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Research and development of hydrocracking catalysts and technologies in China

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Frontiers of Chemical Science and Engineering 2018年第4期12卷 867-877页

作者： Chong Peng Yanze Du Xiang Feng Yongkang Hu xiangchen fang Dalian Research Institute of Petroleum and Petrochemicals SINOPECDalian 116000China State Key Laboratory of Heavy Oil Processing China University of PetroleumQingdao 266580China

Hydrocracking of petroleum feedstock represents a compelling route for the production of industrial clean fuels, which has triggered the continuous research and development of core technology related areas such as catalysts, reaction engineering and engineering design. This review particularly focuses on the research and development of catalysts and catalytic processes for hydrocracking of petroleum feedstock in China. Hydroprocessing technologies of China keep pace with the up-to-date progress of the world, and some of the technologies have achieved leading role in the world. It is noted that China Petroleum and Chemical Corporation has a full range of hydroprocessing technologies and provides corresponding “tailor-made” catalysts. Through the efforts of several generations, 20 categories of the catalysts including more than 60 brands have been developed, among which more than 40 brands have been successfully applied for more than 130 times. Importantly, the pivotal technical improvements including the deep drawing vacuum gas-oil (VGO) and de-asphalting oil hydrocracking technology to improve material adaptability, the high value-added hydrogenation technology to convert high aromatic diesel conversion to naphtha, the hydrocracking technology using VGO-catalytic diesel blends, the Fushun Research Institute of Petroleum and Petrochemicals’ diesel to gasoline and diesel hydrocracking technologies, and the Sheer hydrocracking technology to reduce energy are reviewed.

关键词： hydrocracking process catalyst China

Development and application of ex-situ presulfurization technology for hydrotreating catalysts in China

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Frontiers of Chemical Science and Engineering 2011年第3期5卷 287-296页

作者： Yulan GAO xiangchen fang Zhenmin CHENG School of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Fushun Research Institute of Petroleum and Petrochemicals SINOPECFushun 113001China

The development and application of ex-situ presulfurization(EPRES)technology for hydrotreating catalysts has been reviewed in the present article.The studies in laboratory scale and commercial practice indicated that the adoption of the EPRES catalyst in industrial application can significantly enhance the degree of presulfurization of metal oxide components,shorten the start-up period,and effectively reduce the environmental impact as well as the danger of start-up procedure in industrial hydrotreating unit.This catalyst has been proved to be versatile for different types of hydrogenation reactions.Different types of active site models are also discussed for better understanding the nature of presulfur-ized catalysts.

关键词： ex-situ presulfurization in situ presulfuriza-tion hydrotreating catalyst hydrotreating catalyst sulfur utilization ratio

Simultaneous recovery of carbon and sulfur resources from reduction of CO_2 with H_2S using catalysts

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Journal of Energy Chemistry 2016年第1期25卷 110-116页

作者： Hui Su Yuyang Li Ping Li Yongxiu Chen Zhizhi Zhang xiangchen fang State Key Laboratory of Chemical Engineering East China University of Science and Technology Fushun Research Institute of Petroleum & Petrochemicals Sinopec

An approach to the simultaneous reclamation of carbon and sulfur resources from CO2 and H2S has been proposed and effectively implemented with the aid of catalysts. A brief thermodynamic study reveals the potential of direct reduction of CO2 with H2S（15：15 mol% balanced with N2） for selective production of CO and elemental sulfur. The experiments carried out in a fixed-bed flow reactor over the temperature range of 400–800 °C give evidence of the importance of the employment of catalysts. Both the conversions of the reactants and the selectivities of the target products can be substantially promoted over most catalysts studied. Nevertheless, little difference appears among their catalytic performance. The results also prove that the presence of CO2 can remarkably enhance H2S conversion and the sulfur yield in comparison with H2S direct decomposition. A longtime reaction test on Mg O catalyst manifests its superior durability at high temperature（700 °C） and huge gas hourly space velocity（100,000 h-1）. Free radicals initiated by catalysts are supposed to dominate the reactions between CO2 and H2S.

