skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: The surface triple-coupling on single crystalline cathode for lithium ion batteries

Journal Article · · Nano Energy
 [1];  [2]; ORCiD logo [3];  [4];  [5]; ORCiD logo [3];  [1];  [6];  [1]; ORCiD logo [7]
  1. Tianjin Univ. of Technology, Tianjin (China)
  2. Tianjin Univ. of Technology, Tianjin (China); Univ. of Tennessee, Knoxville, TN (United States); Tianjin Institute of Power Sources, Tianjin (China)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Univ. of Pittsburgh, PA (United States)
  5. Guizhou Zhenhua New Material Co., Ltd, Guiyang (China)
  6. Tianjin Institute of Power Sources, Tianjin (China). National Key Laboratory of Science and Technology on Power Sources
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Single crystalline (SC) cathode materials, which are less susceptible to micro/nano-cracks formation and offer better structure stability compared to the polycrystalline counterpart, have attained great attention. However, the parasitic side reactions at the cathode-electrolyte interface induces the loss of active species, which consequently leads to continual degradation of the electrochemical performances. Herein, a triple coupling of concentration-gradient Na+, F- co-doping and surface NaF coating are exploited for the first time on SC LiNi0.5Co0.2Mn0.3O2 cathode by the hydrolysis of NaPF6. This process regulates the external structure of materials by constructing a “sandwich” configuration from surface to bulk: rock salt - mixing zone - layered phase. The detailed interface transformation mechanism is revealed by Neutron powder diffraction (NPD), spherical aberration corrected high-resolution scanning transmission electron microscopy (HR-STEM), electron energy loss spectroscopy (EELS), and Ar+ sputtering assisted X-ray photoelectron spectroscopy (XPS). The synergistic effects endow the SC cathode with outstanding capacity retentions: 91.3% at 25 °C and 85% at 45 °C, after 500 cycles at 5 C between 3.0 and 4.5 V. In addition, a high full-cell reversible capacity of 168.9 mAh g-1 with a capacity retention of 92.4% is achieved after 300 cycles at 1 C. Multiple characterizations further indicate that these superior results are mainly ascribed to the overall structure integrity of SC material, the thin cathode electrolyte interface, high content of lithium fluoride, and the low solubility of transition metal ions. This work opens a new avenue to construct a benign interface towards high-performance lithium ion batteries.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1808177
Alternate ID(s):
OSTI ID: 1817265
Journal Information:
Nano Energy, Vol. 86, Issue 1; ISSN 2211-2855
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (67)

Single-crystal based studies for correlating the properties and high-voltage performance of Li[Ni x Mn y Co 1−x−y ]O 2 cathodes journal January 2019
Safety-Reinforced Succinonitrile-Based Electrolyte with Interfacial Stability for High-Performance Lithium Batteries journal August 2017
Modified High‐Nickel Cathodes with Stable Surface Chemistry Against Ambient Air for Lithium‐Ion Batteries journal April 2018
X-ray/Neutron Diffraction and Electrochemical Studies of Lithium De/Re-Intercalation in Li 1 - x Co 1/ 3 Ni 1/3 Mn 1/3 O 2 ( x = 0 → 1) journal April 2006
Controlling the Growth and Luminescence Properties of Well-Faceted ZnO Nanorods journal June 2007
A novel synthesis strategy to improve cycle stability of LiNi0.8Mn0.1Co0.1O2 at high cut-off voltages through core-shell structuring journal August 2019
Improving cycling performance and rate capability of Ni-rich LiNi0.8Co0.1Mn0.1O2 cathode materials by Li4Ti5O12 coating journal April 2018
Lithium-ion (de)intercalation mechanism in core-shell layered Li(Ni,Co,Mn)O2 cathode materials journal December 2020
Structural and Electrochemical Aspects of LiNi 0.8 Co 0.1 Mn 0.1 O 2 Cathode Materials Doped by Various Cations journal January 2019
The effects of Na doping on performance of layered Li1.1−xNax[Ni0.2Co0.3Mn0.4]O2 materials for lithium secondary batteries journal February 2006
An effective etching-induced coating strategy to shield LiNi0.8Co0.1Mn0.1O2 electrode materials by LiAlO2 journal February 2019
Unravelling the influence of quasi single-crystalline architecture on high-voltage and thermal stability of LiNi0.5Co0.2Mn0.3O2 cathode for lithium-ion batteries journal August 2020
Syntheses and electrochemical properties of layered Li 0.95 Na 0.05 Ni 1/3 Co 1/3 Mn 1/3 O 2 and LiNi 1/3 Co 1/3 Mn 1/3 O 2 journal February 2014
