Self-assembly of nanocrystal (NC) building blocks into mesoscopic superstructures with well-defined symmetry and geometry is essential for creating new materials with rationally designed properties. Despite the tremendous progress in colloidal assembly, it remains a fundamental challenge to assemble isotropic spherical NCs into one-dimensional (1D) ordered superstructures. Here, we report a new and general methodology that utilizes molecular clusters to induce the anisotropic assembly of NCs in solution, yielding polymer-like, single-NC-wide linear chains comprising as many as ∼1000 close-packed NCs. This cluster-assisted assembly process is applicable to various metallic, semiconductor, and magnetic NCs of different sizes and shapes. Mechanistic investigation reveals that the solvent-induced association of clusters plays a key role in driving the anisotropic assembly of NCs. Our work opens a solution-based route for linearly assembling NCs and represents an important step toward the bottom-up construction of 1D ordered NC superstructures.
Three-dimensional superlattices consisting of nanoparticles represent a new class of condensed materials with collective properties arising from coupling interactions between close-packed nanoparticles. Despite recent advances in self-assembly of nanoparticle superlattices, the constituent materials have been limited to those that are attainable as monodisperse nanoparticles. In addition, self-assembled nanoparticle superlattices are generally weakly coupled due to the surface-coating ligands. Here we report the fabrication of three-dimensionally interconnected nanoparticle superlattices with face-centered cubic symmetry without the presynthesis of the constituent nanoparticles. We show that mesoporous carbon frameworks derived from self-assembled supercrystals can be used as a robust matrix for the growth of nanoparticle superlattices with diverse compositions. The resulting interconnected nanoparticle superlattices embedded in a carbon matrix are particularly suitable for energy storage applications. We demonstrate this by incorporating tin oxide nanoparticle superlattices as anode materials for lithium-ion batteries, and the resulting electrochemical performance is attributable to their unique architectures.
While great progress has been achieved in the synthesis of ordered mesoporous carbons in the past decade, it still remains a challenge to prepare highly graphitic frameworks with ordered mesoporosity and high surface area. Reported herein is a simple synthetic methodology, based on the conversion of self-assembled superlattices of Fe3 O4 nanocrystals, to fabricate highly ordered mesoporous graphene frameworks (MGFs) with ultrathin pore walls consisting of three to six stacking graphene layers. The MGFs possess face-centered-cubic symmetry with interconnected mesoporosity, tunable pore width, and high surface area. Because of their unique architectures and superior structural durability, the MGFs exhibit excellent cycling stability and rate performance when used as anode materials for lithium-ion batteries, thus retaining a specific capacity of 520 mAh g(-1) at a current density of 300 mA g(-1) after 400 cycles.
The pursuit of multifunctional, innovative, more efficient, and safer cancer treatment has gained increasing interest in the research of preclinical nanoparticle-mediated photothermal therapy (PTT). Cell nucleus is recognized as the ideal target for cancer treatment because it plays a central role in genetic information and the transcription machinery reside. In this work, an efficient nuclear-targeted PTT strategy is proposed using transferrin and TAT peptide (TAT: YGRKKRRQRRR) conjugated monodisperse magnetic nanoparticles, which can be readily functionalized and stabilized for potential diagnostic and therapeutic applications. The monodisperse magnetic nanoparticles exhibit high photothermal conversion efficiency (≈37%) and considerable photothermal stability. They also show a high magnetization value and transverse relaxivity (207.1 mm s ), which could be applied for magnetic resonance imaging. The monodisperse magnetic nanoparticles conjugated with TAT peptides can efficiently target the nucleus and achieve the imaging-guided function, efficient cancer cells killing ability. Therefore, this work may present a practicable strategy to develop subcellular organelle targeted PTT agents for simultaneous cancer targeting, imaging, and therapy.
Self-assembled nanocrystal (NC) superlattices are emerging as an important class of materials with rationally modulated properties. Engineering the nanoscale structure of constituent building blocks as well as the mesoscale morphology of NC superlattices is a crucial step in widening their range of applications. Here, we report a template-assisted epitaxial assembly strategy, enabling growth of freestanding, carbon-coated tubular monolayer superlattices (TMSLs). Specifically, we design and construct TMSLs of hollow MnO NCs (h-MnO-TMSLs) by exploiting structural evolution of MnO NCs. The tubular superlattices obtained possess a number of unique and advantageous structural features unavailable in conventional NC superlattices, rendering them particularly attractive for energy conversion applications. We demonstrate this by employing h-MnO-TMSLs as electrocatalysts for oxygen reduction, the catalytic performance of which is comparable to that of state-of-the-art Pt/C catalysts and superior to that of most manganese oxide-based catalysts reported.
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