Mechanism of N2 formation over the FeO-MnO2/SiO2 (100) surface in low-temperature NH3-SCR process: Electronic analysis of reaction pathways and key intermediates

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces Pub Date : 2024-10-30 DOI:10.1016/j.surfin.2024.105373

Shilin Bi , Baozhong Zhu , Jun Liu , Xianhang Sun , Fahua Zhu , Minggao Xu , Yunlan Sun

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Abstract

Density Functional Theory (DFT) was used to study the process and details of N₂ formation on the FeO-MnO₂/SiO₂ (100) surface during selective catalytic reduction of NH₃ (NH₃-SCR). The Fe and Mn sites on the surface of the FeO-MnO₂/SiO₂ (100) play important roles in denitrification. NH₃ forms stable chemical adsorption on its surface, especially with stronger adsorption capacity on the Fe sites than on the Mn sites. Furthermore, Fe sites demonstrate better performance in NH₃ dehydrogenation reactions in comparison to Mn sites, but the key intermediate NH₂NO tends to form on the Mn sites. NH₂NO may generate N₂ through a dehydrogenation reaction at the Fe sites on the catalyst surface, while it is more inclined to decompose and generate N₂ through internal migration on the Mn sites. These results help to deepen the understanding of the micro-mechanism of catalysts in N₂ generation, laying a theoretical foundation for improving the denitrification performance and N₂ selectivity of catalysts.

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低温 NH3-SCR 过程中 FeO-MnO2/SiO2 (100) 表面形成 N2 的机理：反应路径和关键中间产物的电子分析

密度泛函理论（DFT）用于研究选择性催化还原 NH3（NH3-SCR）过程中 N2 在 FeO-MnO2/SiO2 (100) 表面形成的过程和细节。FeO-MnO2/SiO2 (100) 表面的铁和锰位点在脱硝过程中起着重要作用。NH3 在其表面形成稳定的化学吸附，尤其是铁位点的吸附能力比锰位点强。此外，与锰位点相比，铁位点在 NH3 脱氢反应中表现出更好的性能，但关键的中间产物 NH2NO 往往在锰位点上形成。NH2NO 可能会在催化剂表面的 Fe 位点上通过脱氢反应生成 N2，而在 Mn 位点上则更倾向于通过内迁移分解并生成 N2。这些结果有助于加深对催化剂生成 N2 的微观机理的理解，为提高催化剂的脱硝性能和 N2 选择性奠定了理论基础。

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来源期刊

Surfaces and Interfaces Chemistry-General Chemistry

CiteScore

8.50

自引率

6.50%

发文量

753

审稿时长

35 days

期刊介绍： The aim of the journal is to provide a respectful outlet for ''sound science'' papers in all research areas on surfaces and interfaces. We define sound science papers as papers that describe new and well-executed research, but that do not necessarily provide brand new insights or are merely a description of research results. Surfaces and Interfaces publishes research papers in all fields of surface science which may not always find the right home on first submission to our Elsevier sister journals (Applied Surface, Surface and Coatings Technology, Thin Solid Films)