TY - JOUR
T1 - Redox-induced engineering of amorphous/crystalline MnFeOx catalyst enables H2O/SO2-tolerant NOx abatement at ultra-low temperatures
AU - Lin, Liang Yi
AU - Huang, Joy In
AU - Tsai, Hsin Yu
N1 - Publisher Copyright:
© 2025 Elsevier B.V.
PY - 2025/6/5
Y1 - 2025/6/5
N2 - 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.
AB - 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.
KW - Fe-doped MnO
KW - Interfacial precipitation
KW - Oxygen defects
KW - Ultra-low temperature SCR
UR - http://www.scopus.com/inward/record.url?scp=85217925930&partnerID=8YFLogxK
U2 - 10.1016/j.jhazmat.2025.137618
DO - 10.1016/j.jhazmat.2025.137618
M3 - Article
AN - SCOPUS:85217925930
SN - 0304-3894
VL - 489
JO - Journal of Hazardous Materials
JF - Journal of Hazardous Materials
M1 - 137618
ER -