{"title":"调节铂催化剂几何和电子结构以高效燃烧丙烷的新策略","authors":"Cai-Hao Wen , Lin-Ya Xu , Wen-Ru Zhao , Hua-Hui Xu , Xi Zhao , Qian Zhou , Cen Tang , Wen-Zhi Jia , Meng-Fei Luo , Jian Chen","doi":"10.1016/j.apcata.2024.119778","DOIUrl":null,"url":null,"abstract":"<div><p>The geometric and electronic structure of Pt active sites plays a crucial role in determining the catalysts performance, but precise regulation remains challenging. Herein, we propose a novel approach to modulate the nature of Pt active sites by combining photo-deposition of Pt nanoparticles with ultra-low Mo loading (0.1 wt%) modification on Pt/SiO<sub>2</sub> catalysts. The addition of ultra-low loading Mo promoter not only effectively reduces the size of Pt particles but also donates electrons to the Pt particles. Furthermore, the photo-deposited Pt particles exhibit a higher proportion of metallic Pt species, which is more stable than that metallic Pt species obtained by H<sub>2</sub> reduction, compared to those prepared using traditional wetness impregnation methods. Propane oxidation activity evaluations confirm that the photo-deposited and Mo-modified Pt/0.1Mo/SiO<sub>2</sub>-P catalyst exhibits the highest activity among all the prepared catalysts. Combined with experiments of C<sub>3</sub>H<sub>8</sub>-TPSR and in-situ DRIFT spectra of propane oxidation, it is found that the Pt/0.1Mo/SiO<sub>2</sub>-P catalyst remarkably promotes propane activation and C-H bond cleavage due to the nature change of Pt active sites, and the presence of gaseous oxygen benefits propane cleavage on active sites. Our primary results provide a promising strategy for designing superior platinum catalysts by regulating Pt active sites nature for efficient propane complete oxidation.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7000,"publicationDate":"2024-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Novel strategy to regulate the geometric and electronic structure of Pt catalyst for efficient propane combustion\",\"authors\":\"Cai-Hao Wen , Lin-Ya Xu , Wen-Ru Zhao , Hua-Hui Xu , Xi Zhao , Qian Zhou , Cen Tang , Wen-Zhi Jia , Meng-Fei Luo , Jian Chen\",\"doi\":\"10.1016/j.apcata.2024.119778\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The geometric and electronic structure of Pt active sites plays a crucial role in determining the catalysts performance, but precise regulation remains challenging. Herein, we propose a novel approach to modulate the nature of Pt active sites by combining photo-deposition of Pt nanoparticles with ultra-low Mo loading (0.1 wt%) modification on Pt/SiO<sub>2</sub> catalysts. The addition of ultra-low loading Mo promoter not only effectively reduces the size of Pt particles but also donates electrons to the Pt particles. Furthermore, the photo-deposited Pt particles exhibit a higher proportion of metallic Pt species, which is more stable than that metallic Pt species obtained by H<sub>2</sub> reduction, compared to those prepared using traditional wetness impregnation methods. Propane oxidation activity evaluations confirm that the photo-deposited and Mo-modified Pt/0.1Mo/SiO<sub>2</sub>-P catalyst exhibits the highest activity among all the prepared catalysts. Combined with experiments of C<sub>3</sub>H<sub>8</sub>-TPSR and in-situ DRIFT spectra of propane oxidation, it is found that the Pt/0.1Mo/SiO<sub>2</sub>-P catalyst remarkably promotes propane activation and C-H bond cleavage due to the nature change of Pt active sites, and the presence of gaseous oxygen benefits propane cleavage on active sites. Our primary results provide a promising strategy for designing superior platinum catalysts by regulating Pt active sites nature for efficient propane complete oxidation.</p></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2024-05-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X24002229\",\"RegionNum\":2,\"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":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X24002229","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Novel strategy to regulate the geometric and electronic structure of Pt catalyst for efficient propane combustion
The geometric and electronic structure of Pt active sites plays a crucial role in determining the catalysts performance, but precise regulation remains challenging. Herein, we propose a novel approach to modulate the nature of Pt active sites by combining photo-deposition of Pt nanoparticles with ultra-low Mo loading (0.1 wt%) modification on Pt/SiO2 catalysts. The addition of ultra-low loading Mo promoter not only effectively reduces the size of Pt particles but also donates electrons to the Pt particles. Furthermore, the photo-deposited Pt particles exhibit a higher proportion of metallic Pt species, which is more stable than that metallic Pt species obtained by H2 reduction, compared to those prepared using traditional wetness impregnation methods. Propane oxidation activity evaluations confirm that the photo-deposited and Mo-modified Pt/0.1Mo/SiO2-P catalyst exhibits the highest activity among all the prepared catalysts. Combined with experiments of C3H8-TPSR and in-situ DRIFT spectra of propane oxidation, it is found that the Pt/0.1Mo/SiO2-P catalyst remarkably promotes propane activation and C-H bond cleavage due to the nature change of Pt active sites, and the presence of gaseous oxygen benefits propane cleavage on active sites. Our primary results provide a promising strategy for designing superior platinum catalysts by regulating Pt active sites nature for efficient propane complete oxidation.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.