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

Journal Article · · Nature (London)
 [1];  [1];  [1];  [2];  [3];  [4];  [1];  [5];  [4];  [1];  [3];  [2];  [4];  [2];  [1]
  1. Univ. of Maryland, College Park, MD (United States)
  2. U.S. Army Research Lab., Adelphi, MD (United States)
  3. Center for High Pressure Science and Technology Advanced Research, Shanghai (China)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. 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, 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. 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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC); USDOE Advanced Research Projects Agency - Energy (ARPA-E)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1559969
Journal Information:
Nature (London), Vol. 569, Issue 7755; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 502 works
Citation information provided by
Web of Science

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Porosity‐ and Graphitization‐Controlled Fabrication of Nanoporous Silicon@Carbon for Lithium Storage and Its Conjugation with MXene for Lithium‐Metal Anode journal December 2019
Boosting Zn‐Ion Energy Storage Capability of Hierarchically Porous Carbon by Promoting Chemical Adsorption journal September 2019
Thick Electrode Batteries: Principles, Opportunities, and Challenges journal July 2019
A Coaxial‐Interweaved Hybrid Lithium Metal Anode for Long‐Lifespan Lithium Metal Batteries journal August 2019
Development of Safe and Sustainable Dual‐Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes journal January 2020
Halogenid‐basierte Materialien und Chemie für wiederaufladbare Batterien journal January 2020
A Dual Plating Battery with the Iodine/[ZnI x (OH 2 ) 4− x ] 2− x Cathode journal September 2019
Exploiting Mechanistic Solvation Kinetics for Dual‐Graphite Batteries with High Power Output at Extremely Low Temperature journal November 2019
Halide‐Based Materials and Chemistry for Rechargeable Batteries journal January 2020
Exploiting Mechanistic Solvation Kinetics for Dual‐Graphite Batteries with High Power Output at Extremely Low Temperature journal December 2019
Superior Selectivity and Tolerance towards Metal‐Ion Impurities of a Fe/N/C Catalyst for CO 2 Reduction journal July 2019
Enhancing Zn‐Ion Storage Capability of Hydrated Vanadium Pentoxide by the Strategic Introduction of La 3+ journal March 2020
Structural Strategies for Germanium‐Based Anode Materials to Enhance Lithium Storage journal August 2019
3D Oxygen‐Defective Potassium Vanadate/Carbon Nanoribbon Networks as High‐Performance Cathodes for Aqueous Zinc‐Ion Batteries journal October 2019
Aqueous batteries get energetic journal July 2019
Graphene-covered transition metal halide molecules as efficient and durable electrocatalysts for oxygen reduction and evolution reactions journal January 2019
Voltage issue of aqueous rechargeable metal-ion batteries journal January 2020
A zinc bromine “supercapattery” system combining triple functions of capacitive, pseudocapacitive and battery-type charge storage journal January 2020
Flexible all-in-one zinc-ion batteries journal January 2019
High performance polyanthraquinone/Co–Ni(OH) 2 aqueous batteries based on hydroxyl and potassium insertion/extraction reactions journal January 2020
Rechargeable aqueous hybrid ion batteries: developments and prospects journal January 2019
Boosting the Zn-ion storage capability of birnessite manganese oxide nanoflorets by La 3+ intercalation journal January 2019
Designing a hybrid electrode toward high energy density with a staged Li + and PF 6 deintercalation/intercalation mechanism journal January 2020
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A Dual Plating Battery with the Iodine/[ZnI x (OH 2 ) 4− x ] 2− x Cathode journal September 2019
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