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期刊论文 49

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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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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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Effect of SiO

Qian WANG, Lei WANG, Hui WANG, Zengxi LI, Xiangping ZHANG, Suojiang ZHANG, Kebin ZHOU

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 79-88 doi: 10.1007/s11705-010-0550-5

摘要： A series of SAPO-34 molecular sieves with different SiO /Al O ratios have been synthesized for the methanol-to-olefin (MTO) reaction. Their physico-chemical properties are characterized by various techniques such as X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), Fourier transform infrared spectroscopy (FT-IR) and N adsorption-desorption. The results are compared with those of the commercial HZSM-5, which show that the crystallinity and particle diameter of SAPO-34 as well as HZSM-5 increase with SiO /Al O ratio. The variation of BET surface area of SAPO-34 is different from that of HZSM-5 and the sample with SiO /Al O ratio of 0.4 exhibits the highest BET surface area. FT-IR spectra indicate that HZSM-5 has both Br?nsted and Lewis acid sites and Br?nsted acid sites are stronger, whereas SAPO-34 samples are dominated only by Lewis acid sites. When the SiO /Al O ratio increases, propylene and butylenes become the predominant product of the MTO reaction over HZSM-5. In contrast, the main products of this reaction catalyzed by SAPO-34 are ethylene and propylene. According to the product distribution, the reaction mechanism over HZSM-5 catalysts is proposed.

关键词： HZSM-5     SAPO-34     methanol-to-olefin (MTO)     SiO2/Al2O3 ratio    

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Impacts of methanol fuel on vehicular emissions: A review

《环境科学与工程前沿（英文）》 2022年 第16卷 第9期 doi: 10.1007/s11783-022-1553-4

摘要：

● Methanol effectively reduces CO, HC, CO2, PM, and PN emissions of gasoline vehicles.

关键词： Methanol fuel     Vehicular emission     Emission reduction     Cleaner fuel     Gasoline substitute    

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生产低硫低烯烃汽油的RIDOS技术

李大东,石亚华,杨清雨

《中国工程科学》 2004年 第6卷 第4期   页码 1-8

摘要：

通过研究高烯烃含量FCC汽油的烃类组成和结构，针对性地开发了具有深度脱硫和烯烃饱和能力并减少辛烷值损失的RIDOS技术。RIDOS技术的多种功能是通过一系列新催化剂实现的，具有良好的原料适应性和操作稳定性。第一套RIDOS技术工业应用结果表明产品中硫的质量分数可小于10 μg/g，烯烃体积分数小于20％，抗爆指数损失仅1.3。RIDOS技术为生产满足更苛刻标准的汽油提供了可能。

关键词： FCC汽油     RIDOS     烯烃     硫     异构化    

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Confinement effects in methanol to olefins catalysed by zeolites: A computational review

German Sastre

《化学科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 76-89 doi: 10.1007/s11705-016-1557-3

摘要： Small pore zeolites, containing 8-rings as the largest, are widely employed as catalysts in the process of methanol-to-olefins (MTO). Reactants and products diffuse with constraints through 8-rings and this is one of the reaction bottlenecks related to zeolite micropore topology. Small pore zeolites and silicon-aluminophosphates(SAPOs) containing cavities, where olefins are mainly formed through the hydrocarbon pool (HP) mechanism, are frequently tested for MTO. Shape selectivity of transition states within the side-chain methylation will be reviewed as this is one of the controlling steps of the MTO process, with particular attention to the role of hexamethylbenzene (HMB) and heptamethylbenzenium cation (HeptaMB ), which are the most tipically detected reaction intermediates, common to the paring and side-chain routes within the HP mechanism. The relative stability of these and other species will be reviewed in terms of confinement effects in different cage-based zeolites. The role of the different alkylating agents, methanol, dimethyl ether (DME), and surface methoxy species (SMS) will also be reviewed from the computational viewpoint.

