Cost-effective and high-performance H2S sensors are required for human health and environmental monitoring. 2D transition-metal carbides and nitrides (MXenes) are appealing candidates for gas sensing due to good conductivity and abundant surface functional groups but have been studied primarily for detecting NH3 and VOCs, with generally positive responses that are not highly selective to the target gases. Here, we report on a negative response of pristine Ti3C2Tx thin films for H2S gas sensing (in contrast to the other tested gases) and further optimization of the sensor performance using a composite of Ti3C2Tx flakes and conjugated polymers (poly[3,6-diamino-10-methylacridinium chloride-co-3,6-diaminoacridine-squaraine], PDS-Cl) with polar charged nitrogen. The composite, preserving the high selectivity of pristine Ti3C2Tx, exhibits an H2S sensing response of 2% at 5 ppm (a thirtyfold sensing enhancement) and a low limit of detection of 500 ppb. In addition, our density functional theory calculations indicate that the mixture of MXene surface functional groups needs to be taken into account to describe the sensing mechanism and the selectivity of the sensor in agreement with the experimental results. Thus, this report extends the application range of MXene-based composites to H2S sensors and deepens the understanding of their gas sensing mechanisms.
Keywords: H2S sensing; MXene; Ti3C2Tx; density functional theory; surface functional groups.