Shanjun Mao , Zhe Wang , Zhirong Chen , Kejun Wu , Kaichao Zhang , Qichuan Li , Huihuan Yan , Guofeng Lü , Guodong Huang , Yong Wang
{"title":"贵金属催化剂上苯酚加氢选择性的区别","authors":"Shanjun Mao , Zhe Wang , Zhirong Chen , Kejun Wu , Kaichao Zhang , Qichuan Li , Huihuan Yan , Guofeng Lü , Guodong Huang , Yong Wang","doi":"10.1016/j.nanoms.2020.11.002","DOIUrl":null,"url":null,"abstract":"<div><p>Selective hydrogenation of phenol to cyclohexanone is intriguing in chemical industry. Though a few catalysts with promising performances have been developed in recent years, the basic principle for catalyst design is still missing owing to the unclear catalytic mechanism. This work tries to unravel the mechanism of phenol hydrogenation and the reasons causing the selectivity discrepancy on noble metal catalysts under mild conditions. Results show that different reaction pathways always firstly converge to the formation of cyclohexanone under mild conditions. The selectivity discrepancy mainly depends on the activity for cyclohexanone sequential hydrogenation, in which two factors are found to be responsible, i.e. the hydrogenation energy barrier and the competitive chemisorption between phenol and cyclohexanone, if the specific co-catalyzing effect of H<sub>2</sub>O on Ru is not considered. Based on the above results, a quantitative descriptor, E<sub>b</sub>(one/pl)/E<sub>a</sub>, in which E<sub>a</sub> can be further correlated to the d band center of the noble metal catalyst, is proposed by the first time to roughly evaluate and predict the selectivity to cyclohexanone for catalyst screening.</p></div>","PeriodicalId":33573,"journal":{"name":"Nano Materials Science","volume":"5 1","pages":"Pages 91-100"},"PeriodicalIF":9.9000,"publicationDate":"2023-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.nanoms.2020.11.002","citationCount":"5","resultStr":"{\"title\":\"Towards the selectivity distinction of phenol hydrogenation on noble metal catalysts\",\"authors\":\"Shanjun Mao , Zhe Wang , Zhirong Chen , Kejun Wu , Kaichao Zhang , Qichuan Li , Huihuan Yan , Guofeng Lü , Guodong Huang , Yong Wang\",\"doi\":\"10.1016/j.nanoms.2020.11.002\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Selective hydrogenation of phenol to cyclohexanone is intriguing in chemical industry. Though a few catalysts with promising performances have been developed in recent years, the basic principle for catalyst design is still missing owing to the unclear catalytic mechanism. This work tries to unravel the mechanism of phenol hydrogenation and the reasons causing the selectivity discrepancy on noble metal catalysts under mild conditions. Results show that different reaction pathways always firstly converge to the formation of cyclohexanone under mild conditions. The selectivity discrepancy mainly depends on the activity for cyclohexanone sequential hydrogenation, in which two factors are found to be responsible, i.e. the hydrogenation energy barrier and the competitive chemisorption between phenol and cyclohexanone, if the specific co-catalyzing effect of H<sub>2</sub>O on Ru is not considered. Based on the above results, a quantitative descriptor, E<sub>b</sub>(one/pl)/E<sub>a</sub>, in which E<sub>a</sub> can be further correlated to the d band center of the noble metal catalyst, is proposed by the first time to roughly evaluate and predict the selectivity to cyclohexanone for catalyst screening.</p></div>\",\"PeriodicalId\":33573,\"journal\":{\"name\":\"Nano Materials Science\",\"volume\":\"5 1\",\"pages\":\"Pages 91-100\"},\"PeriodicalIF\":9.9000,\"publicationDate\":\"2023-03-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1016/j.nanoms.2020.11.002\",\"citationCount\":\"5\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nano Materials Science\",\"FirstCategoryId\":\"1089\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2589965120300611\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"Engineering\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nano Materials Science","FirstCategoryId":"1089","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2589965120300611","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"Engineering","Score":null,"Total":0}
Towards the selectivity distinction of phenol hydrogenation on noble metal catalysts
Selective hydrogenation of phenol to cyclohexanone is intriguing in chemical industry. Though a few catalysts with promising performances have been developed in recent years, the basic principle for catalyst design is still missing owing to the unclear catalytic mechanism. This work tries to unravel the mechanism of phenol hydrogenation and the reasons causing the selectivity discrepancy on noble metal catalysts under mild conditions. Results show that different reaction pathways always firstly converge to the formation of cyclohexanone under mild conditions. The selectivity discrepancy mainly depends on the activity for cyclohexanone sequential hydrogenation, in which two factors are found to be responsible, i.e. the hydrogenation energy barrier and the competitive chemisorption between phenol and cyclohexanone, if the specific co-catalyzing effect of H2O on Ru is not considered. Based on the above results, a quantitative descriptor, Eb(one/pl)/Ea, in which Ea can be further correlated to the d band center of the noble metal catalyst, is proposed by the first time to roughly evaluate and predict the selectivity to cyclohexanone for catalyst screening.
期刊介绍:
Nano Materials Science (NMS) is an international and interdisciplinary, open access, scholarly journal. NMS publishes peer-reviewed original articles and reviews on nanoscale material science and nanometer devices, with topics encompassing preparation and processing; high-throughput characterization; material performance evaluation and application of material characteristics such as the microstructure and properties of one-dimensional, two-dimensional, and three-dimensional nanostructured and nanofunctional materials; design, preparation, and processing techniques; and performance evaluation technology and nanometer device applications.