Letter

http://pubs.acs.org/journal/aelccp

Crack-Engineered Microporous Layer for

Mitigating Cathode Flooding in Polymer
Electrolyte Fuel Cells
Young Je Park,□ Won Young Choi,□ Seong Hyun Park,□ Hyunguk Choi, Seo Won Choi,
Jy-Young Jyoung, Eunsook Lee, Jae-ll Park, Min Jae Ko,* Kang Taek Lee,* and Chi-Young Jung*
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sı Supporting Information

ABSTRACT: Crack engineering within the microporous layer

(MPL) of the gas diffusion layer (GDL) has emerged as a
promising strategy to alleviate severe cathode flooding in
polymer electrolyte fuel cells (PEFCs), especially under high
current operation. Here, we report a connected-crack MPL
architecture that forms continuous liquid water highways,
extending from the catalyst layer (CL) to the GDL backing
layer, effectively separating the liquid/gas transport. Three-
dimensional reconstruction using X-ray computed tomography
reveals that the microengineered cracks significantly reduce
flooding at the CL-MPL interface by providing efficient
drainage. Compared to the noncrack GDL, the connected-
crack GDL (C-GDL) exhibits 20% higher peak power density of
1.23 W cm−2. Pore-scale simulations further validate the antiflooding capabilities of C-GDL, showing a 25-fold enhancement
in water removal. This crack-engineered GDL thus offers an efficient and scalable route to water management challenges,
enabling robust and high-performance PEFCs suitable for heavy-duty vehicle electrification.

A chieving net-zero carbon emissions has become a

global priority, particularly for sectors with substantial
greenhouse gas outputs, e.g., heavy-duty transporta-
tion, where decarbonization remains challenging. In response,
efforts have been dedicated to identifying the primary sources
of liquid water accumulation.13−17 One source of liquid water
accumulation arises from the condensation of water vapor,
which predominantly occurs in the macro-porous backing layer
significant efforts have been directed toward deploying (BL) of the GDL.13−15 During PEFC operation, water vapor
hydrogen (H2) technologies based on renewables, recognizing diffuses from the CL toward cooler regions of the GDL,
the polymer electrolyte fuel cells (PEFCs) as promising particularly beneath the BP ribs, where condensation occurs
enablers for rendering the transportation sector remarkably due to the local saturation level. Along with the operation time,
cleaner. Unlike lithium-ion batteries, PEFCs offer distinctive the resulting liquid water further accumulates, filling the pores
advantages, including refueling time below 5 min and driving and subsequently obstructing gas transport pathways. More
ranges exceeding 300 miles.1 These attributes make them recently identified source is the interfacial condensation
viable power sources for heavy-duty vehicles (HDVs) with between the CL and the microporous layer (MPL) of
demanding, power-intensive operations in harsh environments. GDL.16,17 The interfacial gaps, induced by the surface
However, the development of robust PEFC designs remains roughness of CL and MPL, provide numerous sites for liquid
essential to sustain high power outputs over extended
water buildup, as illustrated in Scheme 1, thus leading to a
operating periods.2−5
During high-current operation, water management in the
cathode is frequently compromised by severe liquid water Received: April 18, 2025
flooding, which obstructs the gas transport pathways from the Revised: May 30, 2025
flow channels carved in the bipolar plate (BP) through the gas Accepted: June 5, 2025
diffusion layer (GDL) to the catalyst layer (CL).6,7 This
blockage limits oxygen (O2) transport and results in ceaseless
voltage decay.8−12 To address these challenges, extensive
© XXXX The Authors. Published by
American Chemical Society https://doi.org/10.1021/acsenergylett.5c01202
3241 ACS Energy Lett. 2025, 10, 3241−3248
ACS Energy Letters http://pubs.acs.org/journal/aelccp Letter

