Fe, Co, N co-doped hollow carbon capsules as a full pH range catalyst for pollutant degradation via a non-radical path in Fenton-like reaction

Abstract

Persulfate (PMS)-based Fenton-like reaction was a highly efficient technique for disposal of organic contaminants. However, high metal leaching and low environmental adaptation were the major concerns for further application. To overcome these two drawbacks, herein, Fe, Co, N atoms co-doped hollow carbon capsules (Fe-Co-N@HCCs) were prepared and used as catalysts for PMS activation. 92.6% of TC was degraded within 40 min and the mineralization efficiency was 55.7%. The degradation rate was 4.7, 3.1 and 1.4 times higher than those of activated carbon, N@HCCs, and Fe-N@HCCs, respectively. Thermodynamic study indicated the TC degradation was an exothermal, chaotic and non-spontaneous process. Radical trapping experiments, electron paramagnetic resonance spectrum, and electrochemical analysis indicated that 1O2 production and electron-transfer path worked together for PMS activation. DFT calculation indicated that the catalytic activity of Co-N4 site was higher than Fe-N4 site for 1O2 production. Fe-Co-N@HCCs were adapted well to the full pH range (0–14) and complex inorganic anions via non-radical PMS activation paths. Meanwhile, the leached Fe and Co ions were lowered to 0.201 and 0.457 mg/L, satisfying the China emission standard. This work gave a better comprehension on preparation of carbonaceous materials with high environmental adaptation and low leached metal ions for PMS activation.