Removal of Ampicillin by Heterogeneous Photocatalysis: Combined Experimental and DFT Study

被引:14
作者
Belhacova, LenkaY [1 ]
Bibova, Hana [1 ]
Marikova, Tereza [2 ,3 ]
Kuchar, Martin [3 ]
Zouzelka, Radek [2 ]
Rathousky, Jiri [2 ]
机构
[1] J Heyrovsky Inst Phys Chem, CAS, Dept Electrochem Mat, Dolejskova 3, Prague 18223, Czech Republic
[2] J Heyrovsky Inst Phys Chem, CAS, Ctr Innovat Field Nanomat & Nanotechnol, Dolejskova 3, Prague 18223, Czech Republic
[3] Univ Chem & Technol Prague, Dept Chem Nat Cpds, Forens Lab Biologically Active Subst, Technicka 3, Prague 16628, Czech Republic
关键词
water treatment; photocatalysis; TiO2; DFT; ampicillin; antibiotics; ANTIBIOTIC-RESISTANT BACTERIA; WATER TREATMENT PLANTS; DEGRADATION; OXIDATION; GENES; AMOXICILLIN;
D O I
10.3390/nano11081992
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A long-term exposition of antibiotics represents a serious problem for the environment, especially for human health. Heterogeneous photocatalysis opens a green way for their removal. Here, we correlated the structural-textural properties of TiO2 photocatalysts with their photocatalytic performance in ampicillin abatement. The tested nanoparticles included anatase and rutile and their defined mixtures. The nominal size range varied from 5 to 800 nm, Aeroxide P25 serving as an industrial benchmark reference. The degradation mechanism of photocatalytic ampicillin abatement was studied by employing both experimental (UPLC/MS/MS, hydroxyl radical scavenger) and theoretical (quantum calculations) approaches. Photocatalytic activity increased with the increasing particle size, generally, anatase being more active than rutile. Interestingly, in the dark, the ampicillin concentration decreased as well, especially in the presence of very small nanoparticles. Even if the photolysis of ampicillin was negligible, a very high degree of mineralization of antibiotic was achieved photocatalytically using the smallest nanoparticles of both allotropes and their mixtures. Furthermore, for anatase samples, the reaction rate constant increases with increasing crystallite size, while the degree of mineralization decreases. Importantly, the suggested degradation pathway mechanism determined by DFT modeling was in very good agreement with experimentally detected reaction products.
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页数:13
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