4.8 Article

High Coulombic efficiency aluminum-ion battery using an AlCl3-urea ionic liquid analog electrolyte

Publisher

NATL ACAD SCIENCES
DOI: 10.1073/pnas.1619795114

Keywords

aluminum-ion battery; urea electrolyte; ionicity; ionic liquid; energy storage

Funding

  1. US Department of Energy [DOE DE-SC0016165]
  2. Global Networking Talent 3.0 Plan from the Ministry of Education of Taiwan [NTUST 104DI005]
  3. Taishan Scholar Project for Young Scholars of Shandong Province of China
  4. U.S. Department of Energy (DOE) [DE-SC0016165] Funding Source: U.S. Department of Energy (DOE)

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In recent years, impressive advances in harvesting renewable energy have led to a pressing demand for the complimentary energy storage technology. Here, a high Coulombic efficiency (similar to 99.7%) Al battery is developed using earth-abundant aluminum as the anode, graphite as the cathode, and a cheap ionic liquid analog electrolyte made from a mixture of AlCl3 and urea in a 1.3:1 molar ratio. The battery displays discharge voltage plateaus around 1.9 and 1.5 V (average discharge = 1.73 V) and yielded a specific cathode capacity of similar to 73 mAh g(-1) at a current density of 100 mA g(-1) (similar to 1.4 C). High Coulombic efficiency over a range of charge-discharge rates and stability over similar to 150-200 cycles was easily demonstrated. In situ Raman spectroscopy clearly showed chloroaluminate anion intercalation/deintercalation of graphite (positive electrode) during charge-discharge and suggested the formation of a stage 2 graphite intercalation compound when fully charged. Raman spectroscopy and NMR suggested the existence of AlCl4-, Al2Cl7- anions and [AlCl2 center dot(urea)(n)](+) cations in the AlCl3/urea electrolyte when an excess of AlCl3 was present. Aluminum deposition therefore proceeded through two pathways, one involving Al2Cl7 anions and the other involving [AlCl2 center dot(urea)(n)](+) cations. This battery is a promising prospect for a future high-performance, low-cost energy storage device.

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