Scheme 1. Illustration of the PEFC Structures and CL-MPL comprehensive understanding of flooding mechanisms within
Interfacial Gaps as Primary Sources of Liquid Water the MPL and devising robust antiflooding strategies largely
Flooding at the Cathode underestimated, or even with MPLs, often lacked precise
control over the crack penetration depth, which may play as a
critical factor governing water removal capacity. Intricately
smaller pore sizes and greater rigidity of MPLs pose further
obstacles to direct perforation.26−28 In this Letter, we propose
an engineered connected-crack MPL structure as a more
practicable strategy to create additional water evacuation
channels. These cracks effectively act as water highways,
bridging the CL−MPL and MPL−BL interfaces and facilitating
improved drainage in low-temperature, high-humidity, and
high-current operations. We used advanced X-ray computed
tomography (X-CT) to visualize and quantify the three-
dimensional (3-D) crack morphology followed by systematic
higher O2 transport resistance and lower limiting current electrochemical performance evaluations. Pore-scale simula-
density. In either case, water condensation is further intensified tions further elucidate the benefits of this connected-crack
with an increase in current density, as consequence of lower GDL design, which significantly reduces water flooding,
temperature and insufficient water drainage. This results in the enhances power output, and offers robust operating stability.
formation of continuous water films or clusters until sufficient By providing a straightforward and scalable solution to critical
pressure is generated to achieve a breakthrough. Therefore, the water-management challenges, this design holds promise for
innovations in microstructure and surface properties of the advancing emerging PEFC technologies in HDVs.
GDL are crucial for reducing the water breakthrough pressure. The depth and continuity of cracks were experimentally
Recent efforts have concentrated on modifying the GDL controlled by the carbon binder contents and ramping rates
parameters related to reactant transport, such as patterning the during the heat-treatment procedure, as shown in Figure 1a. By
hydrophilic−hydrophobic domains,18,19 creating the artificial reducing the carbon binder content in the MPL slurry, the
perforations,19−21 introducing cracks within the MPL22−24 and cracking intensity during heat treatment governed by binder
gradient pore structure of MPL25 to enhance the liquid water concentration was effectively regulated in Figures S1−S3 and
removal. Forner-Cuenca et al. were the first to tailor surface Table S1. Due to seamless crack initiation and propagation
wettability via using a radiation grafting method, successfully arising from the weak interparticle cohesion, the connected
creating the hydrophilic patterns arranged in a straight-line cracks in connected-crack GDL (C-GDL) extended continu-
array.18 The hydrophilic lines acted as a liquid water reservoir, ously from the CL-MPL interface to the MPL-BL interface. In
while the hydrophobic lines remained dry and thus served as contrast, the cracks in disconnected-crack GDL (D-GDL) are
the gas transport pathways. Building upon this approach, Janus disconnected, with propagation limited to within the MPL,
GDL concept was developed using a layer-by-layer filtration without reaching the MPL-BL interface. For evaluation of the
method for surface modification, which created an inherent MPL microstructures, cross-sectional X-CT imaging was
wettability gradient that promotes spontaneous, directional conducted with three types of GDLs, i.e., noncrack GDL
liquid water transport.19 However, these approaches suffer (N-GDL), D-GDL, and C-GDL, as shown in Figure 1b. To
from poor precision and scalability due to the complexity of analyze the 3-D microstructure, the X-CT reconstruction
their manufacturing procedures. To address this issue, process was conducted, as illustrated in Figure S4. Figure 1c
substantial efforts have been directed toward developing a displays the 3-D reconstructed microstructures of the three
more straightforward solution, that involves creating suffi- GDL types, featuring their distinct crack morphologies. The C-
ciently large holes within the BL, thereby increasing pore size GDL exhibited the connected cracks that are visually evident,
and enhancing the antiflooding performance of the GDL. extending into the BL region, in contrast to the more confined
Csoklich et al. demonstrated that laser-perforated structures in cracks observed in the D-GDL. Topological characterization of
BL significantly reduced the mass transport resistance (MTR) the MPL surfaces is further presented in Figure S5, revealing
by promoting the removal of liquid water, although membrane that the cracks in C-GDL penetrate deeper compared to those
dehydration was identified as a limiting factor.20 More recently, in D-GDL. These findings enabled a clear classification of the
Lin et al. proposed quadrilaterally patterned perforations, cracks as either connected or disconnected, based on their
which significantly improved in-plane permeability and penetration depth into the BL region (Figure 1d).
reduced liquid water saturation.21 Although the PEFC Figure 1e shows the quantified solid volume fraction as a
performance was evaluated under somewhat impractical function of the distance from the cathode derived from the
conditions (small electrode areas: 4−5 cm2 and high air flow reconstructed microstructures. The similar MPL penetration
rates: stoichiometric ratios of 3−18), both studies have depths, BL starting points, and solid volume fraction profiles
successfully demonstrated higher power densities exceeding confirm the structural comparability among the three GDL
20%. In parallel, several studies attempted to leverage cracks types. Pore size distribution, determined by mercury intrusion
within the MPL to facilitate gas and water transport porosimetry (Figure 1f), revealed similar pore sizes across the
behaviors.22−25 They have investigated the impact of crack samples ranging from 12 to 27 μm. These differences are
areal ratio, crack elongation morphology, and MPL graded attributed to the presence of cracks in the D-GDL and C-GDL,
porosity on the high-current performance as well as catalyst whereas the N-GDL exhibited no visible cracks. Additionally,
durability. the MPL surface wettability was intentionally designed to be
Despite these advancements, prior research and develop- comparable across all of the GDLs, as shown in Figure 1g.
ment efforts have either focused on the BLs, leaving a Surface roughness measurements are 4.4, 4.3, 3.8, and 0.59 μm
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ACS Energy Lett. 2025, 10, 3241−3248
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Figure 1. Characterization of a three-type GDL. (a) Schematic representation of a three-type GDL manufactured procedure. (b) Cross-
sectional X-CT image. (c) 3-D reconstructed microstructure of the N-GDL, D-GDL, and C-GDL. Two-phase transport parameters in GDL
consisted of (d) crack depth, (e) solid volume fraction, (f) pore size distribution, (g) MPL surface wettability, and (h) surface roughness. (i)
Radar graph of comprehensive characteristics of the three-type GDL.

