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The synergic effects of highly selective bimetallic Pt-Pd/SAPO-41 catalysts for the

Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1111-1124 doi: 10.1007/s11705-020-2031-9

摘要： The hydroisomerization of -hexadecane over Pt-Pd bimetallic catalysts is an effective way to produce clean fuel oil. This work reports a useful preparation method of bimetallic bifunctional catalysts by a co-impregnation or sequential impregnation process. Furthermore, monometallic catalysts with loading either Pt or Pd are also prepared for comparison. The effects of the metal species and impregnation order on the characteristics and catalytic performance of the catalysts are investigated. The catalytic test results indicate that the maximum -hexadecane yield over different catalysts increases as follows: Pt/silicoaluminophosphate SAPO-41

关键词： SAPO-41 molecular sieve     Pt-Pd bimetallic site     bifunctional catalysts     n-hexadecane     hydroisomerization    

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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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Preparation and characterization of novel carbon molecular sieve membrane/PSSF composite by pyrolysis

Ying Yan, Peng Huang, Huiping Zhang

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 772-783 doi: 10.1007/s11705-019-1827-y

摘要： Carbon molecular sieve membrane (CMSM)/paper-like stainless steel fibers (PSSF) has been manufactured by pyrolyzing poly (furfuryl alcohol) (PFA) coated on the metal fibers. PFA was synthesized using oxalic acid dihydrate as a catalyst and coated on microfibers by dip coating method. For the purpose of investigating the effects of final carbonization temperature, the composites were carbonized between 400°C and 800°C under flowing nitrogen. The morphology and microstructure were examined by X-ray diffraction, Fourier transforms infrared spectroscopy, scanning electron microscopy, thermogravimetric analysis, N adsorption and desorption, Raman spectra and X-ray photoelectron spectra. The consequences of characterization showed that the CMSM containing mesopores of 3.9 nm were manufactured. The specific surface area of the CMSM/PSSF fabricated in different pyrolysis temperature varies from 26.5 to 169.1 m ∙g and pore volume varies from 0.06 to 0.23 cm ∙g . When pyrolysis temperature exceeds 600°C, the specific surface, pore diameter and pore volume decreased as carbonization temperature increased. Besides, the degree of graphitization in carbon matrix increased with rising pyrolysis temperature. Toluene adsorption experiments on different structured fixed bed that was padded by CMSM/PSSF and granular activated carbon (GAC) were conducted. For the sake of comparison, adsorption test was also performed on fixed bed packed with GAC. The experimental results indicated that the rate constant ′ was dramatically increased as the proportion of CMCM/PSSF composites increased on the basis of Yoon-Nelson model, which suggested that structured fixed bed padded with CMSM/PSSF composite offered higher adsorption rate and mass transfer efficiency.

关键词： carbon molecular sieve membrane     stainless steel fibers     pyrolysis     structured fixed bed     toluene    

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Thermal decomposition of poly(ethylene terephthalate)/mesoporous molecular sieve composites

RUN Mingtao, ZHANG Dayu, WU Sizhu, WU Gang

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 50-54 doi: 10.1007/s11705-007-0010-z

摘要： The nonisothermal and isothermal degradation processes of poly (ethylene terephthalate)/mesoporous molecular sieve (PET/MMS) composites synthesized by in-situ polymerization were studied by using thermogravimetric analysis in nitrogen. The nonisothermal degradation of the composite is found to be the first-order reaction. An iso-conversional procedure developed by Ozawa is used to calculate the apparent activation energy (), which is an average value of about 260 kJ/mol with the weight conversion from 0% to 30%, and is higher than that of neat PET. Isothermal degradation results are confirmed with the nonisothermal process, in which PET/MMS showed higher thermal stability than neat PET. The polymer in mesoporous channels has more stability due to the protection of the inorganic pore-wall. These results indicate that mesoporous MMS in PET/MMS composites improve the stability of the polymer.

