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

Kentaro Nakamura, Tsunaki Takahashi (), Takuro Hosomi, Wataru Tanaka, Yu Yamaguchi, Jiangyang Liu, Masaki Kanai, Yuta Tsuji and Takeshi Yanagida ()
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Kentaro Nakamura: The University of Tokyo
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

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-53577-8

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