Poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) has shown significant achievements in organic thermoelectrics (TEs) as an alternative for inorganic counterparts. However, PEDOT:PSS films have limited practical applications because their performance is sensitive to humidity. Crosslinking additives are utilized to improve the reliability of PEDOT:PSS film through enhancing hydrophobicity; among these, polyethylene glycol (PEG) is a widely-used additive. However, ether groups in PEG induce water molecules in the film through the hydrogen bond, which deteriorates the TE reliability. Here, we enhance the TE reliability of the PEDOT:PSS film using glycerol as an additive through the crosslinking reaction between the hydroxyl group in glycerol and the sulfonic acid in PEDOT:PSS. The TE reliability (1/Power factor (PF)) of PEG solution-treated PEDOT:PSS film (PEG solution-treated film) was 57% of its initial absolute value (0 h), after 288 h (two weeks) in a humid environment (95% relative humidity, 27 °C temperature). On the other hand, the glycerol solution-treated PEDOT:PSS film (glycerol solution-treated film) exhibited superior TE reliability and preserved 75% of its initial 1/PF. Furthermore, glycerol vapor treatment enabled the film to have stronger TE humid reliability, maintaining 82% of its initial 1/PF, with the same condition. This enhancement is attributed to the increased hydrophobicity and lower oxygen content of the glycerol vapor-treated PEDOT:PSS film (glycerol vapor-treated film), which provides little change in the chemical composition of PEDOT:PSS.
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