摘要：SummaryThe carbon-free production of hydrogen from water splitting holds grand promise for the critical energy and environmental challenges. Herein, few-atomic-layers iron (FeFAL) anchored on GaN nanowire arrays (NWs) is demonstrated as a highly active hydrogen evolution reaction catalyst, attributing to the spatial confinement and the nitrogen-terminated surface of GaN NWs. Based on density functional theory calculations, the hydrogen adsorption on FeFAL:GaN NWs is found to exhibit a significantly low free energy of −0.13 eV, indicative of high activity. Meanwhile, its outstanding optoelectronic properties are realized by the strong electronic coupling between atomic iron layers and GaN(10ī0) together with the nearly defect-free GaN NWs. As a result, FeFAL:GaN NWs/n+-p Si exhibits a prominent current density of ∼ −30 mA cm−2at an overpotential of ∼0.2 V versus reversible hydrogen electrode with a decent onset potential of +0.35 V and 98% Faradaic efficiency in 0.5 mol/L KHCO3aqueous solution under standard one-sun illumination.Graphical AbstractDisplay OmittedHighlights•Few-atomic-layers iron was anchored on GaN nanowires as an efficient HER catalyst•The spatial-confinement and N-rich GaN is essential for forming atomic iron layers•Low hydrogen absorption free energy is theoretically revealed over Fe3L:GaN•The device exhibits a prominent performance for PEC water splitting to H2Catalysis; Electrochemical Energy Production; Nanoelectrochemistry; Atomic Electronic Structure; Nanomaterials
