共查询到18条相似文献,搜索用时 265 毫秒
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焙烧对HZSM—5分子筛结构的影响 总被引:2,自引:0,他引:2
运用魔角自转固态核磁共振谱(MAS-NMR),研究了焙烧对HZSM-5分子筛结构的影响,结果表明,高温焙烧将引起HZSM-5分子筛骨架的脱铝,当焙烧温度从500℃增加到700℃时,HZSM-5的骨架Si/Al比由16.7增加至22.7;而当焙烧温度由700℃到800℃时,骨架Si/Al比则由22.7增加到48.5,Al-MASNMR结果表明,从骨架上脱下来铝,部分地形成了NMR不可见的无定形态,随 相似文献
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使用固体高分辨^27Al MASNMR技术研究了改良HZSM-5分子筛在不同预处理条件及催化反应与再生时结构热稳定性。结果表明,预处理条件对HZSM-5骨架的热稳定性有着明显影响。骨架脱顺序为:水热处理>热处理;GaHZSM-5>HZSM-5HZSM-5>>ZnHZSM-5。水热处理样品HZSM-5,GaHZSM-5在反应后非骨架铝重新迁入了沸石骨架,即存在“反应补铝”效应。 相似文献
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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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应用XRD、XPS、IR、^29sIMASNMR,^27AlMASNMR和NO-IR吸附等手段对一系列经不同温度焙烧的Mo/USY催化剂中USY骨架结构破坏过程和Mo在USY分子筛中的烧结行为进行了研究。结果表明,Mo在USY上分散和烧结时,存在一个Mo对USY分子筛骨架铝的抽提过程,Mo和USY分子筛表面分散时,抽提该分筛骨架Si(2Al)中少量的Al,但当焙烧温度升高,Mo开始烧结时,Mo主要 相似文献
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对合成的SAPO-5分子筛进行了高温和水热处理,并用IR,XRD和MAS NMR对处理过的分子筛进行了表征。结果表明,短时间的高温焙烧并不破坏分子筛的结构,而使分子筛中的骨架元素P,Al和Si发生重构;长时间的高温焙烧使分子筛的结晶度降低,主要是由于P和Al游离出分子筛的骨架而形成磷酸铝盐。水热处理使分筛的Si经历一个转晶和重构过程,在使SAPO-5分子筛结构更加完整的同时,未完全结晶的杂质形成了 相似文献
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负载型钼基催化剂上甲烷,乙烷无氧芳构化反应研究 总被引:1,自引:0,他引:1
研究了不同载体钼基催化剂上甲烷,乙烷的无氧芳构化反应。在所采用的载体中,HZSM-5具有最佳性能,对甲烷的芳构化反应,Mo/HZSM-5催化剂表现出较高的活性和芳烃选择性;而Mo/Al2O3或Mo/SiO2催化剂则相对较差。对于乙烷的反应,钼物种的存在更有利于甲烷或乙烯的生成,芳烃选择性相对较低。钼物种较强的断键能力可能是使甲烷C-H键活化的原因。 相似文献
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W. Liu Y. Xu She-Tin Wong L. Wang J. Qiu N. Yang 《Journal of molecular catalysis. A, Chemical》1997,120(1-3):257-265
By using a high-resolution solid state nuclear magnetic resonance spectrometer with 27Al and 29Si probes, the interaction between Mo species and HZSM-5 of frsol|Mo/HZSM-5 catalysts has been studied. The results show that there is a strong interaction between Mo species and HZSM-5 zeolite. The framework aluminum in the zeolite can be easily extracted by the introduction of Mo species. The extractability of framework aluminum by Mo species increases with increasing Mo loading and the calcination temperature. The extraction process leads to the formation of non-framework Al at first and then a new crystalline phase of Al2(MoO4)3. The dealumination of the catalyst having a Mo loading of 15% and had been calcined at 973 K is so severe that all the aluminum in the framework are extracted and no framework Al could be detected by 27Al MAS NMR. The catalyst, therefore, lost its catalytic activity for methane dehydrogenation and aromatization in the absence of oxygen. The Si/Al ratio measured from 29Si MAS NMR further confirms the dealumination process observed by 27Al MAS NMR. The MAS NMR results give us an evidence that Al2(MoO4)3 crystallites are much less active for the reaction. 相似文献
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处理条件对Mo/HZSM-5催化剂结构及性能的影响 总被引:2,自引:0,他引:2
