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Lead halide perovskites present a versatile class of solution-processable semiconductors with highly tunable bandgaps that span ultraviolet, visible, and near-infrared portions of the spectrum. We explore phase-separated chloride and iodide lead perovskite mixtures as candidate materials for intermediate band applications in future photovoltaics. X-ray diffraction and scanning electron microscopy reveal that deposition of precursor solutions across the MAPbCl/MAPbI composition space affords quasi-epitaxial cocrystallized films, in which the two perovskites do not alloy but instead remain phase-segregated. First-principle calculations further support the formation of an epitaxial interface and predict energy offsets in the valence band and conduction band edges that could result in intermediate energy absorption. The charge dynamics of variable mixtures of the relatively narrow bandgap (1.57 eV) MAPbI perovskite and wide bandgap (3.02 eV) MAPbCl are probed to map charge and energy flow direction and kinetics. Time-resolved photoluminescence and transient absorption measurements reveal charge transfer of photoexcited carriers in MAPbCl to MAPbI in tens of picoseconds. The rate of quenching can be further tuned by replacing MAPbI with two-dimensional Ruddlesden-Popper (BA)(MA) Pb I ( n = 3, 2, and 1) perovskites, which also remain phase-separated.
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http://dx.doi.org/10.1021/acsami.8b20928 | DOI Listing |
Angew Chem Int Ed Engl
December 2024
Northeast Normal University, Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education, Institute of Functional Material Chemistry, Local United Engineering Lab for Power Battery, CHINA.
Construction of metal-organic cages (MOCs) with internal modifications is a promising avenue to build enzyme-like cavities and unlocking the mystery of highly catalytic activity and selectivity of enzymes. However, current interests are mainly focused on single-metal-node cages, little achievement has been expended to metalloclusters-based architectures, and the in situ endogenous generation of metal clusters. Herein, based on the hard-soft-acids-bases (HSAB), the metalloclusters-based heterometallic MOC (Cu3VMOP) constructed of [Cu3OPz3]+ and [V6O6(OCH3)9(SO4)(CO2)3]2- clusters was obtained by one-pot method.
View Article and Find Full Text PDFAnal Chem
December 2024
Department of Chemistry, College of Sciences, Northeastern University, Shenyang 110819, China.
In microwave (MW) thermotherapy, it is challenging to regulate the temporal and spatial distribution of the temperature at the nanoscale. Herein, we report a nanothermometer for simultaneous MW heating and temperature distribution measurement. The nanothermometer was prepared by free radical polymerization with vinylbenzyl trimethylammonium chloride (VBTMACl) as the MW thermosensitizer and isopropylacrylamide (NIPAM) as the thermoresponsive unit, followed by anion exchange with fluorophore sodium 3-(4-(1,2,2-triphenylvinyl)phenoxy)propane-1-sulfonate (TPESONa).
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
December 2024
Department of Materials Science, University of Milano-Bicocca, Via Roberto Cozzi 55, 20125 Milano, Italy.
The adsorption of (X = Ni, Pd, and Pt) nanoclusters is simulated by using first-principles methods on MgO(100) and on a MgO monolayer supported on Ag(100), considering the presence of interfacial oxygen. On both the free-standing MgO surface and MgO/Ag, all clusters exhibit robust adhesion and negative charge transfer. molecular dynamics calculations at 200 K demonstrate the stability of the nanoparticles on the MgO/Ag support.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
December 2024
Leiden Institute of Chemistry, Leiden University, P.O. Box 9502, Leiden 2300 RA, The Netherlands.
Understanding the electrolyte factors governing the electrochemical CO reduction reaction (CORR) is fundamental for selecting the optimized electrolyte conditions for practical applications. While noble metals are frequently studied, the electrolyte effects on the CORR on Sn catalysts are not well explored. Here, we studied the electrolyte effect on Sn metallic electrodes, investigating the impact of electrolyte concentration, cation identity, and anion properties, and how it shapes the CORR activity and selectivity.
View Article and Find Full Text PDFChem Sci
December 2024
Institute of Condensed Matter and Nanosciences, Molecular Chemistry, Materials and Catalysis, Université Catholique de Louvain Louvain-la-Neuve Belgium
Facilitating rapid charge transfer in electrode materials necessitates the optimization of their ionic transport properties. Currently, only a limited number of Li/Na-ion organic cathode materials have been identified, and those exhibiting intrinsic solid-phase ionic conductivity are even rarer. In this study, we present tetra-lithium and sodium salts with the generic formulae: A-Ph-CHP and A-Ph-PhP, wherein A = Li, Na; Ph-CHP = 2,5-dioxido-1,4-phenylene bis(methylphosphinate); Ph-PhP = 2,5-dioxido-1,4-phenylene bis(phenylphosphinate), as novel alkali-ion reservoir cathode materials.
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