Tuning the Thermoelectric Properties of a Conducting Polymer through Blending with Open-Shell Molecular Dopants

Tomlinson, Edward P.; Willmore, Matthew; Zhu, Xiaoqin; Hilsmier, Stuart W; Boudouris, Bryan W.

doi:10.1021/acsami.5b05860

Cited by 31 publications

(20 citation statements)

References 30 publications

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“…The first was the de-doping process through tuning the charge carrier concentration along the polymer chains. Bubnova et al reported the use of tetrakis(dimethylamino)ethylene to tune the electron distribution along PEDOT: p -toluenesulfonate (PEDOT:Tos) to enhance electrical conductivity significantly (Bubnova et al, 2011; Tomlinson et al, 2015). The second approach is the secondary doping with organic solvents or counter-ions so as to tune the polymer chain conformation.…”

Section: Resultsmentioning

confidence: 99%

Improved Alignment of PEDOT:PSS Induced by in-situ Crystallization of “Green” Dimethylsulfone Molecules to Enhance the Polymer Thermoelectric Performance

et al. 2019

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Dimethylsulfone (DMSO2), a small organic molecule, was observed to induce the alignment of poly(3,4-ethylenedioxythiophene): poly(4-styrenesulfonate) (PEDOT:PSS) via in-situ crystallization in PEDOT:PSS mixture, which was verified by field emission scanning electron microscopy (FESEM), X-ray diffraction (XRD) and atomic force microscopy (AFM). A chemically stable dopant, DMSO2, remarkably raised the electrical conductivity of the PEDOT:PSS film, which was fabricated from pre-mixed solution of PEDOT:PSS and DMSO2, up to 1080 S/cm, and more importantly, such a PEDOT:PSS film showed a long-term humidity stability and it retained near 90% electric conductivity after 60 days, suggesting DMSO2 is promising for an eco-friendly alternative to replace dimethyl sulfoxide (DMSO), ethylene glycol (EG) and various acids dopants that have been widely employed to dope and post-treat PEDOT:PSS. Pairwise interaction energies and free energy of solvation between PEDOT:PSS and DMSO2 were calculated by first-principles and molecular mechanics, respectively, revealing the mechanism of DMSO2 in enhancing the electrical conductivity.

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Section: Resultsmentioning

confidence: 99%

Improved Alignment of PEDOT:PSS Induced by in-situ Crystallization of “Green” Dimethylsulfone Molecules to Enhance the Polymer Thermoelectric Performance

et al. 2019

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“…DMSO with NaOH dedoping ~15.8 ~785 ~19.6 [120] Post DMSO + Hydrazin dedoping 49.3 1310 318.4 [115] Sorbitol + TDAE dedoping 27.47 ~295 ~22.3 [111] HI + DMSO (post treatment) ~30.8 ~475 ~45.1 [114] DMSO and Sorbitol 11.98 1063 15.3 [121] H2SO4 + NaOH 39.2 2170 333.5 [91] Multi-layered DMSO 10.6 187 2.1 [122] Salt + DMF 28 1831 143.6 [108] H2SO4 149.47 65.82 147.1 [123] DMSO and EMIMBF4 post treatment ~23.5 ~680 ~37.6 [124] TEMPO-OH ~22.5 ~33 ~1.7 [125] Depicted in Figure 10 is a collection of thermopower-conductivity data from literature obtained for PEDOT:PSS subjected to different treatments; for completeness also data for the PEDOT:Tos system are plotted. As noticed before, the majority of the data does not follow the empirical -¼ power-law relationship between conductivity and thermopower observed for most doped thiophenes and other doped polymers.…”

Section: Pedot:pssmentioning

confidence: 99%

“…Collection of various thermopower-conductivity data from literature as indicated in the legend. [6,7,91,111,[123][124][125]127] The grey line indicates a power law with slope -1/4, the black solid line is a fit to the transport edge model Eq. 11 (same parameters as in Figure 3c of Ref.…”

