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Journal of Natural Gas Chemistry 2011年第3期20卷 261-265页

作者： ruchao wei chunyi li chaohe yang honghong shan State Key Laboratory of Heavy Oil Processing China University of Petroleum Qingdao 266555 Shandong China

One type of ZSM-5 zeolite with large partical size was prepared and characterized by XRD, SEM, N2 adsorption-desorption, XRF, Py-IR and NH3-TPD techniques. Effects of ammonium exchange and SiO2/Al2O3 molar ratios on the reaction of methanol to propylene （MTP） over Na-ZSM-5 and H-ZSM-5 zeolites have been studied in a fixed-bed flow reactor under the operating conditions of T = 500 °C, P = 1 atm, and WHSV = 6 h-1. Ammonium exchange led to a rapid decrease in Na content for Na-ZSM-5 zeolite. The reaction results indicated that Na-ZSM-5 and H-ZSM-5 with different SiO2/Al2O3 molar ratios all exhibited high activity for methanol conversion. Ammonium exchange and the decreased SiO2/Al2O3 molar ratio of ZSM-5 zeolite led to an increase both in strong acid sites and weak acid sites. Na-ZSM-5 with high SiO2/Al2O3 molar ratio was favorable for the formation of propylene. The highest propylene selectivity （45.9%） was obtained over Na-ZSM-5 zeolite catalyst with SiO2/Al2O3 molar ratio of 220.

关键词： ZSM-5 MTP propylene ammonium exchange acidity

Preparation and characterization of Mn/MgAlFe as transfer catalyst for SO_x abatement

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Journal of Natural Gas Chemistry 2011年第2期20卷 191-197页

作者： Ruiyu Jiang honghong shan chunyi li chaohe yang State Key Laboratory of Heavy Oil Processing China University of Petroleum （East China） Qingdao 266555 Shandong China

A series of manganese-promoted MgAlFe mixed oxides, used as sulfur transfer catalysts, were prepared by acid-processed gelatin method and characterized by TGA-DTA, XRD, N2 adsorption-desorption and FT-IR techniques. It was found that the sulfur transfer catalysts with 0.5？3.0 wt% manganese showed its good dispersion in the precursor. The novel Mn/MgAlFe catalysts with 0.5？5.0 wt% manganese oxide showed a high oxidative adsorption rate and sulfur adsorption capacity, and 5.0 wt% Mn/MgAlFe sample was superior to the others for SO2 removal. Moreover, the presence of CO had no obvious effect on the adsorption activity of sulfur transfer catalysts for SO2 uptake.

关键词： sulfur transfer catalyst Mn/MgAlFe SO2 emission control FCC unit

Effects of Temperature and Catalyst to Oil weight Ratio on the Catalytic Conversion of Heavy Oil to Propylene Using ZSM-5 and USY Catalysts

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Journal of Natural Gas Chemistry 2007年第1期16卷 92-99页

作者： Xiaohong li chunyi li Jianfang Zhang chaohe yang honghong shan State Key Laboratory of Heavy Oil Processing China University of Petroleum （Huadong） Dongying 257061 Shandong China

It is useful for practical operation to study the rules of production of propylene by the catalytic conversion of heavy oil in FCC （fluid catalytic cracking）. The effects of temperature and C/O ratio （catalyst to oil weight ratio） on the distribution of the product and the yield of propylene were investigated on a micro reactor unit with two model catalysts, namely ZSM-5/Al2O3 and USY/Al2O3, and Fushun vacuum gas oil （VGO） was used as the feedstock. The conversion of heavy oil over ZSM-5 catalyst can be comparable to that of USY catalyst at high temperature and high C/O ratio. The rate of conversion of heavy oil using the ZSM-5 equilibrium catalyst is lower compared with the USY equilibrium catalyst under the general FCC conditions and this can be attributed to the poor steam ability of the ZSM-5 equilibrium catalyst. The difference in pore topologies of USY and ZSM-5 is the reason why the principal products for the above two catalysts is different, namely gasoline and liquid petroleum gas （LPG）, repspectively. So the LPG selectivity, especially the propylene selectivity, may decline if USY is added into the FCC catalyst for maximizing the production of propylene. Increasing the C/O ratio is the most economical method for the increase of LPG yield than the increase of the temperature of the two model catalysts, because the loss of light oil is less in the former case. There is an inverse correlation between HTC （hydrogen transfer coefficient） and the yield of propylene, and restricting the hydrogen transfer reaction is the more important measure in increasing the yield of propylene of the ZSM-5 catalyst. The ethylene yield of ZSM-5/A1203 is higher, but the gaseous side products with low value are not enhanced when ZSM-5 catalyst is used. Moreover, for LPG and the end products, dry gas and coke, their ranges of reaction conditions to which their yields are dependent are different, and that of end products is more severe than that of LPG. So it is clear that maximizin

关键词： fluid catalytic cracking heavy oil propylene temperature catalyst to oil weight ratio ZSM-5 USY

Synthesis, Characterization and Evaluation of Sulfur Transfer Catalysts for FCC Flue Gas