关键词： small pore zeolites     SAPOs     methanol-to-olefins     hydrocarbon pool mechanism     alkylation of polymethylbenzenes    

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Hydrogen production from methanol through dielectric barrier discharge

Baowei WANG, Xu ZHANG, Haiying BAI, Yijun Lü, Shuanghui HU

《化学科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 209-214 doi: 10.1007/s11705-010-1018-3

摘要： The hydrogen fuel cell is a promising option as a future energy resource and the production of hydrogen is mainly depended on fossil fuels now. In this paper, methanol reforming to produce H through dielectric-barrier discharge (DBD) plasma reaction was studied. Effects of the power supply parameters, reactor parameters and process conditions on conversion of methanol and distribution of products were investigated. The best reaction conditions were following: input power (45 W), material of inner electrode (stainless steel), discharge gap (3.40 mm), length of reaction zone (90.00 mm), dielectric thickness (1.25 mm), and methanol content (37.65%). The highest conversion of methanol and the yield of H were 82.38% and 27.43%, respectively.

关键词： methanol     dielectric-barrier discharge     hydrogen     plasma    

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Experimental study on premixed combustion of spherically propagating methanol-air-nitrogen flames

Xiangang WANG, Zhiyuan ZHANG, Zuohua HUANG, Xibin WANG, Haiyan MIAO,

《能源前沿（英文）》 2010年 第4卷 第2期   页码 223-233 doi: 10.1007/s11708-010-0016-y

摘要： The outward propagation and development of surface instability of the spark-ignited spherical premixed flames for methanol-air-nitrogen mixtures were experimentally studied by using a constant volume combustion chamber and a high-speed schlieren photography system. The laminar burning velocities, the mass burning fluxes, and the Markstein lengths were obtained at different equivalence ratios, dilution ratios, initial temperatures, and pressures. The laminar burning velocities and the mass burning fluxes give a similar curve versus the equivalence ratios. They increase with the increase of initial temperature and decrease with the increase of dilution ratio. The laminar burning velocity decreases with elevating the initial pressure, while the mass burning flux increases with the increase of the initial pressure. Markstein length decreases slightly with the increase of initial temperature for the rich mixtures. High initial pressure corresponds to low Markstein length. Markstein length increases with the increase of dilution ratio, which is more obvious when the mixture becomes leaner. Equivalence ratio has a slight impact on the development of the diffusive-thermal cellular structure at elevated initial pressures. The initial pressure has a significant influence on the occurrence of the flame front cellular structure. At the elevated pressures, the cracks on the flame surface branch and develop into the cell structure. These cells are bounded by cracks emitting a bright light, which may indicate soot formation. For very lean mixture combustion, the buoyancy effect and cooling effect from the spark electrodes have a significant impact on the flame propagation. The hydrodynamic instability, inhibited with the increase of initial temperature around the stoichiometric equivalence ratio, is enhanced with the increase of initial pressure and suppressed by mixture dilution.

关键词： methanol     spherical flame     propagation characteristics     flame instabilities    

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Mechanism of methanol decomposition on the Pd/WC(0001) surface unveiled by first-principles calculations

Jinhua Zhang, Yuanbin She

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 1052-1064 doi: 10.1007/s11705-019-1908-y

摘要： In this study, the decomposition of methanol into the CO and H species on the Pd/tungsten carbide (WC)(0001) surface is systematically investigated using periodic density functional theory (DFT) calculations. The possible reaction pathways and intermediates are determined. The results reveal that saturated molecules, i.e., methanol and formaldehyde, adsorb weakly on the Pd/WC(0001) surface. Both CO and H prefer three-fold sites, with adsorption energies of ‒1.51 and ‒2.67 eV, respectively. On the other hand, CH O stably binds at three-fold and bridge sites, with an adsorption energy of ‒2.58 eV. However, most of the other intermediates tend to adsorb to the surface with the carbon and oxygen atoms in their sp and hydroxyl-like configurations, respectively. Hence, the C atom of CH OH preferentially attaches to the top sites, CHOH and CH O adsorb at the bridge sites, while COH and CHO occupy the three-fold sites. The DFT calculations indicate that the rupture of the initial C–H bond promotes the decomposition of CH OH and CH OH, whereas in the case of CHOH, O–H bond scission is favored over the C–H bond rupture. Thus, the most probable methanol decomposition pathway on the Pd/WC(0001) surface is CH OH → CH OH → -CHOH → CHO → CO. The present study demonstrates that the synergistic effect of WC (as carrier) and Pd (as catalyst) alters the CH OH decomposition pathway and reduces the noble metal utilization.

