Geng Chuanhui, Chen Qingguo, Li Zhenzhen, Liu Mei, Chen Zhi, Tao Hengcong, Yang Qiao, Zhu Baikang, Feng Lijuan
Zhejiang Key Laboratory of Petrochemical Environmental Pollution, Zhejiang Ocean University, Zhoushan, 316022, PR China; School of Naval Architecture and Maritime, Zhejiang Ocean University, Zhoushan, 316022, PR China.
Zhejiang Key Laboratory of Petrochemical Environmental Pollution, Zhejiang Ocean University, Zhoushan, 316022, PR China; National & Local Joint Engineering Research Center of Harbor Oil & Gas Storage and Transportation Technology, Zhejiang Ocean University, Zhoushan, 316022, PR China.
Environ Res. 2023 Nov 15;237(Pt 2):116960. doi: 10.1016/j.envres.2023.116960. Epub 2023 Aug 23.
In this study, we investigated the doping of Fe-N-C with ZnO (Fe-N-C@ZnO) to enhance its performance in the reduction of biological toxicity and degradation of enrofloxacin (ENR) in seawater. The steady-state/transient fluorescence analysis and free radical quenching test indicated an extremely low electron-hole recombination rate and the generation of reactive oxygen species in Fe-N-C@ZnO, leading to an improvement in the energy efficiency. We compared the ENR degradation efficiencies of Fe-N-C@ZnO and ZnO using both freshwater and seawater. In freshwater, Fe-N-C@ZnO exhibited a slightly higher degradation efficiency (95.00%) than ZnO (90.30%). However, the performance of Fe-N-C@ZnO was significantly improved in seawater compared to that of ZnO. The ENR degradation efficiency of Fe-N-C@ZnO (58.87%) in seawater was 68.39% higher than that of ZnO (34.96%). Furthermore, the reaction rate constant for ENR degradation by Fe-N-C@ZnO in seawater (7.31 × 10 min) was more than twice that of ZnO (3.58 × 10 min). Response surface analysis showed that the optimal reaction conditions were a pH of 7.42, a photocatalyst amount of 1.26 g L, and an initial ENR concentration of 6.56 mg L. Fe-N-C@ZnO prepared at a hydrothermal temperature of 128 °C and heating temperature of 300 °C exhibited the optimal performance for the photocatalytic degradation of ENR. Based on liquid chromatography-mass spectrometry analysis, the degradation processes of ENR were proposed as three pathways: two piperazine routes and one quinolone route.
在本研究中，我们研究了用氧化锌（Fe-N-C@ZnO）对Fe-N-C进行掺杂，以提高其在降低生物毒性和降解海水中恩诺沙星（ENR）方面的性能。稳态/瞬态荧光分析和自由基猝灭试验表明，Fe-N-C@ZnO中电子-空穴复合率极低，并产生了活性氧物种，从而提高了能量效率。我们比较了Fe-N-C@ZnO和ZnO在淡水和海水中对ENR的降解效率。在淡水中，Fe-N-C@ZnO的降解效率（95.00%）略高于ZnO（90.30%）。然而，与ZnO相比，Fe-N-C@ZnO在海水中的性能有显著提高。Fe-N-C@ZnO在海水中的ENR降解效率（58.87%）比ZnO（34.96%）高68.39%。此外，Fe-N-C@ZnO在海水中降解ENR的反应速率常数（7.31×10⁻³ min⁻¹）是ZnO（3.58×10⁻³ min⁻¹）的两倍多。响应面分析表明，最佳反应条件为pH值7.42、光催化剂用量1.26 g·L⁻¹、初始ENR浓度6.56 mg·L⁻¹。在128℃水热温度和300℃加热温度下制备的Fe-N-C@ZnO对ENR的光催化降解表现出最佳性能。基于液相色谱-质谱分析，提出了ENR的降解过程为三条途径：两条哌嗪途径和一条喹诺酮途径。
