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采用等量浸渍法制得一系列不同担载量的Mo/HZSM-5催化剂,运用XRD和FTIR方法考察了Mo物种在催化剂表面的分散状态,首次采用微分吸一热技术对Mo/HzSM-5催化剂的表面酸性进行表征。同时研究了催化剂对丙烷芳构化的反应活性。结果表明:对于担载Mo的HZSM-5分子筛催化剂,Mo物种在HZSM-5分子筛表面上顺序为HZSM-5〉1%Mo/HZSM-5〉2%Mo/HZSM-5分子筛本身表面的酸 相似文献
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XIE Mao-Song YANG Xu CHEN Wen-Heng TAO Long-Xiang WANG Xuc-Lin XU Gui-Fen 《天然气化学杂志》1996,5(3):210-221
IntroductionMethancisthcmaJorcomponcntofnaturalgasanditscatalyticconvcrsiontodcsiredchemicalproductsorliquidfiJcIisnotonl}'apromisingapproachtotheutilizationofnaturalgasrcsourccbutalsoagrcatsubjcctforcatalysissciencctt'hichdcaIst"iththcactivationofsmallmolcculesThcx"orldrcscrvcofnaturalgashasbccnexplorcdasaboutl382562xl()8m3IllTheMTGprocessdcvclopedbythcMobilcorpcangctliquidfuelfrommethancthroughsteamreformingofmethanctoproduccsynthcsisgaswhichisassociatedt'ithamaJorityofthecostsofthcprocc… 相似文献
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采用Mo及稀土元素对HZSM-5分子筛进行改性并用于丙烷的芳构化反应。考察了Mo含量、引入方法及反应条件对催化活性的影响。在La、Ce、Nd、Sm、Dy等五种稀土元素中,以La的改性效果最佳,在550℃、600h-1的反应条件下,Mo-LaHZSM-5分子筛催化剂上丙烷转化率及芳烃选择性分别达到8843%、6847%,催化剂活性稳定性也得到提高 相似文献
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添加Ru的Mo/HZSM-5催化体系上的甲烷无氧脱氢芳构化 总被引:4,自引:0,他引:4
研究了在Mo/HZSM5催化剂中添加过渡金属阳离子以改变催化剂的反应性能,提高甲烷无氧脱氢芳构化的反应活性和稳定性.在添加第二组分的催化剂中,MoRu/HZSM5具有最佳的反应活性和稳定性.Ru的加入使甲烷的转化率由原来的6%~7%提高到98%.采用比表面积及孔分布测定,X射线衍射,程序升温还原,程序升温氨脱附和差热分析等表征方法研究了MoRu/HZSM5催化剂的物理化学性质.结果表明,Ru的加入引起Mo/HZSM5催化剂强酸酸量的下降,并促进了Mo物种的还原. 相似文献
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水蒸气存在时Mo/HZSM-5催化剂上的甲烷芳构化反应性能 总被引:2,自引:0,他引:2
研究了水蒸气存在条件下Mo/HZSM-5沸石分子筛催化剂上的甲烷芳构化反应行为,发现水蒸气的引入可以明显地降低甲烷芳构化反应的起始温度,从而在较为温和的条件下实现甲烷的活化.适量水蒸气的加入可以在一定程度上改善Mo/HZSM-5催化剂的稳定性,过量水蒸气的引入则会抑制甲烷芳构化反应.在反应温度为973 K时,引入适量的水蒸气对芳构化反应产物的分布没有明显影响在低温条件下的甲烷芳构化反应过程中检测到有乙烯生成,该结果支持了甲烷芳构化反应可能经历了乙烯这一中间产物的机理.实验结果还表明,水蒸气对催化剂上的积炭量没有明显的影响. 相似文献
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Mo/HZSM-5上甲烷芳构化的诱导期钼物种的部分还原和碳物种的沉积 总被引:4,自引:0,他引:4
在无氧条件下,Mo/HZSM-5催化剂表现出良好的催化甲烷芳构化性能.采用脉冲反应,TPSR,TPR,UV Raman,XRD和BET等手段研究了反应的诱导期.BET和XRD结果表明,钼物种较好地分散于分子筛的外表面和孔道内.TPSR和TPR结果表明,在苯产生之前催化剂上至少有两种不同形式的高价钼物种被部分还原.参照MoO3/Al2O3的TPR结果,认为这两种高价钼物种可能是以多聚酸盐和微晶形式存在的MoO3.UV Raman光谱表明,催化剂表面确实存在八面体配位的多聚酸盐铝物种;而XRD没有检测到微晶铝物种的存在.脉冲反应结果表明,预还原可以缩短反应诱导期,而某种类型积碳的存在对缩短反应诱导期更为有利.根据以上结果,认为诱导期是反应活性相逐渐形成的过程,包括高价钼物种的部分还原和碳物种的沉积,而后者可能对反应更为重要. 相似文献
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YipingZhang DongjieWang JinhuaFei XiaomingZheng 《天然气化学杂志》2003,12(2):145-149
Mo/HZSM-5 is a good catalyst for methane aromatization, and the reaction performance of Mo/HZSM-5 and Cu modified Mo/HZSM-5 catalysts under various pretreatment conditions has been studied. The results indicate that the catalyst presented a distinguished catalytic activity, benzene selectivity and a high stability when the bed temperature was raised in N2 atmosphere. 相似文献
