摘要
Cobalt iron spinel(CoFe_(2)O_(4)) has been considered as a good heterogeneous catalysis to peroxymonosulfate(PMS) in the degradation of persistent organic pollutants due to its magnetic properties and good chemical stability. However, its catalytic activity needs to be further improved. Here, a facial strategy, “in-situ substitution”, was adopted to modify CoFe_(2)O_(4) to improve its catalytic performance just by suitably increasing the Co/Fe ratio in synthesis process. Compared with CoFe_(2)O_(4), the newly synthesized Co_(1.5)Fe_(1.5)O_(4), could not only significantly improve the degradation efficiency of phenol, from 50.69 to 93.6%, but also exhibited more effective mineralization ability and higher PMS utilization. The activation energy advantage for phenol degradation using Co_(1.5)Fe_(1.5)O_(4)was only 44.2 k J/mol, much lower than that with CoFe_(2)O_(4)(127.3 k J/mol). A series of related representations of CoFe_(2)O_(4) and Co_(1.5)Fe_(1.5)O_(4) were compared to explore the possible reasons for the outstanding catalytic activity of Co_(1.5)Fe_(1.5)O_(4). Results showed that Co_(1.5)Fe_(1.5)O_(4)as well represented spinel crystal as CoFe_(2)O_(4)and the excess cobalt just partially replaced the position of iron without changing the original structure. Co_(1.5)Fe_(1.5)O_(4) had smaller particle size(8.7 nm), larger specific surface area(126.3 m^(2)/g), which was more favorable for exposure of active sites. Apart from the superior physical properties, more importantly, more reactive centers Co(Ⅱ) and surface hydroxyl compounds generated on Co_(1.5)Fe_(1.5)O_(4), which might be the major reason. Furthermore, Co_(1.5)Fe_(1.5)O_(4) behaved good paramagnetism, wide range of pH suitability and strong resistance to salt interference, making it a new prospect in environmental application.
基金
financially supported by the Key Research and Development(R&D)Projects of Shanxi Province(No.201803D31050)。