关键词： density functional theory     methanol     direct methanol fuel cells     WC(0001)-supported Pd monolayer     decomposition mechanism    

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Calculation and analysis of sub/supercritical methanol preheating tube for continuous production of biodieselvia supercritical methanol transesterification

Wen CHEN, Weiyong YING, Cunwen WANG, Weiguo WANG, Yuanxin WU, Junfeng ZHANG,

《能源前沿（英文）》 2009年 第3卷 第4期   页码 423-431 doi: 10.1007/s11708-009-0075-0

摘要： Biodiesel is an important renewable energy. Supercritical methanol transesterification for biodiesel has recently been concerned because of its obvious advantages. The tubular reactor is an ideal reactor for continuous preparation of biodiesel via supercritical methanol transesterification. A methanol preheating tube is necessary for the tubular reaction system because the reaction temperature for supercritical methanol transesterification is usually 520―600K. Therefore, in the range of 298―600K, changes of the density, isobaric capacity, viscosity and thermal conductivity of sub/supercritical methanol with temperature are first discussed. Then on the basis of these thermophysical properties, an integration method is adopted for the design of sub/supercritical methanol preheating tube when methanol is preheated from 298K to 600K at 16MPa and the influencing factors on the length of the preheating tube are also studied. The computational results show that the Reynolds number and the local convection heat-transfer coefficient of sub/supercritical methanol flowing in ф6mm×1.5mm preheating tube change drastically with temperature. For the local overall heat transfer coefficient and the average overall heat transfer coefficient , temperature also has an important influence on them when the inlet velocity of methanol is lower than 0.5m/s. But when the inlet velocity of methanol is higher than 0.5m/s, and almost keep invariable with temperature. Additionally, both the outlet temperature and the inlet velocity of methanol are the key affecting factors for the length of the preheating tube, especially when the outlet temperature is over the critical temperature of methanol. At the same time, the increase of tin bath’s temperature can shorten the required length of the preheating tube. At the inlet flow rate of 0.5m/s, the required length of the preheating tube is 2.0m when methanol is preheated from 298K to 590K at 16MPa with keeping the tin bath’s temperature 620K, which is in good agreement with the experimental results.

关键词： sub/supercritical methanol     preheating tube     integration method     biodiesel    

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烯烃生产新趋势

Ismaël Amghizar,Laurien A. Vandewalle,Kevin M. Van Geem,Guy B. Marin

《工程（英文）》 2017年 第3卷 第2期   页码 171-178 doi: 10.1016/J.ENG.2017.02.006

摘要：

在未来10 年内，蒸汽裂解仍将是主要的烯烃( 如乙烯和丙烯) 生产方式。由于日用品市场较大的不确定性，尽管原油储量下降和全球变暖在定程度上制约了裂解工艺，但其他替代技术和原料因为较低的经济可行，尚无法在化学工业界得到足够的投资。本文将些最有潜力的替代术与传统的蒸汽裂解工艺进行了对比，着重强调了这些替代术的主要瓶颈。部分上述工艺主要得益于页岩气和闲置天然气中大量廉价的丙烷乙烷和甲烷。从经济的角度来看，以甲烷为原料生产化工产品的路线如果行得，其经济效益将会十分显著原油的巨大储量以及未来市场对燃料需求下跌的预期则表明，些拥有成熟路线的工艺如费托合成或甲醇制汽油的前景并不光明。另方面，丰富廉价的乙烷和储量巨大的原油导致了蒸汽裂解工艺两极分化的趋势，这也给低碳烯烃的定向生产工艺，如丙烷催化脱氢，创了空间。

