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受限空间内的超细 Ru 物种:一种用于苯的超深度脱硫的有效吸附剂。

Ultrafine Ru species within confined space: An efficient adsorbent for ultra-deep desulfurization of benzene.

机构信息

State Key Laboratory of Advanced Technologies for Comprehensive Utilization of Platinum Metals, Kunming Institute of Precious Metals, Kunming, 650106, China.

College of Chemistry, Jilin University, Changchun, 130021, China.

出版信息

Chemosphere. 2020 Oct;256:127077. doi: 10.1016/j.chemosphere.2020.127077. Epub 2020 May 14.

DOI:10.1016/j.chemosphere.2020.127077
PMID:32438124
Abstract

The ultra-deep adsorptive desulfurization (ppb level) of benzene remains a challenging subject with the need to construct efficient adsorbent systems. Herein, a kind of ruthenium-based adsorbent functionalized with bimetallic Ru-Al was rationally designed using AlO as support (denoted as 0.8%Ru-1.2%Al/AlO). It was found that the co-anchoring of Ru and Al species endows the Ru-based adsorbent unique adsorption capability, which is able to completely eliminate sulfur compounds in benzene, and exhibiting a much higher breakthrough sulfur capacity than that of the 0.8%Ru/AlO. Remarkably, under the industrial experiment conditions, 0.8%Ru-1.2%Al/AlO exhibited excellent long-term stability for more than 1200 h, showing the potential for industrial application. Various characterization techniques, including BET, XRD, SEM, TEM, TPD-MS, TPR and XPS, were used to investigate the correlation between the adsorption performance and the microstructure of the adsorbents. Over 0.8%Ru-1.2%Al/AlO, the ultra-thin aluminum additive is beneficial to improve the dispersion of Ru species, which therefore exhibits desirable desulfurization efficiency. Moreover, the enhanced performance is also correlated to the presence of the suitable Ru active centers generated from the selective coverage by Al species. It leads to an optimal exposure of the Ru active centers, which would facilitate the interaction of S-Ru and the improvement of the desulfurization activity.

摘要

苯的超深度吸附脱硫(ppb 级)仍然是一个具有挑战性的课题,需要构建高效的吸附剂体系。在此,本文通过以 AlO 为载体合理设计了一种负载双金属 Ru-Al 的钌基吸附剂(记为 0.8%Ru-1.2%Al/AlO)。结果表明,Ru 和 Al 物种的共锚定赋予了基于 Ru 的吸附剂独特的吸附能力,能够完全去除苯中的硫化合物,并且表现出比 0.8%Ru/AlO 更高的突破硫容量。值得注意的是,在工业实验条件下,0.8%Ru-1.2%Al/AlO 表现出优异的长期稳定性,超过 1200 h,显示出工业应用的潜力。各种表征技术,包括 BET、XRD、SEM、TEM、TPD-MS、TPR 和 XPS,用于研究吸附性能与吸附剂微观结构之间的相关性。在 0.8%Ru-1.2%Al/AlO 上,超薄的铝添加剂有利于提高 Ru 物种的分散性,从而表现出理想的脱硫效率。此外,性能的增强还与 Al 物种选择性覆盖产生的合适 Ru 活性中心的存在有关。这导致 Ru 活性中心的最佳暴露,从而促进 S-Ru 的相互作用和脱硫活性的提高。

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