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catalytic cracking of Cycloparaffins Admixed with Olefins:2. Single-Event Microkinetic(SEMK) Assessment

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China Petroleum Processing & Petrochemical Technology 2014年第2期16卷 84-90页

作者： Xue Gaoping Weng Huixin Joris W.Thybaut Guy B.Marin Research Institute of Petroleum Processing East China University of Science and Technology Laboratory for Chemical Technology Ghent University

The developed SEMK model is used to provide an insight into the contribution of individual reactions in the cracking of methylcyclohexane as well as the site coverage by various carbenium ions. The preferred reaction pathways for the conversion of methylcyclohexane are hydride transfer reactions followed by PCP-isomerizations, deprotonation and endocyclic β-scission, accounting for 61%, 22% and 12% of its disappearance, respectively, at 693 K and 30% conversion of methylcyclohexane. Protolysis plays a minor role in the cracking of methylcyclohexane. Once cyclic diolefins are formed, all of them can be instantaneously transformed to aromatics, which are easily interconverted via disproportionation. Judging from the carbenium ion concentrations it is evident that, at the investigated operating conditions, less than 5% of the acid sites are covered by carbenium ions, less than 2% of which corresponds to cyclic type species including allylic ones.

关键词： catalytic cracking single-event microkinetic model cycloparaffin olefin site coverage by carbenium ions

catalytic cracking and PSO-RBF Neural Network Model of FCC Cycle Oil

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China Petroleum Processing & Petrochemical Technology 2013年第4期15卷 63-69页

作者： Liu Yibin Tu Yongshan Li Chunyi Yang Chaohe State Key Laboratory of Heavy Oil Processing China University of Petroleum

catalytic cracking experiments of FCC cycle oil were carried out in a fixed fluidized bed reactor. Effects of reac- tion conditions, such as temperature, catalyst to oil ratio and weight hourly space velocity, were investigated. Hydrocarbon composition of gasoline was analyzed by gas chromatograph. Experimental results showed that conversion of cycle oil was low on account of its poor crackability performance, and the effect of reaction conditions on gasoline yield was obvi- ous. The paraffin content was very high in gasoline. Based on the experimental yields under different reaction conditions, a model for prediction of gasoline and diesel yields was established by radial basis function neural network （RBFNN）. In the model, the product yield was viewed as function of reaction conditions. Particle swarm optimization （PSO） algorithm with global search capability was used to obtain optimal conditions for a highest yield of light oil. The results showed that the yield of gasoline and diesel predicted by RBF neural network agreed well with the experimental values. The optimized reac- tion conditions were obtained at a reaction temperature of around 520 ~C, a catalyst to oil ratio of 7.4 and a space velocity of 8 h~. The predicted total yield of gasoline and diesel reached 42.2% under optimized conditions.

关键词： catalytic cracking cycle oil radical basis function neural network particle swarm optimization

catalytic cracking of Cycloparaffins Admixed with Olefins:1. Single-Event Microkinetic(SEMK) Modeling

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China Petroleum Processing & Petrochemical Technology 2014年第1期16卷 71-80页

作者： Xue Gaoping Weng Huixin Thybaut Joris W. Marin Guy B. Research Institute of Petroleum Processing East China University of Science and Technology Laboratory for Chemical Technology Ghent University

Single-event microkinetic(SEMK) model of the catalytic cracking of methylcyclohexane admixed with 1-octene over REUSY zeolites at 693 K—753 K in the absence of coke formation is enhanced. To keep consistency with the wellknown carbenium ion chemistry, hydride transfer forming and consuming allylic carbenium ions in the aromatization of cycloparaffins are further investigated and differentiated. The reversibility of endocyclic β-scission and cyclization reactions is refined by accounting explicitly for the reacting olefins and resulting cycloparaffins in the corresponding thermodynamics. 24 activation energies for the reactions involved in the cracking of cycloparaffins are obtained by the regression of 15 sets of experimental data upon taking the resulting 37 main cracking products, i. e., responses into account. The enhanced SEMK model can adequately describe the catalytic behavior of 37 main products with conversion and temperature.

