Program of Shaanxi(2024GX-YBXM-427),China.
文摘A novel tetraethylenepentamine(TEPA) functionalized magnetic mesoporous silica adsorbent(FNMs/TEPA) was prepared for the adsorption of Cr(Ⅲ)-ethylenediaminetetraacetic acid(EDTA)from wastewater. The characterization of the prepared adsorbent certified that TEPA was modified onto the magnetic mesoporous silicon(FNMs), while FNMs/TEPA maintained the ordered mesoporous and pristine magnetic properties. The batch adsorption experiments demonstrated that TEPA significantly enhanced the removal capacity of the adsorbent for Cr(Ⅲ)-EDTA. FNMs/TEPA exhibited an excellent adsorption property(13.84 mg·g-1) at p H 4.0. Even in the presence of high concentrations of coexisting ions and organic acids, the adsorption performance of FNMs/TEPA was stable. Experimental characterization and DFT demonstrated that the adsorption of Cr(Ⅲ)-EDTA was ascribed to the electrostatic interaction, hydrogen bonding, and complexation between Cr(Ⅲ)-EDTA and amino groups on the adsorbent surface. The analysis of the independent gradient model(IGM) shows that electrostatic interaction is the main mode of action in the adsorption process. Moreover, FNMs/TEPA demonstrated remarkable reusability in three regeneration cycles. These findings indicated that FNMs/TEPA possessed excellent application prospects in the disposal of wastewater containing Cr(Ⅲ)-EDTA.
基金supported by the National Natural Science Foundation of China(No.52374350)China Postdoctoral Science Foundation(Nos.2020M680347 and 2021T140051)the Fundamental Research Funds for the Central Universities(No.FRF-TP-20-045A1)。
文摘Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.
基金Financial support from the National Natural Science Foundation of China (22075320)。
文摘To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li metal has low transport kinetics and is easy to causes the growth of lithium dendrites and accumulation of dead Li,which seriously affects the cycle life of batteries and even causes safety problems.Here,by comparing graphite with two types of hard carbon,it was found that hybrid anode formed by hard carbon and lithium metal,possessing more disordered mesoporous structure and lithophilic groups,presents better performance.Results indicate that the mesoporous structure provides abundant active site and storage space for dead lithium.With the synergistic effect of this structure and lithophilic functional groups(–COOH),the reversibility of hard carbon/lithium metal hybrid anode is maintained,promoting uniform deposition of lithium metal and alleviating formation of lithium dendrites.The hybrid anode maintains a 99.5%Coulombic efficiency(CE)after 260 cycles at a specific capacity of 500 m Ah/g.This work provides new insights into the hybrid anodes formed by carbon-based materials and lithium metal with high specific energy and fast charging ability.
基金supported by the National Natural Science Committee of China-Liaoning Provincial People's Government Joint Fund(U1908204)National Natural Science Foundation of China(21876006,21976009,and 21961160743)+2 种基金Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions(IDHT20190503)Natural Science Foundation of Beijing Municipal Commission of Education(KM201710005004)Development Program for the Youth Outstanding-Notch Talent of Beijing Municipal Commission of Education(CIT&TCD201904019)。
文摘Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.
基金supported by the National Key R&D program of China(2019YFA0706802)National Natural Science Foundation of China(52063029)+2 种基金Natural Science Basic Research Program of Shaanxi(2022JM-200,2021JQ-716)China Postdoctoral Science Foundation(2020M672269)Doctoral Research Program of Yan’an University(YDBK2019-02)
文摘Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar guest species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.
基金supported by the Science Foundation of China University of Petroleum,Beijing(No.ZX20230047)Open Research Fund of State Key Laboratory of Coking Coal Exploitation and Comprehensive Utilization,China Pingmei Shenma Group(No.41040220201308).
文摘Due to their low cost,environmental friendliness and high energy density,the lithium-sulfur batteries(LSB)have been regarded as a promising alternative for the next generation of rechargeable battery systems.However,the practical application of LSB is seriously hampered by its short cycle life and high self-charge owing to the apparent shuttle effect of soluble lithium polysulfides.Using MgSO_(4)@MgO composite as both template and dopant,template-guided S-doped mesoporous graphene(SMG)is prepared via the fluidized-bed chemical vapor deposition method.As the polypropylene(PP)modifier,SMG with high specific surface area,abundant mesoporous structures and moderate S doping content offers a wealth of physical and chemical adsorptive sites and reduced interfacial contact resistance,thereby restraining the serious shuttle effects of lithium polysulfides.Consequently,the LSB configured with mesoporous graphene(MG)as S host material and SMG as a separator modifier exhibits an enhanced electrochemical performance with a high average capacity of 955.64 mA h g^(-1) at 1C and a small capacity decay rate of 0.109%per cycle.Additionally,the density functional theory(DFT)calculation models have been rationally constructed and demonstrated that the doped S atoms in SMG possess higher binding energy to lithium polysulfides than that in MG,indicating that the SMG/PP separator can effectively capture soluble lithium polysulfides via chemical binding forces.This work would provide valuable insight into developing a versatile carbon-based separator modifier for LSB.
