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Modified iron-molybdate catalysts with various metal oxides by a mechanochemical method: enhanced formaldehydeyield in methanol partial oxidation

Xue Liu, Lingtao Kong, Shengtao Xu, Chaofan Liu, Fengyun Ma

《化学科学与工程前沿(英文)》 2021年 第15卷 第5期   页码 1099-1110 doi: 10.1007/s11705-020-2008-8

摘要: A mechanochemical method was employed to prepare modified iron molybdate catalysts with various metal salts as precursors. The physicochemical properties of the iron molybdate catalysts were characterized, and their performances in catalyzing the reaction from methanol to formaldehyde (HCHO) were evaluated. Iron molybdate catalysts doped with Co(NO ) ·6H O and Al(NO ) ·9H O resulted in high HCHO yields. Compared with a commercial catalyst, the HCHO yields in the reaction with the modified catalyst at an optimal Co/Mo molar ratio reached 97.37%. According to chemical state analysis, the formation of CoO and the efficient decrease in the MoO sublimation rate could be important factors enhancing the HCHO yield in reactions catalyzed with iron molybdate doped with different Co/Mo mole ratios.

关键词: iron molybdate catalyst     metal oxides     methanol to formaldehyde     Co/Mo ratio     formaldehyde yield    

Catalytic activities and mechanism of formaldehyde oxidation over gold supported on MnO

Guanglong PANG,Donghui WANG,Yunhong ZHANG,Chunyan MA,Zhengping HAO

《环境科学与工程前沿(英文)》 2016年 第10卷 第3期   页码 447-457 doi: 10.1007/s11783-015-0808-8

摘要: MnO microspheres with various surface structures were prepared using the hydrothermal method, and Au/MnO catalysts were synthesized using the sol-gel method. We obtained three MnO microspheres and Au/MnO samples: coherent solid spheres covered with wire-like nanostructures, solid spheres with nanosheets, and hierarchical hollow microspheres with nanoplatelets and nanorods. We investigated the properties and catalytic activities of formaldehyde oxidation at room temperature. Crystalline structures of MnO are the main factor affecting the catalytic activities of these samples, and γ-MnO shows high catalytic performance. The excellent redox properties are responsible for the catalytic ability of γ-MnO . The gold-supported interaction can change the redox properties of catalysts and accelerate surface oxygen species transition, which can account for the catalytic activity enhancement of Au/MnO . We also studied intermediate species. The dioxymethylene (DOM) and formate species formed on the catalyst surface were considered intermediates, and were ultimately transformed into hydrocarbonate and carbonate and then decomposed into CO . A proposed mechanism of formaldehyde oxidation over Au/MnO catalysts was also obtained.

关键词: MnO2 microspheres     Au/MnO2     formaldehyde oxidation     γ-MnO2    

Synthesis of TiO2 nano-particles and their photocatalytic activity for formaldehyde and methyl orange

XIAO Xinyan, ZHANG Huiping, CHEN Huanqin, LIAO Dongliang

《化学科学与工程前沿(英文)》 2007年 第1卷 第2期   页码 178-183 doi: 10.1007/s11705-007-0033-5

摘要: TiO nano-particles were synthesized by sol-gel technique and characterized by X-ray diffractometer (XRD) and transmission electron microscope (TEM). Their photocatalytic activities for formaldehyde (FA) and methyl orange (MO) degradation were tested using degradation rate (η) as an evaluation index. Based on the orthogonal test results, the optimal condition for TiO preparation was obtained. Results showed that particle sizes were in the range of 10 40 nm, and that prepared TiO had better photocatalytic activity than P25. A simplified model was developed to evaluate the apparent quantum efficiency (Φapp) of this photocatalytic reaction system.

关键词: prepared     photocatalytic activity     apparent     photocatalytic     orthogonal    

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    

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    

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    

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    

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    

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    

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    

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    

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    

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    

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    

Tailoring the simultaneous abatement of methanol and NO on Sb-Ce-Zr catalysts via copper modification

《环境科学与工程前沿(英文)》 2022年 第16卷 第10期 doi: 10.1007/s11684-022-1565-0

摘要:

● Cu addition enhances CH3OH oxidation and alleviates its inhibitory effect on SCR.

关键词: Copper modification     Sb-CeZr2Ox catalyst     NOx     Methanol     Simultaneous removal    

标题 作者 时间 类型 操作

Modified iron-molybdate catalysts with various metal oxides by a mechanochemical method: enhanced formaldehydeyield in methanol partial oxidation

Xue Liu, Lingtao Kong, Shengtao Xu, Chaofan Liu, Fengyun Ma

期刊论文

Catalytic activities and mechanism of formaldehyde oxidation over gold supported on MnO

Guanglong PANG,Donghui WANG,Yunhong ZHANG,Chunyan MA,Zhengping HAO

期刊论文

Synthesis of TiO2 nano-particles and their photocatalytic activity for formaldehyde and methyl orange

XIAO Xinyan, ZHANG Huiping, CHEN Huanqin, LIAO Dongliang

期刊论文

Impacts of methanol fuel on vehicular emissions: A review

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

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

Mehdi SEDIGHI,Kamyar KEYVANLOO

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

Tailoring the simultaneous abatement of methanol and NO on Sb-Ce-Zr catalysts via copper modification

期刊论文