Publications by authors named "Krzysztof Pupek"

In pursuit of the highest possible energy density, researchers shift their focus to the ultimate anode material, lithium metal (Li), and high-capacity cathode materials with high nickel content (Ni > 80%). The combination of these aggressive electrodes presents unprecedented challenges to the electrolyte. Here, we report a hybrid electrolyte consisting of a highly fluorinated ionic liquid and a weakly solvating fluorinated ether, whose hybridization structure enables the reversible operation of a battery chemistry based on Li and LiNiO (Ni = 100%), delivering nearly theoretical capacity of the latter (up to 249 mAh g) for >300 cycles with retention of 78.

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Article Synopsis
  • - Synchrotron X-ray in situ metrology effectively monitors battery material synthesis thanks to its high precision and chemical sensitivity, but the challenge lies in managing the vast amount of data generated in real-time.
  • - A new method called weighted lagged cross-correlation (WLCC) is introduced, enabling automated analysis of X-ray diffraction data to quickly track the calcination of nickel-based cathodes like LiNiO.
  • - This approach allows for quick identification of material phase changes, with insights gained within 10 seconds, thus supporting immediate experimental adjustments and enhancing quality control in battery cathode production.
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Calcination is a solid-state synthesis process widely deployed in battery cathode manufacturing. However, its inherent complexity associated with elusive intermediates hinders the predictive synthesis of high-performance cathode materials. Here, correlative in situ X-ray absorption/scattering spectroscopy is used to investigate the calcination of nickel-based cathodes, focusing specifically on the archetypal LiNiO from Ni(OH).

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Lithium-ion batteries play a crucial role in decarbonizing transportation and power grids, but their reliance on high-cost, earth-scarce cobalt in the commonly employed high-energy layered Li(NiMnCo)O cathodes raises supply-chain and sustainability concerns. Despite numerous attempts to address this challenge, eliminating Co from Li(NiMnCo)O remains elusive, as doing so detrimentally affects its layering and cycling stability. Here, we report on the rational stoichiometry control in synthesizing Li-deficient composite-structured LiNiMnO, comprising intergrown layered and rocksalt phases, which outperforms traditional layered counterparts.

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As state-of-the-art (SOA) lithium-ion (Li-ion) batteries approach their specific energy limit (∼250 Wh kg), layer-structured, nickel-rich (Ni-rich) lithium transition metal oxide-based cathode materials, e.g., LiNiMnCoO (NMC811), have attracted great interest owing to their practical high specific capacities (>200 mAhg).

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Fluorides have been identified as a key ingredient in interphases supporting aggressive battery chemistries. While the precursor for these fluorides must be pre-stored in electrolyte components and only delivered at extreme potentials, the chemical source of fluorine so far has been confined to either negatively-charge anions or fluorinated molecules, whose presence in the inner-Helmholtz layer of electrodes, and consequently their contribution to the interphasial chemistry, is restricted. To pre-store fluorine source on positive-charged species, here we show a cation that carries fluorine in its structure is synthesized and its contribution to interphasial chemistry is explored for the very first time.

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A fluorine-substituted ionic liquid based on a pyrrolidinium cation and a bis(fluorosulfonyl)imide anion was synthesized using a facile one-step reaction. The resulting ionic liquid is highly pure and when dissolved with LiFSI, the IL-based electrolyte showed good compatibility both in Li and graphite anodes, and superior voltage stability is demonstrated in a LiNiMnCoO cell.

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Nonaqueous electrolyte has become one of the technical barriers in enabling Li-ion battery comprising of a high voltage cathode and high capacity anode. In this work, we demonstrate a saturated piperidinum bis(fluorosulfonyl)imide ionic liquid (IL) with a LiFSI salt not only supports the redox reaction on the cathode at high voltages, but also shows exceptional kinetic stability on the lithiated anode as evidenced by its improved cycling performance in a NMC532/Si-graphite full cells cycled between 4.6 and 3.

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Fluorinated carbonates are pursued as liquid electrolyte solvents for high-voltage Li-ion batteries. Here we report aggregation of [Li(+)(FEC)3]n polymer species in fluoroethylene carbonate containing electrolytes and scrutinize the causes for this behavior.

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Antibiotics are typically more effective against replicating rather than nonreplicating bacteria. However, a major need in global health is to eradicate persistent or nonreplicating subpopulations of bacteria such as Mycobacterium tuberculosis (Mtb). Hence, identifying chemical inhibitors that selectively kill bacteria that are not replicating is of practical importance.

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Pyranocoumarin compounds were identified to embody a novel and unique pharmacophore for anti-TB activity. A systematic approach was taken to investigate the structural characteristics. Focused libraries of compounds were synthesized and evaluated for their anti-TB activity in primary screening assays.

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