Bi2Te3-based materials are dominating thermoelectrics
for almost all of the room-temperature applications. To meet the future
demands, both their thermoelectric (TE) and mechanical properties
need to be further improved, which are the requisite for efficient
TE modules applied in areas such as reliable micro-cooling. The conventional
zone melting (ZM) and powder metallurgy (PM) methods fall short in
preparing Bi2Te3-based alloys, which have both
a highly textured structure for high TE properties and a fine-grained
microstructure for high mechanical properties. Herein, a mechanical
exfoliation combined with spark plasma sintering (ME-SPS) method is
developed to prepare Bi0.5Sb1.5Te3 with highly improved mechanical properties (correlated mainly to
the dislocation networks), as well as significantly improved thermoelectric
properties (correlated mainly to the texture structure). In the method,
both the dislocation density and the orientation factor (F) can be tuned by the sintering pressure. At a sintering pressure
of 20 MPa, an exceptional F of up to 0.8 is retained,
leading to an excellent power factor of 4.8 mW m–1 K–2 that is much higher than that of the PM polycrystalline.
Meanwhile, the method can readily induce high-density dislocations
(up to ∼1010 cm–2), improving
the mechanical properties and reducing the lattice thermal conductivity
as compared to the ZM ingot. In the exfoliated and then sintered (20
MPa) sample, the figure-of-merit ZT = 1.2 (at 350 K), which has increased
by about ∼20%, and the compressive strength has also increased
by ∼20%, compared to those of the ZM ingot, respectively. These
results demonstrate that the ME-SPS method is highly effective in
preparing high-performance Bi2Te3-based alloys,
which are critical for TE modules in commercial applications at near-room
temperature.