Construction of g-C3N4/PDI@MOF heterojunctions for the highly efficient visible light-driven degradation of pharmaceutical and phenolic micropollutants

Construction of g-C3N4/PDI@MOF heterojunctions for the highly efficient visible light-driven degradation of pharmaceutical and phenolic micropollutants
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构建 g-C3N4/PDI@MOF 异质结,用于高效可见光驱动降解药物和酚类微污染物

DOI:
10.1016/j.apcatb.2019.03.024
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发表时间:
2019-08-05
影响因子:
22.1
通讯作者:
Lu, Jianmei
Lu, Jianmei
中科院分区:
化学1区
文献类型:
--
作者:
Li, Yuanyuan;Fang, Yu;Lu, Jianmei

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通过在g-C3 N4/PDI层上原位生长NH 2-MIL-53(Fe),制备了一种新型的g-C3 N4/PDI@MOF异质结。在H2 O2和可见光LED(420 < lambda <800 nm)的存在下,将该异质结作为光催化剂用于去除药物和酚类微污染物。在可见光照射下,该复合异质结对几种水溶性有毒有机污染物(50 ppm)的光催化降解表现出优异的光催化性能,对四环素(TC)的最高降解效率可达90%(1 h),对苯甲酸(苯甲酸)的最高降解效率可达78%(1 h),对苯甲酸(苯甲酸)的最高降解效率可达90%(1 h),对苯甲酸(苯甲酸)的最高降解效率可达90%(1 h),对苯甲酸(苯甲酸)的最高降解效率可达90%(1 h),对苯甲酸的最高降解效率可达78%(1 h),对苯甲酸(苯甲酸)的最高降解效率可达90%(1 h)。对卡马西平(CBZ)为2.5 h,对双酚A(BPA)为100%(10 min),对对硝基苯酚(PNP)为100%(30 min)。此外,低浓度的酚类有机污染物(2 ppm)也可以迅速降解成小分子(HPLC分析)在10分钟内。这种性能是上级优于一些以前报道的可见光光催化剂。提高的光催化活性归因于g-C3 N4/PDI和NH 2-MIL-53(Fe)之间的界面接触和电子能带结构匹配有效地形成了异质结,这有利于电荷分离并促进光降解过程。重复实验研究和降解前后光催化剂的结构分析(XRD和FT-IR)表明,该光催化剂具有良好的稳定性和重复使用性。该工作为构建基于FeMOF的异质结光催化剂用于可见光下H2 O2对有机污染物的非均相光催化降解提供了新的思路。
A novel g-C3N4/PDI@MOF heterojunction was synthesized by the in situ growth of NH2-MIL-53(Fe) onto the g-C3N4/PDI layer. The heterojunction was applied as a photocatalyst for the removal of pharmaceutical and phenolic micropollutants in the present of H2O2 and visible LED light (420 < lambda < 800nm). The synergistic heterojunction displays excellent photocatalytic performance for the removal of several water-soluble and toxic organic pollutants (50 ppm) under visible light irradiation, with a maximum efficiency of up to 90% (1 h) for tetracycline (TC), 78% (2.5 h) for carbamazepine (CBZ), 100% (10 min) for bisphenol A (BPA) and 100% (30 min) for p-nitrophenol (PNP). Furthermore, the low concentration of phenolic organic pollutants (2 ppm) can also be rapidly degraded into small molecules (analyzed by HPLC) within 10 min. This performance is superior to some previously reported visible-light photocatalysts. The improved photocatalytic activity is attributed to the efficient formation of heterojunctions derived from the interface contact and electronic band structure matching between g-C3N4/PDI and NH2-MIL-53(Fe), which is beneficial to charge separation and facilitates the photodegradation process. Repeated experimental studies and structural analysis of photocatalyst before and after degradation (XRD and FT-IR) demonstrated that the photocatalyst exhibits good stability and reusability. This work provides a new insight into the construction of heterojunction photocatalysts based on FeMOF for the heterogeneous photodegradation of organic contaminants with H2O2 under visible light.