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Nanocrystals composed of copper(II) sulfide (CuS), a degenerately doped semiconductor with a direct optical bandgap, have been observed to exhibit both visible wavelength excitonic emission and strong localized surface plasmon resonances (LSPRs) in the near-infrared, making them prime candidates for exploring phenomena such as coupled light–matter interactions, quantum entanglement, and optical nonlinearity. Here, we report a computation-motivated synthetic approach for modulating the optical bandgap energy of plasmonic nanocrystals relative to their LSPR energies by tuning the composition of alloyed CuSexS1–xnanocrystals. CuSexS1–xalloys are examined by first-principles density functional theory (DFT) to understand the effects of composition tuning on the electronic and optical properties of CuSexS1–x, using high-throughput methods to probe Se occupation within a parent CuS unit cell. Results from this DFT analysis are used as input parameters for predicting the LSPR of CuSexS1–xnanostructures. To validate these DFT results against experimental observations, we synthesize CuSexS1–xusing CuS nanodisks as a template for a novel anion-exchange protocol. Optical characterization reveals qualitative agreement between our experimental and predicted materials properties, and we discuss how quantitative deviations from our predicted values are likely the result of interfacial and morphological characteristics that are unaccounted for in DFT models.

All-solid-state sodium–carbon dioxide (Na-CO2) battery is an emerging technology that effectively utilizes the greenhouse gas, CO2, for energy storage with the virtues of minimized electrolyte leakage and suppressed Na dendrite growth for the Na metal anode. However, the sluggish reduction/evolution reactions of CO2on the solid electrolyte/CO2cathode interface have caused premature battery failure. Herein, nitrogen (N)-doped nanocarbon derived from metal–organic frameworks is designed as a cathode catalyst to solve this challenge. The porous and highly conductive N-doped nanocarbon possesses superior uptake and binding capability with CO2, which significantly accelerates the CO2electroreduction and promotes the formation of thin sheetlike discharged products (200 nm in thickness) that can be easily decomposed upon charging. Accordingly, reduced discharge/charge overpotential, high discharge capacity (>10 000 mAh g–1), long cycle life, and high energy density (180 Wh kg–1in pouch cells) are achieved at 50 °C.