关键词： Carbon dioxide Hydrogen sulfide Simultaneous recovery Reduction Catalyst

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加氢裂化理论创新与实践

石油炼制与化工 2024年第1期55卷 164-170页

作者：范思强张通王继峰方向晨侯栓弟中石化(大连)石油化工研究院有限公司辽宁大连116000

中石化(大连)石油化工研究院有限公司通过深入研究烃类分子多相催化反应过程,发现烃分子的诱导偶极矩和反应中间体碳正离子的稳定性是影响烃类分子吸附和反应的关键因素,并在此基础上提出渐次反应理论,用于指导加氢裂化工艺与催化材料... 详细信息

中石化(大连)石油化工研究院有限公司通过深入研究烃类分子多相催化反应过程,发现烃分子的诱导偶极矩和反应中间体碳正离子的稳定性是影响烃类分子吸附和反应的关键因素,并在此基础上提出渐次反应理论,用于指导加氢裂化工艺与催化材料的开发与升级。渐次反应理论的应用避免了低效无秩序反应的发生,使得加氢裂化反应过程科学有序,从而在低能耗、低氢耗的反应环境下提升了加氢裂化过程的产品选择性与产品质量,有效推进中国炼油结构调整,实现科学有序的“油转化”、“油转特”转型发展。

关键词：加氢裂化渐次反应吸附催化反应转型升级

Regulating catalyst morphology to boost the stability of Ni–Mo/Al_(2)O_(3) catalyst for ebullated-bed residue hydrotreating

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Green Energy & Environment 2021年第2期6卷 283-290页

作者： Huihong Zhu Zhiwei Mao Bin Liu Tao Yang Xiang Feng Hao Jin Chong Peng Chaohe Yang Jifeng Wang xiangchen fang Dalian Re search Institute of Petroleum and Petrochemicals SINOPECDadian116045China State Key Lab of Heavy Oil Processing China University of PetroleumQingdao266580China State Key Lab of Chemical Engineering East Chind University of Science and TechnologoyShanghui200237China

Hydrotreating of vacuum residue by ebullated-bed shows tremendous significance due to more stringent environmental regulations and growing demand for lighter fuels. However, enhancing the catalyst stability still remains as a challenging task. Herein, two Ni–Mo/Al_(2)O_(3) catalysts with distinct morphologies(i.e., spherical and cylindrical) were first designed, and the morphology effect on deactivation was systematically elucidated employing multi-characterizations, such as HRTEM with EDX mapping, electron microprobe analysis, FT-IR, TGA and Raman. It is found that spherical catalyst exhibits superior hydrotreating stability over 1600 h. The carbonaceous deposits on spherical catalyst with less graphite structure are lighter, and the coke weight is also smaller. In addition, the metal deposits uniformly distribute in the spherical catalyst, which is better than the concentrated distribution near the pore mouth for the cylindrical catalyst. Furthermore, the intrinsic reason for the differences was analyzed by the bed expansion experiment. Higher bed expansion rate together with the better mass transfer ability leads to the enhanced performance. This work sheds new light on the design of more efficient industrial hydrotreating catalyst based on morphology effect.

关键词： Deactivation Ebullated-bed Hydrotreating Vacuum residue Morphology

Separation-and-Recovery Technology for Organic Waste Liquid with a High Concentration of Inorganic Particles

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Engineering 2018年第3期4卷 406-415页

作者： Hualin Wang Pengbo Fu Jianping Li Yuan Huang Ying Zhao Lai Jiang xiangchen fang Tao Yang Zhaohui Huang Cheng Huang National Engineering Laboratory for Industrial Wastewater Treatment East China University of Science and Technology Shanghai 200237 China Sinopec Luoyang Petrochemical Engineering Corporation Luoyang 471003 China Sinopec Jinling Petrochemical Corpora tion Nanjing 210033 China Sinopec Dalian (Fushun) Research Institute of Petroleum and Petrochemicals Fushun 113001 China Sinopec Zhenhai Refining and Chemical Company Ningbo 315207 China

The environmentally friendly and resourceful utilization of organic waste liquid is one of the frontiers of environmental engineering. With the increasing demand for chemicals, the problem of organic waste liquid with a high concentration of inorganic pollutants in the processing of petroleum, coal, and natural gas is becoming more serious. In this study, the high-speed self-rotation and flipping of particles in a threedimensional cyclonic turbulent field was examined using a synchronous high-speed camera technique; the self-rotation speed was found to reach 2000–6000 rad·s−1. Based on these findings, a cyclonic gasstripping method for the removal of organic matter from the pores of particles was invented. A technological process was developed to recover organic matter from waste liquid by cyclonic gas stripping and classifying inorganic particles by means of airflow acceleration classification. A demonstration device was built in Sinopec’s first ebullated-bed hydro-treatment unit for residual oil. Compared with the T-STAR fixed-bed gas-stripping technology designed in the United States, the maximum liquid-removal efficiency of the catalyst particles in this new process is 44.9% greater at the same temperature, and the time required to realize 95% liquid-removal efficiency is decreased from 1956.5 to 8.4 s. In addition, we achieved the classification and reuse of the catalyst particles contained in waste liquid according to their activity. A proposal to use this new technology was put forward regarding the control of organic waste liquid and the classification recovery of inorganic particles in an ebullated-bed hydro-treatment process for residual oil with a processing capacity of 2 × 106 t·a−1. It is estimated that the use of this new technology will lead to the recovery of 3100 ta−1 of diesel fuel and 647 t·a−1 of high-activity catalyst; in addition, it will reduce the consumption of fresh catalyst by 518 t·a−1. The direct economic bene

