Soumya B. Narendranath, N. P. Nimisha, S. Namitha, K. Khadheejath Shabana, N. J. Venkatesha, Chamundi P. Jijil, A. Sakthivel
{"title":"用于芳香族衍生物氢化的钌负载中酸性 SAPO-11","authors":"Soumya B. Narendranath, N. P. Nimisha, S. Namitha, K. Khadheejath Shabana, N. J. Venkatesha, Chamundi P. Jijil, A. Sakthivel","doi":"10.1007/s10934-024-01572-1","DOIUrl":null,"url":null,"abstract":"<div><p>Hydrotreating of lignin molecules by heterogeneous catalysts has been a significant area of research in recent eras. The current study describes the hydrotreatment of lignin-derived phenol, <i>m</i>-cresol, over ruthenium-incorporated SAPO-11. The developed catalyst hydrogenates <i>m</i>-cresol completely at 160 °C and 10 bar of hydrogen pressure, yielding 22% methyl cyclohexane, 22% methyl cyclohexanol, and 55% methyl cyclohexanone. Temperature-programmed reduction (TPR) studies using hydrogen as probe molecules show that metallic-ruthenium species exist on the SAPO-11. The desorption profile at 147–215 °C reveals the formation of dispersed metallic ruthenium on SAPO-11. The above observation is consistent with the in-situ formation of metallic ruthenium as an active species during the hydrotreating process at 160 °C in a hydrogen environment. The presence of ruthenium species increases the acidity of the ruthenium-incorporated SAPO-11 system, as demonstrated by the ammonia-temperature-programmed desorption profile. The increase in surface acidity and metallic ruthenium on the surface contribute to the hydrogenation of <i>m</i>-cresol via a hydrogen spillover process, as evidenced by hydrogen desorption in TPR using both fresh and reduced catalysts. The catalyst works for several cycles of <i>m</i>-cresol hydrotreating, and the system is easily regenerated, allowing it to maintain its original activity. The ruthenium incorporated SAPO-11 catalyst is a promising system as it can hydrogenate many other model systems, including guaiacol, toluene, anisole, and cumene.</p></div>","PeriodicalId":660,"journal":{"name":"Journal of Porous Materials","volume":"31 3","pages":"1077 - 1086"},"PeriodicalIF":2.5000,"publicationDate":"2024-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ruthenium loaded moderate acidic SAPO-11 for hydrogenation of aromatic derivatives\",\"authors\":\"Soumya B. Narendranath, N. P. Nimisha, S. Namitha, K. Khadheejath Shabana, N. J. Venkatesha, Chamundi P. Jijil, A. Sakthivel\",\"doi\":\"10.1007/s10934-024-01572-1\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Hydrotreating of lignin molecules by heterogeneous catalysts has been a significant area of research in recent eras. The current study describes the hydrotreatment of lignin-derived phenol, <i>m</i>-cresol, over ruthenium-incorporated SAPO-11. The developed catalyst hydrogenates <i>m</i>-cresol completely at 160 °C and 10 bar of hydrogen pressure, yielding 22% methyl cyclohexane, 22% methyl cyclohexanol, and 55% methyl cyclohexanone. Temperature-programmed reduction (TPR) studies using hydrogen as probe molecules show that metallic-ruthenium species exist on the SAPO-11. The desorption profile at 147–215 °C reveals the formation of dispersed metallic ruthenium on SAPO-11. The above observation is consistent with the in-situ formation of metallic ruthenium as an active species during the hydrotreating process at 160 °C in a hydrogen environment. The presence of ruthenium species increases the acidity of the ruthenium-incorporated SAPO-11 system, as demonstrated by the ammonia-temperature-programmed desorption profile. The increase in surface acidity and metallic ruthenium on the surface contribute to the hydrogenation of <i>m</i>-cresol via a hydrogen spillover process, as evidenced by hydrogen desorption in TPR using both fresh and reduced catalysts. The catalyst works for several cycles of <i>m</i>-cresol hydrotreating, and the system is easily regenerated, allowing it to maintain its original activity. The ruthenium incorporated SAPO-11 catalyst is a promising system as it can hydrogenate many other model systems, including guaiacol, toluene, anisole, and cumene.</p></div>\",\"PeriodicalId\":660,\"journal\":{\"name\":\"Journal of Porous Materials\",\"volume\":\"31 3\",\"pages\":\"1077 - 1086\"},\"PeriodicalIF\":2.5000,\"publicationDate\":\"2024-03-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Porous Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10934-024-01572-1\",\"RegionNum\":4,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Porous Materials","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s10934-024-01572-1","RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
