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Enhancing thermoelectric performance in hierarchically structured BiCuSeO by increasing bond covalency and weakening carrier–phonon coupling

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Abstract

BiCuSeO oxyselenides are promising thermoelectric materials at intermediate temperatures, primarily due to their ultralow lattice thermal conductivity (κL) and high Seebeck coefficient. The intrinsically low carrier mobility in these materials, normally below ∼20 cm2 V−1 s−1 at 300 K, however, largely limits further improvements of their thermoelectric properties. In this study, by introducing less electronegative Te into the conductive Cu–Se layers, we demonstrate that the enhanced chemical bond covalency results in smaller effective mass and thus improved carrier mobility, through the weakening of carrier-phonon coupling. The improved carrier mobility by Te-doping largely retains the electrical conductivity values and thus high power factors even with decreased carrier concentrations. Meanwhile, the hierarchical structural features including dual point defects, nanoinclusions, grain boundaries, etc., originating from the nonequilibrium self-propagating high-temperature synthesis (SHS) processes, further reduce κL close to the amorphous limit. Ultimately, a maximum ZT value of ∼1.2 at 873 K is achieved in Bi0.96Pb0.04CuSe0.95Te0.05O, ∼35% improvement as compared with that of Te-free Bi0.96Pb0.04CuSeO and ∼2.4 times higher than that of the pristine sample. Furthermore, our study elucidates that weakening of carrier–phonon coupling through regulating chemical bonding within the conductive functionalities can be an effective avenue for further improving the thermoelectric performance of BiCuSeO.

Graphical abstract: Enhancing thermoelectric performance in hierarchically structured BiCuSeO by increasing bond covalency and weakening carrier–phonon coupling

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Publication details

The article was received on 17 Feb 2017, accepted on 29 Mar 2017 and first published on 29 Mar 2017


Article type: Paper
DOI: 10.1039/C7EE00464H
Citation: Energy Environ. Sci., 2017, Advance Article
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    Enhancing thermoelectric performance in hierarchically structured BiCuSeO by increasing bond covalency and weakening carrier–phonon coupling

    G. Ren, S. Wang, Y. Zhu, K. J. Ventura, X. Tan, W. Xu, Y. Lin, J. Yang and C. Nan, Energy Environ. Sci., 2017, Advance Article , DOI: 10.1039/C7EE00464H

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