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Springer Science and Business Media LLC Nano-Micro Letters 16(1)
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    초록·키워드

    Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia (NH<sub>3</sub>). In this study, we propose to exploit single-atom catalytic activation and targeted adsorption properties to achieve highly sensitive and selective NH<sub>3</sub> gas detection. Specifically, Ni single-atom active sites based on N, C coordination (Ni-N-C) were interfacially confined on the surface of two-dimensional (2D) MXene nanosheets (Ni-N-C/Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>), and a fully flexible gas sensor (MNPE-Ni-N-C/Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>) was integrated. The sensor demonstrates a remarkable response value to 5 ppm NH<sub>3</sub> (27.3%), excellent selectivity for NH<sub>3</sub>, and a low theoretical detection limit of 12.1 ppb. Simulation analysis by density functional calculation reveals that the Ni single-atom center with N, C coordination exhibits specific targeted adsorption properties for NH<sub>3</sub>. Additionally, its catalytic activation effect effectively reduces the Gibbs free energy of the sensing elemental reaction, while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas-solid interface. The sensor has a dual-channel sensing mechanism of both chemical and electronic sensitization, which facilitates efficient electron transfer to the 2D MXene conductive network, resulting in the formation of the NH<sub>3</sub> gas molecule sensing signal. Furthermore, the passivation of MXene edge defects by a conjugated hydrogen bond network enhances the long-term stability of MXene-based electrodes under high humidity conditions. This work achieves highly sensitive room-temperature NH<sub>3</sub> gas detection based on the catalytic mechanism of Ni single-atom active center with N, C coordination, which provides a novel gas sensing mechanism for room-temperature trace gas detection research.

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