首页|基于MIL-53(Fe)构建异相UV/H2O2活化体系高效降解水中四氢呋喃

基于MIL-53(Fe)构建异相UV/H2O2活化体系高效降解水中四氢呋喃

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为克服均相光-芬顿体系中pH范围窄、H2O2 活化效率低、Fe2+无法循环使用等缺陷,制备了Fe基MOFs材料MIL-53(Fe)以构建异相H2O2 高效活化体系,并通过XRD、XPS以及UV-vis等表征,以探究MIL-53(Fe)/UV/H2O2 体系去除THF的性能及机理等。降解实验结果表明MIL-53(Fe)/UV/H2O2 体系相比于 UV/H2O2,降解效率提升了 2。4倍,其准一阶降解速率常数(0。0487 min-1)是 UV/H2O2 体系(0。0205 min-1)的2。375倍,并在pH≈6。8(原水),H2O2 添加量为20 mmol·L-1,MIL-53(Fe)投加量为0。1 g·L-1时,降解效果最佳,50 min达到了 94。7%;通过LC-MS分析确定了中间产物,提出了可能的THF降解途径,并利用Gaussian软件通过DFT计算作了验证;从OUR、BOD5/COD、AOS(高级氧化态)、COS(碳氧化态)4方面证明了降解前后溶液可生化性由弱到强的提升;结合活性物种淬灭实验、Fe3+、e-蒙蔽实验以及价导带分析提出了潜在的THF降解机理,验证出·OH是THF降解过程中最重要的活性物种,而光生e-是反应速率提升的主要驱动者。
Efficient degradation of tetrahydrofuran in water by constructing heterogeneous H2O2 activation system based on Fe-based MOFs
To overcome the defects of narrow pH range,low activation efficiency of H2O2 and non-recyclability of Fe2+in homogeneous photo-fenton system,the Fe-based MOFs material MIL-53(Fe)was prepared to construct a heterogeneous and efficient H2O2 activation system,and characterized by XRD,XPS and UV-vis diffuse reflection to investigate the performance and mechanism of THF removal by MIL-53(Fe)/UV/H2O2 system.The degradation experiments results showed that the degradation efficiency of MIL-53(Fe)/UV/H2O2 system was 2.4 times higher than that of UV/H2O2,and its pseudo-first-order degradation rate constant(0.0487 min-1)was 2.375 times higher than that of UV/H2O2 system(0.0205 min-1),the best degradation efficiency was achieved at pH ≈ 6.8(raw water),H2O2 addition of 20 mmol·L-1 and MIL-53(Fe)dosing of 0.1 g·L-1,reaching 94.7%within 50 minutes;the intermediate products were identified by LC-MS analysis and a possible THF degradation pathway was proposed and verified by DFT calculation using Gaussian software;the biodegradability of the solution was improved from weak to strong before and after degradation was demonstrated in four aspects:OUR,BOD5/COD,AOS(Advanced Oxidation State)and COS(Carbon Oxidation State);combined with the active species quenching experiment,blinding experiment of Fe3+,e-and the valence/conduction band analysis,the potential THF degradation mechanism was proposed,which verified that·OH was the most important active species in the THF degradation process,and photogenerated e-was the main driver of the increasment of reaction rate.

tetrahydrofuranMIL-53(Fe)photocatalysisbiodegradabilitydegradation mechanism

邢云青、吴天阳、黄敏轩、冀世锋

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上海海洋大学,海洋生态与环境学院,上海,201306

上海海洋大学,海洋环境监测与评价中心,上海,201306

曼彻斯特大学,英格兰曼彻斯特市,M13 9PL

四氢呋喃 MIL-53(Fe) 光催化 可生化性 降解机理

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D-8006-19-0063

2024

环境化学
中国科学院生态环境研究中心

环境化学

CSTPCD北大核心
影响因子:1.049
ISSN:0254-6108
年,卷(期):2024.43(7)
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