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Polycrystalline ZSM-5 Aggregates Induced by Seed and Catalytic Performance in Methanol to Hydrocarbon

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无机材料学报 2024年第8期39卷 945-954,I0010-I0013页

作者： WANG Xuchang JIAO Chuyu JI Zhuo JIAO Qirui QIN Bo DU Yanze ZHENG Jiajun LI Ruifeng Key Laboratory of Coal Science and Technology MOE Research Centre of Energy Chemical&Catalytic TechnologyTaiyuan University of TechnologyTaiyuan 030024China SINOPEC Dalian Research Institute of petroleum and Petrochemicals Co. Ltd.SINOPECDalian 116045China

Synthesis of ZSM-5 zeolite typically utilizes small molecule polyamines or quaternary ammonium salts as organic structure guiding agent(OSDA).By contrast,the OSDA-free hydrothermal synthesis system eliminates the use of organic templates and the subsequent calcination *** not only reduces the cost of synthesis,but also prevents environmental pollution from the combustion of organic templates,representing an eco-friendly *** this,literature suggests that even so-called template-free synthesis systems often involve trace amount of organic substances like *** the present work,a calcined commercial ZSM-5 zeolite was served as seed,with sodium aluminate as aluminum source and silica sol as silicon source,ensuring an entirely template-free synthesis *** ZSM-5 aggregates consisted of rod-like nanocrystals were successfully prepared in the completely OSDA-free *** of the Si/Al ratio in ZSM-5 seed,dosage and crystallization conditions such as crystallization temperature and crystallization time on ZSM-5 synthesis were *** results show that a highly crystallinity ZSM-5 aggregate consisting of primary nano-sized crystals less than 100 nm is produced from a gel precursor with 5.6%(in mass)seed after hydrothermal treatment for 48 ***,the Si/Al ratio in ZSM-5 seed has little effect on the topological structure and pore structure of the synthesized ***,the seeds with a low Si/Al ratio facilitate faster crystallization of zeolite and enhance the acidity,especially the strong acid centers,of the *** catalytic performance of the synthesized polycrystalline ZSM-5 was evaluated during dehydration of methanol and compared with a commercial reference *** results exhibit that as compared with the reference catalyst,the fabricated sample has a longer catalytic lifetime(16 h vs 8 h)attributed to its hierarchical pores derived from the loosely packed primary ***

关键词： ZSM-5 polycrystalline aggregate crystal seed structure guiding agent

Simulation Study on the Migration Range of CO_(2) in the Offshore Saline Aquifer

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哈尔滨工程大学学报（英文版） 2024年第3期23卷 599-607页

作者： Jiayi Wu Zhichao Sheng Jiudi Li SINOPEC Shanghai Offshore Oil&Gas Company Shanghai 200120China

The geological storage of carbon dioxide(CO_(2)) is a crucial technology for mitigating climate change. Offshore deep saline aquifers have elicited increased attention due to their remarkable potential for storing CO_(2). During long-term storage, CO_(2) migration in a deep saline aquifer needs special attention to prevent it from reaching risk points and leading to security issues. In this paper, a mechanism model is established according to the geological characteristics of saline aquifers in an offshore sedimentary basin in china. The CO_(2) migration over 100 years is simulated considering geological changes such as permeability, dip angle, thickness, and salinity. The effects of injection conditions on the CO_(2) migration range are also investigated. Results reveal that the migration range of CO_(2) in the injection period exceeds 70%, even if the postinjection period's duration is five times longer than that of the injection period. As the values of the above geological parameters increase, the migration range of CO_(2) increases, and permeability has a particularly substantial influence. Moreover, the influences of injection rate and well type are considerable. At high injection rates, CO_(2) has a greater likelihood of displacing brine in a piston-like scheme. CO_(2) injected by long horizontal wells migrates farther compared with that injected by vertical wells. In general, the plane migration range is within 3 000 m, although variations in the reservoir and injection parameters of the studied offshore saline aquifers are considered. This paper can offer references for the site selection and injection well deployment of CO_(2) saline aquifer storage. According to the studied offshore aquifers, a distance of at least 3 000 m from potential leakage points, such as spill points, active faults, and old abandoned wells, must be maintained.

