New insights into the effect of adsorption on catalysis in the metal-free persulfate activation process for removing organic pollutants

Abstract

• Sucrose-derived N-doped CXs were prepared by a simple hydrothermal method. • Pollutants degradation were mainly by nonradical pathway in CXs/PS system. • High adsorption capacity was beneficial to organic pollutants degradation in Mode 1. • Inhibitory effect of adsorption on catalytic PS activation was found in Mode 2. • The sulfonic group on pollutants might play a crucial role in the inhibitory effect. Coupling adsorption and advanced oxidation processes (AOPs), two widely used wastewater treatment technologies, has been an attractive idea pursued by many researchers. Although many studies have demonstrated that adsorption could facilitate AOPs such as persulfate (PS) activation, the inhibitory effect of adsorption on PS activation was ignored. In this work, both as adsorbents and catalysts, sucrose-derived carbon xerogels (CXs) were prepared to investigate the effect of adsorption on PS activation. The results showed that the specific surface areas (SSAs) and N contents of CXs varied with the HCl concentration. Among different CXs, CX-0.5 with the highest SSA and N content exhibited the highest adsorption capacity and catalytic activity for acid orange 7 (AO7) degradation by simultaneously adding CXs and PS, where the promoting effect of adsorption on catalysis was found. Quenching tests demonstrated that degradation of pollutants in the CX-0.5/PS system were mainly by nonradical pathway. However, the catalytic activities of CXs were inhibited after the pre-adsorption of AO7 on CXs. Comparing the molecular structures of several compounds, the sulfonic group on chemicals might play a crucial role in the inhibitory effect. We concluded that if CXs have the same adsorption sites for pollutants and PS, adsorption of pollutants would inhibit the catalytic PS activation. These findings provided a comprehensive understanding of the effect of adsorption on AOPs, which had a significant guidance for future researches and applications.