The self-organization of colloidal nanoparticles into programmed suprastructures is an important research area in various disciplines of nano, colloid, and polymer sciences. However, despite the recent advances in their fundamental understanding and practical applications, the selforganization of organic-free inorganic nanoparticles remains unexplored. Herein, we present the controlled organization of oppositely charged allinorganic nanoparticles through the electrostatic interaction and the colloidal behaviors of organized suprastructures. Depending on the charge states of the assembled suprastructures, three different phases, including patchy, patchy bridged, and fully coated particles, are identified, enabling the construction of the phase diagram with nanoparticle concentrations. Especially, the fully coated particles exhibit unexpected colloidal stability through the action of nanoparticles as surface stabilizers to induce the overcharged surface state; thus, we propose the concept of "nanoligands". It is demonstrated that this concept can be extended to a wide range of material combinations, including semiconducting, metallic, and oxide nanoparticles. The currently developed approach will enable the chemical designing of self-organized nanostructures.
Pt- and Ni-based thiometallates were developed as precursors to synthesize highly durable and monodispersed Pt/C and PtNi/C nano-sized electrocatalysts.
Optical three-dimensional (3D) printing techniques have attracted tremendous attention owing to their applicability to mask-less additive manufacturing, which enables the cost-effective and straightforward creation of patterned architectures. However, despite their potential use as alternatives to traditional lithography, the printable materials obtained from these methods are strictly limited to photocurable resins, thereby restricting the functionality of the printed objects and their application areas. Herein, we report a generalised direct optical printing technique to obtain functional metal chalcogenides via digital light processing. We developed universally applicable photocurable chalcogenidometallate inks that could be directly used to create 2D patterns or micrometre-thick 2.5D architectures of various sizes and shapes. Our process is applicable to a diverse range of functional metal chalcogenides for compound semiconductors and 2D transition-metal dichalcogenides. We then demonstrated the feasibility of our technique by fabricating and evaluating a micro-scale thermoelectric generator bearing tens of patterned semiconductors. Our approach shows potential for simple and cost-effective architecturing of functional inorganic materials.
Molecular and nanoscale amphiphiles have been extensively studied as building blocks for organizing macroscopic matter through specific and local interactions. Among various amphiphiles, inorganic Janus nanoparticles have attracted a lot of attention owing to their ability to impart multifunctionalities, although the programmability to achieve complicated self-assembly remains a challenge. Here, we synthesized matchstick-shaped Janus nano-surfactants that mimic organic surfactant molecules and studied their programmable self-assembly. High amphiphilicity was achieved through the hard–soft acid–base-based ligand-exchange reaction with strong selectivity on the surface of nano-matchsticks consisting of Ag2S heads and CdS stems. The obtained nano-surfactants spontaneously assembled into diverse ordered structures such as lamellar, curved, wrinkled, cylindrical, and micellar structures depending on the vertical asymmetry and the interfacial tension controlled by their geometry and surface ligands. The correlation between the phase selectivity of suprastructures and the characteristics of nano-surfactants is discussed. This study realized the molecular amphiphile-like programmability of inorganic Janus nanostructures in self-assembly with the precise control on the surface chemistry.
Optical three-dimensional (3D) printing techniques have attracted tremendous attention owing to their applicability to mask-less additive manufacturing, which enables the cost-effective and straightforward creation of patterned architectures. However, despite their potential use as alternatives to traditional lithography, the printable materials obtained from these methods are strictly limited to photocurable resins, thereby restricting the functionality of the printed objects and their application areas. Herein, we report a generalised direct optical printing technique to obtain functional metal chalcogenides via digital light processing. We developed universally applicable photocurable chalcogenidometallate inks that could be directly used to create 2D patterns or 3D architectures of various sizes and shapes. Our process is applicable to a diverse range of functional metal chalcogenides for compound semiconductors and 2D transition-metal dichalcogenides. We then demonstrated the feasibility of our technique by fabricating and evaluating a micro-scale thermoelectric generator bearing tens of patterned semiconductors. Our approach shows potential for simple and cost-effective architecturing of functional inorganic materials.
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