Two-dimensional (2D) materials often show a range of intriguing electronic, catalytic, and optical properties that differ greatly from conventional nanoparticles. While planar configuration is often desirable, a range of applications such as catalysis and sensing benefit greatly from the accessibility to large surface areas. The 2D materials generally tend to form stacks in order to reduce the overall surface energy. Such densely packed structures however are detrimental when access to high surface area is required. Herewith we demonstrate a chemical strategy to generate Pd three-dimensional (3D) structures from its flexible 2D nanosheets. Solvent polarity is shown to play an important role to control the final morphology of these nanosheets. Our data indicate when these Pd 3D materials were integrated into hydrogen sensing devices, response time was found to be an order of magnitude faster than their 2D-constrained counterparts. The easy accessibility to the surfaces by hydrogen gas is considered to be an important factor for the observed fast response time based on the sensing model.

Widespread testing and isolation of infected patients is a cornerstone of viral outbreak management, as underscored during the ongoing COVID-19 pandemic. Here, we report a large-area and label-free testing platform that combines surface-enhanced Raman spectroscopy and machine learning for the rapid and accurate detection of SARS-CoV-2. Spectroscopic signatures acquired from virus samples on metal–insulator–metal nanostructures, fabricated using nanoimprint lithography and transfer printing, can provide test results within 25 min. Not only can our technique accurately distinguish between different respiratory and nonrespiratory viruses, but it can also detect virus signatures in physiologically relevant matrices such as human saliva without any additional sample preparation. Furthermore, our large area nanopatterning approach allows sensors to be fabricated on flexible surfaces allowing them to be mounted on any surface or used as wearables. We envision that our versatile and portable label-free spectroscopic platform will offer an important tool for virus detection and future outbreak preparedness.

Self‐folding broadly refers to the assembly of 3D structures by bending, curving, and folding without the need for manual or mechanized intervention. Self‐folding is scientifically interesting because self‐folded structures, from plant leaves to gut villi to cerebral gyri, abound in nature. From an engineering perspective, self‐folding of sub‐millimeter‐sized structures addresses major hurdles in nano‐ and micro‐manufacturing. This review focuses on self‐folding using surface tension or capillary forces derived from the minimization of liquid interfacial area. Due to favorable downscaling with length, at small scales capillary forces become extremely large relative to forces that scale with volume, such as gravity or inertia, and to forces that scale with area, such as elasticity. The major demonstrated classes of capillary force assisted self‐folding are discussed. These classes include the use of rigid or soft and micro‐ or nano‐patterned precursors that are assembled using a variety of liquids such as water, molten polymers, and liquid metals. The authors outline the underlying physics and highlight important design considerations that maximize rigidity, strength, and yield of the assembled structures. They also discuss applications of capillary self‐folding structures in engineering and medicine. Finally, the authors conclude by summarizing standing challenges and describing future trends.

With the discovery of graphene, significant research has focused on the synthesis, characterization, and applications of ultrathin materials. Graphene has also brought into focus other ultrathin materials composed of organics, polymers, inorganics, and their hybrids. Together, these ultrathin materials have unique properties of broad significance. For example, ultrathin materials have a large surface area and high flexibility which can enhance conformal contact in wearables and sensors leading to improved sensitivity. When porous, the short transverse diffusion length in these materials allows rapid mass transport. Alternatively, when impermeable, these materials behave as an ultrathin barrier. Such controlled permeability is critical in the design of encapsulation and drug delivery systems. Finally, ultrathin materials often feature defect-free and single-crystal-like two-dimensional atomic structures resulting in superior mechanical, optical, and electrical properties. A unique property of ultrathin materials is their low bending rigidity, which suggests that they could easily be bent, curved, or folded into 3D shapes. In this Account, we review the emerging field of 2D to 3D shape transformations of ultrathin materials. We broadly define ultrathin to include materials with a thickness below 100 nm and composed of a range of organic, inorganic, and hybrid compositions. This topic is important for both fundamental and applied reasons. Fundamentally, bending and curving of ultrathin films can cause atomistic and molecular strain which can alter their physical and chemical properties and lead to new 3D forms of matter which behave very differently from their planar precursors. Shape change can also lead to new 3D architectures with significantly smaller form factors. For example, 3D ultrathin materials would occupy a smaller space in on-chip devices or could permeate through tortuous media which is important for miniaturized robots and smart dust applications. Our Account highlights several differences between ultrathin and traditional shape change materials. The latter is typically associated with hydrogels, liquid crystals, or shape memory elastomers. As compared to bulk materials, ultrathin materials can much more easily bend and fold due to the significantly reduced bending modulus. Consequently, it takes much less energy to alter the shape of ultrathin materials, and even small environmental stimuli can trigger a large response. Further, the energy barriers between different configurations are small which allow a variety of conformations and enhances programmability. Finally, due to their ultrathin nature, the shape changes are typically not slowed down by sluggish mass or thermal transport, and thus, responses can be much faster than those of bulk materials. The latter point is important in the design of high-speed actuators. Consequently, ultrathin materials could enable low-power, rapid, programmable, and complex shape transformations in response to a broad range of stimuli such as pH, temperature, electro...

The local structure and geometry of catalytic interfaces can influence the selectivity of chemical reactions. Selectivity is often critical for the practical realization of reactions such as the electroreduction of carbon dioxide (CO2). Previously developed strategies to manipulate the structure and geometry of catalysts for electroreduction of CO2 involve complex processes or fail to efficiently alter the selectivity. Here, using a prestrained polymer, we uniaxially and biaxially compress a 60 nm gold film to form a nano-folded electrocatalyst for CO2 reduction. We observe two kinds of folds and can tune the ratio of loose to tight folds by varying the extent of prestrain in the polymer. We characterize the nano-folded catalysts using X-ray diffraction, scanning, and transmission electron microscopy. We observe grain reorientation and coarsening in the nano-folded gold catalysts. We measure an enhancement of Faradaic efficiency for carbon monoxide formation with the biaxially compressed nano-folded catalyst by a factor of about nine as compared to the flat catalyst (up to 87.4%). We rationalize this observation by noting that an increase of the local pH in the tight folds of the catalyst outweighs the effects of alterations in grain characteristics. Together, our studies demonstrate that nano-folded geometries can significantly alter grain characteristics, mass transport, and catalytic performance.

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Flexible, charged Pd nanosheets were prepared by using short chain thiolated carboxylic acids and amines. They could wrap around amine or hydroxyl functionalized micron-sized spheres driven by electrostatic interactions. When incubation with HepG2 cells, positively charged cysteamine (CA) functionalized Pd nanosheets exhibited a much higher cytotoxicity, showing more than 80% cell death at 100 ppm than the negatively charged 3-mecaptopropionic acid (MPA) functionalized ones which caused 30% of the cell death. The results show through surface functionalization, Pd nanosheets can be modified to interact differently with HepG2 cancerous cells, resulting in varied cytotoxicity.

Favorable scaling of capillary forces at small sizes makes them attractive for micro‐ and nanoscale assembly. In article number 1901677, Kam Sang Kwok, Qi Huang, Massimo Mastrangeli, and David H. Gracias review design principles, theoretical and experimental advances, and applications of 3D assembly by folding, bending, and curving using capillary forces.