Sulfur-Resistant Ceria-Based Low-Temperature SCR Catalysts with the Non-bulk Electronic States of Ceria

氮氧化物 催化作用 硫黄 化学工程 选择性催化还原 材料科学 粒子(生态学) 无机化学 化学 物理化学 冶金 有机化学 燃烧 海洋学 地质学 工程类
作者
Xiaolei Hu,Junxiao Chen,Weiye Qu,Rui Liu,Dongrun Xu,Zhen Ma,Xingfu Tang
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:55 (8): 5435-5441 被引量:57
标识
DOI:10.1021/acs.est.0c08736
摘要

Although ceria-based catalysts serve as an appealing alternative to traditional V2O5-based catalysts for selective catalytic reduction (SCR) of NOx with NH3, the inevitable deactivation caused by SO2 at low temperatures severely hampers the ceria-based catalysts to efficiently control NOx emissions from SO2-containing stack gases. Here, we rationally design a strong sulfur-resistant ceria-based catalyst by tuning the electronic structures of ceria highly dispersed on acidic MoO3 surfaces. By using Ce L3-edge X-ray absorption near edge structure spectra in conjunction with various surface and bulk structural characterizations, we report that the sulfur resistance of the catalysts is closely associated with the electronic states of ceria, particularly expressed by the Ce3+/Ce4+ ratio related to the size of the ceria particles. As the Ce3+/Ce4+ ratio increases up to or over 50%, corresponding to CeO2/MoO3(x %, x ≤ 2.1) with the particle size of approximately 4 nm or less, the non-bulk electronic states of ceria appear, where the catalysts start to show strong sulfur resistance. This work could provide a new strategy for designing sulfur-resistant ceria-based SCR catalysts for controlling NOx emissions at low temperatures.

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