关键词： polymerization     isothermal degradation     conversion     nonisothermal degradation     activation    

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Effects of the SAPO-11 synthetic process on dehydration of ethanol to ethylene

Lina WU, Xiaoxing SHI, Qun CUI, Haiyan WANG, He HUANG

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 60-66 doi: 10.1007/s11705-010-0540-7

摘要： The effects of the synthetic condition of SAPO-11 molecular sieves on ethanol dehydration to ethylene were studied. Product-compositions, ethanol conversion, and selectivity to ethylene of synthesized and commercial SAPO-11 molecular sieves were compared. Results are as follows: the optimal synthetic conditions for SAPO-11 molecular sieves are adding pseudoboehmite before orthophoshporic, using di-n- propylamine as the template, having a mass fraction of 40% colloidal silica as the silica source and the starting gel obtained, and running at 200°C for 48 h. From the patterns of NH -TPD, the amount of acid synthesized by SAPO-11 molecular sieves is less than that by commercial SAPO-11 molecular sieves, and has a stronger weak acid. Also, ethanol conversion and selectivity to ethylene reached 99% at 280°C on synthesized SAPO-11, lower by 20°C compared to commercial SAPO-11. For two SAPO-11 molecular sieves, the by-products in the gas phase are mainly ethane, propane, propene, isobutane, n-butane, propadiene, butylene and some higher hydrocarbons. The by-products in the liquid phase are ethyl ether and acetaldehyde.

关键词： SAPO-11 molecular sieves     synthesis     ethanol     ethylene     dehydration    

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Kinetic study of the methanol to olefin process on a SAPO-34 catalyst

Mehdi SEDIGHI,Kamyar KEYVANLOO

《化学科学与工程前沿（英文）》 2014年 第8卷 第3期   页码 306-311 doi: 10.1007/s11705-014-1440-z

摘要： In this paper, a new kinetic model for methanol to olefin process over SAPO-34 catalyst was developed using elementary step level. The kinetic model fits well to the experimental data obtained in a fixed bed reactor. Using this kinetic model, the effect of the most important operating conditions such as temperature, pressure and methanol space-time on the product distribution has been examined. It is shown that the temperature ranges between 400 °C and 450 °C is appropriate for propene production while the medium temperature (450 °C) is favorable for total olefin yield which is equal to 33%. Increasing the reactor pressure decreases the ethylene yield, while medium pressure is favorable for the propylene yield. The result shows that the ethylene and propylene and consequently the yield of total olefins increase to approximately 35% with decreasing the molar ratio of inlet water to methanol.

关键词： methanol to olefin     SAPO-34     kinetic modeling     elementary step    

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Preparation of lithium ion-sieve and utilizing in recovery of lithium from seawater

Lu WANG, Changgong MENG, Wei MA

《化学科学与工程前沿（英文）》 2009年 第3卷 第1期   页码 65-67 doi: 10.1007/s11705-009-0105-9

摘要： Lithium is one of the most important light metals, which is widely used as raw materials for large-capacity rechargeable batteries, light aircraft alloys and nuclear fusion fuel. Seawater, which contains 250 billion tons of lithium in total, has thus recently been noticed as a possible resource of lithium. While, since the average concentration of lithium in seawater is quite low (0.17 mg·L ), enriching it to an adequate high density becomes the primary step for industrial applications. The adsorption method is the most prospective technology for increasing the concentration of lithium in liquid. Among the adsorbents for lithium, the ion-sieve is a kind of special absorbent which has high selectivity for Li , especially the spinel manganese oxides (SMO), which among the series of ion-sieves, has become the most promising adsorption material for lithium. In this study, the SMO ion-sieve was prepared by a coprecipitation method. The preparation conditions were discussed and the sample characters were analyzed. Recovery of Li from seawater were studied in batch experiments using prepared ion-sieve, and the effect of solution pH and the uptake rates were also investigated in different Li solutions.

关键词： lithium     ion-sieve     seawater     spinel manganese oxide    

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Oxidation-extraction desulfurization of model oil over Zr-ZSM-5/SBA-15 and kinetic study

Chuanzhu LU,Hui FU,Huipeng LI,Hua ZHAO,Tianfeng CAI

《化学科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 203-211 doi: 10.1007/s11705-014-1420-3

摘要： ZSM-5/SBA-15 composite molecular sieves were synthesized using post-synthesis method and characterized by X-ray diffraction and N adsorption-desorption. The oxidative-extration desulfurization of model oil was investigated by using hydrogen peroxide as the oxidant, tetrabutyl ammonium bromide as phase transfer catalyst, dimethyl sulfoxide as extractant, and Zr-ZSM-5/SBA-15, Ag-ZSM-5/SBA-15, Ce-ZSM-5/SBA-15 as catalyst. Under the optimal conditions, the desulfurization rate decreases in the order: Zr-ZSM-5/SBA-15>Ce-ZSM-5/SBA-15>Ag-ZSM-5/SBA-15. The highest desulfurization rate is 84.53% under the catalysis of Zr-ZSM-5/SBA-15. Kinetics analysis shows that the reaction is pseudo-first-order with the activation energy of 44.23 kJ/mol.

