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2015 Vol.32 Issue.2,Published 2015-03-15
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2015 Vol. 32 (2): 0-0 [Abstract] ( 1404 ) [HTML 1KB] [ PDF 577KB] ( 1491 )
1 Effect of Calcination Temperature on the Catalytic Performance of CuO/Co3O4-CeO2 Catalyst for Preferential CO Oxidation
Chen Yena, Meng Ming
CuO/Co3O4-CeO2 (CuCoCe10) catalysts were prepared by impregnation method and calcined at different temperatures (250, 300, 350, 400 and 450 ℃). The catalytic performance of the CuCoCe10 catalysts for preferential CO oxidation (CO PROX) was evaluated. Many techniques such as N2-sorption, XRD, H2-TPR and Cu K-edge XAFS were used for characterizing the structures of the catalysts. It is found that in the catalysts calcined at different temperatures, the main copper species are CuO. The catalyst calcined at 350 ℃ exhibits the largest specific surface area and the best reduction/oxidation properties. The complete CO conversion for CuCoCe10 catalyst calcined at 350 ℃ was achieved in the temperature region of 98—173 ℃; moreover, this catalyst also exhibits the highest stability of catalytic activity.
2015 Vol. 32 (2): 1-5,12 [Abstract] ( 4885 ) [HTML 1KB] [ PDF 1365KB] ( 1527 )
6 Effect of Milling Time on the Cu/SiO2 Monolithic Catalyst for Hydrogenation of Dimethyl Oxalate and the Adhesion of Washcoat
Wang Bo, Zhao Shuo, Zhao Yujun, Wang Shengping, Ma Xinbin
The Cu/SiO2 monolithic catalyst was prepared by washcoating the slurry, which was obtained through milling the Cu/SiO2 powder prepared by ammonia-evaporation method, onto the wall of the cordierite monoliths. Subsequently, the slurry and catalyst were characterized by laser particle size analyzer (LPSA), N2 physical adsorption, mercury intrusion porosimetry (MIP), N2O titration, X-ray diffraction (XRD), scanning electron microscope (SEM). The characterization results indicated that the milling time had little influence on the physicochemical properties and phase structure. However, increasing the milling time could modulate the particle size distribution of the slurry and improve the surface morphology of the catalyst. Then, the adhesion of washcoat was strengthened and the Cu/SiO2 monolithic catalyst showed higher catalytic performance in hydrogenation of dimethyl oxalate to ethylene glycol.
2015 Vol. 32 (2): 6-12 [Abstract] ( 2431 ) [HTML 1KB] [ PDF 1420KB] ( 3794 )
13 Effect of Pt Adding Method on the NSR Activity of the Mn-Based Oxide at Low Temperature
Li Xingang, Ge Chaoyi, Guo Li, Xian Hui
The Mn-based catalysts were prepared by three different methods: Pt directly impregnating on Mn2O3, Pt/Al2O3 and Mn2O3 delamination and mechanical mixing. And the Pt content of the catalysts was 1% (mass fraction). The NOx storage capacity and NOx storage-reduction cycle activity indicated that the sample mixing by machine exhibited the biggest NOx storage capacity and highest eliminated efficiency. Compared with the Mn2O3 sample, the NOx storage capacity of the mechanical mixing sample increased more than twice and reached 368.1 mmol·g-1 at 150 ℃. Meanwhile, the NOx eliminated efficiency increased from 0 to 48.1%. This was due to the Pt in the mechanical mixing sample could promote the oxygen dissociation and enhance NOx storage efficiency. In addition, Pt had a significant synergistic effect on Mn in the mechanical mixing sample, then increasing the NSR activity of the catalyst.
