Abstract:
Zeolite imidazolate frameworks (ZIFs) derived high surface area materials have been
established as the promising electrode materials in supercapacitors due to their tunable
morphology, profuse N species and abundance heteroatom based electroactive sites. In
this work, manganese-doped ZIF-67 derived nitrogen-doped carbon-based sulfide
Mn/Co/NC/S electrode is synthesized for augmented performance in supercapacitors. The
manganese doped ZIF-67 (MnCo-ZIF) is synthesized by the simple co-precipitation
method. MnCo-ZIF is converted to nitrogen doped porous carbon structure (Mn/Co/NC)
through heat treatment in controlled environment (Ar/H2 90:10) at a very slow heating
rate of 3 ºC/min. Subsequently, the ion exchange sulfidation reaction is conducted in
hydrothermal autoclave at 180 ºC for 12 hours to convert Mn/Co/NC to Mn/Co/NC/S.
MnCo-ZIF(ZIF_8/1) exhibits 2D leaf-like morphology with dimension of 5.51 × 2.61 µm.
Mn/Co/NC(C_8/1) material shows a highly porous carbon structure. The synthesized
Mn/Co/NC/S (CS_8/1) material exhibits porous 2D sheet-like morphology and active
sites of MnS2 are created on the porous carbon surface. Among all synthesized materials,
CS_8/1 has shown high surface area of 971 m
. Cyclic voltammetry results of all
electrodes show a pseudocapacitive behavior. The CS_8/1 electrode exhibits ultra-high
specific capacitance of 1194 F g
2
-1
g
at 1080
W kg
-1
-1
at 1 A g
and specific energy of 214.89 Wh kg
-1
-1
. Furthermore, the CS_8/1 electrode has shown exceptional cyclic stability with
specific capacitance retention of 82% after 5000 cycles. EIS measurements show the
charge transfer resistance Rct to be as minimum as 0.96 Ω for CS_8/1 electrode. Mn and
S ions play important role in boosting the charge transfer and ultimately promoting
pseudocapacitive properties with capacitive controlled reaction kinetics percentage as
high as 94%. This improved performance is attributed to the synergistic impact of Mn ions
paired with Co ions, as well as increased redox reaction and structural rearrangements.