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Synthesis, characterization and catalytic properties of mesoporous MCM-48 containing zeolite secondary

LI Qiang, ZHANG Ying, DOU Tao, LI Yuping, WANG Shan, SUN Famin

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 1-5 doi: 10.1007/s11705-007-0001-0

摘要： Mesoporous aluminosilicate MCM-48 containing zeolite secondary building units in the pore wall has been synthesized in alkaline media with a two-step procedure. The aluminosilicate precursors comprising zeolite secondary building units were first synthesized by carefully controlling reaction conditions and then were assembled using cotemplates of gemini surfactant [CHN(CH)(CH)N(CH)CH] (18-3-18) and triethanolamine (TEA). X-ray Diffraction (XRD) patterns of the as-made samples indicated that highly ordered mesostructured MCM-48 was formed. Transmission Electron Microscopy (TEM) images further verified the formation of MCM-48 with uniform cubic pore channel system having the pore opening diameter of about 25 Å. Compared with the conventionally synthesized MCM-48, the as-synthesized MCM-48 sample showed an adsorption band at 520 600 cm in its FT-IR spectrum, which was assigned to five-membered ring vibration from zeolite structure. This suggested the presence of zeolite building units in the pore wall. N2 adsorption data showed that the material had a much higher specific surface area (1 200 m/g) than the conventional MCM-48(1 100 m/g). Finally, the catalytic performance of the as-made MCM-48 was evaluated by hydrogenation dealkylation reaction of heavy aromatic hydrocarbons. Catalytic results showed that the as-made MCM-48 catalyst exhibited higher conversion than the conventional MCM-48 catalyst. The as-made mesostructured MCM-48 may have a potential catalytic application in the conversion of bulky molecules.

关键词： diameter     mesostructured MCM-48     Catalytic     presence     five-membered    

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Porous silica synthesis out of coal fly ash with no residue generation and complete silicon separation

《环境科学与工程前沿（英文）》 2023年 第17卷 第9期 doi: 10.1007/s11783-023-1712-2

摘要：

● Both amorphous and crystalline silicon are completely separated from coal fly ash.

关键词： Coal fly ash     Alkali fusion     Micro-/meso-porous Si     Zeolite MCM-48     Crystalline transformation    

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Atomistic simulations for adsorption and separation of flue gas in MFI zeolite and MFI/MCM-41 micro/mesoporous

Shengchi ZHUO, Yongmin HUANG, Jun HU, Honglai LIU

《化学科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 264-273 doi: 10.1007/s11705-010-1007-6

摘要： Adsorption of pure CO and N and separation of CO /N mixture in MFI zeolite and MFI/MCM-41 micro/mesoporous composite have been studied by using atomistic simulations. Fully atomistic models of MFI and MFI/MCM-41 are constructed and characterized. A bimodal pore size distribution is observed in MFI/MCM-41 from simulated small- and broad-angle X-ray diffraction patterns. The density of MFI/MCM-41 is lower than MFI, while its free volume and specific surface area are greater than MFI due to the presence of mesopores. CO is preferentially adsorbed than N , and thus, the loading and isosteric heat of CO are greater than N in both MFI and MFI/MCM-41. CO isotherm in MFI/MCM-41 is similar to that in MFI at low pressures, but resembles that in MCM-41 at high pressures. N shows similar amount of loading in MFI, MCM-41 and MFI/MCM-41. The selectivity of CO over N in the three adsorbents decreases in the order of MFI>MFI/MCM-41>MCM-41. With increasing pressure, the selectivity increases in MFI and MFI/MCM-41, but decreases in MCM-41. The self-diffusivity of CO and N in MFI decreases as loading increases, while in MFI/MCM-41, it first increases and then drops.

关键词： adsorption     diffusion     CO2     flue gas     zeolite     micro/mesoporous composite    

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Enhanced CuCl dispersion by regulating acidity of MCM-41 for catalytic oxycarbonylation of ethanol to

Pengzhen CHEN, Shouying HUANG, Jijie ZHANG, Shengping WANG, Xinbin MA

《化学科学与工程前沿（英文）》 2015年 第9卷 第2期   页码 224-231 doi: 10.1007/s11705-014-1447-5

摘要： CuCl supported on molecular sieves has attracted increasing attention in catalyzing oxidative carbonylation of ethanol to diethyl carbonate. Mesoporous MCM-41 has been widely used as catalyst support due to its large surface area and well defined mesoporous structure. Considering its intrinsic weak acidity, MCM-41 was modified by a simple impregnation method to incorporate Al. The incorporation of Al components resulted in the high dispersion of Cu species and the increase of acid sites without changing the mesoporous structure of MCM-41, and thus enhanceed the catalytic activity of CuCl/MCM-41for diethyl carbonate synthesis.

