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| 1 | Catalyst design strategies towards highly shape-selective HZSM-5 for paraxylene through toluene alkylation显示文摘With the shape selective zeolite catalyst,toluene alkylation with methanol to para-xylene(MTPX)technology could produce highly pure para-xylene(PX)in one step.The lower feedstock cost and less energy consumption in products separation make it more competitive compared to the current toluene disproportionation route.Thus,MTPX is regarded as the most reasonable production route for PX production.This article reviews the strategies that applied to the preparation of high-performance catalysts for MTPX,with special focus on the precise control of pore dimension and acid sites distribution in zeolite to achieve the highest selectivity to PX.The outlook of the MTPX catalyst is also proposed to guide the catalyst development in the field. | Xin Huang Ruizhuang Wang Xu Pan Chuanfu Wang Maohong Fan Yufei Zhu Yonggang Wang Jin Peng | 2020 | Green Energy & Environment2020，5，4： | 10 |
| 2 | Alkylation Activity of Benzene with Syngas over Cu-based Catalysts显示文摘A series of Cu-based catalysts were developed for alkylation of benzene with syngas. The catalyst samples were prepared by the impregnation method, and were characterized by XRD, XRF, NH3-TPD, and TEM and evaluated in a fixed bed reactor. The optimized reaction temperature of Cu/Al2O3/ZSM-5 catalyst was 350 ℃, while higher contents of copper were conducive to alkylation of benzene with syngas. The new medium strength acid centers in the catalyst created by Cu were beneficial to alkylation. Hydrogenation reaction of CO was executed on the metal centers without dissociation, Dimethyl ether(DME) was the major intermediate over Cu-based catalysts. Higher selectivity of methylation and lower selectivity of heavy aromatics were confirmed after the second metal(Zn, Mn, or V) was added to the copper catalyst. Cu was partly covered by Zn in the Cu-Zn/Al2O3/ZSM-5 catalyst leading to low dispersion and low activity of copper. Cu-Mn/Al2O3/ZSM-5 catalyst possessed the best yield of methylation product. Cu-Mn composite oxides were probably formed in fresh catalyst, which blocked the sintering of Cu in the reaction process. The loading of Cu decreased dramatically after the introduction of V, while causing an increase of the amount of medium strength acid centers at the same time. V prevented the sintering of copper particles during the reducing process and had a promoting effect on the activity of Cu. | Zhao Xuebin Zeng Feng Zhao Bin Gu Haohui | 2015 | China Petroleum Processing & Petrochemical Technology2015，17，1： | 8 |
| 3 | H_3PO_4/MCM-41催化苯酚与叔丁醇气相烷基化反应(英文)显示文摘The catalytic performance of Al-MCM-41 containing 5-35 wt% H3PO4 was studied for the vapor phase alkylation of phenol with tert-butyl alcohol(TBA) from 383 to 493 K.4-Tert-butyl phenol was produced as the main product with moderate selectivity.The product distribution depends on the reaction temperature,number of acid sites,and the Brnsted to Lewis sites ratios.A lower molar ratio of reactants(TBA/phenol = 2) and a higher space velocity facilitated the production of 4-tert-butyl phenol.The influence of various parameters such as temperature,reactant feed molar ratio,feed rate,and time on stream were investigated for conversion yield and product selectivity. | Mehran GHIACI | 2010 | 催化学报2010，31，7： | 7 |
| 4 | Alkylation mechanism of benzene with 1-dodecene catalyzed by Et_3NHCl-AlCl_3显示文摘The isotope exchange method was employed to investigate the catalytic mechanism of ionic liquid in alkylation of benzenes with olefins.It is proposed that alkylation was induced by the Lewis acid AlCl3 which attracted π electrons of 1-dodecene to shift toward 1-carbon,thus forming a carbonium ion.The carbonium ion further reacted with benzenes to form a complex.Due to unstabilit of the complex,a deuterated ring proton was transferred into an electronegative 1-carbon of the side chain to substitute for the AlCl3,accordingly 2-phenyldodecane was generated. | QI GuoPeng 1,JIANG Feng 1,SUN XueWen 2 & ZHAO SuoQi 2 1School of Chemical Engineering,Tianjin University,Tianjin 300072,China 2State key Laboratory of Heavy Oil Processing,Petroleum University of China,Beijing 102249,China | 2010 | Science China Chemistry2010，53，5： | 7 |
