Li Jing, Tang Yu, Ma Yuanyuan, Zhang Zhiyun, Tao Franklin Feng, Qu Yongquan
Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, College of Chemistry and Chemical Engineering , Liaocheng University , Liaocheng 252059 , China.
Center for Applied Chemical Research, Frontier Institute of Science and Technology and Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology , Xi'an Jiaotong University , Xi'an 710049 , China.
ACS Appl Mater Interfaces. 2018 Nov 7;10(44):38134-38140. doi: 10.1021/acsami.8b15585. Epub 2018 Oct 24.
Identification of the chemical states of catalytic sites is critical for an atomic-level understanding of catalytic mechanisms. Herein, hydrogen thermal pretreatment of the Pt single atoms on porous nanorods of CeO (Pt/ PN-CeO) induced the formation of isolated bimetallic PtCe sites as a new type of active center for CO oxidation. The evolutions of Pt/ PN-CeO catalysts during the hydrogen pretreatment and CO oxidation were examined by various in situ techniques including infrared, ambient-pressure X-ray photoelectron and X-ray absorption spectroscopy. The experimental results demonstrate that these bimetallic sites can be partially preserved or reoxidized into Pt-O-Ce with a low coordination number with oxygen under realistic conditions, leading to the appropriate CO adsorption and activating the efficient activity of Pt/ PN-CeO for CO oxidation at low temperature.
确定催化位点的化学状态对于从原子水平理解催化机制至关重要。在此,对CeO多孔纳米棒上的Pt单原子(Pt/PN-CeO)进行氢热预处理,诱导形成了孤立的双金属PtCe位点,作为CO氧化的新型活性中心。通过包括红外、常压X射线光电子能谱和X射线吸收光谱等各种原位技术研究了Pt/PN-CeO催化剂在氢预处理和CO氧化过程中的演变。实验结果表明,在实际条件下,这些双金属位点可以部分保留或重新氧化为与氧配位较低的Pt-O-Ce,从而导致适当的CO吸附并激活Pt/PN-CeO在低温下对CO氧化的高效活性。