关键词： MCM-41     acidity     oxidative carbonylation     diethyl carbonate    

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Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis

Shengping WANG, Changqing MA, Yun SHI, Xinbin MA

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 95-103 doi: 10.1007/s11705-014-1405-2

摘要： Titanium-containing mesoporous materials (Ti-MCM-41) were obtained by hydrothermal synthesis. Such materials are active catalysts for the transesterification of dimethyl oxalate and phenol to produce diphenyl oxalate. To understand the role of the Ti in the catalytic process, Ti-MCM-41 samples with different Si/Ti ratios (from 5 to 100) were prepared and the samples were analyzed by Fourier transform infrared spectroscopy, UV-visible spectroscopy, and ammonia temperature programmed desorption. It was concluded that the Ti is incorporated into the framework of the MCM-41 and formed weak Lewis acid sites. In addition, the number of Ti(IV) sites increased as the amount of titanium increased. X-ray powder diffraction, N adsorption-desorption and transmission electron microscopy results showed that the Ti-MCM-41 samples have a hexagonal arrangement of mono-dimensional pores. A large number of Ti(IV) sites coupled with the mesoporous structure and large pore diameters are favorable for the transesterification catalytic properties of Ti-MCM-41.

关键词： Ti-MCM-41     mesoporous molecular sieve     acid sites     transesterification     hydrothermal synthesis    

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Factors affecting the formation of zeolite seed layers and the effects of seed layers on the growth ofzeolite silicalite-1 membranes

ZHANG Xiongfu, WANG Jinqu, LIU Hai′ou, WANG Anjie

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 172-177 doi: 10.1007/s11705-007-0032-6

摘要： The present study investigates the formation of silicalite-1 seed layers on a porous carbon support of 0.5 μm pore size and α-A1O supports with different pore sizes (0.1 μm and 4 μm) via the slip-casting technique. The effects of support property, seed size and solvent on the formation of seed layers were investigated in detail. The growth of silicalite-1 membranes on different seeded supports by hydrothermal synthesis was also evaluated. The scanning electron microscopy (SEM) and X-ray diffraction (XRD) characterizations indicate that a continuous seed layer can be obtained on the smooth support of 0.1 μm pore size by using any seed of 100 nm, 600 nm or 2.2 μm in size, whereas, on the coarse supports with either 0.5 μm or 4 μm pore size, a continuous seed layer cannot be formed using the above seed sizes and the same seeding time. At a longer contact time, a seed layer can also be formed using 100 nm seed on the supports with larger pore size. However, the layer is not uniform and smooth. For a hydrophobic porous carbon support, seeding ethanol suspension, which has weak polarity, favors the formation of a continuous seed layer. The seed layers and membranes grown from the smaller seed are more uniform and continuous and possess smoother surfaces than those from the larger seed. The seed layer and respective grown membrane formed from nanosized seed (100 nm) are the most uniform and compact. With this method of seeded secondary synthesis of zeolite membranes, the quality of a membrane mainly depends on the quality of the seed layer.

关键词： silicalite-1     α-A1O     growth     seeding ethanol     quality    

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Synthesis of nanofluids composed of deep eutectic solvents and metal-modified MCM-41 particles as multifunctional

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1776-1787 doi: 10.1007/s11705-023-2314-z

摘要： Compared with traditional hydrodesulfurization, new nonhydrodesulfurization methods have the advantage of a high removal efficiency for thiophene compounds under mild conditions. However, independent nonhydrodesulfurization technologies are faced with their own shortcomings, such as limitations of the desulfurization performance and regeneration of materials. To overcome these limitations, four nanofluids were prepared by dispersing different metal-modified MCM-41 particles in deep eutectic solvent as multifunctional promoters to develop a comprehensive desulfurization method. Based on the excellent adsorbability and high catalytic activity of the dispersed particles and the outstanding extractability of deep eutectic solvent in nanofluids, a high sulfur removal of 99.33% was achieved for model oil under mild conditions in 15 min. The nanofluids also showed excellent reusability due to their high structural stability. In addition, NF@Cu/Al-MCM-41-2.5% exhibited the best desulfurization performance among the prepared nanofluids. This result was obtained because the introduction of Al ions increased the number of acid sites and defect sites to improve the catalytic activity and adsorbability, and the best affinity of Cu/Al-MCM-41 for the deep eutectic solvent favored the reaction mass transfer. This work opens the door to the development of a comprehensive nonhydrodesulfurization method based on the design of nanofluid materials.

