Enhanced ozonation of Cu(II)-organic complexes and simultaneous recovery of aqueous Cu(II) by cathodic reduction

Enhanced ozonation of Cu(II)-organic complexes and simultaneous recovery of aqueous Cu(II) by cathodic reduction
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通过阴极还原增强 Cu(II)-有机络合物的臭氧化并同时回收 Cu(II) 水溶液

DOI:
10.1016/j.jclepro.2021.126837
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发表时间:
2021-03
影响因子:
11.1
通讯作者:
Min Zhao
Min Zhao
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Cong Chen;Anqi Chen;Xianfeng Huang;Ran Ju;Xuchun Li;Jin Wang;Aimin Hao;Min Zhao

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在实际废水中,有毒重金属通常与有机配体络合,其脱除目前仍是一个挑战。绿色氧化剂o3在污染物的氧化中得到了广泛的应用,但存在HO·产率对水化学的依赖性和金属回收率低的问题。在此,我们开发了一种新的方法,即电解- o3 -GF-Ti,通过HO·氧化有效地去除络合的Cu(II),并以石墨毡涂覆Ti网(GF-Ti)为阴极同时回收Cu。对于Cu(II)-EDTA解解,该工艺TOC去除率达80%以上,Cu(II)回收率达90%以上,显著高于电解、臭氧化或电解- o3 - ti。阴极o3还原对HO·的生成起着重要的作用,同时促进了o3的分解和HO·探针(对氯苯甲酸)的降解,但对h2o2的生成作用不明显。结合HPLC谱和质谱证据,结合SEM-EDX和XRD分析,对Cu(II)-EDTA的电解- o3 -GF-Ti的机理进行了研究,结果表明,Cu(II)-EDTA的电解- o3 -GF-Ti是一个逐步脱羧的过程,形成的解配Cu(II)中间体在GF-Ti表面被还原为cu0。阴极表征和连续5循环实验结果表明,GF-Ti是一种优良的可再生阴极。与不同螯合剂(硝基三乙酸、柠檬酸盐、酒石酸盐等)络合处理Cu(II),回收率达90%以上,电镀废水回收率达80%以上。该研究为金属配合物的破坏和重金属的回收提供了一种有希望的替代方法。
The removal of toxic heavy metals, which are usually complexed with organic ligands in real wastewater, is still a challenge currently. The green oxidant O3has been widely applied in the oxidation of pollutants, but suffers from the dependency of HO· yield on water chemistry and also low recovery of metals. Here, we developed a new method, namely electrolysis-O3-GF-Ti, for efficiently removing the complexed Cu(II) via HO· oxidation and for simultaneously recovering Cu using graphite felt coated Ti mesh (GF-Ti) as the cathode. For Cu(II)-EDTA decomplexation, this process achieved more than 80% of TOC removal and 90% of Cu(II) recovery, which was significantly more efficient than those of electrolysis, ozonation or electrolysis-O3-Ti. The cathodic O3reduction was responsible for the efficient production of HO· in the process, as proved by the simultaneous enhanced decomposition of O3and degradation of HO· probe (p-chlorobenzoic acid) but insignificant formation of H2O2by electrolysis. Mechanism study with HPLC spectrum and mass spectrometry evidence combined with SEM-EDX and XRD analysis revealed electrolysis-O3-GF-Ti of Cu(II)-EDTA was a stepwise decarboxylation process, and the formed decomplexed Cu(II) intermediates were reduced as Cu0at the GF-Ti surface. The results of cathodic characterization and continuous 5-cycle experiments demonstrated GF-Ti is an excellent renewable cathode. Moreover, over 90% of Cu was recovered in treatment of Cu(II) complexed with different chelators (nitrilotriacetic acid, citrate, tartrate, etc.), and more than 80% from authentic electroplating wastewater. This study would provide a promising alternative for destruction of metal complexes and recovery of heavy metals.
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影响因子: 11.4
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影响因子: 12.8
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紫外和阴极还原活化过硫酸盐增强 Cu-EDTA 光电催化解络和铜回收
DOI: 10.1021/acs.est.6b00632
发表时间: 2016
影响因子: 11.4
作者:
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DOI: 10.1016/j.seppur.2015.10.012
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影响因子: 8.6
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