Separation and Purification Technology ( IF 8.6 ) Pub Date : 2021-12-29 , DOI: 10.1016/j.seppur.2021.120409 Haoyun Chen 1, 2 , Xingzhong Yuan 1, 2 , Longbo Jiang 1, 2, 3 , Hou Wang 1, 2 , Guanjun Zeng 4
It has been ever attracting increasingly growing demand to develop highly efficient method of aqueous arsenites [As(III)] removal due to the high toxicity of arsenic in drinking water. This work presents an oil vine-like structural MIL-53(Fe) modified by nitrogen doped carbon quantum dots (N-CQDs) with excellent As(III) removal property, which is achieved through the photocatalytic oxidation of the As(III) and simultaneous adsorbed the generated arsenate [As(V)]. The abilities of As(III) oxidation and removal efficiency for N-CQDs3/MIL-53(Fe) are over 6 times higher than that of pure MIL-53(Fe). The impressively capability of N-CQDs3/MIL-53(Fe) in photocatalytic oxidation and adsorption is attributed to the accelerated separation of photogenerated electron-hole by the in situ embedded N-CQDs. Moreover, the results of the experimental analysis and density functional theory (DFT) DFT calculations confirm that the edge structure of C/O site significantly improves the removal ability of As(III) by forming bidentate C-O-As bonds and occupying coordinatively unsaturated atoms. Therefore, based on the excellent performance and reusability of N-CQDs3/MIL-53(Fe) in As(III) removal, it offers a new potential strategy to develop high efficient MOF based materials for As(III) removal.
中文翻译:
通过 N-CQD 改性的 MIL-53(Fe) 同时氧化和吸附高效去除 As(III)
由于饮用水中砷的高毒性,开发高效去除水性亚砷酸盐 [As(III)] 的方法一直吸引着日益增长的需求。这项工作提出了一种油藤状结构 MIL-53(Fe),由氮掺杂碳量子点 (N-CQDs) 改性,具有优异的 As(III) 去除性能,这是通过 As(III) 的光催化氧化和同时吸附生成的砷酸盐 [As(V)]。N-CQDs3/MIL-53(Fe)的As(III)氧化能力和去除效率是纯MIL-53(Fe)的6倍以上。N-CQDs3/MIL-53(Fe) 在光催化氧化和吸附方面的出色能力归因于原位嵌入的 N-CQD 加速了光生电子空穴的分离。而且,实验分析和密度泛函理论(DFT)DFT计算的结果证实,C/O位点的边缘结构通过形成双齿CO-As键并占据配位不饱和原子,显着提高了As(III)的去除能力。因此,基于 N-CQDs3/MIL-53(Fe) 在 As(III) 去除方面的优异性能和可重复使用性,它为开发用于去除 As(III) 的高效 MOF 基材料提供了新的潜在策略。