关键词： fuel oil desulfurization     nanofluids     catalytic ozonation    

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CuO/zeolite catalyzed oxidation of gaseous toluene under microwave heating

Longli BO, Jianbo LIAO, Yucai ZHANG, Xiaohui WANG, Quan YANG

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 395-402 doi: 10.1007/s11783-012-0417-8

摘要： The development of a combined process of catalytic oxidation and microwave heating for treatment of toluene waste gas was described in this work. Toluene, a typical toxic volatile organic compound, was oxidized through a fixed bed reaction chamber containing zeolite-supported copper oxide (CuO/zeolite) catalyst mixed with silicon carbide (SiC), an excellent microwave-absorbing material. The target compound was efficiently degraded on the surface of the catalyst at high reaction temperature achieved by microwave-heated SiC. A set of experimental parameters, such as microwave power, air flow and the loading size of CuO etc., were investigated, respectively. The study demonstrated these parameters had critical impact on toluene degradation. Under optimal condition, 92% toluene was removed by this combined process, corresponding to an 80%–90% TOC removal rate. Furthermore, the catalyst was highly stable even after eight consecutive 6-h runs. At last, a hypothetical degradation pathway of toluene was proposed based on the experimental data obtained from gas chromatography-mass spectrum and Fourier transform infrared spectroscopy analyses.

关键词： microwave     catalytic oxidation     CuO/zeolite catalyst     silicon carbide (SiC)     toluene    

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Effects of natural zeolite and sulfate ions on the mechanical properties and microstructure of plastic

《结构与土木工程前沿（英文）》 2022年 第16卷 第1期   页码 86-98 doi: 10.1007/s11709-021-0793-x

摘要： One of the strategic materials used in earth-fill embankment dams and in modifying and preventing groundwater flow is plastic concrete (PlC). PlC is comprised of aggregates, water, cement, and bentonite. Natural zeolite (NZ) is a relatively abundant mineral resource and in this research, the microstructure, unconfined strength, triaxial behavior, and permeability of PlC made with 0%, 10%, 15%, 20%, and 25% replacement of cement by NZ were studied. Specimens of PIC-NZ were subjected to confined conditions and three different confining pressures of 200, 350, and 500 kPa were used to investigate their mechanical behavior and permeability. To study the effect of sulfate ions on the properties of PlC-NZ specimens, the specimens were cured in one of two different environments: normal condition and in the presence of sulfate ions. Results showed that increasing the zeolite content decreases the unconfined strength, elastic modulus, and peak strength of PlC-NZ specimens at the early ages of curing. However, at the later ages, increasing the zeolite content increases unconfined strength as well as the peak strength and elastic modulus. Specimens cured in the presence of sulfate ions indicated lower permeability, higher unconfined strength, elastic modulus, and peak strength due to having lower porosity.

关键词： plastic concrete     sulfate resistance     natural zeolite     triaxial compression test     SEM     permeability    

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Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO

Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 365-381 doi: 10.1007/s11783-013-0520-5

摘要： In this work, xylene removal from waste gas streams was investigated via catalytic oxidation over Pd/carbon-zeolite and Pd/carbon-CeO nanocatalysts. Activated carbon was obtained from pine cone chemically activated using ZnCl and modified by H PO . Natural zeolite of clinoptilolite was modified by acid treatment with HCl, while nano-ceria was synthesized via redox method. Mixed supports of carbon-zeolite and carbon-ceria were prepared and palladium was dispersed over them via impregnation method. The prepared samples were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Brunauer-Emmett-Teller surface area (BET), Fourier transform infrared spectroscopy (FTIR) and thermogravimetric (TG) techniques. Characterization of nanocatalysts revealed a good morphology with an average particle size in a nano range, and confirmed the formation of nano-ceria with an average crystallite size below 60 nm. BET analysis indicated a considerable surface area for catalysts (~1000 m ·g ). FTIR patterns demonstrated that the surface groups of synthesized catalysts are in good agreement with the patterns of materials applied in catalyst synthesis. The performance of catalysts was assessed in a low-pressure catalytic oxidation pilot in the temperature range of 100°C–250°C. According to the reaction data, the synthesized catalysts have been shown to be so advantageous in the removal of volatile organic compounds (VOCs), representing high catalytic performance of 98% for the abatement of xylene at 250°C. Furthermore, a reaction network is proposed for catalytic oxidation of xylene over nanocatalysts.

