Issue 11, 2022

Photocatalyzed electron exchange between organic chromophores and hematite nanoparticles and the role of solid-state charge transport

Abstract

Understanding photocatalyzed redox interactions between Fe(III)–(oxyhydr)oxide mineral nanoparticles and adsorbed chromophoric organic matter is critical for accurately predicting bioavailable iron fluxes in the euphotic zone of natural aquatic systems, and for improving the effectiveness of nano-iron-based water purification systems. However, the electron transfer processes that underpin photoreductive dissolution at particle/organic/solution interfaces occur on ultrafast timescales and thus remain difficult to probe. Here we report an ultrafast transient absorption spectroscopy (TAS) study of suspensions of hematite nanoplatelets (HNPs) sensitized by adsorbed rhodamine B (RhB) dye as a function of solution media and pH. The TAS results indicate a substantially longer fluorescence lifetime of RhB adsorbed on HNPs across a wide range of pH conditions, consistent with transient photoinduced electron transfer to the oxide with recombination kinetics controlled by electron migration back to the interface via small polaron hopping. Normalization of the observed kinetics to the measured surface loading of RhB at different pH values shows that the recombination rates are insensitive to environmental variables, likely controlled instead by particle properties that determine small polaron diffusion behavior.

Graphical abstract: Photocatalyzed electron exchange between organic chromophores and hematite nanoparticles and the role of solid-state charge transport

Supplementary files

Article information

Article type
Paper
Submitted
13 Jūn. 2022
Accepted
17 Sept. 2022
First published
03 Okt. 2022

Environ. Sci.: Nano, 2022,9, 4119-4135

Author version available

Photocatalyzed electron exchange between organic chromophores and hematite nanoparticles and the role of solid-state charge transport

M. D. Boamah, X. Huang, A. Joly, Z. Wang and K. M. Rosso, Environ. Sci.: Nano, 2022, 9, 4119 DOI: 10.1039/D2EN00567K

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