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Title: Stabilizing electrode–electrolyte interfaces to realize high-voltage Li||LiCoO2 batteries by a sulfonamide-based electrolyte

Journal Article · · Energy & Environmental Science
DOI:https://doi.org/10.1039/d1ee01265g· OSTI ID:1830205
ORCiD logo [1];  [1];  [1];  [2];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [1];  [1]; ORCiD logo [4];  [5];  [5];  [2];  [2];  [6]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Shanghai Jiao Tong Univ. (China)
  4. Tongji Univ., Shanghai (China)
  5. Honda Research Institute, USA, Inc., San Jose, CA (United States)
  6. Honda Research Institute, USA, Inc., San Jose, California 95134, USA
+ Show Author Affiliations

High-voltage lithium-metal batteries (LMBs) with LiCoO2 (LCO) as the cathode have high volumetric and gravimetric energy densities. However, it remains a challenge for stable cycling of LCO >4.5 VLi. Here we demonstrate that a rationally designed sulfonamide-based electrolyte can greatly improve the cycling stability at high voltages up to 4.7 VLi by stabilizing the electrode–electrolyte interfaces (EEIs) on both the Li-metal anode (LMA) and high-voltage LCO cathode. With the sulfonamide-based electrolyte, commercial LCO cathodes retain 89% and 85% of their capacities after 200 and 100 cycles under high charging voltages of 4.55 VLi and 4.6 VLi, respectively, significantly outperforming traditional carbonate-based electrolytes. The surface degradation, impedance growth, and detrimental side reactions in terms of gas evolution and Co dissolution are well suppressed. Our work demonstrates a promising strategy for designing new electrolytes to realize high-energy Li||LCO batteries.

Research Organization:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Honda Research Institute
Grant/Contract Number:
SC0012704; CBET-2034902; DMR-1419807
OSTI ID:
1830205
Report Number(s):
BNL-222383-2021-JAAM
Journal Information:
Energy & Environmental Science, Vol. 14, Issue 11; ISSN 1754-5692
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (59)

