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1.
Angew Chem Int Ed Engl ; 63(6): e202310905, 2024 Feb 05.
Article in English | MEDLINE | ID: mdl-38100193

ABSTRACT

Electrolytes that can keep liquid state are one of the most important physical metrics to ensure the ions transfer with stable operation of rechargeable lithium-based batteries at a wide temperature window. It is generally accepted that strong polar solvents with high melting points favor the safe operation of batteries above room temperatures but are susceptible to crystallization at low temperatures (≤-40 °C). Here, a crystallization limitation strategy was proposed to handle this issue. We demonstrate that, although the high melting points of ethylene sulfite (ES, -17 °C) and fluoroethylene carbonate (FEC, ≈23 °C), their mixtures can avoid crystallization at low temperatures, which can be attributed to low intermolecular interactions and altered molecular motion dynamics. A suitable ES/FEC ratio (10 % FEC) can balance the bulk and interface transport of ions, enabling LiNi0.8 Mn0.1 Co0.1 O2 ||lithium (NCM811||Li) full cells to deliver excellent temperature resilience and cycling stability over a wide temperature range from -50 °C to +70 °C. More than 66 % of the capacity retention was achieved at -50 °C compared to room temperature. The NCM811||Li pouch cells exhibit high cycling stability under realistic conditions (electrolyte weight to cathode capacity ratio (E/C)≤3.5 g Ah-1 , negative to positive electrode capacity ratio (N/P)≤1.09) at different temperatures.

2.
ChemSusChem ; 16(18): e202300590, 2023 Sep 22.
Article in English | MEDLINE | ID: mdl-37302979

ABSTRACT

Ether-based electrolytes that are endowed with decent compatibility towards lithium anode have been regarded as promising candidates for constructing energy-dense lithium metal batteries (LMBs), but their applications are hindered by low oxidation stability in conventional salt concentration. Here, we reported that regulating the chelating power and coordination structure can remarkably increase the high-voltage stability of ether-based electrolytes and lifespan of LMBs. Two ether molecules of 1,3-dimethoxypropane (DMP) and 1,3-diethoxypropane (DEP) are designed and synthesized as solvents of electrolytes to replace the traditional ether solvent (1,2-dimethoxyethane, DME). Both computational and spectra reveal that the transition from five- to six-membered chelate solvation structure by adding one methylene on DME results in the formation of weak Li solvates, which increase the reversibility and high-voltage stability in LMBs. Even under lean electrolyte (5 mL Ah-1 ) and low anode to cathode ratio (2.6), the fabricated high-voltage Li||LiNi0.8 Co0.1 Mn0.1 O2 LMBs using electrolyte of 2.30 M Lithiumbisfluorosulfonimide (LiFSI)/DMP still show capacity retention over 90 % after 184 cycles. This work highlights the importance of designing the coordination structures in non-fluorine ether electrolytes for rechargeable batteries.

3.
Angew Chem Int Ed Engl ; 61(39): e202209642, 2022 Sep 26.
Article in English | MEDLINE | ID: mdl-35909226

ABSTRACT

Quinone compounds, which are capable of accommodating proton (H+ ), are emerging electrodes in aqueous batteries. However, the storage mechanism of proton in quinone compounds is less known and the energy/power density of quinone-based proton battery is still limited. Here we design a series of quinone anodes and study their electrochemical properties in acidic electrolyte, in which tetramethylquinone (TMBQ) delivers a high capacity of 300 mAh g-1 with an extremely low polarization of 20 mV at 1 C, and maintains over 50 % theoretical capacity in less than 16 seconds. The fast kinetics of TMBQ is attributed to the continuous H+ migration channel, high H+ diffusion coefficient (10-6  cm2 s-1 ), and low H+ migration energy barrier (0.26 eV). When coupling with MnO2 cathode, the battery shows a long lifespan of 4000 cycles with a capacity retention of 77 % at 5 C. This study reveals the proton transport in quinone-electrodes and offers new insights to design advanced aqueous batteries.

4.
Org Biomol Chem ; 17(13): 3409-3415, 2019 03 27.
Article in English | MEDLINE | ID: mdl-30869715

ABSTRACT

Rare multiple fluorescence properties including aggregation-induced emission and polymorphism/shape/size-dependent emission were found coexisting in a class of typical non-steroidal anti-inflammatory analgesic drugs, fenamates, which could provide a new approach toward future drug evaluation. Different from the complexity and biological incompatibility of the traditional AIE molecular design, this work opens new avenues to the development of new AIE systems.


Subject(s)
Analgesics/chemistry , Anti-Inflammatory Agents, Non-Steroidal/chemistry , Fenamates/chemistry , Fluorescent Dyes/chemistry , Drug Evaluation , Fluorescence , Molecular Structure , Particle Size , Quantum Theory
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