| 铁铜双金属有机骨架MIL-101(Fe,Cu)活化双氧水降解染料性能 |
| 摘要点击 1535 全文点击 668 投稿时间：2020-03-03 修订日期：2020-04-23 |
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| 中文关键词 MIL-101(Fe,Cu) 类芬顿 双金属 羟基自由基(·OH) 染料废水 |
| 英文关键词 MIL-101(Fe,Cu) Fenton-like reaction bimetallic synergy hydroxyl radical (·OH) dye wastewater |
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| 中文摘要 |
| 针对非均相芬顿传质效率低和Fe（Ⅲ）Fe（Ⅱ）转化慢导致活性低等问题，采用溶剂热法制备铁铜双金属有机骨架材料[MIL-101（Fe，Cu）]，并研究了材料界面性质、催化降解染料（亚甲基蓝）性能以及活化催化机制.结果表明，MIL-101（Fe，Cu）晶体结构完整且呈三维八面体形状；比表面积和平均孔径分别为667.2 m2 ·g-1和1.9 nm，可充分暴露反应活性位点.MIL-101（Fe，Cu）在广谱pH范围可活化H2 O2高效降解亚甲基蓝.当pH=5、反应20 min，MIL-101（Fe，Cu）/H2 O2对20 mg ·L-1亚甲基蓝的去除率为100%，较MIL-101（Fe）/H2O2和单独H2 O2分别提高43.1%和88.9%.自由基猝灭实验与反应前后铁和铜价态变化结果表明，羟基自由基（·OH）是MIL-101（Fe，Cu）/H2 O2催化降解亚甲基蓝的主要活性物种；Cu（Ⅱ）掺杂引入新的活性位点，且Cu（Ⅱ）/Cu（Ⅰ）循环和Fe（Ⅲ）/Fe（Ⅱ）循环可协同产生·OH，进而提高催化效率.MIL-101（Fe，Cu）作为新型非均相类芬顿催化剂，无需复杂pH调节即可获得良好催化效果，在工业废水处理上具有较好地应用前景. |
| 英文摘要 |
| Practical use of heterogeneous Fenton-like catalysis is inhibited by poor mass transfer and slow conversion of Fe(Ⅲ) to Fe(Ⅱ). In this study, we prepared a novel iron-copper bimetallic organic framework (MIL-101 (Fe,Cu)) using the solvothermal method, and carefully investigated its interfacial characters, catalytic efficacy toward dyes with methylene blue as a model pollutant, and the catalytic activating mechanisms involved in it. The MIL-101(Fe,Cu) exhibited a three-dimensional octahedral shape with a complete crystal structure. The specific BET surface area and average pore size were determined to be as high as 667.2 m2 ·g-1 and 1.9 nm, respectively. These characteristics benefits the exposure of the reactive sites and accelerates mass transfer accordingly. The MIL-101(Fe,Cu)/H2 O2 exhibited promising efficiency toward the degradation of methylene blue in a wide pH range; moreover, at a pH value of 5, the removal efficiency observed was as high as 100% after 20 min of reaction, which was 43.1% and 88.9% higher than that of MIL-101(Fe)/H2 O2 and H2 O2, respectively. Hydroxyl radical ( ·OH) is a dominant active species involved in the degradation of methylene blue using MIL-101(Fe,Cu)/H2 O2 as indicated in radicals quenching experiments. The results of species transformation in Fe and Cu indicated that Cu(Ⅱ) doping provided more active sites, and the Cu(Ⅱ)/Cu(Ⅰ) and Fe(Ⅲ)/Fe(Ⅱ) cycles synergistically facilitated ·OH generation to improve the Fenton-like catalytic efficiency accordingly. The MIL-101(Fe,Cu) as a novel heterogeneous Fenton-like catalyst achieved good performance without any significant pH adjustment and is practically viable for industrial wastewater treatment. |
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