Development of carbon neutral and sustainable energy sources should be considered as a top priority solution for the growing worldwide energy demand. Photovoltaics are a strong candidate, and more specifically organic photovoltaics (OPV), enabling the design of flexible, light-weight, semi-transparent and low-cost solar cells. However, the active layer of OPV is, for now, mainly deposited from chlorinated solvents, harmful for the environment and for human health. Active layers processed from health and environmentally friendly solvents have over recent years formed a key focus topic of research, with the creation of aqueous dispersions of conjugated polymer nanoparticles arising. These nanoparticles are formed from organic semi-conductors (molecules and macromolecules) initially designed for organic solvents. The topic of nanoparticle OPV has gradually garnered more attention, up to a point where in 2018 it was identified as a "trendsetting strategy" by leaders in the international OPV research community. Hence, this review has been prepared to provide a timely roadmap of the formation and application of aqueous nanoparticle dispersions of active layer components for OPV. We provide a thorough synopsis of recent developments in both nanoprecipitation and miniemulsion for preparing photovoltaic inks, facilitating readers in acquiring a deep understanding of the crucial synthesis parameters affecting particle size, colloidal concentration, ink stability, and more. This review also showcases the experimental levers for identifying and optimizing the internal donor-acceptor morphology of the nanoparticles, featuring cutting-edge X-ray spectromicroscopy measurements reported over the past decade. The different strategies to improve the incorporation of these inks into OPV devices and to increase their efficiency (to the current record of 7.5%) are reported, in addition to critical design choices of surfactant type and the advantages of single-component vs. binary nanoparticle populations. The review naturally culminates by presenting the upscaling strategies in practice for this environmentally friendly and safer production of solar cells.

Polymer films with hierarchical micro- and nano-porosities were prepared by combining the fast solvent evaporation "Breath Figure" (BF) method, exhibiting a highly regular honeycomb micro-porous texture, with the additional nanoscale self-assembly of polylactide-block-polystyrene (PLA-b-PS) diblock copolymers, PLA being used thereafter as a sacrificial component for nano-porosity.