关键词： catalytic cracking single-event microkinetic model cycloparaffin olefin catalysis

Targeted catalytic cracking to Olefins(TCO):Reaction Mechanism,Production Scheme,and Process Perspectives

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Engineering 2023年第11期30卷 100-109页

作者： Youhao Xu Yanfen Zuo Wenjie Yang Xingtian Shu Wei Chen Anmin Zheng Research Institute of Petroleum Processing SinopecBeijing 100083China Economics and Development Research Institute SinopecBeijing 100029China State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics National Center for Magnetic Resonance in WuhanKey Laboratory of Magnetic Resonance in Biological SystemsWuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430071China

Light olefins are important organic building blocks in the chemicals *** main low-carbon olefin production methods,such as catalytic cracking and steam cracking,have considerable room for improvement in their utilization of *** review provides a thorough overview of recent studies on catalytic cracking,steam cracking,and the conversion of crude oil *** maximize the production of light olefins and reduce carbon emissions,the perceived benefits of various technologies are *** olefin generation and conversion as a link to expand upstream and downstream processes,a targeted catalytic cracking to olefins(TCO)process is proposed to meet current demands for the transformation of oil refining into chemical *** main innovations of this process include a multiple feedstock supply,the development of medium-sized catalysts,and a diameter-transformed fluidizedbed reactor with different feeding *** combination with other chemical processes,TCO is expected to play a critical role in enabling petroleum refining and chemical processes to achieve low carbon dioxide emissions.

关键词： Light olefins Steam cracking catalytic cracking TCO process Oil processing revolution

catalytic cracking of endothermic fuels in coated tube reactor

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Frontiers of Chemical Science and Engineering 2008年第2期2卷 181-185页

作者： Jia LI Jijun ZOU Xiangwen ZHANG Wei GUO Zhentao MI Key Laboratory of Green Chemical Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Suspensoid of HZSM-5 or HY zeolites mixed with a self-made ceramic-like binder was coated on the inner wall of a tubular reactor by gas-aided fluid displacement *** coated zeolites were characterized by means of X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FT-IR)and scanning electron microscopy(SEM).The coating thickness is 10–20 mm and the particle size of the zeolites is in the range of 1–5 *** the coated reactor,cracking of endothermic fuels including n-dodecane and aviation fuel RP-3 was carried out separately under supercritical conditions at 600uC and 625uC to investigate their heat sinks and conversion of catalytic *** the reaction catalyzed by HY(25%mass fraction)coating,the heat sink capacity of ndodecane are 815.7 and 901.9 kJ/kg higher than that of the bare tube at 600uC and at 625uC,*** of n-dodecane also increases from 42%to 60%at 600uC and from 66%to 80%at *** coated zeolite can significantly inhibit the carbon deposition during supercritical cracking reactions.

关键词： endothermic fuel catalyst coating catalytic cracking heat sink supercritical

Transformation of Bio-oil into BTX by Bio-oil catalytic cracking

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Chinese Journal of Chemical Physics 2013年第4期26卷 477-483,J0002页

作者：朱九方汪继聪李全新中国科学技术大学化学物理系合肥230026

Production of benzene, toluene and xylenes （BTX） from bio-oil can provide basic feedstocks for the petrochemical industry. catalytic conversion of bio-oil into BTX was performed by using different pore characteristics zeolites （HZSM-5, HY-zeolite, and MCM-41）. Based on the yield and selectivity of BTX, the production of aromatics decreases in the following order： HZSM-5〉MCM-41〉HY-zeolite. The highest BTX yield from bio-oil using HZSM-5 reached 33.1% with aromatics selectivity of 86.4%. The reaction conditions and catalyst characterization were investigated in detail to make clear the optimal operating parameters and the relation between the catalyst structure and the production of BTX.

关键词： Bio-oil BTX catalytic cracking

Production of Low-carbon Light Olefins from catalytic cracking of Crude Bio-oil

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Chinese Journal of Chemical Physics 2013年第2期26卷 237-244,I0004页

