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铁助剂对Rh-Mn-Li/SiO2催化剂表面上的CO脱附和CO加氢行为的影响 总被引:3,自引:0,他引:3
采用一氧化碳程序升温脱附(CO-TPD)和吸附的一氧化碳加氢程序升温表面反应(TPSR)考察了Fe助剂对Rh基催化剂上CO的脱附行为及吸附CO的加氢行为的影响.CO-TPD实验表明,在Rh/SiO2催化剂上CO有三个脱附峰.在Rh-Mn-Li/SiO2中加入0.05%Fe后,高温脱附CO比Rh/SiO2催化剂上相应的CO量大.增加Fe的负载量,CO的脱附量减少.TPSR实验中,CO加氢反应的主要产物是甲烷.不同组分的催化剂上甲烷的生成温度有如下顺序:Rh/SiO2(482K)<Rh-Mn-Li/SiO2(489K)<Rh-Fe/SiO2(494K)<Rh-Mn-Li-Fe/SiO2(501K).甲烷峰的产生伴随着CO(s)高温脱附峰的消失,说明甲烷是由强吸附的CO加氢生成的. 相似文献
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本文叙述了R-磷钼酸盐的年鉴轩及其催化性能的表征。利用气相色谱法和红外光谱-程序升温脱附法(FTIR-TPD),测定了不同制备条件下,R-磷钼酸盐的固体酸性质(酸量、酸类型和酸强度),结果表明,当R含量不同,其固体酸性质也不同,通过控制R含量可能调节R-磷钼酸的固体酸性质。利用R-磷钙酸盐作为固体酸催化剂合成邻苯二甲酸二辛酯(DOP)的酯化反应表明,当R-磷钙酸盐的表面呈L酸较大时,酯化率就较高, 相似文献
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烷基化催化剂表面酸性及催化性能的动力学研究 总被引:2,自引:0,他引:2
在确定关联升温速率、脱附峰温和脱附峰覆盖率的程序升温脱附动力学模型的基础上,通过TPD实验和模型参数估值,建立了表征催化剂酸密度、酸强度及强度分布情况的方法。研究表明,随着活化温度的提高,固体酸催化剂表面酸中心强度分布先变宽后趋于均匀,350?℃活化催化剂的强度分布最宽;催化剂表面酸强度和酸密度随活化温度提高均呈先增大后降低、分别在350 ℃和250 ℃活化温度达到极大值的变化规律。催化剂酸性与催化性能关联的结果表明,随着活化温度的提高,烷基化反应速率常数与总脱附量的变化趋势相同,而催化剂失活速率常数与脱附活化能变化趋势相同;催化剂活性稳定性随其酸强度的增大而变差,催化剂活性与催化剂酸量和酸强度有关。 相似文献
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微波辐射下稀土交换ZSM-5分子筛的制备及裂解反应研究 总被引:3,自引:0,他引:3
借助微波技术制备出一系列具有不同La3+交换度的LaHZSM-5样品。初步探讨了微波强度、微波作用时间及Si/Al比对交换度的影响。对其表面酸性的考察发现,样品均含有B酸和L酸中心,并且随La3+进入ZSM-5沸石的量的不同,强弱酸中心的强度与数量均有所改变。对样品催化性能的研究结果表明,催化活性与La3+含量及酸量呈顺变关系。 相似文献
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One type of ZSM-5 zeolite with large partical size was prepared and characterized by XRD, SEM, N2 adsorption-desorption, XRF, Py-IR and NH3-TPD techniques. Effects of ammonium exchange and SiO2/Al2O3 molar ratios on the reaction of methanol to propylene (MTP) over Na-ZSM-5 and H-ZSM-5 zeolites have been studied in a fixed-bed flow reactor under the operating conditions of T = 500 °C, P = 1 atm, and WHSV = 6 h-1. Ammonium exchange led to a rapid decrease in Na content for Na-ZSM-5 zeolite. The reaction results indicated that Na-ZSM-5 and H-ZSM-5 with different SiO2/Al2O3 molar ratios all exhibited high activity for methanol conversion. Ammonium exchange and the decreased SiO2/Al2O3 molar ratio of ZSM-5 zeolite led to an increase both in strong acid sites and weak acid sites. Na-ZSM-5 with high SiO2/Al2O3 molar ratio was favorable for the formation of propylene. The highest propylene selectivity (45.9%) was obtained over Na-ZSM-5 zeolite catalyst with SiO2/Al2O3 molar ratio of 220. 相似文献
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NorAishahSaidinaAmin DidiDwiAnggoro 《天然气化学杂志》2003,12(2):123-119
