Phosphorus modified hierarchically structured ZSM-5 zeolites for enhanced hydrothermal stability and intensified propylene production from 1-butene cracking
Phosphorus modified hierarchically structured ZSM-5 zeolites for enhanced hydrothermal stability and intensified propylene production from 1-butene cracking
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磷改性分级结构 ZSM-5 沸石可增强水热稳定性并强化 1-丁烯裂解生产丙烯
DOI：
10.1016/j.micromeso.2017.03.037
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发表时间：
2017-07
期刊：
影响因子：
--
通讯作者：
Jianlin Shi
中科院分区：
文献类型：
--
作者：
Jian Lv;Zile Hua;TongGuang Ge;Jinlin Zhou;Jian Zhou;ZhiCheng Liu;Hangle Guo;Jianlin Shi
采用无介孔剂的方法合成了具有分级结构的ZSM-5分子筛（HSZ），并通过磷酸溶液浸渍法用不同磷含量（1- 3wt%）对其进行了改性。采用多种技术对材料进行表征，结果表明，磷改性后HSZ的分级结构得到了很好的保留，更有趣的是，其水热稳定性得到了显著提高，即使在750 °C下100%水蒸汽中处理4 h，其主要织构性质几乎没有变化。磷诱导四面体骨架铝（TFAL）脱铝后，HSZ的强酸位逐渐消失，而弱酸位几乎保持完整。在1-丁烯裂解反应中，磷改性的HSZ在辅助介孔和磷改性的作用下，丙烯的选择性（约52%）和收率（约43%）得到显著提高，并表现出良好的上级抗失活能力。磷改性HSZ的这些性质使其成为一种具有工业应用前景的催化剂。
Hierarchically structured ZSM-5 zeolites (HSZ) were synthesized by a mesoporogen-free procedure and subsequently modified with varied amounts of phosphorus (1–3 wt%) through impregnation of phosphoric acid solution. Materials characterization using various techniques showed that the hierarchical structures of HSZ were well preserved after phosphorus modification, and more interestingly, their hydrothermal stability were improved significantly and the main textural properties kept almost unchanged even after hydrothermally treated at 750 °C for 4 h in 100% steam. The strong acid sites of HSZ were found to be gradually eliminated by the phosphorus induced dealumination of tetrahedral framework aluminum (TFAL), however, weak acid sites remained almost intact. In the 1-butene cracking reactions, benefitting from the auxiliary mesopores and phosphorus modification, P-modified HSZ showed remarkably improved selectivity (∼52%) and yield (∼43%) of propylene as well as superior anti-deactivation ability. All these properties of P-modified HSZ made it a promising catalyst for industrial application.
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