<br>用于光驱动水污染物降解的 UiO(Zr) 基 MOF 催化剂,Reaction Chemistry & Engineering

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用于光驱动水污染物降解的 UiO(Zr) 基 MOF 催化剂
Reaction Chemistry & Engineering ( IF 3.4 ) Pub Date : 2024-06-12 , DOI: 10.1039/d4re00172a
Samuel C. Moore ₁ , Isabella L. Hubble ₂ , Alyssa L. Ritchie ₂ , Jeffrey E. Barzach ₂ , Michele L. Sarazen _{1,

2}

Affiliation

研究了等网状晶体形态和对比孔径的羧酸锆金属有机框架 (MOF)，以了解连接体尺寸（UiO-67 与 UiO-68）和二次金属掺入对光催化水污染物降解的相对影响。这里选择铁 (Fe) 是因为铁 (Fe) 毒性低且能够激活良性氧化剂，因此在废水处理文献和应用中广泛使用。通过初湿浸渍掺入 Fe 的 UiO-67 (Fe-UiO-67) 表现出相对于 UiO-67 母体的带隙能量降低，并且在紫外光下使用过氧化氢 (H ₂ )，催化剂质量标准化准一级速率常数为 6.8 ± 0.5 g ⁻¹ ks ⁻¹ 和 2.0 ± 0.3 g <分别为 b4> ks ⁻¹ 。虽然通过 X 射线衍射进行的结构表征在反应前后 Fe-UiO-67 保持不变，但如滤液中的补给实验所示，一些 Fe 浸出是明显的。合成的 UiO-68 孔径增大，带隙能量降低，从而比 UiO-67 具有更高的紫外光活化能力（伪一级速率常数为 3.5 ± 0.4 g ⁻¹ ks ⁻¹ ）。此外，UiO-68 表现出高稳定性，并表现出比任一 UiO-67 催化剂更高的 H ₂ O ₂ 利用率。总之，这项工作阐明了 UiO-MOF 中连接基调制和活性金属掺入对污染物降解和广泛的水应用的相对影响。

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UiO(Zr)-based MOF catalysts for light-driven aqueous pollutant degradation

Zirconium-carboxylate metal–organic frameworks (MOFs) of isoreticular crystal morphologies and contrasting pore sizes are examined to understand the relative influence of linker size (UiO-67 vs. UiO-68) and secondary metal incorporation in photocatalytic aqueous pollutant degradation. Here, iron (Fe) is chosen given its prevalence in wastewater treatment literature and applications, resulting from its low toxicity and ability to activate benign oxidants. UiO-67 with Fe incorporated (Fe-UiO-67) via incipient wetness impregnation demonstrates reduced band gap energy relative to the UiO-67 parent and higher apparent photocatalytic degradation under UV light toward methylene blue dye using hydrogen peroxide (H₂O₂), with catalyst mass-normalized pseudo-first order rate constants of 6.8 ± 0.5 g⁻¹ ks⁻¹ and 2.0 ± 0.3 g⁻¹ ks⁻¹, respectively. While structural characterization via X-ray diffraction remains unperturbed for Fe-UiO-67 before and after reaction, some Fe leaching is evident, as indicated by recharge experiments in the filtrate. Synthesized UiO-68, which possesses increased pore size, also has reduced band gap energy resulting in higher UV-light activation than UiO-67 (pseudo-first order rate constant of 3.5 ± 0.4 g⁻¹ ks⁻¹). Further, UiO-68 demonstrates high stability and exhibits a higher productive H₂O₂ utilization fraction than either of the UiO-67 catalysts. Together, this work clarifies the relative influence of linker modulation and active metal incorporation in UiO-MOFs for pollutant degradation and aqueous applications broadly.

更新日期：2024-06-12

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