Selective Catalytic Reduction of NOx with NH3 Over Fe Modified MOF-Derived MnOx Catalyst

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2024-08-01 DOI:10.1007/s10562-024-04792-x

Yao Wang, Ruiyang Chen, Jianglong Zhao, Zhiming Liu

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Abstract

A Fe modified MOF-derived MnO_x catalyst has been synthesized and studied for the selective catalytic reduction of NO_x with NH₃ (NH₃-SCR). Compared with pure MnO_x, Fe-modified MnO_x showed a broader activity temperature window, enhanced N₂ selectivity, and improved sulfur tolerance. On one hand, the incorporation of Fe into MnO_x increased acidity, thereby facilitating the adsorption of NH₃ as well as its activation, which plays a crucial role for the reduction of NO_x. On the other hand, the presence of Fe resulted in decreased Mn⁴⁺, which contributes to improved N₂ selectivity. Over Fe modified MnO_x catalyst, the coordinated NH₃, NH₄⁺, bridging nitrate and bidentate nitrate are reactive, and participate in the NH₃-SCR reaction following both “Eley–Rideal(E-R)” and “Langmuir–Hinshelwood(L–H)” mechanism. The present research provides an idea for broadening the activity temperature window and enhancing the sulfur tolerance of MnO_x catalyst for the reduction of NO_x, making it more suitable for practical application.

Graphical Abstract

Abstract Image

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在铁改性 MOF 衍生氧化锰催化剂上用 NH3 选择性催化还原氮氧化物

我们合成并研究了一种铁改性 MOF 衍生氧化锰催化剂，用于选择性催化还原氮氧化物与 NH3（NH3-SCR）。与纯 MnOx 相比，Fe 改性 MnOx 显示出更宽的活性温度窗口、更高的 N2 选择性和更好的硫耐受性。一方面，在 MnOx 中加入 Fe 增加了酸性，从而促进了 NH3 的吸附和活化，这对还原氮氧化物起着至关重要的作用。另一方面，铁的存在导致 Mn4+ 减少，从而提高了 N2 的选择性。在铁修饰的 MnOx 催化剂上，配位的 NH3、NH4+、桥接硝酸盐和双齿硝酸盐都具有活性，并按照 "E-R "和 "Langmuir-Hinshelwood "机制参与 NH3-SCR 反应。本研究为拓宽 MnOx 催化剂还原氮氧化物的活性温度窗口和提高硫耐受性提供了思路，使其更适合实际应用。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.