Advanced search
Start date
(Reference retrieved automatically from Web of Science through information on FAPESP grant and its corresponding number as mentioned in the publication by the authors.)

Hot Electrons, Hot Holes, or Both? Tandem Synthesis of Imines Driven by the Plasmonic Excitation in Au/CeO(2)Nanorods

Full text
Teixeira, Ivo F. [1] ; Homsi, Mauricio S. [2] ; Geonmonond, Rafael S. [2] ; Rocha, Guilherme F. S. R. [2] ; Peng, Yung-Kang [3] ; Silva, Ingrid F. [4] ; Quiroz, Jhon [5] ; Camargo, Pedro H. C. [2, 5]
Total Authors: 8
[1] Univ Fed Sao Carlos, Dept Chem, BR-13565905 Sao Carlos - Brazil
[2] Univ Sao Paulo, Dept Fundamental Chem, Inst Chem, BR-05508000 Sao Paulo - Brazil
[3] City Univ Hong Kong, Dept Chem, Yeung Kin Man Acad Bldg, Hong Kong - Peoples R China
[4] Univ Fed Minas Gerais, Dept Chem, ICEx, BR-31270901 Belo Horizonte, MG - Brazil
[5] Univ Helsinki, Dept Chem, AI Virtasen Aukio 1, Helsinki 00100 - Finland
Total Affiliations: 5
Document type: Journal article
Source: NANOMATERIALS; v. 10, n. 8 AUG 2020.
Web of Science Citations: 0

Solar-to-chemical conversion via photocatalysis is of paramount importance for a sustainable future. Thus, investigating the synergistic effects promoted by light in photocatalytic reactions is crucial. The tandem oxidative coupling of alcohols and amines is an attractive route to synthesize imines. Here, we unravel the performance and underlying reaction pathway in the visible-light-driven tandem oxidative coupling of benzyl alcohol and aniline employing Au/CeO(2)nanorods as catalysts. We propose an alternative reaction pathway for this transformation that leads to improved efficiencies relative to individual CeO(2)nanorods, in which the localized surface plasmon resonance (LSPR) excitation in Au nanoparticles (NPs) plays an important role. Our data suggests a synergism between the hot electrons and holes generated from the LSPR excitation in Au NPs. While the oxygen vacancies in CeO(2)nanorods trap the hot electrons and facilitate their transfer to adsorbed O(2)at surface vacancy sites, the hot holes in the Au NPs facilitate the alpha-H abstraction from the adsorbed benzyl alcohol, evolving into benzaldehyde, which then couples with aniline in the next step to yield the corresponding imine. Finally, cerium-coordinated superoxide species abstract hydrogen from the Au surface, regenerating the catalyst surface. (AU)

FAPESP's process: 17/50118-9 - Plasmonic nanoparticles supported on semiconductors and its applications in photocatalysis
Grantee:Ivo Freitas Teixeira
Support type: Regular Research Grants