关键词： 烯烃生产     蒸汽裂解     甲烷转化     页岩气     碳排放    

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Co-conversion of methanol and

Shumei Wei, Yarong Xu, Zhaoyang Jin, Xuedong Zhu

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 783-792 doi: 10.1007/s11705-019-1868-2

摘要： The conversion of -hexane and methanol into value-added aromatic compounds is a promising method for their industrially relevant utilization. In this study, intergrown ZSM-5/ZSM-11 crystals were synthesized and their resulting catalytic performance was investigated and compared to those of the isolated ZSM-5 and ZSM-11 zeolites. The physicochemical properties of ZSM-5/ZSM-11 intergrown zeolite were analyzed using X-ray diffraction, N isothermal adsorption-desorption, the temperature-programmed desorption of ammonium, scanning electron microscopy, Fourier transform infrared spectra of adsorbed pyridine, and nuclear magnetic resonance of Al , and compared with those of the ZSM-5 and ZSM-11 zeolites. The catalytic performances of the materials were evaluated during the co-feeding reaction of methanol and -hexane under the fixed bed conditions of 400°C, 0.5 MPa (N ), methanol꞉ -hexane= 7꞉3 (mass ratio), and weight hourly space velocity= 1 h (methanol). Compared to the ZSM-5 and ZSM-11 zeolites, the ZSM-5/ZSM-11 zeolite exhibited the largest specific surface area, a unique crystal structure, moderate acidity, and suitable Brønsted/Lewis acid ratio. The evaluation results showed that ZSM-5/ZSM-11 catalyst exhibited better catalytic reactivity than the ZSM-5 and ZSM-11 catalysts in terms of methanol conversion rate, -hexane conversion rate, and aromatic selectivity. The outstanding catalytic property of the intergrown ZSM-5/ZSM-11 was attributed to the enhanced diffusion associated with its unique crystal structure. The benefit of using zeolite intergrowth in the co-conversion of methanol and alkanes offers a novel route for future catalyst development.

关键词： ZSM-5/ZSM-11     methanol     n-hexane     cofeeding     aromatics    

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Design and analysis of dual fuel methanol-power poly-generation

Minghua WANG , Zheng LI , Weidou NI ,

《能源前沿（英文）》 2009年 第3卷 第3期   页码 341-347 doi: 10.1007/s11708-009-0023-z

摘要： A dual fuel head poly-generation flowsheet was designed based on coal gas and coke oven gas. To help clearly understand the system performance, a 1.2×10−3.2×10kg methanol and 274―496MW power poly-generation system was simulated by using the commercially available software ASPEN Plus and GT Pro. The technology scheme, the operating parameters, and the efficiency of the system were also analyzed and evaluated, which will be used for building industrial devices.

关键词： dual fuel     methanol-power poly-generation     CO2 and CH4 reforming     splitting ratio    

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Sensitivity analysis of a methanol and power polygeneration system fueled with coke oven gas and coal

Guoqiang ZHANG, Lin GAO, Hongguang JIN, Rumou LIN, Sheng LI

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 491-497 doi: 10.1007/s11705-010-0511-z

摘要： The sensitivity analysis of a polygeneration energy system fueled with duo fuel of coke oven gas and coal gas is performed in the study, and the focus is put on the relations among syngas composition, conversation rate and performance. The impacts of the system configuration together with the fuel composition on the performance are investigated and discussed from the point of cascading utilization of fuel chemical energy. First, the main parameters affecting the performance are derived along with the analysis of the system configuration and the syngas composition. After the performance is being simulated by means of the Aspen Plus process simulator of version 11.1, the variation of the performance due to the composition of syngas and the conversion rate of chemical subsystem is obtained and discussed. It is obtained from the result that the proper conversion rate of the chemical subsystem according to the specific syngas composition results in better performance. And the syngas composition affects the optimal conversion rate of the chemical subsystem, the optimal point of which is around the stoichiometric composition for methanol production (CO/H = 0.5). In all, the polygeneration system fueled with coke oven gas and coal gas, which can realize the reasonable conversion of syngas to power and chemical product according to the syngas composition, is a promising method for coal energy conversion and utilization.

