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Shape dependence and sulfate promotion of CeO2 for selective catalytic reduction of NOx with NH3
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2018-03-20 , DOI: 10.1016/j.apcatb.2018.03.065
Lei Ma , Chang Yup Seo , Mohit Nahata , Xiaoyin Chen , Junhua Li , Johannes W. Schwank

Thermally stable CeO2 cubes and nanospheres were synthesized and modified by sulfation treatment. Non-sulfated CeO2 cubes and nanospheres did not exhibit good catalytic performance for selective catalytic reduction of NOx with NH3 (NH3-SCR), but mainly contributed towards an undesired side reaction of NH3 oxidation above 350 °C. Based on the structural, morphological and physicochemical characterization, it was observed that CeO2 nanospheres comprising small crystallites could easily release active oxygen species, which resulted in strong NH3 oxidation. However, sulfation treatment greatly improved the catalytic performance of NH3-SCR on both CeO2 cubes and nanospheres. Sulfated CeO2 catalysts did not contribute to significant NH3 oxidation due to the inhibited reducibility of Ce4+ coordinated with the surface sulfates. The adsorbed ammonia could be activated on Brønsted acid sites generated by the formation of surface Ce2(SO4)3 species, while gaseous NOx could be activated on separate surface sites of Ce4+. The presence of separate reaction sites for NH3 and NOx is believed to be important for the improved catalytic performance of SCR reaction. Sulfated CeO2 cubes outperformed sulfated CeO2 nanospheres in the entire test temperature window (200–500 °C). The improved performance of sulfated CeO2 cubes appears to be related to surfaces with abundant Brønsted acid sites and relatively weak reducibility of Ce4+. These fundamental findings contribute to a better mechanistic understanding needed for designing efficient CeO2-based NOx reduction catalysts in the future.



中文翻译:

CeO 2的形状依赖性和硫酸盐促进作用,用于NH 3选择性催化还原NO x

通过硫化处理合成并改性了热稳定的CeO 2立方体和纳米球。非硫酸化的CeO 2米的立方体,纳米球没有表现出用于选择性催化还原的良好催化性能NO X与NH 3(NH 3 -SCR),但主要是朝向贡献NH的不希望的副反应3高于350℃氧化。基于结构,形态和物理化学特征,观察到包含小微晶的CeO 2纳米球可以轻松释放活性氧,从而导致强烈的NH 3氧化。但是,硫酸化处理大大提高了NH的催化性能。CeO 2立方体和纳米球上的3 -SCR 。硫酸化的CeO 2催化剂没有抑制明显的NH 3氧化,因为与表面硫酸盐配位的Ce 4+的还原性受到抑制。吸附的氨可以在由铈的形成面的产生布朗斯台德酸位点被激活2(SO 43种,而气态的NO X可以在铈的单独的表面位点被激活4+。NH 3和NO x的单独反应位点的存在被认为对于改善SCR反应的催化性能是重要的。硫酸铈在整个测试温度窗口(200–500°C)中,有2个立方体的性能优于硫酸CeO 2纳米球。硫酸化的CeO 2立方体的性能改善似乎与具有丰富的布朗斯台德酸位和相对较弱的Ce 4+还原性的表面有关。这些基本发现有助于需要设计高效的总裁开了个更好的机制理解2为基础的NO X还原催化剂的未来。

更新日期:2018-03-20
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