摘要
摘要 利用异相催化剂对木质素分子进行加氢处理是近年来的一个重要研究领域。本研究介绍了在钌掺杂的 SAPO-11 上对木质素衍生的苯酚间甲酚进行加氢处理的情况。所开发的催化剂可在 160 °C 和 10 巴氢压条件下完全氢化间甲酚,生成 22% 的甲基环己烷、22% 的甲基环己醇和 55% 的甲基环己酮。使用氢气作为探针分子进行的温度编程还原(TPR)研究表明,SAPO-11 上存在金属钌物种。147-215 °C 时的解吸曲线显示 SAPO-11 上形成了分散的金属钌。上述观察结果与 160 °C 氢环境下加氢处理过程中金属钌作为活性物种在原位形成的情况一致。钌物种的存在增加了钌结合的 SAPO-11 系统的酸度,这一点可以通过氨-温度编程解吸曲线得到证明。表面酸度的增加和表面金属钌通过氢溢出过程促进了间甲酚的氢化,使用新鲜催化剂和还原催化剂在 TPR 中进行的氢解吸证明了这一点。该催化剂可在间甲酚加氢处理的多个循环中发挥作用,而且该系统易于再生,使其能够保持原有的活性。加入钌的 SAPO-11 催化剂是一种很有前途的系统,因为它可以加氢许多其他模型系统,包括愈创木酚、甲苯、苯甲醚和癸烯。
Ruthenium loaded moderate acidic SAPO-11 for hydrogenation of aromatic derivatives
Hydrotreating of lignin molecules by heterogeneous catalysts has been a significant area of research in recent eras. The current study describes the hydrotreatment of lignin-derived phenol, m-cresol, over ruthenium-incorporated SAPO-11. The developed catalyst hydrogenates m-cresol completely at 160 °C and 10 bar of hydrogen pressure, yielding 22% methyl cyclohexane, 22% methyl cyclohexanol, and 55% methyl cyclohexanone. Temperature-programmed reduction (TPR) studies using hydrogen as probe molecules show that metallic-ruthenium species exist on the SAPO-11. The desorption profile at 147–215 °C reveals the formation of dispersed metallic ruthenium on SAPO-11. The above observation is consistent with the in-situ formation of metallic ruthenium as an active species during the hydrotreating process at 160 °C in a hydrogen environment. The presence of ruthenium species increases the acidity of the ruthenium-incorporated SAPO-11 system, as demonstrated by the ammonia-temperature-programmed desorption profile. The increase in surface acidity and metallic ruthenium on the surface contribute to the hydrogenation of m-cresol via a hydrogen spillover process, as evidenced by hydrogen desorption in TPR using both fresh and reduced catalysts. The catalyst works for several cycles of m-cresol hydrotreating, and the system is easily regenerated, allowing it to maintain its original activity. The ruthenium incorporated SAPO-11 catalyst is a promising system as it can hydrogenate many other model systems, including guaiacol, toluene, anisole, and cumene.
期刊介绍:
The Journal of Porous Materials is an interdisciplinary and international periodical devoted to all types of porous materials. Its aim is the rapid publication
of high quality, peer-reviewed papers focused on the synthesis, processing, characterization and property evaluation of all porous materials. The objective is to
establish a unique journal that will serve as a principal means of communication for the growing interdisciplinary field of porous materials.
Porous materials include microporous materials with 50 nm pores.
Examples of microporous materials are natural and synthetic molecular sieves, cationic and anionic clays, pillared clays, tobermorites, pillared Zr and Ti
phosphates, spherosilicates, carbons, porous polymers, xerogels, etc. Mesoporous materials include synthetic molecular sieves, xerogels, aerogels, glasses, glass
ceramics, porous polymers, etc.; while macroporous materials include ceramics, glass ceramics, porous polymers, aerogels, cement, etc. The porous materials
can be crystalline, semicrystalline or noncrystalline, or combinations thereof. They can also be either organic, inorganic, or their composites. The overall
objective of the journal is the establishment of one main forum covering the basic and applied aspects of all porous materials.