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Isobutane Dehydrogenation Assisted by C02 over Silicalite-i-Supported ZnO Catalysts: Influence of Support Crystallite Size

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Chinese Journal of Chemistry 2020年第7期38卷 703-708页

作者： Yajun Luo Chunling Wei changxi miao Yinghong Yue Weiming Hua Zi Gao Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China Shanghai Research Institute of Petrochemical Technology SINOPEC Shanghai 201208China

The ZnO catalysts supported on Silicalite-1 zeolites with different crystallite sizes(0.08,0.35,1 and 1.7 jjm,respectively)and 5%Zn were synthesized via an incipient wetness *** catalysts were characterized by XRD,N2 adsorption,SEM,TEM-EDX,DRIFT spectra and NH3-TPD,and their catalytic performance in isobutane dehydrogenation assisted by C02 was *** catalytic activity is strongly dependent on the crystallite size of Silicalite-1 *** ZnO/S-l-O.35 catalyst with ca.0.35 μmcrystallite size displays the highest activity,affording an initial isobutane conversion of 51.0%and 74.5%isobutene *** can be attributed to a higher amount of acid sites present on this catalyst as well as the largest amount of nest silanols possessed by the S-l-0.35 support.

关键词： method. crystallite catalyst

Liquid-phase a-Pinene Isomerization over Fe-doped Sulfated Zirconia Prepared by a Hydrothermal Treatment-assisted Process

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Chinese Journal of Chemistry 2011年第6期29卷 1095-1100页

作者： Liu, Jianfeng Zhao, Jie miao, changxi Yue, Yinghong Hua, Weiming Gao, Zi Shanghai Research Institute of Petrochemical Technology Shanghai 201208 China Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of Chemistry Fudan University Shanghai 200433 China

A series of Fe-doped （0.5%--3%） sulfated zirconia have been prepared by a hydrothermal treatment-assisted process. Textural and structural characterizations of the as-synthesized materials were performed by means of N2 adsorption, X-ray diffraction, transmission electron microscopy, scanning electron microscopy and thermogravimetric analysis. Temperature-programmed desorption of ammonia was used to determine the acidity of the samples. The effects of Fe-doping on the structure, acidity and catalytic activity of sulfated zirconia for liquid-phase a-pinene isornerization were investigated. The incorporation of small amounts of Fe into sulfated zirconia results in the increase of sulfate content and the number of acid sites, which is responsible for the enhanced activity of Fe-doped catalysts in comparison with the undoped one. Meanwhile, hydrothermal treatment helps to improve the activity of the catalyst.

关键词： sulfated zirconia Fe-doping hydrothermal treatment promoting effect acidity isomerization

Oxidative Dehydrogenation of 1-Butene to 1,3-Butadiene Using CO2 over Cr-SiO2 Catalysts Prepared by Sol-gel Method

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Chemical Research in Chinese Universities 2018年第4期34卷 609-615页

作者： GAO Biao LUO Yajun miao changxi YUE Yinghong YANG Weimin HUA Weiming GAO Zi Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of Chemistry Fudan University Shanghai 200433 P. R. China Shanghai Research Institute of PetrochemicaI Technology SINOPEC Shanghai 201208 P. R. China

A series of Cr-SiO2 catalysts with a Cr content（mass fraction） ranging from 0.5% to 9% was prepared by a sol-gel method. The catalysts were characterized by XRD, N2 adsorption, EDX elemental mapping, Raman spectros- copy, UV-Vis spectroscopy, XPS and H2-TPR, and their catalytic behavior in the dehydrogenation of 1-butene to 1,3-butadiene（BD） using CO2 as a soft oxidant was studied. The initial BD yield is well correlated with the amount of Cr6~ in the fresh catalysts. The highest BD yield of ca. 34% is achieved on the catalysts with 5%--9% Cr at 600 ~C -1 -1 and weight hourly space velocity（WHSV） of 4.5 g＇geat＇h ~ The promoting effect of CO2 on the BD yield was ob- served, which can be attributed to the reaction coupling between a simple dehydrogenation of 1-butene and the re- verse water-gas shift reaction as well as regaining the oxidation state（lattice oxygen） of reduced Cr3＋ species due to the mild oxidation ability of CO2. The Cr-SiO2 catalyst exhibits higher BD yield than the Cr catalyst supported on SBA-15, which is attributed to the higher amount of Cr6＋ present on the former catalyst.

