Lithium–air batteries are considered to be a potential alternative to lithium-ion batteries for transportation applications, owing to their high theoretical specific energy1. So far, however, such systems have been largely restricted to pure oxygen environments (lithium–oxygen batteries) and have a limited cycle life owing to side reactions involving the cathode, anode and electrolyte2,3,4,5. In the presence of nitrogen, carbon dioxide and water vapour, these side reactions can become even more complex6,7,8,9,10,11. Moreover, because of the need to store oxygen, the volumetric energy densities of lithium–oxygen systems may be too small for practical applications12. Here we report a system comprising a lithium carbonate-based protected anode, a molybdenum disulfide cathode2 and an ionic liquid/dimethyl sulfoxide electrolyte that operates as a lithium–air battery in a simulated air atmosphere with a long cycle life of up to 700 cycles. We perform computational studies to provide insight into the operation of the system in this environment. This demonstration of a lithium–oxygen battery with a long cycle life in an air-like atmosphere is an important step towards the development of this field beyond lithium-ion technology, with a possibility to obtain much higher specific energy densities than for conventional lithium-ion batteries.
The work of A.S.-K., M. A., B. S. and P. A. was supported by the National Science Foundation (NSF-DMREF Award #1729420). Work by B.N., K.C.L., R.S.A., L.A.C., R.F.K., A.M., X. H. and J.R.J. was supported by the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the US Department of Energy, Office of Science, Basic Energy Sciences. Work by A.N. and C.L. was supported by the Center for Electrical Energy Storage: Tailored Interfaces, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences. The work of F.K.A. and K.K. was supported by a University of Illinois at Chicago start-up fund. C.L. was also supported by programme development funds provided by the Chemical Sciences and Engineering division at Argonne National Laboratory. We acknowledge the MRSEC Materials Preparation and Measurement Laboratory shared user facility at the University of Chicago (NSFDMR-1420709); the EPIC facility (NUANCE Center, Northwestern University), which has received support from the MRSEC program (NSF DMR-1121262) at the Materials Research Center; the Nanoscale Science and Engineering Center (NSF EEC−0647560) at the International Institute for Nanotechnology; and the State of Illinois, through the International Institute for Nanotechnology. This work also made use of the Integrated Molecular Structure Education and Research Center at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205). The acquisition of the UIC JEOL JEM ARM200CF was supported by an MRI-R2 grant from the National Science Foundation (DMR-0959470). The use of instrumentation at University of Illinois at Chicago Research Resources Center (RRC-East) is acknowledged. A. Nicholls at UIC’s Electron Microscopy Service is also acknowledged for help and support. This research used high performance computing resources of the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract DE-AC02-06CH11357. Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract DE-AC02-06CH11357. F.K.A. acknowledges the use of the University of Illinois at Chicago High Performance Computing Cluster to perform molecular dynamics simulations. We thank K. Gallagher, P. Redfern, H.-H. Wang, J. Jureller and X. Chen.
This file contains Supplementary Text and Data, Supplementary Figures 1-50, Supplementary Tables 1-6 and Supplementary References – see contents page for details.