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Frontiers of Chemical Science and Engineering 2020年第4期14卷 651-660页

作者： Feichao Wu Yanling Wang xiongfu zhang State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian 116024China

In this work,a thin zirconium-based UiO-66 membrane was successfully prepared on an alumina hollow fiber tube by flow synthesis,and was used in an attempt to remove p-nitrophenol from water through a nanofiltration *** main factors,including flow rate and synthesis time,were investigated to optimize the conditions for membrane *** optimal synthesis conditions,a thin UiO-66 membrane of approximately 2 um in thickness was fabricated at a flow rate of4 mL.h for 30 *** p-nitrophenol rejection rate for the as-prepared UiO-66 membrane applied in the removal of p-nitrophenol from water was only 78.1%due to the existence of membrane defects caused by coordinative defects during membrane ***-synthetic modification of the UiO-66 membrane was carried out using organic linkers with the same flow approach to further improve the nanofiltration *** result showed that the p-nitrophenol rejection for the post-modified membrane was greatly improved and reached over 95%.Moreover,the post-modified UiO-66 membrane exhibited remarkable long-term operational stability,which is vital for practical application.

关键词： UiO-66 membrane flow synthesis nanofiltra-tion p-nitrophenol removal

Wormholelike mesoporous carbon supported Pt Ru catalysts toward methanol electrooxidation

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Journal of Energy Chemistry 2017年第1期26卷 200-206页

作者： Weifeng Liu Xiaoping Qin xiongfu zhang Zhigang Shao Baolian Yi State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian Institute of Chemical Physics Chinese Academy of Sciences

Wormholelike mesoporous carbons (WMCs) with three different pore diameters (D-P), namely WMC-F7 (D-p = 8.5 nm), WMC-F30 (D-p =4.4 nm), and WMC-F0 (D-p =3.1 nm) are prepared via a modified sol-gel process. Then PtRu nanoparticles with the particle size (40 of 3.2 nm supported on WMCs are synthesized with a modified pulse microwave-assisted polyol method. It is found that the pore diameter of WMCs plays an important role in the electrochemical activity of PtRu toward alcohol electrooxidation reaction. PtRu/WMC-F7 with D-p > 2d(pt) exhibits the largest electrochemical surface area (ESA) and the highest activity toward methanol electrooxidation. With the decrease in Dp, PtRu/WMC-F30 and PtRu/WMC-F0 have much lower ESA and electrochemical activity, especially for the isopropanol electrooxidation with a larger molecular size. When D-p is more than twice d(pt), the mass transfer of reactants and electrolyte are easier, and thus more PtRu nanoparticles can be utilized and the catalysts activity can be enhanced. (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： Wormholelike mesoporous carbon PtRu catalyst Pore diameter Methanol electrooxidation

Growth of ZnO self-converted 2D nanosheet zeolitic imidazolate framework membranes by an ammoniaassisted strategy

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Nano Research 2018年第4期11卷 1850-1860页

作者： Yujia Li Lu Lin Min Tu Pei Nian Ashlee J. Howarth Omar K. Farha Jieshan Qiu xiongfu zhang State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 China International Institute for Nanotechnology Department of Chemistry Northwestern University 2145 Sheridan Road Evanston IL 60208 USA Center for Surface Chemistry and Catalysis KU Leuven-University ofLeuven Leuven Belgium Department of Chemistry Faculty of Science King Abdulaziz University Jeddah Saudi Arabia

Shaping crystalline porous materials such as metal organic frameworks （MOFs） and zeolites into two-dimensional （2D） nanosheet forms is highly desirable for developing high-performance molecular sieving membranes. However, conventional exfoliation-deposition is complex and challenging for the large-scale fabrication of nanosheet MOF tubular membranes. Here, for the first time, we report a direct growth technique by ZnO self-conversion and ammonia assistance to fabricate zeolitic imidazolate framework （ZIF） membranes consisting of 2D nanosheets on porous hollow fiber substrates; the membranes are suitable for large-scale industrial gas separation processes. The proposed fabrication process for ZIF nanosheet membranes is based on the localized self-conversion of a pre-deposited thin layer of ZnO in a ligand solution containing ammonium hydroxide as a modulator. The resulting ZIF 2D nanosheet tubular membrane is highly oriented and only 50 nm in thickness. It exhibits excellent molecular sieving performance, with high H2 permeance and selectivity for H2/CO2 separation. This technique shows great promise in MOF nanosheet membrane fabrication for large-scale molecular sieving applications.

