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Abstract Structural color arises from light scattering rather than organic pigments and can be found in Nature, such as in bird feathers and butterfly wings. Synthetic materials can mimic Nature by leveraging materials with contrasting optical characteristics by controlling each materials’ spatial arrangement in a heterostructure. Two-dimensional MXene nanosheets are particularly interesting due to their unique optical properties, but MXenes have not been used directly as a structural colorant because it is challenging to control the spatial placement of MXenes at the nanometer level. Here, we report the emergence of structural color in layer-by-layer (LbL) assemblies of Ti₃C₂T_zMXene nanosheets and polyelectrolyte heterostructures with controlled block thicknesses. The block thickness and spatial placement of MXene are controlled by the assembly’s salt concentration and number of layer pairs. This work demonstrates that optical characteristics of MXene/polyelectrolyte heterostructures depend on MXene content and placement, while deepening the understanding of MXenes within structural color films. 

The major challenge to fabricate MXene/polymer composites are the processing conditions and poor control over the distribution of the MXene nanosheets within the polymer matrix. Traditional ways involve the direct mix of fillers and polymers to form a random homogeneous composite, which leads to inefficient use of fillers. To address these challenges, researchers have focused on the development of ordered MXene/polymer composite structures using various fabrication strategies. In this review, we summarize recent advances of structured MXene/polymer composites and their processing-structure-property relationships. Two main forms of MXene/polymer composites (films and foams) are separately discussed with a focus on the detailed fabrication means and corresponding structures. These architected composites complement those in which MXenes nanosheets are isotropically dispersed throughout, such as those formed by aqueous solution mixing approaches. This review culminates in a perspective on the future opportunities for architected MXene/polymer composites. 

Although surface terminations (such as ═O, –Cl, –F, and –OH) on MXene nanosheets strongly influence their functional properties, synthesis of MXenes with desired types and distribution of those terminations is still challenging. Here, it is demonstrated that thermal annealing helps in removing much of the terminal groups of molten salt-etched multilayered (ML) Ti3C2Tz. In this study, the chloride terminations of molten salt-etched ML-Ti3C2Tz were removed via thermal annealing at increased temperatures under an inert (argon) atmosphere. This thermal annealing created some bare sites available for further functionalization of Ti3C2Tz. XRD, EDS, and XPS measurements confirm the removal of much of the terminal groups of ML-Ti3C2Tz. Here, the annealed ML-Ti3C2Tz was refunctionalized by −OH groups and 3-aminopropyl triethoxysilane (APTES), which was confirmed by FTIR. The −OH and APTES surface-modified ML-Ti3C2Tz are evaluated as a solid lubricant, exhibiting ∼70.1 and 66.7% reduction in friction compared to a steel substrate, respectively. This enhanced performance is attributed to the improved interaction or adhesion of functionalized ML-Ti3C2Tz with the substrate material. This approach allows for the effective surface modification of MXenes and control of their functional properties.