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

被引:13
作者
Asaduzzaman, Abu Md [1 ]
Schreckenbach, Georg [1 ]
机构
[1] Univ Manitoba, Dept Chem, Winnipeg, MB R3T 2N2, Canada
基金
加拿大自然科学与工程研究理事会; 加拿大创新基金会;
关键词
Iodide; Dye-sensitized solar cell (DSSC); Density functional theory (DFT); Anatase; Cluster calculations; Adsorption; NANOCRYSTALLINE TIO2; ENERGY CONVERSION; ORGANIC-DYES; AB-INITIO; DENSITY; SOLVATION; DFT; APPROXIMATION; EFFICIENCY; COMPLEXES;
D O I
10.1007/s00214-011-0920-1
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
First principle density-functional theory calculations have been carried out on the interaction of I- and I-3 (-) 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 I-3 (-)) 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.
引用
收藏
页码:199 / 208
页数:10
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