Design Rules for Polymer Blends with High Thermoelectric Performance

A combinatorial study of the effect of in-mixing of various guests on the thermoelectric properties of the host workhorse polymer poly[2,5-bis(3-tetradecylthiophen-2-yl)thieno[3,2-b]thiophene] (PBTTT) is presented. Specifically, the composition and thickness for doped films of PBTTT blended with different polymers are varied. Some blends at guest weight fractions around 10-15% exhibit up to a fivefold increase in power factor compared to the reference material, leading to zT values around 0.1. Spectroscopic analysis of the charge-transfer species, structural characterization using grazing-incidence wide-angle X-ray scattering, differential scanning calorimetry, Raman, and atomic force microscopy, and Monte Carlo simulations are employed to determine that the key to improved performance is for the guest to promote long-range electrical connectivity and low disorder, together with similar highest occupied molecular orbital levels for both materials in order to ensure electronic connectivity are combined.Funding Agencies|Spanish Ministry of Science and InnovationSpanish Government [CEX2019-000917-S, PGC2018-095411- B-I00, PGC2018-094620-A-I00, MAT2017-90024-P]; European Research Council (ERC)European Research Council (ERC)European Commission [648901, 963954]; Ministerio de Ciencia, Innovacion y UniversidadesSpanish Government; European Regional Development FundEuropean Commission; European Social FundEuropean Social Fund (ESF); CSIC Open Access Publication Support Initiative through its Unidad de Recursos de Informacion Cientifica para la Investigacion (URICI); Carl Zeiss Foundation; Alexander von Humboldt FoundationAlexander von Humboldt Foundation