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Differences in oxidation-reduction kinetics and mobility of Cu species in fresh and SO2-poisoned Cu-SSZ-13 catalysts
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2020-11-27 , DOI: 10.1016/j.apcatb.2020.119756
Vitaly V. Mesilov , Susanna L. Bergman , Sandra Dahlin , Yang Xiao , Shibo Xi , Ma Zhirui , Lian Xu , Wei Chen , Lars J. Pettersson , Steven L. Bernasek

Fresh and SO2-poisoned Cu-SSZ-13 selective catalytic reduction (SCR) catalysts were studied using near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) in the presence of NH3, O2, and NO, as well as by in situ X-ray absorption spectroscopy (XAS) using H2, He, and CO. In contrast to the fresh catalyst, inhibited reduction of Cu-species and the absence of Cu-metal nanoparticles was found in the SO2-poisoned catalyst during heating/cooling in H2 and CO. High structural disorder and differences in the formation of Cu-carbonyl species were seen for the SO2-poisoned catalyst compared to the fresh catalyst. Suppressed oxidation-reduction and low mobility of Cu-species during exposure to NH3-SCR-related gases were observed in the SO2-poisoned catalyst, unlike in the fresh catalyst. These observations help explain catalyst deactivation during the standard NH3-SCR reaction. The formation of Cu-metal nanoparticles in the fresh catalyst revealed another possible deactivation pathway for the SCR-catalyst in combined LNT-SCR systems during fuel-rich periods.



中文翻译:

新鲜和SO 2中毒的Cu-SSZ-13催化剂中Cu物种的氧化还原动力学和迁移率的差异

在NH 3,O 2和NO存在的情况下,使用近环境压力X射线光电子能谱(NAP-XPS)研究了新鲜的和SO 2中毒的Cu-SSZ-13选择性催化还原(SCR)催化剂。如使用H 2,He和CO的原位X射线吸收光谱法(XAS)相比。与新鲜催化剂相反,在SO 2中毒后发现抑制了铜物种的还原,并且不存在铜金属纳米颗粒H 2和CO中加热/冷却过程中的催化剂。对于SO 2,观察到高结构无序性和Cu-羰基物质形成的差异与新鲜催化剂相比中毒的催化剂。与新鲜催化剂不同,在SO 2中毒的催化剂中观察到了Cu物种在暴露于NH 3 -SCR相关气体期间抑制了氧化还原和低迁移率。这些观察结果有助于解释标准NH 3 -SCR反应过程中催化剂的失活。新鲜催化剂中Cu-金属纳米颗粒的形成揭示了在富油期间组合LNT-SCR系统中SCR催化剂的另一种可能的失活途径。

更新日期:2020-11-27
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