摘要
Rough spherical O v -rich Fenton-like catalysts were fabricated by hard-template method and chemical reduction. • Dimethylamine could be mineralized to non-toxic carbon dioxide, water and NO 3 − . • Rich oxygen vacancies and bimetallic synergism promoted the activation of PMS. • The catalyst could adsorb DMA and PMS, thus shortening the distance between DMA and ROS. As a widely used volatile organic solvent, dimethylamine (DMA) easily escapes into atmosphere, causing great threat to the environment. In this study, a novel heterogeneous Fenton-like catalyst, spherical CoFe 2 O x with rich oxygen vacancies and rough surface (S-CoFe 2 O x -O v ) is fabricated with the hard-template method to effectively activate PMS for removing DMA. Compared with CoFe 2 O x prepared by traditional coprecipitation method, the DMA degradation rate is enhanced by 13 times over S-CoFe 2 O x -O v . Quenching experiments, EPR analysis, and electrochemical tests confirmed that SO 4 •− , O 2 •− , 1 O 2 , and electron transfer pathway are responsible for the degradation of DMA. XPS analysis proves that O v and the Co 2+ –Co 3+ redox cycle are responsible for the production of ROS from PMS, and the presence of Fe 2+ facilitated the redox cycle of Co 2+ –Co 3+ . DFT calculations prove that the adsorption and activation of PMS on the surface of catalyst is thermodynamically favorable. In addition, DMA could also be adsorbed on the catalyst surface, which can shorten the migration distance between DMA and ROS. The degradation mechanism of DMA is proposed and verified using the detected intermediates. The catalyst also exhibits effective degradation of other organic amines, demonstrating the broad applicability. Therefore, this study provides a feasible hard-template method for fabricating efficient Fenton-like catalyst. Download: Download high-res image (153KB) Download: Download full-size image
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