Perovskite Nanocrystals Protected by Hermetically Sealing for Highly Bright and Stable Deep-Blue Light-Emitting Diodes.

Metal-halide perovskite nanocrystals (NCs) have emerged as suitable light-emitting materials for light-emitting diodes (LEDs) and other practical applications. However, LEDs with perovskite NCs undergo environment-induced and ion-migration-induced structural degradation during operation; therefore, novel NC design concepts, such as hermetic sealing of the perovskite NCs, are required. Thus far, viable synthetic conditions to form a robust and hermetic semiconducting shell on perovskite NCs have been rarely reported for LED applications because of the difficulties in the delicate engineering of encapsulation techniques. Herein, a highly bright and durable deep-blue perovskite LED (PeLED) formed by hermetically sealing perovskite NCs with epitaxial ZnS shells is reported. This shell protects the perovskite NCs from the environment, facilitates charge injection/transport, and effectively suppresses interparticle ion migration during the LED operation, resulting in exceptional brightness (2916 cd m-2 ) at 451 nm and a high external quantum efficiency of 1.32%. Furthermore, even in the unencapsulated state, the LED shows a long operational lifetime (T50 ) of 1192 s (≈20 min) in the air. These results demonstrate that the epitaxial and hermetic encapsulation of perovskite NCs is a powerful strategy for fabricating high-performance deep-blue-emitting PeLEDs.

Microfluidics-Assisted Synthesis of Hierarchical Cu2 O Nanocrystal as C2 -Selective CO2 Reduction Electrocatalyst.

Copper-based catalysts have attracted enormous attention due to their high selectivity for C2+ products during the electrochemical reduction of CO2 (CO2 RR). In particular, grain boundaries on the catalysts contribute to the generation of various Cu coordination environments, which have been found essential for C-C coupling. However, smooth-surfaced Cu2 O nanocrystals generally lack the ability for the surface reorganization to form multiple grain boundaries and desired Cu undercoordination sites. Flow chemistry armed with the unparalleled ability to mix reaction mixture can achieve a very high concentration of unstable reaction intermediates, which in turn are used up rapidly to lead to kinetics-driven nanocrystal growth. Herein, the synthesis of a unique hierarchical structure of Cu2 O with numerous steps (h-Cu2 O ONS) via flow chemistry-assisted modulation of nanocrystal growth kinetics is reported. The surface of h-Cu2 O ONS underwent rapid surface reconstruction under CO2 RR conditions to exhibit multiple heterointerfaces between Cu2 O and Cu phases, setting the preferable condition to facilitate C-C bond formation. Notably, the h-Cu2 O ONS obtained the increased C2 H4 Faradaic efficiency from 31.9% to 43.5% during electrocatalysis concurrent with the morphological reorganization, showing the role of the stepped surface. Also, the h-Cu2 O ONS demonstrated a 3.8-fold higher ethylene production rate as compared to the Cu2 O nanocube.

Mn-Dopant Differentiating the Ru and Ir Oxidation States in Catalytic Oxides Toward Durable Oxygen Evolution Reaction in Acidic Electrolyte.

Designing an efficient and durable electrocatalyst for the sluggish oxygen evolution reaction (OER) at the anode remains the foremost challenge in developing proton exchange membrane (PEM) electrolyzers. Here, a highly active and durable cactus-like nanoparticle with an exposed heterointerface between the IrO2 and the low oxidation state Ru by introducing a trace amount of Mn dopant is reported. The heterostructure fabrication relies on initial mixing of the Ru and Ir phases before electrochemical oxidation to produce a conjoined Ru/IrO2 heterointerface. Benefitting from electron transfer at the heterointerface, the low oxidation state Ru species shows excellent initial activity, which is maintained even after 180 h of continuous OER test. In a half-cell test, the Mn-doped RuIr nanocactus (Mn-RuIr NCT) achieves a mass activity of 1.85 A mgIr+Ru -1 at 1.48 VRHE , which is 139-fold higher than that of commercial IrO2 . Moreover, the superior electrocatalytic performance of Mn-RuIr NCT in the PEM electrolysis system ensures its viability in practical uses. The results of the excellent catalytic performance for acidic OER indicate that the heterostructuring robust rutile IrO2 and the highly active Ru species with a low oxidation state on the catalyst surface drive a synergistic effect.

Pt2+-Exchanged ZIF-8 nanocube as a solid-state precursor for L10-PtZn intermetallic nanoparticles embedded in a hollow carbon nanocage.

Nanoparticles with an atomically ordered alloy phase have received enormous attention for application as catalysts in fuel cells because of their unique electronic properties resulting from unusually strong d-orbital interactions between two metal components. However, the synthesis of intermetallic nanoparticles requires a high reaction temperature, thus necessitating the protection of nanoparticles with inorganic layers to prevent aggregation of nanoparticles during synthesis. The protective layer needs to be removed later for application as a catalyst, which is a cumbersome process. Herein, a novel synthetic strategy is reported for the preparation of L10-PtZn intermetallic nanoparticles by utilizing Pt2+-exchanged ZIF-8 nanocubes as a solid-state precursor. The Pt2+-exchanged ZIF-8 phase plays a dual role as a metal ion source for L10-PtZn nanoparticles and as a carbonaceous matrix that restrains the aggregation of nanoparticles during thermal treatment. The L10-PtZn nanoparticles embedded in a hollow carbon nanocage obtained from one-step annealing of Pt2+-exchanged ZIF-8 showed better electrocatalytic activity and durability toward methanol oxidation under acidic electrolyte conditions than those obtained from commercial Pt/C catalysts.

