Poly(nickel-ethylenetetrathiolate) and Its Analogs: Theoretical Prediction of High-Performance Doping-Free Thermoelectric Polymers

Poly(nickel-ethylenetetrathiolate) and Its Analogs: Theoretical Prediction of High-Performance Doping-Free Thermoelectric Polymers

Journal of the American Chemical Society

10.1021/jacs.8b08270

https://doi.org/10.1021/jacs.8b08270

Wen Shi, Gang Wu, Kedar Hippalgaonkar, Jian-Sheng Wang, Jianwei Xu, Shuo-Wang Yang

02 October 2018

J. Am. Chem. Soc. 2018, 140, 41, 13200-13204

It is generally deemed that doping is a must for polymeric materials to achieve their high thermoelectric performance. We herein present the first report that intrinsically metallic behaviors and high-performance thermoelectric power factors can coexist within doping-free linear-backbone conducting polymers, poly(nickel-ethylenetetrathiolate) and its analogs. On the basis of density functional calculations, we have corroborated that four crystalline π-d conjugated transition-metal coordination polymers, including poly(Ni-C2S4), poly(Ni-C2Se4), poly- (Pd-C2S4) and poly(Pt-C2S4) exhibit intrinsically metallic behavior arising from the formation of dense intermolecular interaction networks between sulfur/selenium atoms. They show moderate carrier concentrations (1019−1021 cm−3) and decent conductivities (103−104 S cm−1), among which, poly(Ni-C2S4), poly(Ni-C2Se4) and poly(Pd-C2S4) possess high power factors (∼103 μW m−1 K−2).

PublisherCopyrights

This work was supported by the Agency for Science, Technology and Research (A*STAR) of Singapore (1527200024 and 1527200019). Computational resources are provided by the National Supercomputing Centre Singapore (NSCC) and A*STAR Computational Resource Centre (A*CRC).

This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of the American Chemical Society, copyright © American Chemical Society after peer review. To access the final edited and published work see https://doi.org/10.1021/jacs.8b08270

https://oar.a-star.edu.sg/communities-collections/articles/15659

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