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.

Stable immobilization of lithium polysulfides using three-dimensional ordered mesoporous Mn_(2)O_(3) as the host material in lithium-sulfur batteries

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.

Ordered mesoporous materials for water pollution treatment:Adsorption and catalysis

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.

Bimetallic CoNi single atoms supported on three-dimensionally ordered mesoporous chromia:highly active catalysts for n-hexane combustion

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.

Single-Atom Lithiophilic Sites Confined within Ordered Porous Carbon for Ultrastable Lithium Metal Anodes

Attributing to the high specific capacity and low electrochemical reduction potential,lithium(Li)metal is regarded as the most promising anode for high-energy Li batteries.However,the growth of lithium dendrites and huge volume change seriously limit the development of lithium metal batteries.To overcome these challenges,an ordered mesoporous N-doped carbon with lithiophilic single atoms is proposed to induce uniform nucleation and deposition of Li metal.Benefiting from the synergistic effects of interconnected three-dimensional ordered mesoporous structures and abundant lithiophilic single-atom sites,regulated local current density and rapid mass transfer can be achieved,leading to the uniform Li deposition with inhibition of dendrites and buffered volume expansion.As a result,the as-fabricated anode exhibits a high CE of 99.8%for 200 cycles.A stable voltage hysteresis of 14 mV at 5 mA cm^(−2)could be maintained for more than 1330 h in the symmetric cell.Furthermore,the full cell coupled with commercial LiFePO_(4)exhibits high reversible capacity of 108 mAh g^(−1)and average Coulombic efficiency of 99.8%from 5th to 350th cycles at 1 C.The ordered mesoporous carbon host with abundant lithiophilic single-atom sites delivers new inspirations into rational design of high-performance Li metal anodes.

Preparation and improved photocatalytic activity of ordered mesoporous TiO_2 by evaporation induced self-assembly technique using liquid crystal as template

Ordered mesoporous TiO2 （OMPT） was prepared by an evaporation induced self-assembly technique using liquid crystal as template. The key factors affecting the methylene blue （MB） oxidation efficiency were investigated, including the initial concentration of MB, pH value and catalyst concentration. The results show that the obtained OMPT has high thermal stability and shows a 2D hexagonal mesostructure with the small particle size and high surface area, which lead to higher degradation efficiency than commercial P25 or nanoparticle TiO2 （NPT） fabricated by sol-gel process. The optimal conditions are 5 mg/L MB, pH 6 and 1.5 g/L OMPT for the fastest rate of MB degradation. Total organic carbon （TOC） analysis indicates complete mineralization of MB in 240 min by OMPT, with rate constant higher than NPT or P25.

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.

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.

Ordered mesoporous Fe/TiO_2 with light enhanced photo-Fenton activity

Ordered mesoporous Fe/TiO2 was prepared by an evaporation-induced self-assembly method. The iron ions were in situ embedded in the pore wall of the TiO2 framework. The catalyst has excellent light-assisted Fenton catalytic performance under UV and visible light irradiation. X-ray diffraction and transmission electron microscopy results showed that the TiO2 samples have an ordered two-dimensional hexagonal pore structure and an anatase phase structure with high crystallinity. The ordered pore structure of the TiO2 photocatalyst with a large specific surface area is beneficial to mass transfer and light harvesting. Furthermore, iron ions can be controlled by embedding them into the TiO2 framework to prevent iron ion loss and inactivation. After five cycles, the reaction rate of the ordered mesoporous Fe/TiO2 remained unchanged, indicating that the material has stable performance and broad application prospects for the purification of environmental pollutants.

Synthesis of a new ordered mesoporous NiMoO_4 complex oxide and its efficient catalytic performance for oxidative dehydrogenation of propane

Highly ordered mesoporous NiMoO4 material was successfully synthesized using mesoporous silica KIT-6 as hard template via vacuum nanocasting method. The structure was characterized by means of XRD, TEM, N2 adsorption-desorption, Raman and FT-IR. The mesoporous NiMoO4 with the coexistence of a-NiMoO4 and fl-NiMoO4 showed well-ordered mesoporous structure, a bimodal pore size distribution and crystalline framework. The catalytic performance of NiMoOa was investigated for oxidative dehydrogenation of propane. It is demonstrated that the mesoporous NiMoO4 catalyst with more surface active oxygen species showed better catalytic performance in oxidative dehydrogena- tion of propane in comparison with bulk NiMoO4.

