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Peroxydisulfate Activation by Atomically-dispersed Fe-Nx on N-doped Carbon: Mechanism of Singlet Oxygen Evolution for Nonradical Degradation of Aqueous Contaminants
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2020-10-28 , DOI: 10.1016/j.cej.2020.127545
Ningjie Du , Ying Liu , Qiuju Li , Wei Miao , Dandan Wang , Shun Mao

Single-atom catalysts have drawn increasing attention in advanced oxidation due to their unique structure and significant promise in heterogeneous catalysis. Herein, single-atom iron anchored on nitrogen-doped carbon (SAFe-N-C) was synthesized with iron phthalocyanine (FePc) and metal-organic framework (ZIF-8). With thermal treatment and acid leaching, atomically-dispersed Fe-Nx sites were successfully formed on the surface of N-C support derived from ZIF-8. The prepared catalyst was demonstrated to activate peroxydisulfate (PDS) for chloramphenicol (CAP) degradation. Compared with N-C, SAFe-N-C shows 6 times enhanced removal efficiency (from 15.3% to 93.1%) for CAP. Moreover, the catalyst shows high catalytic activity in a wide pH range of 5 to 9 and good resistance to inorganic anions, in which a singlet oxygen-dominated process is found. This study reveals the role of single-atom site in singlet oxygen evolution and offers a new catalytic approach for selective removal of organic pollutants in complex water matrix.



中文翻译:

原子分散的Fe-N x在N掺杂碳上的过氧二硫酸盐活化:单态氧演化对水污染物非自由基降解的机理

单原子催化剂由于其独特的结构和在多相催化中的重大前景而在高级氧化中引起了越来越多的关注。在此,用铁酞菁(FePc)和金属有机骨架(ZIF-8)合成了锚固在氮掺杂碳(SAFe-NC)上的单原子铁。通过热处理和酸浸,原子分散的Fe-N x在ZIF-8衍生的NC支持表面上成功形成位点。经证明,所制备的催化剂可激活过氧二硫酸盐(PDS)降解氯霉素(CAP)。与NC相比,SAFe-NC对CAP的去除效率提高了6倍(从15.3%到93.1%)。此外,该催化剂在5至9的宽pH范围内显示出高催化活性,并且对无机阴离子具有良好的抗性,其中发现了单线态氧为主的过程。这项研究揭示了单原子位在单线态氧释放中的作用,并为选择性去除复杂水基质中的有机污染物提供了新的催化方法。

更新日期:2020-10-30
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