One-step preparation of anti-ferromagnetic single-atom nickel to improve oxygen evolution reaction of photoelectrochemical water splitting

Abstract

Noble metal single-atom catalysts (SACs) have been extensively investigated due to their unique electronic structure and high-efficiency catalytic performance. However, there are relatively few studies on the preparation of non-noble metal single atoms and their application in oxygen evolution reaction (OER). In this paper, nickel single-atom catalyst was prepared using a facile one pot method. Ni-SAC-2.5% showed uniform SACs distribution and anti-ferromagnetic property as evidenced by the aberration-corrected high resolution electron microscopy and the first-principle calculations, achieving the lowest overpotential of 220 mV (10 mA/cm2) and stable performance in 1 M KOH solution. Meanwhile, it exhibited the largest specific capacitance value of 1.77 mF/cm2 and the lowest charge transfer resistance value of 40.75 Ω due to the accelerated kinetic process. First-principle calculations further confirmed the lowest computed overpotential of 0.54 eV for Ni-SAC-2.5%. However, Ni small clusters and nanoclusters with superparamagnetic performance were observed when the Ni content was further increased to 3.5% and 4.5%, resulting in higher overpotentials of 0.85 eV and 2.01 eV for OER process as indicated by the theoretical simulation. This paper provides a facile method to prepare non-noble metal SACs and useful guidance for designing high performance OER catalysts.