关键词： 1,3-Butadiene CO2 oxidative dehydrogenation Cr-based catalyst Sol-gel method

Dehydrogenation of Isobutane to Isobutene with Carbon Dioxide over SBA-15-Supported Chromia-Ceria Catalysts

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Chinese Journal of Chemistry 2017年第10期35卷 1619-1626页

作者： Chunling Wei Fangqi Xue changxi miao Yinghong Yue Weimin Yang Weiming Hua Zi Gao Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of Chemistry Fudan University Shanghai 200433 China Shanghai Research Institute of Petrochemical Technology SINOPEC Shanghai 201208 China

A series of SBA-15-supported chromia-ceria catalysts with 3% Cr and 1%--5% Ce （3Cr-Ce/SBA） were pre- pared using an incipient wetness impregnation method. The catalysts were characterized by XRD, N2 adsorption, SEM, TEM-EDX, Raman spectroscopy, UV-vis spectroscopy, XPS and H2-TPR, and their catalytic performance for isobutane dehydrogenation with CO2 was tested. The addition of ceria to SBA-15-supported chromia improves the dispersion of chromium species. 3Cr-Ce/SBA catalysts are more active than SBA-15-supported chromia （3Cr/SBA）, which is due to a higher concentration of Cr^6＋ species present on the former catalysts. The 3Cr-3Ce/SBA catalyst shows the highest activity, which gives 35.4% isobutane conversion and 89.6% isobutene selectivity at 570℃ after 10 min of the reaction.

关键词： isobutane dehydrogenation carbon dioxide chromia-ceria SBA-15 supported catalyst

n-BUTANE ISOMERIZATION ON Al-PROMOTED SULFATED ZIRCONIA CATALYSTS

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Chinese Journal of Catalysis 1998年第2期 4-5页

作者： Xia Yongde, Hua Weiming, miao changxi, Gao Zi**(Department of Chemistry, Fudan University, Shanghai 200433)

ｎＢＵＴＡＮＥＩＳＯＭＥＲＩＺＡＴＩＯＮＯＮＡｌＰＲＯＭＯＴＥＤＳＵＬＦＡＴＥＤＺＩＲＣＯＮＩＡＣＡＴＡＬＹＳＴＳＸｉａＹｏｎｇｄｅ，ＨｕａＷｅｉｍｉｎｇ，ＭｉａｏＣｈａｎｇｘｉ，ＧａｏＺｉ（Ｄｅｐａｒｔｍ... 详细信息

ｎＢＵＴＡＮＥＩＳＯＭＥＲＩＺＡＴＩＯＮＯＮＡｌＰＲＯＭＯＴＥＤＳＵＬＦＡＴＥＤＺＩＲＣＯＮＩＡＣＡＴＡＬＹＳＴＳＸｉａＹｏｎｇｄｅ，ＨｕａＷｅｉｍｉｎｇ，ＭｉａｏＣｈａｎｇｘｉ，ＧａｏＺｉ（ＤｅｐａｒｔｍｅｎｔｏｆＣｈｅｍｉｓｔｒｙ，Ｆｕ...

关键词： Butane Isomerization Sulfuric acid Alumina Zirconia Acid strength distribution

TiO_2对乙苯脱氢制苯乙烯催化剂中KFe_(11)O_(17)活性相结构的影响

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化学反应工程与工艺 2007年第3期23卷 259-262,278页

作者：朱敏缪长喜宋磊范勤陈铜中国石油化工股份有限公司上海石油化工研究院上海201208

采用穆斯堡尔谱,X-射线衍射和程序升温还原等方法,研究了乙苯脱氢铁钾系催化剂中氧化钛对铁钾活性相KFe_(11)O_(17)结构形成的影响。发现添加适量的氧化钛对形成KFe_(11)O_(17)物相有利,当催化剂中Fe_2O_3,K_2O,CeO_2和Mo_2O_3的质量比... 详细信息

采用穆斯堡尔谱,X-射线衍射和程序升温还原等方法,研究了乙苯脱氢铁钾系催化剂中氧化钛对铁钾活性相KFe_(11)O_(17)结构形成的影响。发现添加适量的氧化钛对形成KFe_(11)O_(17)物相有利,当催化剂中Fe_2O_3,K_2O,CeO_2和Mo_2O_3的质量比固定为75.0:12.0:7.0:3.0,而Fe_2O_3与TiO_2质量比为75.0:0.1时,TiO_2对铁钾尖晶石结构形成的促进作用最明显,催化剂的活性也最高。但当TiO_2添加的质量比继续提高,会抑制铁钾尖晶石的形成,从而使催化剂的活性下降。当Fe_2O_3与TiO_2的质量比为75.0:1.0时,催化剂内的铁钾尖晶石结构遭到破坏。

