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1.
Oxidative desulfurization of fuel oil was investigated using a process consisting of oxidation and distillation steps. In the oxidation step, various organic carboxylic acid/H2 O2 systems, especially acetic acid/H2 O2, were used as oxidant. They oxidize both easy and refractory sulfur compounds and convert them into oxidized sulfur compounds. The oxidized sulfur compounds are finally removed from fuel oil by distillation in the presence of water. The sulfur content of fuel oil was decreased to levels as low as 20 ppm (up to 90%) in a short contact time, ambient temperature, and atmospheric pressure. The results showed that applying this process did not have any deleterious influence on the distillation characteristic, composition, and content of fuel oil that was examined. An artificial neural network, using back propagation (BP), was also utilized for modeling oxidative desulfuration process of fuel oil. The comparison between the output of ANN modeling and the experimental data showed satisfactory agreement.  相似文献   

2.
The sulfur recovery unit converts H2S to elemental sulfur by the Claus process. The process occurs during two combustion and catalytic reactions. Alumina (γ-Al2O3) and bauxite (Al2O3H2O) are the main Claus catalysts in crude oils. The volume distribution of micro- and macropores and the parameter of Bethe lattice representing the complex structure of catalyst pellets pores are the most important parameters affecting catalyst performance. This research is aimed at evaluating these parameters impact on effective efficiency of catalyst bed after blocking by liquid sulfur for the second and third reactors. It can be done by considering micro- and macropores as a function of pellet diameter. The results show that pellets with a minimum coordination number or Bethe lattice parameter of 6 are more suitable to use in catalytic reactors. There is a great consistency between the modeling results and the industrial ones. In addition, a catalytic pellet with a diameter of 4.55 mm has the most optimal performance for sulfur recycling processes in industrial crude oil.  相似文献   

3.
Abstract

In recent years, many countries have drawn up strict laws regarding the sulfur-containing compounds of fossil fuels, especially the gasoline and diese. Ultra-deep desulfurization of fuel is a main component of fossil fuel development. The experiment imposes the photochemistry field on the catalytic oxidation system in order to broaden the newly desulfurization technology. The sulfur-containing compounds, such as dibenzothiophene (DBT) and its derivatives, in diesel fuel are oxidized to corresponding sulfones using H2O2-CH3COOH-FeSO4 oxidation systems via ultrasonic irradiation. Later, the oxidized sulfur compounds (sulfones) are extracted by a suitable polar solvent. The influences of the catalytic system, reaction time, and ultrasonic source (frequency, intensity) are tested on desulfurization efficiency. Experimental results show that the removal efficiency of the sulfur compound could amount to 97.5%, and the recovery of oil is above 92% under the catalytic system of H2O2-CH3COOH-FeSO4 by the assistance of ultrasound.  相似文献   

4.
目的 解决Cansolv尾气处理装置胺液净化单元(APU)废水高盐、高有机物与还原性硫的高浓水质特征影响水处理系统的稳定运行问题。方法 详细分析了两个天然气净化厂的文丘里和APU废水的水质特征,其中,APU废水成分复杂,是影响水处理系统稳定运行的关键。采用臭氧(O3)、O3耦合催化剂、臭氧/双氧水(O3/H2O2) 3种氧化技术处理APU废水,通过废水中COD值和TOC值变化来评价有机物降解效果,研究了反渗透膜污堵原因和O3/H2O2降解有机物机理。结果 O3/H2O2氧化技术为去除废水中有机物的最优方法,当200 mL废水中O3质量浓度为22 500 mg/L、H2O2投加量为2 mL、反应时间为60 min时,达到最佳处理效果,COD去除率为60.8%。结论 采用O3<...  相似文献   

5.
Three amphiphilic peroxophosphomolybdates [C4mim]3PMo4O24, [C8mim]3PMo4O24 and [C16mim]3PMo4O24 were synthesized and characterized. These catalysts were used for extraction and catalytic oxidative desulfurization of fuel with H2O2 as an oxidant and ionic liquid [C4mim]BF4 as an extractant. It was found that [C16mim]3PMo4O24 showed the highest catalytic activity and the sulfur content could decrease to 7.5 ppm. In contrast, the desulfurization system shows very low performance without H2O2 or ionic liquid. The detailed reaction conditions were optimized including reaction time, temperature, the dosage of H2O2 and catalyst, and different sulfur compounds. After the reaction, the catalysts and the ionic liquid can be cycled 8 times with a little decrease in desulfurization efficiency.  相似文献   

