Systematic Study on Morphological, Electrochemical Impedance, and Electrocatalytic Activity of Graphitic Carbon Nitride Modified on a Glassy Carbon Substrate from Sequential Exfoliation in Water.

Abstract

Several researchers have synthesized graphitic carbon nitride (GCN) from various precursors and attached it to electrode substrates after exfoliation under different conditions and have reported inconsistent data on electrochemical impedance, electroactive surface areas, and electrocatalytic activity. Thus, the present study aims to study the same systematically in addition to morphology after modifying GCN on the GC substrate from different exfoliation times in water assisted by sonication. The GCN was prepared from urea by bulk condensation pyrolysis and then attached to the GC substrate by drop casting to study its morphology, electrochemical impedance, and electrocatalytic activity with respect to exfoliation. The SEM image of a GCN-modified GC plate after 15 and 30 min of exfoliation shows bulky structure whereas thin sheets of GCN were noticed after 120 min of exfoliation. On the other hand, broken sheets were observed when GCN was coated from beyond 120 min of exfoliation. The electrochemical impedance studies show that the charge transfer resistance (RCT) of GCN modified from 15 and 30 min of exfoliation was higher than that for the bare GC electrode. However, it started to decrease while increasing the exfoliation time, and 1.8 kΩ was obtained after 120 min of exfoliation. The RCT value was again increased to 3.2 and 5.0 kΩ for GCN coated after 150 and 180 min of exfoliation, respectively. The electroactive surface area (EASA) of GCN modified by 15 and 30 min of exfoliation was less than that of the bare GC electrode, whereas it was 3.8-fold higher for GCN coated from 120 min of exfoliation. The electrocatalytic activity of the GC electrodes modified with GCN was then tested by studying ascorbic acid (AA) and dopamine (DA) oxidation and reduction of hydrogen peroxide (HP). Among the different exfoliation times, GCN modified from 120 min of exfoliation displayed the highest electrocatalytic activity toward AA, DA, and HP. This was attributed to its higher EASA and lower charge-transfer resistance.