On The Thermal Conductivity of Conjugated Polymers for Thermoelectrics

Author:

Rodríguez‐Martínez Xabier1ORCID,Saiz Fernan1ORCID,Dörling Bernhard1ORCID,Marina Sara2,Guo Jiali1,Xu Kai1,Chen Hu3,Martin Jaime245,McCulloch Iain367,Rurali Riccardo1ORCID,Reparaz Juan Sebastian1ORCID,Campoy‐Quiles Mariano1ORCID

Affiliation:

1. Institut de Ciència de Materials de Barcelona (ICMAB‐CSIC) Campus UAB Bellaterra 08193 Spain

2. POLYMAT and Polymer Science and Technology Department Faculty of Chemistry University of the Basque Country UPV/EHU Manuel de Lardizabal 3 Donostia‐ San Sebastián 20018 Spain

3. King Abdullah University of Science and Technology (KAUST) Solar Center (KSC) Thuwal 23955‐6900 Saudi Arabia

4. Universidade da Coruña Campus industrial de Ferrol CITENI Ferrol 15403 Spain

5. Ikerbasque Basque Foundation for Science Bilbao 48011 Spain

6. Department of Chemistry University of Oxford Oxford OX1 3TA UK

7. Andlinger Center for Energy and the Environment, and Department of Electrical and Computer Engineering Princeton University Princeton NJ 08544 USA

Abstract

AbstractThe thermal conductivity (κ) governs how heat propagates in a material, and thus is a key parameter that constrains the lifetime of optoelectronic devices and the performance of thermoelectrics (TEs). In organic electronics, understanding what determines κ has been elusive and experimentally challenging. Here, by measuring κ in 17 π‐conjugated materials over different spatial directions, it is statistically shown how microstructure unlocks two markedly different thermal transport regimes. κ in long‐range ordered polymers follows standard thermal transport theories: improved ordering implies higher κ and increased anisotropy. κ increases with stiffer backbones, higher molecular weights and heavier repeat units. Therein, charge and thermal transport go hand‐in‐hand and can be decoupled solely via the film texture, as supported by molecular dynamics simulations. In largely amorphous polymers, however, κ correlates negatively with the persistence length and the mass of the repeat unit, and thus an anomalous, albeit useful, behavior is found. Importantly, it is shown that for quasi‐amorphous co‐polymers (e.g., IDT‐BT) κ decreases with increasing charge mobility, yielding a 10‐fold enhancement of the TE figure‐of‐merit ZT compared to semi‐crystalline counterparts (under comparable electrical conductivities). Finally, specific material design rules for high and low κ in organic semiconductors are provided.

Funder

European Commission

H2020 Marie Skłodowska-Curie Actions

European Research Council

Ministerio de Ciencia e Innovación

Publisher

Wiley

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