Electrically supported mediator Co(II)-activated peroxydisulfate synergistic process for organic contaminants elimination
Electrically supported mediator Co(II)-activated peroxydisulfate synergistic process for organic contaminants elimination
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电支持介体 Co(II) 激活的过二硫酸盐协同工艺消除有机污染物
DOI：
10.1016/j.envres.2022.113778
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发表时间：
2022
影响因子：
8.3
通讯作者：
Huaili Zheng
中科院分区：
文献类型：
--
作者：
Bingzhi Liu;Zizeng Wang;Haitao Lu;Baorong Huang;Li Feng;Huaili Zheng
在均相催化剂中，钴离子表现出超高的过硫酸盐活化性能。在这项工作中，建立了一种电负载介质Co（II）活化过硫酸氢盐协同工艺来去除水中的有机污染物。通过比较不同偶联体系的氧化降解性能和反应速率常数，验证了其协同催化作用。进出口公司的脱色能力(2)PDS对活性黑5 (RB5)探索,结果表明RB5的去除率可以达到93.21%的优化条件下电流密度为5.71 mA /厘米2,初始pH值为4,(II)浓度的0.2毫米和PDS 5毫米的浓度。水的影响矩阵RB5的去除进行了研究,并发现HCO 3−和胡敏酸显著地抑制RB5退化,而Cl−和h2po4−在一定浓度下能有效促进反应。值得注意的是，RB5在E-Co(II)-PDS系统中的降解能耗较低，单位体积能耗（EE/O）值为0.4304 kWh·m−3。EPR测试、淬火实验和贡献率分析表明，E-Co(II)-PDS过程中的氧化活性物质为Co（III）、硫酸盐自由基和羟基自由基，其氧化贡献率分别为15.72%、12.69%和53.25%。最后，通过质谱分析提出了RB5的分解过程。电流通过电子转移促进钴离子循环和PDS活化，诱导Co（II）促进PDS活化，这是E-Co(II)-PDS体系实现RB5稳健降解能力的主要机制。•Co（II）大大提高了电活化过硫酸盐体系的活化效果。•电流促进Co(II)/Co（III）循环和过硫酸氢盐活化。E-Co(II)-PDS系统能耗低。•Co(III), so4。•-和•OH有助于E-Co(II)- pds过程中RB5的去除。•E-Co(II)-PDS能有效降解水中的有机污染物。
Among homogeneous catalysts, cobalt ions exhibit ultra-high persulfate activation performance. In this work, an electrically supported medium Co(II) activated peroxydisulfate synergistic process was established to eliminate organic contaminants in water. The synergistic catalytic effect was verified by comparing the oxidative degradation performance and reaction rate constant of different coupling systems. The decolorization ability of E-Co(II)-PDS on reactive black 5 (RB5) was explored, and the results showed that the removal rate of RB5 can reach 93.21% under the optimized conditions of current density of 5.71 mA/cm 2 , initial pH of 4, Co(II) concentration of 0.2 mM and PDS concentration of 5 mM. The effect of water matrix on the removal of RB5 was studied, and it was found that HCO 3 − and humic acid significantly inhibited the degradation of RB5, while Cl − and H 2 PO 4 − could effectively promote it at a certain concentration. Notably, the degradation of RB5 in E-Co(II)-PDS system achieved lower energy consumption, with an energy consumption per unit volume (EE/O) value of 0.4304 kWh·m −3 . EPR test, quenching experiments and contribution rate analysis showed that the oxidation active species in E-Co(II)-PDS process were Co(III), sulfate radicals and hydroxyl radicals , and their oxidation contribution rates were 15.72%, 12.69% and 53.25%, respectively. Finally, the decomposition process of RB5 was proposed by the mass spectrometry results. The electric current promotes cobalt ion cycling and PDS activation through electron transfer , and induces Co(II) to promote the activation of PDS, which is the main mechanism of E-Co(II)-PDS system to achieve the robust degradation ability of RB5. • Co(II) greatly improved the activation effect of electroactivated persulfate system. • The current promotes Co(II)/Co(III) cycling and peroxydisulfate activation. • Low energy consumption was achieved by E-Co(II)-PDS system. • Co(III), SO 4 . •– and • OH contributed to RB5 removal in E-Co(II)-PDS process. • E-Co(II)-PDS could robustly degrade organic contaminants in water.