Oxygen vacancies-enriched CoFe2O4 for peroxymonosulfate activation: The reactivity between radical-nonradical coupling way and bisphenol A
Oxygen vacancies-enriched CoFe2O4 for peroxymonosulfate activation: The reactivity between radical-nonradical coupling way and bisphenol A
复制标题
富氧空位CoFe(2)O4用于过一硫酸盐活化：自由基-非自由基偶联方式与双酚A之间的反应性
DOI：
10.1016/j.jhazmat.2021.126357
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发表时间：
2021-06-16
影响因子：
13.6
通讯作者：
Chen, Rongzhi
中科院分区：
文献类型：
--
作者：
Long, Xinxin;Feng, Chuanping;Chen, Rongzhi
氧空位（OV）在催化活性中起着至关重要的作用。在此，制备了一系列 MOF 衍生的 CoFe2O4 纳米材料，其 OV 通过简单的热老化策略进行调整，用于过一硫酸盐 (PMS) 活化。值得注意的是，稳定性、结构和催化性能显示出对退火温度的依赖性。 CoFe2O4 上丰富的表面 OV 和官能团被证实是提高催化活性的活性位点。根据密度泛函理论 (DFT) 计算，暴露在较高温度下的 (1 1 1)、(2 2 2) 和 (4 2 2) 平面有利于催化性能，这归因于强烈的表面吸附能。猝灭和电子顺磁共振（EPR）实验表明催化降解是一个自由基-非自由基耦合过程。通过结合 DFT 和 HPLC-MS 系统地探讨了活性氧 (ROS) 和双酚 A 之间的反应性以及自由基-非自由基双重降解途径。
Oxygen vacancies (OV) play a vital role in catalytic activity. Herein, a series of MOF-derived CoFe2O4 nanomaterials with OV tuned by a simple thermal aging strategy are prepared for peroxymonosulfate (PMS) activation. Remarkably, the stability, structural and catalytic properties show dependence on the annealing temperature. The abundant surface OV and functional groups on CoFe2O4 were verified as active sites to boost catalytic activity. Based on the density functional theory (DFT) calculations, (1 1 1), (2 2 2) and (4 2 2) planes exposed at higher temperatures facilitate catalytic performance, ascribed to the intense surface adsorption energy. The quenching and electron paramagnetic resonance (EPR) experiments indicate catalysis degradation is a radical-nonradical coupling process. The reactivity between reactive oxygen species (ROS) and bisphenol A and the radical-nonradical dual degradation pathways are systematically explored by combined DFT and HPLC-MS.