Ultrafast 2D Nanosheet Assembly via Spontaneous Spreading Phenomenon.

In 2D materials, a key engineering challenge is the mass production of large-area thin films without sacrificing their uniform 2D nature and unique properties. Here, it is demonstrated that a simple fluid phenomenon of water/alcohol solvents can become a sophisticated tool for self-assembly and designing organized structures of 2D nanosheets on a water surface. In situ, surface characterizations show that water/alcohol droplets of 2D nanosheets with cationic surfactants exhibit spontaneous spreading of large uniform monolayers within 10 s. Facile transfer of the monolayers onto solid or flexible substrates results in high-quality mono- and multilayer films with high coverages (>95%) and homogeneous electronic/optical properties. This spontaneous spreading is quite general and can be applied to various 2D nanosheets, including metal oxides, graphene oxide, h-BN, MoS2, and transition metal carbides, enabling on-demand smart manufacture of large-size (>4 inchϕ) 2D nanofilms and free-standing membranes.

Rational Cationic Disorder in Hexagonal Cesium Tungsten Bronze Nanoparticles for Infrared Absorption Materials.

Hexagonal cesium tungsten bronze (Cs0.33WO3) nanoparticles (NPs) have attracted attention for their potential applications in near-infrared (NIR) absorbing materials. However, the insufficient Cs doping in Cs0.33WO3 NPs has limited their NIR absorbing capabilities and practical stability. In this study, we demonstrate the transition pathway from intermediate W-defective Cs0.33WO3 NPs synthesized by flame spray pyrolysis to cationic (Cs, W)-disordered Cs0.33WO3 NPs prepared through appropriate heat treatments. Direct atomic observations reveal the basal shear and prismatic (Cs, W)-defective planes, which contributed to the disorder of full Cs doping in Cs0.33WO3 NPs. The obtained Cs0.33WO3 NPs with cationic disorder exhibited enhanced practical performance compared with conventional Cs0.33WO3 NPs. Therefore, the developed approach that regulates cationic disorder enables the rational design of defective metal oxides for a variety of applications, including NIR absorbing materials.

Gigantic Thermal Shielding in 2D Oxide Nanosheets.

Thermal shielding materials that can block near-infrared (NIR) light from the sunlight while maintaining visible transparency have become increasingly important from an energy-saving perspective. Here, we demonstrate a gigantic NIR shielding by an engineered plasmonic material based on a two-dimensional (2D) polytungstate (Cs4-xW11O35-d). Starting from a charge-neutral polytungstate (Cs4W11O35), we synthesize charge-imbalanced 2D nanosheets (Cs4-xW11O35-d) that undergo an unusual structural change with the semiconductor-to-metal transition in a reduced atmosphere. Layer-by-layer engineering of the 2D nanosheets enables a plasmon-induced enhancement of the NIR reflectance (>53%) with a high visible transparency (>71%), realizing high-performance thermal shielding. Our approach offers a solution for future thermal management technology.