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Here, we present a novel approach to address this issue by combining MXene (Ti3C2Tx) nanosheets with branched ionic nanoparticles from polyhedral oligomeric silsesquioxanes (POSS) using an amphiphilicity driven assembly for the formation of composite monolayers of nanoparticle-decorated MXene nanosheets at the air-water interface. The amphiphilic hybrid MXene/POSS monolayers allow for the fabrication of organized multilayered films with ionic nanoparticles supporting nanoscale gap between MXene nanosheets. For these composite multilayers we observed a 400% enhancement in specific capacitance compared to pure drop-cast MXene films. Furthermore, dramatically enhanced electrochemical cycling stability for ultrathin film electrodes (< 400 nm in thickness) with a 91% capacitance retention over 10,000 cycles has been achieved. Our results suggest that this insertion of 0D ionic nanoparticles with complementary interactions in-between 2D MXene nanosheets could be extended to other hybrid 0D-2D nanomaterials, providing a promising pathway for the development of hybrid electrode architectures with enhanced ionic transport for long term energy cycling and storage, capacitive deionization, and ionic filtration. 

Stacking atomically thin two-dimensional (2D) nanosheet materials leads to unique synergy in their inherent properties due to an intimate combination and matching that is not possible via separate individual components and phases. However, traditional synthesis and assembly methods result in poor architectural control and restricted surface chemistry, thereby limiting their prospective potentials. This brief overview provides consideration of different synthesis and assembly methods for fabrication of diverse novel heterostructures. The advantages and challenges of existing methods are discussed. Finally, future perspectives regarding crafting of heterostructures with highly controllable architectures and interfacial/surface chemistry, and advanced characterization methods are highlighted. 

We discuss current trends in developing novel synthetic polymers, biopolymers, and corresponding soft and functional hybrid nanocomposites for advanced current and future applications with an emphasis on active functional devices and functions. Among a wide variety of polymeric materials and relevant applications, we select the fields, which are close to the authors’ research interests. This selection includes strong but lightweight biopolymer composites, gel-like and porous materials for chemical and energy transport control, fast-actuating responsive materials and structures, and thin film electronic materials for chemical, physical, and biological sensing applications compatible with human and robotic interfaces.