Tuning the Interaction between Platinum Single Atoms and Ceria by Zirconia Doping for Efficient Catalytic Ammonia
Wei Tan1,2, Yandi Cai1, Haowei Yu1
1State Key Laboratory of Pollution Control and Resource Reuse, School of Environment, Jiangsu Key Laboratory of Vehicle Emissions Control, Center of Modern Analysis, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.
Abstract:
Aiming at the development of an efficient NH3 oxidation catalyst to eliminate the harmful NH3 slip from the stationary flue gas denitrification system and diesel exhaust aftertreatment system, a facile ZrO2 doping strategy was proposed to construct Pt1/CeZr1-O2 catalysts with a tunable Pt-CeO2 interaction strength and Pt-O-Ce coordination environment. According to the results of systematic characterizations, Pt species supported on CeZr1-O2 were mainly in the form of single atoms when x ≥ 0.7, and the strength of the Pt-CeO2 interaction and the coordination number of Pt-O-Ce bond (CNPt-O-Ce) on Pt1/CeZr1-O2 showed a volcanic change as a function of the ZrO2 doping amount. It was proposed that the balance between the reasonable concentration of oxygen defects and limited surface Zr-O species well accounted for the strongest Pt-CeO2 interaction and the highest CNPt-O-Ce on Pt/Ce0.9Zr0.1O2. It was observed that the Pt/Ce0.9Zr0.1O2 catalyst exhibited much higher NH3 oxidation activity than other Pt/CeZr1-O2 catalysts. The mechanism study revealed that the Pt1 species with the stronger Pt-CeO2 interaction and higher CNPt-O-Ce within Pt/Ce0.9Zr0.1O2 could better activate NH3 adsorbed on Lewis acid sites to react with O2 thus resulting in superior NH3 oxidation activity. This work provides a new approach for designing highly efficient Pt/CeO2 based catalysts for low-temperature NH3 oxidation.
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