八面体FMN-700活化过硫酸盐产生1O2降解偶氮有机物

钟晴; 叶校圳; 曾静; 蔡蓝燕; 王永全; 洪俊明

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中国环境科学 ›› 2023, Vol. 43 ›› Issue (12) : 6374-6385.

水污染与控制

八面体FMN-700活化过硫酸盐产生¹O₂降解偶氮有机物

钟晴¹, 叶校圳², 曾静², 蔡蓝燕², 王永全², 洪俊明¹

作者信息 +

Efficient decolorization of azo organics by singlet oxygen from activating PMS with octahedral structured FMN-700

ZHONG Qing¹, YE Xiao-zhen², ZENG Jing², CAI Lan-yan², WANG Yong-quan², HONG Jun-ming¹

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摘要

以掺氮普鲁士蓝类似物(PBA)为前驱体,通过高温煅烧法制备了含铁、锰氮化物的催化材料(FMN-700),用于活化过一硫酸盐(PMS)快速降解偶氮有机物.通过扫描电子显微镜(SEM)、X射线粉末衍射仪(XRD)、傅里叶变换红外光谱仪(FTIR)对催化剂进行表征,证明FMN-700具有层状堆叠的正八面体结构,含有铁锰氮化物.研究了催化剂投加量,PMS浓度和初始pH值等因素对偶氮有机物降解的影响,结果表明在初始pH值为7、催化剂投加量为0.2g/L、PMS浓度为2mmol/L的条件下,60min内可使10mg/L的RBK5脱色率达99.5%.淬灭实验、电子顺磁共振(EPR)显示¹O₂为降解体系的主要活性物质.X射线光电子能谱(XPS)表明反应前后Fe(III)/Fe(II)、Mn(III)/Mn(II)比值增大,吡啶N向吡咯N和石墨N转化,该过程可以诱导产生¹O₂.3D-EEM光谱反应后荧光强度大幅升高,表明具有荧光淬灭作用的偶氮键被破坏,实现偶氮有机物的脱色降解.

Abstract

A catalytic material containing iron and manganese nitride (FMN-700) was prepared by high-temperature calcination using nitrogen-doped Prussian blue analogue (PBA) as a precursor for the rapid degradation of azo organic compounds by activated peroxymonosulfate (PMS). The catalysts were characterized by scanning electron microscopy (SEM), X-ray powder diffractometer (XRD) and Fourier transform infrared spectroscopy (FTIR), which demonstrated that FMN-700 has a layered stacked ortho-octahedral structure and contains Fe-Mn-nitride. The effects of catalyst dosage, PMS concentration and initial pH on the catalytic degradation of azo organics were investigated. The results showed that 99.5% decolorization of RBK5 at 10mg/L could be achieved within 60min at an initial pH of 7, a catalyst dosing of 0.2g/L and a PMS concentration of 2mmol/L. The quenching experiments and Electron Paramagnetic Resonance (EPR) indicated that ¹O₂ was the main active substance in the degradation system. X-ray photoelectron spectroscopy (XPS) showed that the Fe(III)/Fe(II) and Mn(III)/Mn(II) ratios increased and the pyridine N content decreased before and after the reaction. This process can induce the production of ¹O₂. The significant increase of fluorescence intensity of 3D-EEM spectrum showed that the azo bond with fluorescence quenching effect was broken during the degradation process and azo organic compounds were successfully decolorized and degraded.

导出引用

钟晴, 叶校圳, 曾静, 蔡蓝燕, 王永全, 洪俊明. 八面体FMN-700活化过硫酸盐产生¹O₂降解偶氮有机物[J]. 中国环境科学. 2023, 43(12): 6374-6385

ZHONG Qing, YE Xiao-zhen, ZENG Jing, CAI Lan-yan, WANG Yong-quan, HONG Jun-ming. Efficient decolorization of azo organics by singlet oxygen from activating PMS with octahedral structured FMN-700[J]. China Environmental Science. 2023, 43(12): 6374-6385

中图分类号： X703.1

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