A new heterogeneous catalytic system for wastewater treatment: Fe-immobilized polyelectrolyte microshells for accumulation and visible light-assisted photooxidative degradation of dye pollutants

A new heterogeneous catalytic system for wastewater treatment: Fe-immobilized polyelectrolyte microshells for accumulation and visible light-assisted photooxidative degradation of dye pollutants
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一种用于废水处理的新型多相催化系统:铁固定聚电解质微壳用于染料污染物的积累和可见光辅助光氧化降解

DOI:
10.1016/j.molcata.2007.11.006
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发表时间:
2008-02
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--
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中科院分区:
化学2区
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以壳聚糖(CHI)和海藻酸钠(ALG)为模板,三聚氰胺甲醛(MF)为载体,通过交替吸附Fe(III)和ALG,成功构建了Fe固定化海藻酸钠微壳。共聚焦激光扫描显微镜(CLSM)直接证明了合成的(ALG/CHI)4(ALG/Fe)n(n=1,2)壳层可以在温和条件下通过简单的混合处理在良好的内部空间中有效地聚集罗丹明B(RhB)、亚甲基蓝(MB)和吖啶橙子(AO)。此外,H2 O2可以穿过Fe-固定的壳壁,并在可见光辐射下与聚集在壳内部的染料反应。利用紫外-可见吸收光谱和激光共聚焦扫描电镜(CLSM)研究了H2 O2存在下微壳中染料的光降解行为。更重要的是,在Fe固定化微壳中发生的光氧化反应可以在从酸性到中性介质的宽pH范围内进行,这比仅允许在pH <4的酸性条件下起作用的常规芬顿反应优越上级。电子顺磁共振(EPR)和其他研究的光活化反应过程的机制提供了初步的证据,不同的光反应发生在中性介质中,光反应发生在封闭的微壳在酸性介质中进行主要是通过HO自由基具有高氧化电位。
Fe-immobilized polyelectrolyte microshells have been successfully constructed by alternative adsorption of Fe(III) and alginate sodium (ALG) onto the precursor shells composed of chitosan (CHI) and ALG templated on melamine formaldehyde (MF) particles. Confocal laser scanning microscopy (CLSM) directly demonstrated that the as-synthesized (ALG/CHI)4(ALG/Fe)n(n=1, 2) shells could accumulate efficiently rhodamine B (RhB), methylene blue (MB) and acridine orange (AO) in well-defined internal space under moderate conditions via a simple mix processing. Further, H2O2could cross the Fe-immobilized shell walls and react with the dyes concentrated in the interior of shells under visible radiation. The photodegradation of dyes accumulated in the microshells in the presence of H2O2was characterized by UV–vis adsorption spectra and CLSM. More importantly, the photooxidative reaction occurring in the Fe-immobilized microshells can be performed at a wide range of pH from acid to neutral media, which is superior to the conventional Fenton reaction that allows taking effect only under acid condition of pH <4. Electron paramagnetic resonance (EPR) and other studies into the mechanism of the light-activated reaction process give tentative evidence that distinct from the photoreaction occurring in neutral medium, the photoreaction taking place in confined microshells in acid medium proceeds mainly through HO radicals with high oxidative potential.
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