Abstract

The use of a methanesulfonic acid (MSA) electrolytic system is recommended as a green method for hydrometallurgical recovery of metallic Pb from waste lead-acid batteries (LABs), contributing to the sustainable protection of the ecosystem. Nevertheless, the system's high energy consumption is a current issue due to the substantial overpotential of the oxygen evolution reaction (OER) and competitive anodic oxidation of Pb2+. Herein, we propose an IrFe/nitrogen-doped pyrolytic carbon black (IrFe/NCBp) composite as a novel OER catalyst for the MSA electrolytic system, which demonstrates advanced OER catalytic efficiency and selectivity for H2O oxidation. This can be ascribed to the catalyst's thoughtful design, which enhances the number and uniformity of Ir and Fe species via increasing the specific surface area and employing NCBp as a sustainable substrate. The optimized IrFe/NCBp composite exhibits superior OER performance, with a low 252 mV@10 mA cm-2 overpotential and a 62 mV dec-1 Tafel slope, and excellent durability in a 1 M MSA electrolyte for 30 h operation compared to commercial Ir/C. In contrast to carbon paper (CP) and commercial Ir/C anodes, the anodic reaction of IrFe/NCBp is primarily OER-driven (97%) in 1 M MSA and 0.2 M Pb2+ electrolyte for Pb recovery. This effectively circumvents the high potential oxidation of Pb2+ into PbO2, reducing the electrolytic voltage to 488 kWh for the recovery of 1 ton Pb metal. This work provides a green, low-carbon footprint solution for the MSA electrolytic system, thereby promoting the commercialization of the hydrometallurgical Pb recovery.

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