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采用超声辅助水热法合成的不同 O 压力下 CeO-LaMnO 对 soot 的催化氧化评价。

Evaluation of the catalytic oxidation of soot by CeO-LaMnO at different O pressures synthesized by ultrasonic-assisted hydrothermal method.

机构信息

Universidad Autónoma de Nuevo León, Facultad de Ingeniería Civil, Av. Universidad S/N, Cd. Universitaria, 66455, San Nicolás de los Garza, Nuevo León, México.

Universidad Autónoma de Nuevo León, Facultad de Agronomía, Francisco Villa, S/N, 66050, General Escobedo, Nuevo León, México.

出版信息

Environ Sci Pollut Res Int. 2020 May;27(13):15475-15487. doi: 10.1007/s11356-020-08003-z. Epub 2020 Feb 19.

Abstract

In this work, the synthesis of catalyst with perovskite structure and chemical formula LaCeMnO at x = 0 - 0.5 were successfully obtained by an ultrasonic-assisted hydrothermal method. Results show that the addition of Ce in LaCeMnO have not substantial effect in textural and morphological properties; however, the formation of a new crystalline phase with final composition CeO-LaCeMnO was detected at values x > 0.3. All synthesized catalysts were tested in the soot oxidation under both, loose and tight contact in 20% O/N or 5% O/N atmospheres. CeO-LaCeMnO at x = 0.3 resulted in the best catalytic activity with activation energy values of 57.9 kJmol. The interaction between Ce and Mn species in this catalyst can transfer electrons generating Mn and Ce. This reduction from Mn to Mn is accompanied by migration of vacancies to the surface promoting the adsorbed oxygen from the gas phase, need for balancing the chemical states. By increasing the temperature above 300 °C, the bulk oxygen migration to the surface is enhanced being the responsible for the oxygen availability. The formation of CeO-LaCeMnO promotes a stable redox cycle allowing the reusability of this catalyst even at low oxygen pressures after three different reaction cycles.

摘要

在这项工作中,通过超声辅助水热法成功合成了具有钙钛矿结构和化学式 LaCeMnO 的催化剂,其中 x = 0-0.5。结果表明,Ce 的加入对 LaCeMnO 的结构和形貌特性没有实质性影响;然而,在 x > 0.3 时,检测到具有最终组成 CeO-LaCeMnO 的新晶相形成。所有合成的催化剂都在 20% O/N 或 5% O/N 气氛下的松散和紧密接触下进行了烟灰氧化测试。在 x = 0.3 时,CeO-LaCeMnO 表现出最佳的催化活性,其活化能值为 57.9 kJmol。该催化剂中 Ce 和 Mn 物种之间的相互作用可以转移电子,生成 Mn 和 Ce。这种从 Mn 到 Mn 的还原伴随着空位向表面的迁移,促进气相中吸附氧的平衡,以维持化学状态。当温度高于 300°C 时,体相中的氧迁移到表面,这是表面氧可用性增强的原因。CeO-LaCeMnO 的形成促进了稳定的氧化还原循环,使得即使在三个不同的反应循环后,在低氧气压力下,该催化剂也可以重复使用。

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