2015 Vol. 32 (2): 13-17 [Abstract] ( 2234 ) [HTML 1KB] [ PDF 1381KB] ( 1384 )
18 Synthesis of Cyclic Carbonate from CO2 and Epoxide Catalyzed by Inorganic Silica Supported Acidic Ionic Liquid
Tang Jingya, Wang Hua, Han Jinyu, Yao Rui
Four efficient catalysts composed of inorganic silica supported acidic ionic liquid were developed and showed high activities for the coupling reaction of expoxide and CO2. The effects of catalysts, CO2 pressure, reaction temperature, reaction time and catalyst amount have been investigated systematically. When all the silica supported ionic liquids were used as the catalyst, the conversion of PO was more than 95%. The highest selectivity of PC was 90.6% when 0.5 g [Smim]HSO4 was used as the catalysts. A high conversion of PO (96.3%) could be reached at 140 ℃ with a low CO2 pressure (1.0 MPa) and 2.5 mL PO for 5 h in the present of 0.5 g [Smim] HSO4. The catalyst could be reused for six times without apparent loss of catalytic activity. A proposed mechanism for the coupling reaction of CO2 and PO is suggested.
2015 Vol. 32 (2): 18-24 [Abstract] ( 4359 ) [HTML 1KB] [ PDF 1661KB] ( 1862 )
25 Hydrogenolysis of Glycerol to 1,2-Propanediol on Cu-Based Catalysts Derived from Hydrotalcite-Like Precursors
Tian Shasha, Yang Juan, Chen Jixiang
Cu-Zn-Al and Cu-Mg-Al catalysts were prepared from hydrotalcite-like precursors after calcination and reduction. The effect of M2+ (M=Zn or Mg) and M2+/Al3+ ratio on the catalyst structure and performance were investigated by means of XRD, H2-TPR, N2-sorption, H2-TPD, NH3-TPD, CO2-TPD and activity test. The hydrotalcite-like precursors were transformed to the spinel and/or metal oxides after calcination at 450 ℃, from which the highly dispersed Cu-based catalysts were prepared after reduction at 270 ℃. Compared with the Cu-Mg-Al catalysts, the Cu-Zn-Al catalysts had more amounts of adsorbed hydrogen due to the role of Zn species. With increasing Al2O3 content, the specific surface area and acid amount increased. The Cu-Mg-Al catalysts had more basic sites than the Cu-Zn-Al catalysts. In the hydrogenolysis of glycerol, Cu-Zn-Al[n(Cu):n(Zn):n(Al)=1:1:4] had the highest activity and selectivity to 1,2-propanediol, which is due to the largest amounts of surface Cu and acid sites. For the Cu-Mg-Al catalysts, there may be a synergism between the Cu and basic sites.
2015 Vol. 32 (2): 25-30 [Abstract] ( 5097 ) [HTML 1KB] [ PDF 1573KB] ( 1632 )
31 Catalytic Dehydration of Ethanol to Ethylene over Phosphorus-Nickel Modified HZSM-5 Catalysts
Li Fengyi, Liu Zongzhang, Zhang Minhua
Based on the Ni-modified HZSM-5 synthesized via ion-exchange method, a series of phosphorus-nickel modified HZSM-5 catalysts were prepared by impregnating the Ni-HZSM-5 with phosphoric acid aqueous solution. The influence of modification on the structure and acid properties of HZSM-5 was investigated by means of X-ray diffraction(XRD), N2 physisorption, temperature programmed desorption of pyridine(Py-TPD) and 27Al nuclear magnetic resonance(27Al MAS NMR). The results indicated that the addition of phosphoric acid promoted the dealumination from framework, and reduced the amount of strong acid, which was responsible for the enhancement of anti-carbon deposition ability and extension of its service life. The results of catalytic activity test revealed that the catalyst with H3PO4 content of 8%(3-PN-Z) showed the best performance. The effect of operating parameters on the dehydration of ethanol to ethylene over 3-PN-Z was also investigated and the optimal reaction conditions obtained were 260 ℃, 1.5 h-1 (WHSV) and 50%(volumetric fraction) of ethanol concentration. The stability evaluation showed that during the initial 50 hours, the ethanol conversion and ethylene selectivity kept higher than 97% and 98% respectively, which was better than the Ni-modified HZSM-5 catalyst.