关键词： Offshore saline aquifer Carbon dioxide(CO_(2)) Geological storage Migration range Geological changes

Tuning electronic properties of cobalt phthalocyanines for oxygen reduction and evolution reactions

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Science china Chemistry 2024年第1期67卷 398-407页

作者： Jianlin Jiang Zhen Liu Shuaijun Pan Xinnian Xia Bing Qin Yang Hu Xuxu Wang Jiamin Lan Yu Gu Encai Ou Weijian Xu Joseph J.Richardson Rui Guo SINOPEC Research Institute of petroleum Processing Co. Ltd.Beijing 100083China College of Chemistry and chemical Engineering Hunan UniversityChangsha 410082China College of Chemistry and Materials Science Hunan Agricultural UniversityChangsha 410128China Department of chemical Engineering The University of MelbourneParkville 3010Australia College of Environmental Science and Engineering Hunan UniversityChangsha 410082China School of Engineering RMIT UniversityMelbourneVictoria 3001Australia

Metal–phthalocyanines are a class of catalytically active materials promising in energy conversion and storage fields(e.g.,electrocatalysis).However,understanding and controlling the electrochemical properties in metal-phthalocyanine systems is ***,we elucidate the electrocatalytic origins of a series of cobalt-phthalocyanine molecular catalysts and finetune their electronic properties at the atomic level,both experimentally and *** interactions between the cobalt center and the local coordination environment are regulated by introducing either electron-donating or electron-withdrawing groups on the phthalocyanine ligand,and the spin-orbit splitting of cobalt is increased by~0.15 eV compared with the nonsubstituted ***,the aminated cobalt phthalocyanine-based electrocatalysts exhibit low free energies in the ratedetermining steps of the oxygen reduction(-1.68 eV)and oxygen evolution reactions(0.37 eV).This contributes to the high electrocatalytic activity(e.g.,a halfwave potential of 0.84 V and an overpotential of 0.30 V at 10 mAcm^(-2)),featuring a high selectivity of a four-electron pathway(i.e.,a negligible by-product of hydrogen peroxide).These catalysts also exhibit exceptional kinetic current density(Tafel slope of 100 mV dec^(-1))in oxygen reduction reactions,in addition to a superior power density(158 mWcm^(-2))and a high cycling stability(>1,300 cycles)in Zn-air batteries,outperforming the commercial Pt/C and/or RuO2counterparts.

关键词： interfacial wettability molecular catalysts carbon nanotubes density functional theory electrochemistry

Lewis acid-oxygen vacancy interfacial synergistic catalysis over SO4^2-/Ce0.84Zr0.16O2-WO3-ZrO2 for N,N-diethylation of aniline with ethanol

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Journal of Rare Earths 2020年第11期38卷 1190-1200,I0002页

作者： Yacheng Liu Qifan Mao Xiaoyan Cao Xin Huang Kaijun Wang Can Wang Shuo Li Zhenggui Gu School of Chemistry and Materials Science Nanjing Normal UniversityNanjing 210023China Jiangsu Province Key Laboratory of Materials Cycling and Pollution Control Nanjing 210023China

Herein,a new mechanism involving Lewis acid-oxygen vacancy interfacial synergistic catalysis fo r aniline N,N-diethylation with ethanol was proposed,and the SO4^2-/Ce0.84Zr0.16O2-WO3-ZrO2 catalyst(SCWZ)with both Lewis acid sites and oxygen vacancies was synthesized by the hydrothermal method,which shows better catalytic activity than the reported solid acidic ***,the SO4^2-/ZrO2(SZ)and SO4^2-/WO3-ZrO2(SWZ)catalysts were also prepared and compared with SCWZ to investigate the synergistic effect of each *** SO4^2-and WO3 mainly generate Lewis acid by bonding with ZrO2,which is beneficial for the fracture of the N-H bond in *** Ce0.84Zr0.16O2 solid solution mainly plays a vital role in generating the oxygen vacancies as the interface active species,which can participate in stripping-OH from ethanol,then the carbocation will also be released,which only needs1.3805 kcal/mol energy,calculated by density functional theory(DFT),to be *** comparison,the traditional reaction mechanism needs the Br■nsted acidic sites to promote the protonation of ethanol,then dehydration and subsequent formation of carbocation followed,and 108.6846 kcal/mol energy needs to be input,which is far higher than that of the new *** apparent activation energy(Ea)over SCWZ was measured by experiment to be 34.09 kJ/mol,which is much lower than that of SWZ(47.10 kJ/mol)and SZ(54.37 kJ/mol),illustrating comparatively preferable kinetics for SCWZ than that of SWZ and ***,the conversion of aniline and selectivity to N,N-diethylaniline over SCWZ reach almost 100%and 73%,respectively,The SCWZ can be renewed for 4 times without rapid deactivation,and the longevity of SCWZ is longer than that of SWZ and SZ,as the loaded SO4^2-and tetragonal ZrO2 are stabilized by Ce0.84Zr0.16O2 and WO3,respectively.

