Use of sustainable electrode components in Li-ion battery
technology
is essential for large-scale applications while addressing environmental
concerns. Considering elemental abundance, Fe-based compounds can,
in principle, work as the most economic cathodes. Fe-based hydroxysulfates
Li
x
FeSO4OH (x = 0 –1) can be harnessed as low-cost, sustainable, high-voltage,
and moisture-resistant battery cathode materials. In this system,
monoclinic (m) FeSO4OH and layered m-FeSO4OH were previously reported as Li-ion battery cathode materials.
Here, we introduce orthorhombic (o) FeSO4OH as a potential low-cost cathode for Li-ion batteries synthesized
by using a facile low-temperature hydrothermal route. The o-FeSO4OH cathode delivers a reversible capacity of 100 mA h/g at
a current rate of C/20 (1e– = 159 mAh/g) at a working
potential of ca. 3.2 V vs Li+/Li. A higher overpotential
and faster rate kinetics compared with that of m-FeSO4OH
stem from the subtle deviations in the structural framework affecting
the Li coordination environment. Operando analytical tools, electrochemical
titration techniques, and computational modeling are combined to characterize
the complex phase transformation during the (de)lithiation process.