Electrostatic self-assembly enabled flexible paper-based humidity sensor with high sensitivity and superior durability

Humidity sensors have been widely used for humidity monitoring in industrial fields. However, the application of conventional sensors is limited due to the structural rigidity, high cost, and time-consuming integration process. Owing to the good hydrophilicity, biodegradability, and low cost of cellulose, the sensors built on cellulose bulk materials are considered a feasible method to overcome these drawbacks while providing reasonable performance. Herein, we design a flexible paper-based humidity sensor based on conductive 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose fibers/carbon nanotubes (TOCFs/CNTs) conformal fibers network. The CNTs are dispersed by cationic cetyl trimethyl ammonium bromide (CTAB), which introduces positive charges on the CNTs surface. The conductive fibers are achieved by an electrostatic self-assembly process that positively charged CNTs are adsorbed to the surface of negatively charged TOCFs. The vast number of hydrophilic hydroxyl groups on the surface of TOCFs provide more water molecules adsorption sites and facilitate the electron transfer from water molecules to CNTs, endowing the sensor with an excellent humidity responsive property. Besides, the swelling of the TOCFs greatly damages the conductive CNTs network and further promotes the humidity sensitive performance of the sensor. Benefiting from the unique structure, the obtained sensor exhibits a maximum response value of 87.0% (ΔI/I0 , and the response limit is 100%), outstanding linearity (R2 = 0.995) between 11 and 95% relative humidity (RH), superior bending (with a curvature of 2.1 cm-1) and folding (up to 50 times) durability, and good long-time stability (more than 3 months). Finally, as a proof of concept, the sensor demonstrates an excellent responsive property to human breath, fingertip humidity, and the change of air humidity, indicating a great potential towards practical applications.