Aging process of PEDOT:PSS dispersion and robust recovery of aged PEDOT:PSS as a hole transport layer for organic solar cells

• The aging process of PEDOT:PSS dispersion was investigated.
• Aqueous PEDOT:PSS dispersion undergoes phase separation.
• Nano and microscale PEDOT-rich agglomerates formed due to the aging of PEDOT:PSS dispersion.
• Isopropyl alcohol facilitated the solvation of PEDOT-rich agglomerates.

Conducting p-type polymer of poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) has been widely used for organic optoelectronics, particularly as a hole transport layer for organic solar cells. While the aged PEDOT:PSS dispersion impacts device performance, the aging of PEDOT:PSS dispersion have not been well investigated. Moreover, the recovery process of aged (two-year-old) PEDOT:PSS dispersion has not been demonstrated yet. Herein, it is found that aqueous PEDOT:PSS dispersion undergoes extensive phase separation during the aging process, resulting in both nanoscale and macroscale hydrophobic PEDOT-rich agglomerates. When the aged PEDOT:PSS thin film is integrated into P3HT:PCBM organic solar cells, the PEDOT-rich agglomerates trap the photogenerated holes at the PEDOT:PSS/P3HT interface, resulting in poor extraction efficiency in organic solar cells. To recover a hole transport functionality from aged PEDOT:PSS, three different solvents such as isopropyl alcohol (C3H7OH), ethanol (C2H5OH) and methanol (CH3OH) are investigated. Among them, it is found that isopropyl alcohol (IPA) yielded very uniform PEDOT:PSS thin film layer. This is because hydrophobic functional groups of IPA solvent facilitated the preferential solvation of phase separated hydrophobic PEDOT-rich agglomerates. However, when non-optimal concentration of IPA solvents was added into the aged PEDOT:PSS dispersion, the size of PEDOT-rich agglomerates was adversely enlarged. When organic solar cells were fabricated using more than a two-year-old PEDOT:PSS that was treated with IPA solvent, the resulting device performance of organic solar cells was fully recovered and became comparable or better than that of organic solar cells fabricated with fresh PEDOT:PSS.

Recovery of aged PEDOT:PSS illustrating the preferential solvation of PEDOT-rich (black) agglomerates with IPA solvent.Figure optionsDownload as PowerPoint slide