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使用 TiO-P25 和 N/S 掺杂 TiO 催化剂进行光催化去除氟尿嘧啶:动力学和机理研究。

Photocatalytical removal of fluorouracil using TiO-P25 and N/S doped TiO catalysts: A kinetic and mechanistic study.

机构信息

Department of Chemistry, Aristotle University of Thessaloniki, 54124 Thessaloniki, Greece.

Department of Environmental and Natural Resources Management, University of Patras, 30100 Agrinio, Greece.

出版信息

Sci Total Environ. 2017 Feb 1;578:257-267. doi: 10.1016/j.scitotenv.2016.08.208. Epub 2016 Nov 14.

Abstract

In the present study, the photocatalytic activity of TiO-based photocatalysts toward degradation and mineralization of the anti-cancer drug 5-fluorouracil (5-FU) in aqueous phase was investigated under simulated solar and visible irradiation. Commercial TiO (P25) and N/S-doped TiO catalysts synthesized by a simple sol-gel method were used as photocatalysts. TiO P-25 was found to be the most photoactive catalyst for the removal of 5-FU, under simulated solar irradiation. Among N/S-doped TiO catalysts, the one with molar Ti:N/S ratio equal to 0.5 was the most efficient under simulated solar irradiation. In contrast, under visible irradiation the catalyst with equimolar Ti:N/S ratio showed the highest performance for the removal of 5-FU. Scavenging experiments revealed that HO radicals and h were the major reactive species mediating photocatalytic degradation of 5-FU using TiO P-25 and N/S-doped TiO catalysts, under simulated solar irradiation. On the other hand, the essential contribution of O and O in the degradation of 5-FU under visible light was proved. The transformation products (TPs) of 5-FU, were identified by LC-MS-TOF suggesting that defluorination followed by hydroxylation and oxidation are the main transformation pathways, under all the studied photocatalytic systems.

摘要

在本研究中,研究了在模拟太阳光和可见光照射下,基于 TiO 的光催化剂对水溶液中抗癌药物 5-氟尿嘧啶(5-FU)的降解和矿化的光催化活性。使用商业 TiO(P25)和通过简单的溶胶-凝胶法合成的 N/S 掺杂 TiO 催化剂作为光催化剂。在模拟太阳光照射下,TiO P-25 被发现是去除 5-FU 的最活跃的催化剂。在 N/S 掺杂的 TiO 催化剂中,摩尔比 Ti:N/S 等于 0.5 的催化剂在模拟太阳光照射下的效率最高。相比之下,在可见光照射下,具有等摩尔 Ti:N/S 比的催化剂对于去除 5-FU 表现出最高的性能。猝灭实验表明,在模拟太阳光照射下,HO 自由基和 h 是 TiO P-25 和 N/S 掺杂 TiO 催化剂光催化降解 5-FU 的主要活性物质。另一方面,证明了在可见光下 O 和 O 在 5-FU 降解中的重要贡献。通过 LC-MS-TOF 鉴定了 5-FU 的转化产物(TPs),表明在所有研究的光催化体系中,脱氟后羟化和氧化是主要的转化途径。

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