{"title":"多孔金属硅酸盐材料中的封闭三金属位催化惰性芳香化合物在温和条件下的氢化反应","authors":"Zikun Liu, Chuan-De Wu","doi":"10.1016/j.apcata.2024.119901","DOIUrl":null,"url":null,"abstract":"<div><p>Complete hydrogenation of aromatic compounds is an important subject in various industry fields. However, due to the high stabilization energy of aromatic compounds resulting from their high aromaticity and non-polarity, the hydrogenation reaction is usually performed under harsh reaction conditions in the presence of noble metal-based catalysts. We report herein a porous metal silicate (PMS) material PMS-58, which consists of Cu, Ce and Co trimetal active sites, demonstrating high catalytic activity and selectivity in hydrogenating of a series of aromatic compounds under mild conditions (60 °C and 0.5 MPa H<sub>2</sub>). PMS-58 is superior to the previously reported non-noble metal-based catalysts and could be favorably compared to noble metal-based catalysts. The unique catalytic properties of PMS-58 are derived from the synergistic work of trimetal sites with Ce species serving as strong Lewis acid sites for dissociation of dihydrogen, Co species stabilizing Cu(I) species, and Cu(I) species playing a crucial role in activating aromatic rings. Therefore, this work provides a new approach in developing highly efficient non-noble metal catalysts for complete hydrogenation of arenes under mild conditions, which could be applied in removal of aromatic compounds in petroleum products.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"685 ","pages":"Article 119901"},"PeriodicalIF":4.7000,"publicationDate":"2024-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hydrogenation of inert aromatic compounds under mild conditions catalyzed by confined trimetal sites in porous metal silicate materials\",\"authors\":\"Zikun Liu, Chuan-De Wu\",\"doi\":\"10.1016/j.apcata.2024.119901\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Complete hydrogenation of aromatic compounds is an important subject in various industry fields. However, due to the high stabilization energy of aromatic compounds resulting from their high aromaticity and non-polarity, the hydrogenation reaction is usually performed under harsh reaction conditions in the presence of noble metal-based catalysts. We report herein a porous metal silicate (PMS) material PMS-58, which consists of Cu, Ce and Co trimetal active sites, demonstrating high catalytic activity and selectivity in hydrogenating of a series of aromatic compounds under mild conditions (60 °C and 0.5 MPa H<sub>2</sub>). PMS-58 is superior to the previously reported non-noble metal-based catalysts and could be favorably compared to noble metal-based catalysts. The unique catalytic properties of PMS-58 are derived from the synergistic work of trimetal sites with Ce species serving as strong Lewis acid sites for dissociation of dihydrogen, Co species stabilizing Cu(I) species, and Cu(I) species playing a crucial role in activating aromatic rings. Therefore, this work provides a new approach in developing highly efficient non-noble metal catalysts for complete hydrogenation of arenes under mild conditions, which could be applied in removal of aromatic compounds in petroleum products.</p></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":\"685 \",\"pages\":\"Article 119901\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2024-08-05\",\"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/S0926860X24003466\",\"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/S0926860X24003466","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
芳香族化合物的完全氢化是各工业领域的一个重要课题。然而,由于芳香族化合物的高芳香性和非极性导致其具有较高的稳定能,氢化反应通常需要在贵金属基催化剂存在下的苛刻反应条件下进行。我们在此报告了一种多孔金属硅酸盐(PMS)材料 PMS-58,它由 Cu、Ce 和 Co 三金属活性位点组成,在温和条件下(60 °C 和 0.5 MPa H2)氢化一系列芳香族化合物时表现出很高的催化活性和选择性。PMS-58 优于之前报道的非贵金属基催化剂,并可与贵金属基催化剂进行比较。PMS-58 的独特催化特性源于三金属位点的协同作用,其中 Ce 物种是二氢解离的强路易斯酸位点,Co 物种稳定 Cu(I) 物种,Cu(I) 物种在活化芳香环方面发挥关键作用。因此,这项工作为开发在温和条件下完全氢化茴香的高效非贵金属催化剂提供了一种新方法,这种催化剂可用于去除石油产品中的芳香族化合物。
Hydrogenation of inert aromatic compounds under mild conditions catalyzed by confined trimetal sites in porous metal silicate materials
Complete hydrogenation of aromatic compounds is an important subject in various industry fields. However, due to the high stabilization energy of aromatic compounds resulting from their high aromaticity and non-polarity, the hydrogenation reaction is usually performed under harsh reaction conditions in the presence of noble metal-based catalysts. We report herein a porous metal silicate (PMS) material PMS-58, which consists of Cu, Ce and Co trimetal active sites, demonstrating high catalytic activity and selectivity in hydrogenating of a series of aromatic compounds under mild conditions (60 °C and 0.5 MPa H2). PMS-58 is superior to the previously reported non-noble metal-based catalysts and could be favorably compared to noble metal-based catalysts. The unique catalytic properties of PMS-58 are derived from the synergistic work of trimetal sites with Ce species serving as strong Lewis acid sites for dissociation of dihydrogen, Co species stabilizing Cu(I) species, and Cu(I) species playing a crucial role in activating aromatic rings. Therefore, this work provides a new approach in developing highly efficient non-noble metal catalysts for complete hydrogenation of arenes under mild conditions, which could be applied in removal of aromatic compounds in petroleum products.
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.