Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol

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.

Core-shell mesoporous carbon hollow spheres as Se hosts for advanced Al-Se batteries

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.

Hard-carbon hybrid Li-ion/metal anode enabled by preferred mesoporous uniform lithium growth mechanism

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.

Mesoporous Carbon Nanofibers Loaded with Ordered PtFe Alloy Nanoparticles for Electrocatalytic Nitrate Reduction to Ammonia

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.

Electrochemical hydrogen evolution efficiently boosted by interfacial charge redistribution in Ru/MoSe_(2) embedded mesoporous hollow carbon spheres

The strong metal-support interaction inducing combined effect plays a crucial role in the catalysis reaction. Herein, we revealed that the combined advantages of MoSe_(2), Ru, and hollow carbon spheres in the form of Ru nanoparticles(NPs) anchored on a two-dimensionally ordered MoSe_(2) nanosheet-embedded mesoporous hollow carbon spheres surface(Ru/MoSe_(2)@MHCS) for the largely boosted hydrogen evolution reaction(HER) performance. The combined advantages from the conductive support, oxyphilic MoSe_(2), and Ru active sites imparted a strong synergistic effect and charge redistribution in the Ru periphery which induced high catalytic activity, stability, and kinetics for HER. Specifically, the obtained Ru/MoSe_(2)@MHCS required a small overpotential of 25.5 and 38.4 mV to drive the kinetic current density of 10 mA cm^(-2)both in acid and alkaline media, respectively, which was comparable to that of the Pt/C catalyst. Experimental and theoretical results demonstrated that the charge transfer from MoSe_(2) to Ru NPs enriched the electronic density of Ru sites and thus facilitated hydrogen adsorption and water dissociation. The current work showed the significant interfacial engineering in Ru-based catalysts development and catalysis promotion effect understanding via the metal-support interaction.

Sulfur-doped hard carbon hybrid anodes with dual lithium-ion/metal storage bifunctionality for high-energy-density lithium-ion batteries

Bifunctional hybrid anodes(BHAs),which are both a high-performance active host material for lithium-ion storage as well as a guiding agent for homogeneous lithium metal nucleation and growth,exhibit significant potential as anodes for next-generation high-energy-density lithium-ion batteries(LIBs).In this study,sulfur-doped hard carbon nanosphere assemblies(S-HCNAs)were prepared through a hydrothermal treatment of a liquid organic precursor,followed by high-temperature thermal annealing with elemental sulfur for application as BHAs for LIBs.In a carbonate-based electrolyte containing fluoroethylene carbonate additive,the S-HCNAs showed high lithium-ion storage capacities in sloping as well as plateau voltage sections,good rate capabilities,and stable cyclabilities.In addition,high average Coulombic efficiencies(CEs)of~96.9%were achieved for dual lithium-ion and lithium metal storage cycles.In the LIB full-cell tests with typical NCM811 cathodes,the S-HCNA-based BHAs containing~400 mA h g^(−1) of excess lithium led to high energy and power densities of~500Wh kg^(−1) and~1695Wkg^(−1),respectively,and a stable cycling performance with~100%CEs was achieved.

N-doped ordered mesoporous carbon as a multifunctional support of ultrafine Pt nanoparticles for hydrogenation of nitroarenes

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.

Influence of Preparation Conditions on Structural Stability of Ordered Mesoporous Carbons Synthesized by Evaporation-induced Triconstituent Co-assembly Method

Various ordered mesoporous carbons （OMCs） have been prepared by evaporation-induced trieonstituent co-assembly method. Their mesostructural stability under different carbon content, aging time and acidity were conveniently monitored by X-ray diffraction, transmission electron microscopy, and N2 sorption isotherms techniques. The results show mesostruetural stability of OMCs is enhanced as the carbon content increases from 36% to 46%, further increasing carbon content deteriorates the mesostructural stability. Increasing aging time from 0.5 h to 5.0 h make the mesostructural stability go through an optimum （2.0 h） and gradually reduce framework shrinkage of the OMCs. Highly OMCs can only be obtained in the acidity range of 0.2-1.2 mol/L HC1, when the acidity is near the isoelectrie point of silica, the resulting OMCs have the best mesostructure stability. Under the optimum condition, the carbon content of 46%, aging time of 2.0 h, and 0.2 mol/L HCl, the resulting OMCs have the best mesostrueture stability and the highest BET surface areas of 2281 m2/g.

