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具有优异氨选择性催化氧化性能的Ru-W/CeZrO催化剂的合成:Ru与W物种之间的协同作用。

Synthesis of Ru-W/CeZrO catalyst with superior NH-SCO performance: Synergy between Ru and W species.

作者信息

Tian You, Han Zhitao, Zeng Qingliang, Zhao Hongzhe, Li Yeshan, Ma Dong

机构信息

Marine Engineering College, Dalian Maritime University, Dalian 116026, China.

Marine Engineering College, Dalian Maritime University, Dalian 116026, China.

出版信息

J Hazard Mater. 2025 Mar 15;486:137108. doi: 10.1016/j.jhazmat.2025.137108. Epub 2025 Jan 2.

Abstract

Ammonia selective catalytic oxidation (NH-SCO) is an effective method for NH removal. However, it is still a great challenge to develop catalysts with a wide operating temperature window, high catalytic activity and N selectivity, particularly for the removal of high-concentration NH from NH-fueled engine exhaust gas. Herein, a small amount of Ru (0.5 wt%) together with W were used to co-modify CeZrO through impregnation method to synthesize a novel NH-SCO catalyst. The as-prepared Ru-W/CeZrO catalyst could achieve a complete NH conversion at 300 °C, and a superior N selectivity, which exceeded 95.7 % over a wide temperature range of 225-400 °C. The physicochemical properties of the prepared catalysts were compared using various characterization techniques to reveal the possible roles of Ru and W species in NH-SCO reaction. XPS results showed that the introduction of Ru species was in favor of forming abundant surface adsorbed oxygen species on the surface of Ru-W/CeZrO catalyst, significantly enhancing the low-temperature activity. Besides, the co-existing W species could suppress the excessive oxidation of NH on catalyst surface, which was crucial for improving N selectivity. In-situ DRIFTS results suggested that Ru-W/CeZrO catalyst followed both the internal selective catalytic reduction (i-SCR) and amide (-NH) mechanisms during NH-SCO reaction. More importantly, the NH species adsorbed on Ru-W/CeZrO catalyst surface reacted more rapidly than that of W/CeZrO catalyst, and were mainly converted to N rather than NO or NO under the synergy of Ru and W species.

摘要

氨选择性催化氧化(NH-SCO)是一种去除氨的有效方法。然而,开发具有宽操作温度窗口、高催化活性和N选择性的催化剂仍然是一个巨大的挑战,特别是对于从以氨为燃料的发动机废气中去除高浓度氨而言。在此,通过浸渍法使用少量Ru(0.5 wt%)与W共同改性CeZrO,以合成一种新型NH-SCO催化剂。所制备的Ru-W/CeZrO催化剂在300°C时可实现氨的完全转化,并且具有优异的N选择性,在225-400°C的宽温度范围内超过95.7%。使用各种表征技术比较了所制备催化剂的物理化学性质,以揭示Ru和W物种在NH-SCO反应中的可能作用。XPS结果表明,Ru物种的引入有利于在Ru-W/CeZrO催化剂表面形成丰富的表面吸附氧物种,显著提高了低温活性。此外,共存的W物种可以抑制催化剂表面氨的过度氧化,这对于提高N选择性至关重要。原位DRIFTS结果表明,Ru-W/CeZrO催化剂在NH-SCO反应过程中遵循内部选择性催化还原(i-SCR)和酰胺(-NH)机制。更重要的是,吸附在Ru-W/CeZrO催化剂表面的氨物种比W/CeZrO催化剂的反应更快,并且在Ru和W物种的协同作用下主要转化为N而不是NO或NO。

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