基金National Natural Science Foundation of China(Nos.52225204,52173233 and 52202085)Innovation Program of Shanghai Municipal Education Commission,China(No.2021-01-07-00-03-E00109)+3 种基金Natural Science Foundation of Shanghai,China(No.23ZR1479200)“Shuguang Program”Supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission,China(No.20SG33)Fundamental Research Funds for the Central Universities,China(No.2232024Y-01)DHU Distinguished Young Professor Program,China(Nos.LZA2022001 and LZB2023002)。
文摘Highly dispersed bimetallic alloy nanoparticle electrocatalysts have been demonstrated to exhibit exceptional performance in driving the nitrate reduction reaction(NO_(3)RR)to generate ammonia(NH_(3)).In this study,we prepared mesoporous carbon nanofibers(mCNFs)functionalized with ordered PtFe alloys(O-PtFe-mCNFs)by a composite micelle interface-induced co-assembly method using poly(ethylene oxide)-block-polystyrene(PEO-b-PS)as a template.When employed as electrocatalysts,O-PtFe-mCNFs exhibited superior electrocatalytic performance for the NO_(3RR)compared to the mCNFs functionalized with disordered PtFe alloys(D-PtFe-mCNFs).Notably,the NH_(3)production performance was particularly outstanding,with a maximum NH_(3)yield of up to 959.6μmol/(h·cm~2).Furthermore,the Faraday efficiency(FE)was even 88.0%at-0.4 V vs.reversible hydrogen electrode(RHE).This finding provides compelling evidence of the potential of ordered PtFe alloy catalysts for the electrocatalytic NO_(3)RR.
基金supported by the National Natural Science Foundation of China(21325731,21221004 and 51478241)~~
文摘Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the mesoporous characteristics of the template,with cubic symmetry(ia3d).It consists of a β-MnO2 crystalline phase corresponding to pyrolusite,with a rutile structure.Transmission electron microscopy and X-ray photoelectron spectroscopy showed that the 3D-MnO2 catalyst has a large number of exposed Mn4+ ions on the(110)crystal plane surfaces,with a lattice spacing of 0.311 nm; this enhances oxidation of HCHO.Complete conversion of HCHO to CO2 and H2O was achieved at 130 °C on 3D-MnO2; the same conversions on α-MnO2 and β-MnO2 nanorods were obtained at 140 and 180 °C,respectively,under the same conditions.The specific mesoporous structure,high specific surface area,and large number of surface Mn4+ ions are responsible for the catalytic activity of 3D-MnO2 in HCHO oxidation.
基金supported by the National Nature Science Foundation of China(21276117,21376111,21406092)~~
文摘A series of functional,tungsten-containing mesoporous silica materials(W-SiO2) have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and metal source respectively.These materials were then characterized through X-ray diffraction(XRD),transmission electron microscopy(TEM),Raman spectroscopy,Fourier transform infrared spectra(FTIR),diffuse reflectance spectra(DRS),and N2 adsorption-desorption,which were found to contain tungsten species that were effectively dispersed throughout the structure.The as-prepared materials W-SiO2 were also found to possess a mesoporous structure.The pore diameters of the respective sample W-SiO2-20 determined from the TEM images ranged from 2 to 4 nm,which was close to the average pore size determined from the nitrogen desorption isotherm(2.9 nm).The materials were evaluated as catalysts for the heterogeneous oxidative desulfurization of dibenzothiophene(DBT),which is able to achieve deep desulfurization within 40 min under the optimal conditions(Catalyst(W-SiO2-20)= 0.01 g,temperature = 60℃,oxidant(H2O2)= 20 μL).For the removal of different organic sulfur compounds within oil,the ability of the catalyst(W-SiO2-20) under the same conditions to remove sulfur compounds decreased in the order:4,6-dimethyldibenzothiophene Dibenzothiophene Benzothiophene 1-dodecanethiol.Additionally,they did not require organic solvents as an extractant in the heterogeneous oxidative desulfurization process.After seven separate catalytic cycles,the desulfurization efficiency was still as high as 90.3%.From the gas chromatography-mass spectrometer analysis,DBT was entirely oxidized to its corresponding sulfone DBTO2 after reaction.A mechanism for the heterogeneous desulfurization reaction was proposed.