| 5 | Study on Catalytic Alkylation of Benzene with Methanol over ZSM-22 and ZSM-35显示文摘The ZSM-22 and ZSM-35 zeolites were synthesized via the hydrothermal crystallization method. The samples were characterized by XRD, SEM, N_2 adsorption-desorption, NH_3-TPD, TPO, TG, and Raman spectrometry, and the results showed that ZSM-22 and ZSM-35 possessed similar microporous volume and acidity. In the alkylation of benzene with methanol, ZSM-22 and ZSM-35 showed different coke location, coking rate and graphitizing degree. Compared with the industrial ZSM-5, ZSM-22 and ZSM-35 both showed higher selectivity of toluene and xylene(93.63% and 96.50%,respectively) during the alkylation of benzene with methanol, and the selectivity of para-xylene in xylene isomers was51.96% and 41.45%, respectively. Meanwhile, the selectivity of ethylbenzene and C_9^+ aromatics was also lower than that of industrial ZSM-5. | Li Yunsheng Wen Zhenhao Wei Zhenhao Yang Fan Zhu Xuedong | 2017 | China Petroleum Processing & Petrochemical Technology2017，19，4： | 5 |
| 6 | Synthesized high-silica hierarchical porous ZSM-5 and optimization of its reaction conditions in benzene alkylation with methanol显示文摘In our present work, the high-silica hierarchical porous ZSM-5 with appropriate Br(o|¨)nsted acidity and hierarchical porous structure was synthesized by sol-gel method for continuously catalytic conversion of benzene alkylation with methanol to xylene. The effects of temperature, pressure, benzene/methanol molar ratio and weight hour space velocity(WHSV) on the catalytic performance of the catalyst were investigated as well. As a result, the high-silica hierarchical porous ZSM-5 showed great performance as the yield of xylene was up to 41.1% under the optimum reaction conditions(500 ℃,0.1 MPa,M_(benzene)/M_(methanol)= 1:1.5 and WHSV=4 h 1), while the selectivity to by-product, ethylbenzene, was well suppressed(below 0.1%). In addition, the catalyst structure and properties were characterized by the means of XRD, IR, TPD,SEM, TEM and N_2 physical adsorption technologies. | Jiayao Rui Jinghui Lyu Hualei Hu Qunfeng Zhang Qingtao Wang Xiaonian Li | 2019 | Chinese Chemical Letters2019，30，3： | 5 |
| 7 | 铂和HF掺杂的H-ZSM-5分子筛催化甲苯与甲醇烷基化反应(英文)显示文摘Toluene was alkylated with methanol in a flow type reactor at temperatures between 300 and 500 °C using H-ZSM-5 zeolite, 0.2%Pt/H-ZSM-5 and hydrofluorinated 0.2%Pt/H-ZSM-5 with HF concentrations of 1.0%, 2.0%, 3.0%, or 4.0%. Pt primarily enhances toluene conversion, total xylenes production, and p-xylene relative to its thermodynamic equilibrium. As the concentration of HF increases from 1.0% to 3.0%, the catalyst activity increases because of the increase in the number of acid sites and their strength. Additionally, the surface area and Pt dispersion also increases. An advantage of increased HF doping is that the formation of voluminous trimethylbenzene (TMB) byproducts is inhibited. However, at a HF concentration of 4.0%, Al and Si are partially leached and then deposited mostly in the wider catalytic pores. This was determined by evaluating the pore volume distribution and we determined that reactivity inhibition was ob-viously present and was due to diffusion restriction. | Ahmed K. ABOUL-GHEIT Ateyya A. ABOUL-ENEIN Ahmed E. AWADALLAH Salwa A. GHONEIM Eman A. EMAM | 2010 | 催化学报2010，31，10： | 4 |
| 8 | Deactivation mechanism of beta-zeolite catalyst for synthesis of cumene by benzene alkylation with isopropanol显示文摘The alkylation of benzene with isopropanol over beta-zeolite is a more cost-effective solution to cumene production. During the benzene alkylation cycles, the cumene selectivity slowly increased, while the benzene conversion presented the sharp decrease due to catalyst deactivation. The deactivation mechanism of betazeolite catalyst was investigated by characterizing the fresh and used catalysts. The XRD, SEM and TEM results show that the crystalline and particle size of the beta-zeolite catalyst almost remained stable during the alkylation cycles. The drop in catalytic activity and benzene conversion could be explained by the TG, BET,NH_3-TPD and GC–MS results. The organic matters mainly consisted of ethylbenzene, p-xylene and 1-ethyl-3-(1-methyl) benzene produced in the benzene alkylation deposited in the catalyst, which strongly reduced the specific surface area of beta-zeolite catalyst. Moreover, during the reaction cycles, the amount of acidity also significantly decreased. As a result, the catalyst deactivation occurred. To maintain the catalytic performance,the catalyst regeneration was carried out by using ethanol rinse and calcination. The deactivated catalyst could be effectively regenerated by the calcination method and the good catalytic performance was obtained. | Yefei Liu Yang Zou Hong Jiang Huanxin Gao Rizhi Chen | 2017 | Chinese Journal of Chemical Engineering2017，25，9： | 4 |
