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Stability and Kinetics of Silica-Protected Plasmonic Photocatalysts for Gas-Phase Degradation of Total Volatile Organic Compounds

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Abstract

Stability and kinetics of plasmonic photocatalysts for gas-phase toluene degradation were assessed by monitoring total volatile organic compound (TVOC) concentration versus UV-A illumination time in a recirculating batch reactor (plate-type flow-through). Plasmonic samples were produced by either coating silver on, or layering silica-protected or unprotected silver beneath, the photocatalyst. Samples were modeled using Finite difference time domain simulations, and characterized. Experimental results show that silver-coated photocatalysts, and photocatalysts layered over unprotected silver, exhibit initially high TVOC degradation rates compared to TiO2, but suffer from relatively rapid deactivation attributed to silver oxidation. Photocatalysts layered over silica-protected (i.e., silica-coated) silver exhibited improved stability versus photocatalysts layered over unprotected (i.e., uncoated) silver, and demonstrated more than 50% increase in reaction rate constant and more than a threefold increase in apparent quantum yield over the non-plasmonic control sample (TiO2 over SiO2). The results of this study demonstrate that a silica layer can help slow down fouling of silica nanoparticles, and that silica-coated silver nanoparticles not only help speed up reaction rate overall but also appear to speed up release of adventitious carbon from the photocatalyst surface during the initial phase of a reaction.

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Abbreviations

TVOC:

Total volatile organic compounds

UV-A:

Ultraviolet-A

UV–Vis:

Ultraviolet–Visible

FT-IR:

Fourier Transform – Infrared

XPS:

X-ray photoelectron spectroscopy

FDTD:

Finite difference time domain

NPs:

Nanoparticles

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Acknowledgements

The authors thank the following staff and students at the University of South Florida (USF) for their assistance: Dr. Shuangming Li for assistance on operating the electron-beam evaporator and rapid thermal annealing oven; Dr. Jay Bieber for XPS analysis and advice regarding interpretation of XPS data; Dr. Jay Bieber, Richard “Chip” Curtis, and Stephen Fry for assistance and training on the scanning electron microscope (SEM) and electron beam (e-beam) evaporator; Richard Everly for assistance and training on the rapid thermal annealing oven; Dave Young for advice regarding FT-IR; Dr. Krishnendu Maity for training on the FT-IR; and Craig Chase of the Kurt J. Lesker Company for advice on e-beam deposition of silica.

Funding

Funding for this research was provided by the Clean Energy Research Center (CERC) at the University of South Florida (USF), and by the USF Signature Research Fellowship.

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Authors and Affiliations

  1. Clean Energy Research Center, College of Engineering, University of South Florida, 4202 E Fowler Avenue, ENB 118, Tampa, FL, 33620, USA

    Amaury P. Betancourt & D. Yogi Goswami

  2. Department of Chemical, Biological, and Materials Engineering, University of South Florida, 4202 E Fowler Avenue, ENG 030, Tampa, FL, 33620, USA

    Amaury P. Betancourt, D. Yogi Goswami, Venkat R. Bhethanabotla & John N. Kuhn

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  1. Amaury P. Betancourt
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Contributions

The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript. The following lists the contributions of each author. Amaury Betancourt: Conceptualization; Data curation; Formal analysis; Investigation; Methodology; Project Administration; Validation; Writing—original draft; Writing—review & editing. DYG: Conceptualization; Funding acquisition; Project administration; Resources; Supervision; Writing—review & editing. JNK: Formal analysis; Validation; Writing—review & editing. VRB: Conceptualization; Methodology; Resources; Validation; Visualization; Writing—review & editing.

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Betancourt, A.P., Goswami, D.Y., Bhethanabotla, V.R. et al. Stability and Kinetics of Silica-Protected Plasmonic Photocatalysts for Gas-Phase Degradation of Total Volatile Organic Compounds. Catal Lett 152, 641–658 (2022). https://doi.org/10.1007/s10562-021-03666-w

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