In this paper, a simple hydrothermal approach is employed to prepare nitrogen-doped graphene quantum dots (N-GQDs) with controllable size and structural features, where citric acid and ethylenediamine served as the carbon and nitrogen precursors, respectively. The influence of hydrothermal temperature and duration on the structural features, surface chemistry, and electrochemical behavior of N-GQDs is systematically investigated. The capacitive behavior of N-GQD electrodes exhibits typical pseudocapacitive characteristics, primarily attributed to the surface functional groups. The NG-2 electrode (180 °C, 6 h) demonstrates a specific capacitance of 309.8 F g⁻¹ at 1 A g⁻¹ and maintains 98.1% of its initial capacitance after 8000 cycles, confirming excellent stability. Density functional theory (DFT) results demonstrate that the co-presence of graphitic and pyrrolic nitrogen induces a synergistic modulation of the electronic structure, resulting in improved charge-transfer kinetics and surface reactivity of N-GQDs compared to single-type nitrogen doping. Additionally, NG-2//activated carbon (AC)-asymmetric supercapacitor (ASC) achieves an energy density of 22.5 Wh kg⁻¹ at 500 W kg⁻¹ and maintains outstanding cycling stability. This work provides valuable insights into the design and application of N-GQDs for advanced energy storage devices.

Electrochemical water splitting for hydrogen production is a key technological route toward the large-scale generation of green hydrogen. However, the anodic oxygen evolution reaction (OER) suffers from sluggish kinetics and high overpotential, necessitating the development of non-noble metal catalysts that simultaneously possess low cost, high activity, and excellent stability. In this work, a nitrogen-doped graphene quantum dots@nickel–iron layered double hydroxide (N-GQDs@NiFe-LDH) composite catalyst was in situ constructed via a facile hydrothermal strategy. Benefiting from the electronic modulation and structural confinement effects of N-GQDs, the intrinsic catalytic activity and structural stability of the catalyst were simultaneously enhanced. The as-prepared catalyst requires an overpotential of only 320 mV to deliver a current density of 500 mA cm⁻² and maintains 98% of its initial activity after 100 h of chronoamperometric stability testing, demonstrating promising potential for practical applications. Multiscale characterizations revealed that N-GQDs formed strong electronic interactions with Ni/Fe active sites at the interface, significantly enhanced interfacial electron transport, and accelerated the OER kinetics. This study demonstrates that the N-GQDs@NiFe-LDH catalytic system constructed via an interfacial heterostructure engineering strategy provides a new insight for the rational design and development of efficient non-noble-metal OER electrocatalysts.