Juan Meng, Huidong Liu, Jianing Xu, Yu-Jiao Lou, Haixin Sun, Bo Jiang, Yongzhuang Liu, Hengfei Qin, Shuo Dou, Haipeng Yu
{"title":"具有共活 S-P-C 位点的纳米碳催化剂可增强醇的无金属直接氧化作用","authors":"Juan Meng, Huidong Liu, Jianing Xu, Yu-Jiao Lou, Haixin Sun, Bo Jiang, Yongzhuang Liu, Hengfei Qin, Shuo Dou, Haipeng Yu","doi":"10.1002/sus2.221","DOIUrl":null,"url":null,"abstract":"In this study, a sulfur–phosphorus co‐doped nanocarbon (SPC) catalyst was synthesized using a straightforward one‐step colloidal carbonization method and demonstrated high performance in the metal‐free direct oxidation of alcohols to aldehydes. This metal‐free SPC catalyst showed exceptional efficiency, achieving a conversion rate of 90% for benzyl alcohol and a selectivity of 94% toward benzaldehyde within only 1 h at 130°C. Moreover, it displays exceptional cycle stability and a high turnover frequency (17.1 × 10−3 mol g−1 h−1). Theoretical analysis suggested that the catalyst's superior performance is attributed to the presence of unsaturated edge defects and S−P− moieties, which increase the density of states at the Fermi level, lower the band gap energy, and promote electron localization. Additionally, the doping introduces cooperative co‐active S−P−C sites, facilitating a synergistic multisite catalytic effect that lowers the energy barriers. These findings represent a significant advancement in the field of metal‐free direct alcohol oxidation.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"31 1","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Nanocarbon catalysts with co‐active S−P−C sites enhance metal‐free direct oxidation of alcohols\",\"authors\":\"Juan Meng, Huidong Liu, Jianing Xu, Yu-Jiao Lou, Haixin Sun, Bo Jiang, Yongzhuang Liu, Hengfei Qin, Shuo Dou, Haipeng Yu\",\"doi\":\"10.1002/sus2.221\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"In this study, a sulfur–phosphorus co‐doped nanocarbon (SPC) catalyst was synthesized using a straightforward one‐step colloidal carbonization method and demonstrated high performance in the metal‐free direct oxidation of alcohols to aldehydes. This metal‐free SPC catalyst showed exceptional efficiency, achieving a conversion rate of 90% for benzyl alcohol and a selectivity of 94% toward benzaldehyde within only 1 h at 130°C. Moreover, it displays exceptional cycle stability and a high turnover frequency (17.1 × 10−3 mol g−1 h−1). Theoretical analysis suggested that the catalyst's superior performance is attributed to the presence of unsaturated edge defects and S−P− moieties, which increase the density of states at the Fermi level, lower the band gap energy, and promote electron localization. Additionally, the doping introduces cooperative co‐active S−P−C sites, facilitating a synergistic multisite catalytic effect that lowers the energy barriers. These findings represent a significant advancement in the field of metal‐free direct alcohol oxidation.\",\"PeriodicalId\":506315,\"journal\":{\"name\":\"SusMat\",\"volume\":\"31 1\",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-07-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"SusMat\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1002/sus2.221\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"SusMat","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1002/sus2.221","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Nanocarbon catalysts with co‐active S−P−C sites enhance metal‐free direct oxidation of alcohols
In this study, a sulfur–phosphorus co‐doped nanocarbon (SPC) catalyst was synthesized using a straightforward one‐step colloidal carbonization method and demonstrated high performance in the metal‐free direct oxidation of alcohols to aldehydes. This metal‐free SPC catalyst showed exceptional efficiency, achieving a conversion rate of 90% for benzyl alcohol and a selectivity of 94% toward benzaldehyde within only 1 h at 130°C. Moreover, it displays exceptional cycle stability and a high turnover frequency (17.1 × 10−3 mol g−1 h−1). Theoretical analysis suggested that the catalyst's superior performance is attributed to the presence of unsaturated edge defects and S−P− moieties, which increase the density of states at the Fermi level, lower the band gap energy, and promote electron localization. Additionally, the doping introduces cooperative co‐active S−P−C sites, facilitating a synergistic multisite catalytic effect that lowers the energy barriers. These findings represent a significant advancement in the field of metal‐free direct alcohol oxidation.