| 9 | Enhancement of Bio-based para-Xylene Selectivity in Catalytic Fast Pyrolysis of Cellulose Using a Surface-modified Mg/P/HZSM-5 Catalyst显示文摘With the growing consumption of oil, the production of /?-xylene(PX) from renewable biomass has gained significant attention recently. This work demonstrated that cellulose, a main component in lignocellulosic biomass, was directly converted into PX over the Mg/P surface-modified zeolites. The catalysts modified by the incorporation of P2O5 and MgO into HZSM-5(HZ) promoted the isomerization of zw-/o-xylenes to p-xylene. The PX selectivity was greatly enhanced using the modified zeolites due to the deactivation of external surface and the adjustment of pore entrance. In addition, the addition of methanol to cellulose was beneficial to increase the selectivity of xylenes due to the alkylation reactions and the Diels-Alder reactions between cellulose-derived furans and methanol-derived olefins. The highest PX yield of 10.7%(molar fraction) with a high PX selectivity in xylenes(97.1%) was obtained over the 10%Mg/5%P/HZ catalyst. The reaction pathway for the formation ofp-xylene was addressed according to the study of the key reactions and the characterization of catalysts. | WANG Yulan FAN Minghui ZHU Lijuan WANG Shengfei HE Yuting LI Quanxin | 2019 | Chemical Research in Chinese Universities2019，35，3： | 4 |
| 10 | Modeling of Isobutane/Butene Alkylation Using Solid Acid Catalysts in a Fixed Bed Reactor显示文摘A dynamic mass transfer model of isobutane/butene alkylation over solid acid catalysts in a fixed bed reactor was established. In the model, a modified equation for the relationship between point activity and effective diffusion coefficient was proposed. It is found that the simulation results fit the experimental data well and the breakthrough time of the bed layer is predicted accurately. By modeling the alkylation process, the time-space distribution of butene and point activity profiles of catalysts can be obtained. Furthermore, the reasons for the deactivation of solid acid catalysts were investigated. It indicates that the main reason for the deactivation of catalysts is the site coverage near the inlet of the reactor, while it is ascribed to the steric effect in the region far away from the inlet. | Liu Zheng Tang Xiaojin Hu Lifeng Hou Shuandi | 2016 | China Petroleum Processing & Petrochemical Technology2016，18，2： | 3 |
| 11 | Shaped binderless ZSM-11 zeolite catalyst prepared via a dry-gel conversion method:Characterization and application for alkylation of benzene with dimethyl ether显示文摘Shaped binderless ZSM-11 zeolite catalysts were synthesized via a dry-gel conversion technique from 70ZSM-11/30 SiO_2mix extrudates. 1,6-hexanediamine combined with tetrabutylammonium bromide was proved to be the best structure directing agent for the synthesis of the binderless ZSM-11 catalyst, without adding other alkaline materials. The 70HZSM-11/30 SiO_2mix serials materials crystallized for different times were detected by X-ray diffraction(XRD), nuclear magnetic resonance(NMR), scanning electron microscopy(SEM), transmission electron microscopy(TEM), scanning transmission electron microscopy–energy dispersive spectroscopy(STEM–EDS) techniques, and so on. In order to investigate the possible crystallization mechanism, the textural and structural properties of 70HZSM-11/30 SiO_2mix serials samples were further characterized by N_2 adsorption–desorption. Acid properties were determined by temperature-programed desorption of NH_3(NH_3-TPD) and pyridine adsorption-infrared(Py-IR) measurements. In the alkylation of benzene with dimethyl ether, the serials catalysts exhibited different benzene conversions. 70HZSM-11/30 SiO_2mix showed the lowest benzene conversion while sample 70HZSM-11/30 SiO_2mix-6.5h synthesized only for 6.5h displayed a higher benzene conversion, even higher than the value over 70HZSM-11/30Al_2O_3mix. Extending the crystallization time, the obtained samples displayed the increased benzene conversion in general under the same reaction conditions. In the end, the relation of physicochemical properties with the reaction performance was investigated. | Wanshuo Zhang Shuang Zhang Wenjie Xin Hui Liu Yongchen Shang Xiangxue Zhu Shenglin Liu Longya Xu | 2017 | Journal of Energy Chemistry2017，26，3： | 3 |