关键词： nanosheet nanosheet membrane metal organic framework membrane oriented growth gas separation

Factors affecting the formation of zeolite seed layers and the effects of seed layers on the growth of zeolite silicalite-1 membranes

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Frontiers of Chemical Science and Engineering 2007年第2期1卷 172-177页

作者： zhang xiongfu LIU Hai’ou WANG Anjie WANG Jinqu Department of Chemical and Technology Dalian University of TechnologyDalian 116012China Department of Catalytic Chemistry and Engineering Dalian University of TechnologyDalian 116012China

The present study investigates the formation of silicalite-1 seed layers on a porous carbon support of 0.5µm pore size andα-Al_(2)O_(3) supports with different pore sizes(0.1µm and 4µm)via the slip-casting *** effects of support property,seed size and solvent on the formation of seed layers were investigated in *** growth of sili-calite-1 membranes on different seeded supports by hydro-thermal synthesis was also *** scanning electron microscopy(SEM)and X-ray diffraction(XRD)character-izations indicate that a continuous seed layer can be obtained on the smooth support of 0.1µm pore size by using any seed of 100 nm,600 nm or 2.2µm in size,whereas,on the coarse supports with either 0.5µm or 4µm pore size,a continuous seed layer cannot be formed using the above seed sizes and the same seeding *** a longer contact time,a seed layer can also be formed using 100 nm seed on the supports with larger pore ***,the layer is not uniform and *** a hydrophobic porous carbon support,seeding ethanol suspension,which has weak polarity,favors the formation of a continuous seed *** seed layers and membranes grown from the smaller seed are more uniform and continu-ous and possess smoother surfaces than those from the larger *** seed layer and respective grown membrane formed from nanosized seed(100 nm)are the most uniform and *** this method of seeded secondary synthesis of zeolite membranes,the quality of a membrane mainly depends on the quality of the seed layer.

关键词： zeolite membrane molecular sieving mem-brane inorganic membrane zeolite coating

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苯直接一步氧化合成苯酚

化学进展 2008年第2期20卷 386-395页

作者：张雄福大连理工大学化工学院化学工艺系精细化工国家重点实验室大连116012

苯直接一步氧化合成苯酚是开辟苯酚合成路线具有挑战性的热点课题之一。近年来研究和开发了以N2O、H2O2和O23种不同氧化剂体系为核心和主流的苯氧化合成苯酚路线。本文详细综述了目前3种不同氧化体系的研究进展和趋势,分析了各种合成路... 详细信息

苯直接一步氧化合成苯酚是开辟苯酚合成路线具有挑战性的热点课题之一。近年来研究和开发了以N2O、H2O2和O23种不同氧化剂体系为核心和主流的苯氧化合成苯酚路线。本文详细综述了目前3种不同氧化体系的研究进展和趋势,分析了各种合成路线的特点和工业应用前景。以N2O为氧化剂合成苯酚路线,技术趋于成熟,但N2O来源受限而影响其经济性和推广应用;以H2O2为氧化剂合成苯酚路线,是环境友好过程,有开发潜力,但技术还很不成熟,而且也因H2O2价格昂贵带来了经济成本问题;以O2为氧化剂、氢气为还原剂体系合成苯酚路线,是环境清洁可持续发展制备路线,具有很好的开发潜力,此外无机膜催化合成苯酚路线也更具吸引力。

关键词：苯氧化苯酚一氧化二氮过氧化氢分子氧无机膜

ZnO诱导的Pd/Al2O3@ZIF-8核壳催化剂制备及其催化性能

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化工学报 2015年第10期66卷 3925-3930页

作者：张祖强张通张雄福大连理工大学化工学院精细化工国家重点实验室辽宁大连116024

利用同源氧化锌有利于ZIF-8结构的成核生长原理,采用粒径为1~2mm的负载型Pd/Al2O3微球作为核、ZIF-8膜作为外壳,ZnO诱导生长制备了Pd/Al2O3@ZIF-8核壳催化剂,用XRD、EDX、SEM、ICP等分析手段对其结构进行了表征,并采用不同大小分子烯烃... 详细信息

利用同源氧化锌有利于ZIF-8结构的成核生长原理,采用粒径为1~2mm的负载型Pd/Al2O3微球作为核、ZIF-8膜作为外壳,ZnO诱导生长制备了Pd/Al2O3@ZIF-8核壳催化剂,用XRD、EDX、SEM、ICP等分析手段对其结构进行了表征,并采用不同大小分子烯烃加氢反应对其壳层连续完整性进行了性能测试。结果表明,Pd/Al2O3微球表面预先引入的ZnO纳米粒子层对外层连续ZIF-8膜壳层的形成,起到了很好的成核生长点和连接点的作用,诱导合成了连续完整的ZIF-8膜包覆的Pd/Al2O3@ZIF-8核壳结构材料,ZIF-8膜层的厚度可通过ZIF-8合成的次数进行调变。该Pd/Al2O3@ZIF-8核壳催化剂对不同分子大小的烯烃加氢反应表现出明显的筛分选择性,并对外加苯并噻唑作为毒物分子的反应体系具有良好的抗中毒性能和防催化活性金属Pd组分流失的功能。

关键词：催化剂核-壳结构 ZIF-8 膜加氢

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催化裂解多产丙烯新技术

炼油技术与工程 2006年第4期36卷 4-8页

作者：徐占武中国石油天然气股份有限公司大庆炼化分公司黑龙江省大庆市163411

介绍了国内外利用蜡油或常压渣油等重质原料的增产丙烯技术CPP,ARGG+FDFCC和TSRMP;还介绍了利用富含烯烃的混合碳四和催化裂化汽油等轻质原料的增产丙烯技术OCP,Propylur,Superflex,OCT,Meta-4和BASF公司的丁烯歧化工艺技术。

