Journal of Cleaner Production ( IF 9.7 ) Pub Date : 2021-09-16 , DOI: 10.1016/j.jclepro.2021.129059 Junfei Liu 1, 2 , Yingbo Dong 1, 2 , Liping Zhang 1, 2 , Wei Liu 1, 2 , Conghui Zhang 1, 2 , Yuanyuan Shi 3 , Hai Lin 1, 2
Nano molybdenum disulfide (Nano-MoS2) can be as a photocatalyst for antibiotic removal under visible light. However, the low energy of visible light and limited radicals restrict the applications of nano-MoS2. In this study, ceria dioxide (CeO2) rich in adsorbed oxygen was introduced into MoS2@Z (MoS2@Zeolite) to synthesize full-spectrum CeO2/MoS2@Z photocatalysts (CeO2/MoS2@Zs). The CeO2/MoS2@Z-3 (Ce: 1.5 mmol; Mo: 3.5 mmol) shows the best photocatalytic ability (98.32%) for tetracycline within 150 min, which is 18.20% improvement over MoS2@Z. The UV–vis diffuse reflection spectra of photocatalysts shows that the ultraviolet absorption ability of CeO2/MoS2@Z-3 improved when CeO2 was introduced. The active species trapping experiment and electron paramagnetic resonance (EPR) test prove h+ and superoxide radicals (•O2−) are the main active species, and CeO2 rich in adsorbed oxygen improves the amounts of •O2− in photocatalytic process. Moreover, singlet oxygen (1O2), producing by oxygen vacancies of CeO2, also plays an important role. The enhanced photocatalytic activity is attributed to full-spectrum (200 nm–800 nm) absorption performance, improved content of •O2−, and electron-hole (e−/h+) pairs separation. After five times recycle, the photodegradation efficiency of CeO2/MoS2@Z-3 only decreased by 2.59%. Meantime, the proposed three photocatalytic pathways show that tetracycline eventually degraded into small organics (like C5H8O3), H2O and CO2 by dehydration, demethylation, deamination, dihydroxylation, deamidation, ring-opening reaction and carbonylation. The results show that CeO2/MoS2@Z-3 may become a high efficiency, stable, and promising photocatalyst for tetracycline wastewater treatment.
中文翻译:
调节超氧自由基和光吸收能力以提高富含吸附氧的 CeO2 对 MoS2@Z 的光催化性能
纳米二硫化钼(Nano-MoS 2)可作为光催化剂在可见光下去除抗生素。然而,可见光的低能量和有限的自由基限制了纳米MoS 2的应用。在本研究中,将富含吸附氧的二氧化铈 (CeO 2 ) 引入 MoS 2 @Z (MoS 2 @Zeolite) 以合成全光谱 CeO 2 /MoS 2 @Z 光催化剂 (CeO 2 /MoS 2 @Zs)。CeO 2 /MoS 2 @Z-3(Ce:1.5 mmol;Mo:3.5 mmol)在150分钟内对四环素表现出最佳的光催化能力(98.32%),比MoS 2提高了18.20%@Z。光催化剂的紫外-可见漫反射光谱表明,当引入CeO 2时,CeO 2 /MoS 2 @Z-3的紫外吸收能力提高。活性物质捕获实验和电子顺磁共振(EPR)测试证明h +和超氧自由基(•O 2 -)是主要的活性物质,富含吸附氧的CeO 2提高了光催化过程中•O 2 -的量。此外,单线态氧 ( 1 O 2 ),由 CeO 2 的氧空位产生,也起着重要的作用。增强的光催化活性归因于全光谱 (200 nm–800 nm) 吸收性能、改进的 •O 2 -含量和电子-空穴 (e - /h + ) 对分离。循环五次后,CeO 2 /MoS 2 @Z-3的光降解效率仅下降2.59%。同时,提出的三种光催化途径表明四环素最终降解为小的有机物(如 C 5 H 8 O 3)、H 2 O 和 CO 2通过脱水、脱甲基、脱氨基、二羟基化、脱酰胺、开环反应和羰基化。结果表明,CeO 2 /MoS 2 @Z-3 可能成为一种高效、稳定、有前景的四环素废水处理光催化剂。