Heterogeneous Engineering-Induced Electron Enrichment in Carbon Support for High-Stability Proton Exchange Membrane Fuel Cells

TY - JOUR

T1 - Heterogeneous Engineering-Induced Electron Enrichment in Carbon Support for High-Stability Proton Exchange Membrane Fuel Cells

AU - Liu, Rui

AU - Dong, Feilong

AU - Lv, Zunhang

AU - Fan, Haiyang

AU - Tian, Chongao

AU - Li, Jiaxin

AU - Feng, Xiao

AU - Wang, Bo

AU - Yang, Wenxiu

N1 - Publisher Copyright: © 2025 Wiley-VCH GmbH.

PY - 2026/1/28

Y1 - 2026/1/28

N2 - The widespread adoption of proton exchange membrane fuel cells (PEMFCs) is significantly hindered by the rapid degradation of oxygen reduction reaction (ORR) catalysts under harsh operational conditions. Here, a CeOx-integrated heterogeneous carbon support engineering strategy is proposed to stabilize the Co-N4-C catalyst (Co SAs/CeOx-NC), achieving simultaneous activity-stability enhancement in PEMFCs. Density functional theory (DFT) calculations reveal that the enhanced binding energy between Co and the carbon support, combined with the reducibility provided by the electron-rich nature of the carbon support, synergistically suppresses Co dissolution and carbon oxidation corrosion. Concurrently, the CeOx-induce interfacial charge redistribution downshifts the Co d-band center by 0.12 eV, weakening the over-adsorption of oxygenated intermediates and enhancing ORR kinetics. The optimized Co SAs/CeOx-NC catalyst demonstrates exceptional durability in acidic media (ΔE1/2 = 8 mV after 5k cycles at high potential of 1.0–1.6 V), outperforming the control Co SAs/NC catalyst (ΔE1/2 = 30 mV). The Co SAs/CeOx-NC-based PEMFC achieves outstanding peak power density of 1.04 W cm−2 and durability (95% voltage retention after 150 h open-circuit conditions test).

AB - The widespread adoption of proton exchange membrane fuel cells (PEMFCs) is significantly hindered by the rapid degradation of oxygen reduction reaction (ORR) catalysts under harsh operational conditions. Here, a CeOx-integrated heterogeneous carbon support engineering strategy is proposed to stabilize the Co-N4-C catalyst (Co SAs/CeOx-NC), achieving simultaneous activity-stability enhancement in PEMFCs. Density functional theory (DFT) calculations reveal that the enhanced binding energy between Co and the carbon support, combined with the reducibility provided by the electron-rich nature of the carbon support, synergistically suppresses Co dissolution and carbon oxidation corrosion. Concurrently, the CeOx-induce interfacial charge redistribution downshifts the Co d-band center by 0.12 eV, weakening the over-adsorption of oxygenated intermediates and enhancing ORR kinetics. The optimized Co SAs/CeOx-NC catalyst demonstrates exceptional durability in acidic media (ΔE1/2 = 8 mV after 5k cycles at high potential of 1.0–1.6 V), outperforming the control Co SAs/NC catalyst (ΔE1/2 = 30 mV). The Co SAs/CeOx-NC-based PEMFC achieves outstanding peak power density of 1.04 W cm−2 and durability (95% voltage retention after 150 h open-circuit conditions test).

KW - carbon corrosion resistance

KW - catalyst durability

KW - metal-support interaction

KW - oxygen reduction reaction

KW - proton exchange membrane fuel cells

UR - https://www.scopus.com/pages/publications/105022607365

U2 - 10.1002/aenm.202504582

DO - 10.1002/aenm.202504582

M3 - Article

AN - SCOPUS:105022607365

SN - 1614-6832

VL - 16

JO - Advanced Energy Materials

JF - Advanced Energy Materials

IS - 4

M1 - e04582

ER -