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1.
Sci Adv ; 6(42)2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-33055155

RESUMO

It remains a central challenge to the information display community to develop red light-emitting diodes (LEDs) that meet demanding color coordinate requirements for wide color gamut displays. Here, we report high-efficiency, lead-free (PEA)2SnI4 perovskite LEDs (PeLEDs) with color coordinates (0.708, 0.292) that fulfill the Rec. 2100 specification for red emitters. Using valeric acid (VA)-which we show to be strongly coordinated to Sn2+-we slow the crystallization rate of the perovskite, improving the film morphology. The incorporation of VA also protects tin from undesired oxidation during the film-forming process. The improved films and the reduced Sn4+ content enable PeLEDs with an external quantum efficiency of 5% and an operating half-life exceeding 15 hours at an initial brightness of 20 cd/m2 This work illustrates the potential of Cd- and Pb-free PeLEDs for display technology.

2.
Nat Commun ; 11(1): 4814, 2020 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-32968078

RESUMO

Surface ligands enable control over the dispersibility of colloidal quantum dots (CQDs) via steric and electrostatic stabilization. Today's device-grade CQD inks have consistently relied on highly polar solvents: this enables facile single-step deposition of multi-hundred-nanometer-thick CQD films; but it prevents the realization of CQD film stacks made up of CQDs having different compositions, since polar solvents redisperse underlying films. Here we introduce aromatic ligands to achieve process-orthogonal CQD inks, and enable thereby multifunctional multilayer CQD solids. We explore the effect of the anchoring group of the aromatic ligand on the solubility of CQD inks in weakly-polar solvents, and find that a judicious selection of the anchoring group induces a dipole that provides additional CQD-solvent interactions. This enables colloidal stability without relying on bulky insulating ligands. We showcase the benefit of this ink as the hole transport layer in CQD optoelectronics, achieving an external quantum efficiency of 84% at 1210 nm.

3.
Angew Chem Int Ed Engl ; 59(24): 9579-9585, 2020 Jun 08.
Artigo em Inglês | MEDLINE | ID: mdl-32115827

RESUMO

Commonly used methods to assess crystallinity, micro-/mesoporosity, Brønsted acid site density and distribution (in micro- vs. mesopores), and catalytic activity suggest nearly invariant structure and function for aluminosilicate zeolite MFI two-dimensional nanosheets before and after superheated steam treatment. Yet, pronounced reaction rate decrease for benzyl alcohol alkylation with mesitylene, a reaction that cannot take place in the zeolite micropores, is observed. Transmission electron microscopy images reveal pronounced changes in nanosheet thickness, aspect ratio and roughness indicating that nanosheet coarsening and the associated changes in the external (mesoporous) surface structure are responsible for the changes in the external surface catalytic activity. Superheated steam treatment of hierarchical zeolites can be used to alter nanosheet morphology and regulate external surface catalytic activity while preserving micro- and mesoporosity, and micropore reaction rates.

4.
Chemistry ; 25(43): 10045-10048, 2019 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-31236993

RESUMO

With the aim of understanding the thermochemistry of the introduction of mesoporosity in zeolites by using surfactants, high temperature oxide melt solution calorimetry was used to determine the change in the enthalpy of formation of USY zeolite before and after the introduction of mesoporosity. Our results confirm that this process only slightly destabilizes the zeolite by the additional surface area. However, this can be overcome by the stabilizing effect of the interactions between the surfactant and the zeolite framework.

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