Faculty of environmental science and engineering, Kunming University of Science and Technology, Kunming, Yunnan, 650500, China; National Regional Engineering Research Center-NCW, Kunming, Yunnan, 650500, China.
School of Environment, Harbin Institute of Technology, Harbin 150090, China.
Water Res. 2023 Oct 1;244:120487. doi: 10.1016/j.watres.2023.120487. Epub 2023 Aug 14.
A novel particle electrode based on antimony tailings microspheres was successfully constructed by ultrasonic immersion calcination method, and the degradation of RhB was studied in a three-dimensional electrochemical reactor (3DER). It was characterized by XRD, SEM, EDS, XPS, cyclic voltammetry and linear sweep voltammetry. When the pH value is 5.00, the dosage of Fe/Cu@antimony tailing is 1.50 g/L, the initial concentration is 100 mg/L, and the current density is 20 mA/cm, the degradation efficiency is the best (99.40% for RhB and 98.81% for TOC) within 15 min. The results show that in the three-dimensional electrochemical oxidation system, electrochemical oxidation and electro Fenton oxidation occur at the same time to cause the increase of hydroxyl radicals. According to LC-MS analysis and EPR characterization, it can be found that the main degradation mechanism of RhB is that hydroxyl radicals continuously attack RhB, and realize rapid degradation of RhB through deethylation, deamination, dealkylation, decarboxylation, chromophore splitting, ring opening and mineralization. Fe/Cu@antimony tailing particles are both electrodes for electrochemical oxidation and catalysts for Fenton oxidation. The degradation effect of RhB remained at 94% after 6 cycles, and the leaching rates of Fe and Cu are only 1.20% and 0.79%, indicating that Fe/Cu@AT had significant stability. This work provides a new insight into the establishment of an efficient and stable three-dimensional electrocatalytic particle electrode.
一种基于锑尾矿微球的新型粒子电极通过超声浸渍煅烧法成功构建,并在三维电化学反应器(3DER)中研究了 RhB 的降解。采用 XRD、SEM、EDS、XPS、循环伏安法和线性扫描伏安法对其进行了表征。当 pH 值为 5.00 时,Fe/Cu@antimony tailing 的用量为 1.50 g/L,初始浓度为 100 mg/L,电流密度为 20 mA/cm 时,15 min 内降解效率最佳(RhB 为 99.40%,TOC 为 98.81%)。结果表明,在三维电化学氧化体系中,同时发生电化学氧化和电芬顿氧化,导致羟基自由基增加。根据 LC-MS 分析和 EPR 表征,可以发现 RhB 的主要降解机制是羟基自由基不断攻击 RhB,通过去乙基化、脱氨、脱烷基、脱羧基、发色团分裂、开环和矿化实现 RhB 的快速降解。Fe/Cu@antimony tailing 颗粒既是电化学氧化的电极,又是 Fenton 氧化的催化剂。RhB 的降解效果在 6 次循环后仍保持在 94%,Fe 和 Cu 的浸出率仅为 1.20%和 0.79%,表明 Fe/Cu@AT 具有显著的稳定性。这项工作为建立高效稳定的三维电催化粒子电极提供了新的思路。