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Pd-M-TiO2 (M=Mn, Cu, Ce and Fe) as passive NOx adsorber (PNA) at low temperature

Pd-M-TiO2 (M=Mn,Cu,Ce and Fe)催化剂的低温氮氧化物吸附性能

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Abstract

A series of transition metal Mn, Cu, Ce and Fe were loaded on TiO2 by sol-gel method with noble metal Pd as promotor for the application of passive NOx absorber. Experiments on adsorption and desorption of NOx were conducted and characterization methods such as X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and in situ Fourier transform infrared spectroscopy (in situ DRIFTS) were involved. The experimental results show that Mn-contained catalysts, Mn-Ti and Pd-Mn-Ti, performed excellent NOx adsorbing ability and appropriate desorption temperature window. On the other hand, Ce- and Cu-contained samples were not suitable for the purpose of PNA. In addition to the low adsorption capacity, these two series of catalysts released massive amount of NO below 150 °C. Characterization results indicated that Pd was highly dispersed on all catalysts. The loading of Pd lowered not only the valence states of transition metals but surface oxygen percentage as well. From in situ DRIFTS tests, the Pd had little influence on the types of adsorbed substances for Mn, Ce and Cu series. However, the storage forms of NOx were obviously different on Pd-Fe-Ti and Fe-Ti.

摘要

本文采用溶胶-凝胶法制备了以TiO2为载体,Mn、Cu、Ce、Fe 为主要活性成分,贵金属Pd为促 进组分的一系列催化剂, 并将其用于氮氧化物的吸附(PNA)。采用XRD、XPS、TEM 以及原位 DRIFTS 等手段对催化剂进行表征。NOx吸脱附试验结果表明,含Mn催化剂(Pd-Mn-Ti 以及Mn-Ti) 有较强的NOx吸附能力且具有合适的脱附温度窗口。而含Ce、Cu 催化剂不适合作低温NOx吸附催化 剂,NOx的吸附量较低,且在随后的程序升温脱附试验中,低于150 °C即有大量NO脱附,不利于在 下游SCR催化剂进行进一步反应。XRD和TEM结果表明,贵金属Pd 在催化剂表面分散较好。XPS结 果显示,负载Pd 以后Mn、Cu、Ce、Fe 这四种金属的价态都有降低,并同时都伴随有表面氧浓度降 低。由此可见,元素价态和表面氧浓度并非是影响NOx吸附性能的主要因素。从原位DRIFTS 结果可 以看出,Pd对于氮氧化物在含Mn、Cu、Ce催化剂表面吸附形式的影响较小,但对于NOx在含Fe 催化 剂上的吸附形式和吸附量都有着显著影响,可推测Pd-Fe 之间有着较强的相互作用。

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Authors and Affiliations

  1. Key Laboratory for Power Machinery and Engineering of Ministry of Education, Shanghai Jiao Tong University, Shanghai, 200240, China

    Yi-nan Wang  (王一男), Xu-teng Zhao  (赵旭腾), Zu-wei Zheng  (郑祖伟), Han Jiang  (蒋涵), Ting Chen  (陈婷), Yi-ran Zhang  (张毅然), He Lin  (林赫) & Reggie Zhan  (湛日景)

  2. Beijing Vehicle Emissions Management Center, Beijing, 100081, China

    Hong-lin Cao  (曹宏林)

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  1. Yi-nan Wang  (王一男)
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Contributions

WANG Yi-nan conducted the experiments and wrote the draft of manuscript. ZHAO Xu-teng revised the manuscript. ZHENG Zu-wei, CHEN Ting, JIANG Han and ZHANG Yi-ran provided the concept. CAO Hong-lin, LIN He and ZHAN Reggie provided funding.

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Correspondence to Reggie Zhan  (湛日景).

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The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Foundation item: Project(52106173) supported by the National Natural Science Foundation of China; Project(2020TQ0187) supported by the Postdoctoral Research Foundation of China

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Wang, Yn., Zhao, Xt., Zheng, Zw. et al. Pd-M-TiO2 (M=Mn, Cu, Ce and Fe) as passive NOx adsorber (PNA) at low temperature. J. Cent. South Univ. 29, 2253–2265 (2022). https://doi.org/10.1007/s11771-022-5083-9

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