Chen Lu, Guan Xuze, Fei Zhaofu, Asakura Hiroyuki, Zhang Lun, Wang Zhipeng, Su Xinlian, Yao Zhangyi, Keenan Luke L, Hayama Shusaku, van Spronsen Matthijs A, Karagoz Burcu, Held Georg, Allen Christopher S, Hopkinson David G, Decarolis Donato, Callison June, Dyson Paul J, Wang Feng Ryan
Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.
Institute of Chemical Sciences and Engineering, École Polytechnique Fedérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.
Nat Commun. 2025 Jan 2;16(1):26. doi: 10.1038/s41467-024-54820-y.
Selective catalytic oxidation (SCO) of NH to N is one of the most effective methods used to eliminate NH emissions. However, achieving high conversion over a wide operating temperature range while avoiding over-oxidation to NO remains a significant challenge. Here, we report a bi-metallic surficial catalyst (PtCuO/AlO) with improved Pt atom efficiency that overcomes the limitations of current catalysts. It achieves full NH conversion at 250 °C with a weight hourly space velocity of 600 ml NH·h·g, which is 50 °C lower than commercial Pt/AlO, and maintains high N selectivity through a wide temperature window. Operando XAFS studies reveal that the surface Pt atoms in PtCuO/AlO enhance the redox properties of the Cu species, thus accelerating the Cu reduction rate and improving the rate of the NH-SCO reaction. Moreover, a synergistic effect between Pt and Cu sites in PtCuO/AlO contributes to the high selectivity by facilitating internal selective catalytic reduction.
将NH选择性催化氧化(SCO)为N是用于消除NH排放的最有效方法之一。然而,在较宽的操作温度范围内实现高转化率同时避免过度氧化为NO仍然是一项重大挑战。在此,我们报道了一种具有提高的Pt原子效率的双金属表面催化剂(PtCuO/AlO),它克服了现有催化剂的局限性。它在250°C、空速为600 ml NH·h·g的条件下实现了NH的完全转化,比商用Pt/AlO低50°C,并在很宽的温度窗口内保持高N选择性。原位XAFS研究表明,PtCuO/AlO中的表面Pt原子增强了Cu物种的氧化还原性能,从而加快了Cu的还原速率并提高了NH-SCO反应的速率。此外,PtCuO/AlO中Pt和Cu位点之间的协同效应通过促进内部选择性催化还原有助于实现高选择性。