关键词：丙烯生产催化裂解工艺原料重质烃轻质烃国内外技术发展水平

杂原子Sn-β分子筛的脱铝补位两步法制备、表征及其催化环己酮Baeyer-Villiger氧化性能

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催化学报 2012年第5期33卷 898-904页

作者：康自华刘海鸥张雄福大连理工大学化工学院精细化工国家重点实验室辽宁大连116024

采用酸处理Al-β脱铝以产生T"空位",再高温焙烧插入Sn,即脱铝补位两步法制备了杂原子Sn-β分子筛.考察了β沸石中T"空位"数量、母体硅铝比和焙烧温度等因素对Sn-β分子筛形成与性能的影响,并利用X射线衍射、红外光谱、紫外-可见光谱、... 详细信息

采用酸处理Al-β脱铝以产生T"空位",再高温焙烧插入Sn,即脱铝补位两步法制备了杂原子Sn-β分子筛.考察了β沸石中T"空位"数量、母体硅铝比和焙烧温度等因素对Sn-β分子筛形成与性能的影响,并利用X射线衍射、红外光谱、紫外-可见光谱、扫描电镜、X射线荧光光谱和电感耦合等离子体原子发射光谱等手段及环己酮Baeyer-Villiger(B-V)氧化反应,对催化剂进行了表征和评价.结果表明,脱铝补位两步法可以制备Sn-β分子筛,且Sn以四配位形式存在于分子筛骨架中,在对环己酮B-V氧化反应中表现出较高的催化活性.

关键词：锡杂原子β沸石环己酮 Baeyer-Villiger氧化反应 ε-己内酯

微通道反应器内“就地”合成沸石膜催化层及其性能

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催化学报 2007年第9期28卷 758-760页

作者：蔡红丽张雄福刘海鸥杨经伦大连理工大学化工学院精细化工国家重点实验室辽宁大连116012 香港科技大学化学工程系

采用简单、新颖的沸石粒子引入方法,将NaX沸石晶种引入不锈钢微反应器的微通道内,并用流动法"就地"直接在微通道内通过沸石生长形成NaX沸石膜层,经铯离子交换处理成为CsNaX催化层,用苯甲醛和氰基乙酸乙酯的Knoevenagel缩合反应评价了该... 详细信息

采用简单、新颖的沸石粒子引入方法,将NaX沸石晶种引入不锈钢微反应器的微通道内,并用流动法"就地"直接在微通道内通过沸石生长形成NaX沸石膜层,经铯离子交换处理成为CsNaX催化层,用苯甲醛和氰基乙酸乙酯的Knoevenagel缩合反应评价了该催化层的催化性能.结果表明,微通道内形成的沸石膜层连续,均匀,具有良好的催化功能.微反应器内缩合反应的结果明显优于传统反应器.

关键词：微反应器 NaX沸石沸石膜涂层 Knoevenagel缩合反应

在大孔陶瓷管载体上引入ZnO连接层诱导合成稳定ZIF-8膜

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膜科学与技术 2014年第5期34卷 65-72页

作者：李绍辉刘海鸥张雄福大连理工大学化工学院精细化工国家重点实验室大连116024

以平均孔径为3μm的大孔α-Al2O3陶瓷管为载体,采用载体表面预先引入一层ZnO作为连接和诱导成膜的策略,合成连续完整且性能稳定的ZIF-8膜.首先在载体的内表面通过溶剂热生长一层厚度约为5μm的连续多孔ZnO层,起到对载体表面的修饰、连... 详细信息

以平均孔径为3μm的大孔α-Al2O3陶瓷管为载体,采用载体表面预先引入一层ZnO作为连接和诱导成膜的策略,合成连续完整且性能稳定的ZIF-8膜.首先在载体的内表面通过溶剂热生长一层厚度约为5μm的连续多孔ZnO层,起到对载体表面的修饰、连接膜与载体和诱导成膜的多功能作用;然后,甲醇体系溶剂热法在ZnO表面合成得到连续的ZIF-8膜.考察和优化了ZnO层的活化、ZIF-8合成条件对成膜的影响,用SEM、XRD和气体渗透等分析方法对所得ZIF-8膜进行表征.研究表明,ZnO层的连续性和活化处理是成膜的关键,ZnO层不连续难以形成完整连续ZIF-8膜,不活化ZnO则起不到很好的诱导成膜作用.最佳条件下获得的ZIF-8膜的H2通量为2.14×10-7 mol/(s·m2·Pa),H2/CO2、H2/N2、H2/CH4的理想分离系数分别为5.18、8.32、8.30.该膜材料具有明显的筛分效应,且150℃条件下长时间测试稳定性良好.

关键词：金属有机骨架膜 ZIF-8膜膜制备气体渗透