Collaborative Innovation Center for Advanced Nuclear Energy Technology, INET, Tsinghua University, Beijing 100084, PR China.
Collaborative Innovation Center for Advanced Nuclear Energy Technology, INET, Tsinghua University, Beijing 100084, PR China; Beijing Key Laboratory of Radioactive Wastes Treatment, Tsinghua University, Beijing, 100084, PR China.
Chemosphere. 2020 Jan;239:124812. doi: 10.1016/j.chemosphere.2019.124812. Epub 2019 Sep 7.
Carbon-based materials have been studied as metal-free catalyst for persulfate activation. At present, the activation performance of carbon materials for persulfate is usually characterized by the removal efficiency of organic pollutants. However, the kinetics of persulfate activation by carbon materials has not been investigated. In this study, the kinetics of peroxymonosulfate (PMS) activation by reduced graphene oxide (RGO) and sludge-derived biochar (BC) were investigated. The experimental results showed that the kinetics of PMS activation followed the two-phase kinetic model (fast phase (a) and slow phase (a)). In the absence of organic pollutants, the a and a were calculated to be 0.320 and 0.0471 min for BC, respectively, and 0.322 and 0.0850 min for RGO, respectively. Based on the characterization of BC and RGO, it can be concluded that the fast phase was mainly due to the formation of surface-bound active species. Competitive adsorption between PMS and targeted pollutants decreased the kinetic constant for the first phase (a) and the kinetic constant for the second phase (a) for both BC and RGO. The value of a and a increased for BC after the addition of phenol, due to the enhanced PMS activation by surface adsorbed phenol. The increase of phenol concentration decreased slightly the value of a and a. The increase of PMS concentration increased significantly the value of a and a. The decrease of a and a in repeated use of carbon materials could be due to the decrease of oxygen-containing functional groups and defect intensity.
碳基材料已被研究作为无金属催化剂用于过硫酸盐的活化。目前,碳材料对过硫酸盐的活化性能通常通过有机污染物的去除效率来表征。然而,碳材料对过硫酸盐的活化动力学尚未得到研究。在这项研究中,研究了还原氧化石墨烯(RGO)和污泥衍生生物炭(BC)对过一硫酸盐(PMS)的活化动力学。实验结果表明,PMS 的活化动力学遵循两相动力学模型(快相(a)和慢相(a))。在不存在有机污染物的情况下,BC 的 a 和 a 分别计算为 0.320 和 0.0471 min,而 RGO 的 a 和 a 分别计算为 0.322 和 0.0850 min。基于 BC 和 RGO 的表征,可以得出结论,快相主要归因于表面结合的活性物种的形成。PMS 和目标污染物之间的竞争吸附降低了第一相(a)和第二相(a)的动力学常数,对于 BC 和 RGO 都是如此。在添加苯酚后,BC 的 a 和 a 值增加,这是由于表面吸附的苯酚增强了 PMS 的活化。苯酚浓度的增加略微降低了 a 和 a 值。PMS 浓度的增加显著提高了 a 和 a 值。在重复使用碳材料时,a 和 a 的降低可能是由于含氧官能团和缺陷强度的减少。