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@ARTICLE{Zhou:888209,
author = {Zhou, Chongjian and Yu, Yuan and Lee, Yea-Lee and Ge,
Bangzhi and Lu, Weiqun and Cojocaru-Mirédin, Oana and Im,
Jino and Cho, Sung-Pyo and Wuttig, Matthias and Shi, Zhongqi
and Chung, In},
title = {{E}xceptionally {H}igh {A}verage {P}ower {F}actor and
{T}hermoelectric {F}igure of {M}erit in n-type {P}b{S}e by
the {D}ual {I}ncorporation of {C}u and {T}e},
journal = {Journal of the American Chemical Society},
volume = {142},
number = {35},
issn = {1520-5126},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2020-04763},
pages = {15172 - 15186},
year = {2020},
note = {Bitte Post-print ergänzen},
abstract = {Thermoelectric materials with high average power factor and
thermoelectric figure of merit (ZT) has been a sought-after
goal. Here, we report new n-type thermoelectric system
CuxPbSe0.99Te0.01 (x = 0.0025, 0.004, and 0.005) exhibiting
record-high average ZT ∼ 1.3 over 400–773 K ever
reported for n-type polycrystalline materials including the
state-of-the-art PbTe. We concurrently alloy Te to the PbSe
lattice and introduce excess Cu to its interstitial voids.
Their resulting strong attraction facilitates charge
transfer from Cu atoms to the crystal matrix significantly.
It follows the increased carrier concentration without
damaging its mobility and the consequently improved
electrical conductivity. This interaction also increases
effective mass of electron in the conduction band according
to DFT calculations, thereby raising the magnitude of
Seebeck coefficient without diminishing electrical
conductivity. Resultantly, Cu0.005PbSe0.99Te0.01 attains an
exceptionally high average power factor of ∼27 μW cm–1
K–2 from 400 to 773 K with a maximum of ∼30 μW cm–1
K–2 at 300 K, the highest among all n- and p-type
PbSe-based materials. Its ∼23 μW cm–1 K–2 at 773 K is
even higher than ∼21 μW cm–1 K–2 of the
state-of-the-art n-type PbTe. Interstitial Cu atoms induce
the formation of coherent nanostructures. They are highly
mobile, displacing Pb atoms from the ideal octahedral center
and severely distorting the local microstructure. This
significantly depresses lattice thermal conductivity to
∼0.2 Wm–1 K–1 at 773 K below the theoretical lower
bound. The multiple effects of the dual incorporation of Cu
and Te synergistically boosts a ZT of Cu0.005PbSe0.99Te0.01
to ∼1.7 at 773 K.},
cin = {PGI-10},
ddc = {540},
cid = {I:(DE-Juel1)PGI-10-20170113},
pnm = {521 - Controlling Electron Charge-Based Phenomena
(POF3-521)},
pid = {G:(DE-HGF)POF3-521},
typ = {PUB:(DE-HGF)16},
pubmed = {32786777},
UT = {WOS:000569271600036},
doi = {10.1021/jacs.0c07712},
url = {https://juser.fz-juelich.de/record/888209},
}