Tuning thermal and electrical properties of MXenes via dehydration

Recently, MXenes (a class of two-dimensional transition metal carbides) have attracted great attention in various applications such as humidity sensors, owing to their unique electrical and thermal properties. However, previous studies of MXenes mostly focus on their humidity-sensing characteristics such as the mechanical response, and only few reports on their electrical and thermal response are available. Herein, we present novel transient electrothermal experiments to demonstrate that a transition from a negative to a positive resistance-temperature relationship can take place when the MXene sample becomes fully dehydrated. This surprising and unusual phenomenon was elucidated through non-equilibrium molecular dynamics simulations and attributed to water absorption/desorption onto the chemically active MXene surface. A linear relationship was also found between electrical/thermal properties and environmental humidity, which could be related to water adsorption on the surface of the MXene sensor. We further decomposed the total measured thermal conductivity and found that phonons were the dominant thermal carriers in the MXene sample. The main breakthrough of this work is the discovery of the unusual resistance-temperature relationship, which should be applicable to the design of MXene-based sensors for various applications.