Piezoelectric polarization promoted spatial separation of photoexcited electrons and holes in two-dimensional g-C3N4 nanosheets for efficient elimination of chlorophenols

Abstract

Graphitic carbon nitride (g-C3N4) has been proved to be a potential photocatalyst for environment purification, but the high recombination rate of photogenerated carriers leads to the low photocatalytic efficiency. Herein, we report the enhanced degradation of chlorophenols by 2D ultrathin g-C3N4 nanosheets with intrinsic piezoelectricity through photopiezocatalysis strategy. Under the simultaneous visible-light irradiation and ultrasonic vibration, the 2D g-C3N4 presented improved removal efficiency for elimination of 2,4-dichlorophenol (2,4-DCP) with an apparent rate constant of 6.65 × 10−2 min−1, which was 6.7 and 2.2 times of the photocatalysis and piezocatalysis, respectively. The improved removal efficiency was attributed to the sufficient separation of free charges driven by the ultrasound-induced piezoelectric field in the 2D g-C3N4, which was demonstrated by the enhanced current response under photopiezocatalysis mode. Additionally, the photopiezocatalysis of 2D g-C3N4 was proved to possess well universality for removing different chlorophenols, as well as high durability and dechlorination efficiency. Finally, a possible photopiezocatalytic mechanism for removal of 2,4-DCP was proposed based on the electron paramagnetic resonance (EPR) technique and the determination of intermediates through liquid chromatography-mass spectrometry (LC-MS) analysis. This work provides a promising strategy for the design of energy-conversion materials towards capturing solar and mechanical energy in ambient environment.