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当期目录

2019年 第21卷 第4期    刊出日期:2019-12-30
目录
 
2019, 21(4):  1-2. 
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 Contents of The issue
Catalyst Research
Effects of recrystallization parameters on the formation of hollow Silicalite-1 zeolite
谭铖 董卓雅 孙凸 张亚萍 章冠群 夏长久 马延航
2019, 21(4):  1-8. 
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Hollow silicalite-1 zeolite can be readily fabricated by hydrothermally treating the parent silicalite-1 with tetrapropylammonium hydroxide. A dissolution-recrystallization mechanism has been previously proposed to explain the formation of such hollow structures, but detailed information of this formation process still remains unclear. Herein, by tracking the evolvement of the hollow voids and morphology of the silicalite-1 under various treatments using PXRD, SEM, TEM and N2 adsorption/desorption techniques, we systematically studied the formation process of the hollow structure of silicalite-1 zeolite and discovered that the organic template, water, and treating temperature and time can significantly influence the morphology and size of hollow structure inside silicalite-1 zeolite crystals. Generally, a diluted synthesis medium with high template content under suitable temperature (for instance 170 °C) and extended treatment time favors the formation of single hexagonal hollow structure within sicalite-1 zeolites; while other conditions favor the formation of rounded hollow voids or even multiple-voids within Silicalite-1 zeolites.
高分散的CoWO4或CuWO4提高WO3的光催化性能
何放 康明亮 宋春冬 杨霞 张静
2019, 21(4):  9-20. 
摘要 ( 247 )   PDF (1310KB) ( 738 )  
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本文采用原位浸渍与固相反应结合,成功地合成了CoWO4或CuWO4高度分散在WO3表面的复合CoWO4/WO3或CuWO4/WO3光催化剂。通过XRD,SEM,TEM,EDS,HR-TEM,UV-vis DRS,SPV和活性物种实验研究了CoWO4/WO3和CuWO4/WO3样品的结构,形貌,光物理性质和光催化降解机理。XRD,SEM和TEM结果表明,当CoWO4或CuWO4的负载量较小时,CoWO4或CuWO4高度分散在WO3表面上。但是当CoWO4或CuWO4的负载量增加时,WO3表面的CoWO4或CuWO4颗粒发生明显的团聚。可见光光催化降解RhB的实验结果表明,所有CoWO4/WO3或CuWO4/WO3样品的光催化活性都优于WO3的活性。这主要是因为WO3和CoWO4或CuWO4之间形成的II型异质结能够显著促进光生电子和空穴的分离。此外,CoWO4/WO3和CuWO4/WO3系列样品中,0.2%CoWO4/WO3和0.2%CuWO4/WO3分别显示了最优异的光催化活性,与WO3相比,其光催化活性分别提高了约9.1倍和6.8倍。此外,活性物种实验表明,光催化过程中在0.2%CoWO4/WO3和0.2%CuWO4/WO3催化剂上产生的?OH,h+和?O2?都是光催化降解RhB的活性物种。本文为设计高活性的光催化剂提供了一种思路。
Comparison on Adsorptive Separation of n-Paraffins Based on Binderless and Binder-containing Zeolite 5A Pellets
孔瑞琦 姜豪 王丹 谭家伦 任丹妮 孙辉 沈本贤 刘纪昌 汤晟 赵德银 常小虎
2019, 21(4):  21-28. 
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Binderless zeolite is considered to be a potential alternative for binder-containing zeolite in the industrial applications of adsorptive separation process. Synthesized binderless zeolite and commercial binder-containing products were used in adsorptive separation of n-paraffins from a model oil, with their performance compared. It is indicated that the binderless zeolite exhibits by 25%-35% higher in saturated adsorption capacity and by 115%-130% more adsorption amount at the breakthrough point with much shorter length of mass-transfer zone. Adsorptive separation of n-paraffins from naphtha was carried out in a fixed-bed adsorber containing the synthesized binderless zeolite 5A under the operating conditions covering a feed space velocity of 90 h-1 and an adsorption temperature of 573 K. As compared to original naphtha, the raffinate shows by 34 units more in research octane number and by around 10% more of potential aromatic content, while the desorption oil exhibits by 13.3% more ethylene yield and by 11.7% higher in total olefins yield.