关键词： N,N-diethylation Lewis acid Bronsted acid Oxygen vacancy Activation energy Density functional theory

A Study of Lead Corrosion of Diesel Engine Oil

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china petroleum Processing & Petrochemical Technology 2018年第2期20卷 71-78页

作者： Xu Jie Xia Qinghong Zhang Feng Wu Zhiqiang SINOPEC Research Institute of petroleum Processing Beijing 100083

The effect of base oils,sulfur-containing multi-functional additives and dispersants in formulated diesel lubricants on lead corrosion was evaluated by a self-established high temperature corrosion bench *** lead coupons were analyzed by XPS to determine the resulting surface *** results showed a close correlation between the oxidation stability of base oil blend and the lead corrosion of formulated diesel *** zinc dialkyldithiophosphate(ZDDP)and zinc dialkyldithiocarbamate(ZDDC)have formed different protective films on lead coupon surfaces.A more or less amount of the protective film formed is the main factor affecting the degree of lead *** glassy zinc phosphates protective film formed by ZDDP is more effective than the zinc sulfides film formed by *** interaction between dispersants and ZDDP had a significant impact on lead corrosion.

关键词： diesel engine oil lead corrosion base oil ZDDP ZDDC XPS

Oxidation of Fe-Cr-Ni Alloys in a Low Oxygen Partial Pressure Atmosphere to Mitigate Coke Formation

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中国炼油与石油化工:英文版 2023年第3期25卷 49-59页

作者： Wang Hongxia Wang Guoqing Zhang Lijun Wang Shenxiang Jia Jingsheng Cui Lishan Sinopec(Beijing)Research Institute of chemical Industry Co. Ltd.Beijing 100013China Departments of Materials Science and Engineering China University of PetroleumBeijing 102249China

Anti-coking oxide films were prepared on a 25Cr35Ni and 35Cr45Ni alloy surface under the low oxygen partialpressure atmosphere of a H2-H2O mixture. The composition and phase structure of the oxide films were analyzed by energydispersive spectroscopy (EDS), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The anti-cokingperformance of a mini tube made of a HP40 (25Cr35Ni) alloy was evaluated on a bench scale pyrolysis and coking test *** results showed that the surface Fe and Ni content decreased after the oxidation of the two alloys in a low oxygen partialpressure atmosphere. The oxide films were mainly composed of MnCr_(2)O_(4) and Cr_(2)O_(3). The average mass of coke in the minitube with oxide film decreased by 87% relative to that of a tube without an oxide film when the cracking temperature was 900℃. The ethylene, propylene, and butadiene yields in the pyrolysis tests were almost the same for the mini tubes withand without an oxide film. The oxide film on the alloy surface effectively inhibited catalytic filamentous coke *** industrial test showed that the run length of the cracking furnace with the in-situ coating technology was significantlyextended.

关键词： Fe-Cr-Ni alloy low oxygen partial pressure oxide film anti-coking ethylene cracking furnace in-situ coating

Multiscale Modeling and Simulations of Flows in Naturally Fractured Karst Reservoirs

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Communications in Computational Physics 2009年第6期6卷 162-184页

作者： Peter Popov Yalchin Efendiev Guan Qin Institute for Scientific Computation Texas A&M UniversityCollege StationTX 77843 Department of Mathematics Texas A&M UniversityCollege StationTX 77843

Modeling and numerical simulations of fractured,vuggy,porus media is a challenging problem which occurs frequently in reservoir *** problem is especially relevant in flow simulations of karst reservoirs where vugs and caves are embedded in a porous rock and are connected via fracture networks at multiple *** this paper we propose a unified approach to this problem by using the StokesBrinkman equations at the fine *** equations are capable of representing porous media such as rock as well as free flow regions(fractures,vugs,caves)in a single system of *** then consider upscaling these equations to a coarser *** cell problems,needed to compute coarse-scale permeability of Representative Element of Volume(REV)are discussed.A mixed finite element method is then used to solve the Stokes-Brinkman equation at the fine scale for a number of flow problems,representative for different types of vuggy *** is also performed by numerical solutions of Stokes-Brinkman cell problems in selected *** isolated vugs in porous matrix as well as vugs connected by fracture networks are analyzed by comparing fine-scale and coarse-scale flow *** different types of fracture networks,representative of short-and long-range fractures are studied *** is also shown that the Stokes-Brinkman equations can naturally be used to model additional physical effects pertaining to vugular media such as partial fracture with fill-in by some material and/or fluids with suspended solid particles.

