Structural Dependent Persulfate Activation by Coke Powder for Aniline Degradation

Structural Dependent Persulfate Activation by Coke Powder for Aniline Degradation
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焦粉活化结构依赖性过硫酸盐以降解苯胺

DOI:
10.1016/j.cej.2021.134088
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发表时间:
2021-12
影响因子:
15.1
通讯作者:
Gui Xiahui
Gui Xiahui
中科院分区:
工程技术1区
文献类型:
--
作者:
Zheng Xi;Xu Tianyuan;Kang Xueyan;Xing Yaowen;Cao Yijun;Gui Xiahui

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系统研究了焦化副产物焦粉的过硫酸盐活化活性。详细讨论了结构依赖的有机污染物降解性能及相关机理。采用X射线衍射、拉曼光谱、傅里叶变换红外光谱、X射线光电子能谱、电子顺磁共振等方法对CP的结构特征进行了研究。表征结果表明,CP的碳含量约为78%,呈现高度无序的非晶态结构,含有丰富的含氧官能团(OFGs)和持久自由基(PRF)。催化应用表明,CP在3 - 11的宽pH范围内对PS活化具有优异的活性。在0.5 g/L CP、0.25 mM PS和0.021 mM苯胺(pH 7 ± 0.2)存在下,40 min内苯胺降解率>99%。在无机阴离子(Cl-、HCO 3-和SO 42-)的干扰下,苯胺的降解率仍可达到98%。同时,猝灭实验和EPR实验表明,CP/PS体系中苯胺的降解是由超氧阴离子自由基(O2 radical dot−)引起的,其产生与溶解氧无关。PRFs、sp2杂化碳、OFGs和CP缺陷的存在导致PS的O-O键均裂为硫酸根自由基,从而使PS具有优异的苯胺降解和活性氧生成性能.此外,以C-OH和-COOH为电子给体的OFG促进PS分解生成O2自由基dot−.研究结果表明,CP是一种优良的PS活化剂,并阐明了利用焦化废水处理副产物开发修复材料。
Coke powder (CP), the by-product of coal carbonization, its activity of persulfate (PS) activation was systematically investigated. Structural dependent organic pollutant degradation performances and the related mechanisms were discussed in detail. The structural characteristics of CP were studied using X-ray diffraction, Raman, Fourier transform infrared spectra, X-ray photoelectron spectra, and electron paramagnetic resonance (EPR) etc. Characterization results indicate that CP contains ∼ 78% carbon and presents highly disordered amorphous structures with abundant oxygenated functional groups (OFGs) and persistent free radicals (PRFs). The catalytic application reveals that CP held excellent activity for PS activation across a wide pH range from 3 − 11. In the presence of 0.5 g/L CP, 0.25 mM PS and 0.021 mM aniline (pH 7 ± 0.2), >99% aniline was degraded within 40 min. Under the interference of inorganic anions (Cl−, HCO3−and SO42−), 98% aniline degradation efficiency still could be achieved. Meanwhile, quenching tests and EPR demonstrated that the superoxide anion radical (O2radical dot−) was responsible for aniline degradation in CP/PS system, and its generation was independent of dissolved oxygen. The outstanding performance of aniline degradation and ROS generation were attributed to the existence of PRFs, sp2-hybridized carbon, OFGs and defects on CP inducing O–O bonding homolytic cleavage of PS into sulfate radicals. Besides, the OFGs including C–OH and –COOH as electron donors facilitated PS decomposition to generate O2radical dot−. The findings imply that CP is an excellent PS activator, and clarify the development of remediation materials by using by-products of coking process for wastewater treatment.
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