Transition metal type-dependent pseudocapacitance performance of rGO@NiM (M = Cu, Mn, and Co) LDH/SrTiO3 nanocomposites hybrid electrodes for asymmetric supercapacitor application
This study aims to clarify how different transition metals influence the pseudocapacitive performance of layered double hydroxide (LDH)-based nanocomposites. We investigated reduced graphene oxide (rGO)@NiM LDH/SrTiO3 (M = Cu, Mn, or Co) hybrids to examine the role of metal selection in both structural evolution and electrochemical performance. The morphology of the NiM LDH NCs, decorated on SrTiO₃ nanosheets, varies significantly with the metal additive: Cu-containing hybrids exhibit a nanoparticle morphology, while Mn- and Co-based hybrids display a nanoflower-like structure. Raman and X-ray photoelectron spectroscopy confirm the in-situ formation of rGO during the electrodeposition of NiM LDH, without the need for any external carbon source. Furthermore, the characteristics of the interfacial oxygenated carbon bonds between rGO and NiM LDH NCs and the resulting synergistic interactions depend on the incorporated metal type. Electrochemical testing shows that all rGO@NiM LDH@SrTiO3 hybrids outperform pristine SrTiO3, achieving specific capacitances of 2053–2337 mF·cm⁻2 at 1 mA·cm⁻2 compared to 1182 mF·cm⁻2 for bare SrTiO3. Among assembled asymmetric supercapacitors, Co-based devices deliver the highest energy density (82.3 μWh·cm⁻2 at 5.59 mW·cm⁻2), Mn-based devices provide moderate performance (59.5 μWh·cm⁻2 at 6.12 mW·cm⁻2), and Cu-based devices show the lowest energy density (55.26 μWh·cm⁻2 at 5.87 mW·cm⁻2). However, Cu-based devices exhibit better energy retention, maintaining 46.5 μWh·cm⁻2 at a higher power density of 57.7 mW·cm⁻2. These findings highlight that metal choice critically governs both morphological features and energy storage characteristics, providing guidelines for the design of LDH-based pseudocapacitive materials. Graphical abstract