Gradient-morph LiCoO 2 single crystals with stabilized energy density above 3400 W h L −1 journal January 2020
LiCoO 2 Degradation Behavior in the High-Voltage Phase Transition Region and Improved Reversibility with Surface Coating journal November 2016
Generalized Gradient Approximation Made Simple journal October 1996
Performance and cost of materials for lithium-based rechargeable automotive batteries journal April 2018
Surface Engineering Strategies of Layered LiCoO 2 Cathode Material to Realize High-Energy and High-Voltage Li-Ion Cells journal October 2016
Pathways for practical high-energy long-cycling lithium metal batteries journal February 2019
Oxidation of Ethylene Carbonate on Li Metal Oxide Surfaces journal April 2018
Projector augmented-wave method journal December 1994
Inhibiting Polysulfide Shuttle in Lithium-Sulfur Batteries through Low-Ion-Pairing Salts and a Triflamide Solvent journal May 2017
Scavenging Materials to Stabilize LiPF 6 ‐Containing Carbonate‐Based Electrolytes for Li‐Ion Batteries journal November 2018
Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights journal October 2015
Unveiling Nickel Chemistry in Stabilizing High‐Voltage Cobalt‐Rich Cathodes for Lithium‐Ion Batteries journal November 2019
Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries journal June 2020
High‐Safety and High‐Energy‐Density Lithium Metal Batteries in a Novel Ionic‐Liquid Electrolyte journal May 2020
FSI-inspired solvent and “full fluorosulfonyl” electrolyte for 4 V class lithium-metal batteries journal January 2020
Long cycle life and dendrite-free lithium morphology in anode-free lithium pouch cells enabled by a dual-salt liquid electrolyte journal July 2019
Designing Advanced In Situ Electrode/Electrolyte Interphases for Wide Temperature Operation of 4.5 V Li||LiCoO 2 Batteries journal November 2020
Improving the Capacity Retention of LiCoO[sub 2] Cycled to 4.5 V by Heat-Treatment journal January 2004
Ligand-Dependent Energetics for Dehydrogenation: Implications in Li-Ion Battery Electrolyte Stability and Selective Oxidation Catalysis of Hydrogen-Containing Molecules journal July 2019
Recent advances and historical developments of high voltage lithium cobalt oxide materials for rechargeable Li-ion batteries journal June 2020
Enabling Stable High‐Voltage LiCoO 2 Operation by Using Synergetic Interfacial Modification Strategy journal September 2020
Reviving lithium cobalt oxide-based lithium secondary batteries-toward a higher energy density journal January 2018
Reliable liquid electrolytes for lithium metal batteries journal September 2020
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
A Surface Se‐Substituted LiCo[O 2− δ Se δ ] Cathode with Ultrastable High‐Voltage Cycling in Pouch Full‐Cells journal November 2020
Molecular Design of Stable Sulfamide- and Sulfonamide-Based Electrolytes for Aprotic Li-O2 Batteries journal October 2019
Realizing long-term cycling stability and superior rate performance of 4.5 V–LiCoO2 by aluminum doped zinc oxide coating achieved by a simple wet-mixing method journal September 2020
Monolithic solid–electrolyte interphases formed in fluorinated orthoformate-based electrolytes minimize Li depletion and pulverization journal September 2019
Polymer Electrolyte Enlightens Wide-Temperature 4.45 V-Class LiCoO 2 /Li Metal Battery journal January 2019
An In Situ Formed Surface Coating Layer Enabling LiCoO 2 with Stable 4.6 V High‐Voltage Cycle Performances journal June 2020
High-Voltage “Single-Crystal” Cathode Materials for Lithium-Ion Batteries journal January 2021
Multi-scale stabilization of high-voltage LiCoO2 enabled by nanoscale solid electrolyte coating journal August 2020
Realizing High Voltage Lithium Cobalt Oxide in Lithium-Ion Batteries journal May 2019
Chemical Reactivity Descriptor for the Oxide-Electrolyte Interface in Li-Ion Batteries journal August 2017
Gravimetric and volumetric energy densities of lithium-sulfur batteries journal December 2017
Electrochemical surface passivation of LiCoO2 particles at ultrahigh voltage and its applications in lithium-based batteries journal November 2018
Special points for Brillouin-zone integrations journal June 1976
Gradient Li-rich oxide cathode particles immunized against oxygen release by a molten salt treatment journal December 2019
Fluorinated Solid-Electrolyte Interphase in High-Voltage Lithium Metal Batteries journal November 2019
Revealing electrolyte oxidation via carbonate dehydrogenation on Ni-based oxides in Li-ion batteries by in situ Fourier transform infrared spectroscopy journal January 2020
A multifunctional polymer electrolyte enables ultra-long cycle-life in a high-voltage lithium metal battery journal January 2018
Three-Component Functional Additive in a LiPF 6 -Based Carbonate Electrolyte for a High-Voltage LiCoO 2 /Graphite Battery System journal July 2017
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Polycrystalline and Single Crystalline NCM Cathode Materials—Quantifying Particle Cracking, Active Surface Area, and Lithium Diffusion journal March 2021
Diphenyl disulfide as a new bifunctional film-forming additive for high-voltage LiCoO2/graphite battery charged to 4.4 V journal August 2016
Functional Electrolyte of Fluorinated Ether and Ester for Stabilizing Both 4.5 V LiCoO 2 Cathode and Lithium Metal Anode journal January 2020
Non-flammable electrolyte enables Li-metal batteries with aggressive cathode chemistries journal July 2018
Surface regulation enables high stability of single-crystal lithium-ion cathodes at high voltage journal June 2020
Enabling High-Voltage Lithium-Metal Batteries under Practical Conditions journal July 2019
Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries journal October 2017
Coupled LiPF 6 Decomposition and Carbonate Dehydrogenation Enhanced by Highly Covalent Metal Oxides in High-Energy Li-Ion Batteries journal October 2018
Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte journal March 2021
Trace doping of multiple elements enables stable battery cycling of LiCoO2 at 4.6 V journal June 2019
Approaching the capacity limit of lithium cobalt oxide in lithium ion batteries via lanthanum and aluminium doping journal June 2018
Intercalation-conversion hybrid cathodes enabling Li–S full-cell architectures with jointly superior gravimetric and volumetric energy densities journal March 2019
Mg‐Pillared LiCoO 2 : Towards Stable Cycling at 4.6 V journal January 2021
Fluorine-donating electrolytes enable highly reversible 5-V-class Li metal batteries journal January 2018
Structural origin of the high-voltage instability of lithium cobalt oxide journal February 2021
Visualization of Electrochemical Reactions in Battery Materials with X-ray Microscopy and Mapping journal April 2017

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