CoMnMgAl Hydrotalcite-like Compounds and their Complex Oxides: Facile Synthesis and FCC De-SOx Removal
姜瑞雨 朱涛 王敏 宋欣钰 丁亮 高健
2019, 21(4):  29-35. 
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The X-CoMnMgAl hydrotalcite-like precursors (X-LDHs) were first synthesized by the coprecipitation method using Cl-, CO32-, NO3- and SO42- as the corresponding guest anions, which were further used to prepare X-CoMnMgAl complex oxides (X-LDOs) through calcination. The structure and the surface morphology of the as-prepared samples were characterized by FT–IR, XRD, N2 adsorption-desorption and SEM. These as-prepared X-LDOs could act as sulfur-transfer catalysts for desulfurization. The activity of SOx adsorption and regeneration were evaluated via a self-assembled fixed-bed reactor simulating the conditions found in the fluid catalytic cracking units. These four types of sulfur-transfer catalysts with the same phase but different structure displayed the following order of desulfurization efficiency: CO3-LDO >Cl-LDO >NO3-LDO > SO4-LDO.
Scientific Research
5A分子筛的晶粒尺寸对其乙烯/乙烷吸附分离性能的影响
边青敏 忻睦迪 徐广通 陈帅 邹亢 史延强
2019, 21(4):  36-41. 
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The adsorptive separation of ethylene and ethane exhibits a less energy-intensive -alternative technique with development potential among all separation processes currently. In this approach, zeolite 5A with different particle sizes from 3340 nm to 440 nm was synthesized by in-situ hydrothermal synthesis. The effect of particle size on the adsorptive separation performance of zeolite 5A was investigated. The results show that the accessibility of Ca2+ enhance dramatically with gradually declined particle size. At the initial stage of particle size reduction, the ethylene IAST (Ideal Adsorbed Solution Theory) selectivity of zeolite 5A increased up to 5.6 with reduced diffusion resistance and the strengthened π-complexation. With the further shrunk particle size (< 710 nm), the ethylene IAST selectivity of zeolite 5A deteriorate sharply, which stems from competitive adsorption between ethylene and moisture on Ca2+ adsorption sites.
Doping effect of vanadium dioxide on oxidative desulfurization
赵雨桐 宗梦雅 范存正 陈坤 王丹红 张明慧
2019, 21(4):  42-48. 
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VO2 (M) doped with different metals (Ti, Ce, Nb, Zr, W, and Mo) was successfully synthesized by the hydrothermal reduction process using oxalic acid as the reductant. The results showed that doping metals in the VO2 (M) lattice could enhance the oxidative desulfurization (ODS) activity. The DSC and Raman spectra revealed that VO2 (M) retained its monoclinic structure after doping. Mechanism for the improvement of ODS activity by doping was investigated. Electron transfer to V (V) atom occurs upon doping, and then V (V) changes into V (IV), which can promote the ODS reaction. This explanation can be confirmed by the fact that doping can promote the proportion of V (Ⅳ) after doping as revealed by the XPS analysis.
长链醇的添加对航空煤油宏观喷雾特性的影响
李奉誉 刘燕菊 黄启福 付炜 史卫东 林其钊
2019, 21(4):  49-57. 
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长链醇被认为是有前景的替代燃料和燃料添加剂。 本工作旨在研究将长链醇与航空煤油混合对宏观喷雾特性的影响。本研究选择正丁醇和正戊醇作为实验所用替代燃料,使用共轨喷射系统产生高压喷射条件。 使用纹影成像系统捕获喷雾过程。 结果表明,随着长链醇的添加,喷雾贯穿度和峰值速度增大,而喷雾锥角和喷雾面积减小。 还对AKB混合物和AKP混合物的宏观喷雾特性进行了比较。 与AKB混合物相比,AKP混合物表现出相似的喷雾贯穿度,更大的峰值速度,更小的喷雾锥角和喷雾面积。
Research on the impact of the new and renewable energy replacing fossil energy resources under constraint of carbon emissions
赵立祥 杨楚潇
2019, 21(4):  58-67. 
