Atomic-scale Ru anchored on chromium-shavings as a precursor for a pH-universal hydrogen evolution reaction electrocatalyst

Abstract

In the leather manufacturing industry, the management of substantial quantities of solid waste containing chrome shavings remains a formidable challenge. Concurrently, there is a pressing need for the development of pH-universal and economically viable electrocatalysts for the hydrogen evolution reaction (HER). In response to these intertwined challenges, this study proposes an innovative approach wherein the amino groups present on the surface of chrome shavings are utilized to immobilize single ruthenium atoms during pyrolysis, thereby facilitating the synthesis of hydrogen evolution electrocatalysts. The optimized sample, denoted as CN/Cr₂O₃/Ru-1, demonstrates exceptional electrocatalytic performance, exhibiting an ultra-low overpotential of −28 mV in 1.0 M KOH at a current density of 10 mA cm⁻², and it also exhibits good performance in acidic and neutral electrolytes. Importantly, these overpotentials surpass those reported for many previous ruthenium-based catalysts. Density functional theory (DFT) calculations elucidate that both oxygen (O) and chromium (Cr) moieties within Cr₂O₃ can engage in favorable interactions with the coordination patterns of the ruthenium (Ru) atoms, thereby elucidating the synergistic enhancement conferred by the chromium element in CN/Cr₂O₃/Ru, which ultimately facilitates and promotes the catalytic activity of the ruthenium atoms serving as the catalytic center. This facile synthesis route not only presents a green solution for addressing waste chromium pollutants but also offers a promising avenue for the development of high-performance, cost-efficient electrocatalysts.