首页|Ce离子改性对Cu-SSZ-13催化剂NH3-SCR反应性能的影响研究

Ce离子改性对Cu-SSZ-13催化剂NH3-SCR反应性能的影响研究

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Cu-SSZ-13催化剂已被证实是高效NH3-SCR催化剂.然而,其经过严重水热老化(950 ℃)后仍会导致不可逆失活.本文通过考察引入的第二活性金属(Ce)离子浓度对Cu-SSZ-13催化剂的活性位性质及其催化活性的影响,揭示了活性位与催化活性之间的关系.结果表明,Cu-SSZ-13中引入的Ce离子并不会成为NH3-SCR反应的活性中心,而仅起到调节Cu活性位和表面酸性位的位置和数量的作用.通过XPS、H2-TPR、NH3-TPD和活性分析结果可知,低铈负载(约0.2%)下,少量的Ce可进入离子交换位点,有助于稳定SSZ-13骨架结构和抑制CuOx团簇生成的作用(950 ℃老化后劣化率仅为6%),还能实现高铜负载(Cu负载量为3.01%)与丰富的L酸、B酸位,从而使其具有高的NO转化率、更宽的NO反应温度窗口和优异的水热稳定性.而引入过量的铈离子对Cu-SSZ-13的催化活性和水热稳定性产生不利影响,导致SCR性能下降.
Effect of Ce Ions Modification on NH3-SCR Reaction Performance of the Cu-SSZ-13 Catalyst
The Cu-SSZ-13 catalyst has been proved to be a high-efficiency NH3-SCR catalyst.However,it will still cause irreversible inactivation after severe hydrothermal aging(950 ℃).This paper reveals the relationship between the active sites and the catalytic activity of the Cu-SSZ-13 catalyst by investigating the effect of the concentration of the second metal ion(Ce)introduction on the properties of the active sites(copper sites,acid sites)and the catalytic activity.The results show that the Ce ion introduction in Cu-SSZ-13 does not become the active center of the NH3-SCR reaction,but only plays a role in regula-ting the position and quantity of Cu sites in the CHA cage and the amount of acid sites on the surface of the catalyst.Accord-ing to XPS,H2-TPR,NH3-TPD and activity analysis results,a small amount of Ce under low cerium loading(about 0.2%)can enter the ion exchange site,which is conducive to stabilizing the skeleton structure of SSZ-13 and inhibiting the formation of CuOx clusters(the degradation rate after aging at 950 ℃ is only 6%),it can also achieve high copper loading(3.01%Cu loading)and rich L acid and B acid sites,resulting in high NO conversion,wider reaction temperature window and excellent hydrothermal stability.Nevertheless,the introduction of excessive cerium ions has a negative effect on the catalytic activity and the hydrothermal stability of the Cu-SSZ-13 catalyst,leading to a decrease in SCR performance.

NH3-SCRSSZ-13copper ioncerium ionacid sites

赵文怡、申孟林、朱悦然、任旭东、李新刚

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天津大学化工学院,天津 300350

包头稀土研究院白云鄂博稀土资源研究与综合利用全国重点实验室,内蒙古 包头 014030

NH3-SCR SSZ-13 Cu离子 Ce离子 酸性位

2024

稀土
中国稀土学会 包头稀土研究院

稀土

CSTPCD北大核心
影响因子:1.172
ISSN:1004-0277
年,卷(期):2024.45(2)
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