for N-GDL, D-GDL, C-GDL, and the cathode CL, respectively presents a comprehensive analysis of the GDL characteristics
(Figure 1h). The MPL, with its significantly higher roughness by using a radar chart. This analysis confirms that, apart from
than the CL, is known to contribute to the interfacial differences in crack microstructures, all other parameters
compressed cell configurations, a transparent cell was designed relevant to water management, including MPL porosity,
to replicate the channel and rib structure of the BP for the surface roughness, wettability, and MPL penetration depth,
electrochemical test (Figure S6). The formation of interfacial remain consistent across the three GDL types.
gaps, induced by the surface roughness, was observed across all Subsequently, single cell tests were carried out on all three
GDL types, as shown in Figure S7. Consequently, Figure 1i GDL types to evaluate their electrochemical performance, as
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well as corresponding MTRs, along with their underlying condensed water trapped in 200 to 300 μm interfacial gaps
mechanisms. Figure 2a−c shows the polarization curves between the catalyst layer and MPL, thereby improving water
management during fuel cell operation.27,31
To identify the dominant resistance components during cell
operation, electrochemical impedance spectroscopy (EIS)
analysis was carried out. Nyquist plots were fitted using an
equivalent circuit model (Figure S9), and the fitting results are
presented in Figures S10 and S11. As quantified in Figure 2g,
the MTR was identified as the dominant contributor to total
resistance, which also included the HFR and charge transfer
resistance (CTR). Under LDV conditions at RH 120%, the
MTR for C-GDL was 277 mΩ·cm2, which is 25 times lower
than the 7048 mΩ·cm2 measured for the N-GDL (Table S4).
Moreover, as the RH increased, the impact of water flooding
became more prominent, resulting in significant variations in
the MTR across different GDLs. For the N-GDL, increasing
the RH from 40% to 120% led to a 10-fold increase in the
MTR under LDV conditions and a 3-fold increase under HDV
conditions. In contrast, the corresponding MTR of C-GDL
increased by only 4-fold under LDV conditions and 2-fold
under HDV conditions. The pronounced sensitivity of N-GDL
to humidity indicates potential limitations for long-term
operations, particularly where durability under high RH
Figure 2. Electrochemical analysis in the active area of a 25 cm2 conditions is critical. To further distinguish the local O2
single cell with N-GDL, D-GDL, and C-GDL. H2−air polarization transport resistance within the electrodes and GDL, pressure-
curves under LDV testing conditions at 80 °C, 150 kPaabs gas dependent resistance measurements were performed using
pressure, and (a) RH 120%, (b) RH 80%, and (c) RH 40%. H2−air limiting current techniques, as shown in Figure 2h.32,33 The
polarization curves under HDV testing conditions at 90 °C, 250 pressure-dependent resistance (slope) was consistent across all
kPaabs gas pressure, and (d) RH 120%, (e) RH 80%, and (f) RH GDL types, indicating that the crack microstructures did not
40%. (g) Resistances obtained from EIS analysis at a current
significantly affect the O2 transport pathway. However, these
density of 2.2 A cm−2. (h) Local oxygen transport resistance splits
into pressure-dependent regions (slope). microstructural differences have a substantial impact on the
transport of liquid water, which in turn leads to the observed
performance variations.
obtained under light-duty vehicle (LDV) testing conditions As presented in Figure 3, the stability tests over 25 h
