High energy-efficiency decomplexation of metal-complexes by H*-mediated electro-reduction on hydroxyphenyl Co-porphyrin catalysts.

ABSTRACT

Electrochemical reduction of metal-organic complex pollutants has been recognized as an environmental benign method that operates at mild condition. However, the selective reduction of metal complexes and energy consumption in cathodic process are still a big challenge. Herein, we found that hydroxyphenyl Co-porphyrin catalyst (CoTH@NG) realizes the highly selective decomplexation of metal-organic complexes by H* -mediated reduction, and simultaneously the impressive recovery efficiency of metal ions. Density functional theory (DFT) confirms the generation and capturing ability of H* on CoTH@NG, verifying the dominant role of H* -mediated reduction in the selective decomplexation of Cu-EDTA. CoTH@NG realizes the superior energy efficiency for Cu-EDTA removal (279.3 g kWh-1 of EEOCu-EDTA) and Cu recovery (48.6 g kWh-1 of EEOCu), which are remarkably 3.3 × 102 and 9.7 × 102 times higher than traditional carbon cloth electrode. Moreover, the recovered Cu0(s) nanowires on the electrode surface can be efficiently regenerated in HCOOH by a galvanic reaction through the electron channel of CoTH@NG, regenerating catalytic electrode. This is one of the pioneer studies on H* -mediated electro-reduction decomplexation of metal-complexes, metal recovery, and electrode regeneration on CoTH@NG, which providing a technical strategy for developing efficient electrocatalytic system for pollution control. Environmental Implication Metal complexes is a dramatic increase in the electroplating and mining industries, and seriously affect both public health and environmental sustainability. Our work reported a new hydroxyphenyl Co-porphyrin catalyst (CoTH@NG) which achieves the selective decomplexation of metal-organic complexes, and simultaneously the recovery of metal ions. CoTH@NG realizes the superior energy efficiency for Cu-EDTA removal (279.3 g kWh-1) and Cu0(s) recovery (48.6 g kWh-1), which are remarkably 3.3 × 102 and 9.7 × 102 times higher than traditional carbon cloth electrode. Moreover, the recovered Cu0(s) can be efficiently regenerated in HCOOH by a galvanic reaction through the electron channel of CoTH@NG, regenerating catalytic electrode.