Size-control growth of thermally stable Au nanoparticles encapsulated within ordered mesoporous carbon framework

Simultaneously controlling the size of Au nanoparticles and immobilizing their location to specific active sites while hindering migration and sintering at elevated temperatures is a current challenge within materials chemistry.Typical methods require the use of protecting agents to control the properties of Au nanoparticles and therefore it is difficult to decouple the influence of the protecting agent and the support material.By functionalizing the internal surface area of mesoporous carbon supports with thiol groups and implementing a simple acid extraction step,we are able to design the resulting materials with precise control over the Au nanoparticle size without the need for the presence of any protecting group,whilst simultaneously confining the nanoparticles to within the internal porous network.Monodispersed Au nanoparticles in the absence of protecting agents were encapsulated into ordered mesoporous carbon at various loading levels via a coordination-assisted self-assembly approach.The X-ray diffractograms and transmission electron microscopy micrographs show that the particles have controlled and well-defined diameters between 3 and 18 nm at concentrations between 1.1 and 9.0 wt%.The Au nanoparticles are intercalated into the pore matrix to different degrees depending on the synthesis conditions and are stable after high temperature treatment at 600 °C.N2 adsorption-desorption isotherms show that the Au functionalized mesoporous carbon catalysts possess high surface areas（1269–1743 m^2/g）,large pore volumes（0.78–1.38 cm^3/g）and interpenetrated,uniform bimodal mesopores with the primary larger mesopore lying in the range of 3.4–5.7 nm and the smaller secondary mesopore having a diameter close to 2 nm.X-ray absorption near extended spectroscopy analysis reveals changes to the electronic properties of the Au nanoparticles as a function of reduced particle size.The predominant factors that significantly determine the end Au nanoparticle size is both the thiol group concentration and subjecting the as-made materials to an additional concentrated sulfuric acid extraction step.

Pt nanoparticles entrapped in ordered mesoporous carbons:An efficient catalyst for the liquid-phase hydrogenation of nitrobenzene and its derivatives

Pt nanoparticles entrapped in ordered mesoporous CMK-3 carbons with p6mm symmetry were prepared using a facile impregnation method, and the resulting materials were characterized using X-ray diffraction spectroscopy, N2 adsorption-desorption, scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. The Pt nanoparticles were highly dispersed in the CMK-3 with 43.7% dispersion. The Pt/CMK-3 catalyst was an effective catalyst for the liquid-phase hydrogenation of nitrobenzene and its derivatives under the experimental conditions studied here. The Pt/CMK-3 catalyst was more active than commercial Pt/C catalyst in most cases. A highest turnover frequency of 43.8 s-1 was measured when the Pt/CMK-3 catalyst was applied for the hydrogenation of 2-methyl-nitrobenzene in ethanol under optimal conditions. It is worthy of note that the Pt/CMK-3 catalyst could be recycled easily, and could be reused at least fourteen times without any loss in activity or selectivity for the hydrogenation of nitrobenzene in ethanol.

Ordered mesoporous carbon supported bifunctional PtM(M=Ru,Fe,Mo)electrocatalysts for a fuel cell anode

The deposition onto an ordered mesoporous carbon（OMC）support of well dispersed PtM（M = Ru,Fe,Mo）alloy nanoparticles（NPs）were synthesized by a direct replication method using SBA-15 as the hard template,furfuryl alcohol and trimethylbeneze as the primary carbon sources,and metal acetylacetonate as the alloying metal precursor and secondary carbon source.The physicochemical properties of the PtM-OMC catalysts were characterized by N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,X-ray absorption near edge structure,and extended X-ray absorption fine structure.The alloy PtM NPs have an average size of 2-3 nm and were well dispersed in the pore channels of the OMC support.The second metal（M）in the PtM NPs was mostly in the reduced state,and formed a typical core（Pt）-shell（M）structure.Cyclic voltammetry measurements showed that these PtM-OMC electrodes had excellent electrocatalytic activities and tolerance to CO poisoning during the methanol oxidation reaction,which surpassed those of typical activated carbon-supported PtRu catalysts.In particular,the PtFe-OMC catalyst,which exhibited the best performance,can be a practical anodic electrocatalyst in direct methanol fuel cells due to its superior stability,excellent CO tolerance,and low production cost.

Mesoporous poly(ionic liquid)s with dual active sites for highly efficient CO_(2)conversion

Atmospheric CO_(2)concentrations are soaring due to the continued use of fossil fuels in energy production,an anthropogenic activity that is playing a leading role in global warming.Thus,research aimed at the capture and conversion of CO_(2)into value-added products,such as cyclic carbonates,is booming.While CO_(2)is an abundant,cheap,non-toxic,and readily accessible Cl feedstock,its thermodynamic stability necessitates the development of highly efficient catalysts that are able to promote chemical reactions under mild conditions.In this work,a novel mesoporous poly(ionic liquid)with dual active sites was synthesized through a facile method that involves co-polymerization,post-synthetic metalation,and supercritical CO_(2)drying.Due to a high density of nucleophilic and electrophilic sites,the as-prepared poly(ionic liquid),denoted as P2D-4BrBQA-Zn,offers excellent performance in a CO_(2)cycloaddition reaction using epichlorohydrin as the substrate(98.9%conversion and 96.9%selectivity).Moreover the reaction is carried out under mild,solvent-free,and additive-free conditions.Notably,P2D-4BrBQA-Zn also efficiently promotes the conversion of various other epoxide substrates into cyclic carbonates.Overall,the catalyst is found to have excellent substrate compatibility,stability,and recyclability.

