Effect of praseodymium substitution on La1-xPrxMnO3 (x=0–0.4) perovskites and catalytic activity for NO oxidation

Effect of praseodymium substitution on La1-xPrxMnO3 (x=0–0.4) perovskites and catalytic activity for NO oxidation
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镨替代对La1-xPrxMnO3 (x=0−0.4)钙钛矿的影响及NO氧化催化活性

DOI:
10.1016/j.jpcs.2019.05.001
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发表时间:
2019-10
影响因子:
4
通讯作者:
李星
李星
中科院分区:
材料科学3区
文献类型:
--
作者:
顾清秀;王丽;王颖;李星

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采用柠檬酸溶胶-凝胶法制备了La1-xPrxMnO3(x= 0,0.05,0.1,…,0.4)钙钛矿。采用x射线衍射(XRD)、x射线光电子能谱(XPS)、Brunauer-Emmett-Teller (BET)、n2吸附-解吸分析、O2-TPD、H2-TPR和NO- tpd等表征技术,探讨了Pr取代的影响。然后对样品进行催化NO氧化活性试验。当x ≤ 0.2时,NO转化率随Pr取代量的增加而提高,随Pr取代量的增加而降低。La0.8Pr0.2MnO3在260 °C时的NO转化率最高,达到91%。结果表明,适当的Pr (x≤ 0.2)可以改善LaMnO3的还原性,提高Mn4+/Mn3+和Oads/Ototal的摩尔比,有利于NO的氧化。此外,在适当的Pr组分的帮助下,NO吸附量的增加和硝酸盐分解温度的降低是活性增强的原因。
La1-xPrxMnO3(x= 0, 0.05, 0.1, …, 0.4) perovskites were prepared readily via citric acid sol–gel method in the present study. Several characterization techniques have been employed, such as X-ray diffraction (XRD), X-ray photoelectron spectra (XPS), Brunauer-Emmett-Teller (BET), N2adsorption–desorption analyses, Oxygen temperature-programmed desorption (O2-TPD), Hydrogen temperature-programmed reduction (H2-TPR) and NO temperature-programmed desorption (NO-TPD), with the aim of exploring the effects of Pr substitution. Then the samples were submitted to activity test in catalytic NO oxidation. NO conversion was improved with the increase of Pr substitution when x ≤ 0.2, and then decreased with further addition of Pr. The most excellent catalytic activity with NO conversion of 91% at 260 °C was observed on La0.8Pr0.2MnO3. It was revealed that the appropriate Pr addition (x≤ 0.2) at A-site led to the modified reducibility of LaMnO3, as well as the increased molar ratio of Mn4+/Mn3+and Oads/Ototal, which was benificial for NO oxidation. Moreover, the increase of NO adsorption amount and the shift of the decomposition temperature of nitrates to lower temperautre with the aid of appropriate Pr component accounted for the enhanced activity.
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