Section: Pedot:pssmentioning

confidence: 99%

Conjugated Polymer Blends for Organic Thermoelectrics

Zuo

Abdalla

Kemerink

2019

Adv Elect Materials

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A major attraction of organic conjugated semiconductors is that materials with new, emergent functionality can be designed and made by simple blending, as is extensively used in e.g. bulk heterojunction organic solar cells. Here, we critically review doped blends based on organic semiconductors (OSC) for thermoelectric applications. Several experimental strategies to improve thermoelectric performance, measured in terms of power factor (PF) or figure-ofmerit ZT, have been demonstrated in recent literature. Specifically, density-of-states design in blends of 2 OSCs can be used to obtain electronic Seebeck coefficients up to ∼2000 µV/K. Alternatively, blending with (high-dielectric constant) insulating polymers can improve doping efficiency and thereby conductivity, as well as induce more favorable morphologies that improve conductivity while hardly affecting thermopower. In the PEDOT:PSS blend system, processing schemes to either improve conductivity via morphology or via (partial) removal of the electronically isolating PSS, or both, have been demonstrated. Although a range of experiments have at least quasi-quantitatively been explained by analytical or numerical models, a comprehensive model for organic thermoelectrics is lacking so far.Strategies to increase thermoelectric performance of doped organic semiconductors by blending are reviewed. Experimental results are, where possible, compared to analytical and numerical models. Several promising strategies to increase conductivity and/or thermopower are experimentally identified in recent literature. In contrast, formal understanding, especially of the role of morphology, is somewhat lagging behind.

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“…Efforts have been made in improving the TE performance of the PEDOT:PSS films, including both the electrical conductivity and Seebeck coefficient. One straightforward way is to enhance the electrical conductivity of PEDOT:PSS by a post‐treatment with chemical agents such as organic polar solvents, acids, and small molecules . In terms of the fundamental physics, Seebeck coefficient depends on the energy band structure and the density of states (DOS) of the TE materials.…”

Section: Introductionmentioning

confidence: 99%

Significantly Enhanced Thermoelectric Properties of PEDOT:PSS Films through Sequential Post‐Treatments with Common Acids and Bases

Fan

et al. 2016

Advanced Energy Materials

367

299

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Thermoelectric (TE) materials are important for the sustainable development because they enable the direct harvesting of low‐quality heat into electricity. Among them, conducting polymers have attracted great attention arising from their advantages, such as flexibility, nontoxicity, easy availability, and intrinsically low thermal conductivity. In this work, a novel and facile method is reported to significantly enhance the TE property of poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) films through sequential post‐treatments with common acids and bases. Compared with the as‐prepared PEDOT:PSS, both the Seebeck coefficients and electrical conductivities can be remarkably enhanced after the treatments. The oxidation level, which significantly impacts the TE property of the PEDOT:PSS films, can also be well tuned by controlling the experimental conditions during the base treatment. The optimal PEDOT:PSS films can have a Seebeck coefficient of 39.2 µV K−1 and a conductivity of 2170 S cm−1 at room temperature, and the corresponding power factor is 334 µW (m−1 K−2). The enhancement in the TE properties is attributed to the synergetic effect of high charge mobility by the acid treatment and the optimal oxidation level tuned by the base treatment.

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Tuning the Thermoelectric Properties of a Conducting Polymer through Blending with Open-Shell Molecular Dopants

Cited by 31 publications

References 30 publications

Improved Alignment of PEDOT:PSS Induced by in-situ Crystallization of “Green” Dimethylsulfone Molecules to Enhance the Polymer Thermoelectric Performance

Improved Alignment of PEDOT:PSS Induced by in-situ Crystallization of “Green” Dimethylsulfone Molecules to Enhance the Polymer Thermoelectric Performance

Conjugated Polymer Blends for Organic Thermoelectrics

Significantly Enhanced Thermoelectric Properties of PEDOT:PSS Films through Sequential Post‐Treatments with Common Acids and Bases

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