Overcoming the Limitation of Ionomers on Mass Transport and Pt Activity to Achieve High-Performing Membrane Electrode Assembly.

The membrane electrode assembly (MEA) is one of the critical components in proton exchange membrane fuel cells (PEMFCs). However, the conventional MEA cathode with a covered-type catalyst/ionomer interfacial structure severely limits oxygen transport efficiency and Pt activity, hardly achieving the theoretical performance upper bound of PEMFCs. Here, we design a noncovered catalyst/ionomer interfacial structure with low proton transport resistance and high oxygen transport efficiency in the cathode catalyst layer (CL). This noncovered interfacial structure employs the ionomer cross-linked carbon particles as long-range and fast proton transport channels and prevents the ionomer from directly covering the Pt/C catalyst surface in the CL, freeing the oxygen diffusion process from passing through the dense ionomer covering layer to the Pt surface. Moreover, the structure improves oxygen transport within the pores of the CL and achieves more than 20% lower pressure-independent oxygen transport resistance compared to the covered-type structure. Fuel-cell diagnostics demonstrate that the noncovered catalyst/ionomer interfacial structure provides exceptional fuel-cell performance across the kinetic and mass transport-limited regions, with 77% and 67% higher peak power density than the covered-type interfacial structure under 0 kPa of oxygen and air conditions, respectively. This alternative interfacial structure provides a new direction for optimizing the electrode structure and improving mass-transport paths of MEA.