4.6 Article

Kinetics analysis of the electron transfer from nano-TiO2 to O2 through on-line absorptions and theoretical modeling

Journal

JOURNAL OF APPLIED PHYSICS
Volume 129, Issue 16, Pages -

Publisher

AMER INST PHYSICS
DOI: 10.1063/5.0047822

Keywords

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Funding

  1. National Natural Science Foundation of China (NSFC) [51772230]
  2. National Key Research and Development Program of China [2017YFE0192600]
  3. 101 projects [B18038]
  4. Open Foundation of Key Laboratory for UV-Emitting Materials and Technology of Ministry of Education, Northeast Normal University [135130013]
  5. key R&D project of Hubei Province, China [2020BAB061]

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The electron relaxations during transfer from nano-TiO2 to O-2 were found to be slow and dispersive due to low transfer probability and multi-trapping transport. The amount of O-2 mainly affects electron transfer by changing p(tr), while light intensities and temperatures affect it by changing multi-trapping transport. The disagreement between simulations and later stage relaxations may be due to additional deep traps with a different distribution contributing to the electron relaxations.
On-line optical absorptions were monitored under steady light illuminations to study the electron relaxations happening through the transfer from nano-TiO2 to O-2, which are found to be slow and dispersive. A quasi-equilibrium (QE) theory and Monte Carlo simulations are developed to model the electron transfer, and they give good fittings to the early stage electron relaxations (over 70%). It is shown that the electron QE population at traps is kept during the whole electron relaxations. The slow kinetics is attributed to both the low probability (p(tr)) for an electron transferring to an O-2 from a trap and the multi-trapping transport. The dispersive feature is ascribed to the dynamic decrease in the quasi-Fermi level (E-F). The electron transfer rate constants just after the termination of light illuminations are taken out from the QE model fittings to analyze the relaxation kinetics. It is found that O-2 amounts mainly affect the electron transfer by changing p(tr); light intensities and temperatures mainly affect the electron transfer by changing the multi-trapping transport. The difference between the conduction band edge and the E-F is the thermal barrier of the electron transfer from TiO2 to O-2. The apparent activation energy (E-app) of the electron transfer, determined from the absorption decays measured at different temperatures, is smaller than the real thermal barrier because of the decrease of E-F with temperatures. The disagreement between the simulations and the later stage relaxations is not caused by the none-QE electron distribution at deep traps, and additional deep traps with a different distribution should also contribute to the electron relaxations.

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