在 CoxCry 氧化物上催化氧化 1,2-二氯苯

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2024-10-06 DOI:10.1016/j.apcata.2024.119975

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引用次数: 0

摘要

为了研究以 1,2-二氯苯（1,2-DCB）为模型化合物的氯化芳烃催化燃烧，我们合成了 CoxCry 混合氧化物。表征结果表明，铬可以以 Cr6+Ox 的形式存在于 Co3O4 表面，或以 Cr-O-Co 的形式掺入 Co3O4 中，从而增加了 Co3O4 的分散性。然而，当 Cr/Cr+Co = 0.4 或更高时，会出现 CrO2，Co 会反向分散到 CrO2 中。Co7Cr3 对 1,2-二氯苯氧化的催化活性最好，T90 为 288 ℃，其对 1,2,4-三氯苯的选择性在整个过程中低于 0.06%，远低于 Co3O4（45%）和 Co5Cr5（50%）。尖晶石基质中 Cr6+ 和 Cr-O-Co 的协同作用产生了强酸性和优异的还原性，确保了 Cl 的快速去除，并通过加速 Deacon 过程抑制了 1,2-DCB 的氯化，而 CrO2 则会造成严重的 Cl 沉积和 Cr 损失。因此，具有尖晶石结构的 CoxCry 催化剂性能优异，在 300 ℃ 下至少 50 小时内活性稳定。

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Catalytic oxidation of 1,2-dichlorobenzene over CoxCry oxides

Co_xCr_y mixed oxides were synthesized to investigate the catalytic combustion of chlorinated aromatics with 1,2-dichlorobenzene (1,2-DCB) as model compound. Characterizations show Cr can exist as Cr⁶⁺O_x on Co₃O₄ surface or be incorporated as Cr-O-Co into Co₃O₄, which increases the dispersion of Co₃O₄. However, CrO₂ appears and Co is conversely dispersed into CrO₂ when Cr/Cr+Co = 0.4 or higher. Co₇Cr₃ shows best catalytic activity for 1,2-DCB oxidation with T₉₀ of 288 ℃, and its 1,2,4-trichlorobenzene selectivity is below 0.06 % during whole process, much lower than Co₃O₄ (45 %) and Co₅Cr₅ (50 %). The synergism of Cr⁶⁺ and Cr-O-Co in spinel matrix contributes to the strong acidity and superior reducibility, ensuring the quick Cl removal and inhibiting the chlorination of 1,2-DCB through accelerating Deacon process, while CrO₂ suffers severe Cl deposition and Cr loss. Accordingly, Co_xCr_y catalysts with spinel structure present excellent performance and stable activity at 300 ℃ for at least 50 h.

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来源期刊

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.