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预处理条件对Mo/HZSM—5催化剂上丙烷芳构化的影响 总被引:1,自引:0,他引:1
采用浸渍法制备了Mo/HZSM-5 分子筛催化剂,考察了H2 、N2 、空气预处理对催化剂丙烷芳构化活性的影响。在相同处理条件下,空气气氛更有利于提高催化剂的丙烷芳构化活性。在空气焙烧过程中,氧化钼物种向分子筛内表面分散。在H2 还原处理过程中,表面钼物种部分被还原为Mo4 + 。随还原时间延长,催化剂芳构化活性升高,同时发生少量Mo 物种向分子筛孔道内迁移 相似文献
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碳四烃在改性HZSM-5分子筛上芳构化研究 总被引:8,自引:0,他引:8
研究了炼厂混合C_4烃在Zn、Ga、Cr、La改性的HZSM-5分子筛催化剂上的芳构化反应,采用TPD和IR测定了催化剂的表面酸性质。结果表明,用Zn(3%)和Zn(2%)Ga(1%)改性的HZSM-5分子筛具有较好的芳构化性能;各改性HZSM-5分子筛催化剂芳构化性能变化与表面酸性有关,总酸量下降,芳构化活性下降,强B酸中心减少,深度裂解反应减少;Zn的单组分和双组分改性的HZSM-5分子筛催化剂芳构化活性的增高与表面强L酸浓度增加和吡啶吸附IR谱中的1615cm~(-1)吸收峰出现有关。 相似文献
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Impregnation,mechanical mixing and hydrothermal treatment methods were used to introduce molybdenum species into the HZSM-5 zeolite ,the structure and surface acidity of the catalysts were studied by means of XRD,FT-IR ,NH3-TPD,TPR and XPS,The effects of Mo content and reaction time on stream on the aromatization of propane were investigated,It was found that the performance of the Mo/HZSM-5 catalst prepared by the hydrothermal treatment method was much better than that of the other two catalysts,For example ,under the reaction conditions of 823 K and 600h^-1, propance conversion and aromatics selectivity over the catalyst prepared by hydrothermal pretreatment could reach 89.17% and 78.56%,respectively,XRD and XPS results showed that the Mo species in the catalysts prepared by hydrothermal treatment were highly dispersed on the surface of the HZSM-5,and lartger amounts of them could penetrate into the HZSM-5 channel ,as compared with the other two kinds of catalysts,These factors may be responsibled for their high activities for propane aromatization,IR and NH3-TPD studies indicated that the number of Broensted acid centers decreased and the Lewis acid centers increased after Mo was introduced into the HZSM-5 zeolite. 相似文献
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Junwei Wang Maoqing Kang Zhixin Zhang Xinkui WangInstitute of Coal Chemistry Chinese Academy of Sciences Taiyuan China Manuscript received December revised March 《天然气化学杂志》2002,(Z1)
