The creation of three-dimensional (3D) structures from two-dimensional (2D) nanomaterial building blocks enables novel chemical, mechanical or physical functionalities that cannot be realized with planar thin films or in bulk materials. In this Progress Report, we review the use of emerging 2D materials to create complex out-of-plane surface topographies and 3D material architectures. We focus on recent approaches that yield periodic textures or patterns, and present four techniques as case studies: (i) wrinkling and crumpling of planar sheets, (ii) encapsulation by crumpled nanosheet shells, (iii) origami folding and kirigami cutting to create programmed curvature, and (iv) 3D printing of 2D material suspensions. Work to date in this field has primarily used graphene and graphene oxide as the 2D building blocks, and we consider how these unconventional approaches may be extended to alternative 2D materials and their heterostructures. Taken together, these emerging patterning and texturing techniques represent an intriguing alternative to conventional materials synthesis and processing methods, and are expected to contribute to the development of new composites, stretchable electronics, energy storage devices, chemical barriers, and biomaterials.

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Confined assembly in the intersheet gallery spaces of two-dimensional (2D) materials is an emerging templating route for creation of ultrathin material architectures. Here, we demonstrate a general synthetic route for transcribing complex wrinkled and crumpled topographies in graphene oxide (GO) films into textured metal oxides. Intercalation of hydrated metal ions into textured GO multilayer films followed by dehydration, thermal decomposition, and air oxidation produces Zn, Al, Mn, and Cu oxide films with high-fidelity replication of the original GO textures, including "multi-generational", multiscale textures that have been recently achieved through extreme graphene compression. The textured metal oxides are shown to consist of nanosheet-like aggregates of interconnected particles, whose mobility, attachment, and sintering are guided by the 2D template. This intercalation templating approach has broad applicability for the creation of complex, textured films and provides a bridging technology that can transcribe the wide variety of textures already realized in graphene into insulating and semiconducting materials. These textured metal oxide films exhibit enhanced electrochemical and photocatalytic performance over planar films and show potential as high-activity electrodes for energy storage, catalysis, and biosensing.

This letter demonstrates a simple method to achieve high-yields of 1H semiconducting MoS2 monolayers in concentrated, colloidally-stable aqueous suspension. The method is based on oxidation suppression during the hydrothermal processing step used for metal-to-semiconductor phase reversion. Accompanying DFT calculations on elementary steps in the MoS2 wet oxidation reaction suggest that a two-site corrosion mechanism is responsible for the observed high reactivity and low stability of 1T metallic MoS2.

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There is great interest in exploiting van der Waals gaps in layered materials as nanofluidic channels. Graphene oxide (GO) nanosheets are known to spontaneously assemble into stacked planar membranes with transport properties that are highly selective to molecular structure. Use of conventional GO membranes in liquid-phase applications is often limited by low flux values, due to intersheet nanochannel alignment perpendicular to the desired Z-directional transport, which leads to circuitous fluid pathways that are orders of magnitude longer than the membrane thickness. Here we demonstrate an approach that uses compressive instability in Zr-doped GO thin films to create wrinkle patterns that rotate nanosheets to high angles. Capturing this structure in polymer matrices and thin sectioning produce fully dense membranes with arrays of near-vertically aligned nanochannels. These robust nanofluidic devices offer pronounced reduction in fluid path-length, while retaining the high selectivity for water over non-polar molecules characteristic of GO interlayer nanochannels.

A wide range of technologies requires barrier films to impede molecular transport between the external environment and a desired internal microclimate. Adding stretchability to barrier films would enable the applications in packaging, textiles, and flexible devices, but classical barrier materials utilize dense, ordered molecular architectures that easily fracture under small tensile strain. Here, we show that textured graphene-based coatings can serve as ultrastretchable molecular barriers expandable to 1500% areal strain through programmed unfolding that mimics the elasticity of polymers. These coatings retain barrier function under large deformation and can be conformally applied to planar or curved surfaces, where they are washfast and mechanically robust to cycling. These graphene-polymer bilayer structures also function as sensors or actuators by transducing chemical stimuli into mechanical deformation and electrical resistance change through asymmetric polymer swelling. These results may enable multifunctional fabrics that integrate chemical protection, sensing, and actuation, with further applications as selective barriers, membranes, stretchable electronics, or soft robotics.