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	Controlling the thermoelectric properties of organometallic coordination polymers via ligand design Zilu Liu , Tianjun Liu , Christopher N. Savory , José P. Jurado , Juan Sebastián Reparaz , Jianwei Li , Long Pan , Charl F. J. Faul , Ivan P. Parkin , Gopinathan Sankar , Satoru Matsuishi , Mariano Campoy‐quiles , David O. Scanlon , Martijn A. Zwijnenburg , Oliver Fenwick , Bob C. Schroeder Advanced Functional Materials 134 DOI: 10.1002/adfm.202003106 Open Access Show Abstract ▼ Abstract: Organometallic coordination polymers (OMCPs) are a promising class of thermoelectric materials with high electrical conductivities and thermal resistivities. The design criteria for these materials, however, remain elusive and so far material modifications have been focused primarily on the nature of the metal cation to tune the thermoelectric properties. Herein, an alternative approach is described by synthesizing new organic ligands for OMCPs, allowing modulation of the thermoelectric properties of the novel OMCP materials over several orders of magnitude, as well as controlling the polarity of the Seebeck coefficient. Extensive material purification combined with spectroscopy experiments and calculations furthermore reveal the charge‐neutral character of the polymer backbones. In the absence of counter‐cations, the OMCP backbones are composed of air‐stable, ligand‐centered radicals. The findings open up new synthetic possibilities for OMCPs by removing structural constraints and putting significant emphasis on the molecular structure of the organic ligands in OMCP materials to tune their thermoelectric properties.	Jun 2020

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Controlling the thermoelectric properties of organometallic coordination polymers via ligand design