New SCR Catalysts Based on Mn Supported on Simple or Mixed Aerogel Oxides: Effect of Sulfates Addition

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2024-11-08 DOI:10.1007/s10562-024-04859-9

Jihene Arfaoui, Abdelhamid Ghorbel, Carolina Petitto, Gérard Delahay

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引用次数: 0

Abstract

New SCR catalysts based on Mn supported on simple or mixed aerogel oxides (Mn/ZrO₂, Mn/CeO₂-ZrO₂ and Mn/CeO₂-ZrO₂-SO₄²⁻) were prepared for selective catalytic reduction of nitrogen oxide by ammonia (NO-SCR by NH₃). One step sol gel method followed by supercritical drying process were used for elaborating the catalytic supports, however, Mn species were incorporated into aerogels via impregnation method. Structural, textural, acidic and redox properties of samples were studied using XRD; BET and porosity measurements; NH₃-TPD and H₂-TPR techniques. The results revealed that Mn/ZrO₂ and Mn/CeO₂-ZrO₂ solids develop mesoporous texture, good crystallinity of zirconia tetragonal phase and nano-sized particles but exhibit a poor NO-SCR activity. The addition of SO₄²⁻ induces a disorder in ZrO₂ structure but it generates very active strong acid sites for the high temperature NO reduction. 100% NO conversion into N₂ was achieved above 400 °C over the new Mn/CeO₂-ZrO₂-SO₄²⁻ catalytic system.

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基于简单或混合气凝胶氧化物上支撑的锰的新型 SCR 催化剂：添加硫酸盐的影响

制备了以锰为基础的新型 SCR 催化剂，这些催化剂支撑在简单或混合的气凝胶氧化物（Mn/ZrO2、Mn/CeO2-ZrO2 和 Mn/CeO2-ZrO2-SO42-）上，用于氨对氮氧化物的选择性催化还原（NH3 对 NO-SCR）。采用一步溶胶凝胶法和超临界干燥法制备催化支持物，但锰物种是通过浸渍法加入气凝胶中的。采用 XRD、BET 和孔隙度测量、NH3-TPD 和 H2-TPR 技术研究了样品的结构、质地、酸性和氧化还原特性。结果表明，Mn/ZrO2 和 Mn/CeO2-ZrO2 固体具有介孔质地、良好的氧化锆四方相结晶度和纳米尺寸的颗粒，但 NO-SCR 活性较差。加入 SO42- 会导致 ZrO2 结构紊乱，但会产生非常活跃的强酸位点，用于高温还原 NO。新的 Mn/CeO2-ZrO2-SO42- 催化体系在 400 °C 以上实现了 100% 的 NO 转化为 N2。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.