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H2O2 activation by two-dimensional metal-organic frameworks with different metal nodes for micropollutants degradation: Metal dependence of boosting reactive oxygen species generation
Journal of Hazardous Materials ( IF 13.6 ) Pub Date : 2022-08-11 , DOI: 10.1016/j.jhazmat.2022.129757
Xuheng Li 1 , Xiang Li 1 , Bo Wang 1
Affiliation  

The existence of organic micropollutants (OPMs) in water poses a considerable threat to the environment. A centralized approach towards pollutants abatement has dominated over the recent decades wherein heterogeneous Fenton-like based advanced oxidation processes can be a promising technology. The application of engineered nanomaterials offers more opportunities to enhance their catalyst properties. This study synthesizes a series of ultrathin two-dimensional (2D) Metal-organic frameworks (MOFs) nanosheets with tunable metal clusters. The formation of reactive oxygen species (OH and 1O2) can be significantly boosted via transferring the adsorbed H2O2 onto the solid-liquid interface by systematically tuning the metal species. The Co-MOF nanosheets exhibited an ultrafast degradation kinetic for BPA with a rate of 2.23 min−1 (4.98 times higher than that of the bulk MOF) and TOF (turnover frequency) value of 9.99 min−1, which are observably greater than that of the existing materials reported to date. Density functional theory simulation and experimental results unravel the mechanism for ROS formation, which is strongly metal-depend. We further loaded the powder onto a flow-through poly (vinylidene fluoride) (PVDF) microfiltration membrane and observed that the representative OPMs could be rapidly degraded, indicating promising properties for practical application.



中文翻译:

具有不同金属节点的二维金属-有机骨架对微污染物降解的 H2O2 活化:促进活性氧生成的金属依赖性

水中有机微污染物(OPM)的存在对环境构成了相当大的威胁。近几十年来,集中式减少污染物的方法占主导地位,其中基于异质类芬顿的高级氧化工艺可能是一种有前途的技术。工程纳米材料的应用为增强其催化剂性能提供了更多机会。本研究合成了一系列具有可调金属簇的超薄二维 (2D) 金属有机框架 (MOF) 纳米片。通过转移吸附的 H 2 O 2可以显着促进活性氧( OH 和1 O 2 )的形成通过系统地调整金属种类到固液界面上。Co-MOF纳米片表现出对BPA的超快降解动力学,速率为2.23 min -1(比块体MOF高4.98倍),TOF(周转频率)值为9.99 min -1,明显大于迄今为止报告的现有材料。密度泛函理论模拟和实验结果揭示了强烈依赖金属的 ROS 形成机制。我们进一步将粉末加载到流通式聚(偏二氟乙烯)(PVDF)微滤膜上,并观察到代表性的 OPM 可以快速降解,这表明在实际应用中具有良好的性能。

更新日期:2022-08-11
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