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High-valent iron-oxo species mediated cyclic oxidation through single-atom Fe-N6 sites with high peroxymonosulfate utilization rate
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2021-12-29 , DOI: 10.1016/j.apcatb.2021.121049
Zhiwei Wang 1 , Wenlong Wang 1 , Jin Wang 2 , Yi Yuan 1 , Qianyuan Wu 1 , Hongying Hu 1, 3
Affiliation  

Fe singly anchored onto graphite carbon nitride (Fe-SA/PHCNS) as triple bondFe-N6 was synthesized to realize efficient peroxymonosulfate (PMS) activation and superior organic pollutant oxidation. The triple bondFe-N6 was the core catalytic site of activation via forming high-valent iron–oxo species (triple bondFeN6 =O) as the transient reactive intermediate as evidenced by X-ray adsorption fine spectroscopy (XAFS), in-situ Raman spectrum and theoretical calculation. The cycle of triple bondFe-N6 and triple bondFeN6 =O interconversion was sustainably observed with organic pollutant as the electron-donor and PMS as the electron-acceptor. As results, the equivalent steady state concentration of triple bondFeN6 =O was as high as 2.39 × 10−8 M and this system exhibited 97.2% average PMS utilization rate. Fe-SA/PHCNS can be immobilized onto carbon felt for the simultaneous filtration and oxidation with stable and efficient performance. This study elucidated the mechanism and superiority of triple bondFeN6 =O mediated oxidation pathway and can advance the research and application of this new approach in advanced oxidation processes.



中文翻译:

高价铁氧物种通过单原子 Fe-N6 位点介导循环氧化,具有高过硫酸盐利用率

Fe 单独锚定在石墨氮化碳 (Fe-SA/PHCNS) 上作为三键Fe-N 6被合成以实现有效的过硫酸盐 (PMS) 活化和优异的有机污染物氧化。所述三键FEN 6经由形成高原子价铁氧物种(是激活的核心催化位点三键FEN 6 = O)作为瞬态反应中间体如通过X射线吸附精细光谱(XAFS)证实,原位拉曼光谱和理论计算。三键Fe-N 6三键FeN 6 =O 相互转化的循环可持续观察到,有机污染物为电子供体,PMS 为电子受体。结果,等效稳态浓度为三键FeN 6 =O 高达 2.39 × 10 -8 M,该系统表现出 97.2% 的平均 PMS 利用率。Fe-SA/PHCNS可以固定在碳毡上同时过滤和氧化,性能稳定高效。该研究阐明了三键FeN 6 =O 介导的氧化途径的机制和优越性,可以推动这种新途径在高级氧化过程中的研究和应用。

更新日期:2022-01-02
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