{"title":"二氧化硫对铂催化剂上丙烷全氧化的促进作用","authors":"","doi":"10.1016/j.seppur.2024.129759","DOIUrl":null,"url":null,"abstract":"<div><p>The effect of SO<sub>2</sub> on the total oxidation of propane over supported Pt catalysts (e.g., Pt/AlF<sub>3</sub>, Pt/γ-Al<sub>2</sub>O<sub>3</sub>, Pt/SiO<sub>2</sub>) was investigated in this work. The catalytic testing results revealed that the addition of 100 ppm SO<sub>2</sub> in the reaction feed could significantly improve the activity. The largest improvement was obtained on the Pt/AlF<sub>3</sub> catalyst, on which a 10-fold higher reaction rate (1.15 μmol g<sup>−1</sup> s<sup>−1</sup> at 220 °C) was achieved in the presence of SO<sub>2</sub> compared to that in the absence of SO<sub>2</sub> (0.12 μmol g<sup>−1</sup> s<sup>−1</sup> at 220 °C). Detailed characterizations such as Fourier transform infrared spectroscopy (FTIR), NH<sub>3</sub> temperature-programmed desorption, and X-ray photoelectron spectra results revealed that the presence of SO<sub>2</sub> in the reaction feed resulted in the formation of sulfates on the catalyst surface, which enhanced the surface acidity and lowered surface charge density of Pt species. The in-situ FTIR results of propane oxidation revealed an enhanced C–C bond cleavage of propane molecules by the addition of SO<sub>2</sub>. The kinetic investigation further clarified the origin of such enhancement, that is, the addition of SO<sub>2</sub> slightly strengthened propane adsorption while greatly weakened the oxygen adsorption on the Pt species, and such synergy facilitated the kinetically-relevant surface reaction (i.e., C–C cleavage). Therefore, the findings establish a general agreement on the promoting roles of SO<sub>2</sub> on the reaction. Moreover, the current work emphasizes the influence of surface sulfate on the adsorption/activation of oxygen, which has been rarely recognized in previous works.</p></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Towards the promoting roles of SO2 in total oxidation of propane over Pt catalysts\",\"authors\":\"\",\"doi\":\"10.1016/j.seppur.2024.129759\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The effect of SO<sub>2</sub> on the total oxidation of propane over supported Pt catalysts (e.g., Pt/AlF<sub>3</sub>, Pt/γ-Al<sub>2</sub>O<sub>3</sub>, Pt/SiO<sub>2</sub>) was investigated in this work. The catalytic testing results revealed that the addition of 100 ppm SO<sub>2</sub> in the reaction feed could significantly improve the activity. The largest improvement was obtained on the Pt/AlF<sub>3</sub> catalyst, on which a 10-fold higher reaction rate (1.15 μmol g<sup>−1</sup> s<sup>−1</sup> at 220 °C) was achieved in the presence of SO<sub>2</sub> compared to that in the absence of SO<sub>2</sub> (0.12 μmol g<sup>−1</sup> s<sup>−1</sup> at 220 °C). Detailed characterizations such as Fourier transform infrared spectroscopy (FTIR), NH<sub>3</sub> temperature-programmed desorption, and X-ray photoelectron spectra results revealed that the presence of SO<sub>2</sub> in the reaction feed resulted in the formation of sulfates on the catalyst surface, which enhanced the surface acidity and lowered surface charge density of Pt species. The in-situ FTIR results of propane oxidation revealed an enhanced C–C bond cleavage of propane molecules by the addition of SO<sub>2</sub>. The kinetic investigation further clarified the origin of such enhancement, that is, the addition of SO<sub>2</sub> slightly strengthened propane adsorption while greatly weakened the oxygen adsorption on the Pt species, and such synergy facilitated the kinetically-relevant surface reaction (i.e., C–C cleavage). Therefore, the findings establish a general agreement on the promoting roles of SO<sub>2</sub> on the reaction. Moreover, the current work emphasizes the influence of surface sulfate on the adsorption/activation of oxygen, which has been rarely recognized in previous works.</p></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-09-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586624034981\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624034981","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Towards the promoting roles of SO2 in total oxidation of propane over Pt catalysts
The effect of SO2 on the total oxidation of propane over supported Pt catalysts (e.g., Pt/AlF3, Pt/γ-Al2O3, Pt/SiO2) was investigated in this work. The catalytic testing results revealed that the addition of 100 ppm SO2 in the reaction feed could significantly improve the activity. The largest improvement was obtained on the Pt/AlF3 catalyst, on which a 10-fold higher reaction rate (1.15 μmol g−1 s−1 at 220 °C) was achieved in the presence of SO2 compared to that in the absence of SO2 (0.12 μmol g−1 s−1 at 220 °C). Detailed characterizations such as Fourier transform infrared spectroscopy (FTIR), NH3 temperature-programmed desorption, and X-ray photoelectron spectra results revealed that the presence of SO2 in the reaction feed resulted in the formation of sulfates on the catalyst surface, which enhanced the surface acidity and lowered surface charge density of Pt species. The in-situ FTIR results of propane oxidation revealed an enhanced C–C bond cleavage of propane molecules by the addition of SO2. The kinetic investigation further clarified the origin of such enhancement, that is, the addition of SO2 slightly strengthened propane adsorption while greatly weakened the oxygen adsorption on the Pt species, and such synergy facilitated the kinetically-relevant surface reaction (i.e., C–C cleavage). Therefore, the findings establish a general agreement on the promoting roles of SO2 on the reaction. Moreover, the current work emphasizes the influence of surface sulfate on the adsorption/activation of oxygen, which has been rarely recognized in previous works.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.