Abstract: The advantages of zero emission and high energy efficiency make proton exchange membrane fuel cells (PEMFCs) promising options for future energy conversion devices. To address the cost issue associated with Pt-based electrocatalysts, considerable effort over the past several years has been devoted to catalyst surface modification by means of novel electrocatalysts, such as solid catalysts with an ionic liquid layer (SCILL), which improves both the oxygen reduction reaction (ORR) activity and durability. However, despite numerous reports of dramatically enhanced ORR activity, as determined via the rotating disk electrode (RDE) method, few studies on the application of SCILLs in membrane electrode assembly (MEA) have been reported. The underlying reason lies in the well-acknowledged technological gap between half-cells and full-cells, which originates from the disparate microenvironments for three phase boundaries. Therefore, the objective of this review is to compare the detailed information about improvements in fuel cell performance in both half- and full-cells, thus increasing the fundamental understanding of the mechanism of SCILL. In this review, the concept of SCILL and its origin are introduced, the outstanding electrochemical performance of SCILL catalysts in both RDE and MEA measurements is summarized, and the durability of SCILL catalysts is analysed. Subsequently, proposed mechanisms for the enhanced ORR activity in half-cells, the improved oxygen transport in full-cells and the boosted stability of SCILL catalysts are discussed, while the effects of the IL chemical structure, IL loading as well as the operating conditions on the performance and lifetime of SCILL catalysts are assessed. Finally, comprehensive conclusions are presented, and perspectives are proposed in the last section. It is believed that the new insight presented in this review could provide guidance for the further development of SCILLs in low-Pt PEMFCs.

Key words: Solid catalysts with ionic liquid layer, Proton exchange membrane fuel cells, Membrane electrode assembly, Oxygen reduction reaction activity, Oxygen transport in cathode catalyst layers, Catalyst durability