Direct conversion of methane using a metal-loaded ZSM-5 zeolite prepared via acidic ion exchange was investigated to elucidate the roles of metal and acidity in the formation of liquid hydrocarbons. ZSM-5 (SiO2/A12O3=30) was loaded with different metals (Cr, Cu and Ga) according to the acidic ion-exchange method to produce metal-loaded ZSM-5 zeolite catalysts. XRD, NMR, FT-IR and N2 adsorption analyses indicated that Cr and Ga species managed to occupy the alllmlnum positions in the ZSM-5 framework. In addition, Cr species were deposited in the pores of the structure. However, Cu oxides were deposited on the surface and in the mesopores of the ZSM-5 zeolite. An acidity study using TPD-NH3, FT-IR, and IR-pyridine analyses revealed that the total number of acid sites and the strengths of the BrSusted and Lewis acid sites were significantly different after the acidic ion exchange treatment.Cu loaded HZSM-5 is a potential catalyst for direct conversion of methane to liquid hydrocarbons. The successful production of gasoline via the direct conversion of methane depends on the amount of aluminum in the zeolite framework and the strength of the BrSnsted acid sites. 相似文献
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Nor Aishah Saidina Amin Didi Dwi Anggoro. Faculty of Chemical Natural Resources Engineering Universiti Teknologi Malaysia Skudai Johor Malaysia. Department of Chemical Engineering University of Diponegoro Semarang IndonesiaManusc 《天然气化学杂志》2002,(Z1)
Ethylene oligomerization using ZSM-5 zeolite was investigated to study the role of Bronsted acid sites in the formation of higher hydrocarbons. The oligomerization of olefins, dependent on the acidity of ZSM-5 zeolite, is an important step in the conversion of natural gas to liquid fuels. The framework Si/Al ratio reflects the number of potential acid sites and the acid strength of the ZSM-5 catalyst. ZSM-5 with the mole ratio SiO2/Al2O3 equal to 30 was dealuminated for different periods of time according to the acidic ion-exchange method to produce ZSM-5 with various Si/Al ratios. The FT-IR analysis revealed that the integrated framework aluminum band, non-framework aluminum band, and silanol groups areas of the ZSM-5 zeolites decreased after being dealuminated. The performance of the dealuminated zeolite was tested for ethylene oligomerization. The results demonstrated that the dealumination of ZSM-5 led to higher ethylene conversion, but the gasoline selectivity was reduced compared to the performance 相似文献
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采用脉冲反应技术、原位CO吸附和吡啶吸附红外光谱,考察了Al2O3和SiO2负载的Rh基催化剂上Rh-CeO2相互作用和CH4解离活性.结果表明,载体酸性对Rh-CeO2相互作用有显著影响.Rh/Al2O3催化剂中添加CeO2增加了载体Al2O3的Lewis酸位,使Al2O3接受电子的能力增强,从而降低Rh的电子密度,有利于CH4解离活化.相反,Rh/SiO2催化剂中添加CeO2减少了载体SiO2的Lewis酸位和酸强度,使SiO2难于接受电子,导致Rh的电子密度增加,不利于CH4解离活化. 相似文献
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NorAishahSaidinaAmin DidiDwiAnggoro 《天然气化学杂志》2002,11(1):79-86
