Tuning Li2O2 Formation Routes by Facet Engineering of MnO2 Cathode Catalysts
- Michigan Technological Univ., Houghton, MI (United States). Dept. of Mechanical Engineering-Engineering Mechanics
- The Univ. of Illinois at Chicago, Chicago, IL (United States). Dept. of Mechanical and Industrial Engineering; Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Div.
- Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Div.
- The Univ. of Illinois at Chicago, Chicago, IL (United States). Dept. of Mechanical and Industrial Engineering
- Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Div.; Imam Abdulrahman Bin Faisal Univ., Dammam (Saudi Arabia). Inst. for Research and Medical Consultation
- Michigan Technological Univ., Houghton, MI (United States). Dept. of Mechanical Engineering-Engineering Mechanics; The Univ. of Illinois at Chicago, Chicago, IL (United States). Dept. of Mechanical and Industrial Engineering
In lithium-oxygen batteries, the solubility of LiO2 intermediates in the electrolyte regulates the formation routes of the Li2O2 discharge product. High-donor-number electrolytes with a high solubility of LiO2 tend to promote the formation of Li2O2 large particles following the solution route, which eventually benefits the cell capacity and cycle life. Here, we propose that facet engineering of cathode catalysts could be another direction in tuning the formation routes of Li2O2. In this work, fi-MnO2 crystals with high occupancies of {111} or {100} facets were adopted as cathode catalysts in Li-O2 batteries with a tetra(ethylene)glycol dimethyl ether electrolyte. The {111}-dominated beta-MnO2 catalyzed the formation of the Li2O2 discharge product into large toroids following the solution routes, while {100}-dominated beta-MnO2 facilitated the formation of Li2O2 thin films through the surface routes. Further computational studies indicate that the different formation routes of Li2O2 could be related to different adsorption energies of LiO2 on the two facets of beta-MnO2. Our results demonstrate that facet engineering of cathode catalysts could be a new way to tune the formation route of Li2O2 in a low-donor-number electrolyte. Here, we anticipate that this new finding would offer more choices for the design of lithium-oxygen batteries with high capacities and ultimately a long cycle life.
- Research Organization:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
- Grant/Contract Number:
- AC02-06CH11357
- OSTI ID:
- 1574365
- Journal Information:
- Journal of the American Chemical Society, Vol. 141, Issue 32; ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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