Impregnation, mechanical mixing and hydrothermal treatment methods were used to introduce molybdenum species into the HZSM-5 zeolite. The structure and surface acidity of the catalysts were studied by means of XRD, FT-IR, NH3-TPD, TPR and XPS. The effects of Mo content and reaction time on stream on the aromatization of propane were investigated. It was found that the performance of the Mo/HZSM-5 catalyst prepared by the hydrothermal treatment method was much better than that of the other two catalysts. For example, under the reaction conditions of 823 K and 600 h-1, propane conversion and aromatics selectivity over the catalyst prepared by hydrothermal pretreatment could reach 89.17% and 78.56%, respectively. XRD and XPS results showed that the Mo species in the catalysts prepared by hydrothermal treatment were highly dispersed on the surface of the HZSM-5, and larger amounts of them could penetrate into the HZSM-5 channel, as compared with the other two kinds of catalysts. These factors may be responsi 相似文献
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STUDY OF HYDROGEN TRANSFER REACTIONS IN PROPANE AROMATIZATION OVER Ga MODIFIED HZSM-5 CATALYSTS 下载免费PDF全文
研究了丙烷在不同SiO2/Al2O3比值的HZSM5和Ga改性HZSM5催化剂上的芳构化转化,为探讨氢转移反应的能力,也考察了在丙烷中添加少量氢对芳构化转化的影响。结果表明,随HZSM5分子筛SiO2/Al2O3比值的减小,氢转移反应程度增大;在分子筛中引入Ga,氢转移反应能力增大。最后提出了有Ga参与的反应机理。 相似文献
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以稀土离子交换的HZSM-5为载体的甲烷非氧化芳构化催化剂 总被引:2,自引:0,他引:2
The declining crude oil reserves has led to natural gas being considered as an alternative supply to produce important organic raw materials such as ethene and aromatics. Mo/HZSM-5 is found to be able to act effectively for the title reaction[1]. In order to clarify how the cation in the channel of HZSM-5 effects the behavior of the catalyst, different rare earth ion exchanged HZSM-5 ([ RE3+] HZSM-5 ) zeolites were investigated as supports of the Mo/[ RE3 + ] HZSM-5 catalyst. 相似文献
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Yi-Ping Zhang Dong-jie Wang Jin-hua Fei Xiao-ming Zheng 《Reaction Kinetics and Catalysis Letters》2001,74(1):151-161
The influence of Zn content, reaction temperature and pretreatment conditions on a Zn-modified Mo/HZSM-5 catalyst for methane
aromatization were studied. It was found that the addition of Zn promoted the reaction. Methane conversion of 10.9% and aromatics
selectivity of 96.7% were obtained with a Zn/Mo molar ratio of 0.03 and N2 pretreatment at 973 K. The results of isopropanol decomposition, NH3-TPD and TG-DTA suggest that the addition of Zn decrease the acidity of the catalyst, which may be the reason for the high
activity on the Mo-Zn/HZSM-5 catalyst.
This revised version was published online in June 2006 with corrections to the Cover Date. 相似文献
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Co改性Mo/HZSM-5催化剂上甲烷无氧芳构化反应研究 总被引:6,自引:0,他引:6
甲烷无氧芳构化催化剂Mo/HZSM-5上担载第二组分Co后,提高了催化剂的稳定性,但加快了催化剂上的积炭速率,且积炭速率随Co添加量的增加而提高,因而认为催化剂的失活速率与积炭速率并不成顺比关系,研究认为,一方面,Co的添加增加了催化剂的脱氢能力,使更多的中间产物乙烯进一步脱氢转化成芳烃或积炭,另一方面,增加了催化剂的抗积炭能力。并认为部分积炭可能对提高催化剂的稳定性起到一定的作用,空速实验表明, 相似文献