关键词： composite molecular sieve     oxidation desulfuration     extraction     kinetic    

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Effect of temperature in the conversion of methanol to olefins (MTO) using an extruded SAPO-34 catalyst

Ignacio Jorge Castellanos-Beltran, Gnouyaro Palla Assima, Jean-Michel Lavoie

《化学科学与工程前沿（英文）》 2018年 第12卷 第2期   页码 226-238 doi: 10.1007/s11705-018-1709-8

摘要： The methanol-to-olefin (MTO) reaction was investigated in a bench-scale, fixed-bed reactor using an extruded catalyst composed of a commercial SAPO-34 (65 weight percentage, wt-%) embedded in an amorphous SiO matrix (35 wt-%). The texture properties, acidity and crystal structure of the pure SAPO-34 and its extruded form (E-SAPO-34) were analyzed and results indicated that the extrusion step did not affect the properties of the catalyst. Subsequently, E-SAPO-34 was tested in a temperature range between 300 and 500 °C, using an aqueous methanol mixture (80 wt-% water content) fed at a weight hour space velocity (WHSV) of 1.21 h . At 300 °C, a low conversion was observed combined with catalyst deactivation, which was ascribed to oligomerization and condensation reactions. The coke analysis showed the presence of diamandoid hydrocarbons, which are known to be inactive molecules in the MTO process. At higher temperatures, a quasi-steady state was reached during a 6 h reaction where the optimal temperature was identified at 450 °C, which incidentally led to the lowest coke deposition combined with the highest H/C ratio. Above 450 °C, surges of ethylene and methane were associated to a combination of H-transfer and protolytic cracking reactions. Finally, the present work underscored the convenience of the extrusion technique for testing catalysts at simulated scale-up conditions.

关键词： MTO     SAPO-34     temperature     extrusion     coke     light alkanes    

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Promotional effect of ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

《环境科学与工程前沿（英文）》 2021年 第15卷 第2期 doi: 10.1007/s11783-020-1322-1

摘要： Abstract • K+ hinder the structural degradation of Cu/SAPO-34 under humid condition<100°C. • K+ on Cu/SAPO-34 brings lower acidity and inferior SCR activity at high temperature. • Fe/Beta was used to compensate the low activity of Cu/SAPO-34 at high temperature. • The hybrid catalysts with KCu/SAPO-34 and Fe/Beta show a great potential for using. K ions were introduced onto Cu/SAPO-34 catalysts via the ion-exchange process in order to improve their stability under low-temperature hydrothermal aging. The changes in structure and copper-species contents of these catalysts upon hydrothermal aging were probed in order to investigate their effects on selective catalytic reduction (SCR) activity. For the fresh Cu/SAPO-34 catalysts, K ions had little influence on the chabazite framework but effected their acidities by exchanging with acid sites. After hydrothermal aging, the structural integrity and amount of active sites decreased on pure Cu/SAPO-34. While the K-loaded catalysts showed improved chabazite structure, acidity, and active site conservation with increasing K loading. However, although the 0.7 wt% K catalyst maintained the same crystallinity, active site abundance, and low-temperature SCR activity as the fresh catalyst upon aging, an apparent decrease in SCR activity at high temperature was observed because of the inevitable decrease in the number of Brönsted acid sites. To compensate for the activity disadvantage of K-loaded Cu/SAPO-34 at high temperature, Fe/Beta catalysts were co-employed with K-loaded Cu/SAPO-34, and a wide active temperature window of SCR activity was obtained. Thus, our study reveals that a combined system comprising Fe/Beta and K-loaded Cu/SAPO-34 catalysts shows promise for the elimination of NOx in real-world applications.

