Qingxia Zhang, Dong Peng, Zhong-An Su, Ao Li, Chao Sun, Luhui Wang, Sha Cui, Shuqing Yang, Xianmin Zheng, Liuye Mo, Nannan Zhang, Fengyun Gu and Yali Liu*,
{"title":"通过引入氧空位在介孔 LaCoO3 上选择性氧化对-百里酚","authors":"Qingxia Zhang, Dong Peng, Zhong-An Su, Ao Li, Chao Sun, Luhui Wang, Sha Cui, Shuqing Yang, Xianmin Zheng, Liuye Mo, Nannan Zhang, Fengyun Gu and Yali Liu*, ","doi":"10.1021/acs.inorgchem.4c0352110.1021/acs.inorgchem.4c03521","DOIUrl":null,"url":null,"abstract":"<p >The liquid-phase catalytic oxidation of <i>p</i>-cymene to 4-methylacetophenone is an industrially significant reaction. However, the targeted oxidation of a specific C–H bond of <i>p</i>-cymene is extremely difficult due to there being many branched chains in <i>p</i>-cymene. In here, we designed a simple method to synthesize mesoporous LaCoO<sub>3</sub> catalysts with rich oxygen vacancy (O<sub>ov</sub>) sites. The as-prepared mesoporous LaCoO<sub>3</sub> after 550 °C calcination (mLaCoO<sub>3</sub>) exhibits remarkable catalytic activity for solvent-free oxidation of the <i>p</i>-cymene reaction, with a selectivity of over 80.1% selectivity for 4-methylacetophenone and a conversion of 50.2% for <i>p</i>-cymene (120 °C, 3 MPa). Besides, recycling studies have demonstrated that the mLaCoO<sub>3</sub> catalysts can be reused ten times in the aerobic oxidation of the <i>p</i>-cymene reaction without significant catalytic activity reduce. The experimental and characterization results indicated that the mesoporous structure of the catalyst is conducive to the generation of surface O<sub>ov</sub>, which can properly facilitate ion spread during the catalytic process and afford enough O<sub>2</sub> for intermediate species, thus is beneficial for the generation of 4-methylacetophenone. This work demonstrates that the selectivity oxide <i>p</i>-cymene with an O<sub>2</sub> employing mLaCoO<sub>3</sub> catalyst is highly promising for chemical industrial applications.</p>","PeriodicalId":40,"journal":{"name":"Inorganic Chemistry","volume":"63 45","pages":"21499–21506 21499–21506"},"PeriodicalIF":4.7000,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective Oxidation of p-Cymene over Mesoporous LaCoO3 by Introducing Oxygen Vacancies\",\"authors\":\"Qingxia Zhang, Dong Peng, Zhong-An Su, Ao Li, Chao Sun, Luhui Wang, Sha Cui, Shuqing Yang, Xianmin Zheng, Liuye Mo, Nannan Zhang, Fengyun Gu and Yali Liu*, \",\"doi\":\"10.1021/acs.inorgchem.4c0352110.1021/acs.inorgchem.4c03521\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The liquid-phase catalytic oxidation of <i>p</i>-cymene to 4-methylacetophenone is an industrially significant reaction. However, the targeted oxidation of a specific C–H bond of <i>p</i>-cymene is extremely difficult due to there being many branched chains in <i>p</i>-cymene. In here, we designed a simple method to synthesize mesoporous LaCoO<sub>3</sub> catalysts with rich oxygen vacancy (O<sub>ov</sub>) sites. The as-prepared mesoporous LaCoO<sub>3</sub> after 550 °C calcination (mLaCoO<sub>3</sub>) exhibits remarkable catalytic activity for solvent-free oxidation of the <i>p</i>-cymene reaction, with a selectivity of over 80.1% selectivity for 4-methylacetophenone and a conversion of 50.2% for <i>p</i>-cymene (120 °C, 3 MPa). Besides, recycling studies have demonstrated that the mLaCoO<sub>3</sub> catalysts can be reused ten times in the aerobic oxidation of the <i>p</i>-cymene reaction without significant catalytic activity reduce. The experimental and characterization results indicated that the mesoporous structure of the catalyst is conducive to the generation of surface O<sub>ov</sub>, which can properly facilitate ion spread during the catalytic process and afford enough O<sub>2</sub> for intermediate species, thus is beneficial for the generation of 4-methylacetophenone. This work demonstrates that the selectivity oxide <i>p</i>-cymene with an O<sub>2</sub> employing mLaCoO<sub>3</sub> catalyst is highly promising for chemical industrial applications.</p>\",\"PeriodicalId\":40,\"journal\":{\"name\":\"Inorganic Chemistry\",\"volume\":\"63 45\",\"pages\":\"21499–21506 21499–21506\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2024-10-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Inorganic Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.inorgchem.4c03521\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganic Chemistry","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.inorgchem.4c03521","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
Selective Oxidation of p-Cymene over Mesoporous LaCoO3 by Introducing Oxygen Vacancies
The liquid-phase catalytic oxidation of p-cymene to 4-methylacetophenone is an industrially significant reaction. However, the targeted oxidation of a specific C–H bond of p-cymene is extremely difficult due to there being many branched chains in p-cymene. In here, we designed a simple method to synthesize mesoporous LaCoO3 catalysts with rich oxygen vacancy (Oov) sites. The as-prepared mesoporous LaCoO3 after 550 °C calcination (mLaCoO3) exhibits remarkable catalytic activity for solvent-free oxidation of the p-cymene reaction, with a selectivity of over 80.1% selectivity for 4-methylacetophenone and a conversion of 50.2% for p-cymene (120 °C, 3 MPa). Besides, recycling studies have demonstrated that the mLaCoO3 catalysts can be reused ten times in the aerobic oxidation of the p-cymene reaction without significant catalytic activity reduce. The experimental and characterization results indicated that the mesoporous structure of the catalyst is conducive to the generation of surface Oov, which can properly facilitate ion spread during the catalytic process and afford enough O2 for intermediate species, thus is beneficial for the generation of 4-methylacetophenone. This work demonstrates that the selectivity oxide p-cymene with an O2 employing mLaCoO3 catalyst is highly promising for chemical industrial applications.
期刊介绍:
Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.