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Transformation of Highly Stable Pt Single Sites on Defect Engineered Ceria into Robust Pt Clusters for Vehicle Emission Control
Environmental Science & Technology ( IF 11.4 ) Pub Date : 2021-09-08 , DOI: 10.1021/acs.est.1c02853
Wei Tan 1, 2 , Shaohua Xie 1 , Yandi Cai 2 , Meiyu Wang 3 , Shuohan Yu 2 , Ke-Bin Low 4 , Yuejin Li 4 , Lu Ma 5 , Steven N Ehrlich 5 , Fei Gao 2 , Lin Dong 2 , Fudong Liu 1
Affiliation  

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 H2 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 H2 treatment was systematically investigated on aged Pt/CZO and Pt/CeO2 catalysts. With H2 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.

中文翻译:

将缺陷工程氧化铈上高度稳定的 Pt 单点转变为用于车辆排放控制的稳健 Pt 簇

金属氧化物载体上的工程表面缺陷有助于促进活性位点的分散和负载催化剂的催化性能。在此,提出了一种 ZrO 2掺杂策略,以在 CeO 2 (CZO)上产生丰富的表面缺陷,并利用这些缺陷改善 Pt 分散并增强其作为单个位点对 CZO 载体 (Pt/CZO) 的亲和力。CZO 载体上的强锚定 Pt 单点最初对 CO/C 3 H 6 的催化氧化无效。然而,经过H 2还原的简单活化后,Pt/CZO 催化剂的催化氧化性能显着提高,优于Pt/CeO 2. Pt/CZO 催化剂还表现出更高的热稳定性。在老化的 Pt/CZO 和 Pt/CeO 2催化剂上系统地研究了通过 H 2处理的 Pt 活性位点的结构演变。随着 H 2还原,离子 Pt 单点转化为活性 Pt 簇。由于老化的 Pt/CZO 上更强的 Pt-CeO 2相互作用,在 CZO(1.2 nm)上产生的 Pt 簇比在 CeO 2 上1.8 nm)小得多。因此,在被更多氧缺陷和 Ce 3+包围的较小簇上获得更多暴露的活性 Pt 位点 物种,这直接转化为活化 Pt/CZO 催化剂在车辆排放控制应用中更高的催化氧化性能。
更新日期:2021-09-21
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