M.A. Rodriguez-Olguin , D. Cazac , F. Ruiz-Zepeda , S. Bartling , M. Bosco , H. Atia , R. Eckelt , A. Manzo-Robledo , M. Vandichel , A. Aguirre , J.G.E. Gardeniers , A. Susarrey-Arce
{"title":"用Pd原子和纳米晶体修饰的非均相纳米纤维结构改进低温CO氧化","authors":"M.A. Rodriguez-Olguin , D. Cazac , F. Ruiz-Zepeda , S. Bartling , M. Bosco , H. Atia , R. Eckelt , A. Manzo-Robledo , M. Vandichel , A. Aguirre , J.G.E. Gardeniers , A. Susarrey-Arce","doi":"10.1016/j.mtcata.2025.100093","DOIUrl":null,"url":null,"abstract":"<div><div>Amorphous alumina shaped as nanofibers forming a non-woven network, functioning as a heterogeneous dispersion for palladium (Pd) atoms and nanocrystals, is unique yet unstudied for low-temperature CO oxidation. This work demonstrates that nanometric-size alumina fibers (ANFs) with a surface area of ⁓230 m<sup>2</sup>/g can host Pd species that remain nearly intact after CO oxidation. The ANFs contain various Pd (Pd-ANFs) loadings, ranging from 1 %wt. (Pd1-ANFs), 3 %wt. (Pd3-ANFs), to 5 %wt. (Pd5-ANFs). Among them, Pd3-ANFs show the highest CO chemisorption. Hence, the chemical environment of the Pd3-ANFs is assessed using NAP-XPS under various CO and O<sub>2</sub> mixtures. NAP-XPS shows the presence of metallic and oxidized Pd species. The results are correlated with DRIFT spectroscopy, which unveils the CO species adsorbed over Pd. Furthermore, a computational-based kinetic model for CO oxidation shows that Pd single atoms start the CO-oxidation, followed by larger Pd crystals during light-off. Our results demonstrate that the Pd-ANFs have higher activity when compared with the Pd alumina nanoparticles (Pd-ANP) counterpart that lacks a fibrous structure, highlighting the benefits of the ANF's structural network in stabilizing atomic and nanometric scale metal catalysts for low-temperature CO oxidation.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"9 ","pages":"Article 100093"},"PeriodicalIF":0.0000,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Improved low-temperature CO oxidation using heterogeneous nanofibrous structures decorated with Pd atoms and nanocrystals\",\"authors\":\"M.A. Rodriguez-Olguin , D. Cazac , F. Ruiz-Zepeda , S. Bartling , M. Bosco , H. Atia , R. Eckelt , A. Manzo-Robledo , M. Vandichel , A. Aguirre , J.G.E. Gardeniers , A. Susarrey-Arce\",\"doi\":\"10.1016/j.mtcata.2025.100093\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Amorphous alumina shaped as nanofibers forming a non-woven network, functioning as a heterogeneous dispersion for palladium (Pd) atoms and nanocrystals, is unique yet unstudied for low-temperature CO oxidation. This work demonstrates that nanometric-size alumina fibers (ANFs) with a surface area of ⁓230 m<sup>2</sup>/g can host Pd species that remain nearly intact after CO oxidation. The ANFs contain various Pd (Pd-ANFs) loadings, ranging from 1 %wt. (Pd1-ANFs), 3 %wt. (Pd3-ANFs), to 5 %wt. (Pd5-ANFs). Among them, Pd3-ANFs show the highest CO chemisorption. Hence, the chemical environment of the Pd3-ANFs is assessed using NAP-XPS under various CO and O<sub>2</sub> mixtures. NAP-XPS shows the presence of metallic and oxidized Pd species. The results are correlated with DRIFT spectroscopy, which unveils the CO species adsorbed over Pd. Furthermore, a computational-based kinetic model for CO oxidation shows that Pd single atoms start the CO-oxidation, followed by larger Pd crystals during light-off. Our results demonstrate that the Pd-ANFs have higher activity when compared with the Pd alumina nanoparticles (Pd-ANP) counterpart that lacks a fibrous structure, highlighting the benefits of the ANF's structural network in stabilizing atomic and nanometric scale metal catalysts for low-temperature CO oxidation.</div></div>\",\"PeriodicalId\":100892,\"journal\":{\"name\":\"Materials Today Catalysis\",\"volume\":\"9 \",\"pages\":\"Article 100093\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2025-03-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Materials Today Catalysis\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2949754X25000067\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Today Catalysis","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2949754X25000067","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Improved low-temperature CO oxidation using heterogeneous nanofibrous structures decorated with Pd atoms and nanocrystals
Amorphous alumina shaped as nanofibers forming a non-woven network, functioning as a heterogeneous dispersion for palladium (Pd) atoms and nanocrystals, is unique yet unstudied for low-temperature CO oxidation. This work demonstrates that nanometric-size alumina fibers (ANFs) with a surface area of ⁓230 m2/g can host Pd species that remain nearly intact after CO oxidation. The ANFs contain various Pd (Pd-ANFs) loadings, ranging from 1 %wt. (Pd1-ANFs), 3 %wt. (Pd3-ANFs), to 5 %wt. (Pd5-ANFs). Among them, Pd3-ANFs show the highest CO chemisorption. Hence, the chemical environment of the Pd3-ANFs is assessed using NAP-XPS under various CO and O2 mixtures. NAP-XPS shows the presence of metallic and oxidized Pd species. The results are correlated with DRIFT spectroscopy, which unveils the CO species adsorbed over Pd. Furthermore, a computational-based kinetic model for CO oxidation shows that Pd single atoms start the CO-oxidation, followed by larger Pd crystals during light-off. Our results demonstrate that the Pd-ANFs have higher activity when compared with the Pd alumina nanoparticles (Pd-ANP) counterpart that lacks a fibrous structure, highlighting the benefits of the ANF's structural network in stabilizing atomic and nanometric scale metal catalysts for low-temperature CO oxidation.