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Regulating superoxide radicals and light absorption ability for enhancing photocatalytic performance of MoS2@Z by CeO2 rich in adsorbed oxygen
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
Affiliation  

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。

更新日期:2021-09-20
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