Cu2SnS3 (CTS), a typical ternary copper-based
sulfide, is considered as a potential p-type thermoelectric (TE) material
with the advantages of environmental friendliness and low cost, but
its performance is limited by the high lattice thermal conductivity
and electrical resistivity. Herein, we have successfully synthesized
undoped and In-doped CTS nanoparticles with a pure tetragonal phase
by the colloidal method. More interestingly, plenty of twin boundaries
appear in all the samples sintered from the synthesized nanoparticles
independent of composition. The twin boundaries can effectively reduce
the lattice thermal conductivity, while the tetragonal phase is beneficial
to meliorate the electrical performance of CTS. Consequently, the
highest zT reaches 0.36 at 700 K for Cu2Sn0.85In0.15S3, which is enhanced
by 17 times compared to that of the pristine CTS with mainly the monoclinic
phase. The tunable phase and microstructure via the colloidal method
provide useful guidance to promote the performance of eco-friendly
TE sulfides.
Multiple-band
degeneracy has been widely recognized to be beneficial for high thermoelectric
performance. Here, we discover that the p-type Dirac bands with lower
degeneracy synergistically produce a higher Seebeck coefficient and
electrical conductivity in topological semimetal BaAgBi. The anomalous
transport phenomenon intrinsically originated from the asymmetric
electronic structures: (i) complete p-type Dirac bands near the Fermi
level facilitate high and strong energy-dependent hole relaxation
time; (ii) the presence of additional parabolic conduction valleys
allows for a large density of states to accept scattered electrons,
leading to an enlarged hole–electron relaxation time ratio
and, thus, weakened bipolar effect. In combination with the strong
lattice anharmonicity, an exceptional p-type average ZT of 0.42 is achieved from 300 to 600 K, which can be dramatically
enhanced to 1.38 via breaking the C
3v
symmetry. This work uncovers the underlying mechanisms
governing the abnormal transport behavior in Dirac semimetal BaAgBi
and highlights the asymmetric electronic structures as target features
to discover/design high-performance thermoelectric materials.
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