关键词： Selective catalytic reduction     Cu/SAPO-34 catalyst     Ion-exchanged K     Low-temperature hydrothermal stability     Fe/Beta catalyst    

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Catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over the

Zhidan Fu, Lisha Liu, Yong Song, Qing Ye, Shuiyuan Cheng, Tianfang Kang, Hongxing Dai

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 185-196 doi: 10.1007/s11705-017-1631-5

摘要： The Pd catalyst supported on cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) were prepared. The effect of Pd loading on the catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over Pd/OMS-2 has been investigated. The results show that the Pd loading plays an important role on the physicochemical properties of the Pd/OMS-2 catalysts which outperform the Pd-free counterpart with the 0.5Pd/OMS-2 catalyst being the best. The temperature for 50% conversion was 25, 240 and 160 °C, and the temperature for 90% conversion was 55, 285 and 200 °C for oxidation of CO, toluene, and ethyl acetate, respectively. The low-temperature reducibility and high oxygen mobility of Pd/OMS-2 are the factors contributable to the excellent catalytic performance of 0.5Pd/OMS-2.

关键词： cryptomelane-type manganese oxide octahedral molecular sieve     oxygen mobility     reducibility     carbon monoxide oxidation     volatile organic compound combustion    

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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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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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High-precision diffusion measurement of ethane and propane over SAPO-34 zeolites for methanol-to-olefin

Dali Cai, Yu Cui, Zhao Jia, Yao Wang, Fei Wei

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 77-82 doi: 10.1007/s11705-017-1684-5

摘要： The methanol-to-olefin (MTO) process has attracted much attention and many problems including lifetime and selectivity of light olefins have all been connected to the diffusion problems in zeolite crystals. However, a quantitative study of diffusion problems in SAPO-34 zeolites is lacking. In this paper, we performed a high-precision diffusion measurement of the diffusion behavior of ethane and propane, which represent ethylene and propylene respectively, over SAPO-34. The diffusions of ethane and propane over fresh and coked SAPO-34 zeolites with different crystal sizes were carefully studied. Ethane and propane show different diffusion behavior in SAPO-34. The diffusion of ethane is almost not influenced by the crystal size and coke percentage, whereas that of propane is strongly affected. A slower diffusion velocity was observed in bigger crystals, and the diffusion velocity decline significantly with the coke percentage increasing. The diffusion coefficient was calculated with both the internal and surface diffusion models, and the results show that the surface diffusion plays a key role in the diffusion process of both ethane and propane. We believe that this work would be helpful for understanding the diffusion of different molecules in SAPO-34 zeolites, and may lay the foundation of MTO research.

关键词： diffusion measurement     methanol-to-olefin process    

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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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标题 作者 时间 类型 操作

The synergic effects of highly selective bimetallic Pt-Pd/SAPO-41 catalysts for the

Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu

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

Preparation and characterization of novel carbon molecular sieve membrane/PSSF composite by pyrolysis

Ying Yan, Peng Huang, Huiping Zhang

期刊论文

Thermal decomposition of poly(ethylene terephthalate)/mesoporous molecular sieve composites

RUN Mingtao, ZHANG Dayu, WU Sizhu, WU Gang

期刊论文

Effects of the SAPO-11 synthetic process on dehydration of ethanol to ethylene

Lina WU, Xiaoxing SHI, Qun CUI, Haiyan WANG, He HUANG

期刊论文

Kinetic study of the methanol to olefin process on a SAPO-34 catalyst

Mehdi SEDIGHI,Kamyar KEYVANLOO

期刊论文

Preparation of lithium ion-sieve and utilizing in recovery of lithium from seawater

Lu WANG, Changgong MENG, Wei MA

期刊论文

Oxidation-extraction desulfurization of model oil over Zr-ZSM-5/SBA-15 and kinetic study

Chuanzhu LU,Hui FU,Huipeng LI,Hua ZHAO,Tianfeng CAI

期刊论文

Effect of temperature in the conversion of methanol to olefins (MTO) using an extruded SAPO-34 catalyst

Ignacio Jorge Castellanos-Beltran, Gnouyaro Palla Assima, Jean-Michel Lavoie

期刊论文

Promotional effect of ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

期刊论文

Catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over the

Zhidan Fu, Lisha Liu, Yong Song, Qing Ye, Shuiyuan Cheng, Tianfang Kang, Hongxing Dai

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

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

期刊论文

High-precision diffusion measurement of ethane and propane over SAPO-34 zeolites for methanol-to-olefin

Dali Cai, Yu Cui, Zhao Jia, Yao Wang, Fei Wei

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