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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2021, Vol. 15 Issue (4) : 76    https://doi.org/10.1007/s11783-020-1369-z
RESEARCH ARTICLE
PM-support interfacial effect and oxygen mobility in Pt, Pd or Rh-loaded (Ce,Zr,La)O2 catalysts
Ting Wang, Renxian Zhou()
Institute of Catalysis, Zhejiang University, Hangzhou 310028, China
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Abstract

• Pt/CZL exhibits the optimum catalytic performance for HC and NOx elimination.

• The strong PM-Ce interaction favors the oxygen mobility and DOSC.

• Pd/CZL shows higher catalytic activity for CO conversion due to more Olatt species.

• Great oxygen mobility at high temperature broadens the dynamic operation window.

• The relationship between DOSC and catalytic performance is revealed.

The physicochemical properties of Pt-, Pd- and Rh- loaded (Ce,Zr,La)O2 (shorted for CZL) catalysts before/after aging treatment were systematically characterized by various techniques to illustrate the relationship of the dynamic oxygen storage/release capacity and redox ability with their catalytic performances for HC, NOx and CO conversions. Pt/CZL catalyst exhibits the optimum catalytic performance for HC and NOx elimination, which mainly contribute to its excellent redox ability and dynamic oxygen storage/release capacity (DOSC) at lower temperature due to the stronger PM (precious metals)-support interaction. However, the worse stability of Pt-O-Ce species and volatile Pt oxides easily result in the dramatical decline in catalytic activity after aging. Pd/CZL shows higher catalytic activity for CO conversion by reason of more Olatt species as the active oxygen for CO oxidation reaction. Rh/CZL catalyst displays the widest dynamic operation window for NOx elimination as a result of greater oxygen mobility at high temperature, and the ability to retain more Rh-O-Ce species after calcined at 1100°C effectively restrains sintering of active RhOx species, improving the thermal stability of Rh/CZL catalyst.

Keywords Precious metal-loaded (Ce,Zr,La)O2 catalysts      Oxygen mobility      Catalytic performance     
Corresponding Author(s): Renxian Zhou   
Issue Date: 17 December 2020
 Cite this article:   
Ting Wang,Renxian Zhou. PM-support interfacial effect and oxygen mobility in Pt, Pd or Rh-loaded (Ce,Zr,La)O2 catalysts[J]. Front. Environ. Sci. Eng., 2021, 15(4): 76.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1369-z
https://academic.hep.com.cn/fese/EN/Y2021/V15/I4/76
Fig.1  Light-off curves of HC, CO and NOx over the M/CZL catalysts (M= Pt, Pd and Rh): (A) HC conversion; (B) CO conversion; (C) NOx conversion.
Fig.2  Light-off curves of HC (A), CO (B) and NOx (C) over the M/CZL catalysts (M= Pt, Pd and Rh) and their stability test results (D) under the reaction condition with 10% water and CO2.
Fig.3  Time-course curves of CO/N2, NO over the fresh M/CZL catalysts (M= Pt, Pd and Rh) in HC-CO-NOx-O2 condition (A1, B1), CO-NOx-O2 condition (A2, B2) and HC-NOx-O2 condition (A3, B3).
Fig.4  CO2 response curves (A: Fresh, B: Aged) and O2 intensity curves (C: Fresh, D: Aged) over M/CZL catalyst (M= Pt, Pd and Rh).
Fig.5  CO2 formation curves (A) and production amount (B) over the M/CZL catalysts (M= Pt, Pd and Rh) during 0.1 Hz O2 pulse measurement.
Catalyst Surface composition (at. %) Ce3+ in Ce (%) Oads/Olatt
(%)
M M0 (%) M2+ (%) M3+ (%) M4+ (%)
Pt/CZL 0.14 36.4 51.4 12.1 40.2 81.3
Pd/CZL 0.14 44.1 55.9 22.4 67.4
Rh/CZL 0.17 6.10 59.8 34.1 29.6 73.9
Pt/CZL-a 0.08 65.9 17.2 16.9 19.0 89.3
Pd/CZL-a 0.10 58.9 41.1 18.8 93.1
Rh/CZL-a 0.14 12.0 50.7 37.3 22.4 117.1
Tab.1  Surface elemental composition, oxidation state of Ce, Pt, Pd and Rh measured by XPS of fresh and aged M/CZL catalysts (M=Pt, Pd and Rh)
Fig.6  HRTEM images and EDS elemental mapping images of catalysts (A: Pt/CZL, B: Pd/CZL, C: Rh/CZL).
Fig.7  In situ DRIFTs spectra over Pt/CZL (A), Pd/CZL (B) and Rh/CZL (C) under HC-CO-NOx-O2 reaction condition.
Fig.8  H2-TPR profiles of M/CZL catalysts (M= Pt, Pd and Rh): (A) fresh catalysts; (B) aged catalysts.
Fig.9  CO-TPR profiles of M/CZL catalysts (M= Pt, Pd and Rh): (A) fresh catalysts; (B) aged catalysts.
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