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Nano Research 2020, 13(6): 1668-1676 https://doi.org/10.1007/s12274-020-2790-0
Research Article | Issue | Published: 11 May 2020

Enhanced singlet oxygen generation by hybrid Mn-doped nanocomposites for selective photo-oxidation of benzylic alcohols

Show Author's Information Zhi-Jun Li1,  Shuya Li2,  Andrew Hunter Davis1,  Elan Hofman1,  Gyu Leem2,3,  Weiwei Zheng1( )
Department of Chemistry, Syracuse University, Syracuse, NY 13244, USA
Department of Chemistry, State University of New York College of Environmental Science and Forestry, Syracuse, NY 13210, USA
The Michael M. Szwarc Polymer Research Institute, Syracuse, NY 13210, USA
Keywords:
photocatalysis, singlet oxygen, energy transfer, selective oxidation, doped nanocrystals
Topics:
Cadmium sulfideCatalyst activityCatalytic oxidation CdS nanoparticlesIIMetal ionsNanocompositesOxidationPlatinumSilicaSiliconSiO2 nanoparticlesTransition metalsVI semiconductorsZinc compounds
Cite this article:
Li Z-J, Li S, Hunter Davis A, et al. Enhanced singlet oxygen generation by hybrid Mn-doped nanocomposites for selective photo-oxidation of benzylic alcohols. Nano Research, 2020, 13(6): 1668-1676. https://doi.org/10.1007/s12274-020-2790-0
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Abstract Full text Electronic supplementary material About this article

Transition-metal ions doped nanocrystals (NCs), specifically Mn-doped NCs, hold great potential in the field of photocatalysis, especially, to improve photocatalytic performance for singlet oxygen (1O2) generation. Here, we report the design of a novel Mn-doped NC-based nanocomposites, specifically, silica-coated Mn-doped CdS/ZnS NCs decorated with Pt NCs (denoted as Mn-NCs@SiO2-Pt), which enhance photocatalytic 1O2 generation. Owing to the long-lived Mn excited state (on the order of ms), the energy-transfer between Mn-NCs and molecular oxygen is facilitated with the assistance of the Pt NCs adhered to the Mn-NC@SiO2 surface. Therefore, the Mn-NCs@SiO2-Pt composites, integrate the advantages of Mn-doped NCs, a protective silica layer, and Pt NCs to exhibit excellent catalytic activity and selectivity for the selective oxidation of primary benzylic alcohols to aldehydes through an 1O2 engaged oxidation process under visible-light irradiation. This work paves the way for enhancing catalytic performance via facilitated energy transfer relaxation by utilizing the long-lived excited-state of Mn2+ dopant ions in nanocomposites.


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About this article

Enhanced singlet oxygen generation by hybrid Mn-doped nanocomposites for selective photo-oxidation of benzylic alcohols

Show Author's information Zhi-Jun Li1, Shuya Li2, Andrew Hunter Davis1, Elan Hofman1, Gyu Leem2,3, Weiwei Zheng1( )
Department of Chemistry, Syracuse University, Syracuse, NY 13244, USA
Department of Chemistry, State University of New York College of Environmental Science and Forestry, Syracuse, NY 13210, USA
The Michael M. Szwarc Polymer Research Institute, Syracuse, NY 13210, USA

Abstract

Transition-metal ions doped nanocrystals (NCs), specifically Mn-doped NCs, hold great potential in the field of photocatalysis, especially, to improve photocatalytic performance for singlet oxygen (1O2) generation. Here, we report the design of a novel Mn-doped NC-based nanocomposites, specifically, silica-coated Mn-doped CdS/ZnS NCs decorated with Pt NCs (denoted as Mn-NCs@SiO2-Pt), which enhance photocatalytic 1O2 generation. Owing to the long-lived Mn excited state (on the order of ms), the energy-transfer between Mn-NCs and molecular oxygen is facilitated with the assistance of the Pt NCs adhered to the Mn-NC@SiO2 surface. Therefore, the Mn-NCs@SiO2-Pt composites, integrate the advantages of Mn-doped NCs, a protective silica layer, and Pt NCs to exhibit excellent catalytic activity and selectivity for the selective oxidation of primary benzylic alcohols to aldehydes through an 1O2 engaged oxidation process under visible-light irradiation. This work paves the way for enhancing catalytic performance via facilitated energy transfer relaxation by utilizing the long-lived excited-state of Mn2+ dopant ions in nanocomposites.

Keywords: photocatalysis, singlet oxygen, energy transfer, selective oxidation, doped nanocrystals

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Publication history
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Acknowledgements

Publication history

Received: 13 January 2020
Revised: 19 March 2019
Accepted: 04 April 2020
Published: 11 May 2020
Issue date: June 2020

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020

Acknowledgements

W. Z. acknowledges the support from the start-up grant of Syracuse University, ACS-PRF (No. 59861-DNI5) and NSF CHE MSN (No. 05539CON04700). W. Z. appreciates the valuable discussion on the reaction mechanism with Prof. Timothy Korter.

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