Tuning the Spatial Distribution and Chemical Nature of Acid Sites in MCM-22 Zeolite by Atomically Dispersed Lanthanum Species for Alkylation of 2-Methylnaphthalene

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL
Yaxing Li, Xiaoyu Li, Haotian Zhang, Jiayi He, Kaining Su, Tianxiang Chen, Ruolin Zhang, Hua Xu, Yuchao Wu, Weisheng Yang, Lichen Liu
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Abstract

Rare-earth-promoted zeolites have broad applications in the petrochemical industry because modifying zeolites with rare-earth elements can remarkably improve hydrothermal stability and tune the physicochemical properties of the acid sites, resulting in substantial promotion in catalytic selectivity and long-term stability. However, for a specific reaction, it remains a challenge to elaborate the coordination environment of rare-earth elements within the zeolite structure and establish the structure–reactivity of rare-earth-promoted zeolite catalysts. In this work, we have employed multiple spectroscopy and electron microscopy techniques to elucidate the spatial location and coordination environment of atomically dispersed La species in MCM-22 concertedly. In particular, we have attempted to clarify the variation of the chemical nature of the acid sites in MCM-22 zeolite in response to the introduction of La promotor. By appropriately controlling the spatial distribution and chemical nature of the acid sites, we have obtained a La-modified MCM-22 catalyst with high activity, selectivity, and long-term stability (>800 h) for alkylation of 2-methylnaphthalene with methanol for the production of 2,6-dimethyl-naphthalene under industrially relevant conditions.

Abstract Image

原子分散镧对MCM-22沸石中酸位空间分布和化学性质的影响
稀土促进沸石在石油化工领域有着广泛的应用,因为用稀土元素修饰沸石可以显著提高沸石的水热稳定性,调节酸位的物理化学性质,从而大大提高催化选择性和长期稳定性。然而,对于具体的反应,如何阐述沸石结构中稀土元素的配位环境,建立稀土促进的沸石催化剂的结构-反应性仍然是一个挑战。在这项工作中,我们采用了多种光谱和电子显微镜技术,共同阐明了原子分散的La在MCM-22中的空间位置和配位环境。特别是,我们试图澄清MCM-22分子筛中酸位的化学性质随La促进剂的引入而发生的变化。通过适当控制酸位的空间分布和化学性质,我们获得了一种具有高活性、选择性和长期稳定性(>800 h)的la改性MCM-22催化剂,用于在工业相关条件下将2-甲基萘与甲醇烷基化以生产2,6-二甲基萘。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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