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Ce-N 共掺杂 AC/TiO2 光催化剂增强四环素的吸附-光降解:等温线、动力学、机制和热力学研究。

Enhanced adsorption-photodegradation of tetracycline using Ce-N-co-doped AC/TiO photocatalyst: isotherms, kinetics, mechanism, and thermodynamic insight.

机构信息

Faculty of Chemical Engineering & Technology, Universiti Malaysia Perlis (UniMAP), 02600, Arau, Perlis, Malaysia.

Faculty of Mechanical Engineering & Technology, Universiti Malaysia Perlis (UniMAP), 02600, Arau , Perlis, Malaysia.

出版信息

Environ Sci Pollut Res Int. 2024 Oct;31(49):59398-59415. doi: 10.1007/s11356-024-34948-6. Epub 2024 Oct 1.

Abstract

Excessive use of tetracycline (TC) is alarming owing to its increased detection in water systems. In this study, a photocatalyst was developed to degrade TC using a Ce-N-co-doped AC/TiO photocatalyst, denoted as Ce/N-AC/TiO, prepared using the sol-gel method assisted by microwave radiation, speeding up the synthesis process. Ce/N-AC/TiO achieved maximum TC degradation of 93.1% under UV light with optimum sorption system conditions of an initial concentration of 10 mg L, pH 7, and 30 ℃, under 120 min. Scavenger experiments revealed that holes and superoxide radicals were the active species influencing the photodegradation process. The TC degradation was appropriately fitted with Langmuir isotherms and a pseudo-second-order (PSO) kinetic model. The change in enthalpy (ΔH) (2.43 kJ mol), entropy (ΔS) (0.024 kJ mol), and Gibbs free energy (ΔG) (- 4.941 to - 5.802 kJ mol) suggested that the adsorption process was spontaneous, favourable, and endothermic. Electrostatic interaction, hydrogen bonding, pore-filling, cationic-π, n-π, and π-π interaction were among the interactions involved between TC and Ce/N-AC/TiO. Furthermore, Ce/N-AC/TiO stability was confirmed through 80% removal efficiency even after the fifth reuse cycle. Notably, this work provides new insight into the production of efficient, reusable, and enhanced photocatalysts using a rapid and cost-effective microwave-assisted synthesis process for pollutant remediation.

摘要

由于四环素(TC)在水系中的检出率增加,其过度使用令人担忧。在这项研究中,开发了一种光催化剂,使用 Ce-N 共掺杂 AC/TiO 光催化剂(Ce/N-AC/TiO)降解 TC,Ce/N-AC/TiO 是通过溶胶-凝胶法和微波辐射辅助制备的,加速了合成过程。Ce/N-AC/TiO 在 UV 光下,在最佳吸附体系条件下,初始浓度为 10 mg/L、pH 值为 7 和 30℃,在 120 min 内实现了最大的 TC 降解率 93.1%。猝灭实验表明,空穴和超氧自由基是影响光降解过程的活性物质。TC 降解与 Langmuir 等温线和拟二级动力学模型(PSO)拟合良好。焓变(ΔH)(2.43 kJ/mol)、熵变(ΔS)(0.024 kJ/mol)和吉布斯自由能变(ΔG)(-4.941 至-5.802 kJ/mol)表明吸附过程是自发、有利和吸热的。TC 和 Ce/N-AC/TiO 之间涉及的相互作用包括静电相互作用、氢键、孔填充、阳离子-π、n-π 和 π-π 相互作用。此外,即使经过第五次重复使用循环,Ce/N-AC/TiO 的去除效率仍保持在 80%,从而证实了其稳定性。值得注意的是,这项工作为使用快速且具有成本效益的微波辅助合成工艺生产高效、可重复使用和增强的光催化剂以修复污染物提供了新的思路。

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