基金Projects(51102285,81170912)supported by the National Natural Science Foundation of ChinaProject supported by the Open Foundation of State Key Laboratory of Powder Metallurgy,China
文摘The mesoporous hydroxyapatite (HA) was synthesized by hydrothermal method utilizing cationic surfactant cetyltrimethylammonium bromide (CTAB) as template. The crystalline phase, morphology and porous structure were characterized respectively by different detecting techniques. The results reveal that the particles are highly crystalline hydroxyapatite phase. The surfactant has little influence on the morphology of the crystals, but affects the porous structure obviously. The sample without CTAB has a low surface area not exceeding 33 m^2/g, and no distinct pores can be observed by TEM. While the samples obtained with the surfactant get better parameters. Numerous open-ended pores centered at 2-7 nm spread unequally on the surface of the hydroxyapatite nanorods. The N2 adsorption-desorption experiments show type IV isotherms with distinct hysteresis loops, illustrating the presence of mesoporous structure. When the mole ratio of CTAB to HA is 1:2, the sample has the largest surface area of 97.1 m^2/g and pore volume of 0.466 cm^3/g.
基金supported by the National Natural Science Foundation of China(21373056)the Science and Technology Commission of Shanghai Municipality(13DZ2275200)~~
文摘In this article, we report the preparation of a three-dimensional(3D) interconnected mesoporous anatase TiO2-SiO2 nanocomposite. The nanocomposite was obtained by using an ordered two-dimensional(2D) hexagonal mesoporous anatase 70 TiO2-30 SiO2-950 nanocomposite(crystallized at 950 °C for 2 h) as a precursor, NaO H as an etchant of SiO2 via a "creating mesopores in the pore walls" approach. Our strategy adopts mild conditions of creating pores such as diluted NaO H solution, appropriate temperature and solid/liquid ratio, etc. aiming at ensuring the integrities of mesopores architecture and anatase nanocrystals. XRD, TEM and N2 sorption techniques have been used to systematically investigate the physico-chemical properties of the nanocomposites. The results show that the intrawall mesopores are highly dense and uniform(average pore size 3.6 nm), and highly link the initial mesochannels in a 3D manner while retaining mesostructural integrity. There is no significant change to either crystallinity or size of the anatase nanocrystals before and after creating the intrawall mesopores. The photocatalytic degradation rates of rhodamine B(RhB, 0.303 min^–1) and methylene blue(MB, 0.757 min^–1) dyes on the resultant nanocomposite are very high, which are 5.1 and 5.3 times that of the precursor; even up to 16.5 and 24.1 times that of Degussa P25 photocatalyst, respectively. These results clearly demonstrate that the 3D interconnected mesopores structure plays an overwhelming role to the increments of activities. The 3D mesoporous anatase TiO2-SiO2 nanocomposite exhibits unexpected-high degradation activities to RhB and MB in the mesoporous metal oxide-based materials reported so far. Additionally, the nanocomposite is considerably stable and reusable. We believe that this method would pave the way for the preparation of other 3D highly interconnected mesoporous metal oxide-based materials with ultra-high performance.
基金Projects (21071107, 51002016) supported by the National Natural Science Foundation of ChinaProject (JQ201003) supported by Changzhou University Fund for Young Talent,China
文摘Mesoporous CeO2 with high specific surface area was synthesized using a modified evaporation-induced self-assembly (EISA) method, and a series of different amounts of Ag were loaded to this mesoporous CeO2 by a modified ethylene glycol reduction route. The samples were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), energy-dispersive spectrometry (EDS), nitrogen adsorption-desorption, Brunauer-Emmett-Teller (BET) and Barrett-Joyner- Halenda (BJH) methods. The mesoporous CeO2 structure with different proportions of silver nanoparticles and its antibacterial activity were adequately studied, confinnin~ that obtained novel materials show a good antibacterial effect.
