当前位置: X-MOL 学术Chem. Eng. J. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Effects of different dissolved organic matter on peroxymonosulfate activation over Co-Fe binary metal: Experiments and density functional theory
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-06-28 , DOI: 10.1016/j.cej.2022.137770
Jiayan Wu , Yijing Xu , Pingxiao Wu , Meiqing Chen , Saeed Rehman , Quanyun Ye , Nengwu Zhu

The role of dissolved organic matter (DOM) on sulfate radical (SO4)-mediated advanced oxidation processes (AOPs) remains poorly studied. In this work, we systematically investigated the effects of hydrochar-derived DOM (hyDOM), humic acid (HA), and fulvic acid (FA) on peroxymonosulfate (PMS) activation over Co-Fe bimetallic catalysts (CoFeO). The results showed that the functional groups and surface oxygen vacancies of CoFeO composite were increased after compounding with DOM, which could provide more reactive sites for catalytic reaction and improve the electronic conductivity. More importantly, hydroxyl groups of the loading humic acid-like compounds on hyDOM-CoFeO and FA-CoFeO composites could accelerate the reduction of Co(III) and Fe(III), thus enhancing the PMS activation greatly. Not surprisingly, the degradation efficiency for 10 mg L−1 Bisphenol A (BPA) in PMS activation by composites within 10 min followed the order: FA-CoFeO > hyDOM-CoFeO > HA-CoFeO, and the kinetics constant (k) was 3.6, 2.6, and 8.2 times higher than that of CoFeO composite, respectively. The electron paramagnetic resonance (EPR) and quenching experiments indicated that more reactive oxygen species (ROS) were generated after compounding DOM, and SO4 was the dominant ROS in the degradation process. Furthermore, the LC-MS analysis and density functional theory (DFT) calculation were conducted to prove the proposed degradation pathways of BPA. Our work is expected to clarify the effects of DOM on Co-Fe bimetallic catalysts/PMS system for environmental remediation.



中文翻译:

不同溶解有机物对 Co-Fe 二元金属上过氧单硫酸盐活化的影响:实验和密度泛函理论

溶解有机物 (DOM) 对硫酸根 (SO 4-) 介导的高级氧化过程 (AOP) 的研究仍然很少。在这项工作中,我们系统地研究了水炭衍生的 DOM (hyDOM)、腐植酸 (HA) 和富里酸 (FA) 在 Co-Fe 双金属催化剂 (CoFeO) 上对过一硫酸盐 (PMS) 活化的影响。结果表明,与DOM复合后CoFeO复合材料的官能团和表面氧空位增加,可为催化反应提供更多的反应位点,提高电子导电性。更重要的是,在 hyDOM-CoFeO 和 FA-CoFeO 复合材料上负载类腐植酸化合物的羟基可以加速 Co(III) 和 Fe(III) 的还原,从而大大增强 PMS 的活化。毫不奇怪,10 mg L -1的降解效率复合材料在 10 min 内激活 PMS 中的双酚 A (BPA) 依次为:FA-CoFeO > hyDOM-CoFeO > HA-CoFeO,其动力学常数 ( k ) 分别是 CoFeO 复合材料的 3.6、2.6 和 8.2 倍, 分别。电子顺磁共振(EPR)和猝灭实验表明,复合DOM后产生了更多的活性氧(ROS),SO 4-是降解过程中的主要活性氧。此外,还进行了 LC-MS 分析和密度泛函理论 (DFT) 计算,以证明所提出的 BPA 降解途径。我们的工作有望阐明 DOM 对用于环境修复的 Co-Fe 双金属催化剂/PMS 系统的影响。

更新日期:2022-06-28
down
wechat
bug