{"title":"非贵金属Co@hollow碳球通过温控结构工程高效一小时苯酚转化为环己醇","authors":"Luqingshan Xiao, Shuo Ma, Chunli Li, Hao Li","doi":"10.1016/j.cep.2025.110470","DOIUrl":null,"url":null,"abstract":"<div><div>Cyclohexanol is an important intermediate in the chemical industry and the synthesis of cyclohexanol from phenol by hydrogenation is a green and efficient process. In this paper, hollow carbon sphere nanoreactors ([email protected], T: temperature) with tunable microenvironment were synthesized by adjusting the pyrolysis temperature using soft template method. The characterization analysis demonstrated that the pyrolysis temperature could adjust the defect density and pore structure of the catalyst. When combined with experimental results and mechanistic studies, hydrogen and phenol were found to diffuse through multistage orifices into the cavities of the catalysts with enhanced mass transfer efficiency, and high defect density and highly dispersed cobalt nanoparticles were found to promote the activation and reaction of hydrogen and phenol. The [email protected]–600 catalyst shows significant catalytic activity at 140 °C for 1 h with 88.9 % phenol conversion and 99.9 % cyclohexanol selectivity. The good reaction activity of [email protected]–600 can be attributed to the catalyst's high defect density (I<sub>D</sub>/I<sub>G</sub>=2.77), substantial metal dispersion (45.67 %), a specific surface area of 588 m²/g, and an average pore size of 3.53 nm. Concurrently, [email protected]–600 demonstrated remarkable universality in catalyzing the hydrogenation of a diverse array of lignin-derived monomers and dimers.</div></div>","PeriodicalId":9929,"journal":{"name":"Chemical Engineering and Processing - Process Intensification","volume":"217 ","pages":"Article 110470"},"PeriodicalIF":3.9000,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Non-noble metal Co@hollow carbon spheres for highly efficient one-hour phenol conversion to cyclohexanol via temperature-controlled structural engineering\",\"authors\":\"Luqingshan Xiao, Shuo Ma, Chunli Li, Hao Li\",\"doi\":\"10.1016/j.cep.2025.110470\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Cyclohexanol is an important intermediate in the chemical industry and the synthesis of cyclohexanol from phenol by hydrogenation is a green and efficient process. In this paper, hollow carbon sphere nanoreactors ([email protected], T: temperature) with tunable microenvironment were synthesized by adjusting the pyrolysis temperature using soft template method. The characterization analysis demonstrated that the pyrolysis temperature could adjust the defect density and pore structure of the catalyst. When combined with experimental results and mechanistic studies, hydrogen and phenol were found to diffuse through multistage orifices into the cavities of the catalysts with enhanced mass transfer efficiency, and high defect density and highly dispersed cobalt nanoparticles were found to promote the activation and reaction of hydrogen and phenol. The [email protected]–600 catalyst shows significant catalytic activity at 140 °C for 1 h with 88.9 % phenol conversion and 99.9 % cyclohexanol selectivity. The good reaction activity of [email protected]–600 can be attributed to the catalyst's high defect density (I<sub>D</sub>/I<sub>G</sub>=2.77), substantial metal dispersion (45.67 %), a specific surface area of 588 m²/g, and an average pore size of 3.53 nm. Concurrently, [email protected]–600 demonstrated remarkable universality in catalyzing the hydrogenation of a diverse array of lignin-derived monomers and dimers.</div></div>\",\"PeriodicalId\":9929,\"journal\":{\"name\":\"Chemical Engineering and Processing - Process Intensification\",\"volume\":\"217 \",\"pages\":\"Article 110470\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-07-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering and Processing - Process Intensification\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0255270125003186\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering and Processing - Process Intensification","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0255270125003186","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Non-noble metal Co@hollow carbon spheres for highly efficient one-hour phenol conversion to cyclohexanol via temperature-controlled structural engineering
Cyclohexanol is an important intermediate in the chemical industry and the synthesis of cyclohexanol from phenol by hydrogenation is a green and efficient process. In this paper, hollow carbon sphere nanoreactors ([email protected], T: temperature) with tunable microenvironment were synthesized by adjusting the pyrolysis temperature using soft template method. The characterization analysis demonstrated that the pyrolysis temperature could adjust the defect density and pore structure of the catalyst. When combined with experimental results and mechanistic studies, hydrogen and phenol were found to diffuse through multistage orifices into the cavities of the catalysts with enhanced mass transfer efficiency, and high defect density and highly dispersed cobalt nanoparticles were found to promote the activation and reaction of hydrogen and phenol. The [email protected]–600 catalyst shows significant catalytic activity at 140 °C for 1 h with 88.9 % phenol conversion and 99.9 % cyclohexanol selectivity. The good reaction activity of [email protected]–600 can be attributed to the catalyst's high defect density (ID/IG=2.77), substantial metal dispersion (45.67 %), a specific surface area of 588 m²/g, and an average pore size of 3.53 nm. Concurrently, [email protected]–600 demonstrated remarkable universality in catalyzing the hydrogenation of a diverse array of lignin-derived monomers and dimers.
期刊介绍:
Chemical Engineering and Processing: Process Intensification is intended for practicing researchers in industry and academia, working in the field of Process Engineering and related to the subject of Process Intensification.Articles published in the Journal demonstrate how novel discoveries, developments and theories in the field of Process Engineering and in particular Process Intensification may be used for analysis and design of innovative equipment and processing methods with substantially improved sustainability, efficiency and environmental performance.