摘要 ( 178 )   PDF (653KB) ( 1325 )  
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For studying new and renewable energy substitutes fossil energy in primary energy consumption and its impact on carbon emissions in confront with economic uncertainties, a multi-sector DSGE model was employed to simulate the dynamic impact on carbon emissions and macroeconomy development. The structural adjustment of energy consumption and the carbon emissions mitigation policy were considered in the model. The simulation results showed that using new and renewable energy instead of fossil energy is the optimal choice for the firms under the constraint of carbon emission mitigation policy. Structure adjustment of energy consumption is the best routine to achieve the dual goal of economic development and carbon emission reduction goal. Unexpected sharp fall in free carbon quota has a negative impact on the economy.
Process Research
Simultaneous removal of sulfide, nitrate and ammonium from wastewater in one reactor
刘春爽 李伟 Xue Bai Yongxing Wang 王永强 刘芳 赵朝成
2019, 21(4):  68-72. 
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Simultaneous removal of sulfide, nitrate and ammonium was achieved in an upflow anaerobic sludge blanked (UASB) reactor by the start-up strategy of gradually decreasing influent nitrite to null. The sulfide/nitrate-nitrogen ratio could affect the distributions of end products of sulfur and a sulfide/nitrate-nitrogen ratio of 1:0.76 is a proposed optimum for S0 accumulation. The Denittrasoma, Thiobacillus and Candidatus_Kuenenia presented the functional strains in the studied reactor. This result provides theoretical and technical basis for the large-scale application of anaerobic ammonium oxidation process.
离子液体催化碳酸乙烯酯和甲醇酯交换反应及其理论过程模拟
郭立颖 吴浩 王亦荣
2019, 21(4):  73-80. 
摘要 ( 164 )   PDF (865KB) ( 625 )  
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首先合成了三种离子液体[Bmim]OH、[Bmim]IM和[Bmim]PF6,并对其化学结构进行了红外表征。再将其分别与助催化剂CaO、K2CO3和(CH3O)2Mg复合,研究离子液体复合体系催化碳酸乙烯酯和甲醇合成碳酸二甲酯的反应过程。通过正交试验研究了不同离子液体、助催化剂和反应温度对催化剂性能的影响。利用密度泛函理论研究了离子液体中阳离子和阴离子以及助催化剂的路易斯碱位对催化活性的协同关系,证明了一种易于制备的功能化咪唑盐具有较高的催化活性。碳酸乙烯酯的单程转化率为65.23%,碳酸二甲酯二甲基选择性为98.95%。通过实验和DFT研究,提出了反应机理。
基于主成分分析法和响应曲面法对Halomonas菌株生长因子的分析与优化
史可 黄国富 徐化春 薛建良 孙静宽 肖新峰 李琳
2019, 21(4):  81-87. 
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The biomass of petroleum-degrading bacteria, such as Halomonas spp., is crucial to the alleviation of severe oil spills through bioremediation. In this paper, the bacterium (HDMP1) was isolated and identified. Growth factors were analysed and optimised through the single-factor experiments, the factor analysis (FA), the principal component analysis (PCA), and the response surface methodology (RSM). Results indicated that HDMP1 was identified as genus Halomonas. In the single-factor experiments, the range of suitable growth conditions for HDMP1 covered: a salt concentration of 2%-4%, a medium pH value of approximately 9, an inoculum concentration of 1.0%, a substrate concentration of 1.0%-1.4%, and a rotation rate of 140 r/min. The evaluation by FA and PCA indicated that three significant growth factors were the salt concentration, the pH value, and the rotation rate. A maximum biomass of HDMP1 was obtained under the conditions covering a salt concentration of 3.5%, a medium pH of 8, and a rotation rate of 151 r/min by optimization.