A novel polyaniline/mesoporous carbon nano-composite electrode for asymmetric supercapacitor

A novel nano-composite of polyaniline/mesoporous carbon（PANI/CMK-3） was prepared with mesoporous carbon（CMK-3） serving as the support.Electrochemical asymmetric capacitors have been successfully designed by using PANI/CMK-3 composite and CMK-3 as positive and negative electrode,respectively.The results showed that the discharge capacity of the asymmetric capacitor could reach 87.4 F/g under the current density of 5 mA/cm^2 and cell voltage of 1.4 V.The energy density of the asymmetric capacitor was up to 23.8 Wh/kg with a power density of 206 W/kg.Furthermore,PANI/CMK-3-CMK-3 asymmetric capacitor using this PANI/CMK-3 nano-composite could be activated quickly and possess high charge-discharge efficiency.

Conversion of Malaysian low-rank coal to mesoporous activated carbon:Structure characterization and adsorption properties

Malaysian Selantik low-rank coal(SC)was used as a precursor to prepare a form of mesoporous activated carbon(SC-AC)with greater surface area(SA)via a microwave induced KOH-activation method.The characteristics of the SC and SC-AC were evaluated by the iodine number,ash content,bulk density,and moisture content The structure and surface characterization was carried out using pore structure analysis(BET),scanning electron microscopy with energy dispersive X-ray spectroscopy(SEM-EDX),X-ray diffraction(XRD),Fourier Transform Infrared(FTIR),elemental analysis(CHNS),thermogravimetric analysis(TGA),and determination of the point of zero charge(pH(PZC)).These results signify a mesoporous structure of SC-AC with an increase of ca.1160 times(BET SA=1094.3 m^2·g^-1)as compared with raw SC without activation(BET SA=1.23 m^2·g^-1).The adsorptive properties of the SC-AC with methylene blue(MB)was carried out at variable adsorbent dose(0.2-1.6 g·L^-1),solution pH(2-12),initial MB concentrations(25-400 mg·L^-1),and contact time(0-290 min)using batch mode operation.The kinetic profiles follow pseudo-second order kinetics and the equilibrium uptake of MB conforms to the Langmuir model with a maximum monolayer adsorption capacity of 491.7 mg g^-1 at 303 K.Thermodynamic functions revealed a spontaneous endothermic adsorption process.The mechanism of adsorption included mainly electrostatic attractions,hydrogen bonding interaction,andπ-πstacking interaction.This work shows that Malaysian Selantik low-rank coal is a promising precursor for the production of low-cost and efficient mesoporous activated carbon with substantive surface area.

Preparation of a kind of mesoporous carbon and its performance in adsorptive desulfurization

Carbon materials were prepared using mesoporous silica HMS with different pore sizes as the hard templates and water-soluble phenolic resin as the carbon source. The obtained materials were characterized by powder X-ray diffraction, transmission electron microscopy and N2 physical adsorption, and were used in adsorptive desulfurization. It has been shown that the carbon material prepared using HMS with larger pore size （〉3 nm） presented uniform wormlike mesopore of 2.3 nm and large BET surface area （1903 m2/g）. The mesoporous carbon was an excellent adsorbent to remove the refractory sulfur compound in diesel, especially dibenzothiophene and 4, 6-dimethyldibenzothiophene.

Microwave-assisted conversion of biomass wastes to pseudocapacitive mesoporous carbon for high-performance supercapacitor

Developing an efficient approach of transforming biomass waste to functional carbon-based electrode materials applied in supercapacitor offers an important and high value-added practical application due to the abundance and considerable low price of biomass wastes.Herein,a hierarchical carbon functionalized with electrochemical-active oxygen-containing groups was fabricated by microwave treatment from the biomass waste of camellia oleifera.The obtained mesoporous carbon(MAC)owns nanosheet morphology,rich mesoporosity,large surface area(1726 m2/g)and very high oxygenic functionalities(16.2 wt%)with pseudocapacitive activity.Prepared electrode of supercapacitor and tested in 2.0 M H2 SO4,the MAC exhibits an obvious pseudocapacitive activity and achieved a superior supercapacitive performance to that of directly activated carbon(DAC-800)including high specific capacitance(367 F/g vs.298 F/g)and better rate performance(66%vs.44%).The symmetrical supercapacitor based on MAC shows a high capacity of275 F/g,large energy density of 9.55 Wh/kg(at power density of 478 W/kg)and excellent cycling stability with 99%capacitance retention after 10000 continuous charge-discharge,endowing the obtained MAC a promising functional material for electrochemical energy storage.

