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A-site defects in LaSrMnO_(3) perovskite-based catalyst promoting NOx storage and reduction for lean-burn exhausts

Journal of Rare Earths 2021年第8期39卷 959-968页

作者： Dongyue Zhao Yuexi Yang Zhongnan Gao Ye Tian Jing Zhang Zheng Jiang Xingang Li Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) State Key Laboratory of Chemical EngineeringTianjin Key Laboratory of Applied Catalysis Science and TechnologySchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800China

Herein,we report the high De-NOx performance of the A-site defective perovskite-based Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst.The formation of the defective perovskite structure can be proved by both the increased Mn^(4+)/Mn^(3+) ratio and serious lattice contraction due to cationic nonstoichiometry.It promotes the Sr doping into perovskite lattice and reduces the formation of the SrCO_(3) phase.Our results demonstrate that below 300℃ the A-site defective perovskite can be more efficiently regenerated than the SrCO_(3) phase as NOx storage sites due to the latter’s stronger basicity,and also exhibits the higher NO oxidation ability than the A-site stoichiometric and excessive catalysts.Both factors promote the lowtemperature De-NOx activity of the Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst through improving its NOx trapping efficiency.Nevertheless,above 300℃,the NOx reduction becomes the determinant of the De-NOx activity of the perovskite-based catalysts.A-site defects can weaken the interactions between perovskite and Pd,inducing activation of Pd sites by in-situ transformation from PdO to metallic Pd in the alternative leanburn/fuel-rich atmospheric alternations,which boosts the De-NOx activity of the Pd/La_(0.5)Sr_(0.3)MnO_(3) catalyst.The Pd/L_(0.5)Sr_(0.3)MnO_(3) catalyst exhibits the high sulfur tolerance as well.These findings provide insight into optimizing the structural properties and catalytic activities of the perovskite-based catalysts via tuning formulation,and have potential to be applied for various related catalyst systems.

关键词： Dc-NOx Nonstoichiometric perovskite Pd NOx storage and reduction Lean-burn exhausts Rare earths

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