Targeted Decomplexation of Metal Complexes for Efficient Metal Recovery by Ozone/Percarbonate

Traditional methods cannot efficiently recover Cu from Cu(II)- EDTA wastewater and encounter the formation of secondary contaminants. In this study, an ozone/percarbonate (O3/SPC) process was proposed to efficiently decomplex Cu(II)-EDTA and simultaneously recover Cu. The results demonstrate that the O3/SPC process achieves 100% recovery of Cu with the corresponding kobs value of 0.103 min-1 compared with the typical center dot OH-based O3/H2O2 process (81.2%, 0.042 min-1). The carbonate radical anion (CO3 center dot-) is generated from the O3/SPC process and carries out the targeted attack of amino groups of Cu(II)-EDTA for decarboxylation and deamination processes, resulting in successive cleavage of Cu-O and Cu-N bonds. In comparison, the center dot OH-based O3/H2O2 process is predominantly responsible for the breakage of Cu-O bonds via decarboxylation and formic acid removal. Moreover, the released Cu(II) can be transformed into stable copper precipitates by employing an endogenous precipitant (CO32-), accompanied by toxic-free byproducts in the O3/SPC process. More importantly, the O3/SPC process exhibits excellent metal recovery in the treatment of real copper electroplating wastewater and other metal-EDTA complexes. This study provides a promising technology and opens a new avenue for the efficient decomplexation of metal-organic complexes with simultaneous recovery of valuable metal resources.

Automated summary

Traditional methods are not efficient in recovering Cu from Cu(II)-EDTA wastewater and result in the formation of secondary contaminants. This study proposes an ozone/percarbonate (O3/SPC) process that can efficiently decomplex Cu(II)-EDTA and recover Cu simultaneously. The results show that the O3/SPC process achieves 100% Cu recovery with a kobs value of 0.103 min-1, compared to 81.2% recovery and a kobs value of 0.042 min-1 for the typical ·OH-based O3/H2O2 process. The O3/SPC process generates the carbonate radical anion (CO3·-) to selectively attack the amino groups of Cu(II)-EDTA, leading to the cleavage of Cu-O and Cu-N bonds.