2015 Vol. 32 (2): 31-36 [Abstract] ( 3545 ) [HTML 1KB] [ PDF 1459KB] ( 1631 )
37 Thermal Decomposition of n-Octane in Regenerative Cooling Microchannels at Supercritical Conditions: Product Distributions and Kinetics
Fang Qinghai, Zhang Xiangwen
Thermal cracking of supercritical hydrocarbon aviation fuels was conducted in an electrically heated tube(2 mm i.d.), detailed information on the product distributions of thermal cracking of n-octane under supercritical conditions(5 MPa, 560—665 ℃) were obtained. And residence times along the tube were reported too. Through a new secondary mechanism of C5—C11, the PPD kinetic model proposed by Ward et al. is modified. The reliability of the modified PPD kinetic model is confirmed by the comparison of model predictions with the experimental values.
2015 Vol. 32 (2): 37-42,73 [Abstract] ( 4103 ) [HTML 1KB] [ PDF 2074KB] ( 2315 )
43 Supported Gas Membrane Process for Removal/Recovery of Ammonia from Wastewater by Using Dilute Nitric Acid as Absorbent
Hao Xingge, Wang Yuanxi, Li Haiqing, Qin Yingjie, Liu Liqiang, Cui Dongsheng
In this study, the feasibility and long-term operational stability of PTFE hydrophobic microporous hollow fiber-based supported gas membrane process is demonstrated by using dilute nitric acid as absorbent solution to remove/recover ammonia from a wastewater stream. Under similar operation conditions, the separation performance of three kinds of membrane contactors made from PTFE, PP and PVDF were compared; the influence of inlet feed concentration, velocity and temperature on the mass transfer performance of PP, PVDF and PTFE contactors was also studied. Experimental results showed that the lumen-side diameter and wall thickness of the hollow fibers were the most dominant factor influencing the mass transfer process, and that, the overall mass transfer coefficient K, membrane mass transfer coefficient kM, lumen-side mass transfer coefficient kL increased significantly with the increase of temperature. The long-term experimental results showed that the PVDF membrane contactor had a leakage problem after 7 days, the mass transfer coefficient of the PP membrane contactor had dropped notably after 20 days, while the PTFE membrane contactor still had a stable performance after running for 30 days. This study indicates that PTFE membrane has good resistance to nitric acid oxidation, it provides basic guarantee to remove/recover ammonia from wastewater (or chemical feed solution) streams as a by-product of ammonium nitrate by using gas supported membrane separation process.
2015 Vol. 32 (2): 43-49,79 [Abstract] ( 4148 ) [HTML 1KB] [ PDF 2166KB] ( 1854 )
50 Facile Synthesis and Characterisation of IrO2/ATO as Novel OER Electrocatalysts
Wang Pan, Guo Jianzhao, Wang Yuxin
Water electrolysers of solid polymer electrolyte (SPE) have been shown to be a promising method of producing hydrogen, but it is short of a stable oxygen electrocatalysts. In the current study, we seek to explore an advanced and facile method for the preparation of IrO2 deposited on Sb-doped SnO2 (ATO) nanoparticles. The IrO2/ATO particulates were characterized by SEM, TEM, XRD and XPS. The electrochemical properties were examined via cyclic voltammetry(CV), steady state polarization, electrochemical impedance spectroscopy(EIS) and chronoamperometry(CA) measurements. In fact, it was found that the IrO2/ATO synthesized with the novel method maintained an enhanced electrocatalytic activity and got a current density of 105 mA·cm-2 at 1.6 V. Its stability toward oxygen evolution reaction (OER) in acidic media was tested at 1.5 V, and the current density decaying rate was 1.687×10-2 (mA·cm-2)·h-1. To improve the loading of the catalysts, the current density toward OER was enhanced significantly, even if the current density of unit mass of Ir will decrease.
