Electrocatalytic denitrification is considered as the most promising technology to transform nitrates to nitrogen gas in sewage so far. Although noble metal-based catalysts as a cathode material have reached decent removal capacity of nitrate, the high cost is the main hamper of electrocatalytic reduction. Therefore, the development of alternative catalysis toward highly effective denitrification is imperative yet still remains a significant challenge. Herein, a corchorifolius-like structure, where Fe nanoparticles are sealed in carbon microspheres (CL-Fe@C) with a rough surface, has been elaborately designed by self-assemble strategy. Impressively, the architectured CL-Fe@C microspheres are surrounded with a lot of small iron nanoparticles and contain the high iron content of ∼74%. As a result, an excellent removal capacity of 1816 mg N/g Fe and a high nitrogen selectivity of 98% under a very low nitrate concentration of 100 mg/L are achieved when using the CL-Fe@C microspheres as electrocatalytic denitrification. The present work not only explores high performance electrocatalysis for the denitrification but also promote new inspiration for the preparation of other iron-based functional materials for diverse applications.

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.