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通过氧空位改善铋掺杂二氧化钛催化活化过一硫酸盐去除难降解有机污染物的新途径。

A novel route for catalytic activation of peroxymonosulfate by oxygen vacancies improved bismuth-doped titania for the removal of recalcitrant organic contaminant.

作者信息

Gul Ikhtiar, Sayed Murtaza, Shah Noor S, Rehman Faiza, Khan Javed Ali, Gul Saman, Bibi Noorina, Iqbal Jibran

机构信息

Radiation Chemistry Laboratory, National Centre of Excellence in Physical Chemistry, University of Peshawar, Peshawar, 25120, Pakistan.

Department of Environmental Sciences, COMSATS University Islamabad, Vehari Campus, Vehari, 61100, Pakistan.

出版信息

Environ Sci Pollut Res Int. 2021 May;28(18):23368-23385. doi: 10.1007/s11356-020-11497-2. Epub 2021 Jan 14.

DOI:10.1007/s11356-020-11497-2
PMID:33443740
Abstract

In this work, bismuth-doped titania (BiTiO) with improved oxygen vacancies was synthesized by sol-gel protocol as a novel peroxymonosulfate (PMS, HSO) activator. HSO and adsorbed oxygen molecules could efficiently be transformed into their respective radicals through defect ionization to attain charge balance after their trapping on oxygen vacancies of the catalyst. XRD study of BiTiO with 5 wt% Bi (5BiT) revealed anatase, crystalline nature, and successful doping of Bi into TiO crystal lattice. The particle size obtained from BET data and SEM observations was in good agreement. PL spectra showed the formation rates of OH by 3BiT, 7BiT, 5BiTC, and 5BiT as 0.720, 1.200, 1.489, and 2.153 μmol/h, respectively. 5BiT catalyst with high surface area (216.87 m g) and high porosity (29.81%) was observed the excellent HSO activator. The catalytic performance of 0BiT, 3BiT, 5BiT, and 7BiT when coupled with 2 mM HSO for recalcitrant flumequine (FLU) removal under dark was 10, 27, 55, and 37%, respectively. Only 5.4% decrease in catalytic efficiency was observed at the end of seventh cyclic run. Radical scavenging studies indicate that SO is the dominant species that caused 62.0% degradation. Moreover, strong interaction between Bi and TiO through Bi-O-Ti bonds prevents Bi leaching (0.081 mg L) as shown by AAS. The kinetics, degradation pathways, ecotoxicity, and catalytic mechanism for recalcitrant FLU were also elucidated. Cost-efficient, environment-friendly, and high mineralization recommends this design strategy; BiTiO/HSO system is a promising advanced oxidation process for the aquatic environment remediation.

摘要

在本研究中,通过溶胶 - 凝胶法合成了具有改善氧空位的铋掺杂二氧化钛(BiTiO)作为新型过一硫酸盐(PMS,HSO)活化剂。HSO和吸附的氧分子在捕获到催化剂的氧空位后,可通过缺陷电离有效地转化为各自的自由基以实现电荷平衡。对含5 wt% Bi的BiTiO(5BiT)进行XRD研究,结果表明其具有锐钛矿型晶体结构,且Bi成功掺杂到TiO晶格中。由BET数据和SEM观察得到的粒径结果吻合良好。PL光谱显示,3BiT、7BiT、5BiTC和5BiT产生·OH的速率分别为0.720、1.200、1.489和2.153 μmol/h。具有高比表面积(216.87 m²/g)和高孔隙率(29.81%)的5BiT催化剂表现出优异的HSO活化性能。0BiT、3BiT、5BiT和7BiT与2 mM HSO耦合在黑暗条件下去除难降解的氟甲喹(FLU)时,催化性能分别为10%、27%、55%和37%。在第七次循环运行结束时,催化效率仅下降了5.4%。自由基清除研究表明,SO₄·⁻是导致62.0%降解的主要物种。此外,如原子吸收光谱(AAS)所示,Bi与TiO之间通过Bi - O - Ti键形成的强相互作用可防止Bi浸出(0.081 mg/L)。还阐明了难降解FLU的动力学、降解途径、生态毒性和催化机理。成本效益高、环境友好且矿化程度高,推荐这种设计策略;BiTiO/HSO体系是一种有前景的用于水环境修复的高级氧化工艺。

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