Catalytic performance enhancement by alloying Pd with Pt on ordered mesoporous manganese oxide for methane combustion

Ordered mesoporous Mn2O3 (meso‐Mn2O3) and meso‐Mn2O3‐supported Pd, Pt, and Pd‐Pt alloy x(PdyPt)/meso‐Mn2O3; x = (0.10?1.50) wt%; Pd/Pt molar ratio (y) = 4.9?5.1 nanocatalysts were prepared using KIT‐6‐templated and poly(vinyl alcohol)‐protected reduction methods, respectively.The meso‐Mn2O3 had a high surface area, i.e., 106 m2/g, and a cubic crystal structure. Noble‐metalnanoparticles (NPs) of size 2.1?2.8 nm were uniformly dispersed on the meso‐Mn2O3 surfaces. AlloyingPd with Pt enhanced the catalytic activity in methane combustion; 1.41(Pd5.1Pt)/meso‐Mn2O3gave the best performance; T10%, T50%, and T90% (the temperatures required for achieving methaneconversions of 10%, 50%, and 90%) were 265, 345, and 425 °C, respectively, at a space velocity of20000 mL/(g?h). The effects of SO2, CO2, H2O, and NO on methane combustion over1.41(Pd5.1Pt)/meso‐Mn2O3 were also examined. We conclude that the good catalytic performance of1.41(Pd5.1Pt)/meso‐Mn2O3 is associated with its high‐quality porous structure, high adsorbed oxygen species concentration, good low‐temperature reducibility, and strong interactions between Pd‐Pt alloy NPs and the meso‐Mn2O3 support.

Nitrogen-doped ordered mesoporous carbon:Effect of carbon precursor on oxygen reduction reactions

Aniline,pyrrole and phenanthroline,which have different nitrogen compositions,are used as carbon precursors to synthesize nitrogen-doped ordered mesoporous carbons（NOMCs） by the nanocasting method.The effect of the precursor on the resultant NOMC is extensively investigated by nitrogen adsorption-desorption measurements,scanning electron microscopy,X-ray photoelectron spectroscopy（XPS）,cyclic voltammetry and rotating ring-disk electrode measurements.Salient findings are as follows.First,the precursor has a significant influence on the specific surface area and textural properties.The NOMC materials derived from pyrrole（C-PY-900：765 m^2/） and phenanthroline（C-Phen-900：746 m^2/） exhibit higher specific surface areas than the aniline analog（C-PA-900：569 m^2/）.Second,the XPS results indicate that the total nitrogen content（ca.3.1–3.3 at%） is similar for the three carbon sources,except for a slight difference in the nitrogen configuration.Furthermore,the content of the nitrogen-activated carbon atoms is found to closely depend on the precursor,which is the highest for the phenanthroline-derived carbon.Third,the electrochemical results reveal that the electrocatalytic activity follows in the order C-PA-900 C-PY-900 C-Phen-900,confirming that the nitrogen-activated carbon atoms are the active sites for the oxygen reduction reaction（ORR）.In summary,the precursor has considerable influence on the composition and textural properties of the NOMC materials,of which the ORR electrocatalytic activity can be enhanced through optimization of the NOMCs.

The effect of chelating agent on hydrodesulfurization reaction of ordered mesoporous alumina supported Ni Mo catalysts

In this paper,ordered mesoporous alumina(OMA)support with the high surface area(328 m^(2)g^(-1))and the large pore volume 0.74(cm^(3)·g^(-1))was synthesized by homogeneous precipitation method.And the influence of EDTA on the physical and chemical properties of the modified catalysts was also studied.The characteristic results showed that the addition of EDTA could adjust the metal-support interaction and improved the acidity of the corresponding catalyst.Combined with the catalytic performance results,the EDTA-modified Ni Mo E(1.0)/OMA catalyst displays the highest DBT hydrodesulfurization conversion(97.7%).

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.

Synthesis and Characterization of Titanium-doped Ordered Mesoporous Alumina

Titanium-doped ordered mesoporous alumina with specific structural properties has been prepared by the evaporation induced self-assembly sol-gel method. The results show that the doped titanium helps to stabilize the ordered mesoporous alumina material without influencing the ordered mesoporosity. The textural properties of the obtained sample are related to the amount of doped titanium. When the molar ratio of aluminum to titanium （n（Al）/n（Ti）） is controlled as 10.2, the titanium-doped ordered mesoporous alumina exhibits high surface area （up to 218 m^2 g^-1）, large pore volume （0.42 cm^3 g^-1） and narrow pore diameter （6.1 nm） after treating at 900 ℃, showing high thermal stability. Moreover, the obtained sample calcined at 900 ℃ still maintains ordered mesoporous structure and exhibits high thermal stability.

