期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 55, 期 18, 页码 12607-12618出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.1c02853
关键词
engineering surface defects; Pt single sites; structural evolution; activation treatment; catalytic oxidation reactions
资金
- University of Central Florida (UCF)
- Preeminent Postdoctoral Program (P3) at UCF
- National Natural Science Foundation of China [21972063]
- Natural Science Foundation of Jiangsu Province [BK20200012]
- DOE Office of Science by Brookhaven National Laboratory [DE-SC0012704]
This study explores the engineering of surface defects on CeO2 supports through ZrO2 doping to enhance the catalytic performance of Pt/CZO catalysts. Activation by H-2 reduction significantly boosts the catalytic oxidation performance of Pt/CZO catalyst and improves thermal stability, making it superior to Pt/CeO2 in vehicle emission control applications.
Engineering surface defects on metal oxide supports could help promote the dispersion of active sites and catalytic performance of supported catalysts. Herein, a strategy of ZrO2 doping was proposed to create rich surface defects on CeO2 (CZO) and, with these defects, to improve Pt dispersion and enhance its affinity as single sites to the CZO support (Pt/CZO). The strongly anchored Pt single sites on CZO support were initially not efficient for catalytic oxidation of CO/C3H6. However, after a simple activation by H-2 reduction, the catalytic oxidation performance over Pt/CZO catalyst was significantly boosted and better than Pt/CeO2. Pt/CZO catalyst also exhibited much higher thermal stability. The structural evolution of Pt active sites by H-2 treatment was systematically investigated on aged Pt/CZO and Pt/CeO2 catalysts. With H-2 reduction, ionic Pt single sites were transformed into active Pt clusters. Much smaller Pt clusters were created on CZO (ca. 1.2 nm) than on CeO2 (ca. 1.8 nm) due to stronger Pt-CeO2 interaction on aged Pt/CZO. Consequently, more exposed active Pt sites were obtained on the smaller clusters surrounded by more oxygen defects and Ce3+ species, which directly translated to the higher catalytic oxidation performance of activated Pt/CZO catalyst in vehicle emission control applications.
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