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Synergy between Iron and Selenide on FeSe2(111) Surface Driving Peroxymonosulfate Activation for Efficient Degradation of Pollutants
Environmental Science & Technology ( IF 11.4 ) Pub Date : 2020-11-18 , DOI: 10.1021/acs.est.0c06091
Guodong Fang 1 , Teng Zhang 1, 2 , Hongbiao Cui 2 , Dionysios D. Dionysiou 3 , Cun Liu 1 , Juan Gao 1 , Yujun Wang 1 , Dongmei Zhou 1, 4
Affiliation  

In this study, iron selenide nanoparticles (FeSe2) were synthesized and applied in Fenton-like reactions for degradation of pollutants. It was found that FeSe2 exerts excellent catalytic reactivity toward different oxidants including peroxymonosulfate (PMS), peroxydisulfate, and H2O2, which can degrade a wide range of pollutants such as 2,4,4′-trichlorobiphenyl, bisphenol A, sulfamethoxazole, chlortetracycline, and perfluorooctanoic acid, with the degradation efficiency and TOC removal of pollutants reaching 55–95 and 20.3–50.9%, respectively. The mechanism of PMS activation by FeSe2 was elucidated, and the synergistic effect between Fe and Se for PMS activation was discovered to be the dominant catalytic mechanism, as evidenced by free-radical quenching, electron paramagnetic resonance, and density functional theory studies. Briefly, the Fe(II) site on the FeSe2 surface (111) accounted for PMS activation, while the reducing Se species on the surface not only acted as an electron donor contributing to Fe(II) regeneration but also produced Se vacancies further facilitating Fe(II) regeneration to improve the performance of PMS activation. In addition, FeSe2 exhibited high catalytic activity and stability for PMS activation with different pH, and can degrade PCBs efficiently in the presence of anions, natural organic matter water matrices or in complex soil eluents. This study presents the development and evaluation of FeSe2 as a novel and highly efficient activator that exhibits promise for practical applications for the degradation of pollutants in wastewater and soil wash eluent with Fenton-like reactions.

中文翻译:

FeSe 2(111)表面上的铁与硒化物之间的协同作用驱动过氧单硫酸盐活化,从而有效降解污染物。

在这项研究中,合成了硒化铁纳米颗粒(FeSe 2)并用于类似Fenton的反应中以降解污染物。发现FeSe 2对包括过氧一硫酸盐(PMS),过氧二硫酸盐和H 2 O 2在内的不同氧化剂具有优异的催化反应活性,这些氧化剂可以降解各种污染物,例如2,4,4'-三氯联苯,双酚A,磺胺甲恶唑,金霉素和全氟辛酸,其降解效率和污染物的TOC去除率分别达到55-95%和20.3-50.9%。FeSe 2激活PMS的机理通过自由基猝灭,电子顺磁共振和密度泛函理论研究证明,铁和硒之间的协同作用是PMS活化的主要催化机制。简而言之,FeSe 2表面(111)上的Fe(II)位点引起PMS活化,而表面上的还原性Se物种不仅充当电子供体,有助于Fe(II)的再生​​,而且还产生了Se空位,进一步促进了该过程Fe(II)再生可改善PMS激活的性能。另外,FeSe 2具有不同的pH值对PMS活化具有很高的催化活性和稳定性,并且在阴离子,天然有机物水基质或复杂的土壤洗脱液中可以有效降解PCBs。这项研究提出了一种新型的高效活化剂FeSe 2的开发和评价,它对通过Fenton样反应降解废水和土壤洗涤洗脱液中的污染物具有实际应用前景。
更新日期:2020-12-01
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