BDD 阳极上氯和羟基自由基介导的 Ni-EDTA 电化学去除,ACS ES&T Water

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BDD 阳极上氯和羟基自由基介导的 Ni-EDTA 电化学去除
ACS ES&T Water ( IF 4.8 ) Pub Date : 2023-02-10 , DOI: 10.1021/acsestwater.2c00598
Ming Liu ₁ , Guoshuai Liu ₁ , Penghui Shao ₂ , Yina Tian ₁ , Hua Zou ₁

Affiliation

作为一种高活性氧化物种，氯自由基（E _{Cl ^•}⁰ = 2.47 V vs 标准氢电极，SHE）可以与含羧基和氨基的有机物有效反应。为此，深入研究了活性物质（Cl ^•和^{• OH）介导的 Ni-EDTA 分解的机理。}_{使用的掺硼金刚石 (BDD) 阳极可以显着增强 Ni-EDTA 在 NaCl 电解质中的分解，表现为表观反应动力学常数是 Na 2} SO ₄和 NaClO ₄存在时的 2.7 倍和 4 倍，分别。^{实验结果和理论模拟表明，BDD 阳极上的析氯反应 (CER) 在热力学上是有利的，这促进了 Cl •}的电生成。^{竞争动力学和猝灭实验证明，Cl •}与 Ni–EDTA的二级速率常数为 ∼1.38 × 10 ¹⁰ M ^–1 s ^–1，高于^• OH 与 Ni–EDTA (∼2.68 × 10 ⁹ M ^–1秒^–1）。此外，实验结果和密度泛函理论 (DFT) 计算表明，Ni-EDTA 的分子变化是由 Cl ^•和^{• OH 通过 EDTA}^4–中的氢提取和电子转移途径。这项研究表明对含氯废水的电化学解络具有积极意义，这使得水处理更有效、更经济、更容易。

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Electrochemical Removal of Ni–EDTA Mediated by Chlorine and Hydroxyl Radicals on BDD Anodes

As a highly reactive oxidative species, chlorine radicals (E_Cl^•⁰ = 2.47 V vs standard hydrogen electrode, SHE) could react with carboxylic and amino group-containing organic matter efficiently. To this end, mechanistic insights into the reactive species (Cl^• and ^•OH)-mediated Ni–EDTA decomposition were examined in depth. The used boron-doped diamond (BDD) anode could achieve remarkably enhanced decomposition of Ni–EDTA in NaCl electrolyte, indicated by the apparent reaction kinetics constant being 2.7 and 4 times that in the presence of Na₂SO₄ and NaClO₄, respectively. The experimental results and theoretical simulations revealed that the chlorine evolution reaction (CER) was thermodynamically favorable on the BDD anode, which facilitated the electro-generation of Cl^•. Competitive kinetics and quenching experiments proved that the second-order rate constant of Cl^• with Ni–EDTA is ∼1.38 × 10¹⁰ M^–1 s^–1, which is higher than that of ^•OH with Ni–EDTA (∼2.68 × 10⁹ M^–1 s^–1). Furthermore, the experimental results and density functional theory (DFT) calculations show that the molecular changes of Ni–EDTA are mediated by Cl^• and ^•OH through the H-abstraction and electron-transfer pathway in EDTA^4–. This study demonstrates positive implications in the electrochemical decomplexation of wastewater containing chlorine, which makes water treatment more effective, more economical, and much easier.

更新日期：2023-02-10

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