Self-Enhanced Selective Oxidation of Phosphonate into Phosphate by Cu(II)/H2O2: Performance, Mechanism, and Validation,Environmental Science & Technology

当前位置： X-MOL 学术 › Environ. Sci. Technol. › 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.)

Self-Enhanced Selective Oxidation of Phosphonate into Phosphate by Cu(II)/H2O2: Performance, Mechanism, and Validation
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-12-13 , DOI: 10.1021/acs.est.1c06471
Shuhui Sun ₁ , Chao Shan _{1,

2} , Zhichao Yang ₁ , Shu Wang ₁ , Bingcai Pan _{1,

2}

Affiliation

Phosphonate is an important category of highly soluble organophosphorus in contaminated waters, and its oxidative transformation into phosphate is usually a prerequisite step to achieve the in-depth removal of the total phosphorus. Currently, selective oxidation of phosphonate into phosphate is urgently desired as conventional advanced oxidation processes suffer from severe matrix interferences. Herein, we employed 1-hydroxyethylidene-1,1-diphosphonic acid (HEDP) as a model phosphonate and demonstrated its efficient and selective oxidation by the Cu(II)/H₂O₂ process at alkaline pH. In the presence of trace Cu(II) (0.020 mM), 90.8% of HEDP (0.10 mM) was converted to phosphate by H₂O₂ in 30 min at pH 9.5, whereas negligible conversion was observed by UV/H₂O₂ or a Fenton reaction (pH = 3.0). The oxidation of HEDP by Cu(II)/H₂O₂ was insignificantly affected by natural organic matters (10.0 mg TOC/L) and various anions including chloride, sulfate, and nitrate (10.0 mM). The complexation of Cu(II) with HEDP coupling Cu(III) produced in situ enabled an intramolecular electron transfer process, which features high selective oxidation. Selective degradation of HEDP was further validated by adding stoichiometric H₂O₂ into an industrial effluent, where the existing Cu(II) could serve as the catalyst. This study also provides a successful case to trigger selective oxidation of trace pollutants of concern upon synergizing with the nature of the contaminated water.

中文翻译：

Cu(II)/H2O2 将膦酸盐自增强选择性氧化成磷酸盐：性能、机理和验证

膦酸盐是污染水体中一类重要的高溶解性有机磷，其氧化转化为磷酸盐通常是实现总磷深度去除的前提步骤。目前，迫切需要将膦酸盐选择性氧化成磷酸盐，因为传统的高级氧化工艺会受到严重的基质干扰。在此，我们使用 1-羟基亚乙基-1,1-二膦酸 (HEDP) 作为模型膦酸盐，并在碱性 pH条件下通过 Cu(II)/H ₂ O _{2工艺证明了其高效和选择性氧化。}在痕量 Cu(II) (0.020 mM) 存在下，90.8% 的 HEDP (0.10 mM) 被 H ₂ O _{2转化为磷酸盐}在 pH 9.5 下 30 分钟内，而通过 UV/H ₂ O ₂或芬顿反应 (pH = 3.0) 观察到可忽略不计的转化。_{Cu(II)/H 2} O ₂对 HEDP 的氧化不受天然有机物 (10.0 mg TOC/L) 和各种阴离子（包括氯离子、硫酸根和硝酸根）（10.0 mM）的影响。Cu(II) 与原位产生的 HEDP 偶联 Cu(III) 的络合实现了分子内电子转移过程，该过程具有高选择性氧化的特点。_{通过添加化学计量 H 2} O ₂进一步验证了 HEDP 的选择性降解进入工业废水，其中现有的 Cu(II) 可以用作催化剂。该研究还提供了一个成功的案例，通过与受污染水的性质协同作用，触发关注的痕量污染物的选择性氧化。

更新日期：2022-01-04

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南