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China Petroleum Processing & Petrochemical Technology 2014年第2期16卷 59-64页

作者： Jiang Ruiyu shan honghong Zhang Jiling yang chaohe li chunyi Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province Yancheng Institute of Technology State Key Laboratory of Heavy Oil Processing China University of Petroleum (East China) East-China Design Branch China Petroleum Engineering Construction Corporation

In this work, Zr-M(M=Cu, Mn, Ce) type sulfur transfer agent was prepared by impregnation method. Under the condition similar to that in the regenerator of FCC units, the influence of different active metal components and their contents on sulfur transfer agent were investigated. Moreover, the crystalline structure of sulfur transfer agent was characterized by X-ray diffraction(XRD) and Fourier transforms infrared spectroscopy(FT-IR). The result showed that the Zr-Mn sulfur transfer agent could effectively reduce the SO2 content in FCC regenerator flue gas, featuring high SO2 adsorption capacity. The sulfur transfer agent was inactivated in 40—60 min during the test. In the course of reduction reaction, after several reaction cycles, the formation of SO2 ceased and only H2 S was detected as the reduction product.

关键词： fluid catalytic cracking sulfur-transfer catalyst flue gas zirconium

Characterization of Nitrogen Compounds in Vacuum Residue and Their Structure Comparison with Coker Gas Oil

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China Petroleum Processing & Petrochemical Technology 2014年第3期16卷 33-41页

作者： Chen Xiaobo li Teng liu Yibin shan honghong yang chaohe li chunyi State Key Laboratory of Heavy Oil Processing China University of Petroleum

In this study, the heteroatom classes and molecular structures of nitrogen compounds in vacuum residue are characterized by the electrospray ionization(ESI) Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS) combined with the Fourier transform infrared(FT-IR) spectroscopy. The results demonstrate that three basic nitrogen compounds, N1(in which a molecule contains one nitrogen atom, similarly hereinafter), N1O1 and N2, are identified by their positive-ion mass spectra, and three non-basic nitrogen compounds, N1, N1O1, and N1S1, are characterized by their negative-ion mass spectra. Among these nitrogen compounds, the N1 class species are the most predominant. Combined with the data of ESI FT-ICR MS and FT-IR, the basic N1 class species are likely alkyl quinolines, naphthenic quinolines, acridines, benzonacridines, while the abundant non-basic N1 class species are derivatives of benzocarbazole. In comparison with CGO, the N1 basic nitrogen compounds in VR exhibit a higher average degree of condensation and have much longer alkyl side chains.

关键词： nitrogen compounds vacuum residue coker gas oil ESI FT-ICR MS characterization

A high-surface-area silicoaluminophosphate material rich in Brnsted acid sites as a matrix in catalytic cracking

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Journal of Natural Gas Chemistry 2012年第6期21卷 685-693页

作者： Shaoiun Xu Qiang Zhang Zhaoxuan Feng Xiaojing Meng Tongyu Zhao chunyi li chaohe yang honghong shan State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266555ShandongChina School of Chemical Science and Engineering KTH Royal Institute of TechnologySE 10044StockholmSweden Mork Family Department of Chemical Engineering and Materials Science University of Southern CaliforniaCA 90089Los AngelesUSA

A transparent gel-like mesoporous silicoaluminophosphate material （SAP） with molar ratio of Si/Al = 20 was synthesized by hydrothermal method. The physicochemical features of SAP were characterized by XRD, XRF, BET, SEM and FT-IR spectroscopy of pyridine adsorption techniques. The results indicated that incorporation of phosphorus （P） into aluminasilica system altered the basic textural characteristics of aluminasilica. Especially after hydrothermal treatment, the material with large special surface area （up to 492 m2/g） exhibited a good performance on hydrothermal stability. Moreover, the phosphorus modifier can not only increase the amount of Br／＂{o}nsted acidic sites （up to 48.44 μmol/g） and the percentage of weak acidic sites in total acidic sites, but also regulate the acid type, such as the ratio of B/L （Lewis acid/Br？nsted acid） increased to 1.15. The performances of samples as matrices for the catalytic cracking of heavy VGO were investigated. At 520 ℃, the catalysts showed much higher gasoline and diesel oil yields achieving to 45.59 wt% and 19.20 wt%, respectively, and lower coke selectivity （2.86%） than conventional FCC matrices, such as kaolin and amorphous silica-alumina.

关键词： silicoaluminophosphate hydrothermal stability Br nsted acid sites mesoporous hydrothermal synthesis

Synergistic effect of W and P on ZSM-5 and its catalytic performance in the cracking of heavy oil

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Journal of Energy Chemistry 2014年第4期23卷 519-526页

作者： Dongmin Han Nannan Sun Jianwei liu chunyi li honghong shan chaohe yang State Key Laboratory of Heavy Oil Processing China University of Petroleum (East China)

In order to develop the conversion of heavy oil with a high yield of propylene in the catalytic cracking process, ZSM-5 zeolite was modified by tungsten and phosphorus, which was proved to be an effective method. Characterization results show that the improvement of catalytic performance could be correlated to the interaction of phosphorus and tungsten species on ZSM-5. P inhibited the aggregation of tungsten species on ZSM-5 and was conductive to convert the tungsten species with octahedral coordination into tetrahedral coordination. And this ultimately led to that more acid sites were reserved after hydrothermal treatment in the tungsten and phosphorus co-modified ZSM-5 catalyst. Phosphorus species played an important role to restrain the dehydrogenation activity of tungsten. In addition, a model reflecting the interaction between tungsten species and ZSM-5 framework was proposed.