6.
A simple extraction and catalytic oxidative desulfurization (ECODS) system composed of VO(acac)2, 30% H2O2, and 1-butyl-3-methylimidazolium tetrafluoroborate ([Bmim]BF4) has been found to be suitable for the deep removal of dibenzothiophene (DBT) in model oil at room temperature. The optimal conditions were as follows: [n(H2O2)/n(DBT)/n(catalyst) = 100:20:1], model oil = 5 mL, ionic liquid [IL] = 1 mL, T = 30°C, t = 2 hr. With the ECODS system, the sulfur removal of DBT could reach 99.6%, which was superior to that of the simple extraction with IL (15.6%) or oxidation without catalyst (17.1%). The IL could be recycled five times without a significant decrease in activity.  相似文献   

7.
 利用[(C16H33) N(CH3)3]3-[PW12O40]双亲催化剂与H2O2组成的催化氧化体系对汽油进行氧化后,以介孔SiO2为载体等体积浸渍法制备的介孔CuO/SiO2为吸附剂,采用固定床连续流动式吸附脱硫评价装置,考察了CuO/SiO2的CuO负载量、焙烧温度、焙烧时间和吸附温度对汽油脱硫率的影响,并对介孔CuO/ SiO2吸附剂性质进行了XRD表征。结果表明,采用在焙烧温度为400℃、焙烧时间为2.0 h、CuO负载量为2%制备的CuO/SiO2, 在吸附温度为120℃时,汽油氧化-脱硫的脱硫效果较好,汽油脱硫率可达56.82%。  相似文献   

8.
In this research the feasibility of chemical oxidation with H2O2 and Fenton's reagent for degradation of petroleum hydrocarbons before and after composting of bottom sludge from crude oil storage tanks was investigated. Results showed that total petroleum hydrocarbons removal in composting reactor was 80.2%. In chemical oxidation steps, petroleum hydrocarbons removal enhanced with increasing oxidant concentrations. Increasing oxidation time from 24 to 48 h had a little effect on petroleum hydrocarbons removal. The study showed that chemical oxidation as a pre-treatment step was more effective than post-treatment. It was also deduced that petroleum hydrocarbons in the sludge and composted mixture can be oxidized by hydrogen peroxide without adding supplementary iron.  相似文献   

9.
In this study, the removal of sulfur compounds from diesel samples using ultrasound-assisted oxidative desulfurization (UAODS) process in presence of different types of oxidizing agents was studied. Experiments were performed to assess the effects of influential parameters on the performance of UAODS process including ultrasonic irradiation time, oxidant type, mass ratio of oxidant to diesel fuel (oxidant: diesel), and finally acetic acid as an oxidative promoter. The efficiency of sulfur compounds removal from the diesel fuel dramatically improved using appropriate oxidative process with the assistance of ultrasound irradiation. H2O2 was found to be the most promising oxidant component whose concentration in the media directly affected total sulfur removal and thiol group conversion efficiencies. Using 4 wt% of H2O2 followed by 15 min of ultrasonic irradiation leaded to sulfur removal efficiency of 76% and thiol group conversion of 79% at ambient temperature and atmospheric pressure. Using acid acetic as the promoter of H2O2 also leaded to further sulfur compounds removal.  相似文献   

10.
 分别采用超声波辐照浸渍法和普通浸渍法制备了MnO2/γ-Al2O3催化剂,运用电感耦合等离子体原子发射光谱(ICP-AES)和X射线衍射(XRD)对催化剂进行表征,在空气-异丁醛-MnO2/γ-Al2O3体系中评价其对加氢柴油的氧化脱硫催化性能,并考察了反应温度、异丁醛用量、空气流量、溶剂类型和剂/油体积比对柴油氧化脱硫反应的影响。结果表明,超声波辐照浸渍法制备的MnO2/γ-Al2O3催化剂对柴油氧化脱硫的催化性能明显优于普通浸渍法制备的催化剂。最适宜的催化柴油氧化脱硫反应的条件为:乙腈为溶剂、加氢柴油30 mL、温度35℃、异丁醛20 mmol、空气流量0.06 L/min、超声波辐照浸渍法制备的MnO2/γ-Al2O3催化剂0.08 g、剂/油体积比1/6和催化氧化时间10 min。在此条件下可将柴油硫质量分数从542μg/g 降至31μg/g,柴油脱硫率和回收率分别为94.3%和93.3%。  相似文献   

