Highly Sensitive Ammonia Gas Sensors at Room Temperature Based on the Catalytic Mechanism of N, C Coordinated Ni Single-Atom Active Center

IF 26.6 1区材料科学 Q1 Engineering Nano-Micro Letters Pub Date : 2024-08-27 DOI:10.1007/s40820-024-01484-4

Wenjing Quan, Jia Shi, Min Zeng, Wen Lv, Xiyu Chen, Chao Fan, Yongwei Zhang, Zhou Liu, Xiaolu Huang, Jianhua Yang, Nantao Hu, Tao Wang, Zhi Yang

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Abstract

Highlights

Exploiting single-atom catalytic activation and targeted adsorption properties, Ni single-atom active sites based on N, C coordination are constructed on the surface of two-dimensional MXene nanosheets (Ni–N–C/Ti₃C₂T_x), enabling highly sensitive and selective NH₃ gas detection.
The catalytic activation effect of Ni–N–C/Ti₃C₂T_x 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.
An end-sealing passivation strategy utilizing a conjugated hydrogen bond network of the conductive polymer was employed on MXene-based flexible electrodes, effectively mitigating the oxidative degradation of MXene-based gas sensors.

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基于 N、C 配位镍单原子活性中心催化机理的室温高灵敏度氨气传感器。

由于气体传感机制的局限性，氨（NH3）的痕量检测面临巨大挑战。在本研究中，我们提出利用单原子催化活化和定向吸附特性来实现高灵敏度和高选择性的 NH3 气体检测。具体来说，我们在二维（2D）MXene 纳米片（Ni-N-C/Ti3C2Tx）表面界面限制了基于 N、C 配位（Ni-N-C）的镍单原子活性位点，并集成了一种全柔性气体传感器（MNPE-Ni-N-C/Ti3C2Tx）。该传感器对 5 ppm 的 NH3 具有显著的响应值（27.3%），对 NH3 具有出色的选择性，理论检测限低至 12.1 ppb。密度泛函计算的模拟分析表明，具有 N、C 配位的镍单原子中心对 NH3 具有特定的定向吸附特性。此外，其催化活化效应有效降低了传感元素反应的吉布斯自由能，而其电子结构则促进了气固界面上活性氧物种的溢出效应。该传感器具有化学敏化和电子敏化的双通道传感机制，有利于电子高效地转移到二维 MXene 导电网络，从而形成 NH3 气体分子传感信号。此外，共轭氢键网络对 MXene 边缘缺陷的钝化增强了基于 MXene 的电极在高湿度条件下的长期稳定性。该研究基于 N、C 配位的 Ni 单原子活性中心的催化机理，实现了高灵敏度的室温 NH3 气体检测，为室温痕量气体检测研究提供了一种新的气体传感机制。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano-Micro Letters NANOSCIENCE & NANOTECHNOLOGY-MATERIALS SCIENCE, MULTIDISCIPLINARY

CiteScore

32.60

自引率

4.90%

发文量

981

审稿时长

1.1 months

期刊介绍： Nano-Micro Letters is a peer-reviewed, international, interdisciplinary, and open-access journal published under the SpringerOpen brand. Nano-Micro Letters focuses on the science, experiments, engineering, technologies, and applications of nano- or microscale structures and systems in various fields such as physics, chemistry, biology, material science, and pharmacy.It also explores the expanding interfaces between these fields. Nano-Micro Letters particularly emphasizes the bottom-up approach in the length scale from nano to micro. This approach is crucial for achieving industrial applications in nanotechnology, as it involves the assembly, modification, and control of nanostructures on a microscale.