Investigation of the Dual-Regulatory Mechanism of Zr in MnRE1-xZrxO2+δ Oxide Catalysts for NO Oxidation,Small

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Investigation of the Dual-Regulatory Mechanism of Zr in MnRE1-xZrxO2+δ Oxide Catalysts for NO Oxidation
Small ( IF 13.0 ) Pub Date : 2024-09-06 , DOI: 10.1002/smll.202405740
Zihao Xu _{1,

2,

3,

4} , Dongming Chen _{2,

3,

4} , Rui Chen _{2,

3,

4} , Ziteng Mao _{2,

3,

4} , Zheng Zhao _{2,

3,

4} , Yongqi Zhang _{2,

3} , Meisheng Cui _{2,

3,

4} , Yongke Hou _{2,

3} , Chong Han ₁ , Juanyu Yang _{2,

3,

4} , Xiaowei Huang _{1,

2,

3,

4}

Affiliation

Utilizing Diesel Oxidation Catalysts (DOC) to partially oxidize NO to NO₂ is a crucial step in controlling NO_x emissions from diesel engines. However, enhancing both catalytic activity and hydrothermal stability remains a significant challenge. Benefiting from abundant asymmetric oxygen vacancies and increased Mn⁴⁺ content, MnRE_0.5Zr_0.5 exhibits superior NO oxidation performance (T₆₃ = 337 °C) and hydrothermal aging resistance (T₅₂ = 340 °C) compared to the undoped sample (T₅₃ = 365 °C). XPS, Raman, TPR, and XAS are employed to verify the elevation of oxygen vacancy concentration and Mn valence state modulation due to Zr introduction. Furthermore, compared to MnRE (1.36 eV), the formation energy of oxygen vacancies in MnRE_0.5Zr_0.5 is significantly reduced (0.17 eV). This work elucidates the dual regulatory role of Zr in the Mn-RE-Zr ternary system, providing theoretical support and guidance for the design of catalysts for atmospheric pollutant purification and industrial catalysis.

中文翻译：

MnRE1-xZrxO2+δ 氧化物催化剂中 Zr 的 NO 氧化作用研究

利用柴油氧化催化剂（DOC）将 NO 部分氧化为 NO₂ 是控制柴油发动机 NO_x 排放的关键步骤。然而，提高催化活性和水热稳定性仍然是一个重大挑战。得益于丰富的不对称氧空位和增加的 Mn⁴⁺ 含量，与未掺杂样品（T₅₃ = 365 °C）相比，MnRE_0.5Zr_0.5 表现出优异的 NO 氧化性能（T₆₃ = 337 °C）和耐水热老化性（T₅₂ = 340 °C）。XPS、Raman、TPR 和 XAS 用于验证由于 Zr 引入而导致的氧空位浓度升高和 Mn 价态调制。此外，与 MnRE （1.36 eV）相比，MnRE_0.5Zr_0.5 中氧空位的形成能显著降低（0.17 eV）。本工作阐明了 Zr 在 Mn-RE-Zr 三元体系中的双重调控作用，为大气污染物净化和工业催化催化剂的设计提供了理论支持和指导。

更新日期：2024-09-06

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