作者：袁燕妮王铁军李全新中国科学技术大学化学物理系合肥230026 中国科学院广巾能源所可再生能源与天然气水合物重点实验室广州510640

Low-carbon light olefins are the basic feedstocks for the petrochemical industry. catalytic cracking of crude bio-oil and its model compounds （including methanol, ethanol, acetic acid, acetone, and phenol） to light olefins were performed by using the La/HZSM-5 catalyst. The highest olefins yield from crude bio-oil reached 0.19 kg/（kg crude bio-oil）. The reaction conditions including temperature, weight hourly space velocity, and addition of La into the HZSM-5 zeolite can be used to control both olefins yield and selectivity. Moderate adjusting the acidity with a suitable ratio between the strong acid and weak acid sites through adding La to the zeolite effectively enhanced the olefins selectivity and improved the catalyst stability. The production of light olefins from crude bio-oil is closely associated with the chemical composition and hydrogen to carbon effective ratios of feedstock. The comparison between the catalytic cracking and pyrolysis of bio-oil was studied. The mechanism of the bio-oil conversion to light olefins was also discussed.

关键词： Crude bio-oil Low-carbon olefin catalytic cracking Zeolite catalyst

Experiment and modeling of coke formation and catalyst deactivation in n-heptane catalytic cracking over HZSM-5 zeolites

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Chinese Journal of Chemical Engineering 2023年第3期55卷 165-172页

作者： Zhenzhou Ma Xu Hou Bochong Chen Liu Zhao Enxian Yuan Tingting Cui School of Chemical Engineering Changchun University of TechnologyChangchun 130012China Advanced Institute of Materials Science Changchun University of TechnologyChangchun 130012China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China Department of Chemistry Tsinghua UniversityBeijing 100084China

Since paraffins catalytic cracking was of significant importance to light olefins and aromatics production,this work was intended to gain insights into the feature and model of coke formation and catalyst deactivation in n-heptane catalytic cracking over HZSM-5 zeolites. 18 tests of n-heptane catalytic cracking were designed and carried out over HZSM-5 zeolites in a wide range of operating conditions. A particular attention was paid to the measurement of the conversion, product distribution, coke content, and the porosity and acidity of the fresh and spent HZSM-5 zeolites. It was found that alkene and aromatic promoted coke formation, and it reduced the pore volume and acid site of HZSM-5 zeolites, tailoring its performance in n-heptane catalytic cracking. The specific relationship between HZSM-5 zeolites, n-heptane conversion, product distribution and coke formation was quantitively characterized by the exponential and linear function. Based on the reaction network, the coupled scheme of coke formation and catalyst deactivation were specified for n-heptane catalytic cracking. The dual-model was proposed for the process simulation of n-heptane catalytic cracking over HZSM-5 zeolites. It predicted not only the conversion and product distribution but also coke content with the acceptable errors.

关键词： n-Heptane HZSM-5 catalytic cracking Coke Deactivation Dual-model

Fischer-Tropsch wax catalytic cracking for the production of low olefin and high octane number gasoline: Process optimization and heat effect calculation

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Petroleum Science 2023年第2期20卷 1255-1265页

作者： Mei Yang Gang Wang Jian-Nian Han Cheng-Di Gao Jin-Sen Gao State Key Laboratory of Heavy Oil Processing College of Chemical Engineering and and EnvironmentChina University of PetroleumBeijing 102249China College of Science China University of PetroleumBeijing 102249China

To produce low olefin gasoline with high octane number by Fischer-Tropsch (F-T) wax fluid catalytic cracking (FCC) process, operating conditions optimization were carried out in the pilot-scale riser and turbulent fluidized bed (TFB) FCC unit. The experimental results in the riser indicated that under the condition of low reaction temperature and regenerated catalyst temperature, large catalyst-to-oil weight ratio (C/O) and long reaction time, the gasoline olefin content could be reduced to 20.28 wt%, but there is large octane number loss owing to a great loss in high octane number olefin. Therefore, a novel FCC process using the TFB reactor was proposed to strengthen the aromatization reaction. The reaction performance of TFB reactor were investigated. The result demonstrated that the TFB reactor has more significant effect in reducing olefins and improving aromatics. At the expense of certain gasoline yield, the gasoline olefin content reduced to 23.70 wt%, aromatics content could increase to 26.79 wt% and the RON was up to 91.0. The comparison of reactor structure and fluidization demonstrated that the TFB reactor has higher catalyst bed density. The reaction heat and coke combustion heat was calculated indicating the feasibility of its industrial application of the TFB process.

关键词： Fischer-Tropsch wax catalytic cracking Riser TFB Gasoline olefin Reaction heat