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This content will become publicly available on January 17, 2019

Title: Stochasticity of Pores Interconnectivity in Li–O 2 Batteries and its Impact on the Variations in Electrochemical Performance

While large dispersions in electrochemical performance have been reported for lithium oxygen batteries in the literature, they have not been investigated in any depth. The variability in the results is often assumed to arise from differences in cell design, electrode structure, handling and cell preparation at different times. An accurate theoretical framework turns out to be needed to get a better insight into the mechanisms underneath and to interpreting experimental results. Here, we develop and use a pore network model to simulate the electrochemical performance of three-dimensionally resolved lithium-oxygen cathode mesostructures obtained from TXM nano-computed tomography images. Here, we apply this model to the 3D reconstructed object of a Super P carbon electrode and calculate discharge curves, using identical conditions, for four different zones in the electrode and their reversed configurations. The resulting galvanostatic discharge curves show some dispersion, (both in terms of capacity and overpotential) which we attribute to the way pores are connected with each other. Based on these results, we propose that the stochastic nature of pores interconnectivity and the microscopic arrangement of pores can lead, at least partially, to the variations in electrochemical results observed experimentally.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ; ORCiD logo [3] ;  [6] ; ORCiD logo [7]
  1. Univ. de Picardie Jules Verne, Amiens (France); ALISTORE-European Research Institute, Amiens (France); Univ. of Cambridge, Cambridge (United Kingdom)
  2. Univ. de Picardie Jules Verne, Amiens (France); Reseau sur le Stockage Electrochimique de l'Energie (RS2E), Amiens (France)
  3. ALISTORE-European Research Institute, Amiens (France); Univ. of Cambridge, Cambridge (United Kingdom)
  4. Univ. de Picardie Jules Verne, Amiens (France); ALISTORE-European Research Institute, Amiens (France); Reseau sur le Stockage Electrochimique de l'Energie (RS2E), Amiens (France)
  5. Argonne National Lab. (ANL), Lemont, IL (United States)
  6. Univ. of Cambridge, Cambridge (United Kingdom); Reseau sur le Stockage Electrochimique de l'Energie (RS2E), Amiens (France); Univ. de Toulouse, Toulouse cedex (France)
  7. Univ. de Picardie Jules Verne, Amiens (France); ALISTORE-European Research Institute, Amiens (France); Reseau sur le Stockage Electrochimique de l'Energie (RS2E), Amiens (France); Institut Univ. de France, Paris (France)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 4; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); European Research Council (ERC)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Li-O2 battery; pore interconnectivity; stochasticity; pore network; model; tomography
OSTI Identifier:
1454504