Human-centered Sensing Laboratory, Department of Mechanical and Process Engineering, ETH Zurich, CH-8092 Zurich, Switzerland.
Department of Endocrinology, Diabetology, and Clinical Nutrition, University Hospital Zurich (USZ) and University of Zurich (UZH), CH-8091 Zürich, Switzerland.
Nanoscale. 2023 Feb 23;15(8):3967-3977. doi: 10.1039/d2nr06599a.
Formaldehyde is a toxic and carcinogenic indoor air pollutant. Promising for its routine detection are gas sensors based on localized surface plasmon resonance (LSPR). Such sensors trace analytes by converting tiny changes in the local dielectric environment into easily readable, optical signals. Yet, this mechanism is inherently non-selective to volatile organic compounds (like formaldehyde) and yields rarely detection limits below parts-per-million concentrations. Here, we reveal that chemical reaction-mediated LSPR with nanohybrids of Ag/AgO core-shell clusters on TiO enables highly selective formaldehyde sensing down to 5 parts-per-billion (ppb). Therein, AgO is reduced by the formaldehyde to metallic Ag resulting in strong plasmonic signal changes, as measured by UV/Vis spectroscopy and confirmed by X-ray diffraction. This interaction is highly selective to formaldehyde over other aldehydes, alcohols, ketones, aromatic compounds (as confirmed by high-resolution mass spectrometry), inorganics, and quite robust to relative humidity changes. Since this sensor works at room temperature, such LSPR nanohybrids are directly deposited onto flexible wristbands to quantify formaldehyde between 40-500 ppb at 50% RH, even with a widely available smartphone camera (Pearson correlation coefficient = 0.998). Such chemoresponsive coatings open new avenues for wearable devices in environmental, food, health and occupational safety applications, as demonstrated by an early field test in the pathology of a local hospital.
甲醛是一种有毒且致癌的室内空气污染物。基于局域表面等离激元共振(LSPR)的气体传感器有望实现其常规检测。这些传感器通过将局部介电环境的微小变化转化为易于读取的光学信号来追踪分析物。然而,这种机制对挥发性有机化合物(如甲醛)本质上是非选择性的,很少能达到百万分之几浓度以下的检测限。在这里,我们揭示了 Ag/AgO 核壳纳米簇在 TiO 上的化学反中介导的 LSPR 能够实现低至 5 十亿分比浓度(ppb)的高选择性甲醛传感。其中,AgO 被甲醛还原为金属 Ag,导致强等离子体信号变化,这可以通过紫外/可见光谱测量并通过 X 射线衍射确认。这种相互作用对甲醛具有高度选择性,而对其他醛、醇、酮、芳香族化合物(如高分辨率质谱所证实)、无机物的选择性较低,对相对湿度变化也相当稳健。由于这种传感器在室温下工作,因此这种 LSPR 纳米杂化材料可直接沉积在柔性腕带上,在 50%相对湿度下定量检测 40-500 ppb 之间的甲醛,甚至可以使用广泛可用的智能手机摄像头(皮尔逊相关系数 = 0.998)。这种化学响应性涂层为环境、食品、健康和职业安全应用中的可穿戴设备开辟了新途径,这在当地医院病理学的早期现场测试中得到了证明。