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Citation: HE Chenghuan, GUO Yanglong, GUO Yun, WANG Yunsong, WANG Li, ZHAN Wangcheng. Catalytic Activity of Au Nanoparticles Supported on LaMnO3 Perovskite with Different Composition and Structure[J]. Acta Physico-Chimica Sinica, ;2019, 35(4): 422-430. doi: 10.3866/PKU.WHXB201805301 shu

Catalytic Activity of Au Nanoparticles Supported on LaMnO3 Perovskite with Different Composition and Structure

  • Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, P. R. China

  • Corresponding author: ZHAN Wangcheng, zhanwc@ecust.edu.cn
  • Received Date: 25 April 2018
    Revised Date: 18 May 2018
    Accepted Date: 24 May 2018
    Available Online: 30 April 2018

    Fund Project: the National Natural Science Foundation of China 21571061The project was supported by the National Natural Science Foundation of China (21571061) and the National Key Research and Development Program of China (2016yfc0204300)the National Key Research and Development Program of China 2016yfc0204300

  • Perovskite is widely used as catalyst supports because of its flexible composition, good redox performance, and excellent thermal stability. However, the use of perovskite oxides as catalyst supports has two disadvantages: low surface area due to synthesizing the perovskite structure at high temperatures, and native perovskite surfaces preferentially have A-sites instead of catalytically active sites. On the other hand, interaction between the support and metal affects the size and valence state of noble metals. Therefore, perovskite oxides with different structures were prepared and were used to support Au catalysts, in order to obtain excellent catalytic activity and high stability. Specifically, stoichiometric LaMnO3 and nonstoichiometric LaMn1.2O3 perovskites were prepared by the ethylene glycol sol-gel method, and then the LaMnO3-AE oxide was prepared by treating LaMnO3 perovskite with dilute nitric acid. The perovskite-supported Au catalyst was prepared by the deposition precipitation method and its catalytic activity for CO oxidation was evaluated. Using X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and H2 temperature-programmed reduction (H2-TPR), it was found that LaMnO3 and LaMn1.2O3 perovskite carriers were beneficial for the dispersion of Au; however, the Au nanoparticle size significantly increased with increasing calcination temperature, indicating poor Au thermal stability. In contrast, LaMnO3 perovskite (LaMnO3-AE) etched by nitric acid is not conducive to dispersion of Au, but it is beneficial for improving the thermal stability of Au. Au was always maintained in the zero-valence state after calcination at different temperature. H2-TPR results revealed that the reducibility of the catalysts changed largely after thermal treatment at high temperatures, and was mainly influenced by the agglomeration of Au nanoparticles. Although the reducibility of the Au/LaMnO3-AE catalyst calcined at 250 ℃ is lower than that of Au/LaMn1.2O3 and Au/LaMnO3 catalysts calcined at the same temperature, the former exhibited higher reducibility when the catalyst was calcined at high temperatures (500 and 900 ℃). In the CO oxidation reaction, the catalytic activity of all the prepared catalysts decreased when the calcination temperature was increased from 250 to 500, 700, and 900 ℃. However, the catalytic activity of the Au/LaMn1.2O3 catalyst was significantly higher than those of LaMnO3- and LaMnO3-AE-supported Au catalyst, when calcination temperature was below 500 ℃, while the activity of the Au/LaMnO3-AE catalyst was significantly higher than those of the Au/LaMnO3 and Au/LaMn1.2O3 catalysts when the calcination temperature was more than 700 ℃. As shown in characterization results, after the catalyst was calcined at high temperatures (700 and 900 ℃), the Au nanoparticle size on the Au/LaMnO3-AE catalyst was lower than those on Au/LaMnO3 and Au/LaMn1.2O3 catalysts, leading to high reducibility and catalytic activity of the Au/LaMnO3-AE catalyst. The Au/LaMnO3-AE catalyst also exhibited high stability in CO oxidation. The catalytic activity of the Au/LaMnO3-AE catalyst can be maintained for 20 h at 130 ℃.
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