Graphitic Carbon Cloth-Based Hybrid Molecular Catalyst: A Non-conventional, Synthetic Strategy of the Drop Casting Method for a Stable and Bifunctional Electrocatalyst for Enhanced Hydrogen and Oxygen Evolution Reactions.

Hydrogen energy production through water electrolysis is envisaged as one of the most promising, sustainable, and viable alternate sources to cater to the incessant demands of renewable energy storage. Germane to our effort in this field, we report easily synthesizable and very cost-effective isoperthiocyanic acid (IPA) molecular complexes as electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) under acidic and alkaline conditions. The Pd(II)IPA, Co(II)IPA, and Ni(II)IPA complexes were synthesized and were evaluated for HER and OER applications. These complexes when embedded onto graphitized carbon cloth (GrCC) exhibited a significant enhancement in the HER activity in contrast to their pristine counterparts. The hybrid electrocatalyst Pd(II)IPA among the three showed an extremely low overpotential of 94.1 mV to achieve a current density of 10 mA cm -2 , while Co(II)IPA and Ni(II)IPA complexes showed overpotentials of 367 and 394 mV, respectively, to achieve a current density of 10 mA cm -2 . These complexes on carbon cloth showed decreased charge transfer resistance compared to that of pristine metal complexes. The enhanced catalytic activity of the complexes on carbon cloth can be attributed to the porous and conducting nature of the graphitized carbon cloth. For OER activity, the Pd(II)IPA complex showed an excellent performance with an overpotential value of 210 mV, while Co(II)IPA and Ni(II)IPA exhibited overpotentials of 400 and 270 mV, respectively, to drive a current density of 10 mA cm -2 in 0.1 M KOH. This work further widens the scope and application of molecular complexes in combination with an excellent carbon support for renewable energy storage applications.