使用付立叶变换红外光谱和固体高分辨核磁技术,考察了在不同处理条件下,甲烷无氧芳构化催化剂Mo/HZSM5分子筛骨架结构的变化情况.结果显示,较高的焙烧温度和较高的预处理温度,都会造成催化剂中担载的钼物种对分子筛骨架铝的严重抽提,特别是在钼物种含量较高时,这种情况更明显.以不同担体及不同钼物种构成的前驱态催化剂的催化反应评价结果表明,以微晶状态存在的MoO3和与担体间以相对较弱作用力存在的高分散钼物种,在反应过程中被活化成具有催化活性钼物种的几率更大;而晶相状态的Al2(MoO4)3以及与载体间存在较强相互作用力的钼物种,在甲烷无氧芳构化过程中不起主要催化活性作用.计算得出,甲烷无氧脱氢芳构化反应的表观活化能为89.8kJ/mol. 相似文献
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Study on Bifunctionality of Mo/HZSM-5 Catalysts for Methane Dehydro-Aromatization under Non-oxidative Condition 下载免费PDF全文
Lingling Su Yide Xu Xinhe BaoState Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Zhongshan Road P. O. Box Dalian ChinaManuscript received June revised July 《天然气化学杂志》2002,(Z1)
The optimum Mo/[H~+] ratio per unit cell of the active precursors in Mo/HZSM-5 catalysts for methane dehydro-aromatization, measured by 1H MAS NMR, was found to be about 1 when adjusting the acid sites by altering either the SiO2/Al2O3 ratios or the Mo loading. This implies that a concerted interaction between the Mo species and the Bronsted acid sites probably features the bifunctionality of the Mo/HZSM-5 catalyst. On the other hand, it was found that the driving force for Mo species to move into the HSZM-5 zeolite channels and the interaction between the Mo species and the Bronsted acid sites are closely and proportionably related with the amount of Bronsted acid sites per unit cell. 相似文献
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Renqing Lü 《天然气化学杂志》2005,14(2):119-124
The density functional theory and the cluster model methods have been employed to investigate the interactions between ethanethiol and HZSM-5 zeolites. Molecular complexes formed by the adsorption of ethanethiol on silanol H3SiOH with two coordination forms, model Bronsted acid sites of zeolite cluster H3Si(OH)Al(OH)2SiH3 interaction with ethanethiol, aluminum species adsorbed ethanethiol have been comparatively studied. Full optimization and frequency analysis of all cluster models have been carried out using B3LYP hybrid method at 3-21G basis level for hydrogen atoms and 6-31G(d) basis set level for silicon, aluminum, oxygen, carbon, and sulfur atoms. The structures and energy changes of different coordination forms of H3Si(OH)Al(OH)2SiH3-ethanethiol, silanol-ethanethiol and Al(OH)3-ethanethiol have been studied. The calculated results showed the nature of interactions was van der Waals force as exhibited by not much change in geometric structures and properties. The preference order of ethanethiol adsorbed on HZSM-5 zeolite may be residual aluminum species, bridging hydroxyl groups and silanol OH groups from the adsorption heat. The adsorbed models of protonized ethanethiol on bridging hydroxyl OH groups and linear hydrogen bonded ethanethiol on bridging OH groups suggested in literature might not exist as revealed by this theoretical calculation. Possible adsorption models were obtained for the first time. 相似文献