MnFe@CeOx 核壳纳米笼在低温下用 NH3 选择性催化还原 NO,ACS Applied Nano Materials

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MnFe@CeOx 核壳纳米笼在低温下用 NH3 选择性催化还原 NO
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2022-03-02 , DOI: 10.1021/acsanm.1c04194
Ziguo Cai _{1,

2} , Guodong Zhang ₁ , Zhicheng Tang _{1,

3,

4} , Jiyi Zhang ₂

Affiliation

为了进一步提高锰基催化剂的催化性能和耐水（H _{2 O）性能，合成了一系列MnFe@CeO}_x核壳纳米笼。通过调整CeO ₂壳层的厚度，发现壳层厚度为60 nm的MnFe@CeO _x -60催化剂在120~250 ℃下的NO去除率可达80%以上。此外，它在 160°C 时表现出更好的 H _{2 O 抗性。}一系列表征证明MnFe@CeO _x -60催化剂具有丰富的氧空位缺陷位点和表面酸性位点。此外，MnFe@CeO _x -60 催化剂具有更多的 Mn ⁴⁺、Fe³⁺、Ce ³⁺和表面吸附的氧（O _ads）物种，以及MnO _x、FeO _x和CeO _x之间的强相互作用，使催化剂具有更好的催化活性。这表明CeO ₂壳的构造所产生的独特的界面扩散效应可以显着提高催化性能和H ₂ O抗性。同时，原位漫反射红外傅里叶变换分析表明，MnFe@CeO _x_{-60催化剂在NH 3}反应过程中主要遵循L-H反应机理。选择性催化还原（SCR）反应。最后，构建壳层可以巧妙地利用不同物种之间的扩散，实现活性物种之间的强相互作用，具有重要意义和普遍性。

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MnFe@CeOx Core–Shell Nanocages for the Selective Catalytic Reduction of NO with NH3 at Low Temperature

To enable the catalytic performance and water (H₂O) resistance of manganese-based catalysts to be further improved, a series of MnFe@CeO_x core–shell nanocages were synthesized. By adjustment of the thickness of the CeO₂ shell layer, it was found that the MnFe@CeO_x-60 catalyst with a shell layer thickness of 60 nm could exhibit more than 80% NO removal efficiency at 120–250 °C. In addition, it could exhibit better H₂O resistance at 160 °C. A series of characterizations proved that the MnFe@CeO_x-60 catalyst had abundant oxygen vacancy defect sites and surface acid sites. In addition, the MnFe@CeO_x-60 catalyst had more Mn⁴⁺, Fe³⁺, Ce³⁺, and surface-adsorbed oxygen (O_ads) species, as well as strong interactions between MnO_x, FeO_x, and CeO_x, so that the catalyst had better catalytic activity. This indicated that the unique interface diffusion effect produced by construction of the CeO₂ shell could remarkably enhance the catalytic performance and H₂O resistance. Simultaneously, the in situ diffuse-reflectance infrared Fourier transform analysis showed that the MnFe@CeO_x-60 catalyst mainly followed the L–H reaction mechanism during the NH₃ selective catalytic reduction (SCR) reaction. Finally, building a shell layer could skillfully utilize the diffusion between different species to realize strong interaction among active species, which was of great significance and universality.

更新日期：2022-03-02

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