关键词： duo fuel of coke oven gas and coal gas     polygeneration of power and methanol     sensitivity analysis     the relation among energy utilization     syngas composition and chemical conversion rate    

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An efficient technique for improving methanol yield using dual CO

Yang Su, Liping Lü, Weifeng Shen, Shun’an Wei

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 614-628 doi: 10.1007/s11705-019-1849-5

摘要： Abstract Steam methane reforming (SMR)-based methanol synthesis plants utilizing a single CO2 feed represent one of the predominant technologies for improving methanol yield and CO2 utilization. However, SMR alone cannot achieve full CO2 utilization, and a high water content accumulates if CO2 is only fed into the methanol reactor. In this study, a process integrating SMR with dry methane reforming to improve the conversion of both methane and CO2 is proposed. We also propose an innovative methanol production approach in which captured CO2 is introduced into both the SMR process and the recycle gas of the methanol synthesis loop. This dual CO2 feed approach aims to optimize the stoichiometric ratio of the reactants. Comparative evaluations are carried out from a techno-economic point of view, and the proposed process is demonstrated to be more efficient in terms of both methanol productivity and CO2 utilization than the existing stand-alone natural gas-based methanol process.

关键词： methanol synthesis     CO2 utilization     dry methane reforming     steam methane reforming     process design    

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标题 作者 时间 类型 操作

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

Mehdi SEDIGHI,Kamyar KEYVANLOO

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

Effect of SiO

Qian WANG, Lei WANG, Hui WANG, Zengxi LI, Xiangping ZHANG, Suojiang ZHANG, Kebin ZHOU

期刊论文

Impacts of methanol fuel on vehicular emissions: A review

期刊论文

生产低硫低烯烃汽油的RIDOS技术

李大东,石亚华,杨清雨

期刊论文

Confinement effects in methanol to olefins catalysed by zeolites: A computational review

German Sastre

期刊论文

Hydrogen production from methanol through dielectric barrier discharge

Baowei WANG, Xu ZHANG, Haiying BAI, Yijun Lü, Shuanghui HU

期刊论文

Experimental study on premixed combustion of spherically propagating methanol-air-nitrogen flames

Xiangang WANG, Zhiyuan ZHANG, Zuohua HUANG, Xibin WANG, Haiyan MIAO,

期刊论文

Mechanism of methanol decomposition on the Pd/WC(0001) surface unveiled by first-principles calculations

Jinhua Zhang, Yuanbin She

期刊论文

Calculation and analysis of sub/supercritical methanol preheating tube for continuous production of biodieselvia supercritical methanol transesterification

Wen CHEN, Weiyong YING, Cunwen WANG, Weiguo WANG, Yuanxin WU, Junfeng ZHANG,

期刊论文

烯烃生产新趋势

Ismaël Amghizar,Laurien A. Vandewalle,Kevin M. Van Geem,Guy B. Marin

期刊论文

Co-conversion of methanol and

Shumei Wei, Yarong Xu, Zhaoyang Jin, Xuedong Zhu

期刊论文

Design and analysis of dual fuel methanol-power poly-generation

Minghua WANG , Zheng LI , Weidou NI ,

期刊论文

Sensitivity analysis of a methanol and power polygeneration system fueled with coke oven gas and coal

Guoqiang ZHANG, Lin GAO, Hongguang JIN, Rumou LIN, Sheng LI

期刊论文

An efficient technique for improving methanol yield using dual CO

Yang Su, Liping Lü, Weifeng Shen, Shun’an Wei

期刊论文