关键词：乙苯脱氢苯乙烯氧化钛铁钾尖晶石

助剂和焙烧条件对乙苯脱氢制苯乙烯催化剂性能的影响

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化学反应工程与工艺 2006年第5期22卷 467-471页

作者：顾松园宋磊廖仕杰缪长喜中国石油化工股份有限公司上海石油化工研究院上海201208

采用改变助剂前躯体和热处理条件的方法对Fe2O3-K2O系催化剂的性能进行改进,通过脱氢反应,扫描电境(SEM),X衍射(XRD),催速老化等手段考察了改进乙苯脱氢制苯乙烯催化剂的性能。发现采用合适量的Ce氧化物助剂有利于催化剂组分的均匀分散... 详细信息

采用改变助剂前躯体和热处理条件的方法对Fe2O3-K2O系催化剂的性能进行改进,通过脱氢反应,扫描电境(SEM),X衍射(XRD),催速老化等手段考察了改进乙苯脱氢制苯乙烯催化剂的性能。发现采用合适量的Ce氧化物助剂有利于催化剂组分的均匀分散,从而提高催化剂的活性和选择性。选择较长的焙烧时间或较高的焙烧温度促进了高铁酸钾KFe11O17晶相的大量形成,使催化剂的稳定性得到明显的提高。

关键词：助剂乙苯脱氢表征稳定性

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分子筛限域丙烷脱氢催化剂的研究进展

化工进展 2024年第10期43卷 5517-5526页

作者：洪学思吴省宋磊缪长喜杨为民中石化(上海)石油化工研究院有限公司绿色化工与工业催化全国重点实验室上海200120 华东理工大学化工学院上海200237

在“双碳”目标的背景下,丙烷直接脱氢制丙烯技术在近年得到迅速推广应用。替代催化剂的开发是丙烷脱氢新型工艺开发的核心问题。分子筛因能将金属团簇封装在孔道内或锚定于骨架上,而成为制备高效、稳定脱氢催化剂的理想载体。本文从不... 详细信息

在“双碳”目标的背景下,丙烷直接脱氢制丙烯技术在近年得到迅速推广应用。替代催化剂的开发是丙烷脱氢新型工艺开发的核心问题。分子筛因能将金属团簇封装在孔道内或锚定于骨架上,而成为制备高效、稳定脱氢催化剂的理想载体。本文从不同活性中心的角度出发,系统阐述了铂基、铑基、锌基、钴基等分子筛限域催化剂的合成方法,金属纳米团簇与分子筛骨架间相互作用以及催化作用机制的研究进展,分析了分子筛限域催化剂在高温下关键组分流失、活性中心团聚的不足,提出了强化金属与分子筛相互作用的调控思路。最后指出为早日实现工业替代,分子筛限域催化剂还应从基础科学问题和适应于工业条件的催化剂放大两方面进行深入研究。

关键词：丙烷脱氢催化剂分子筛限域效应

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粘结剂含量对铁系乙苯脱氢催化剂的影响

化学反应工程与工艺 2011年第2期27卷 151-154页

作者：危春玲宋磊陈铜缪长喜中国石油化工股份有限公司上海石油化工研究院上海201208

考察了粘结剂含量对铁系乙苯脱氢制苯乙烯催化剂的影响,采用X射线衍射(XRD)、M(o|¨)ssbauer谱和H_2程序升温还原(H_2-TPR)等方法对催化剂进行了表征。结果表明,不含粘结剂催化剂的机械强度和活性均较低,添加粘结剂后,可以较大幅度地提... 详细信息

考察了粘结剂含量对铁系乙苯脱氢制苯乙烯催化剂的影响,采用X射线衍射(XRD)、M(o|¨)ssbauer谱和H_2程序升温还原(H_2-TPR)等方法对催化剂进行了表征。结果表明,不含粘结剂催化剂的机械强度和活性均较低,添加粘结剂后,可以较大幅度地提高催化剂的机械强度和活性,当粘结剂含量为4.0%时,催化剂的机械强度和活性较好。随着粘结剂含量的增加,催化剂中铁钾尖晶石K_2Fe_(22)O_(34)和K_2Fe_(10)O_(16)物相增加,催化剂的抗还原性能增加,从而提高催化剂的活性和稳定性。

关键词：粘结剂乙苯脱氢苯乙烯催化剂