(80 °C, 150 kPa) at varying relative humidity (RH) levels. At operation were conducted to evaluate the antiflooding
low current densities (<1.0 A·cm−2), where electrode kinetics characteristics of the three GDL types. Figure 3a shows the
dominate, performance differences across GDL types and RH stability of each GDL during an antiflooding test conducted at
conditions were negligible.29 However, at 0.5 V under RH a constant cell voltage of 0.6 V under HDV conditions of the
120%, the current densities for C-GDL, D-GDL, and N-GDL cell temperature at 90 °C with RH 40% under 250 kPa. This
were 2.46, 1.97, and 1.86 A·cm−2, respectively, indicating that test was designed to assess the relationship between crack
the C-GDL exhibited a 32% higher performance compared to microstructure and water management during long-term fuel
the N-GDL (Figure 2a). The peak power density of C-GDL cell operation.19 Unlike the C-GDL, both the N-GDL and D-
reached 1.23 W cm−2, about 1.3 times higher than that of N- GDL exhibited pronounced drops in current density, with the
GDL (0.946 W cm−2), with the performance gap widening at N-GDL showing more frequent and larger drops magnitude.
higher RH and lower cell voltages (Table S2). Compared with These fluctuations indicate the occurrence of liquid water
N-GDL, the D-GDL and C-GDL exhibited a slight increase of accumulation and poor drainage, which disrupted cell
high frequency resistance (HFR) by 4−6 mOhm·cm2, performance. As quantified in Figure 3b, the current density
primarily due to the MEA dehydration.30 A similar trend was drop frequencies for C-GDL, D-GDL, and N-GDL were 0.08,
observed under HDV testing conditions at 90 °C and 250 kPa 1.12, and 2.88 h−1, respectively. The frequency observed for C-
(Figure 2d−f and Table S3). It is worthwhile noting that the GDL was 36 times lower than that of N-GDL, underscoring its
increase of contact resistances after the use of N-GDL, D- superior water management capability. The frequent and
GDL, and C-GDL, either at the MPL-BL interface or at the severe current density drops in N-GDL signify a limited ability
MPL/CL interface, is expected to be negligibly lower, as the to effectively remove accumulated liquid water, leading to
HFR differences are below 2 mOhm·cm2 under HDV performance instability. In contrast, C-GDL demonstrated
conditions. Following an accelerated stress test, a decrease in highly stable two-phase transport of reactants and products,
oxygen reduction reaction kinetics, electrochemically available attributed to the presence of connected cracks that facilitated
surface area (ECSA), and cell performance were determined efficient liquid water drainage. Figure 3c presents the
with crack formation. Both C-GDL and N-GDL MEAs performance degradation observed after the antiflooding test
exhibited similar losses in mass activity (C-GDL: 43%, N- for each GDL. The current density decreased from 1.15 to 0.93
GDL: 45%), ECSA (C-GDL: 71%, N-GDL: 72%), and A·cm−2 for N-GDL, from 1.14 to 1.03 A·cm−2 for D-GDL, and
performance (C-GDL: 29%, N-GDL: 27%), indicating that from 1.27 to 1.19 A·cm−2 for C-GDL. These changes
crack formation did not accelerate degradation (Figure S8). correspond to reduction rates of 19.4%, 9.6%, and 6%,
This highlights that continuous cracks facilitate the removal of respectively. The higher degradation rates observed in N-
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Figure 3. Stability test for long-term fuel cell operation for targeting HDV applications. (a) Antiflooding test at 90 °C, 250 kPaabs gas
pressure, and RH 40% for 25 h with a constant voltage at 0.6 V. (b) Distribution of current density drops of drainage peaks of N-GDL, D-
GDL, and C-GDL. (c) Performance decrease rate after conducting an antiflooding test.

