With the high theoretical capacity and the ability of
large current
discharge, NiS2 has been expected as a new cathode material
for thermal batteries. However, its lower decomposition temperature
(∼500 °C) restricts its application on thermal batteries
because of the high operating temperature of thermal batteries (500–600
°C). In this case, Cr, Fe, Co, and Cu multielement-doped NiS2 (NiS2-d) has been successfully prepared by low-temperature
solid-phase sintering. Owing to the effect of high entropy, the multielement
doping improved the thermodynamic system stability of NiS2, and the decomposition temperature (2NiS2 → 2NiS
+ S2) increased from 482 to 610 °C. Interestingly,
doping also reduces the particle size of NiS2, resulting
in defects on the surface of NiS2 particles and improving
the conductivity of NiS2.The actual discharge capacity
of NiS2 enhanced significantly from 516 to 643 mA h g–1 at 500 °C, with a current density of 100 mA
cm–2 and a cut-off voltage of 1.5 V. This is due
to a more complete release of the first discharge reaction (NiS2 + 2Li+ + 2e– → NiS +
Li2S) as the decomposition temperature rises. The enhancement
of conductivity, meanwhile, lessens polarization during the discharge
process, raises the voltage of the NiS2 discharge platform,
and improves the stability of the NiS2 later discharge
platform. Additionally, the smaller particle size enables improved
contact between the cathode and the electrolyte interface, allowing
electrolyte ions to quickly come into touch with the NiS2 surface. These results show that the discharge performance of NiS2 at high temperatures could be effectively improved by multielement
doping. It provides a new method for improving the stability of a
metal sulfide and its application at high-temperature discharge.