Aqueous Li-ion battery enabled by halogen conversion–intercalation chemistry in graphite

Yang, Chongyin; Chen, Ji; Ji, Xiao; Pollard, Travis P.; Lü, Xujie; Sun, Cheng -Jun; Hou, Singyuk; Liu, Qi; Liu, Cunming; Qing, Tingting; Wang, Yingqi; Borodin, Oleg; Ren, Yang; Xu, Kang; Wang, Chunsheng

doi:10.1038/s41586-019-1175-6

Aqueous Li-ion battery enabled by halogen conversion–intercalation chemistry in graphite

Journal Article · Wed May 08 00:00:00 EDT 2019 · Nature (London)

DOI:https://doi.org/10.1038/s41586-019-1175-6· OSTI ID:1559969

Yang, Chongyin ^[1]; Chen, Ji ^[1]; Ji, Xiao ^[1]; Pollard, Travis P. ^[2]; Lü, Xujie ^[3]; Sun, Cheng -Jun ^[4]; Hou, Singyuk ^[1]; Liu, Qi ^[5]; Liu, Cunming ^[4]; Qing, Tingting ^[1]; Wang, Yingqi ^[3]; Borodin, Oleg ^[2]; Ren, Yang ^[4]; Xu, Kang ^[2]; Wang, Chunsheng ^[1]

Univ. of Maryland, College Park, MD (United States)
U.S. Army Research Lab., Adelphi, MD (United States)
Center for High Pressure Science and Technology Advanced Research, Shanghai (China)
Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); City Univ. of Hong Kong, Hong Kong (China)

The use of 'water-in-salt' electrolytes has considerably expanded the electrochemical window of aqueous lithium-ion batteries to 3 to 4 volts, making it possible to couple high-voltage cathodes with low-potential graphite anodes. However, the limited lithium intercalation capacities (less than 200 milliampere-hours per gram) of typical transition-metal-oxide cathodes preclude higher energy densities. Partial or exclusive anionic redox reactions may achieve higher capacity, but at the expense of reversibility. Here we report a halogen conversion-intercalation chemistry in graphite that produces composite electrodes with a capacity of 243 milliampere-hours per gram (for the total weight of the electrode) at an average potential of 4.2 volts versus Li/Li⁺. Experimental characterization and modelling attribute this high specific capacity to a densely packed stage-I graphite intercalation compound, C_3.5[Br_0.5Cl_0.5], which can form reversibly in water-in-bisalt electrolyte. By coupling this cathode with a passivated graphite anode, we create a 4-volt-class aqueous Li-ion full cell with an energy density of 460 watt-hours per kilogram of total composite electrode and about 100 per cent Coulombic efficiency. Here, this anion conversion-intercalation mechanism combines the high energy densities of the conversion reactions, the excellent reversibility of the intercalation mechanism and the improved safety of aqueous batteries.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1559969

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7755 Vol. 569; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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