<br>通过 MOF 衍生的 BiFeO3 活化过氧一硫酸盐对可见光降解萘普生的调控机制的新见解,Journal of Hazardous Materials

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通过 MOF 衍生的 BiFeO3 活化过氧一硫酸盐对可见光降解萘普生的调控机制的新见解
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2022-02-19 , DOI: 10.1016/j.jhazmat.2022.128513
Juanjuan Yao ₁ , Zihan Chen ₁ , Huiying Zhang ₁ , Naiyun Gao ₂ , Zhi Zhang ₁ , Wenchao Jiang ₁

Affiliation

采用金属有机框架衍生化（MOF-d）制备的 BiFeO3 （BFO）纳米笼作为活化剂，首次研究了可见光通过过氧一硫酸盐（PMS）活化降解萘普生的影响机制。由于高度有序的介孔，MOF-d BFO 比热液合成 BFO 表现出更优异的 PMS 活化能力。引入可见光后，伪一阶降解速率常数提高了 3.0 倍。淬灭实验表明，在MOF-d BFO/PMS/暗体系中，ROS在萘普生降解中的贡献顺序为SO4•->1O2 ≈ •OH，而在可见光引入EPR测试后转变为h+>1O2 > >O2•-≈SO4•-> •OH首先显示可见光促进1O2产量（非自由基途径），但抑制了•OH和SO4•-的产生（自由基途径）。N2 吹扫实验进一步证明，1O2 主要来源于 h+ 和 PMS 之间的反应，相当于 MOF-d BFO/PMS/vis 系统中 O2 和 e--h+ 之间的反应。在可见光下，通过 Fe （III）激活 PMS 可能会受到 Fe 3d 轨道上 e- 填充的阻碍，阴离子 PMS 更喜欢接近 h+ 而不是 e-，导致 •OH 和 SO4•- 产率降低。此外，PMS 还面临着来自吸附 O2 和氧空位的 e-capture 竞争。在 MOF-d BFO/PMS 系统中提出了萘普生在黑暗和可见光下的降解途径。

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New insight into the regulation mechanism of visible light in naproxen degradation via activation of peroxymonosulfate by MOF derived BiFeO3

BiFeO3 (BFO) nanocage prepared by metal-organic-framework derivatization (MOF-d) was adopted as activator to first investigate the effect mechanism of visible-light on naproxen-degradation via peroxymonosulfate (PMS) activation. MOF-d BFO expressed more excellent PMS activation ability than hydrothermal-synthetic BFO, due to highly ordered mesopores. A 3.0 times higher pseudo-first-order degradation rate constant was achieved after visible-light introduced. The quenching experiments indicated that the contribution of ROS in naproxen degradation followed the order of SO4•->1O2 ≈ •OH in MOF-d BFO/PMS/dark system, while changed into h+>1O2 > >O2•-≈SO4•-> •OH after visible-light introduced. EPR tests first revealed that visible-light promoted 1O2 yield (non-radical pathway) but suppressed •OH and SO4•- generation (free-radical pathways). N2-purging experiments further proved that 1O2 primarily originates from the reaction between h+ and PMS, equivalently to that between O2 and e--h+ in MOF-d BFO/PMS/vis system. Under visible-light, PMS activation via Fe (III) might be hindered by e- filling on Fe 3d orbital and anion PMS preferred to approach h+ rather than e-, resulting in the decrease of •OH and SO4•- yields. Moreover, PMS faces competition from adsorbed-O2 and oxygen-vacancies for e- capture. The degradation-pathways for naproxen in dark and under visible light were both proposed in MOF-d BFO/PMS system.

更新日期：2022-02-19

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