载MnOx分级β沸石催化降解大体积芳烃的研究

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL
Shurui Duan , Yuan Xu , Li Xu , Si Wu , Tan Guo , Yu Wang
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引用次数: 0

摘要

传统的β沸石由于其有限的孔径和相对较低的外表面积,阻碍了大体积反应物分子的有效扩散,限制了活性位点的可及性和负载。在此,我们通过合理的水热和随后的氧化还原沉淀策略开发了分层加载MnOx的β沸石(MnOx/m-β)。与传统的MnOx/β相比,分层结构赋予MnOx/m-β更高的外表面积和优化的孔隙结构,有利于MnOx物种的均匀分散和大分子的快速扩散。以邻二甲苯、邻二甲苯和1,3,5-三甲苯(TMB)的吸附和催化氧化为探针反应,m-β对邻二甲苯(45.3 mg/g)和TMB(91.4 mg/g)的吸附能力显著提高,分别是常规β的1.7倍和3.8倍。此外,MnOx/m-β在260 °C、300 °C和250 °C的温度下分别实现了甲苯、邻二甲苯和TMB的完全氧化,显著低于MnOx/β所需的温度。这种优异的催化性能归因于增强的Mn4 +活化晶格氧迁移率、分层传质通道和丰富的可达活性位点的协同作用。设计的β分层结构有望有效去除大块芳香烃。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Hierarchical MnOx loaded β zeolite as efficient catalyst for bulky aromatic hydrocarbon catalytic degradation
Conventional β zeolite exhibits limitations stemming from its constrained pore size and relatively low external surface area, impeding the efficient diffusion of bulky reactant molecules and limiting the accessibility and loading of active sites. Herein, we developed a hierarchical MnOx loaded β zeolite (MnOx/m-β) via a rational hydrothermal and subsequent redox-precipitation strategy. The hierarchical structure endows MnOx/m-β with a higher external surface area and optimized pore architecture, facilitating both the uniform dispersion of MnOx species and rapid diffusion of bulky molecules than conventional MnOx/β. Taking adsorption and catalytic oxidation of toluene, o-xylene, and 1,3,5-trimethylbenzene (TMB) as probe reactions, m-β exhibits significantly enhanced adsorption capacities for o-xylene (45.3 mg/g) and TMB (91.4 mg/g), representing 1.7 and 3.8 times increases compared to conventional β, respectively. Furthermore, MnOx/m-β achieves complete oxidation of toluene, o-xylene, and TMB at ca. 260 °C, 300 °C and 250 °C, respectively, significantly lower than those required for MnOx/β. This superior catalytic performance is attributed to the synergistic effects of enhanced Mn4 + -activated lattice oxygen mobility, hierarchical mass transfer channels, and abundant accessible active sites. The designed hierarchical architecture of β holds promise for the efficient removal of bulky aromatic hydrocarbon.
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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