Unveiling the Local Effects of PTL Passivation in PEM Electrolyzers through Gas and Current Mapping Using Operando Neutron Radiography and Polarized Neutron Imaging

Anodic Ti-based porous transport layers (PTLs) are paramount for advancing high-efficiency proton exchange membrane water electrolyzers (PEMWEs). One of the major challenges with the development of PEMWE is the PTL/catalyst layer interface passivation, which is commonly alleviated by coating precious metals such as Pt. Herein, we report, for the first time, the usage of polarized neutron imaging (PNI) on a half-half PTL approach to investigate current distribution inside the PTL layer under the influence of Ti passivation under PEMWE operando condition. First, the electrochemical study of PEMWE reveals an obvious advantage of Pt coating in preventing Ti passivation by showing 822 mV less overpotential at 1 A cm^-2 (1.771 V) for the superior sample (Pt-coated PTL) compared to the PEMWE with pristine Ti PTL (2.539 V). Second, it is confirmed that using ex situ electronic and structural characterizations, Ti passivation cannot be recognized, suggesting a temporary passivation process in an operating PEMWE. Employing PNI for operando mapping of the current distribution inside the PEMWE shows that most of the electrical current favors the Pt-coated PTL, perfectly aligned with the results obtained from the high-resolution operando neutron radiography in which around 60% of the produced oxygen was found in the Pt-coated PTL.