CO-tolerant hydrogen oxidation on Pt enabled by ultrathin silica overlayers
- 1aMESA+ Institute of Nanotechnology, Department of Chemical Engineering, Faculty of Science and Technology, University of Twente, Drienerlolaan 5, 7522 NB Enschede, The Netherlands.
- 2aMESA+ Institute of Nanotechnology, Department of Chemical Engineering, Faculty of Science and Technology, University of Twente, Drienerlolaan 5, 7522 NB Enschede, The Netherlands.bFakultät für Chemie & Biochemie, Technische Chemie - Energie und Umweltrelevante Katalyse, Ruhr-Universität Bochum, Germany.
Abstract
Low-temperature electrochemical hydrogen compression can combine H2 compression and purification, but CO impurities in practical H2 feeds rapidly poison Pt anodes. Here, we use sputter- and electrodeposited Pt on Ti disk model electrodes to assess whether ultrathin polydimethylsiloxane (PDMS)-derived amorphous silica overlayers can improve CO tolerance during the hydrogen oxidation reaction (HOR). Fourier-transform infrared reflection–absorption and low-energy ion-scattering spectroscopy confirmed conformal and amorphous silica overlayer formation on Pt. Nominal thickness-dependent measurements revealed a narrow activity-protection window within the sub-10 nm regime. 2–3 nm silica overlayers provided limited CO tolerance, whereas increasing the nominal thickness from 7 to 8 nm strongly suppressed HOR activity. Benchmarking against active electrochemical regeneration showed that bare Pt operated at 0.15 V vs. RHE with 15 s CO-stripping pulses at 0.85 V vs. RHE delivered a 1.8 times higher time-averaged HOR power density than silica-coated Pt. However, the pulses introduced an 8% energy-efficiency loss and rely on repeated high-potential cycling that accelerates electrode degradation. Importantly, under fixed-current operation, silica-coated Pt reduced the cumulative HOR energy demand under CO contamination by a factor of up to 3.6. These results establish ultrathin silica overlayers as a promising interfacial design strategy for CO-tolerant hydrogen oxidation and motivate translation to gas-diffusion electrodes (GDEs), where homogeneous and selective coating of porous electrodes remains the key challenge.
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BibTeX
@article{englezos2026cotolerant,
title = {{CO-tolerant hydrogen oxidation on Pt enabled by ultrathin silica overlayers}},
author = {Christos Englezos and Marco Altomare and Guido Mul and Bastian Mei and Georgios Katsoukis},
journal = {EES Catalysis},
year = {2026},
month = aug,
doi = {10.1039/d6ey00101g},
url = {https://doi.org/10.1039/d6ey00101g},
note = {CC BY},
}
RIS
TY - JOUR
TI - CO-tolerant hydrogen oxidation on Pt enabled by ultrathin silica overlayers
AU - Christos Englezos
AU - Marco Altomare
AU - Guido Mul
AU - Bastian Mei
AU - Georgios Katsoukis
PY - 2026
DA - 2026/08/01
JO - EES Catalysis
DO - 10.1039/d6ey00101g
UR - https://doi.org/10.1039/d6ey00101g
AB - Low-temperature electrochemical hydrogen compression can combine H2 compression and purification, but CO impurities in practical H2 feeds rapidly poison Pt anodes. Here, we use sputter- and electrodeposited Pt on Ti disk model electrodes to assess whether ultrathin polydimethylsiloxane (PDMS)-derived amorphous silica overlayers can improve CO tolerance during the hydrogen oxidation reaction (HOR). Fourier-transform infrared reflection–absorption and low-energy ion-scattering spectroscopy confirmed conformal and amorphous silica overlayer formation on Pt. Nominal thickness-dependent measurements revealed a narrow activity-protection window within the sub-10 nm regime. 2–3 nm silica overlayers provided limited CO tolerance, whereas increasing the nominal thickness from 7 to 8 nm strongly suppressed HOR activity. Benchmarking against active electrochemical regeneration showed that bare Pt operated at 0.15 V vs. RHE with 15 s CO-stripping pulses at 0.85 V vs. RHE delivered a 1.8 times higher time-averaged HOR power density than silica-coated Pt. However, the pulses introduced an 8% energy-efficiency loss and rely on repeated high-potential cycling that accelerates electrode degradation. Importantly, under fixed-current operation, silica-coated Pt reduced the cumulative HOR energy demand under CO contamination by a factor of up to 3.6. These results establish ultrathin silica overlayers as a promising interfacial design strategy for CO-tolerant hydrogen oxidation and motivate translation to gas-diffusion electrodes (GDEs), where homogeneous and selective coating of porous electrodes remains the key challenge.
SN - 2753-801X
ER -