Morphology-Controlled Metal Sulfides and Phosphides for Electrochemical Water Splitting.

Because H2 is considered a promising clean energy source, water electrolysis has attracted great interest in related research and technology. Noble-metal-based catalysts are used as electrode materials in water electrolyzers, but their high cost and low abundance have impeded them from being used in practical areas. Recently, metal sulfides and phosphides based on earth-abundant transition metals have emerged as promising candidates for efficient water-splitting catalysts. Most studies have focused on adjusting the composition of the metal sulfides and phosphides to enhance the catalytic performance. However, morphology control of catalysts, including faceted and hollow structures, is much less explored for these systems because of difficulties in the synthesis, which requires a deep understanding of the nanocrystal growth process. Herein, representative synthetic methods for morphology-controlled metal sulfides and phosphides are introduced to provide insights into these methodologies. The electrolytic performance of morphology-controlled metal sulfide- and phosphide-based nanocatalysts with enhanced surface area and intrinsically high catalytic activity is also summarized and the future research directions for this promising catalyst group is discussed.

Synthesis of nano-sized urchin-shaped LiFePO4 for lithium ion batteries.

In this article, the facile synthesis of sea urchin-shaped LiFePO4 nanoparticles by thermal decomposition of metal-surfactant complexes and application of these nanoparticles as a cathode in lithium ion secondary batteries is demonstrated. The advantages of this work are a facile method to synthesize interesting LiFePO4 nanostructures and its synthetic mechanism. Accordingly, the morphology of LiFePO4 particles could be regulated by the injection of oleylamine, with other surfactants and phosphoric acid. This injection step was critical to tailor the morphology of LiFePO4 particles, converting them from nanosphere shapes to diverse types of urchin-shaped nanoparticles. Electron microscopy analysis showed that the overall dimension of the urchin-shaped LiFePO4 particles varied from 300 nm to 2 µm. A closer observation revealed that numerous thin nanorods ranging from 5 to 20 nm in diameter were attached to the nanoparticles. The hierarchical nanostructure of these urchin-shaped LiFePO4 particles mitigated the low tap density problem. In addition, the nanorods less than 20 nm attached to the edge of urchin-shaped nanoparticles significantly increased the pathways for electronic transport.

Recent advances in electrocatalysts toward the oxygen reduction reaction: the case of PtNi octahedra.

Designing highly efficient and durable electrocatalysts for the oxygen reduction reaction (ORR), the key step for the operation of polymer electrolyte membrane fuel cells (PEMFCs), is of a pivotal importance for advancing PEMFC technology. Since the most significant progress has been made on Pt3Ni(111) alloy surfaces, nanoscale PtNi alloy octahedra enclosed by (111) facets have emerged as promising electrocatalysts toward the ORR. However, because their practical uses have been hampered by the cost, sluggish reaction kinetics, and poor durability, recent advances have engendered a wide variety of structure-, size-, and composition-controlled bimetallic PtNi octahedra. Herein, we therefore review the important recent developments of PtNi octahedral electrocatalysts point by point to give an overview of the most promising strategies. Specifically, the present review article focuses on the synthetic methods for the PtNi octahedra, the core-shell and multi-metallic strategies for performance improvement, and their structure-, size-, and composition-control-based ORR activity. By considering the results achieved in this field, a prospect for this alloy nanocatalysts system for future sustainable energy applications is also proposed.

NiOOH Exfoliation-Free Nickel Octahedra as Highly Active and Durable Electrocatalysts Toward the Oxygen Evolution Reaction in an Alkaline Electrolyte.

A layered ß-NiOOH crystal with undercoordinated facets is an active and economically viable nonnoble catalyst for the oxygen evolution reaction (OER) in alkaline electrolytes. However, it is extremely difficult to enclose the ß-NiOOH crystal with undercoordinated facets because of its inevitable crystal transformation to γ-NiOOH, resulting in the exfoliation of the catalytic surfaces. Herein, we demonstrate {111}-faceted Ni octahedra as the parent substrates whose surfaces are easily transformed to catalytically active ß-NiOOH during the alkaline OER. Electron microscopic measurements demonstrate that the horizontally stacked ß-NiOOH on the surfaces of Ni octahedra has resistance to further oxidation to γ-NiOOH. By contrast, significant crystal transformation and thus the exfoliation of the γ-NiOOH sheets can be observed on the surfaces of Ni cubes and rhombic dodecahedra (RDs). Electrocatalytic measurements show that the ß-NiOOH formed on Ni octahedra exhibits highly enhanced OER durability compared to the Ni cubes, Ni RDs, and the state-of-the-art Ir/C catalysts.