| 12 | Effect of Particle Shape on Catalyst Deactivation during 2-Butene and Isobutane Alkylation of Liquid Phase in Fixed-Bed Reactor Using Particle-Resolved CFD Simulation显示文摘How catalyst shape affects its deactivation is a crucial issue for quickly decaying catalysts such as zeolite in 2-butene and isobutane alkylation.In this work,steady simulations are used to determine the temperature and species distribution in fixed beds filled with particles of four shapes.Subsequently,unsteady simulations are used to study the deactivation behavior of the catalysts based on the steady simulation results.We describe the deactivation rate and type of catalyst deactivation by defining a local internal diffusivity,which is affected by catalytic activity.The results reveal that the internal diffusion distance of the catalyst determines the deactivation rate,whereas the local internal diffusivity determines its deactivation type. | Zhang Sizhen Zhu Zhenxing Xin Feng Chu Menghan | 2022 | China Petroleum Processing & Petrochemical Technology2022，24，4： | 2 |
| 13 | Catalytic process modeling and sensitivity analysis of alkylation of benzene with ethanol over MIL-101(Fe) and MIL-88(Fe)显示文摘A solvothermal method was used to synthesize MIL-101(Fe)and MIL-88(Fe),which were used for alkylation of benzene.The synthesized catalysts were characterized by X-ray diffraction,Fourier transform infrared spectroscopy,field emission scanning electron microscope,dynamic light scattering,and BET techniques.Metal-organic frameworks(MOFs)were modeled to investigate the catalytic performance and existence of mass transfer limitations.Calculated effectiveness factors revealed absence of internal a nd external mass transfer.Sensitivity analysis revealed best operating conditions over MIL-101 at 120℃ and 5 bar and over MIL-88 at 142℃ and 9 bar. | Ehsan Rahmani Mohammad Rahmani | 2020 | Frontiers of Chemical Science and Engineering2020，14，6： | 2 |
| 14 | Synthesis of 2-Isopropyl Naphthalene Catalyzed by Et_3NHCl-AlCl_3 Ionic Liquids显示文摘In this paper, 2-isopropyl naphthalene has been synthesized by the reaction of naphthalene and isopropyl bromide, using triethylamine hydrochloride-aluminum chloride ionic liquid as the catalyst. The effect of the catalyst composition, the reaction time, the reaction temperature, the ionic liquid dosage, as well as the molar ratio of the reagents on the 2-isopropyl naphthalene yield was systematically investigated. The optimal reaction conditions cover: an AlCl3 to Et3NHCl ratio of 2.0, a reaction time of 3 h, a reaction temperature of 15.0 ℃, a volume fraction of ionic liquid to the mixture(isopropyl bromide, n-dodecane and n-hexane) of 9%, and a naphthalene/isopropyl bromide molar ratio of 4.0. Under the optimal reaction conditions, the conversion of isopropyl bromide reached 98% and the selectivity of 2-isopropyl naphthalene was equal to 80%. The test results verified good catalytic activity upon using Et3NHCl-AlCl3 ionic liquid as the catalyst for alkylation of naphthalene with isopropyl bromide. The activity of the ionic liquid remains unchanged after it has been recycled for 4 times. | Li Chenmin Qi Xin Tang Xiangyang | 2014 | China Petroleum Processing & Petrochemical Technology2014，16，1： | 2 |
| 15 | Alkylation of Isobutane and Isobutene in Acidic Polyether Ionic Liquids显示文摘The Br?nsted-acidic polyether ionic liquids(ILs)with different polymerization degrees(n value)were prepared via the reaction of tetramethylguanidine and epoxy ethane,followed by successive reactions with 1,3-propane sultone and trifluoromethanesulfonic acid(TfOH).The prepared ILs were characterized by infrared spectroscopy and 1H nuclear magnetic resonance spectroscopy,and their thermal stability was determined by thermal gravimetry.The synthesized polyether ILs coupled with TfOH were used to catalyze the alkylation reaction of isobutane and isobutene for the preparation of alkylate gasoline.The polyether ILs could improve the substrate dissolution and promote the separation of the catalyst from the products.The ideal IL(n=94)was determined.The optimized alkylation reaction conditions covered:a VTfOH/VIL ratio of 0.35,a reaction temperature of 40℃,a reaction time of 50 min,and a stirring speed of 800 r/min.The conversion of isobutene was 92.4%and the selectivity for the C8-product was 81.6%.Under optimal conditions,the catalyst life was determined and TfOH showed improved cyclic performance in the polyether ILs.After 8 operating cycles,the catalytic activity of the catalyst showed negligible decline. | Yu Fengli Gu Yulong Liu Qichun Xie Congxia | 2019 | China Petroleum Processing & Petrochemical Technology2019，21，3： | 2 |
