Directing the formation of nanoscale architectures from nanoparticles is one of the key challenges in designing nanomaterials with prescribed functions. Atomic systems, given their ability to form molecules and crystals via directional chemical bonds, provide an inspiration for establishing approaches where nanoparticles with designed anisotropic binding modalities can be assembled into nanoscale architectures. However, fabricating such nanoparticles has been challenging due to their small dimensions and limited ways for site-specific control of their surface. To this end, we present a molecular stamping (MOST) approach to pattern DNA-coated nanoparticles with molecules at the predefined positions on a nanoparticle surface. This patterning is realized by use of a rigid and coordinative DNA frame as a molecular stamping apparatus (MOST App). The MOST App transfers multiple types of molecular “inks”, DNA sequences, onto a nanoparticle surface and fixes these molecular inks into place to form a designed pattern. After a nanoparticle is released the from MOST App, it possesses single-molecule patches that can provide anisotropic bonds with distinctive affinities. We further use these stamped nanoparticles to assemble prescribed clusters, whose structure is determined by the locations of patches. Using electron microscopy and tomographic methods, we investigate the efficiency of cluster formation and the resulting spatial arrangements of nanoparticles. The presented approach provides a single-molecule and spatially determined control over nanoparticle functionalization for creating nanoparticles with designed placement of different molecules and for realizing a rational fabrication of nanomaterial architectures.

Flow batteries are a compelling grid-scale energy storage technology because the stored energy is decoupled from the system power. Aqueous redox flow batteries (RFBs), however, are limited by low open-circuit voltages (OCVs). Replacing the aqueous negative electrolyte (negolyte) with liquid alkali metals-of which Na-K, a room-temperature liquid metal alloy, is attractivewould increase the OCV considerably. However, a suitable solid electrolyte has not been reported for Na-K. Here we show that K-b 00-alumina is a selective and robust K + ion conductor in contact with Na-K, to which it is stable with minimal exchange of Na. We report the cycling of cells with OCVs of 3.1-3.4 V employing aqueous and nonaqueous positive electrolytes (posolytes), and power density tests showing promising maximum power densities of 65 mW cm À2 at 22 C and >100 mW cm À2 at 57 C, ohmically limited by 330-mm K-b 00-alumina membranes. Further development of Na-KjK-b 00-alumina batteries could unlock cost-effective energy storage.

Rapid developments of DNA-based assembly methods provide versatile capabilities in organizing nanoparticles (NPs) in three-dimensional (3D) organized nanomaterials, which is important for optics, catalysis, mechanics, and beyond. However, the use of these nanomaterials is often limited by the narrow range of conditions in which DNA lattices are stable. We demonstrate here an approach to creating an inorganic, silica-based replica of 3D periodic DNA-NP structures with different lattice symmetries. The created ordered nanomaterials, through the precise 3D mineralization, maintain the spatial topology of connections between NPs by DNA struts and exhibit a controllable degree of the porosity. The formed silicated DNA-NP lattices exhibit excellent resiliency. They are stable when exposed to extreme temperatures (>1000°C), pressures (8 GPa), and harsh radiation conditions and can be processed by the conventional nanolithography methods. The presented approach allows the use of a DNA assembly strategy to create organized nanomaterials for a broad range of operational conditions.