An electron transfer tuning strategy for the efficient degradation of tetracycline hydrochloride by Fe-N co-doped carbon materials activated with peroxymonosulfate
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING(2023)
摘要
In order to address the problems of metal leaching and low electron transfer efficiency, the iron (Fe) nitrogen (N) co-doped MOFs derived carbon catalysts presented a promising strategy to activate peroxymonosulfate (PMS) for water purification. In this work, using the MOF-5 as a template and iron phthalocyanine (FePc) and dicyandiamide (DCD) as a source, Fe, N co-doped carbons were prepared through milling and two-step pyrolysis. The catalytic performance and mechanism of the materials on tetracycline hydrochloride (TC) degradation in the PMS activation system (0.1Fe/N-CPMS) was systematically investigated. The results showed that the stable framework structure of MOFs-derived carbon conduced to encapsulate the Fe nanoparticles within the carbon skeleton, and then the xFe/N-C catalyst with hierarchical pore structure and good electrical conductivity was obtained, which significantly improved the TC catalytic performance. Notably, the 0.1Fe/N-C exhibited the greatest degradation performance achieving a degradation rate of 0.6315 min-1, which was approximately five times higher than that of N-C. Moreover, the degradation performance of the 0.1Fe/N-C kept the stability in various interference conditions, and still remained over 80% after three cycles test. Combine with the characterization and DFT calculation, the mechanism of the TC degradation in 0.1Fe/N-CPMS system was revealed by a non-radical process dominated by electron transfer, and the degradation efficiency was greatly improved by the synergistic effect of Fe/N on the as-prepared material. The received findings provide an electron transfer tuning strategy of Fe/N co-doped carbon nanomaterials synthesis for promoting the non-radical degradation pathways in the application of organic pollutants removal.
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关键词
Fe-N co-doped,MOFs-derived carbon,Encapsulate,Electron transfer,Degradation efficiency
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