关键词： ZSM-5 tungsten phosphorus catalytic cracking propylene

Studies on the preliminary cracking: The reasons why matrix catalytic function is indispensable for the catalytic cracking of feed with large molecular size

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Journal of Energy Chemistry 2016年第4期25卷 641-653页

作者： Bin Wang Nan li Qiang Zhang chunyi li chaohe yang honghong shan State Key Laboratory of Heavy Oil Processing China University of Petroleum

The matrix catalytic function when cracking the feed oil with large molecular size was systematically studied using three different catalyst configurations, including staged bed, partly mixed bed and completely mixed bed. Results showed that molecules in the feed oil with large molecular size indeed preferred to be first precracked on the matrix surface and then entered into the zeolite pores during the practical reaction process. Furthermore, the matrix catalytic function exhibited a great matrix-precracking ability to large feed molecules, which considerably increased the catalyst activity and the light oil selectivity. Besides the much better accessibility, the matrix-precracking ability was also from the similar capability to crack large feed hydrocarbons into the moderate fragments with that of the zeolite component. More interestingly, the interactions between the matrix catalytic function and the zeolite catalytic function made the catalyst not only exhibit much more catalytic advantages of the zeolite component, but also retain the matrix-precracking ability. As a result, the interactions enhanced the catalyst activity and improved the product distribution at the same time. The matrix catalytic function is indispensable for the catalytic cracking of feed with large molecular size, although the matrix component itself presented an inferior catalytic performance than the zeolite component did. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： Fluid catalytic cracking Matrix Precracking Large hydrocarbons Catalysis relay

Hierarchical ZSM-11 with intergrowth structures:Synthesis,characterization and catalytic properties

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Journal of Energy Chemistry 2013年第5期22卷 761-768页

作者： Qingjun Yu Chaoyue Cui Qiang Zhang Jing Chen yang li Jinpeng Sun chunyi li Qiukai Cui chaohe yang honghong shan State Key Laboratory of Heavy Oil Processing Department of Chemical Engineering China University of Petroleum (East China) Dagang Petrochemical Company PetroChina Corporation

Hierarchical ZSM-11 microspheres with intercrystalline mesoporous properties and rod-like crystals intergrowth morphology have been synthesized using a spot of tetrabutylammonium as a single ***,FTIR,SEM,TEM and N2 adsorption analysis revealed that each individual particle was composed of nanosized rod crystals inserting each other and the intercrystalline voids existing among rods gave a significant mesopore size *** treatment result demonstrated the excellent hydrothermal stability of *** crystallization modes including constant temperature crystallization (one-stage crystallization) and two-stage temperature-varying crystallization with different 1st stage durations were *** results suggested that the crystallization modes were mainly responsible for the adjustable particle size and textural properties of samples while the small amount of tetrabutylammonium bromide was mainly used to direct the formation of both ZSM-11 framework and its intergrowth ***,the performance of optimal ZSM-11 as an active component for the catalytic pyrolysis of heavy oil was also *** with the commercial pyrolysis catalyst,the hierarchical ZSM-11 catalyst exhibited a high selectivity to desired products(LPG+gasoline+diesel),as well as a much lower dry gas and coke yield,plus a high selectivity and yield of light olefins(C=3 C=4)and very poor selectivity to ***,fully open micropore-mesopore connectivity would make such hierarchically porous ZSM-11 zeolites very attractive for applications in clean petrochemical catalysis field.

关键词： intercrystalline mesopore rod-like crystal single template crystallization modes accessibility hydrothermal stability catalytic pyrolysis

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催化裂化技术面临的挑战与机遇

中国石油大学学报（自然科学版） 2017年第6期41卷 171-177页

作者：杨朝合陈小博李春义山红红中国石油大学重质油国家重点实验室山东青岛266580

回顾催化裂化技术的发展历史,提出主要以不同生产目的为依据区分催化裂化、催化裂解和催化热裂解技术的建议;阐述催化裂化技术在现代炼化企业的重要地位,分析催化裂化技术面临的挑战;根据"分子炼油"理念指出催化裂解技术的发展机遇,讨... 详细信息

回顾催化裂化技术的发展历史,提出主要以不同生产目的为依据区分催化裂化、催化裂解和催化热裂解技术的建议;阐述催化裂化技术在现代炼化企业的重要地位,分析催化裂化技术面临的挑战;根据"分子炼油"理念指出催化裂解技术的发展机遇,讨论环烷芳烃有效转化的关键问题;指出催化裂化技术在车用汽油质量升级和炼油化工一体化过程中将持续发挥重要作用。

关键词：催化裂化催化裂解催化热裂解环烷芳烃