11.
采用连续流动的固定床微反装置考察了Pt/SO24-/ZrO2-Al2O3(PSZA)在正己烷异构化反应中的催化行为。采用NH3-TPD、H2-TPR及TG表征了催化剂的酸性、还原性能及硫物种含量。结果表明,PSZA的初始异构化催化活性几乎不受反应温度的影响,而稳定性则与反应温度密切相关。低温下反应,催化剂在短时间内迅速失活,而提高反应温度可大大提高PSZA的反应稳定性。PSZA具有良好的再生性能,与新鲜催化剂相比,多次再生后的催化剂异构化催化活性基本没有变化。PSZA在低温下的快速失活与其催化活性中心产生的机理有关,而与其硫损失或硫物种的还原无关。在异构化反应过程中,催化剂通过氢溢流可产生强酸活性中心,并在反应过程中不断被消耗;在高温下通过氢溢流不断产生新的强酸中心,使催化活性保持稳定;而低温下氢溢流难以发生,消耗的强酸活性中心不能及时补充,使催化活性下降。  相似文献   

12.
Abstract

Mordenite modified with Al2O3 (Al2O3/mordenite) was synthesized and used for the desulfurization of FCC gasoline. The influences of operating parameters on the results were studied for the model solution composed of dibenzothiophene (DBT) and isooctane. Al2O3/mordenite exhibits higher sulfur capacity than other kinds of chemisorbents. The suitable composition of the chemisorbent is 30 wt% Al2O3 to 70 wt% mordenite. The optimal operating parameters are: temperature 160°C; velocity 3 h?1 (WHSV). Under the stated conditions, desulfurization was carried out for the FCC gasoline with sulfur content of 220.4 μg/g. The chemisorbent can maintain the sulfur content under 50 μg/g for 40 h and has good regeneration ability after desorption using benzene.  相似文献   

13.
采用水热合成法制备了MIL-101(Cr)催化剂,考察了反应条件对其在H2O2氧化环己烷反应中催化性能的影响。利用XRD、FT-IR和UV-Vis等手段对MIL-101(Cr)反应前后结构的变化进行了表征。结果表明,MIL-101(Cr)在所选择的反应体系中存在Cr析出现象,其结构在以H2O2为氧化剂的反应体系中不稳定,经反应后形成了无定型物质,但催化活性不仅远高于新鲜MIL-101(Cr),而且还在重复利用中表现出良好的稳定性。  相似文献   

14.
Abstract

Semi-empirical molecular orbital theory and parametric model 3 methods were used to calculate the quantum chemistry properties of dibenzothiophene (DBT) and its corresponding sulfone compounds to investigate the essential theory of a formic acid/H2O2 oxidation desulfurization system. To study oxidation kinetics of the oxidation desulfurization reaction, DBT was also employed as a model compound to obtain the oxidation kinetic parameters. Desulfurization of fluid catalytic cracking (FCC) diesel was also performed in this process, and the sulfur content was reduced from 7,200 μg·g?1 to 598 μg·g?1 after being extracted by polyethylene glycol 200.  相似文献   

15.
Abstract

In this research, different concentrations of H2O2 and H2SO4 solutions were used in order to remove the sulfur from high sulfur contented No. 6 fuel oil. In desulphurization experiments, reaction temperature, reaction time, and the concentration of H2O2 and H2SO4 were varied in a range of 20–50C, 30–150 min, 5–35%, and 0.05–2.00 N, respectively. The ratio of reagent/fuel oil was taken as 10/1 and the stirring speed as 1,000 rpm. According to the results obtained, considering the desulphurization and the organic structure of the fuel, the most appropriate method was found as the H2O2 leaching method. It was barely determined that the highest desulphurization was achieved by H2O2/0.1N H2SO4 leaching method. The optimum process parameters for H2O2 leaching method were found as a concentration of 15%, reaction temperature of 30C, and reaction time of 60 min; and for H2SO4 leaching method were found as concentration of 0.1 N, reaction temperature of 30C, and reaction time of 150 min.

