Redox-induced engineering of amorphous/crystalline MnFeOx catalyst enables H2O/SO2-tolerant NOx abatement at ultra-low temperatures

Liang Yi Lin*, Joy In Huang, Hsin Yu Tsai

*此作品的通信作者

研究成果: Article同行評審

摘要

Enhancing resistance to H2O and SO2 poisoning below 150 °C is essential for advancing Mn-based oxide catalysts in ultra-low temperature NH3-SCR of NO. To address this challenge, an amorphous/crystalline MnFey catalyst with engineered Mn-O-Fe interfaces and abundant surface defects was developed using a redox-induced precipitation method. The optimized MnFe0.2 catalyst demonstrates exceptional catalytic performance, achieving over 90 % NO conversion and N2 selectivity across a broad 120–260 °C range under highly humid conditions (15 vol% H2O). Most significantly, MnFe0.2 maintains remarkable stability under high humidity and SO2 at 120 °C for 60 h, vastly outperforming conventionally coprecipitated MnFe0.2(CP), which gradually deactivates. This superior performance is attributed to the uniform elemental distribution in MnFe0.2, which enhances the Mn-O-Fe redox cycle through improved electron transfer. These features promote superior low-temperature reducibility and acidity, enabling effective reactant adsorption and activation. Mechanistic studies further reveal that SO2 exposure deactivates MnFe0.2(CP) by forming ammonium (bi)sulfates and MnSO4, which hinder reactant adsorption and subsequent reactions. In contrast, the engineered Mn-O-Fe interfaces in MnFe0.2 enable Fe species to preferentially interact with SO2, shielding Mn from sulfation and significantly reducing deactivation. This work demonstrates a significant breakthrough in catalyst design for ultra-low temperature NH3-SCR, paving the way for the broader application of Mn-based catalysts in industrial NOx control technologies.

原文English
文章編號137618
期刊Journal of Hazardous Materials
489
DOIs
出版狀態Published - 5 6月 2025

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