Sulphur-doped ordered mesoporous carbon with enhanced electrocatalytic activity for the oxygen reduction reaction

Metal-free, heteroatom functionalized carbon-based catalysts have made remarkable progress in recent years in a wide range of applications related to energy storage and energy generation. In this study, high surface area mesoporous ordered sulphur doped carbon materials are obtained via one-pot hydrothermal synthesis of carbon/SBA-15 composite after removal of in-situ synthesized hard template SiO2. 2-thiophenecarboxy acid as sulphur source gives rise to sulphur doping level of 5.5 wt%. Comparing with pristine carbon, the sulphur doped mesoporous ordered carbon demonstrates improved electro-catalytic activity in the oxygen reduction reaction in alkaline solution. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

In Situ Synthesis of Fluorescent Mesoporous Silica–Carbon Dot Nanohybrids Featuring Folate Receptor-Overexpressing Cancer Cell Targeting and Drug Delivery

Multifunctional nanocarrier-based theranostics is supposed to overcome some key problems in cancer treatment.In this work,a novel method for the preparation of a fluorescent mesoporous silica–carbon dot nanohybrid was developed.Carbon dots(CDs),from folic acid as the raw material,were prepared in situ and anchored on the surface of amino-modified mesoporous silica nanoparticles(MSNs–NH2) via a microwave-assisted solvothermal reaction.The as-prepared nanohybrid(designated MSNs–CDs) not only exhibited strong and stable yellow emission but also preserved the unique features of MSNs(e.g.,mesoporous structure,large specific surface area,and good biocompatibility),demonstrating a potential capability for fluorescence imagingguided drug delivery.More interestingly,the MSNs–CDs nanohybrid was able to selectively target folate receptor-overexpressing cancer cells(e.g.,HeLa),indicating that folic acid still retained its function even after undergoing the solvothermal reaction.Benefited by these excellent properties,the fluorescent MSNs–CDs nanohybrid can be employed as a fluorescence-guided nanocarrier for the targeted deliveryof anticancer drugs(e.g.,doxorubicin),thereby enhancing chemotherapeutic efficacy and reducing side effects.Our studies may provide a facile strategy for the fabrication of multifunctional MSN-based theranostic platforms,which is beneficial in the diagnosis and therapy of cancers in future.

Preparation of mesoporous activated carbons from coal liquefaction residue for methane decomposition

Mesoporous activated carbons were prepared from direct coal liquefaction residue （CLR） by KOH activation method, and the experiments were carried out to investigate the effects of KOH/CLR ratio, solvent for mixing the CLR and KOH, and carbonization procedure on the resultant carbon texture and catalytic activity for catalytic methane decomposition （CMD）. The results showed that optimal KOH/CLR ratio of 2 ： 1; solvent with higher solubility to KOH or the CLR, and an appropriate carbonization procedure are conductive to improving the carbon pore structure and catalytic activity for CMD. The resultant mesoporous carbons show higher and more stable activity than microporous carbons. Additionally, the relationship between the carbon textural properties and the catalytic activity for CMD was also discussed.

Ammonia-treatment assisted fully encapsulation of Fe_2O_3 nanoparticles in mesoporous carbons as stable anodes for lithium ion batteries

To improve the initial coulombic efficiency and bulk density of ordered mesoporous carbons, active Fe203 nanoparticles were introduced into tubular mesopore channels of CMK-5 carbon, which possesses high specific surface area （〉1700 m2.g-1） and large pore volume （〉1.8 cm3-g-1）. Fine Fe203 nanoparticles with sizes in the range of 5-7 nm were highly and homogenously encapsulated into CMK-5 matrix through ammonia-treatment and subsequent pyrolysis method. The Fe203 loading was carefully tailored and designed to warrant a high Fe203 content and adequate buffer space for improving the electrochemical performance. In particular, such Fe203 and mesoporous carbon composite with 47 wt% loading exhibits a considerably stable cycle performance （683 mAh.g-1 after 100 cycles, 99% capacity retention against that of the second cycle） as well as good rate capability. The fabrication strategy can effectively solve the drawback of single material, and achieve a high-performance lithium electrode material.