Microelectronics Research Unit, Faculty of Information Technology and Electrical Engineering, University of Oulu, P.O. Box 4500, FIN-90014 Oulu, Finland.
Department of Chemical and Metallurgical Engineering, Aalto University, FIN-00076 Aalto, Finland.
Nanoscale Horiz. 2023 May 30;8(6):794-802. doi: 10.1039/d2nh00591c.
MXenes are emerging sensing materials due to their metallic conductivity and rich surface chemistry for analytes; they, however, suffer from poor stability. Incorporation with functional polymers can largely prevent the performance decay and enhance the sensing performance. Herein, we demonstrate a core-shell composite, TiCT@croconaine (poly(1,5-diaminonaphthalene-croconaine), PDAC) prepared by a facile polymerization reaction, suitable for NH detection. Compared to pristine TiCT, the sensor made of a TiCT-polycroconaine composite exhibits a significantly enhanced sensitivity of 2.8% ppm and an estimated achievable limit of detection of 50 ppb. The improved sensing performance could be attributed to the presence of PDAC facilitating the adsorption of NH and changing the tunneling conductivity between TiCT domains. Density functional theory (DFT) calculations reveal that the adsorption energy of NH on PDAC is the highest among the tested gases, which supports the selectivity of the sensor to this analyte. Benefiting from the protection conferred by the PDAC shell, the composite has a reliable operation period of at least 40 days. In addition, we demonstrated a flexible paper-based sensor of the TiCT@PDAC composite, without attenuated performance upon mechanical deformation. This work proposed a novel mechanism and a feasible methodology to synthesize MXene-polymer composites with improved sensitivity and stability for chemical sensing.
MXenes 作为新兴的传感材料,由于其具有金属导电性和丰富的表面化学性质,可用于分析物;然而,它们的稳定性较差。与功能聚合物结合可以在很大程度上防止性能下降并提高传感性能。本文通过简便的聚合反应制备了核壳复合材料 TiCT@croconaine(聚(1,5-二氨基萘-克罗腙),PDAC),适用于 NH 检测。与原始 TiCT 相比,由 TiCT-聚克罗腙复合材料制成的传感器表现出显著增强的灵敏度 2.8%ppm 和估计可达到的检测限 50ppb。传感性能的提高可归因于 PDAC 的存在促进了 NH 的吸附并改变了 TiCT 畴之间的隧道导电性。密度泛函理论 (DFT) 计算表明,NH 在 PDAC 上的吸附能在测试的气体中最高,这支持了传感器对该分析物的选择性。得益于 PDAC 壳的保护,该复合材料具有至少 40 天的可靠工作周期。此外,我们展示了一种基于纸张的 TiCT@PDAC 复合柔性传感器,其机械变形后性能没有衰减。这项工作提出了一种新的机制和可行的方法来合成具有提高的灵敏度和稳定性的 MXene-聚合物复合材料,用于化学传感。