{"title":"在未煅烧的TS-1上浸渍光稳定金前驱体以促进丙烷的催化加氢氧化","authors":"Zhihua Zhang, Erchuan Yang, Fan Liu, Kesheng Xu, Yuxia Zhong, Jinwei Sun, Shudong Shi, Xuezhi Duan, Xinggui Zhou","doi":"10.1007/s11426-024-2403-7","DOIUrl":null,"url":null,"abstract":"<div><p>Immobilizing highly dispersed Au nanoparticles onto titanium silicalite-1 (TS-1) by a simple impregnation method under light is still a challenging task. In this work, a high photostable Au precursor protected by thiol ligands was firstly synthesized, and the as-prepared Au precursor displayed excellent stability under light for over 30 days, while the Au precursor without thiol ligands formed precipitates after just 2 h under light. Subsequently, the Au precursor protected by thiol ligands was immobilized on the external surface of uncalcined TS-1 (i.e., TS-1-B) by the incipient wetness impregnation method (IWI method) to prepare Au/TS-1-B catalyst. The activity of as-prepared Au/TS-1-B catalyst in the hydro-oxidation of propane to acetone was 1.4 times higher than that of the catalyst prepared by the deposition-precipitation urea method (DPU method). The structures of the Au/TS-1-B catalysts prepared by different methods were analyzed by multiple characterizations. Compared to the Au/TS-1-B catalyst prepared by the DPU method, the Au/TS-1-B catalyst synthesized by the IWI method exhibited a narrower size distribution of Au nanoparticles and had more small Au particles (<2 nm), which is the main reason for its superior activity. Additionally, the effects of gold loadings, reaction temperature and Si/Ti molar ratio on the catalytic performance of the Au/TS-1-B catalyst prepared by the IWI method were also investigated. In addition, the Au/TS-1-B catalyst prepared by the IWI method also exhibited excellent stability for over 140 h.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 4","pages":"1585 - 1596"},"PeriodicalIF":10.4000,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane\",\"authors\":\"Zhihua Zhang, Erchuan Yang, Fan Liu, Kesheng Xu, Yuxia Zhong, Jinwei Sun, Shudong Shi, Xuezhi Duan, Xinggui Zhou\",\"doi\":\"10.1007/s11426-024-2403-7\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Immobilizing highly dispersed Au nanoparticles onto titanium silicalite-1 (TS-1) by a simple impregnation method under light is still a challenging task. In this work, a high photostable Au precursor protected by thiol ligands was firstly synthesized, and the as-prepared Au precursor displayed excellent stability under light for over 30 days, while the Au precursor without thiol ligands formed precipitates after just 2 h under light. Subsequently, the Au precursor protected by thiol ligands was immobilized on the external surface of uncalcined TS-1 (i.e., TS-1-B) by the incipient wetness impregnation method (IWI method) to prepare Au/TS-1-B catalyst. The activity of as-prepared Au/TS-1-B catalyst in the hydro-oxidation of propane to acetone was 1.4 times higher than that of the catalyst prepared by the deposition-precipitation urea method (DPU method). The structures of the Au/TS-1-B catalysts prepared by different methods were analyzed by multiple characterizations. Compared to the Au/TS-1-B catalyst prepared by the DPU method, the Au/TS-1-B catalyst synthesized by the IWI method exhibited a narrower size distribution of Au nanoparticles and had more small Au particles (<2 nm), which is the main reason for its superior activity. Additionally, the effects of gold loadings, reaction temperature and Si/Ti molar ratio on the catalytic performance of the Au/TS-1-B catalyst prepared by the IWI method were also investigated. In addition, the Au/TS-1-B catalyst prepared by the IWI method also exhibited excellent stability for over 140 h.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":772,\"journal\":{\"name\":\"Science China Chemistry\",\"volume\":\"68 4\",\"pages\":\"1585 - 1596\"},\"PeriodicalIF\":10.4000,\"publicationDate\":\"2025-01-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science China Chemistry\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11426-024-2403-7\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science China Chemistry","FirstCategoryId":"1","ListUrlMain":"https://link.springer.com/article/10.1007/s11426-024-2403-7","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Impregnating photo-stable gold precursor onto uncalcined TS-1 to boost catalytic hydro-oxidation of propane
Immobilizing highly dispersed Au nanoparticles onto titanium silicalite-1 (TS-1) by a simple impregnation method under light is still a challenging task. In this work, a high photostable Au precursor protected by thiol ligands was firstly synthesized, and the as-prepared Au precursor displayed excellent stability under light for over 30 days, while the Au precursor without thiol ligands formed precipitates after just 2 h under light. Subsequently, the Au precursor protected by thiol ligands was immobilized on the external surface of uncalcined TS-1 (i.e., TS-1-B) by the incipient wetness impregnation method (IWI method) to prepare Au/TS-1-B catalyst. The activity of as-prepared Au/TS-1-B catalyst in the hydro-oxidation of propane to acetone was 1.4 times higher than that of the catalyst prepared by the deposition-precipitation urea method (DPU method). The structures of the Au/TS-1-B catalysts prepared by different methods were analyzed by multiple characterizations. Compared to the Au/TS-1-B catalyst prepared by the DPU method, the Au/TS-1-B catalyst synthesized by the IWI method exhibited a narrower size distribution of Au nanoparticles and had more small Au particles (<2 nm), which is the main reason for its superior activity. Additionally, the effects of gold loadings, reaction temperature and Si/Ti molar ratio on the catalytic performance of the Au/TS-1-B catalyst prepared by the IWI method were also investigated. In addition, the Au/TS-1-B catalyst prepared by the IWI method also exhibited excellent stability for over 140 h.
期刊介绍:
Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field.
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