Defect Engineering of Ce-Modified Mullite Oxide Nanostructures for Low-Temperature Selective Catalytic Oxidation of NH 3 to N 2

作者：Tong Zhang, Lisha Wang, Zhiyuan Wang, Chenxu Wang, Yijian Liu, Guangwei Wang, Da Chen · 发表于：ACS Applied Nano Materials · 年份：2025 · DOI：10.1021/acsanm.5c04033 · 被引用次数：1 · 研究领域：Catalytic Processes in Materials Science、Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques

A high surface area Ce-modified YMn 2 O 5 –CeO 2 mixed oxide (YCMO) catalyst, featuring nanoscale phase dispersion, was prepared via a facile hydrothermal approach. The introduction of Ce suppressed further mullite phase formation and generated abundant oxygen vacancies and modulated the redox properties of Mn sites. The resulting nanoscale interfacial structure facilitates oxygen activation and transfer, leading to superior low-temperature NH 3 oxidation performance. The YCMO achieved 90% NH 3 conversion ( T 90 ) at 160 °C under a GHSV of 100,000 h –1 with 500 ppm of NH 3 and 21% O 2 in N 2, approximately 29 °C lower than YMn 2 O 5 (YMO) and 62 °C lower than commercial 1% Pt/Al 2 O 3, while maintaining stable N 2 selectivity across a broad temperature range (160–236 °C). Combined XRD, TEM, and O 2 -TPD analyses confirm the coexistence of finely dispersed CeO 2 and YMn 2 O 5 nanophases, which synergistically enhance surface oxygen mobility. Fundamentally, the exceptional performance arises from CeO 2 ’s role as an oxygen reservoir, supplying reactive oxygen species that enable rapid NH 3 deep oxidation and diverse nitrate intermediate formation via the internal SCR (i-SCR) mechanism, coupled with their facile thermal desorption to prevent deactivation. In situ DRIFTS revealed that bridged and bidentate nitrates exhibit high thermal sensitivity, desorbing readily without intermediate accumulation, thus sustaining efficient active-site regeneration. This work demonstrates that ...