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解析Pt-V串联催化剂上氨选择性催化氧化中高氮选择性的机理

Unraveling the Mechanism of High N Selectivity in Ammonia Selective Catalytic Oxidation on Pt-V Tandem Catalyst.

作者信息

Gao Yu, Li Pingshang, Mei Wan

机构信息

China Waterborne Transport Research Institute, Beijing 100083, China.

School of Environment, Beijing Jiaotong University, Beijing 100044, China.

出版信息

Materials (Basel). 2025 Apr 14;18(8):1782. doi: 10.3390/ma18081782.

Abstract

V/Pt/TiO tandem catalysts exhibit both an outstanding low-temperature NH conversion rate and high N selectivity in NH-SCO reactions, but the mechanism of high N selectivity remains unclear. In this work, V/Pt/TiO tandem catalysts were synthesized through a two-step impregnation-deposition method. The modulating effect of the V loading mount on NH-SCO performance was evaluated, and the relevant reaction mechanism was explored systematically. The results demonstrated that the synergistic effect of tandem NH oxidation and NH-SCR reactions could be regulated by changing the V loading amount, thereby modulating N selectivity. Compared with other V/Pt/TiO catalysts and previously reported SCO catalysts, the V/Pt/TiO catalyst with a V loading amount of 0.5 wt.% exhibited outstanding NH-SCO performance, which achieved complete NH conversion and >90% of N selectivity within a range of 250-450 °C. XPS, NH-TPD, and O-TPD results suggested that the increase in the V loading amount from 0.1 wt.% to 0.5 wt.% was conducive to increasing the relative contents of Pt and V species, as well as the amount of acid sites, oxygen species, and oxygen vacancies. Consequently, the synergistic effect of tandem NH oxidation and NH-SCR reactions was significantly enhanced, enabling the catalyst to exhibit excellent N selectivity. A further increase in the V loading amount from 0.5 wt.% to 0.9 wt.% would bring about the opposite effect to the above, resulting in a decline in catalytic performance. In situ DRIFTS results showed that a V loading amount of 0.5 wt.% was beneficial for -NH species to participate in NH-SCO reactions, thereby boosting N selectivity.

摘要

V/Pt/TiO 串联催化剂在 NH-SCO 反应中表现出出色的低温 NH 转化率和高 N 选择性,但高 N 选择性的机理尚不清楚。在这项工作中,通过两步浸渍-沉积法合成了 V/Pt/TiO 串联催化剂。评估了 V 负载量对 NH-SCO 性能的调节作用,并系统地探索了相关反应机理。结果表明,通过改变 V 负载量可以调节串联 NH 氧化和 NH-SCR 反应的协同效应,从而调节 N 选择性。与其他 V/Pt/TiO 催化剂和先前报道的 SCO 催化剂相比,V 负载量为 0.5 wt.% 的 V/Pt/TiO 催化剂表现出出色的 NH-SCO 性能,在 250-450 °C 范围内实现了 NH 的完全转化和 >90% 的 N 选择性。XPS、NH-TPD 和 O-TPD 结果表明,V 负载量从 0.1 wt.% 增加到 0.5 wt.% 有利于增加 Pt 和 V 物种的相对含量,以及酸位点、氧物种和氧空位的数量。因此,串联 NH 氧化和 NH-SCR 反应的协同效应显著增强,使催化剂表现出优异的 N 选择性。V 负载量从 0.5 wt.% 进一步增加到 0.9 wt.% 将产生与上述相反的效果,导致催化性能下降。原位 DRIFTS 结果表明,0.5 wt.% 的 V 负载量有利于 -NH 物种参与 NH-SCO 反应,从而提高 N 选择性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e6b5/12028860/2ffcb9f9cc1a/materials-18-01782-g001.jpg

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