Ultrasonic-assistance influence on the impregnation method for high metal loading CoMo/Ti-HMS catalysts

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-01-25 DOI:10.1016/j.apcata.2025.120135
T.A. Zepeda
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Abstract

Here, it reports the influence of ultrasonic assistance during the impregnation process using traditional precursor salts of cobalt nitrate, molybdenum heptamolybdate, and citric acid as a chelating agent. The variation in metal loading (CoO + MoO3) from 16.1 wt% (12.7 wt% MoO3, 3.4 wt% CoO) to 46.8 wt% (35.7 wt% MoO3, 10.1 wt% CoO) was evaluated in the HDS of DBT. Ultrasonically-assisted impregnation demonstrated improved metal dispersion, improved the Co-Mo interactions and complete sulfidation of cobalt species, and enhanced the formation of well-dispersed CoMoS phase, unlike traditional impregnation catalysts that even exhibited non-sulfided Co species. Catalysts prepared using ultrasonic assistance exhibited a higher initial reaction rate for the HDS of DBT than their traditionally impregnated counterparts. Although the direct desulfurization pathway was the primary reaction route, the ultrasonic-assisted catalysts exhibited higher selectivity toward the hydrogenation pathway (higher HYD/DDS ratios), especially at higher metal loadings. The increased surface acidity, which correlated with rising metal content, enhanced the hydrogenation pathway during the HDS of DBT. Despite the superior catalytic performance of ultrasonic-assisted catalysts, the effectiveness of increasing metal content decreases at higher metal loadings, likely due to limitations in active site dispersion on the surface.
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超声辅助对高载金属量CoMo/Ti-HMS催化剂浸渍方法的影响
本文以硝酸钴、七钼酸钼、柠檬酸等传统前驱体盐为螯合剂,研究了超声辅助对浸渍过程的影响。在DBT的HDS中评估了金属载荷(CoO + MoO3)从16.1 wt%(12.7 wt% MoO3, 3.4 wt% CoO)到46.8 wt%(35.7 wt% MoO3, 10.1 wt% CoO)的变化。超声辅助浸渍改善了金属分散,改善了Co- mo相互作用和钴种的完全硫化,并促进了分散良好的CoMoS相的形成,而传统浸渍催化剂甚至表现出未硫化的Co种。超声辅助制备的催化剂对DBT HDS的初始反应速率高于传统浸渍的催化剂。虽然直接脱硫途径是主要的反应途径,但超声波辅助催化剂对加氢途径表现出更高的选择性(HYD/DDS比更高),特别是在高金属负载下。表面酸度的增加与金属含量的增加相关,增强了DBT HDS过程中的加氢途径。尽管超声波辅助催化剂具有优异的催化性能,但由于活性位点在表面的分散受到限制,金属负载越高,增加金属含量的效果越低。
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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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