基金supported by Guangdong Science and Technology Planning Project(2015A020216002)Guangdong Natural Science Foundation(2014A030313259)the National Natural Science Foundation of China(21543014,21173086,U1301245)~~
文摘The heterogeneously copper-catalyzed oxidative cleavage of styrene was studied using copper-doped mesoporous KIT-6(CU-KIT-6_x) prepared via pH adjustment(where x is the pH:1.43,2.27,3.78,3.97,4.24 or 6.62).Variations in the catalyst structure and morphology with pH values were characterized by X-ray power diffraction,nitrogen adsorption-desorption analysis,transmission electron microscopy and X-ray photoelectron spectroscopy.As the pH value applied during the initial synthesis,the resulting Cu-KIT-6_x exhibited different structural,textural and surface characteristics,especially in terms of specific copper species and copper content At a pH value of 3.78,approximately 4.6 wt%copper(Ⅱ) was successfully incorporated into the framework of the initial KIT-6,in the form of-Cu-O-Si- groups.The catalytic performance of each catalyst was evaluated by following the epoxidation of styrene,employing tert-butyl hydroperoxide as the oxidant and CH_3CN as the solvent.A significant styrene conversion of 43.5%with 86.6%selectivity for the desired styrene epoxide was obtained over the Cu-KIT-63.78.A higher Cu content,an ordered cubic laid mesoporous architecture and various specific textural characteristics all combined to endow the Cu-KIT-63.78 with high catalytic activity and good stability.
基金supported by the National Natural Science Foundation of China(201573136,U1510105)the Scientific Research Start-up Funds of Shanxi University(RSC723)~~
文摘Due to the advantages of high surface areas, large pore volumes and pore sizes, abundant nitrogen content that favored the metal-support interactions, N-doped ordered mesoporous carbons are regarded as a kind of fascinating and potential support for the synthesis of effective supported cat-alysts. Here, a N-doped ordered mesoporous carbon with a high N content (9.58 wt%), high surface area (417 m^2/g), and three-dimensional cubic structure was synthesized successfully and used as an effective support for immobilizing Pt nanoparticles (NPs). The positive effects of nitrogen on the metal particle size enabled ultrasmall Pt NPs (about 1.0 ± 0.5 nm) to be obtained. Moreover, most of the Pt NPs are homogeneously dispersed in the mesoporous channels. However, using the ordered mesoporous carbon without nitrogen as support, the particles were larger (4.4 ± 1.7 nm) and many Pt NPs were distributed on the external surface, demonstrating the important role of the nitrogen species. The obtained N-doped ordered mesoporous material supported catalyst showed excellent catalytic activity (conversion 100%) and selectivity (〉99%) in the hydrogenation of halogenated nitrobenzenes under mild conditions. These values are much higher than those achieved using a commercial Pt/C catalyst (conversion 89% and selectivity 90%). This outstanding catalytic perfor-mance can be attributed to the synergetic effects of the mesoporous structure, N-functionalized support, and stabilized ultrasmall Pt NPs. Moreover, such supported catalyst also showed excellent catalytic performance in the hydrogenation of other halogenated nitrobenzenes and nitroarenes. In addition, the stability of the multifunctional catalyst was excellent and it could be reused more than 10 times without significant losses of activity and selectivity. Our results conclusively show that a N-doped carbon support enable the formation of ultrafine metal NPs and improve the reaction ac-tivity and selectivity.
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Project (51162026) supported by the National Natural Science Foundation of ChinaProjects (20100480949, 201104509) supported by China Postdoctoral Science FoundationProject (133274341015501) supported by Postdoctoral Science Foundation of Central South University, China
文摘Li3V2(PO4)3 precursor was obtained with V2Os.nH2O , LiOH'H2O, NH4H2PO4 and sucrose as starting materials by grinding-sol-gel method, and then the monoclinic-typed Li3Vz(PO4)3 cathode material was prepared by sintering the amorphous Li3V2(PO4)3. The as-sintered samples were investigated by X-ray diffraction (XRD), transmission electron microscopy (TEM), N2 adsorption-desorption and electrochemical measurement. It is found that Li3Vz(PO4)3 sintered at 700 ℃ possesses good wormhole-like mesoporous structure with the largest specific surface area of 188 cmZ/g, and the smallest pore size of 9.3 nm. Electrochemical test reveals that the initial discharge capacity of the 700 ℃ sintered sample is 155.9 mA.h/g at the rate of 0.2C, and the capacity retains 154 mA.h/g after 50 cycles, exhibiting a stable discharge capacity at room temperature.