Computational studies of the interactions of I- and I3- with TiO2 clusters: Implications for dye-sensitized solar cells

Abu Asaduzzaman, Georg Schreckenbach

Research output: Contribution to journalArticle

10 Citations (Scopus)

Abstract

First principle density-functional theory calculations have been carried out on the interaction of I- and I3- with TiO2 anatase surfaces, modeled by finite clusters that range in size from 48 to 180 atoms. The total energy per TiO2 unit and the HOMO-LUMO gaps decrease with increasing the size of the clusters. Both redox species (I- and I3-) are strongly adsorbed on the TiO2 surface with the adsorbtion of I- being stronger. Adsorption of triiodide leads to its dissociation. The positions of the HOMO and LUMO of the adsorbed systems shift negatively from their respective cluster values. Solvation effects have been modeled using the CPCM model. Introducing solvent reduces the shifting of HOMO and LUMO. Implications for dye-sensitized solar cells (DSSC) are discussed. Both the HOMO-LUMO shifting and the strong adsorption might affect the performance of the cell. Graphical Abstract: I3- dissociates upon adsorption but I- adsorbs strongly[Figure not available: see fulltext.]

Original languageEnglish (US)
Pages (from-to)199-208
Number of pages10
JournalTheoretical Chemistry Accounts
Volume129
Issue number2
DOIs
StatePublished - May 1 2011

Fingerprint

solar cells
dyes
Adsorption
adsorption
Solvation
interactions
anatase
Density functional theory
solvation
dissociation
density functional theory
Atoms
shift
cells
atoms
Dye-sensitized solar cells
energy
titanium dioxide
Oxidation-Reduction

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry

Cite this

@article{ec1d673e97074768947da85cd056e666,
title = "Computational studies of the interactions of I- and I3- with TiO2 clusters: Implications for dye-sensitized solar cells",
abstract = "First principle density-functional theory calculations have been carried out on the interaction of I- and I3- with TiO2 anatase surfaces, modeled by finite clusters that range in size from 48 to 180 atoms. The total energy per TiO2 unit and the HOMO-LUMO gaps decrease with increasing the size of the clusters. Both redox species (I- and I3-) are strongly adsorbed on the TiO2 surface with the adsorbtion of I- being stronger. Adsorption of triiodide leads to its dissociation. The positions of the HOMO and LUMO of the adsorbed systems shift negatively from their respective cluster values. Solvation effects have been modeled using the CPCM model. Introducing solvent reduces the shifting of HOMO and LUMO. Implications for dye-sensitized solar cells (DSSC) are discussed. Both the HOMO-LUMO shifting and the strong adsorption might affect the performance of the cell. Graphical Abstract: I3- dissociates upon adsorption but I- adsorbs strongly[Figure not available: see fulltext.]",
author = "Abu Asaduzzaman and Georg Schreckenbach",
year = "2011",
month = "5",
day = "1",
doi = "10.1007/s00214-011-0920-1",
language = "English (US)",
volume = "129",
pages = "199--208",
journal = "Theoretical Chemistry Accounts",
issn = "1432-881X",
publisher = "Springer New York",
number = "2",

}

Computational studies of the interactions of I- and I3- with TiO2 clusters : Implications for dye-sensitized solar cells. / Asaduzzaman, Abu; Schreckenbach, Georg.

In: Theoretical Chemistry Accounts, Vol. 129, No. 2, 01.05.2011, p. 199-208.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Computational studies of the interactions of I- and I3- with TiO2 clusters

T2 - Implications for dye-sensitized solar cells

AU - Asaduzzaman, Abu

AU - Schreckenbach, Georg

PY - 2011/5/1

Y1 - 2011/5/1

N2 - First principle density-functional theory calculations have been carried out on the interaction of I- and I3- with TiO2 anatase surfaces, modeled by finite clusters that range in size from 48 to 180 atoms. The total energy per TiO2 unit and the HOMO-LUMO gaps decrease with increasing the size of the clusters. Both redox species (I- and I3-) are strongly adsorbed on the TiO2 surface with the adsorbtion of I- being stronger. Adsorption of triiodide leads to its dissociation. The positions of the HOMO and LUMO of the adsorbed systems shift negatively from their respective cluster values. Solvation effects have been modeled using the CPCM model. Introducing solvent reduces the shifting of HOMO and LUMO. Implications for dye-sensitized solar cells (DSSC) are discussed. Both the HOMO-LUMO shifting and the strong adsorption might affect the performance of the cell. Graphical Abstract: I3- dissociates upon adsorption but I- adsorbs strongly[Figure not available: see fulltext.]

AB - First principle density-functional theory calculations have been carried out on the interaction of I- and I3- with TiO2 anatase surfaces, modeled by finite clusters that range in size from 48 to 180 atoms. The total energy per TiO2 unit and the HOMO-LUMO gaps decrease with increasing the size of the clusters. Both redox species (I- and I3-) are strongly adsorbed on the TiO2 surface with the adsorbtion of I- being stronger. Adsorption of triiodide leads to its dissociation. The positions of the HOMO and LUMO of the adsorbed systems shift negatively from their respective cluster values. Solvation effects have been modeled using the CPCM model. Introducing solvent reduces the shifting of HOMO and LUMO. Implications for dye-sensitized solar cells (DSSC) are discussed. Both the HOMO-LUMO shifting and the strong adsorption might affect the performance of the cell. Graphical Abstract: I3- dissociates upon adsorption but I- adsorbs strongly[Figure not available: see fulltext.]

UR - http://www.scopus.com/inward/record.url?scp=79955471378&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=79955471378&partnerID=8YFLogxK

U2 - 10.1007/s00214-011-0920-1

DO - 10.1007/s00214-011-0920-1

M3 - Article

AN - SCOPUS:79955471378

VL - 129

SP - 199

EP - 208

JO - Theoretical Chemistry Accounts

JF - Theoretical Chemistry Accounts

SN - 1432-881X

IS - 2

ER -