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Van der Waals interactions between nonpolar alkyl chains and polar oxide surfaces prevent catalyst deactivation in aldehyde gas sensing

Author

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  • Kentaro Nakamura

    (The University of Tokyo
    Kyushu University)

  • Tsunaki Takahashi

    (The University of Tokyo)

  • Takuro Hosomi

    (The University of Tokyo)

  • Wataru Tanaka

    (The University of Tokyo)

  • Yu Yamaguchi

    (The University of Tokyo)

  • Jiangyang Liu

    (The University of Tokyo)

  • Masaki Kanai

    (Kyushu University)

  • Yuta Tsuji

    (Kyushu University)

  • Takeshi Yanagida

    (The University of Tokyo
    Kyushu University)

Abstract

Catalysis-based electrical sensing of volatile organic compounds on metal oxide surfaces is a powerful method for molecular discrimination. However, catalyst deactivation caused by the poisoning of catalytic sites by analytes and/or catalyzed products remains a challenge. This study highlights the underestimated role of van der Waals interactions between hydrophobic aliphatic alkyl chains and hydrophilic ZnO surfaces in mitigating catalyst deactivation during aliphatic aldehyde sensing. By immobilizing octadecylphosphonic acid (ODPA) on ZnO nanowire sensors, recovery times for nonanal detection are significantly reduced without compromising sensitivity. Temperature-programmed measurements demonstrate a reduction in desorption temperature of carboxylates on ODPA-modified ZnO to below 150 °C, whereas carboxylates on bare ZnO remain above 300 °C, indicating a significant decrease in catalyst deactivation. Density functional theory calculations reveal that accumulated van der Waals interactions between alkyl chains and ZnO surfaces significantly contributed to adsorption molecular kinetics. IR spectroscopy using deuterated self-assembled monolayers (SAMs) reveals conformational changes of alkyl chains within the SAMs caused by aldehyde adsorption, supporting the suggested adsorption kinetics. A model is proposed based on the dynamic surface-covering by alkyl chains destabilizes catalytically oxidized carboxylic acids.

Suggested Citation

  • Kentaro Nakamura & Tsunaki Takahashi & Takuro Hosomi & Wataru Tanaka & Yu Yamaguchi & Jiangyang Liu & Masaki Kanai & Yuta Tsuji & Takeshi Yanagida, 2024. "Van der Waals interactions between nonpolar alkyl chains and polar oxide surfaces prevent catalyst deactivation in aldehyde gas sensing," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53577-8
    DOI: 10.1038/s41467-024-53577-8
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    References listed on IDEAS

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    1. Simon H. Pang & Carolyn A. Schoenbaum & Daniel K. Schwartz & J. Will Medlin, 2013. "Directing reaction pathways by catalyst active-site selection using self-assembled monolayers," Nature Communications, Nature, vol. 4(1), pages 1-6, December.
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