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负载于CeO、MnO和CeMnO混合氧化物上的Ag催化剂用于CH选择性催化还原NO

Ag Catalysts Supported on CeO, MnO and CeMnO Mixed Oxides for Selective Catalytic Reduction of NO by CH.

作者信息

La Greca Eleonora, Kharlamova Tamara S, Grabchenko Maria V, Consentino Luca, Savenko Daria Yu, Pantaleo Giuseppe, Kibis Lidiya S, Stonkus Olga A, Vodyankina Olga V, Liotta Leonarda Francesca

机构信息

Institute for the Study of Nanostructured Materials (ISMN), (Italian) National Research Council (CNR), Via Ugo La Malfa 153, 90146 Palermo, Italy.

Laboratory of Catalytic Research, Tomsk State University, Lenin Ave. 36, 634050 Tomsk, Russia.

出版信息

Nanomaterials (Basel). 2023 Feb 26;13(5):873. doi: 10.3390/nano13050873.

DOI:10.3390/nano13050873
PMID:36903752
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10005331/
Abstract

In the present study CeO, MnO and CeMnO mixed oxide (with molar ratio Ce/Mn = 1) were prepared by sol-gel method using citric acid as a chelating agent and calcined at 500 °C. The silver catalysts (1 wt.% Ag) over the obtained supports were synthesized by the incipient wetness impregnation method with [Ag(NH)]NO aqueous solution. The selective catalytic reduction of NO by CH was investigated in a fixed-bed quartz reactor using a reaction mixture composed of 1000 ppm NO, 3600 ppm CH, 10 vol.% O, 2.9 vol.% H and He as a balance gas, at WHSV of 25,000 mL g h.The physical-chemical properties of the as-prepared catalysts were studied by several characterization techniques, such as X-ray fluorescence analysis, nitrogen adsorption/desorption, X-ray analysis, Raman spectroscopy, transmission electron microscopy with analysis of the surface composition by X-ray energy dispersive spectroscopy and X-ray photo-electron spectroscopy. Silver oxidation state and its distribution on the catalysts surface as well as the support microstructure are the main factors determining the low temperature activity in NO selective catalytic reduction. The most active Ag/CeMnO catalyst (NO conversion at 300 °C is 44% and N selectivity is ~90%) is characterized by the presence of the fluorite-type phase with high dispersion and distortion. The characteristic "patchwork" domain microstructure of the mixed oxide along with the presence of dispersed Ag/Ag species improve the low-temperature catalyst of NO reduction by CH performance compared to Ag/CeO and Ag/MnO systems.

摘要

在本研究中，以柠檬酸为螯合剂，采用溶胶-凝胶法制备了CeO、MnO和CeMnO混合氧化物（Ce/Mn摩尔比 = 1），并在500℃下煅烧。以[Ag(NH₃)₂]NO₃水溶液，通过初湿浸渍法在所得载体上合成了银催化剂（1 wt.% Ag）。在固定床石英反应器中，使用由1000 ppm NO、3600 ppm CH₄、10 vol.% O₂、2.9 vol.% H₂和作为平衡气的He组成的反应混合物，在25,000 mL g⁻¹ h⁻¹的空速下研究了CH₄选择性催化还原NO的性能。通过多种表征技术研究了所制备催化剂的物理化学性质，如X射线荧光分析、氮吸附/脱附、X射线分析、拉曼光谱、透射电子显微镜以及通过X射线能量色散光谱和X射线光电子能谱分析表面组成。银的氧化态及其在催化剂表面的分布以及载体微观结构是决定NO选择性催化还原低温活性的主要因素。活性最高的Ag/CeMnO催化剂（300℃时NO转化率为44%，N₂选择性约为90%）的特征是存在具有高分散性和畸变的萤石型相。与Ag/CeO和Ag/MnO体系相比，混合氧化物特有的“拼凑”畴微观结构以及分散的Ag⁺/Ag物种的存在提高了CH₄还原NO的低温催化剂性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9a9/10005331/7b1057f575a3/nanomaterials-13-00873-g013.jpg
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