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Selective dealumination of large pore Zeolite Beta for effective Brønsted acid site utilization
Journal of Catalysis ( IF 6.5 ) Pub Date : 2024-10-16 , DOI: 10.1016/j.jcat.2024.115796
Pranit Samanta, Mohd. Ussama, Gourav Shrivastav, M. Ali Haider, K.K. Pant, Manjesh Kumar

Tuning of Al sites through spatial and geometric distribution is a novel pursuit for deterministic catalytic performance. To design an efficient Zeolite Beta for phenol alkylation with optimal physicochemical attributes, we conducted a systematic study with a series of dicarboxylic acids to selectively extract the framework and/or non-framework Aluminium. Herein, the post-synthetic treatment resulted in dealuminated catalysts of silicon-to-aluminum ratio ∼15–53. Extensive Al and Si NMR studies glean the selective extraction of aluminum from the zeolitic framework along with recomposition in T sites. The potency study alludes to the convoluted role of pH, chelating ability, and/or site accessibility for complexation. The differentiated Al extraction results in the emergence of unique super-strong acid sites. The novelty of our approach was established using phenol alkylation with cyclohexanol wherein we observed the highest conversion and desired CC alkylated product formation for the malonic acid-treated Zeolite Beta.

中文翻译:


大孔沸石 β 的选择性脱离以实现有效的 Brønsted 酸位点利用



通过空间和几何分布调整 Al 位点是确定性催化性能的一种新颖追求。为了设计一种具有最佳物理化学属性的用于酚烷基化的高效沸石 β,我们对一系列二羧酸进行了一项系统研究,以选择性提取框架和/或非框架铝。在此,合成后处理产生了硅铝比 ∼15-53 的脱硫催化剂。广泛的铝和硅 NMR 研究收集了从沸石框架中选择性提取铝以及 T 位点的重组。效价研究暗示了 pH 值、螯合能力和/或位点可及性对络合的复杂作用。差异化的 Al 提取导致独特的超强酸位点的出现。我们方法的新颖性是使用苯酚烷基化与环己醇建立的,其中我们观察到丙二酸处理的沸石 β 具有最高的转化率和所需的 CC 烷基化产物形成。
更新日期:2024-10-16
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