关键词： Homogenization Stokes equation Brinkman equation porous media

Improving Catalytic Stability and Coke Resistance of Ni/Al_(2)O_(3) Catalysts with Ce Promoter for Relatively Low Temperature Dry Reforming of Methane Reaction

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chemical Research in Chinese Universities 2022年第4期38卷 1032-1040页

作者： HE Lulu CHEN Xin REN Yuanhang YUE Bin TSANG Shik Chi Edman HE Heyong Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan UniversityShanghai200438P.R.China Wolfson Catalysis Centre Department of ChemistryUniversity of OxfordOxfordOX13QRUK

A series of Ni catalysts supported on alumina with different Ce contents(1.0%–6.0%,mass fraction)was prepared by the impregnation method and used for dry reforming of methane(DRM)at a relatively low temperature of 650°*** promotion effect of Ce with different loading amounts on the physicochemical properties of the catalysts was systematically characterized by transmission electron microscopy(TEM),X-ray diffraction(XRD),N_(2) adsorption-desorption,thermo elemental IRIS Intrepid inductively coupled plasma atomic emission spectrometer(ICP-AES),UV-visible diffuse reflectance spectroscopy(UV-Vis DRS),Fourier transformation infrared(FTIR)spectra,H_(2)-temperature programmed reduction(H_(2)-TPR)analysis,H_(2)-temperature programmed desorption(H_(2)-TPD),and The X-ray photoelectron spectroscopy(XPS)*** results indicate that all the catalysts mainly exist in the NiAl_(2)O_(4) phase after being calcined at 750°C with small Ni particle sizes due to the strong metal-support interaction derived from the reduction of the NiAl_(2)O_(4) *** Ce-promoted catalysts show better catalytic performance as well as the resistance against sintering of Ni particles and deposition of carbon compared to the Ni/Al_(2)O_(3) *** Ni-6Ce/Al_(2)O_(3) exhibits the best catalytic stability and coke resistance among the four catalysts studied,which is due to its small Ni nanoparticles sizes,excellent reducibility as well as high amount of active oxygen *** a 400 h stability test for DRM reaction at 650°C,Ni-6Ce/Al_(2)O_(3) exhibits less coke deposition and small growth of Ni *** work provides a simple way to preparing the Ni-Ce/Al_(2)O_(3) catalyst with enhanced catalytic performance in *** Ni-6Ce/Al_(2)O_(3) catalyst has great potential for industrial application due to its anti-sintering ability and resistance to carbon deposition.

关键词： Dry reforming of methane(DRM) Cerium oxide Ni-based catalyst Coke resistance

Fabrication of Pd-Nb bimetallic doped organosilica membranes by different metal doping routes for H_(2)/CO_(2) separation

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Chinese Journal of chemical Engineering 2021年第8期34卷 67-75页

作者： Hengfei Zhang Yibin Wei Shufeng Niu Hong Qi State Key Laboratory of Material-Oriented chemical Engineering Membrane Science and Technology Research CenterNanjing Tech UniversityNanjing 210009China Hongyi Ceramic Membranes Research Institute Nanjing Hongyi Ceramic Nanofiltration Membranes Co.Ltd.Nanjing 210009China

Monometallic doping has proved its superiority in improving either permselectivity or H_(2) permeability of organosilica membranes for H_(2)/CO_(2) separation,but it is still challenging to break the trade-off ***,we report a series of Pd-Nb bimetallic doped 1,2-bis(triethoxysilyl)ethane(Pd-Nb-BTESE,PNB)membranes with different metal doping routes for simultaneously improving H_(2) permeance and H_(2)/CO_(2) permselectivity by the synergetic effects of Pd and *** doped Pd can exist in the BTESE network as nanoparticles while the doped Nb is incorporated into BTESE network forming Nb-O-Si covalent *** metal doping routes significantly influence the microstructure of PNB networks and gas separation performance of the PNB *** found that the PNB membrane with Pd doping priority(PNB-Pd)exhibited the highest surface area and pore volume,comparing with Nb doping priority(PNB-Nb)or Pd-Nb simultaneous doping(PNB-PdNb).The PNB-Pd membrane could not only exhibit an excellent H_(2) permeance of~10^(−6) mol·m^(−2)·s^(−1)·Pa^(−1) but also a high H_(2)/CO_(2) permselectivity of *** findings may provide novel insights into preparation of bimetallic doped organosilica membranes with excellent H_(2)/CO_(2) separation performance.

关键词： Hydrogen Separation Membranes Bimetallic doping Organosilica