GDL and D-GDL were exacerbated by severe flooding, which three GDL types. These trends align with the current density
impaired mass transport and increased resistance under HDV drop frequencies associated with liquid water accumulation, as
conditions. These results indicate the critical role of connected shown in Figure 3a. When a substantial amount of liquid water
cracks in the MPL for enhancing antiflooding performance. accumulates near the MPL surface, it forms a barrier to
The connected crack network in C-GDL facilitates the rapid transport of the O2 at the triple-phase boundary. This
discharge of condensed liquid water, preventing excessive phenomenon results in the performance degradation at high
accumulation at the CL-MPL interface. This enhanced water current densities. However, the presence of separate, dedicated
management significantly improves the operational stability of pathways for gas and liquid transport facilitated by the
PEFCs under both LDV and HDV conditions. connected cracks of C-GDL effectively migrates liquid water,
Finally, pore-scale flow simulations were conducted to preventing flooding and thus maintaining efficient O2 transport
visualize liquid water transport at varying saturation levels, as and stable cell performance under heavy operational loads.
presented in Figure 4a. In the N-GDL, liquid water Herein, we present a novel strategy to mitigate cathode
predominantly migrates through the micropores within the flooding by engineering the MPL with controllable cracks.
MPL, resulting in a relatively lower flow velocity of primarily Unlike previous approaches focused on the BL of GDL, our
below 0.1 m s−1. In contrast, both the D-GDL and C-GDL design integrates cracks extending continuously from the MPL
enabled faster liquid water transport due to the presence of to the backing, creating water highways that effectively remove
larger pores formed by cracks. Notably, the continuous crack excess liquid water during high-current operation. 3-D X-ray
network observed in C-GDL significantly enhances water tomography revealed large interfacial gaps (75−328 μm in
transport efficiency, surpassing that of D-GDL. The accumu- diameter) at the CL−MPL interface, serving as primary
lated liquid water at each specified saturation level, quantified flooding sites. Among the various configurations (no crack,
as the liquid volume per unit cubic volume, is depicted in disconnected crack, connected crack), the connected-crack
Figure 4b. For the N-GDL, liquid water tends to accumulate GDL (C-GDL) achieved a peak power density of 1.23 W·cm−2
within the micropores of MPL, which can impede efficient and a 25-fold higher liquid water transport than the
reactant gas transport. In comparison, the D-GDL and C-GDL noncracked GDL at 2.2 A·cm−2. Antiflooding tests further
exhibit reduced liquid water saturation within the MPL region, confirmed significantly fewer and smaller current-density drops
attributable to the presence of cracks that provide alternative with the C-GDL. Digital twin analysis elucidated the
pathways for liquid drainage. Among the three GDLs, the C- underlying mechanism, showing that the connected cracks
GDL exhibited superior liquid water removal capability, as the facilitate swift water removal at interfacial gaps, thereby
connected crack network acts as effective water drainage lowering local saturation. Overall, these findings highlight
channels, that direct water efficiently toward the BL. As the connected-crack MPL designs as an effective, scalable solution
overall saturation level increases, the differences in liquid water for advanced cathode water management, offering improved
saturation near the MPL become more pronounced across the performance, greater operational stability, and a valuable
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Figure 4. Pore-scale flow simulation of a three-type GDL. (a) Liquid saturation fraction in the through-plane direction from MPL surface to
bipolar plate. (b) Velocity of liquid transport based on the pore-scale simulation.