关键词： Pd/carbon-CeO2     Pd/carbon-zeolite     pine cone     ZnCl2     catalytic oxidation     xylene    

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Photocatalytic degradation of omethoate using NaY zeolite-supported TiO

Dishun ZHAO, Jialei WANG, Zhigang ZHANG, Juan ZHANG

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 206-210 doi: 10.1007/s11705-009-0053-4

摘要： The degradation of omethoate was conducted using H O as oxidant, TiO supported on NaY zeolite as photocatalyst and a 300 W lamp as light source. The effect of the calcination temperature of the photocatalyst, the amount of TiO loaded on NaY zeolite, the photocatalyst amount, the pH value and the radiation time on the degradation ratio of omethoate were investigated. The results show that TiO /NaY zeolite photocatalyst prepared by sol-gel method had good photocatalysis. The photocatalytic optimum oxidation conditions of omethoate are as follows: the calcination temperature of the photocatalyst is 550°C,the amount of TiO loaded on NaY zeolite is 35.2 wt-%, the amount of photocatalyst is 5 g/L, pH=8 and the radiation time is 180 min. Under these conditions, the removal ratio of omethoate is up to 93%.

关键词： TiO2     NaY zeolite     photocatalytic degradation     omethoate    

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Catalytic fast pyrolysis of Kraft lignin with HZSM-5 zeolite for producing aromatic hydrocarbons

Xiangyu LI, Lu SU, Yujue WANG, Yanqing YU, Chengwen WANG, Xiaoliang LI, Zhihua WANG

《环境科学与工程前沿（英文）》 2012年 第6卷 第3期   页码 295-303 doi: 10.1007/s11783-012-0410-2

摘要： Catalytic fast pyrolysis (CFP) of Kraft lignins with HZSM-5 zeolite for producing aromatics was investigated using analytical pyrolysis methods. Two Kraft lignins were fast pyrolyzed in the absence and presence of HZSM-5 in a Curie-point pyrolyzer. Without the catalyst, fast pyrolysis of lignin predominantly produced phenols and guaiacols that were derived from the subunits of lignin. However, the presence of HZSM-5 changed the product distribution dramatically. As the SiO /Al O ratio of HZSM-5 decreased from 200 to 25 and the catalyst-to-lignin ratio increased from 1 to 20, the lignin-derived oxygenates progressively decreased to trace and the aromatics increased substantially. The aromatic yield increased considerably as the pyrolysis temperature increased from 500°C to 650°C, but then decreased with yet further increase of pyrolysis temperature. Under optimal reaction conditions, the aromatic yields were 2.0 wt.% and 5.2 wt.% for the two lignins that had effective hydrogen indexes of 0.08 and 0.35.

关键词： lignin     catalytic fast pyrolysis     HZSM-5     zeolite     aromatic hydrocarbon    

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Hierarchical ZSM-5 zeolite with radial mesopores: Preparation, formation mechanism and application for

Darui Wang, Hongmin Sun, Wei Liu, Zhenhao Shen, Weimin Yang

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 248-257 doi: 10.1007/s11705-019-1853-9

摘要： Hierarchical ZSM-5 zeolite with radial mesopores is controllably synthesized using piperidine in a NaOH solution. The piperidine molecules enter the zeolite micropores and protect the zeolite framework from extensive desilication. The areas containing fewer aluminum atoms contain fewer piperidine protectant molecules and so they dissolve first. Small amounts of mesopores are then gradually generated in areas with more aluminum atoms and more piperidine protectant. In this manner, radial mesopores are formed in the ZSM-5 zeolite with a maximal preservation of the micropores and active sites. The optimal hierarchical ZSM-5 zeolite, prepared with a molar ratio of piperidine to zeolite of 0.03, had a mesopore surface area of 136 m ·g and a solid yield of 80%. The incorporation of the radial mesopores results in micropores that are interconnected which shortened the average diffusion path length. Compared to the parent zeolite, the hierarchical ZSM-5 zeolite possesses more accessible acid sites and has a higher catalytic activity and a longer lifetime for the alkylation of benzene.