| 16 | Radical Heteroarylalkylation of Alkenes via Three-Component Docking-Migration Thioetherification Cascade显示文摘A novel,rational-designed approach to access various heteroaryl-substituted alkyl thioethers was developed via docking-migration cascade process.By utilizing three components involving alkene,dual-function reagent,and thioetherificating reagent,radical heteroarylalkylation of alkenes followed by thiolation of the alkyl radical intermediates proceeded smoothly,manifesting well compatibility of substrates and cascade transformations.Furthermore,this protocol also features mild conditions,broad substrate scope,and wide product diversity. | Tao Niu Jige Liu Xinxin Wu Chen Zhu | 2020 | Chinese Journal of Chemistry2020，38，8： | 2 |
| 17 | Cu-Catalyzed Selective Oxy-Cyanoalkylation of Allylamines with Cycloketone Oxime Esters and CO2显示文摘Summaryof main observation and conclusion The radical-initiated carboxylativecyclization of allylamines with CO2represents an efficientand highly promising strategy to afford valuable 2-oxazolidinones.However,the radical precursorsand pathways to generate radicals in such processes are still lim-ited.Herein,we report the firstCu-catalyzed selective oxy-cyanoalkylation of allylamines with cycloketone oxime esters and CO2viaC-C bond cleavage.Many cyanoalkyl-substituted 2-oxazolidinones are obtained in moderate togood yields withhigh regio-and chemo-selectivities.The utility ofthis re-dox-neutral and cyanide-free method is demonstrated with mild conditions,broad substrate scope,good functional group tolerance and easy scalability. | Chuan-Kun Ran He Huang Xing-Hui Li Wei Wang Jian-Heng Ye Si-Shun Yan Bi-Qin Wang Chun Feng Da-Gang Yu | 2020 | Chinese Journal of Chemistry2020，38，1： | 2 |
| 18 | Enantioselective O-allylic alkylation of Morita-Baylis-Hillman carbonates with oxime显示文摘The enantioselective O-allylic alkylation of acetophenone oxime with various Morita-Baylis-Hillman (MBH) carbonates has been accomplished by the catalysis of a commercially available cinchona alkaloid (DHQD)2PHAL. The corresponding O-allylic products were obtained in moderate to excellent yields up to 96% ee. | HU ZeKai CUI HaiLei JIANG Kun CHEN YingChun | 2009 | Science China Chemistry2009，52，9： | 1 |
| 19 | Controlled direct synthesis of single- to multiple-layer MWW zeolite显示文摘The minimized diffusion limitation and completely exposed strong acid sites of the ultrathin zeolites make it an industrially important catalyst especially for converting bulky molecules.However,the structure-controlled and large-scale synthesis of the material is still a challenge.In this work,the direct synthesis of the single-layer MWW zeolite was demonstrated by using hexamethyleneimine and amphiphilic organosilane as structure-directing agents.Characterization results confirmed the formation of the single-layer MWW zeolite with high crystallinity and excellent thermal/hydrothermal stability.The formation mechanism was rigorously revealed as the balanced rates between the nucleation/growth of the MWW nanocrystals and the incorporation of the organosilane into the MWW unit cell,which is further supported by the formation of MWW nanosheets with tunable thickness via simply changing synthesis conditions.The commercially available reagents,well-controlled structure and the high catalytic stability for the alkylation of benzene with 1-dodecene make it an industrially important catalyst. | Jie-Qiong Chen Yu-Zhao Li Qing-Qing Hao Huiyong Chen Zhao-Tie Liu Chengyi Dai Jianbo Zhang Xiaoxun Ma Zhong-Wen Liu | 2021 | National Science Review2021，8，7： | 1 |
| 20 | SYNTHESIS OF POLYISOBUTYLENE WITH SEC-ARYLAMINO TERMINAL GROUP BY COMBINATION OF CATIONIC POLYMERIZATION WITH ALKYLATION显示文摘The highly reactive polyisobutylenes(PIBs) withα-double bonds(87.5 mol%) or tert-chloro(tert-Cl) groups(95 mol%) could be prepared via the cationic polymerization of isobutylene(IB) coinitiated by BF_3 or TiCl_4 respectively.The Friedel-Crafts alkylation of diphenylamine(DPA) with the highly reactive PIB withα-double bonds was further conducted under different conditions,such as at different alkylation temperature,in the mixed solvents of CH_2Cl_2/n-hexane with different solvent polarity and at DPA conce... | 吴一弦 | 2009 | Chinese Journal of Polymer Science2009，27，4： | 1 |
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