complement to current GDL-focused flood-mitigation strat- 120%, 80%, and 40%; EIS fitting results tested under
egies. LDV testing conditions at 80 °C, 150 kPaabs gas

■ ASSOCIATED CONTENT
Data Availability Statement
pressure, and RH 120%, 80%, and 40% (PDF)

The data that support the major findings of this study are
available in the manuscript or the Supporting Information.
■ AUTHOR INFORMATION
Corresponding Authors
Further data including raw data are available from the
corresponding authors upon reasonable request. Min Jae Ko − Department of Chemical Engineering and
Department of Battery Engineering, Hanyang University,
* Supporting Information
sı
Seoul 04763, Republic of Korea; orcid.org/0000-0002-
The Supporting Information is available free of charge at
4842-3235; Email: [email protected]
https://pubs.acs.org/doi/10.1021/acsenergylett.5c01202.
Kang Taek Lee − Department of Mechanical Engineering,
Fabrication procedure of the GDLs with crack- KAIST, Daejeon 34141, Republic of Korea; KAIST
engineered MPLs; Characterization; Tomographic Graduate School of Green Growth and Sustainability,
methodology based on MIP; Electrochemical character- Daejeon 34141, Republic of Korea; orcid.org/0000-0002-
ization; Schematic representation of the tomographic 3067-4589; Email: [email protected]
process from X-ray microscopy to 3-D reconstruction; Chi-Young Jung − Hydrogen Research and Demonstration
Topological images of cracks and average crack depth Center, Hydrogen Energy Institute, Korea Institute of Energy
(Davg) obtained using a 3-D laser confocal microscope; Research (KIER), Jeollabuk-do 56332, Republic of Korea;
3-D topological profiles of the rib and channel structures Department of Energy Engineering, University of Science and
in a transparent cell and practical 25 cm2 single cell Technology, Yuseong-gu, Daejeon 34113, Republic of Korea;
obtained via laser confocal microscope; Interfacial gaps orcid.org/0000-0003-3393-2333; Email: cyjung@
of three-type GDLs under the compressed catalyst- kier.re.kr
coated-membrane (CCM) configuration; Schematic
representation of an equivalent circuit model for data Authors
fitting; The total resistance consists of HFR, CTR and Young Je Park − Hydrogen Research and Demonstration
MTR; EIS fitting results tested under HDV testing Center, Hydrogen Energy Institute, Korea Institute of Energy
conditions at 90 °C, 250 kPaabs gas pressure, and RH Research (KIER), Jeollabuk-do 56332, Republic of Korea;
3246 https://doi.org/10.1021/acsenergylett.5c01202
ACS Energy Lett. 2025, 10, 3241−3248
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W.Y.C., S.H.P., M.J.K., K.T.L., and C.-Y.J. Matsumoto, Y.; Hayashida, H.; Nozaki, H.; Shinohara, T.; Kato, S. 3D
Notes water management in polymer electrolyte fuel cells toward fuel cell
The authors declare no competing financial interest. electric vehicles. ACS Energy Lett. 2023, 8, 3485−3487.

■ ACKNOWLEDGMENTS
This work was conducted under the framework of the
(16) Simon, C.; Hasché, F.; Gasteiger, H. A. Influence of the gas
diffusion layer compression on the oxygen transport in PEM fuel cells
at high water saturation levels. J. Electrochem. Soc. 2017, 164, F591−
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Research and Development Program of the Korea Institute (17) Fan, J.; Chen, M.; Zhao, Z.; Zhang, Z.; Ye, S.; Xu, S.; Wang, H.;
of Energy Research (KIER) (C5-2409). Also, this work was Li, H. Bridging the gap between highly active oxygen reduction
supported by the National Research Foundation of Korea reaction catalysts and effective catalyst layers for proton exchange
(NRF) grant funded by the Korea government (MSIT) (No. membrane fuel cells. Nat. Energy 2021, 6, 475−486.
RS-2025-02309747). (18) Forner-Cuenca, A.; Biesdorf, J.; Gubler, L.; Kristiansen, P. M.;

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