{"title":"Au-Fe/TS-1双金属催化剂在丙烯气相环氧化反应中的增效作用","authors":"Longzhao Zhang, Xiangyu Huang, Weihua Ma","doi":"10.1007/s10562-025-05191-6","DOIUrl":null,"url":null,"abstract":"<div><p>The introduction of a second metal into Au/TS-1 can increase the number of active sites and control the size of metal particles to enhance catalytic activity. In this study Au-Fe bimetallic catalyst Au-Fe/TS-1 was prepared by the deposition-precipitation (DP) method, the structure and morphology of the catalyst were characterized by XRD, BET, and HRTEM. The effects of Fe source (such as Fe(NO<sub>3</sub>)<sub>3</sub>, Fe<sub>2</sub>(SO<sub>4</sub>)<sub>3</sub>, NaFeEDTA) and Fe/Au ratio on propylene epoxidation performance were systematically investigated. The facile hydrolysis of Fe<sup>3+</sup> and the absence of ligand coordination resulted in substantial coating of the TS-1 surface with Fe(OH)<sub>3</sub> which severely impaired propylene oxide (PO) selectivity and promoted the peroxidation reaction. However, using NaFeEDTA as Fe source can significantly inhibit excessive Fe deposition and the Au nanoparticles of Au-Fe/TS-1 is around 2 nm (smaller than the 3 nm in Au/TS-1). The synergistic effect of Au-Fe enhances the epoxidation activity of the catalyst, thereby increasing the rate of PO formation. Specifically, the optimal catalyst, Au-Fe<sub>0.2</sub>(E)/TS-1(using NaFeEDTA as Fe source), achieved a maximum PO formation rate of 146 g<sub>PO</sub>·h<sup>−1</sup>·kg<sub>Cat</sub><sup>−1</sup> at 200 °C (significantly higher than 96 g<sub>PO</sub>·h<sup>−1</sup>·kg<sub>Cat</sub><sup>−1</sup> of Au/TS-1), with PO selectivity exceeding 90%. These findings provide valuable insights for the rational design and development of more efficient Au-M bimetallic catalysts.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 11","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic Enhancement of Au-Fe/TS-1 Bimetallic Catalysts for Propylene Gas-Phase Epoxidation\",\"authors\":\"Longzhao Zhang, Xiangyu Huang, Weihua Ma\",\"doi\":\"10.1007/s10562-025-05191-6\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The introduction of a second metal into Au/TS-1 can increase the number of active sites and control the size of metal particles to enhance catalytic activity. In this study Au-Fe bimetallic catalyst Au-Fe/TS-1 was prepared by the deposition-precipitation (DP) method, the structure and morphology of the catalyst were characterized by XRD, BET, and HRTEM. The effects of Fe source (such as Fe(NO<sub>3</sub>)<sub>3</sub>, Fe<sub>2</sub>(SO<sub>4</sub>)<sub>3</sub>, NaFeEDTA) and Fe/Au ratio on propylene epoxidation performance were systematically investigated. The facile hydrolysis of Fe<sup>3+</sup> and the absence of ligand coordination resulted in substantial coating of the TS-1 surface with Fe(OH)<sub>3</sub> which severely impaired propylene oxide (PO) selectivity and promoted the peroxidation reaction. However, using NaFeEDTA as Fe source can significantly inhibit excessive Fe deposition and the Au nanoparticles of Au-Fe/TS-1 is around 2 nm (smaller than the 3 nm in Au/TS-1). The synergistic effect of Au-Fe enhances the epoxidation activity of the catalyst, thereby increasing the rate of PO formation. Specifically, the optimal catalyst, Au-Fe<sub>0.2</sub>(E)/TS-1(using NaFeEDTA as Fe source), achieved a maximum PO formation rate of 146 g<sub>PO</sub>·h<sup>−1</sup>·kg<sub>Cat</sub><sup>−1</sup> at 200 °C (significantly higher than 96 g<sub>PO</sub>·h<sup>−1</sup>·kg<sub>Cat</sub><sup>−1</sup> of Au/TS-1), with PO selectivity exceeding 90%. These findings provide valuable insights for the rational design and development of more efficient Au-M bimetallic catalysts.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":\"155 11\",\"pages\":\"\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2025-09-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10562-025-05191-6\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-025-05191-6","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Synergistic Enhancement of Au-Fe/TS-1 Bimetallic Catalysts for Propylene Gas-Phase Epoxidation
The introduction of a second metal into Au/TS-1 can increase the number of active sites and control the size of metal particles to enhance catalytic activity. In this study Au-Fe bimetallic catalyst Au-Fe/TS-1 was prepared by the deposition-precipitation (DP) method, the structure and morphology of the catalyst were characterized by XRD, BET, and HRTEM. The effects of Fe source (such as Fe(NO3)3, Fe2(SO4)3, NaFeEDTA) and Fe/Au ratio on propylene epoxidation performance were systematically investigated. The facile hydrolysis of Fe3+ and the absence of ligand coordination resulted in substantial coating of the TS-1 surface with Fe(OH)3 which severely impaired propylene oxide (PO) selectivity and promoted the peroxidation reaction. However, using NaFeEDTA as Fe source can significantly inhibit excessive Fe deposition and the Au nanoparticles of Au-Fe/TS-1 is around 2 nm (smaller than the 3 nm in Au/TS-1). The synergistic effect of Au-Fe enhances the epoxidation activity of the catalyst, thereby increasing the rate of PO formation. Specifically, the optimal catalyst, Au-Fe0.2(E)/TS-1(using NaFeEDTA as Fe source), achieved a maximum PO formation rate of 146 gPO·h−1·kgCat−1 at 200 °C (significantly higher than 96 gPO·h−1·kgCat−1 of Au/TS-1), with PO selectivity exceeding 90%. These findings provide valuable insights for the rational design and development of more efficient Au-M bimetallic catalysts.
期刊介绍：
Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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