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构建介孔 Zr 掺杂 SiO2 于高效 Z 型 TiO2/g-C3N4 异质结上,通过吸附-光催化降解抗生素及其机理研究。

Constructing mesoporous Zr-doped SiO onto efficient Z-scheme TiO/g-CN heterojunction for antibiotic degradation via adsorption-photocatalysis and mechanism insight.

机构信息

School of Environment, South China Normal University, University Town, Guangzhou, 510006, China.

Guangdong Provincial Research Center for Environment Pollution Control and Remediation Materials, College of Life Science and Technology, Jinan University, Guangzhou, 510632, China.

出版信息

Environ Res. 2022 Nov;214(Pt 4):114189. doi: 10.1016/j.envres.2022.114189. Epub 2022 Aug 27.

DOI:10.1016/j.envres.2022.114189
PMID:36030911
Abstract

Novel modified-TiO/Zr-doped SiO/g-CN ternary composite is fabricated via an in-situ grow of porous Zr-SiO layer to TiO/g-CN heterojunction, which exhibits well adsorption-photocatalytic performance under simulated solar light irradiation. The nano-size mesoporous TiO are dispersed on the lamellar g-CN, and the Zr-SiO is in-situ fabricated onto the surface of g-CN sheets. The adsorption occurs on the SiO layers, and doping Zr element to SiO enhances the adsorption of pollutants, while the photocatalytic reaction occurs on the valence band (VB) of TiO and conduction band (CB) of g-CN, which gives reactive oxygen species of ∙O, h, and ∙OH for high efficient decomposition of antibiotics, i.e. berberine hydrochloride (98.11%), tetracycline (80.76%), and oxytetracycline (84.84%). The excellent adsorption capacity and Z-scheme photoinduced charge carrier migration behavior endowed the novel material with enhanced berberine hydrochloride (BH) removal in water, which approximately 2.5 and 3.8 folds than that of pure g-CN and sole TiO, respectively. Three degradation pathways are unraveled by LC-MS and theoretical calculations. Furthermore, the toxicity of intermediates was evaluated by the Toxicity Estimation Software Tool (T.E.S.T.), the result demonstrated a good application potential of M-TiO/Zr-SiO/g-CN as an novel adsorptive photocatalyst.

摘要

新型改性 TiO/Zr 掺杂 SiO/g-CN 三元复合光催化剂是通过在 TiO/g-CN 异质结上原位生长多孔 Zr-SiO 层来制备的,在模拟太阳光照射下表现出良好的吸附-光催化性能。纳米级介孔 TiO 分散在层状 g-CN 上,Zr-SiO 原位合成在 g-CN 片表面。吸附发生在 SiO 层上,Zr 元素掺杂到 SiO 中增强了污染物的吸附,而光催化反应发生在 TiO 的价带 (VB) 和 g-CN 的导带 (CB) 上,产生活性氧物种 ∙O、h 和 ∙OH,从而高效分解抗生素,即盐酸小檗碱(98.11%)、四环素(80.76%)和土霉素(84.84%)。优异的吸附能力和 Z 型光诱导电荷载流子迁移行为使新型材料在水中对盐酸小檗碱(BH)的去除率提高了约 2.5 倍和 3.8 倍,分别比纯 g-CN 和纯 TiO 提高了约 2.5 倍和 3.8 倍。通过 LC-MS 和理论计算揭示了三条降解途径。此外,通过毒性估计软件工具(T.E.S.T.)评估了中间体的毒性,结果表明 M-TiO/Zr-SiO/g-CN 作为一种新型吸附光催化剂具有良好的应用潜力。

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