Robust Metal Oxide Adhesion Layers for Cellulose Nanofiber-Based QCM Sensors

Here, we demonstrate the significant role of robust metal oxide adhesion layers on the cellulose nanofiber (CNF)-based quartz crystal microbalance (QCM) humidity sensor characteristics including sensitivity and stability. In this study, we deposited various metal oxide films (NiO, TiO₂, ZnO, and WO₃) onto QCM Au electrodes as adhesion layers before drop-casting CNF dispersion water. These metal oxide adhesion layers significantly enhanced the stability of CNF films on QCM sensors even in a high-humidity environment where a conventional adhesion layer (polyethylenimine) for CNF could not maintain stable adhesion. There was a significant difference between different metal oxide layers in the QCM data for humidity sensing. We found a negative correlation between the QCM sensitivity and the water wettability of metal oxide surfaces. Morphology analysis of the deposited CNF films revealed that the center-concentrated CNF microstructures on the metal oxide adhesion layers rigorously explained the observed negative correlation between the sensitivity and the wettability of metal oxide surfaces. This trend was further confirmed by gradually changing the hydrophobicity of the NiO adhesion surfaces. Thus, the proposed strategy using robust metal oxide adhesion layers will be a foundation for further development of various CNF-based QCM gas sensors.