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Novel method for the preparation of Cs-containing FAU(Y) catalysts for aniline methylation

Olga A. Ponomareva, Polina A. Shaposhnik, Marina V. Belova, Boris A. Kolozhvari, Irina I. Ivanova

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 70-76 doi: 10.1007/s11705-017-1694-3

摘要： Cs-containing FAU(Y)-type zeolite catalysts were prepared by conventional and novel ion exchange procedures followed by incipient wetness impregnation with CsOH. The novel ion exchange procedure involved hydrothermal treatment of NaY zeolite in aqueous solution of CsCl at 140–200 °C for 6–24 h. The samples were characterized by low-temperature nitrogen adsorption, X-ray fluorescence analysis, X-ray powder diffraction, scanning electron microscopy, Na, Al and Cs magic angle spinning nuclear magnetic resonance, CO and NH -Temperature programmed desorption. The results show that hydrothermal treatment at 200 °C allows to obtain higher degrees of ion-exchange (up to 83%) with respect to conventional method giving maximum 66%–69%. Catalytic properties of Cs-containing FAU(Y) were studied in aniline methylation. The yield of -methylaniline is shown to correlate with catalyst’s basicity. The best catalyst performance was achieved over the catalyst with the highest ion-exchange degree impregnated with CsOH. The selectivity to -methylaniline over this catalyst reached 96.4%.

关键词： FAU(Y) zeolite     ion exchange with cesium     aniline alkylation     N-methylaniline    

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Layer-like FAU-type zeolites: A comparative view on different preparation routes

Bastian Reiprich, Tobias Weissenberger, Wilhelm Schwieger, Alexandra Inayat

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 127-142 doi: 10.1007/s11705-019-1883-3

摘要： The creation of intergrown layer-like zeolite crystals is one route to form hierarchical zeolites. Faujasite-type (FAU-type) zeolites are among the industrially most important zeolites and the implementation of hierarchical porosity is a promising way to optimise their catalytic and adsorptive performance. After a short general survey into routes for the preparation of hierarchical pore systems in FAU, we will review the currently existing strategies for the synthesis of FAU with layer-like morphology. Those strategies are mainly based on the presence of morphology modifying agents in the synthesis mixture. However, a very recent approach is the synthesis of layer-like FAU-type zeolite crystals assembled in an intergrown manner in the absence of such additives, just by finely adjusting the crystallization temperature. This additive-free preparation route for layer-like FAU, which appears very attractive from an ecological as well as economic point of view, is highlighted in this review. Concluding, a comparison, including powder X-ray diffraction, scanning and transmission electron microscopy, nitrogen physisorption and elemental analysis, between conventional FAU and three layer-like FAU obtained by different synthesis routes was carried out to show the structural, morphological and textural differences and similarities of these materials.

关键词： FAU     hierarchical zeolite     layer-like morphology    

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Biodiesel production from waste frying oil in sub- and supercritical methanol on a zeolite Y solid acid

Jorge MEDINA-VALTIERRA, Jorge RAMIREZ-ORTIZ

《化学科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 401-407 doi: 10.1007/s11705-013-1354-1

摘要： Waste frying oil (WFO) is a very important feedstock for obtaining biodiesel at low cost and using WFO in transesterification reactions to produce biodiesel helps eliminate local environmental problems. In this study biodiesel was produced from WFO in sub- and super-critical methanol on a zeolite Y solid acid catalyst. The procedure was optimized using a design of experiments by varying the methanol to WFO molar ratio, the reaction temperature, and the amount of catalyst. Typical biodiesel yields varied from 83 to nearly 100% with methyl esters content ranging from 1.41–1.66 mol·L and typical dynamic viscosities of 22.1-8.2 cP. Gas chromatography was used to determine the molecular composition of the biodiesel. The reaction products contained over 82 wt-% methyl esters, 4.2 wt-% free acids, 13.5 wt-% monoglycerides, and 0.3 wt-% diglycerides. The transesterification of WFO with methanol around its critical temperature combined with a zeolite Y as an acid catalyst is an efficient approach for the production of biodiesel with acceptable yields.

