Al0-Gr-Fe0活化O2类Fenton氧化降解土霉素的研究

采用高能球磨-高温烧结-液相还原法制备了能活化O₂原位产生H₂O₂/^·OH的新型功能材料（Al⁰-Gr-Fe⁰），通过XRD、SEM、EDS和VSM对Al⁰-Gr-Fe⁰进行了表征，探讨了水中土霉素（OTC）在Al⁰-Gr-Fe⁰/O₂体系中的降解效能和降解途径.结果表明，在初始pH值为6、Al⁰-Gr-Fe⁰投加量为2g/L的条件下反应60min后，OTC和TOC的去除率分别达到100.00%和92.93%.循环使用4次后，Al⁰-Gr-Fe⁰对OTC的去除率仍有79.27%.通过自由基猝灭试验和自由基捕获试验确定了Al⁰-Gr-Fe⁰/O₂体系降解OTC的主要活性物种是^·OH.Al⁰-Gr-Fe⁰/O₂体系对OTC的降解归因于：Al⁰-Gr-Fe⁰高选择性还原O₂为H₂O₂/^·OH；Al⁰-Gr-Fe⁰中的Al⁰还原能促进Fe的循环，从而提高了Fe的催化活性，促进了H₂O₂分解产生^·OH.

Oxidative degradation of oxytetracycline by a Fenton-like process with Al0-Gr-Fe0 activated of O2

Fenton oxidation is an effective method to remove antibiotics from aqueous solution. However, there are main disadvantages in the conventional Fenton system. For example, the inconveniences of transport and storage of H₂O₂, the difficulty of recovering the catalyst, and the acidic pH conditions. To address these issues, this project developed a new functional material novel Fenton-like catalyst (Al⁰-Gr-Fe⁰) capable of activating O₂ to produce H₂O₂/^·OH in situ was prepared by high energy ball milling-high temperature sintering-liquid phase reduction method. The Al⁰-Gr-Fe⁰ could activate O₂ to in-situ produce H₂O₂/^·OH. The Al⁰-Gr-Fe⁰ was characterized by XRD, SEM, EDS and VSM, respectively. The degradation efficiency and degradation pathways of oxytetracycline (OTC) in water by Al⁰-Gr-Fe⁰/O₂ system were discussed explored. The results showed that the removal efficiencies of OTC and total organic carbon (TOC) were 100.00% and 92.93%, respectively, after 60min reaction at the initial pH of 6, and Al⁰-Gr-Fe⁰ dosage of 2g/L and reaction time of 60min, the degradation efficiency of OTC and the removal efficiency of TOC were 100.00% and 92.93%, respectively. After 4cycles, the degradation efficiency of OTC by Al⁰-Gr-Fe⁰ was still decreased to 79.27% after 3 cycles, indicating that Al⁰-Gr-Fe⁰ had a good reusability. It was proved by free radical scavenge experiments and free radical capture experiments that ^·OH was the main active species for OTC degradation in Al⁰-Gr-Fe⁰/O₂ system was determined to be ^·OH by free radical quenching and capture tests. The excellent degradation mechanism ability of OTC degradation by Al0-Gr-Fe0/O₂ system for OTC was attributed to that Al⁰-Gr-Fe⁰ the O₂ could be selectively reduced O₂ into H₂O₂/^·OH; by Al⁰-Gr-Fe⁰ and the reduction of Al⁰ in Al⁰-Gr-Fe⁰ could promote Fe cyclinge, thereby effectively improving the catalytic performance activity of Fe and promoting the decomposition of H₂O₂ to produce ^·OH.