Bo Tang*, , , Xu Zuo, , , Ang Li, , , Jiajun Wang, , , Haojun Zou, , , Lili Xu, , and , Weili Dai*,
{"title":"Lewis酸性沸石包封双金属Au-Pt纳米颗粒作为甘油转化为乳酸甲酯的稳健催化剂","authors":"Bo Tang*, , , Xu Zuo, , , Ang Li, , , Jiajun Wang, , , Haojun Zou, , , Lili Xu, , and , Weili Dai*, ","doi":"10.1021/acscatal.5c03831","DOIUrl":null,"url":null,"abstract":"<p >Alkyl lactates can be produced via a glycerol oxidation-rearrangement route, which is a promising alternative to the microbial fermentation-based technology but is still hindered by the lack of an efficient catalyst. Herein, we reported the successful fabrication of well-defined bimetallic Au–Pt nanoparticles confined inside the Snβ zeolite, i.e., Au<sub><i>x</i></sub>Pt<sub><i>y</i></sub>@Snβ, using a mercaptosilane-assisted structure reconstruction strategy. Owing to the synergistic effect of bimetallic Au–Pt species and the unique Lewis acidic framework Sn, the optimized Au<sub>1</sub>Pt<sub>3</sub>@Snβ demonstrated superior catalytic performance in the conversion of glycerol to methyl lactate, achieving a 78.8% methyl lactate yield and a TOF of 335 h<sup>–1</sup> at 413 K and 0.5 MPa air, which surpasses most previously reported heterogeneous catalysts under similar reaction conditions. The confinement environment of zeolite can not only provide spatial restriction but also induce a strong interaction between encapsulated Au–Pt nanoparticles and framework Sn, thus inhibiting metal sintering and leaching during catalysis. Experimental and theoretical calculations (DFT) results explicated the critical role of bimetallic Au–Pt synergy in activating O<sub>2</sub> and facilitating a lower energy barrier for glycerol dehydrogenation, thereby promoting the catalytic performance.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"15 19","pages":"16953–16967"},"PeriodicalIF":13.1000,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Lewis Acidic Zeolite-Encapsulated Bimetallic Au–Pt Nanoparticles as Robust Catalysts for the Conversion of Glycerol to Methyl Lactate\",\"authors\":\"Bo Tang*, , , Xu Zuo, , , Ang Li, , , Jiajun Wang, , , Haojun Zou, , , Lili Xu, , and , Weili Dai*, \",\"doi\":\"10.1021/acscatal.5c03831\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Alkyl lactates can be produced via a glycerol oxidation-rearrangement route, which is a promising alternative to the microbial fermentation-based technology but is still hindered by the lack of an efficient catalyst. Herein, we reported the successful fabrication of well-defined bimetallic Au–Pt nanoparticles confined inside the Snβ zeolite, i.e., Au<sub><i>x</i></sub>Pt<sub><i>y</i></sub>@Snβ, using a mercaptosilane-assisted structure reconstruction strategy. Owing to the synergistic effect of bimetallic Au–Pt species and the unique Lewis acidic framework Sn, the optimized Au<sub>1</sub>Pt<sub>3</sub>@Snβ demonstrated superior catalytic performance in the conversion of glycerol to methyl lactate, achieving a 78.8% methyl lactate yield and a TOF of 335 h<sup>–1</sup> at 413 K and 0.5 MPa air, which surpasses most previously reported heterogeneous catalysts under similar reaction conditions. The confinement environment of zeolite can not only provide spatial restriction but also induce a strong interaction between encapsulated Au–Pt nanoparticles and framework Sn, thus inhibiting metal sintering and leaching during catalysis. Experimental and theoretical calculations (DFT) results explicated the critical role of bimetallic Au–Pt synergy in activating O<sub>2</sub> and facilitating a lower energy barrier for glycerol dehydrogenation, thereby promoting the catalytic performance.</p>\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":\"15 19\",\"pages\":\"16953–16967\"},\"PeriodicalIF\":13.1000,\"publicationDate\":\"2025-09-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acscatal.5c03831\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acscatal.5c03831","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Lewis Acidic Zeolite-Encapsulated Bimetallic Au–Pt Nanoparticles as Robust Catalysts for the Conversion of Glycerol to Methyl Lactate
Alkyl lactates can be produced via a glycerol oxidation-rearrangement route, which is a promising alternative to the microbial fermentation-based technology but is still hindered by the lack of an efficient catalyst. Herein, we reported the successful fabrication of well-defined bimetallic Au–Pt nanoparticles confined inside the Snβ zeolite, i.e., AuxPty@Snβ, using a mercaptosilane-assisted structure reconstruction strategy. Owing to the synergistic effect of bimetallic Au–Pt species and the unique Lewis acidic framework Sn, the optimized Au1Pt3@Snβ demonstrated superior catalytic performance in the conversion of glycerol to methyl lactate, achieving a 78.8% methyl lactate yield and a TOF of 335 h–1 at 413 K and 0.5 MPa air, which surpasses most previously reported heterogeneous catalysts under similar reaction conditions. The confinement environment of zeolite can not only provide spatial restriction but also induce a strong interaction between encapsulated Au–Pt nanoparticles and framework Sn, thus inhibiting metal sintering and leaching during catalysis. Experimental and theoretical calculations (DFT) results explicated the critical role of bimetallic Au–Pt synergy in activating O2 and facilitating a lower energy barrier for glycerol dehydrogenation, thereby promoting the catalytic performance.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.