Large-Area Oxidized Phosphorene Nanoflakes Obtained by Electrospray for Energy-Harvesting Applications

[Image: see text] Bidimensional (2D) materials are nowadays being developed as outstanding candidates for electronic and optoelectronic components and devices. Targeted applications include sensing, energy conversion, and storage. Phosphorene is one of the most promising systems in this context, but its high reactivity under atmospheric conditions and its small-area/lab-scale deposition techniques have hampered the introduction of this material in real-world applications so far. However, phosphorene oxides in the form of low-dimensional structures (2D PO(x)) should behave as an electroresponsive material according to recent theoretical studies. In the present work, we introduce electrospraying for the deposition of stoichiometric and large-area 2D PO(x) nanoflakes starting from a suspension of liquid-phase-exfoliated phosphorene. We obtained 2D PO(x) nanostructures with a mean surface area two orders of magnitude larger than phosphorene structures obtained with standard mechanical and liquid exfoliation techniques. X-ray spectroscopy and high-resolution electron microscopy confirmed the P(2)O(5)-like crystallographic structure of the electrosprayed flakes. Finally, we experimentally demonstrated for the first time the electromechanical responsivity of the 2D P(2)O(5) nanoflakes, through piezoresponse force microscopy (PFM). This work sheds light on the possible implementation of phosphorus oxide-based 2D nanomaterials in the value chain of fabrication and engineering of devices, which might be easily scaled up for energy-harvesting/conversion applications.