MOF-Derived High-Entropy Oxide: A “Catalytic Engine” That Ignites the HC-SCR Reaction

作者：Mingyu Su, Yaxin Su, Yuhao Wang, Min Cui, Huqin Zheng, Sameer Shahid, Jacob Senior Atta Owusu, Wenyi Deng, Bingtao Zhao, Jarosław Zuwała · 发表于：ACS Catalysis · 年份：2025 · DOI：10.1021/acscatal.5c05308 · 被引用次数：11 · 研究领域：Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions、Electronic and Structural Properties of Oxides

Addressing the challenge of NO x pollution control in exhaust emissions from stationary and mobile sources, this study employed the ultrasonic impregnation method to synthesize high entropy-metal organic framework (HE-MOF) precursors loaded with transition metals (Fe/Co/Ni/Cu/Mn) in a one-step process. The reason for selecting these five metals stems from their known individual performances in the SCR reaction: Mn can efficiently oxidize NO to NO 2 by virtue of its abundant valence states, while Co assists in NO adsorption and the generation of nitrate species; Cu (especially Cu + ) can break the C–H bonds of C 3 H 6 to form active intermediates, and Fe reduces the deep oxidation of the reducing agent to improve its utilization rate; Ni not only stabilizes the structure of the MOF precursor, but also enhances catalytic performance through electron interaction with other metals via valence cycling (Ni 3+ /Ni 2+ ). Subsequently, these precursors were calcined at 350 °C to fabricate a series of catalysts, which show great potential for application in the field of denitrification. C 3 H 6 –SCR tests in a fixed-bed microreactor revealed that the SCR reactivities of the catalysts were improved gradually with the increase in the number of supported metal species. Notably, HEO-350 catalyst, maintained over 83% NO removal within the broad temperature window of 225–300 °C, with the highest NO conversion rate of 93.2% at 250 °C, and exhibited superior N 2 selectivity of higher than 95%....