Efficient PMS activation toward degradation of bisphenol A by metal-free nitrogen-doped hollow carbon spheres

Abstract

Peroxymonosulfate (PMS) activation methods conventionally face challenges such as high energy consumption and the risk of metal leaching, limiting their practical application. Metal-free catalysts often face the problem of low catalytic activity. This study designed an in-situ nitrogen-doped hollow carbon catalyst (DNC-9), which offers balances efficient catalytic performance and metal-free catalysis. The results indicate that the DNC-9/PMS system effectively degrades bisphenol A, achieving complete degradation over a broad pH range (3.0–9.0). Through structure modification, the degradation efficiency of bisphenol A compared with SiO2@DNC-9/PMS system was improved by around 6 times and the degradation kinetic rate can reach 0.346 min−1. DNC-9 can activate PMS, resulting in a higher concentration of singlet oxygen without the generation of free radicals. Graphitic nitrogen in DNC-9 plays a crucial role in this activation, offering adsorption sites that facilitate decomposition of PMS and generating 1O2. In addition, graphitic nitrogen forms a transient active intermediate, DNC-9-PMS*, enhancing bisphenol A degradation. The catalyst recovers its high activity to complete bisphenol A removal with 15 min after thermal regeneration in cyclic experiments, demonstrating its potential as a practical solution for the efficient degradation of emerging contaminants.