It was observed that by increasing the reaction temperature, reaction time, and reagent concentration, the carbon and hydrogen contents of the fuel decreased considerably and on the contrary the oxygen content increased very rapidly. A partial decrease of nitrogen content was also observed.  相似文献   

16.
以MCM-48为载体,通过浸渍法制备了H6P2W18O62/MCM-48催化剂,并采用FT-IR、XRD、SEM、EDS对催化剂进行表征。以微波促进30%(质量分数)H2O2氧化环己酮合成己二酸反应为探针,考察了H6P2W18O62/MCM-48的催化性能,并通过正交实验确定了优化的工艺条件。结果表明,采用H6P2W18O62负载量40%的H6P2W18O62/MCM-48催化剂,在优化的合成己二酸的工艺条件下,即催化剂质量分数(以环己酮质量计)5.1%、n(C6H10O)∶n(H2O2)∶n(H2C2O4.2H2O)=100∶450∶1.88、反应温度95℃、微波功率300 W、反应时间3.5h,己二酸收率可达81.3%;催化剂重复使用5次,己二酸收率仍可达到64.6%。  相似文献   

17.
Abstract

Alumina-silica (Al2O3-SiO2) composite supports were examined to find the optimum state of support (i.e., composition and morphology). SiO2 content in the Al2O3-SiO2 support induced a shift of the main peak to higher frequency ascribed to an increased amount of Mo8O26 4?. A 75 wt% Al2O3-25 wt% SiO2 support had homogeneously dispersed alumina particles of smaller size with high crystallinity. Hydrodesulfurization (HDS) of straight-run gas oil and its conventionally hydrotreated straight-run gas oil was performed over NiMo sulfides supported on Al2O3-SiO2 composites. The high crystallinity of NMASA2-27 may be related to the high HDS and hydrogenation activity of NiMo sulfides due to its moderate interaction with the alumina surface.  相似文献   

18.
在氢氧化铝干胶挤条成型时,调节纳米炭黑的加入量和水/粉质量比,制备了孔径呈双峰分布、具有较大孔容和比表面积的γ-Al2O3载体。当炭黑加入质量分数为13%、水/粉质量比1.15时,制备的孔径呈双峰分布的γ-Al2O3载体的孔容为0.80mL/g、比表面积为309m2/g,4~10nm和10~15nm孔径分别占总孔容50.8%和35.1%(体积分数),采用该载体制备的NiMoP/γ-Al2O3催化剂的孔径呈明显的双峰分布。在反应温度370℃、氢分压10MPa、氢/油体积比700、体积空速1.5h-1的条件下,制备的NiMoP/γ-Al2O3催化剂可使减压和焦化混合蜡油的硫质量分数由25600μg/g降至2070μg/g,脱硫率为91.9%,而参比催化剂仅可使减压和焦化混合蜡油硫质量分数降至3450μg/g,脱硫率为86.5%。  相似文献   

19.
Abstract

Thermal simulation experiments on the reaction between n-C8H18 and CaSO4 were carried out under high temperatures and high pressures. Properties of the reaction products are characterized by advanced analytical methods. Based on the results of simulation experiments, possible reaction pathways and thermodynamic characteristics were tentatively investigated. It was found that n-C8H18 can react with CaSO4 to produce CaCO3, H2S, CO2, H2O, CS2, and a series of organic sulfur compounds (OSCs). The conversion of elemental sulfur in the molecular structure of CaSO4 to small molecule inorganic sulfides and thiophene sulfur increases with the increase of temperature. There is a strong thermodynamic drive for the reaction of n-C8H18 with CaSO4 and high temperature is favorable to the reaction. This study may provide new insights into the origin of OSCs in petroleum.  相似文献   

20.
Abstract

In this research, desulphurization of number 6 fuel oil (residue fuel oil) by chemical methods was studied. Besides, factors like reaction temperature, reaction time, concentration, and stirring speed were examined to determine the effects of various process parameters on desulphurization and on higher heating value. According to the results obtained, the optimum values of process parameters were determined as H2O2 concentration of 15%, reaction temperature of 40C, reaction time of 60–150 min and stirring speed of 1, 000 rpm. Under these conditions, the sulphur content in the fuel oil sample was reduced from 2.78 to 2.29%–1.54% approximately. The degree of desulphurization increased, but higher heating value decreased seriously at high levels of H2O2 concentration, reaction temperature, reaction time, and stirring speed. Some fuel oil samples that are pretreated with H2O2/0.1 N H2SO4 were extracted successively with acetone, ethanol, ethylene glycol, and hydrogen peroxide. In conclusion, the sulphur content decreased approximately from 2.29 to 1.08%. Partial decrease determined in the higher heating value of the sample at the end of extraction.  相似文献   

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