Tuning the Photo-Characteristics of g-C3N4 Incorporated CoCuFe-LDH for Enhanced Hydrogen Evolution Reaction and Dye-Sensitized Solar Cell Performance
摘要
This article details the effective synthesis of a new g-C3N4/CoCuFe-LDH heterostructure using a hydrothermal assembly technique and thermal polymerization. The objective was to improve the performance of dye-sensitized solar cells (DSSCs) and the hydrogen evolution reaction (HER). By generating a hierarchical structure with enhanced interfacial contact, structural characterization verified the effective integration of CoCuFe-LDH nanosheets with g-C3N4 layers. In comparison to pure CoCuFe-LDH, the composite exhibited a specific surface area of 101.8 m2 g⁻1, a pore volume of 0.077 cm3 g⁻1, and an average pore diameter of 2.895 nm, all of which contributed to efficient ion diffusion and charge transfer. Electrochemical hydrogen evolution reactions (HER) in 0.5 M H2SO4 showed that the g-C3N4/CoCuFe-LDH electrode had better catalytic activity than g-C3N4 and CoCuFe-LDH, with a much smaller Tafel slope of 88 mV dec⁻1 compared to 166 mV dec⁻1 and 155 mV dec⁻1, respectively, suggesting faster proton–electron transfer kinetics. In addition, the hybrid catalyst exhibited a significantly improved electrochemical double-layer capacitance (Cdl) of 3.94 mF cm⁻2 and an electrochemically active surface area (ECSA) of 98.5 cm2, which is nearly twice that of CoCuFe-LDH (41.8 cm2). Furthermore, electrochemical impedance spectroscopy results showed that the charge transfer resistance (Rct) was 3.27 Ω and the solution resistance (Rs) was 1.82 Ω, confirming enhanced electrical conductivity and faster electron transport. The catalyst also demonstrated excellent durability, maintaining stable performance after 100 h of continuous HER operation. In DSSC applications, the device using the g-C3N4/CoCuFe-LDH counter electrode achieved a power conversion efficiency (PCE) of 8.78 ± 0.2%, outperforming g-C3N4 (2.21 ± 0.2%) and CoCuFe-LDH (4.67 ± 0.4%) electrodes. The enhanced light absorption, accelerated charge transport, suppressed electron recombination, and abundant catalytic active sites in the g-C3N4/CoCuFe-LDH composite arise from the synergistic coupling between the conductive g-C3N4 nanosheets and the catalytically active trimetallic LDH layers.