Comparison of phenacetin degradation in aqueous solutions by catalytic ozonation with CuFe2O4 and its precursor: Surface properties, intermediates and reaction mechanisms

Comparison of phenacetin degradation in aqueous solutions by catalytic ozonation with CuFe2O4 and its precursor: Surface properties, intermediates and reaction mechanisms
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CuFe2O4 及其前驱体催化臭氧降解水溶液中非那西丁的比较:表面性质、中间体和反应机制

DOI:
10.1016/j.cej.2015.07.095
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发表时间:
2016-01
影响因子:
15.1
通讯作者:
Xu Bingbing
Xu Bingbing
中科院分区:
工程技术1区
文献类型:
--
作者:
Qi Fei;Chu Wei;Xu Bingbing

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本研究以CuFe2O4(CFO)为前驱体,采用一种新型的强化臭氧氧化的磁性催化剂CFOH来强化臭氧氧化。比较了CFO和CFOH在催化臭氧氧化中的表面性质、性能和反应机理。与CFO相比,CFOH具有更高的比表面积、孔容和更强的酸性中心。重要的是,CFOH和CFO都表现出磁化作用,可以用来将催化剂从本体溶液中分离出来,以便重复使用。此外,在CFOH催化臭氧氧化过程中,非那西丁(PNT)的降解和矿化速度更快。在研究过程中发现了中间体和H_2O_2的产生/衰变。反应中过氧化氢的产率和分解速率决定了自由基DOTOH的浓度,这是CFOH具有较好催化活性的关键。此外,还考察了苯环和开环中间体在反应过程中的去向。对于PNT氧化生成的中间产物的矿化,观察了表面反应,包括表面吸附和催化反应。当使用CFOH作为催化剂时,这些表面反应更加明显,说明CFOH具有更好的矿化能力。
In this study, a new magnetic catalyst for enhancing the ozonation process, named as CFOH, a precursor of CuFe2O4(CFO) was used to enhance the ozonation. The comparison of the surface properties, performance, and reaction mechanisms of CFO and CFOH in catalytic ozonation was investigated. The CFOH showed higher surface area, pore volume, and stronger acidic sites than those of CFO. Importantly, both CFOH and CFO exhibited magnetization, which can be used to separate the catalysts from the bulk solution for reuse. In addition, faster degradation and mineralization of phenacetin (PNT) in catalytic ozonation by CFOH were observed. The generation/decay of intermediates and H2O2were identified in the studied processes. The yield and decomposition rate of H2O2in the reaction determined the concentration ofradical dotOH, which was found to be the key for the better catalytic activity of CFOH. Furthermore, the fates of benzene- and open-ring intermediates in the processes were also investigated. The surface reactions, including surface adsorption and catalytic reaction were observed for the mineralization of intermediates generated from PNT oxidation. These surface reactions became more significant when using CFOH as the catalyst, which justifies the better mineralization ability of CFOH.
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