A Novel Anodic Heterostructure Based on Commercial 1J50 Permalloy for Urea‐Assisted Water Splitting

Abstract A commercially available magnetic metallic material, 1J50 permalloy, was employed in this work to fabricate a novel anode for the urea‐assisted electrocatalysis. Featuring the simple surface treatments of electrode substrate, including elemental leaching to modulate the Ni/Fe ratio in KSCN solution and subsequent chronopotentiometric aging in test solution, the as‐fabricated anode can deliver a current density of 10 mA cm −2 at 1.355 V (RHE) in 1 M KOH solution containing 0.33 M urea, without suffering all the disadvantages of traditional anodes, e.g., complicated fabrication process and impossible substrate regeneration. It was evidenced that Ni can be sustained at first and oxidized subsequently to form UOR‐active species in divalent or trivalent states; whereas Fe, after elemental leaching, can be mainly oxidized to form Fe 3 O 4 with acceptable electric conductivity, and the remnant is incorporated into the lattices of Ni‐containing species for Ni–Fe synergy. Thus, the outstanding UOR performance is directly associated with the hetero‐structure composed mainly of the UOR‐active LDH decorated with the electrically conductive Fe 3 O 4 particles and other UOR‐enhancing (oxy)hydroxides.