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Nat Commun ; 10(1): 2842, 2019 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-31253800


Metal halide perovskite semiconductors possess outstanding characteristics for optoelectronic applications including but not limited to photovoltaics. Low-dimensional and nanostructured motifs impart added functionality which can be exploited further. Moreover, wider cation composition tunability and tunable surface ligand properties of colloidal quantum dot (QD) perovskites now enable unprecedented device architectures which differ from thin-film perovskites fabricated from solvated molecular precursors. Here, using layer-by-layer deposition of perovskite QDs, we demonstrate solar cells with abrupt compositional changes throughout the perovskite film. We utilize this ability to abruptly control composition to create an internal heterojunction that facilitates charge separation at the internal interface leading to improved photocarrier harvesting. We show how the photovoltaic performance depends upon the heterojunction position, as well as the composition of each component, and we describe an architecture that greatly improves the performance of perovskite QD photovoltaics.

Nat Chem ; 10(5): 532-539, 2018 05.
Artigo em Inglês | MEDLINE | ID: mdl-29610460


Magnesium-based batteries possess potential advantages over their lithium counterparts. However, reversible Mg chemistry requires a thermodynamically stable electrolyte at low potential, which is usually achieved with corrosive components and at the expense of stability against oxidation. In lithium-ion batteries the conflict between the cathodic and anodic stabilities of the electrolytes is resolved by forming an anode interphase that shields the electrolyte from being reduced. This strategy cannot be applied to Mg batteries because divalent Mg2+ cannot penetrate such interphases. Here, we engineer an artificial Mg2+-conductive interphase on the Mg anode surface, which successfully decouples the anodic and cathodic requirements for electrolytes and demonstrate highly reversible Mg chemistry in oxidation-resistant electrolytes. The artificial interphase enables the reversible cycling of a Mg/V2O5 full-cell in the water-containing, carbonate-based electrolyte. This approach provides a new avenue not only for Mg but also for other multivalent-cation batteries facing the same problems, taking a step towards their use in energy-storage applications.