Simulation and Optimization
Distillation Sequence Optimization Considering Extractive Distillation under Multiple Conditions: A Methanol to Propylene Case Study
于靓 钱锋 王基铭
2019, 21(4):  88-93. 
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This study provides insights into the distillation sequence optimization of refinery system in a methanol to propylene plant with extractive distillation under multiple conditions. The simulated annealing algorithm (SA) with relative cost function was used to solve a meaningful optimization problem. It was observed that different conditions had differed on the flowsheet. Case study show the effectiveness of the proposed method.
基于流动与传热耦模拟的空冷系统铵盐沉积特性研究
金浩哲 周俊锋 刘文文 刘骁飞 偶国富
2019, 21(4):  94-102. 
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铵盐腐蚀是加氢反应出物空冷器(REAC)系统的典型失效形式。为了研究REAC系统中铵盐的腐蚀特性,采用混合模型、流体热传递模型和颗粒跟踪模型进行了数值模拟。结果表明,第一排和第二排管内各截面的温度和速度偏差较小。对于颗粒运动轨迹,颗粒的惯性起着重要作用,颗粒越小,在空冷器中沉积越均匀。然而,对于较大的颗粒,它们更倾向于从垂直弯头内侧下落,并在饱和前优先沉积在入口集箱和管道处。在换热器管材中,第二排管材的沉积数量大于第一排管材,高危管材主要集中在中部和右侧区域。在实际运行条件下,颗粒的动力学参数与堵塞位置相吻合。
Comparison of mass transfer characteristics between countercurrent-flow and crosscurrent-flow rotating packed bed
祁贵生 郭林雅 刘有智 张栋铭
2019, 21(4):  103-111. 
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Rotating packed bed (RPB), mainly including countercurrent-flow RPB (Counter-RPB) and crosscurrent-flow RPB (Cross-RPB) classified from the perspective of gas-liquid contact style, is a novel process intensification device. A significant measure standard to evaluate performance of RPB is mass transfer effect. In order to contrast the mass transfer characteristics of Counter-RPB and Cross-RPB that with the same size, liquid volumetric mass transfer coefficient (klae) and effective interfacial area (ae) were measured under identical operation conditions. Meanwhile, comparison of comprehensive mass transfer performance was conducted with ΔP (pressure drop)/klae as the standard. Experimental results indicated that klae and ae increased with increase of liquid spray density q, gas velocity u and high gravity factor β. Furthermore, compared with Cross-RPB, Counter-RPB has higher liquid volumetric mass transfer coefficient and slightly larger effective interfacial area. The experimental results of comprehensive mass transfer performance showed that the Counter-RPB had higher ΔP/klae than the Cross-RPB with changes of liquid spray density and high gravity factor, and there exists a turning point at 0.71 m/s accompanied by a variation with gas velocity. Moreover, the relative error of experimental values to calculated values calculated by the correlative expressions of klae was less than 5%. In conclusion, the mass transfer characteristics of RPB are deeply impacted by the manner in which the flows are established and Cross-RPB would have a great potential for industrial scale-up applications.
Lubrication Research
硼酸、磷酸对改善复合钙基润滑脂硬化现象的机理探讨
郑会 孙洪伟 何懿峰 苏朔 庄敏阳 刘欣阳
2019, 21(4):  112-118. 
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In the 1950’s, complex calcium lubricating grease had been widely used. However, due to the hardening problem in the process of storage and use, the production of complex calcium lubricating grease decreases year by year. Domestic and foreign researchers have done a lot of work on its hardening problem, and it has been found that boric acid and phosphoric acid can effectively improve the hardening problem. In this paper, the water absorption test of several calcium salts was carried out, and it was found that calcium 12-hydroxystearate did not absorb water, and calcium acetate, calcium phosphate and calcium borate had different degrees of water absorption. Calcium acetate has the highest water absorption rate, and calcium phosphate and calcium borate have comparable water absorption rates. Using molecular simulation technology, it is found that in the complex calcium grease system, calcium phosphate and calcium borate prefers to combine with water, which inhibits the water absorption of calcium acetate and makes the hardening problem better.