In Situ XAFS, XRD, and DFT Characterization of the Sulfur Adsorption Sites on Cu and Ce Exchanged Y Zeolites,The Journal of Physical Chemistry C

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In Situ XAFS, XRD, and DFT Characterization of the Sulfur Adsorption Sites on Cu and Ce Exchanged Y Zeolites
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-01-13 , DOI: 10.1021/acs.jpcc.1c09128
Henry J. Sokol ₁ , Amani M. Ebrahim ₂ , Stavros Caratzoulas ₃ , Anatoly I. Frenkel ₂ , Julia A. Valla ₁

Affiliation

Adsorptive desulfurization with Cu and Ce ion-exchanged Y zeolite (CuCeY) has proven to be an effective method for the removal of sulfur compounds from hydrocarbon fuels. In this study, Cu and Ce exchanged Y materials including CuY, CeY, and CuCeY were prepared and examined to investigate the mechanism behind the superior sulfur adsorption and selectivity of CuCeY. In situ conditions were used to study the materials as prepared for optimal desulfurization. X-ray diffraction (XRD) confirmed the absence of large well-ordered crystalline phases from metallic or oxide Cu and Ce after the reduction of the samples. The oxidation states and local environments of Cu and Ce were determined using X-ray adsorption fine structure (XAFS) analysis and correlated to theoretical findings obtained from density functional theory (DFT) calculations. XAFS data indicate the successful reduction of Cu species to Cu⁺ and Cu⁰, and Ce to Ce³⁺. Analysis of XAFS spectra located Cu and Ce within the Y zeolite framework with Cu cations in the six-member ring sites and as small metallic Cu clusters. Ce cations were found to occupy both six-member ring and hexagonal prism sites. These results reveal the structure of CuCeY as prepared for desulfurization and provide insight into its superior sulfur adsorption performance.

中文翻译：

Cu和Ce交换Y沸石上硫吸附位点的原位XAFS、XRD和DFT表征

使用 Cu 和 Ce 离子交换 Y 沸石 (CuCeY) 吸附脱硫已被证明是从烃类燃料中去除含硫化合物的有效方法。在本研究中，制备并检查了 Cu 和 Ce 交换的 Y 材料，包括 CuY、CeY 和 CuCeY，以研究 CuCeY 优异的硫吸附和选择性背后的机制。原位条件用于研究为最佳脱硫而制备的材料。X 射线衍射 (XRD) 证实在样品还原后不存在来自金属或氧化物 Cu 和 Ce 的大的有序结晶相。使用 X 射线吸附精细结构 (XAFS) 分析确定 Cu 和 Ce 的氧化态和局部环境，并与从密度泛函理论 (DFT) 计算获得的理论结果相关联。⁺和Cu ⁰，以及Ce 到Ce ³⁺。XAFS 光谱分析将 Cu 和 Ce 定位在 Y 沸石框架内，Cu 阳离子位于六元环位点和小的金属 Cu 簇中。发现 Ce 阳离子占据六元环和六角棱柱位点。这些结果揭示了为脱硫而制备的 CuCeY 的结构，并提供了对其优越硫吸附性能的深入了解。

更新日期：2022-01-27

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