Heterogeneous photo-Fenton degradation of bisphenol A over Ag/AgCl/ferrihydrite catalysts under visible light
Heterogeneous photo-Fenton degradation of bisphenol A over Ag/AgCl/ferrihydrite catalysts under visible light
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可见光下Ag/AgCl/水铁矿催化剂非均相光芬顿降解双酚A
DOI：
10.1016/j.cej.2018.04.073
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发表时间：
2018-08
影响因子：
15.1
通讯作者：
He Hongping
中科院分区：
文献类型：
--
作者：
Zhu Yanping;Zhu Runliang;Xi Yunfei;Xu Tianyuan;Yan Lixia;Zhu Jianxi;Zhu Gangqiang;He Hongping
传统的非均相芬顿反应常因Fe 2+的再生率较低而受到限制，从而抑制了H2 O2的分解和dotOH自由基的生成。本文提出了一种新的思路，即通过引入等离子体粒子的光生电子来显著加速非均相芬顿反应中Fe 2 +/Fe 3+的氧化还原循环。为此，已经合成了新颖的等离子体Ag/AgCl纳米颗粒包覆的水铁矿（Ag/AgCl/Fh）。在可见光下，Ag/AgCl/Fh催化剂对双酚（BPA）的光-Fenton降解率比纯Fh催化剂有显著提高。值得注意的是，6%Ag/AgCl/Fh的速率常数为0.0506 min-1，约为纯Fh（0.0099 min-1）的5.1倍。此外，6%Ag/AgCl/Fh催化剂对双酚A的降解仍具有很高的催化活性，且经过4次循环后，铁的浸出率很低。初始pH值的影响的结果表明，Ag/AgCl/FH样品表现出相对较高的光芬顿催化活性，即使在pH值为6。电子自旋共振（ESR）分析表明，自由基dotOH在光Fenton反应中起着重要的作用。60 min后dotOH自由基浓度可达267.6 μmol/L，远高于纯Fh（69.2 μmol/L）。对Ag/AgCl/Fh催化剂降解BPA前后Fe ~（2+）浓度的测定和XPS Fe ~（2+）谱的分析表明，Ag/AgCl的负载可以在可见光照射下，利用表面等离子体共振（SPR）效应，利用Ag纳米粒子的光生电子加速Fe ~（3+）/Fe ~（2+）的转化。
The conventional heterogeneous Fenton reaction is often confined by the lower regeneration of Fe2+, which then inhibits the decomposition of H2O2and the generation of radical dotOH. Here we propose a novel idea to significantly accelerate the redox cycling of Fe2+/Fe3+in heterogeneous Fenton reaction by introducing photo-generated electrons from plasmonic particles. Towards this aim, novel plasmonic Ag/AgCl nanoparticles coated ferrihydrite (Ag/AgCl/Fh) have been synthesized. Compared with pure Fh, a remarkable enhancement in the photo-Fenton degradation towards bisphenol (BPA) can be observed for all Ag/AgCl/Fh samples under visible light. Noticeably, the rate constant of 6%Ag/AgCl/Fh is 0.0506 min−1, which is about 5.1 times as high as that of pure Fh (0.0099 min−1). Moreover, the catalytic activity of 6%Ag/AgCl/Fh on the degradation of BPA remains quite efficient with a low Fe leaching after 4 recycles. The results of the effect of initial pH indicates that Ag/AgCl/Fh samples exhibit relatively high photo-Fenton catalytic activity even at pH 6. The electron spin resonance (ESR) analysis reveals that radical dotOH plays a significant role in the photo-Fenton reaction. The concentration of radical dotOH can even reach 267.6 μmol/L after 60 min, which is much higher than that of pure Fh (69.2 μmol/L). The measurement of Fe2+concentration and the XPS Fe2p spectra of Ag/AgCl/Fh before and after the degradation of BPA indicate the loading of Ag/AgCl can accelerate the conversion of Fe3+/Fe2+by the photo generated electrons from Ag nanoparticles due to the surface plasmon resonance (SPR) effect under the visible light irradiation.
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