Amphichdiral enhancement on singlet oxygen generation and stable thallium immobilization using iron-driven copper oxide

• Published in: Journal of environmental management Vol. 365; p. 121524
• Main Authors: Liu, Zhujun, Dai, Xinning, He, Jun, Lin, Mengyi, Luo, Hongbing, Fan, Liangqian, Zhang, Ke, Ma, Dandan, Wang, Jun, Chen, Wei
• Format: Journal Article
• Language: English
• Published: England Elsevier Ltd 01-08-2024
• Subjects: Iron-doping; Singlet oxygen; Stable immobilization; Thallium; Thallium; Singlet oxygen; Iron-doping; Stable immobilization
• ISSN: 0301-4797; 1095-8630; 1095-8630
• DOI: 10.1016/j.jenvman.2024.121524

Thallium (Tl) as a prominent priority contaminant in aquatic environment necessitates rigorous regulation. However, limited horizon devotes the impact of selective oxidation on the process of thallium purification. In this study, selective active radical of singlet oxygen (1O2) was continually generated for Tl(Ⅰ) oxidation accomplished with efficient Tl(Ⅲ) immobilization using iron-driven copper oxide (CuFe)/peroxymonosulfate (PMS). Fe-doping changed the active center of electronic structure for enhancing the catalytic and adsorptive reactivities, and installed magnetism for solid-liquid separation. Rapid reaction rate (0.253 min−1) coupled with vigorous elimination efficiency (98.32%) relied on electrostatic attraction, surface complexation, and H-bond interaction. EPR and XPS analyses demonstrated that the synergistic effects of ≡ Cu(Ⅰ)/≡Cu(Ⅱ) and ≡ Fe(Ⅲ)/≡Fe(Ⅱ) redounded to the sustained generation of 1O2 through the pathway of PMS → •O2− → 1O2, and 1O2 exploited an advantage to selectively oxidize Tl(Ⅰ) to Tl(Ⅲ). 3D isosurface cubic charts revealed that the immobilizing ability of Tl(Ⅲ) hydrate for CuFe was notably superior to that of Tl(Ⅲ) hydrate for CuO and Tl(Ⅰ) hydrate for CuO/CuFe, which further attested surface reactivity promoted stable immobilization form. This work develops the continuous generation of 1O2 and stable immobilization with the goal of efficiently cleansing Tl-containing wastewater.
[Display omitted]
•The incorporation of Fe improved surface reactivities on catalysis and adsorption.•Selective oxidation for Tl(Ⅰ) occurred in the presence of inorganic ions and humic acid.•1O2 was continuously generated by the circulation of ≡ Cu(Ⅰ/Ⅱ) and ≡ Fe(Ⅲ/Ⅱ).•CuFe/PMS system possessed rapid oxidation rate (0.253 min−1) and removal rate (98.32%).•Tl(H2O)33+ hydrate displayed the highest immobilization property on CuFe.