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Forming pure shaped ZSM-5 zeolite bodies by a steam-assisted method and their application in methanol to aromatic reactions

机译:蒸汽辅助法形成纯形状的ZSM-5分子筛及其在甲醇中的芳烃反应应用

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For an industrial-scale catalytic process with a fixed or packed bed reactor, powder catalysts are not suitable because they may block the reaction pipe and increase the pressure of the reactor. Therefore, catalyst molding is essential for the industrial application of a catalyst. During the catalyst molding, binders are employed as indispensable additives that can achieve the mechanical strength requirements for industrial applications. However, the addition of binders may cover the activity sites of the catalyst and suppress the mass transfer of the reactants and products. So, traditional processes of catalyst molding significantly affect the catalytic performance. In this study, we proposed a vapor-phase-treatment to synthesize a pure shaped ZSM-5 zeolite with the re-crystallization of the binder incorporated silica sol and aluminum nitrate, which were converted into a part of ZSM-5 on a commercial H-ZSM-5 zeolite substrate. Subsequently, the shaped ZSM-5 catalyst was evaluated using the catalytic conversion of methanol to an aromatic (MTA reaction). The results showed that compared to the EPHZ catalyst, the SPHZ catalyst exhibited a long lifetime with a relatively high shape selectivity for methanol and aromatics. To rationalize these results and establish a structure–activity relationship, the zeolite catalysts were thoroughly characterized by XRD, NH _(3) -TPD, FT-IR, N _(2) adsorption, TG, SEM, TEM, ICP and Al MAS-NMR. The results demonstrated that an interesting intra-particle pore structure was formed within the monoliths of the SPHZ catalyst. Moreover, the superior catalytic performance obtained for SPHZ may have also been due to the broad acid strength distribution and the conversion of the silicon aluminum adhesive agent to zeolite crystals.
机译:对于具有固定床或填充床反应器的工业规模催化方法,粉末催化剂是不合适的,因为它们可能阻塞反应管并增加反应器的压力。因此,催化剂成型对于催化剂的工业应用是必不可少的。在催化剂成型过程中,将粘合剂用作必不可少的添加剂,可以达到工业应用的机械强度要求。然而,粘合剂的添加可以覆盖催化剂的活性部位并抑制反应物和产物的质量转移。因此,传统的催化剂成型工艺极大地影响了催化性能。在这项研究中,我们提出了一种汽相处理方法,以合成纯形状的ZSM-5沸石,然后将结合了硅溶胶和硝酸铝的粘合剂重结晶,然后将其在商用H上转化为ZSM-5的一部分。 -ZSM-5沸石基质。随后,使用甲醇到芳族化合物的催化转化(MTA反应)评估ZSM-5成型催化剂。结果表明,与EPHZ催化剂相比,SPHZ催化剂具有较长的使用寿命以及对甲醇和芳烃的较高的形状选择性。为了合理化这些结果并建立结构-活性关系,通过XRD,NH_(3)-TPD,FT-IR,N_(2)吸附,TG,SEM,TEM,ICP和Al MAS对沸石催化剂进行了全面表征。 -NMR。结果表明,在SPHZ催化剂的整料中形成了有趣的颗粒内孔结构。此外,由于宽的酸强度分布和硅铝粘合剂向沸石晶体的转化,也可能由于SPHZ获得了优异的催化性能。

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