Kok Bing Tan , Yiping Liu , Youting Wang , Sajid Ali , Wendong Wang , Jingru Li , Longmei Shang , Xing Yan , Xiaodong Zhang , Guowu Zhan
{"title":"以 MOF 衍生金属氧化物为支撑的 Pt 催化剂催化硬脂酸脱氧生成烯烃","authors":"Kok Bing Tan , Yiping Liu , Youting Wang , Sajid Ali , Wendong Wang , Jingru Li , Longmei Shang , Xing Yan , Xiaodong Zhang , Guowu Zhan","doi":"10.1039/d4cy00189c","DOIUrl":null,"url":null,"abstract":"<div><p>In this study, three different metal oxides derived from metal–organic frameworks (MOFs), including CeO<sub>2</sub>, ZrO<sub>2</sub>, and Fe<sub>2</sub>O<sub>3</sub> were used as porous supports for loading Pt nanoparticles, and the supported catalysts (<em>viz.</em>, Pt/CeO<sub>2</sub>, Pt/ZrO<sub>2</sub>, and Pt/Fe<sub>2</sub>O<sub>3</sub>) were evaluated for the catalytic deoxygenation of stearic acid to produce olefins by analytical pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS). Interestingly, Pt/CeO<sub>2</sub> and Pt/Fe<sub>2</sub>O<sub>3</sub> catalysts demonstrated high selectivity for olefins or aromatics, respectively, with alkanes as minor products, while the Pt/ZrO<sub>2</sub> catalyst demonstrated the lowest deoxygenation efficiency. Among them, the Pt/CeO<sub>2</sub> catalyst demonstrated the highest deoxygenation efficiency due to its highest oxygen vacancy density and the largest specific surface area (53 m<sup>2</sup> g<sup>−1</sup>). It also demonstrated the highest selectivity for olefins (41%) due to the <em>in situ</em> partial formation of the bimetallic PtCe phase during the catalytic reaction at high temperature, which facilitates the decarbonylation pathway and leads to the formation of olefins as the main product. In addition, experimental optimizations of the reaction parameters were conducted on the designed Pt/CeO<sub>2</sub> catalyst to further enhance olefin selectivity. Importantly, the Pt/CeO<sub>2</sub> catalyst also maintained high olefin selectivity and stearic acid conversion even after six consecutive cycles. Therefore, this work has provided an alternative route to produce olefins <em>via</em> the decarbonylation of stearic acid over a supported Pt/CeO<sub>2</sub> catalyst.</p></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":4.4000,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Catalytic deoxygenation of stearic acid into olefins over Pt catalysts supported on MOF-derived metal oxides†\",\"authors\":\"Kok Bing Tan , Yiping Liu , Youting Wang , Sajid Ali , Wendong Wang , Jingru Li , Longmei Shang , Xing Yan , Xiaodong Zhang , Guowu Zhan\",\"doi\":\"10.1039/d4cy00189c\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>In this study, three different metal oxides derived from metal–organic frameworks (MOFs), including CeO<sub>2</sub>, ZrO<sub>2</sub>, and Fe<sub>2</sub>O<sub>3</sub> were used as porous supports for loading Pt nanoparticles, and the supported catalysts (<em>viz.</em>, Pt/CeO<sub>2</sub>, Pt/ZrO<sub>2</sub>, and Pt/Fe<sub>2</sub>O<sub>3</sub>) were evaluated for the catalytic deoxygenation of stearic acid to produce olefins by analytical pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS). Interestingly, Pt/CeO<sub>2</sub> and Pt/Fe<sub>2</sub>O<sub>3</sub> catalysts demonstrated high selectivity for olefins or aromatics, respectively, with alkanes as minor products, while the Pt/ZrO<sub>2</sub> catalyst demonstrated the lowest deoxygenation efficiency. Among them, the Pt/CeO<sub>2</sub> catalyst demonstrated the highest deoxygenation efficiency due to its highest oxygen vacancy density and the largest specific surface area (53 m<sup>2</sup> g<sup>−1</sup>). It also demonstrated the highest selectivity for olefins (41%) due to the <em>in situ</em> partial formation of the bimetallic PtCe phase during the catalytic reaction at high temperature, which facilitates the decarbonylation pathway and leads to the formation of olefins as the main product. In addition, experimental optimizations of the reaction parameters were conducted on the designed Pt/CeO<sub>2</sub> catalyst to further enhance olefin selectivity. Importantly, the Pt/CeO<sub>2</sub> catalyst also maintained high olefin selectivity and stearic acid conversion even after six consecutive cycles. Therefore, this work has provided an alternative route to produce olefins <em>via</em> the decarbonylation of stearic acid over a supported Pt/CeO<sub>2</sub> catalyst.</p></div>\",\"PeriodicalId\":66,\"journal\":{\"name\":\"Catalysis Science & Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.4000,\"publicationDate\":\"2024-06-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Science & Technology\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/org/science/article/pii/S2044475324002958\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Science & Technology","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S2044475324002958","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Catalytic deoxygenation of stearic acid into olefins over Pt catalysts supported on MOF-derived metal oxides†
In this study, three different metal oxides derived from metal–organic frameworks (MOFs), including CeO2, ZrO2, and Fe2O3 were used as porous supports for loading Pt nanoparticles, and the supported catalysts (viz., Pt/CeO2, Pt/ZrO2, and Pt/Fe2O3) were evaluated for the catalytic deoxygenation of stearic acid to produce olefins by analytical pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS). Interestingly, Pt/CeO2 and Pt/Fe2O3 catalysts demonstrated high selectivity for olefins or aromatics, respectively, with alkanes as minor products, while the Pt/ZrO2 catalyst demonstrated the lowest deoxygenation efficiency. Among them, the Pt/CeO2 catalyst demonstrated the highest deoxygenation efficiency due to its highest oxygen vacancy density and the largest specific surface area (53 m2 g−1). It also demonstrated the highest selectivity for olefins (41%) due to the in situ partial formation of the bimetallic PtCe phase during the catalytic reaction at high temperature, which facilitates the decarbonylation pathway and leads to the formation of olefins as the main product. In addition, experimental optimizations of the reaction parameters were conducted on the designed Pt/CeO2 catalyst to further enhance olefin selectivity. Importantly, the Pt/CeO2 catalyst also maintained high olefin selectivity and stearic acid conversion even after six consecutive cycles. Therefore, this work has provided an alternative route to produce olefins via the decarbonylation of stearic acid over a supported Pt/CeO2 catalyst.
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