Effects of Pd doping on N2O formation over Pt/BaO/Al2O3 during NOx storage and reduction process

doi:10.1007/s11783-017-0976-9

Front. Environ. Sci. Eng.

2017, Vol. 11

Issue (6) : 11 https://doi.org/10.1007/s11783-017-0976-9

RESEARCH ARTICLE

Effects of Pd doping on N₂O formation over Pt/BaO/Al₂O₃ during NO_x storage and reduction process

Mingxin Dong¹, Jun Wang¹, Jinxin Zhu¹, Jianqiang Wang¹, Wulin Wang¹, Meiqing Shen^1,^2,³(

)

¹. Key Laboratory for Green Chemical Technology of State Education Ministry, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
². Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China
³. State Key Laboratory of Engines, Tianjin University, Tianjin 300072, China

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Abstract

• The NO_x reduction ability of Pt/BaO/Al₂O₃ can be improved by Pd doping.

• Pd-Ba interaction inhibits the NO dissociation over Pd sites.

• (Pt/BaO/Al₂O₃+Pd/Al₂O₃) exhibits superior NSR performance.

• (Pt-Pd/BaO/Al₂O₃+Al₂O₃) is proved to be an unwished Pd-modified catalyst.

• The N₂O formation mechanism over Pd-modified catalyst is provided.

N₂O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N₂O formation over Pt/BaO/Al₂O₃ catalyst. Three types of catalysts, Pt/BaO/Al₂O₃, Pt/Pd mechanical mixing catalyst (Pt/BaO/Al₂O₃+Pd/Al₂O₃) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al₂O₃) were prepared by incipient wetness impregnation method. These catalysts were first evaluated in NSR activity tests using H₂/CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H₂-TPR techniques. In addition, temperature programmed reactions of NO with H₂/CO were conducted to obtain further information about N₂O formation mechanism. Compared with Pt/BaO/Al₂O₃, (Pt/BaO/Al₂O₃+Pd/Al₂O₃) produced less N₂O and more NH₃ during NO_x storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al₂O₃+Al₂O₃). Temperature programmed reactions of NO with H₂/CO results showed that Pd/Al₂O₃ component in (Pt/BaO/Al₂O₃+Pd/Al₂O₃) played an important role in NO reduction to NH₃, and the formed NH₃ could reduce NO_x to N₂ leading to a decrease in N₂O formation. Most of N₂O formed over (Pt-Pd/BaO/Al₂O₃+Al₂O₃) was originated from Pd/BaO/Al₂O₃ component. H₂-TPR results indicated Pd-Ba interaction resulted in more difficult-to-reduce PdO_x species over Pd/BaO/Al₂O₃, which inhibits the NO dissociation and thus drives the selectivity to N₂O in NO reduction.

Keywords NO_x storage reduction Pt/BaO/Al₂O₃ Pd doping N₂O formation Optimization

Corresponding Author(s): Meiqing Shen

Issue Date: 01 August 2017

Cite this article:

Mingxin Dong,Jun Wang,Jinxin Zhu, et al. Effects of Pd doping on N₂O formation over Pt/BaO/Al₂O₃ during NO_x storage and reduction process[J]. Front. Environ. Sci. Eng., 2017, 11(6): 11.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-017-0976-9
https://academic.hep.com.cn/fese/EN/Y2017/V11/I6/11

Tab.1 Quantified results of NSR activity tests

Fig.1 Outlet gas evolutions during NSR activity tests. (a), (b) and (c): (PtBaAl+ Al), (PtBaAl+ PdAl) and (PtPdBaAl+ Al) at 250℃. (d), (e) and (f): (PtBaAl+ Al), (PtBaAl+ PdAl) and (PtPdBaAl+ Al) at 300℃. The lean phase gas was 600 ppm of NO/10% O₂/N₂ balanced; the rich phase gas was 1.3% H₂/3.9% CO/N₂ balanced; and two delay phases contained pure N₂

Tab.2 BET surface area, amount of chemisorbed CO and noble metal dispersion (NM dispersion)

Fig.2 CO-DRIFTs infrared spectra on the catalysts

Fig.3 H₂-TPR results of the catalysts

Fig.4 TPR of NO (600 ppm), H₂ (1.3%) and CO (3.9%) in N₂ at a ramp of 10℃·min^-¹ over (a) (PtBaAl+ Al), (b) (PtBaAl+ PdAl), (c) (PtPdBaAl+ Al)

Fig.5 TPR of NO (600 ppm), H₂ (1.3%) and CO (3.9%) in N₂ at a ramp of 10℃·min^-¹ over (a) PdAl, (b) PdBaAl. NO conversion, N₂O selectivity and NH₃ selectivity are shown in (c)

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