Guoquan Liu, Zhifei Hao, Xueyue Mi, Nan Ma, He Zhang, Yi Li, Sihui Zhan
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引用次数: 2
摘要
在许多重要的催化反应中,寻找具有优异催化性能的独特结构仍然是一个严峻的挑战。本文报道了负载不同Pt前驱体的ceo2基催化剂在H2还原NO的性能上有显著差异的现象。负载型硝酸铂[PtCe(N)]的低温催化性能优于负载型氯铂酸[PtCe(C)]。在较宽的工作温度(125-200°C)下,通过PtCe(N)实现了80%以上的NOx转化率,并具有优异的热稳定性。采用各种表征方法对其微观结构和化学电子态进行了研究。结果表明,在CeO2中引入低价态Pt后,CeO2表面电荷发生重排,氧空位和Ce3+位的含量增加。此外,x射线光电子能谱(XPS)和拉曼光谱证实,二价Pt原子可以取代Ce原子形成Pt- o - ce3 +结构,这是高性能PtCe(N)催化剂的基本单元。Pt-O-Ce3+结构的可调催化体系为负载型金属催化剂的设计提供了一种策略,并可作为未来许多其他反应研究的模型单元。
The Strategy for Constructing the Structure: Pt-O-Ce3+ Applied in Efficient NOx Removal
Exploring a unique structure with superior catalytic performance has remained a severe challenge in many important catalytic reactions. Here, we reported a phenomenon that CeO2-based catalysts loaded with different Pt precursors showed a significant difference in the performance of the reduction of NO with H2. The supported platinum nitrate [PtCe(N)] exhibited a superior low-temperature catalytic performance than the supported chloroplatinic acid [PtCe(C)]. In a wide operating temperature (125–200°C), more than 80% NOx conversion was achieved over PtCe(N) as well as excellent thermal stability. Various characterizations were used to study the microstructure and chemical electronic states. Results showed the introduction of a low valence state of Pt species into the CeO2 resulted in the rearrangement of charges on the surface of CeO2, accompanied by increasing contents of oxygen vacancies and Ce3+ sites. Furthermore, the X-ray photoelectron spectroscopy (XPS) and Raman spectra confirmed that the divalent Pt atom could substitute Ce atom to form the Pt-O-Ce3+ structure, which was the base unit in the high-performance PtCe(N) catalyst. The tunable catalytic system of the Pt-O-Ce3+ structure provides a strategy for the design of supported metal catalysts and may as a model unit for future studies of many other reactions.