One-Way Continuous Deposition of Monolayer MXene Nanosheets for the Formation of Two Confronting Transparent Electrodes in Flexible Capacitive Photodetector

MXenes based on titanium carbide are promising next-generation transparent electrode materials due to their high metallic conductivity, optical transparency, mechanical flexibility, and abundant hydrophilic surface functionality. MXene electrodes offer a much wider conductive surface coverage than metal nanowires, thereby gaining popularity as flexible electrode materials in supercapacitors and energy devices. However, given that monolayer MXene nanosheets are only a few nanometers thick, meticulous surface treatments and deposition technologies are required for a practical implementation of these transparent electrodes. Unfortunately, a capacitor produced by forming high-quality transparent MXene electrodes on both sides of a film has not yet been reported. We report the successful development of a one-way continuous deposition technology to form high-quality MXene nanosheet-based transparent electrodes on both surfaces of a polymer film without large physical stresses on the MXene nanosheets. One transparent electrode was formed by transferring MXene nanosheets predeposited on a temporary glass substrate to the film surface, while the other was directly deposited on the exposed film surface. The Ti3AlC2 precursor (MAX) was synthesized via a spark plasma sintering crystallization, and the MXene nanosheets were prepared via a subsequent Al-selective etching and delamination. We used this material to implement a capacitive photodetector consisting of two layers of opposing transparent electrodes. The flexible photodetector was based on poly(vinyl butyral) (PVB), which was solidly bonded with MXene nanosheets to serve as a free-standing binder for the Cu-doped ZnS semiconductor particles. The fabricated device exhibited excellent mechanical stability due to the high affinity between the MXene nanosheets and PVB. Furthermore, the device exhibited an initial capacitance of 2 nF, photosensitivity of 12.5 μF/W, and rise and decay times of 0.031 and 0.751 s, respectively. All these parameters were 1 to 2 orders of magnitude higher or faster than reported capacitive photodetectors. Overall, the proposed approach resolves the core issues associated with existing metal nanowire-based electrodes, and it is a breakthrough in the development of next-generation flexible devices comprising two layers of confronting transparent electrodes.