Characterization of electrochemical processes occurring in nonaqueous Li-O2 batteries
Bryan D. McCloskey
IBM Research Division, Almaden, CA. USA
bmcclos@us.ibm.com
 
The 2008 IBM Almaden Research Grand Challenge launched a project with the goal of developing practical rechargeable Li-air batteries. Li-air batteries have received significant attention as a potential high specific energy alternative to current state-of-the-art rechargeable Li-ion batteries.1 Nevertheless, published Li-air embodiments have only achieved a small fraction of their enormous theoretical specific energy with very limited rechargeability, and many operational aspects, including lithium-oxygen electrochemistry, appear to be poorly understood.

This presentation will outline our efforts to characterize various fundamental properties of non-aqueous Li-O2 electrochemistry occurring at the positive electrode.

Quantitative Differential electrochemical Mass Spectrometry (DEMS) and electro-chemical measurements on flat, non-porous glassy carbon electrodes were coupled with ex-situ chemical analysis of electrodes to better understand factors that control, and hinder, the desired rechargeable cathodic reaction (i.e., 2Li+ + O2 + 2e- ↔ Li2O2). Among the topics to be discussed will be Li2O2 electronic conductivity,2,3 heterogeneous electrocatalysis,4 and electrolyte/electrode stability.5,6.
1. Girishkumar, G.; McCloskey, B.; Luntz, A. C.; Swanson, S. & Wilcke, W. Lithium−air battery: promise and challenges. The Journal of Physical Chemistry Letters 2010, 1, 2193-2203.
2. Viswanathan, V.; Thygesen, K. S.; Hummelshoj, J. S.; Norskov, J. K.; Girishkumar, G.; McCloskey, B. D. & Luntz, A. C. Electrical conductivity in Li2O2 and its role in determining capacity limitations in non-aqueous Li-O2 batteries. The Journal of Chemical Physics 2011, 135, 214704.
3. Albertus, P.; Girishkumar, G.; McCloskey, B.; Sanchez-Carrera, R. S.; Kozinsky, B.; Christensen, J. & Luntz, A. C. Identifying capacity limitations in the Li/oxygen battery using experiments and modeling. Journal of the Electrochemical Society 2011, 158, A343-A351.
4. McCloskey, B. D.; Scheffler, R.; Speidel, A.; Bethune, D. S.; Shelby, R. M. & Luntz, A. C. On the efficacy of electrocatalysis in nonaqueous Li–O2 batteries. Journal of the American Chemical Society 2011, 133, 18038-18041.
5. McCloskey, B. D.; Speidel, A.; Scheffler, R.; Miller, D. C.; Viswanathan, V.; Hummelshøj, J. S.; Nørskov, J. K. & Luntz, A. C. Twin problems of interfacial carbonate formation in nonaqueous Li–O2 batteries. The Journal of Physical Chemistry Letters 2012, 3, 997-1001.
6. McCloskey, B. D.; Bethune, D. S.; Shelby, R. M.; Girishkumar, G. & Luntz, A. C. Solvents’ critical role in nonaqueous lithium–oxygen battery electrochemistry. The Journal of Physical Chemistry Letters 2011, 2, 1161-1166.
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