关键词： biodiesel     methanol     critical temperature     waste frying oil     zeolite Y    

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Using ultrasound to improve the sequential post-synthesis modification method for making mesoporous Y

Rongxin Zhang, Peinan Zhong, Hamidreza Arandiyan, Yanan Guan, Jinmin Liu, Na Wang, Yilai Jiao, Xiaolei Fan

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 275-287 doi: 10.1007/s11705-019-1905-1

摘要： Mesoporous Y zeolites were prepared by the sequential chemical dealumination (using chelating agents such as ethylenediaminetetraacetic acid, H EDTA, and citric acid aqueous solutions) and alkaline desilication (using sodium hydroxide, NaOH, aqueous solutions) treatments. Specifically, the ultrasound-assisted alkaline treatment (i.e., ultrasonic treatment) was proposed as the alternative to conventional alkaline treatments which are performed under hydrothermal conditions. In comparison with the hydrothermal alkaline treatment, the ultrasonic treatment showed the comparatively enhanced efficiency (with the reduced treatment time, i.e., 5 min vs. 30 min, all with 0.2 mol·L NaOH at 65°C) in treating the dealuminated Y zeolites for creating mesoporosity. For example, after the treatment of a dealuminated zeolite Y (using 0.1 mol·L H EDTA at 100°C for 6 h), the ultrasonic treatment produced the mesoporous zeolite Y with the specific external surface area ( ) of 160 m ·g and mesopore volume ( ) of 0.22 cm ·g , being slightly higher than that by the conventional method (i.e., = 128 m ·g and = 0.19 cm ·g ). The acidic property and catalytic activity (in catalytic cracking of -octane) of mesoporous Y zeolites obtained by the two methods were comparable. The ultrasonic desilication treatment was found to be generic, also being effective to treat the dealuminated Y zeolites by citric acid. Additionally, the first step of chemical dealumination treatment was crucial to enable the effective creation of mesopores in the parent Y zeolite (with a silicon-to-aluminium ratio, Si/Al= 2.6) regardless of the subsequent alkaline desilication treatment (i.e., ultrasonic or hydrothermal). Therefore, appropriate selection of the condition of the chemical dealumination treatment based on the property of parent zeolites, such as Si/Al ratio and crystallinity, is important for making mesoporous zeolites effectively.

关键词： zeolite Y     mesoporous zeolite     post-synthesis treatment     ultrasound     chemical dealumination treatment     alkaline desilication treatment    

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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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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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Phosphorous removal from wastewater by lanthanum modified Y zeolites

Weikang ZHANG, Ye TIAN

《化学科学与工程前沿（英文）》 2015年 第9卷 第2期   页码 209-215 doi: 10.1007/s11705-014-1448-4

摘要： The adsorption capacities of Y zeolite and La (III)-modified Y zeolite were studied. A series of La(III)-modified Y zeolites with different La/Y zeolite mass ratios were characterized by X-ray diffraction, X-ray fluorescence and Brunauer-Emmett-Teller surface area analysis. Batch experiments were conducted to evaluate the effects of various experimental parameters, such as pH, ionic strength, coexisting anions ( , Cl , and ) and temperature, on the phosphate adsorption. The capacity of the La (III)-modified Y zeolite to remove phosphate increased as the La/Y zeolite mass ratio increased and after 4 h, a phosphate removal efficiency of 95% was achieved for a La/Y zeolite mass ratio of 0.10. The equilibrium adsorption isotherm data correlated better to the Langmuir model than the Freundlich model and the data followed a pseudo-second-order kinetic equation.

关键词： phosphate removal     wastewater     lanthanum     impregnation     Y zeolites    

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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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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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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

Novel method for the preparation of Cs-containing FAU(Y) catalysts for aniline methylation

Olga A. Ponomareva, Polina A. Shaposhnik, Marina V. Belova, Boris A. Kolozhvari, Irina I. Ivanova

期刊论文

Layer-like FAU-type zeolites: A comparative view on different preparation routes

Bastian Reiprich, Tobias Weissenberger, Wilhelm Schwieger, Alexandra Inayat

期刊论文

Biodiesel production from waste frying oil in sub- and supercritical methanol on a zeolite Y solid acid

Jorge MEDINA-VALTIERRA, Jorge RAMIREZ-ORTIZ

期刊论文

Using ultrasound to improve the sequential post-synthesis modification method for making mesoporous Y

Rongxin Zhang, Peinan Zhong, Hamidreza Arandiyan, Yanan Guan, Jinmin Liu, Na Wang, Yilai Jiao, Xiaolei Fan

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

CuO/zeolite catalyzed oxidation of gaseous toluene under microwave heating

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

期刊论文

Phosphorous removal from wastewater by lanthanum modified Y zeolites

Weikang ZHANG, Ye TIAN

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

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

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