Dai Tiantian, Yan Zhi, Li Meng, Han Yulei, Deng Zanhong, Wang Shimao, Wang Ruyang, Xu Xiaohong, Shi Lei, Tong Wei, Bao Jun, Qiao Zhenhua, Li Liang, Meng Gang
Anhui Provincial Key Laboratory of Photonic Devices and Materials, Anhui Institute of Optics and Fine Mechanics, and Key Lab of Photovoltaic and Energy Conservation Materials, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, 230031, P. R. China.
ICQD, Hefei National Laboratory for Physical Sciences at Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, and Department of Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Small Methods. 2022 Oct;6(10):e2200728. doi: 10.1002/smtd.202200728. Epub 2022 Aug 26.
Insufficient limit of detection (LoD) toward volatile organic compounds (VOCs) hinders the promising applications of metal oxide chemiresistors in emerging air quality monitoring and/or breath analysis. There is an inherent limitation of widely adopted strategies of creating sensitive chemiresistors then operating at the optimized temperature via a continuous heating (CH) mode. Herein, a strategy combining Pt single atoms anchoring (chemical sensitization) with pulsed temperature modulation (PTM, physical sensitization) is proposed. Apart from generating abundant surface asymmetric oxygen vacancy (Pt-V -W) active sites at pulsed high temperature (HT) stage, inward diffusion of trace target VOCs across the sensing layer at pulsed low temperature stage (driven by PTM induced concentration gradient), can greatly enhance the charge interaction probability between the generated surface active species and the surrounding VOCs, and thus offers a novel avenue on addressing the bottleneck issue of low LoD by PTM. Triggered by HT of 300 °C, the responses of Pt anchored WO chemiresistor to 1 ppm trimethylamine (TMA) and xylene can be drastically boosted from 1.9 (CH) to 6541.5 (PTM) and 1.5 (CH) to 1001.1 (PTM), respectively. And ultra-low theoretic LoD of 0.78 ppt (TMA) and 0.18 ppt (xylene) are successfully achieved, respectively.
对挥发性有机化合物(VOCs)的检测限不足阻碍了金属氧化物化学电阻器在新兴空气质量监测和/或呼吸分析中的应用前景。通过连续加热(CH)模式制备敏感化学电阻器然后在优化温度下运行的广泛采用策略存在固有局限性。在此,提出了一种将铂单原子锚定(化学敏化)与脉冲温度调制(PTM,物理敏化)相结合的策略。除了在脉冲高温(HT)阶段产生大量表面不对称氧空位(Pt-V-W)活性位点外,在脉冲低温阶段痕量目标VOCs在传感层中的向内扩散(由PTM诱导的浓度梯度驱动),可以大大提高所产生的表面活性物种与周围VOCs之间的电荷相互作用概率,从而为解决PTM导致的低检测限瓶颈问题提供了一条新途径。在300℃的HT触发下,铂锚定的WO化学电阻器对1ppm三甲胺(TMA)和二甲苯的响应分别可以从1.9(CH)大幅提高到6541.5(PTM)和1.5(CH)提高到1001.1(PTM)。并且分别成功实现了0.78ppt(TMA)和0.18ppt(二甲苯)的超低理论检测限。