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

Chongyin Yang, Ji Chen, Xiao Ji, Travis P. Pollard, Xujie Lü, Cheng-Jun Sun, Singyuk Hou, Qi Liu, Cunming Liu, Tingting Qing, Yingqi Wang, Oleg Borodin, Yang Ren, Kang Xu and Chunsheng Wang ()
Additional contact information
Chongyin Yang: University of Maryland
Ji Chen: University of Maryland
Xiao Ji: University of Maryland
Travis P. Pollard: Sensor and Electron Devices Directorate, US Army Research Laboratory
Xujie Lü: Center for High Pressure Science and Technology Advanced Research
Cheng-Jun Sun: Argonne National Laboratory
Singyuk Hou: University of Maryland
Qi Liu: Argonne National Laboratory
Cunming Liu: Argonne National Laboratory
Tingting Qing: University of Maryland
Yingqi Wang: Center for High Pressure Science and Technology Advanced Research
Oleg Borodin: Sensor and Electron Devices Directorate, US Army Research Laboratory
Yang Ren: Argonne National Laboratory
Kang Xu: Sensor and Electron Devices Directorate, US Army Research Laboratory
Chunsheng Wang: University of Maryland

Nature, 2019, vol. 569, issue 7755, 245-250

Abstract: Abstract 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 anodes1–4. However, the limited lithium intercalation capacities (less than 200 milliampere-hours per gram) of typical transition-metal-oxide cathodes5,6 preclude higher energy densities. Partial7,8 or exclusive9 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, C3.5[Br0.5Cl0.5], 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. 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.

Date: 2019
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DOI: 10.1038/s41586-019-1175-6

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