铜掺杂 MIL

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铜掺杂 MIL

2024-07-16 17:23| 来源: 网络整理| 查看: 265

通过Cu掺杂改性制备了双金属有机骨架(MIL-101(Fe/Cu)),并将其用作过硫酸盐(PS)氧化的催化剂,并结合可见光光催化(Vis)降解四环素(TC)。MIL-101(Fe/Cu)/PS/Vis 系统在 Fe 与 Cu 摩尔比为 3:1、pH 5、PS 浓度为 2 mM、催化剂用量为0.05 克/升。MIL-101(Fe/Cu)/PS/Vis 体系中 TC 的降解明显高于 MIL-101(Fe)/PS/Vis 体系(~52.0 %)。通过在 MOF 中掺杂 Cu 来改善光催化和过硫酸盐氧化耦合系统中降解 TC 的原因是(1)更高的吸收能(E abs) 到 PS:基于 DFT 计算的结果,Cu 掺杂的改性 MIL-101(Fe) 可以通过提高 E abs (-5.92 eV) 到 PS 来显着改善 TC 退化;(2)电子-空穴对复合率降低:掺杂Cu可以捕获光生电子,抑制电子-空穴对复合;(3)提高电导率:掺杂Cu通过提高催化剂的态密度(DOS)(1.23电子/eV)来提高电子电导率和催化活性。因此,我们得出结论,Cu掺杂的MOF是提高光催化和过硫酸盐耦合氧化系统中氧化能力的有效方法。

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Improved degradation of tetracycline by Cu-doped MIL-101(Fe) in a coupled photocatalytic and persulfate oxidation system: Efficiency, mechanism, and degradation pathway

A bimetallic organic framework (MIL-101(Fe/Cu)) was fabricated by Cu-doped modification and applied as a catalyst for persulfate (PS) oxidation coupled with visible-light photocatalysis (Vis) to degrade tetracycline (TC). 90.5 % of TC (50 mg/L) was removed by MIL-101(Fe/Cu)/PS/Vis system at Fe to Cu molar ratio of 3:1, pH 5, PS concentration of 2 mM, and catalyst dosage of 0.05 g/L. The degradation of TC was significantly higher in the MIL-101(Fe/Cu)/PS/Vis system than that in the MIL-101(Fe)/PS/Vis system (∼52.0 %). The reasons for the improvement of degrading TC in a coupled photocatalysis and persulfate oxidation system by doping Cu in MOF were (1) the higher absorption energy (Eabs) to PS: based on the results of the DFT calculation, Cu-doped modified MIL-101(Fe) could remarkably improve the TC degradation by enhancing the Eabs (−5.92 eV) to PS; (2) the decrease of the recombination rate of electrons-holes pair: doped Cu could capture the photogenerated electrons to inhibit recombination of electrons-holes pair; (3) the improved electrical conductivity: doped Cu improved electron conductivity and promoted catalytic activity by improving the density of states (DOS) of the catalyst (1.23 electron/eV). Thus, we concluded that Cu-doped MOF is an effective method for improving oxidation ability in a coupled photocatalysis and persulfate oxidation system.



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