Improving the Oxygen Evolution Reaction on Fe₃O₄(001) with Single-Atom Catalysts

Abstract

Doping magnetite surfaces with transition-metal atoms is a promising strategy to improve the catalytic performance toward the oxygen evolution reaction (OER), which governs the overall efficiency of water electrolysis and hydrogen production. In this work, we investigated the Fe 3 O 4 (001) surface as a support material for single-atom catalysts of the OER. First, we prepared and optimized models of inexpensive and abundant transitionmetal atoms, such as Ti, Co, Ni, and Cu, trapped in various configurations on the Fe 3 O 4 (001) surface. Then, we studied their structural, electronic, and magnetic properties through HSE06 hybrid functional calculations. As a further step, we investigated the performance of these model electrocatalysts toward the OER, considering different possible mechanisms, in comparison with the pristine magnetite surface, on the basis of the computational hydrogen electrode model developed by Nørskov and co-workers. Cobalt-doped systems were found to be the most promising electrocatalytic systems among those considered in this work. Overpotential values (∼0.35 V) were in the range of those experimentally reported for mixed Co/Fe oxide (0.2−0.5 V).

Alkali Containing Layered Metal Oxides as Catalysts for the Oxygen Evolution Reaction

“…The OER is an unwanted side reaction in NiO x alkaline batteries, and it has long been found that Fe impurities enhance such a process, [66][67][68][69] with this attracting significant attention to the effects of Fe-doping in NiO x electrodes for OER electrocatalysis in alkaline media. Many studies have indeed shown that Fedoped nickel oxides are promising electrocatalysts for the OER.…”

Insights into the active nickel centers embedded in graphitic carbon nitride for the oxygen evolution reaction

“…6 Transition metals (TMs), especially 3d metals, are the best option as OER catalysts due to their high abundance, affordable price, and high catalytic activity. 7 Among them, nickel is predicted to be the most efficient one. [8][9][10] From the materials science point of view, many efforts have been made in order to improve the performance of TM-based catalysts by modifying their morphology, structure and size, since a strong dependence on their physical form has been reported.…”

“…6 Transition metals (TMs), especially 3d metals, are the best option as OER catalysts due to their high abundance, affordable price, and high catalytic activity. 7 Among them, nickel is predicted to be the most efficient one. 8–10…”

V2O5–Fe3O4/rGO Ternary Nanocomposite with Dual Applications as a Dye Degradation Photocatalyst and OER Electrocatalyst

“…Furthermore, magnetic coral-like Fe 3 O 4 nanoparticles were investigated at different calcining temperatures, displaying the best performance with an overpotential of 234 mV and Tafel slope of 100 mV dec –1 at 450 °C . In a recent theoretical study carried out on the Fe 3 O 4 (001) surface for OER, transition-metal atoms including Co, Cu, Ni, and Ti have been doped on the magnetic surface, and results have predicted an overpotential of about 350 mV for Co-doped Fe 3 O 4 surface in alkaline solution . Immobilized Fe 3 O 4 nanoparticles on Ni-based MOFs (metal–organic frameworks) displayed an overpotential of 295 mV at 10 mA/cm 2 and a Tafel slope of 47.8 mV dec –1 .…”