关键词： hierarchical ZSM-5 zeolite     protective desilication     piperidine     radial mesopores     benzene alkylation    

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Effect of seawater salinity on the synthesis of zeolite from coal fly ash

Yanqing YU, Xiaoliang LI, Xiaolan ZOU, Xiaobin ZHU

《环境科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 54-61 doi: 10.1007/s11783-013-0493-4

摘要： A novel method for the synthesis of zeolite was developed in this paper. The synthesis was carried out by hydrothermal activation after alkali fusion and coal fly ash (CFA) was used as raw material with seawater of different salinities. Seawater salinity was varied from 32 to 88 for zeolite crystallization during the hydrothermal process. The results show that seawater salinity plays an important role in zeolite synthesis with CFA during hydrothermal treatment. The products were a mixture of NaX zeolite and hydroxysodalite; seawater salinity more strongly affected the crystallization than the type and chemical composition of the zeolites. The yield of CFA transformed into zeolite gradually rose with the increase in salinity, reaching a transformation rate of 48%–62% as the salinity increased from 32 to 88, respectively. The proposed method allows for the efficient disposal of by-products; therefore, the application of seawater in zeolite synthesis presents promising economic and ecological benefits.

关键词： coal fly ash (CFA)     seawater salinity     zeolite synthesis    

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Co-pyrolysis of sludge and kaolin/zeolite in a rotary kiln: Analysis of stabilizing heavy metals

《环境科学与工程前沿（英文）》 2022年 第16卷 第7期 doi: 10.1007/s11783-021-1488-1

摘要：

• Adding kaolin/zeolite promotes the formation of stable heavy metals.

关键词： Co-pyrolysis     Sewage sludge     Heavy metals     Rotary kiln     Immobilization mechanism    

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标题 作者 时间 类型 操作

Synthesis, characterization and catalytic properties of mesoporous MCM-48 containing zeolite secondary

LI Qiang, ZHANG Ying, DOU Tao, LI Yuping, WANG Shan, SUN Famin

期刊论文

Porous silica synthesis out of coal fly ash with no residue generation and complete silicon separation

期刊论文

Atomistic simulations for adsorption and separation of flue gas in MFI zeolite and MFI/MCM-41 micro/mesoporous

Shengchi ZHUO, Yongmin HUANG, Jun HU, Honglai LIU

期刊论文

Enhanced CuCl dispersion by regulating acidity of MCM-41 for catalytic oxycarbonylation of ethanol to

Pengzhen CHEN, Shouying HUANG, Jijie ZHANG, Shengping WANG, Xinbin MA

期刊论文

Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis

Shengping WANG, Changqing MA, Yun SHI, Xinbin MA

期刊论文

Factors affecting the formation of zeolite seed layers and the effects of seed layers on the growth ofzeolite silicalite-1 membranes

ZHANG Xiongfu, WANG Jinqu, LIU Hai′ou, WANG Anjie

期刊论文

Synthesis of nanofluids composed of deep eutectic solvents and metal-modified MCM-41 particles as multifunctional

期刊论文

CuO/zeolite catalyzed oxidation of gaseous toluene under microwave heating

Longli BO, Jianbo LIAO, Yucai ZHANG, Xiaohui WANG, Quan YANG

期刊论文

Effects of natural zeolite and sulfate ions on the mechanical properties and microstructure of plastic

期刊论文

Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO

Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI

期刊论文

Photocatalytic degradation of omethoate using NaY zeolite-supported TiO

Dishun ZHAO, Jialei WANG, Zhigang ZHANG, Juan ZHANG

期刊论文

Catalytic fast pyrolysis of Kraft lignin with HZSM-5 zeolite for producing aromatic hydrocarbons

Xiangyu LI, Lu SU, Yujue WANG, Yanqing YU, Chengwen WANG, Xiaoliang LI, Zhihua WANG

期刊论文

Hierarchical ZSM-5 zeolite with radial mesopores: Preparation, formation mechanism and application for

Darui Wang, Hongmin Sun, Wei Liu, Zhenhao Shen, Weimin Yang

期刊论文

Effect of seawater salinity on the synthesis of zeolite from coal fly ash

Yanqing YU, Xiaoliang LI, Xiaolan ZOU, Xiaobin ZHU

期刊论文

Co-pyrolysis of sludge and kaolin/zeolite in a rotary kiln: Analysis of stabilizing heavy metals

期刊论文