Enhanced piezo-phototronic effect in carbon nitride nanosheets via oxidative exfoliation for high-efficiency piezo-photocatalysis†

Abstract

The application of piezo-photocatalysis in wastewater treatment by harnessing both solar and mechanical energy simultaneously offers a promising strategy for sustainable pollutant degradation. Nevertheless, integrating robust piezoelectric and semiconducting properties effectively within a single-component catalyst to achieve optimal synergy remains challenging due to their inherent trade-off. To tackle this limitation, a series of graphitic carbon nitride (g-C₃N₄) nanosheets with a controlled degree of exfoliation have been fabricated through a facile oxidative exfoliation strategy in this work. The exfoliated nanosheets demonstrate substantial improvements in both piezoelectricity (36 pm V⁻¹) and semiconducting properties, significantly enhancing their piezo-photocatalytic performance for organic pollutant degradation. Combined experimental and theoretical analysis reveals that the oxidative exfoliation process not only enables the easy domain deformation feature of the nanosheets, but also introduces surface polar functional groups, thus accelerating polarization and the piezoelectric response. Meanwhile, the charge carrier migration pathway to surface-active sites has been largely shortened, benefiting from the nanosheet structure. Consequently, the optimized material E500-CN (g-C₃N₄ exfoliated at 500 °C) demonstrates superior piezo-photocatalytic degradation performance, achieving a degradation rate of 97% within 20 min and a first-order kinetic rate constant of 0.152 min⁻¹, which is 5.1-fold faster than that of B-CN. The mechanism study highlights the critical role of the enhanced piezo-phototronic effect, where the vibration-induced in-plane piezopotential effectively manipulates the separation and transportation of photogenerated electron–hole pairs. This study offers a feasible design strategy for efficient 2D piezo-photocatalysts in water remediation, enabling a sustainable water treatment approach.