Search for: All records

Aluminum nanocrystals (AlNCs) are of increasing interest as sustainable, earth-abundant nanoparticles for visible wavelength plasmonics and as versatile nanoantennas for energy-efficient plasmonic photocatalysis. Here, we show that annealing AlNCs under various gases and thermal conditions induces substantial, systematic changes in their surface oxide, modifying crystalline phase, surface morphology, density, and defect type and concentration. Tailoring the surface oxide properties enables AlNCs to function as all-aluminum-based antenna-reactor plasmonic photocatalysts, with the modified surface oxides providing varying reactivities and selectivities for several chemical reactions. 

Polycrystalline LiMo8O10 was prepared in a sealed Mo crucible at 1380 °C for 48 h using the conventional high-temperature solid-state method. The polar tetragonal crystal structure (space group I41md) is confirmed based on the Rietveld refinement of powder neutron diffraction and 7Li/6Li solid-state NMR. The crystal structure features infinite chains of Mo4O5 (i.e., Mo2Mo4/2O6/2O6/3) as a repeat unit containing edge-sharing Mo6 octahedra with strong Mo–Mo metal bonding along the chain. X-ray absorption near-edge spectroscopy of the Mo-L3 edge is consistent with the formal Mo valence/configuration. Magnetic measurements reveal that LiMo8O10 is paramagnetic down to 1.8 K. Temperature-dependent resistivity [ρ(T)] measurement indicates a semiconducting behavior that can be fitted with Mott’s variable range hopping conduction mechanism in the temperature range of 215 and 45 K. The ρ(T) curve exhibits an exponential increase below 5 K with a large ratio of ρ1.8/ρ300 = 435. LiMo8O10 shows a negative field-dependent magnetoresistance between 2 and 25 K. Heat capacity measurement fitted with the modified Debye model yields the Debye temperature of 365 K. 

We designed a novel multicoordinating ligand based on the N-heterocyclic carbene (NHC) anchoring molecules and applied them for stabilizing luminescent quantum dots in aqueous media. The ligand is synthesized via nucleophilic addition reaction between amine-appended imidazole/poly(ethylene glycol) compounds and poly(isobutylene-alt-maleic anhydride) (PIMA), followed by carbene generation. We find that these NHC-based polymers exhibit fast and robust coordinating affinity to CdSe QDs overcoated with ZnS shells. The removal of hydrophobic coating and the generation of carbene are demonstrated by 1H NMR spectroscopy. 13C NMR spectroscopy confirms the existence of carbene-Zn complexes which is crucial for binding transition-metals on QD surfaces. These QDs exhibit absorption and emission features with little to no change before and after cap exchange, and their PL intensity is increased under light exposure. Excellent colloidal stability of these QD samples is observed in a wide range of competitive conditions over long period of time. Agarose gel electrophoresis indicates that the polymer coating imparts QDs with good compatibility in different aqueous buffers, and it prevents protein adsorption.