Selective dealumination of large pore Zeolite Beta for effective Brønsted acid site utilization

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Pranit Samanta, Mohd. Ussama, Gourav Shrivastav, M. Ali Haider, K.K. Pant, Manjesh Kumar
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Abstract

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.

Abstract Image

Abstract Image

对大孔隙沸石 Beta 进行选择性脱铝以有效利用勃朗斯特德酸位点
通过空间和几何分布调节铝位点是实现确定性催化性能的一种新方法。为了设计出具有最佳物理化学属性的高效沸石 Beta 用于苯酚烷基化,我们使用一系列二羧酸进行了系统研究,以选择性地提取框架和/或非框架铝。在这里,后合成处理产生了硅铝比为 15-53 的脱铝催化剂。大量的铝和硅核磁共振研究表明,铝从沸石框架中被选择性地提取出来,并在 T 位点上重新合成。效力研究表明,pH 值、螯合能力和/或络合位点的可及性具有复杂的作用。不同的铝萃取导致了独特的超强酸性位点的出现。我们使用苯酚与环己醇进行烷基化,观察到丙二酸处理的沸石 Beta 转化率最高,并形成了所需的 CC 烷基化产物,这证明了我们的方法具有新颖性。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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