Flexible organic-intercalated WSe2 hybrid: electronic structure modification and thermoelectric performance optimization

Two-dimensional tungsten selenide (WSe2) has great potential in thermoelectric (TE) applications, but dimensionality reduction results in a dramatic increase in thermal conductivity, which is not beneficial for improving thermoelectric performance. In this work, an electrochemical intercalation method is utilized to fabricate an organic-inorganic hybrid superlattice structure by decoupling the WSe2 layers without damaging the original bulk structure and then intercalating tetrabutylammonium (TBA) cations into the inorganic layers. The few-layer mixed-staging TBA-WSe2 hybrid with alternating stacking organic TBA cations and WSe2 inorganic layers possesses an electronic structure similar to that of the few-layer WSe2, which is beneficial for an enhanced Seebeck coefficient. The electron injection results in a considerable increase in the carrier concentration while the disorder in the mixed-staging structure succeeds in improving phonon scattering, leading to an enhanced figure-of-merit ZT of 0.25 at 340 K, which is three orders of magnitude higher than that of the pristine WSe2 single crystal and one of the highest ZT values among WSe2-based thermoelectric materials in recent years. This work may guide future research on dimensionality reduction in the electronic structures of bulk materials and the fabrication of flexible superlattice hybrids with considerable TE performance.