2015 Vol. 32 (2): 50-55 [Abstract] ( 2053 ) [HTML 1KB] [ PDF 1972KB] ( 1881 )
56 Flow Field of SAS During the Preparation of Al(NO3)3 Nano-Particles
Wang Zhaoya, Zhang Minhua, Geng Zhongfeng, Li Yonghui
This paper investigated the preparation of Al(NO3)3 spherical nano-particles with the supercritical antisolvent (SAS). At first experiments were carried out at temperature from 32 ℃ to 52 ℃, pressure from 8 MPa to 24 MPa, and CO2 flow rate from 30.0 g·min-1 to 45.0 g·min-1 in order to investigate their effect on the morphology and particle size (PS). The results showed that morphology of the nano-particles changed from spherical to non-spherical, and particle size decreased first and then increased with the increasing of temperature. Particles agglomeration became severe at 48 ℃. When pressure increased, particle size decreased at first and then increased. Particle size reached the minimum at 16 MPa. The particle size exhibited a positive correlation with the CO2 mass flow rate. The effecting mechanism of above factors was explored with CFD and was explained by the effective coefficient distribution in the precipitator. The CFD model for the injection in the precipitator is developed with the Realizable k-ε turbulent model. Deff reflects both the changes of the thermodynamics and hydrodynamics of the system. The result is significant to precipitate particles with controllable particle size and morphology. Some of the above results can also be applied to other systems and can help to optimize the parameters.
2015 Vol. 32 (2): 56-62 [Abstract] ( 3564 ) [HTML 1KB] [ PDF 1944KB] ( 1951 )
63 Behavior of Dynamic Filtration for Ultrasonic Coupling
Wang Xiaojing, Wang Fan, Zhang Ting
Based on the requirements of purification process of the production materials, a new reactor was designed and proposed in this paper, with three functionalities: mixed-pulp, washing-filter and separation. In order to improve mass transfer and filteration effects, ultrasound probes was employed to enhance liquid turbulence intensity. To validate the effectiveness of ultrasound, several 3D computational models were built through Fluent for numerically simulating the mixing-washing process and dynamic filtration process. With the established model, the operating conditions of the mixing and dynamic filtration process stage are calculated, which provides useful information for experiment research and actual production.
2015 Vol. 32 (2): 63-68 [Abstract] ( 1890 ) [HTML 1KB] [ PDF 2574KB] ( 1570 )
69 Simulation of Azeotropic Distillation of Ethanol, 1,4-Dioxane, Methanol and Water
Han Zhenwei, Liu Tong, Fan Yongmei
Considering the ethanol-water mixture with methanol and 1,4-dioxane, an ethanol dehydration process via two-column azeotropic distillation using cyclohexane as entrainer was proposed. Azeotropes analysis of the system was made and the simulation of azeotropic distillation was conducted with Aspen Plus. The simulation results show that the two-column process is feasible and the content of water in the bottom of dehydration column is less than 0.05%(mass percentage). Methanol in the feed was discharged from the bottom of recovery column. The simulation results agree well with the process data.
2015 Vol. 32 (2): 69-73 [Abstract] ( 8386 ) [HTML 1KB] [ PDF 1516KB] ( 2396 )
74 Effect of Overexpression of Succinate Exporter SucE on Anaerobic Succinate Production by Corynebacterium glutamicum
Xia Huihua, Yin Guomin, Zhu Nianqing, Chen Tao
Corynebacterium glutamicum ATCC 13032 produces succinate through the reductive tricarboxylic acid cycle under anaerobic conditions. Efficient export of succinate into the culture supernatant is important to increase its production. In this study, sucE gene overexpression was introduced into strain C. glutamicum XZ. The resulting strain C. glutamicum XZ(pExhsucE)showed a 7% increase in succinate yield and a 19% increase in succinate productivity. Also, the relative flux of the glyoxylate pathway increased by 50%. Using two-stage culture, succinate titer up to 518 mmol·L-1 was achieved with a specific productivity of 0.95 mmol gCDW-1·h-1 and a yield of 1.5 mol (mol glucose)-1.
2015 Vol. 32 (2): 74-79 [Abstract] ( 3097 ) [HTML 1KB] [ PDF 1736KB] ( 1435 )
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