Photogenerated carrier-accelerated 3D mesh-NH2 functionalized Zr-metal organic framework/MgAl-type hydrotalcite composites attacking diclofenac

• Published in: Separation and purification technology 2025-02, Vol.354, p.128839, Article 128839
• Main Authors: Wang, Jia-Hang, Kong, Fanying, Liu, Bing-Feng, Zhuo, Sheng-Nan, Ren, Nan-Qi, Ren, Hong-Yu
• Format: Article
• Language: English
• Subjects: Diclofenac; Layered double hydroxides (LDH); NH2 functionalized Zr-MOF (UiO-66-NH2); One-step thermal synthesis; Photocatalytic
• ISSN: 1383-5866
• DOI: 10.1016/j.seppur.2024.128839

[Display omitted] •∼100 % of diclofenac degradation was achieved within 1 min over the optimal system.•Fine robustness of photocatalyst was demonstrated in various environments.•The photocatalyst under light facilitated the separation of electron-hole pairs.•Immediate products and degradation pathways of diclofenac were elucidated. Developing efficient photocatalysts for high-concentration pharmaceutically active compounds (PhACs) removal in aquatic environments holds immense promise. Metal-organic frameworks (MOF) and layered double hydroxides (LDH), with their metal ions and electron transfer properties, emerge as promising candidates for advanced degradation. The three-dimensional UiO-66-NH2/MgAl-LDH3 (UNL3) composites used in this work exhibited excellent thermal stability and reduced crystallinity. Under optimized conditions, the UNL3/DCF system achieved nearly 100 % DCF degradation in 1 min. Notably, this outstanding photocatalytic activity persisted, maintaining a 90 % DCF removal rate across a pH range of 2–12, even after five cycles. The total organic carbon concentration rapidly halved within 3 min of the initial reaction. Leveraging UNL3′s benign chemical stability (with ion leaching below 0.4 mg/L) and excellent optical properties, photogenerated charges enhanced charge separation and transport, generating ample reactive species (h+) under visible light. This study introduces a novel strategy for designing robust, stable, and environmentally friendly UiO-66-NH2-based photocatalysts for chlorinated PhAC pollutants removal.