电化学制备超细g-C 3 N 4 量子点及其电催化析氢性能

Benefiting from their high concentration of in-plane nitrogen element, superior chemical/thermal stability, tunable electronic band structure and environmental friendly feature, graphite-like carbon nitride (g-C3N4) as a new promising metal-free material has drawn numerous attention in photo-/electric-catalysis. Comparing to the regulation of band structure in photocatalysis, the deliberately synthesis of g-C3N4 electrocatalysts is mainly focused on the construction of catalytic sites and the modulation of the charge transfer kinetics. Herein, this work reports a rapid method for synthesizing ultrafine g-C3N4 quantum dots (QDs) via electrochemical exfoliation using Al3+ ions. The uniform g-C3N4 QDs with smaller lateral dimension and thickness are collected due to the higher charge density and stronger electrostatic forces of Al3+ ions in the lattice of host materials as compared to the conventional univalent alkali cations. The as-obtained g-C3N4 QDs exhibit average lateral dimension and thickness of 3.5 nm and 1.0 nm, respectively, as determined by the TEM and AFM measurements. Also, the presence of the rich C/N defects is verified by the UV-vis spectra. Encouragingly, the ultrafine g-C3N4 QDs exhibit superior hydrogen evolution reaction (HER) performance with an ultra-low onset-potential closely approaching to 0 V, and a low overpotential of 208 mV at 10 mA/cm2, as well as a remarkably low Tafel slope (52 mV·dec-1) in acidic electrolyte. Taking the fabrication of the ultrafine g-C3N4 QDs with rich C/N defects as an example, this work provides a simple and feasible way to exfoliate 2D layered materials into low-dimensional nanomaterials towards highly-efficient electrocatalysis, as well as the exploration of their fascinating physic-chemical properties.