Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-03-03 , DOI: 10.1016/j.jhazmat.2021.125565 Hui Wang , Zhenping Qu , Lianlian Liu , Shicheng Dong , Yujie Qiao
The mesoporous Fe doped CeO2 catalyst after modifying organic sulfate functional groups show an excellent activity with above 80% NOx conversion in a temperature range of 250–450 °C. These organic-like sulfate groups bound to the Fe-O-Ce species leads to the strong electron interaction between Fe3+-O-Ce4+ species and sulfate groups, which modifies the acidity and redox properties of catalyst. The strong ability of S˭O/S-O in sulfate groups to accommodate electrons from a basic molecule is a driving force in the generation of acidic properties, and thus promotes to produce new Brønsted acid sites. The bondage of Fe-O-Ce species obviously inhibits the creation of thermostable bidentate NO3− species. Besides, the redox cycles between Fe3+ and Ce4+ are disrupted, thus inhibiting NH3 oxidation at medium-high temperatures and resulting in the increase of NOx conversion. Furthermore, the in situ DRIFTS results show that for the fresh samples, the coordinate NH3 reacts not only with NO3− through L-H mechanism, but also with oxygen species to form NOx. Differently for sulfated sample, the coordinate NH3 might react with achieved NO2 instead of the oxygen species through E-R mechanism, meanwhile the NH4+ could react with the NO3− species through L-H mechanism.
中文翻译:
介孔Fe掺杂CeO 2催化剂的硫酸盐改性促进NH 3 -SCR活性的结构和机理
改性有机硫酸盐官能团后,介孔铁掺杂的CeO 2催化剂在250-450°C的温度范围内具有出色的活性,NO x转化率超过80%。与Fe-O-Ce物种结合的这些类有机硫酸盐基团导致Fe 3+ -O-Ce 4+物种与硫酸盐基团之间的强电子相互作用,从而改变了催化剂的酸度和氧化还原性能。硫酸盐基团中S˭O/ SO具有较强的适应来自碱性分子的电子的能力,这是产生酸性性质的驱动力,因此促进产生新的布朗斯台德酸位。的Fe-O-Ce的物种的束缚明显抑制热稳定的二齿NO的产生3 -物种。此外,铁之间的氧化还原循环3+和Ce 4+被破坏,从而抑制NH 3的氧化在中等高温下,并导致增加的NO X转化率。此外,原位DRIFTS结果表明,对于新鲜样品,坐标NH 3发生反应不仅与NO 3 -经LH机构,而且还与氧物种以形成NO X。与硫酸盐样品不同的是,配位NH 3可能通过ER机理与获得的NO 2发生反应,而不是与氧发生反应,同时NH 4 +可以与NO反应3 -物种通过LH机制。