Two-Dimensional MoO₂ Nanosheet Composite Hydrogels with High Transmittance and Excellent Photothermal Property for Near-Infrared Responsive Actuators and Microvalves

Stimulus-responsive intelligent hydrogel actuators have highly promising applications in the fields of soft robotics, smart manipulators, and flexible devices. Near-infrared (NIR) light is considered an ideal method to trigger the response behavior remotely and precisely. In order to realize the excellent optical transmittance and photothermal property of NIR-responsive hydrogels at the same time, two-dimensional nonlayered MoO2 nanosheets (2D-MoO2) with excellent photothermal efficiency (62% under an NIR light irradiation of 808 nm), splendid chemistry stability, and low preparation cost are used as photothermal agents and incorporated into the poly(N-isopropylacrylamide) (PNIPAM) hydrogel network, forming the 2D-MoO2/Laponite/PNIPAM ternary nanocomposite hydrogel (TN hydrogel). It is remarkable that compared with the GO and MXene hydrogels with the same agent content (1.0 mg mL–1) and thickness (1 mm) whose transmittance values are only ∼5% at 600 nm, the TN hydrogel shows a similar NIR-responsive temperature, but much higher optical transmittance (∼53%). Besides, of the three hydrogels with similar transmittance, the TN hydrogel shows a much higher NIR-responsive temperature. The TN hydrogel with a low loading of 2D-MoO2 (1.5 mg mL–1) can produce a significant temperature increase of ∼30 °C after the application of 0.8 W cm–2 NIR light irradiation for 15 s. Impressively, the TN hydrogel exhibits excellent anti-fatigue property, keeping a fast response and temperature rise behavior even after 50 times of heating–cooling cycles. The flexibly controllable and reversible deformation is realized by a well-designed bilayer structure even in harsh environments. The transparent and asymmetric bilayer hydrogel is further used as a soft manipulator to capture objects visually and accurately. The NIR light-controlled microvalve based on this composite hydrogel is also demonstrated. This work provides a novel kind of transparent hybrid NIR response hydrogel for the further development of smart, programmable, reversible hydrogel-based actuators and soft robotics.