Ethylene oligomerization using ZSM-5 zeolite was investigated to study the role of Broensted acid sites in the formation of higher hydrocarbons,The oligomeriztion of olefins,dependent on the acidity of ZSM-5 zeolite ,is an important step in the conversion of natural gas to liquied fuels,The framework Si/Al ratio reflects the number of potential acid sites and the acid strength of the ZSM-5 catalyst,ZSM-5 with the mole ratio SiO2/Al2O3 equal to 30 was dealuminated for different periods of time according to the acidic ion-exchange method to produce ZSM-5 with various Si/Al ratios,The FT-IR analysis revealed that the integrated framework aluminum band,non-framework aluminum band,and silanol groups areas of the ZSM-5 zeolites decreased after being dealuminated,The performanc of the dealuminated zeolite was tested for ethylene oligomerization.The results demonstrated that the dealumination of ZSM-5 led to higher ethylene conversion,but the gasoline selectivity was reduced compared to the performance of a ZSM-5 zeolite ,The characterization results revealed the amount of aluminum in the zeolitic framework,the crystallinity of the ZSM-5 zeolite,and the Si/Al ration affected the formation of Broensted acid sites,The number of the Broensted acid sites on the catalyst active sites is important in the olefin conversion to liquied hydrocarbons. 相似文献
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FTIR研究不同硅铝比HZSM-5沸石的酸性质 总被引:9,自引:0,他引:9
用IR和NH3-TPD测定了硅铝比为31.4~137.1的HZSM-5沸石样品的酸中心数;由Lang-muir吸附模型推导出B、L酸的吸附热公式,并由此计算了B酸的吸附热。发现在Al/u.c.为3.64附近,酸中心数与Al/u.c的关系发生了转折,并发现B酸吸附符合Langmuir模型,L酸强度不均匀而不符合该模型,测定了HZSM-5分子筛的B、L酸消光系数8B=7.52×105cm·mol-1、8L=1.09×106cm·mol-1。 相似文献
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通过浸渍法分别在Al(OH)_3和Al_2O_3中引入SiO_2,经焙烧后制备具有不同表面酸性质的SiO_2-Al_2O_3载体,以上述SiO_2-Al_2O_3及Al_2O_3为载体,采用等体积浸渍法制备Ni负载量为15%的Ni/SiO_2-Al_2O_3催化剂(分别为Ni/SA-1和Ni/SA-2)与Ni/Al_2O_3.采用N2物理吸附、Py-FTIR、NH3-TPD、XRD、H2-TPR和H2-TPD手段对催化剂进行表征,考察了表面酸性质对催化剂催化1,4-丁炔二醇高压加氢性能的影响.结果表明,SiO_2引入方式会影响Ni/Al_2O_3催化剂表面酸性质及活性组分Ni在载体表面的分散行为.在Al(OH)3中引入SiO_2时,Ni/SA-1催化剂不仅活性组分具有高分散度,而且表面具有丰富的L酸位点,L酸位点与Ni活性中心协同作用有效提高了催化剂的高压加氢性能.而在Al_2O_3中直接引入SiO_2时,SiO_2覆盖了Al_2O_3表面的L酸位点,催化剂活性组分分散度较低,表现出低的加氢活性. 相似文献
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以低硅铝比(n(SiO2)/n(Al2O3)=20-45)的ZSM-5分子筛为催化剂, 研究了混合C4烃的催化裂解反应, 并对不同硅铝比的ZSM-5分子筛进行了酸性表征. 混合C4烃的催化裂解反应结果表明, 低硅铝比的ZSM-5分子筛具有较高的低温催化活性, 高硅铝比ZSM-5分子筛催化剂上乙烯和丙烯的收率高于低硅铝比ZSM-5分子筛催化剂, 低硅铝比ZSM-5分子筛上苯和甲苯的收率高于高硅铝比ZSM-5分子筛催化剂. 在反应温度为625 ℃时, 硅铝比为20的ZSM-5分子筛催化剂上乙烯、丙烯、苯和甲苯的总收率可达79.42%. 酸性表征结果表明, 硅铝比低的ZSM-5分子筛具有更多的Bronsted(B)酸酸量、Lewis(L)酸酸量及总酸酸量, 这是低硅铝比ZSM-5分子筛具有低温高活性及高的苯和甲苯收率的原因. 相似文献
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CoAPSO—5分子筛的合成与性能 总被引:1,自引:0,他引:1
用水热晶化法合成了CoAPSO-5分子筛,用X射线衍射,电子探针,红外光谱以及吸附吡啶的红外光谱等方法对其结构和表面性质进行了研究,并用甲苯甲醇烷基化反应考察了其催化性能,结果表明,CoAPSO-5为中强酸性分子筛,具有较高的甲苯甲醇烷基化活性和对二甲苯选择性,对二苯收率高于20%,且烷基化活性和对二甲茉选择性出现了“同向效应”。 相似文献