关键词： Organic waste liquid Inorganic particles Cyclonic gas stripping Particle self-rotation Airflow acceleration classification

Experimental Study of Integrated Ebullated-bed and Fixed-bed for Hydrotreating Mid-Low Temperature Coal Tar to Clean Fuel

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China Petroleum Processing & Petrochemical Technology 2016年第3期18卷 1-6页

作者： Meng Zhaohui Yang Tao fang xiangchen SINOPEC Fushun Research Institute of Petroleum and Petrochemicals Fushun 113001

A new hydrotreating technology integrating the ebullated-bed(EB) and the fixed-bed(FB) hydrogenation was proposed to investigate the efficiency for hydrotreating mid- low-temperature coal tar to clean fuel, and multiple tests at the bench scale were carried out. The results showed that the distillates obtained from EB reactors were greatly upgraded and could meet the requirements of FB unit without discarding any tail oil. The naphtha produced from FB reactors could be fed to the catalytic reforming unit, while a high quality diesel was also obtained. The unconverted oil(UCO) could be further hydrocracked to clean fuel. It is found that the removal of impurities from the coal tar oil is related with the molecular aggregation structure and composition of the coal tar. Application of the integrated hydrotreating technology to the hightemperature coal tar processing demonstrated that more than half of heavy components could be effectively upgraded.

关键词： coal tar ebullated bed fixed bed integrated hydrotreating

Application of Discrete Lumped Kinetic Modeling on Vacuum Gas Oil Hydrocracking

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China Petroleum Processing & Petrochemical Technology 2013年第2期15卷 67-73页

作者： Han Longnian fang xiangchen Peng Chong Zhao Tao Liaoning Shihua University SINOPEC Fushun Research Institute of Petroleum and Petrochemicals

The kinetic model of vacuum gas oil (VGO) hydrocracking based on discrete lumped approach was investigated, and some improvement was put forward at the same time in this article. A parallel reaction scheme to describe the conversion of VGO into products (gases, gasoline, and diesel) proposed by Orochko was used. The different experimental data were analyzed statistically and then the product distribution and kinetic parameters were simulated by available data. Furthermore, the kinetic parameters were correlated based on the feed property, reaction temperature, and catalyst activity. An optimization code in Matlab 2011b was written to fine-tune these parameters. The model had a favorable ability to predict the product distribution and there was a good agreement between the model predictions and experiment data. Hence, the kinetic parameters indeed had something to do with feed properties, reaction temperature and catalyst activity.

关键词：集总动力学模型减压瓦斯油加氢裂化动力学参数应用 Matlab 实验数据基础饲料

Performance of Ni-based, Fe-based and Co-based Oxygen Carriers in Chemical-Looping Hydrogen Generation

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China Petroleum Processing & Petrochemical Technology 2013年第2期15卷 53-58页

作者： Liang Hao Zhang Xiwen fang xiangchen Yuan Honggang Fushun Research Institute of Petroleum and Petrochemicals SINOPEC Fushun Research Institute of Environmental Science

Ni-based, Fe-based and Co-based oxygen carriers with perovskite oxides used as the supports were prepared by citric acid complexation method. The oxygen carriers were characterized by thermal analysis, H2-temperature-programmed reduction and X-ray diffraction methods. Performance tests were evaluated through Chemical-Looping Hydrogen Generation in a fixed-bed reactor operating at atmospheric pressure. The characterization results showed that all samples were composed of metal oxides and perovskite oxides. Performance results indicated that CH4 conversion over the oxygen carriers decreased in the following order: NiO/LaNiO3 >Co2O3 /LaCoO3 >Fe2O3 /LaFeO3 . The ability of NiO/LaNiO3 and Fe2O3 / LaFeO3 to decompose water was stronger than that of Co2O3 /LaCoO3 as evidenced by our experiments. H2 amounting to 80 mL upon reacting on methane in every cycle could be completely oxidized by NiO/LaNiO 3 at 900 ℃ in the period from the third cycle to the eighth cycle.

关键词：性能测试氧载体化学循环制氢钙钛矿型氧化物固定床反应器镍基钴基