The SMSI of Pt-TiO2 During the Crystalline Phase Transformation and Its Effect on CO Oxidation Performance

doi:10.6023/A22040162

Abstract

The strong metal-support interaction (SMSI) has long been studied in heterogonous catalysis on account of its importance in stabilizing active metals and tuning catalytic performance. So far, although there are many reports about SMSI in Pt-TiO₂ system, they are mainly focusing on support structure sensitivity (crystal plane effect) and the size of supported noble metals (size effect), it is still unclear whether the TiO₂ crystalline phase influences the creation of SMSI or not. In this study, we choose brookite TiO₂(TiO₂(B)) as support to prepare Pt-TiO₂(B) catalyst by means of traditional impregnation method. Then the as-prepared Pt_imp/TiO₂(B) was treated at different temperature under different atmosphere, specifically, 250 ℃ heat treatment under H₂ (the sample is labeled as Pt_imp/TiO₂(B)-H250), 500 ℃ heat treatment under H₂ (the sample is labeled as Pt_imp/TiO₂(B)-H500), and 400 ℃ heat treatment under O₂ followed by H₂ treatment at 500 ℃ (the sample is labeled as Pt_imp/TiO₂(B)-H500+O400). The experimental results show that the 500 ℃ heat treatment under H₂ atmosphere induces the crystalline phase transformation of TiO₂(B) into anatase, and more importantly, this transformation leads to the TiO_2-_x migration as a result of the encapsulation of Pt particles by TiO_2-_x. After further heat treatment at 400 ℃ under O₂ atmosphere, the TiO_2-_x shell coated on the Pt nanoparticle surfaces was removed, which displays a classical SMSI behavior. According to the high resolution transmission electron microscope (HRTEM) and CO diffuse reflectance infrared Fourier transform spectroscopy (CO-DRIFTS) results, we proposed that the crystalline phase transformation plays a great role in the creation of SMSI. In addition, we selected CO oxidation as a model reaction to compare the catalytic activity of Pt_imp/TiO₂(B) catalysts. The results demonstrate that the activity of the catalysts is simultaneously affected by the TiO_2-_x coating on Pt nanoparticles and the oxygen vacancy concentration within the support. More specifically, compared with TiO₂(B), anatase TiO₂ has abundant oxygen vacancies, which is of great importance to activate O₂. In the case of Pt_imp/TiO₂(B)-H500+O400 catalyst, the active sites of Pt nanoparticles are exposed due to the removal of TiO_2-_x coating, and the anatase TiO₂ has a certain amount of oxygen vacancies. Therefore, Pt_imp/TiO₂(B)-H500+O400 catalyst exhibits the best activity among all compared Pt/TiO₂(B) catalyst. Obviously, this work greatly enriches the SMSI for Pt/TiO₂ system, and provides an important reference value for the creation of SMSI, if any, when other crystalline phase transformation (or phase transformation) involved supports are suitably chosen.

Key words: strong metal-support interaction, TiO₂(B), phase change, physical coating, CO oxidation

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Yahui Jia, Chunsheng Li, Zhongzhen Xu, Wei Liu, Daowei Gao, Guozhu Chen. The SMSI of Pt-TiO₂ During the Crystalline Phase Transformation and Its Effect on CO Oxidation Performance[J]. Acta Chimica Sinica, 2022, 80(9): 1289-1298.

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Fig. & Tab. 10

Figure 1. XRD patterns of Ptimp/TiO2(B)-H250, Ptimp/TiO2(B)-H500 and Ptimp/TiO2(B)-H500+O400

Figure 2. Raman spectra (a) and H2-TPR (b) of Ptimp/TiO2(B)-H250, Ptimp/TiO2(B)-H500 and Ptimp/TiO2(B)-H500+O400

Figure 3. HRTEM images of Ptimp/TiO2(B) series catalysts and corresponding Pt nanoparticles size distribution: (a, b) H250, (c, d) H500, (e, f) H500+O400

Figure 4. CO-DRIFTS spectra (a) and enlarged 1843 cm-1 bridge adsorption peak (b) of Ptimp/TiO2(B) series catalysts

Figure 5. XRD patterns (a) and CO-DRIFTS spectra (b) of TiO2(B) -H500/Pt series catalysts

Figure 6. CO conversion as a function of temperature for Ptimp/TiO2(B) series catalysts

Figure 7. XPS-Ti 2p (a) and XPS-O1s (b) spectra of Ptimp/TiO2(B) series catalysts

Figure 8. In-situ DRIFTS of Ptimp/TiO2(B)-H250 catalyst: (a) CO adsorption at room temperature; (b) CO adsorption at 135 ℃; (c) O2 purge at room temperature; (d) O2 purge at 135 ℃

Figure 9. In-situ DRIFTS of Ptimp/TiO2(B)-H500 catalyst: (a) CO adsorption at room temperature; (b) CO adsorption at 135 ℃; (c) O2 purge at room temperature; (d) O2 purge at 135 ℃

Figure 10. In-situ DRIFTS of Ptimp/TiO2(B)-H500+O400 catalyst: (a) CO adsorption at room temperature; (b) CO adsorption at 135 ℃; (c) O2 purge at room temperature; (d) O2 purge at 135 ℃

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载体相变下Pt-TiO₂ SMSI研究及其对CO催化性能的影响

The SMSI of Pt-TiO₂ During the Crystalline Phase Transformation and Its Effect on CO Oxidation Performance

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载体相变下Pt-TiO2 SMSI研究及其对CO催化性能的影响