Waste-Derived Copper-Lead Electrocatalysts for CO2 Reduction

Abstract

It remains a real challenge to control the selectivity of the electrocatalytic CO₂ reduction (eCO₂R) reaction to valuable chemicals and fuels. Most of the electrocatalysts are made of non-renewable metal resources, which hampers their large-scale implementation. Here, we report the preparation of bimetallic copper-lead (CuPb) electrocatalysts from industrial metallurgical waste. The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and Cu_xPb_y electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X-ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu⁰, Cu¹⁺ and Pb²⁺ domains, and no evidence for alloy formation was found. We found a volcano-shape relationship between eCO₂R selectivity toward two electron products, such as CO, and the elemental ratio of Cu and Pb. A maximum Faradaic efficiency towards CO was found for Cu_9.00Pb_1.00, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. In situ Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu¹⁺ and Pb²⁺ domains to metallic Cu and Pb, which boosted the selectivity towards CO by synergistic effects. This work provides a framework of thinking to design and tune the selectivity of bimetallic electrocatalysts for CO₂ reduction through valorization of metallurgical waste.