Edge‐Functionalized Graphene Nanoplatelets as Metal‐Free Electrocatalysts for Dye‐Sensitized Solar Cells

Abstract A scalable and low‐cost production of graphene nanoplatelets (GnPs) is one of the most important challenges for their commercialization. A simple mechanochemical reaction has been developed and applied to prepare various edge‐functionalized GnPs (EFGnPs). EFGnPs can be produced in a simple and ecofriendly manner by ball milling of graphite with target substances (X = nonmetals, halogens, semimetals, or metalloids). The unique feature of this method is its use of kinetic energy, which can generate active carbon species by unzipping of graphitic CC bonds in dry conditions (no solvent). The active carbon species efficiently pick up X substance(s), leading to the formation of graphitic CX bonds along the broken edges and the delamination of graphitic layers into EFGnPs. Unlike graphene oxide (GO) and reduced GO (rGO), the preparation of EFGnPs does not involve toxic chemicals, such as corrosive acids and toxic reducing agents. Furthermore, the prepared EFGnPs preserve high crystallinity in the basal area due to their edge‐selective functionalization. Considering the available edge X groups that can be selectively employed, the potential applications of EFGnPs are unlimited. In this context, the synthesis, characterizations, and applications of EFGnPs, specifically, as metal‐free carbon‐based electrocatalysts for dye‐sensitized solar cells (DSSCs) in both cobalt and iodine electrolytes are reviewed.