Different Synthesis Methods for Ordered Mesoporous Silicas And Their Characteristics Comparison

Ordered mesoporous silica were synthesized under different conditions:hydrothermal synthesis in basic medium,room temperature synthesis in acid medium and sol gel synthesis in neutral medium,and pore structure,specific surface area and pore size distribution of samples were studied and compared in detail by means of SAXRD,HRTEM,BET,FT IR.The results show that the mesopores in the samples obtained via above three methods all possess uniform hexagonal arrays in short range.Mesoporous silica obtained in acid medium possesses narrow pore size distribution centered around 1.24nm with specific surface area of 1220 m 2·g -1 ;Mesoporous silica obtained in basic medium by hydrothermal synthesis at 160℃ possesses narrow pore size distribution centered around 1.90nm with specific surface area of 542.8 m 2·g -1 ;and mesoporous silica obtained in neutral medium by sol gel synthesis possesses broader pore size distribution centered around 4.01nm,specific surface area of 485.0 m 2·g -1 .Therefore,ordered mesoporous silicas with different pore sizes can be prepared using various synthetic methods and conditions.After heat treatment,Si O Si bending vibration strengthens and the adsorption peak of asymmetrical Si O Si stretching vibration broadens,and the crosslinking and condensation reaction of silica skeleton strengthen, meanwhile the amount of active centers of hydroxyl group on the surface of mesopores may be influenced,thus chemical assembly activity of mesopores may also be influenced.

Chemically Modified Ordered Mesoporous Carbon/Polyaniline Composites for Electrochemical Capacitors

Chemically modified ordered mesoporous carbon CMK-3 materials were prepared by means of an easy wet-oxidative method in 2 mol/L nitric acid aqueous solution. A large amount of oxygen-containing functional groups were introduced onto the CMK-3 surface. Modified CMK-3（m-CMK-3） and aniline monomer were polymerized via an in situ chemical oxidative polymerization method. Morphological characterizations of m-CMK-3/PANI （polyaniline） composites were carried out via field emission scanning electron microscopy（SEM）. Their electrochemical properties were investigated with cyclic voltammetry, galvanostatic charge-discharge, and electrochemical impedance spectroscopy. The m-CMK-3/PANI composites have excellent properties in capacitance, and the highest specific capacitance（SC） value was up to 489 F/g, suggesting their potential application in the electrode material for electrochemical capacitors.

Effect of the pore length and orientation upon the electrochemical capacitive performance of ordered mesoporous carbons

By utilizing hard template method to adjust the mesopore length, and alkali activation to generate micro pores, two hierarchical porous carbons (HPCs) were prepared. With controlling of their mesopore length and the activation conditions, the complex system composed by HPCs and electrolyte was simplified and the effect of mesopore length on the performance of HPCs as electrodes in supercapacitors was investigated. It is found that with the mesopore length getting smaller, the ordered area gets smaller and the aggregation occurs, which is caused by the high surface energy of small grains. HPC with long pores (HPCL) exhibits a donut-like morphology with well-defined ordered mesopores and a regular orientation while in HPC with short pores (HPCS), short mesopores are only orderly distributed in small regions. Longer ordered channels form unobstructed ways for ions transport in the particles while shorter channels, only orderly distributed in small areas, results in blocked paths, which may hinder the electrolyte ions transport. Due to the unobstructed structure, HPCL exhibits good rate capability with a capacitance retention rate over 86% as current density increasing from 50 mA/g to 1000 mA/g. The specific capacitance of HPCL derived from the cyclic voltammetry test at 10 mV/s is up to 201.72 F/g, while the specific capacitance of HPCS is only 193.65 F/g. (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.

Nitrogen-doped cobalt nanoparticles/nitrogen-doped plate-like ordered mesoporous carbons composites as noble-metal free electrocatalysts for oxygen reduction reaction

In this work, nitrogen-doped cobalt nanoparticlesinitrogen-doped plate-like ordered mesoporous carbons (N/Co/OMCs) were used as noble-metal free electrocatalysts with high catalytic efficiency. Compared with OMCs with long channel length, due to more entrances for catalytic target accessibility and a short pathway for rapid diffusion, the utilization efficiency of cobalt nanoparticles inside the plate-like OMCs with short pore length is well improved, which can take full advantage of porous structure in electrocatalysis and increase the utilization of catalysts. The active sites in N/Co/OMCs for oxygen reduction reaction (ORR) are highly exposed to oxygen molecule, which results in a high activity for ORR. By combination of the catalytic properties of nitrogen dopant, incorporation of Co nanoparticles, and structural properties of OMCs, the N/Co/plate-like OMCs are highly active noble-metal free catalysts for ORR 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.