Resolving the Compositional and Structural Defects of Degraded LiNi x Co y Mn z O 2 Particles to Directly Regenerate High-Performance Lithium-Ion Battery Cathodes journal June 2018
The effect of gradient boracic polyanion-doping on structure, morphology, and cycling performance of Ni-rich LiNi 0.8 Co 0.15 Al 0.05 O 2 cathode material journal January 2018
New sulfone electrolytes for rechargeable lithium batteries.: Part I. Oligoether-containing sulfones journal March 2005
Unlocking the passivation nature of the cathode–air interfacial reactions in lithium ion batteries journal June 2020
A disordered rock salt anode for fast-charging lithium-ion batteries journal September 2020
Towards improved structural stability and electrochemical properties of a Li-rich material by a strategy of double gradient surface modification journal July 2019
Stabilizing the Structure of Nickel‐Rich Lithiated Oxides via Cr Doping as Cathode with Boosted High‐Voltage/Temperature Cycling Performance for Li‐Ion Battery journal September 2019
Crack-free single-crystalline Ni-rich layered NCM cathode enable superior cycling performance of lithium-ion batteries journal April 2020
A Wide Range of Testing Results on an Excellent Lithium-Ion Cell Chemistry to be used as Benchmarks for New Battery Technologies journal January 2019
On electrochemical impedance measurements of LixCo0.2Ni0.8O2 and LixNiO2 intercalation electrodes journal February 2000
Synthesis of Single Crystal LiNi 0.6 Mn 0.2 Co 0.2 O 2 with Enhanced Electrochemical Performance for Lithium Ion Batteries journal January 2018
Understanding interfacial chemistry and stability for performance improvement and fade of high-energy Li-ion battery of LiNi0.5Co0.2Mn0.3O2//silicon-graphite journal January 2016
Phase Control on Surface for the Stabilization of High Energy Cathode Materials of Lithium Ion Batteries journal March 2019
Extending the Service Life of High-Ni Layered Oxides by Tuning the Electrode-Electrolyte Interphase journal September 2018
The Role of Sodium in LiNi 0.8 Co 0.15 Al 0.05 O 2 Cathode Material and Its Electrochemical Behaviors journal February 2016
Investigation on the effect of Na doping on structure and Li-ion kinetics of layered LiNi0.6Co0.2Mn0.2O2 cathode material journal February 2016
Single-crystal nickel-rich layered-oxide battery cathode materials: synthesis, electrochemistry, and intra-granular fracture journal May 2020
Enhancing the high voltage interface compatibility of LiNi0.5Co0.2Mn0.3O2 in the succinonitrile-based electrolyte journal March 2019
X-ray photoelectron spectroscopy and auger electron spectroscopy studies of Al-doped ZnO films journal May 2000
A cation/anion co-doped Li1.12Na0.08Ni0.2Mn0.6O1.95F0.05 cathode for lithium ion batteries journal April 2019
A low temperature fluorine substitution on the electrochemical performance of layered LiNi0.8Co0.1Mn0.1O2−zFz cathode materials journal March 2013
Long-Life, Ultrahigh-Nickel Cathodes with Excellent Air Storage Stability for High-Energy Density Lithium-Based Batteries journal August 2020
Improvement of Electrochemical Performances of Li[Ni[sub 0.8]Co[sub 0.1]Mn[sub 0.1]]O[sub 2] Cathode Materials by Fluorine Substitution journal January 2007
Aromatic Polyimide/Graphene Composite Organic Cathodes for Fast and Sustainable Lithium-Ion Batteries journal January 2018
A General One‐Pot Synthesis Strategy of 3D Porous Hierarchical Networks Crosslinked by Monolayered Nanoparticles Interconnected Nanoplates for Lithium Ion Batteries journal June 2019
Enhanced rate performance and high potential as well as decreased strain of LiNi0.6Co0.2Mn0.2O2 by facile fluorine modification journal January 2018
Gradient Li-rich oxide cathode particles immunized against oxygen release by a molten salt treatment journal December 2019
Harnessing the surface structure to enable high-performance cathode materials for lithium-ion batteries journal January 2020
Dead lithium: mass transport effects on voltage, capacity, and failure of lithium metal anodes journal January 2017
Investigation of capacity fade for 18650-type lithium-ion batteries cycled in different state of charge (SoC) ranges journal March 2021
Surface regulation enables high stability of single-crystal lithium-ion cathodes at high voltage journal June 2020
Enhanced Electrochemical Performance of Ni‐Rich Layered Cathode Materials by using LiPF 6 as a Cathode Additive journal January 2019
Reversible planar gliding and microcracking in a single-crystalline Ni-rich cathode journal December 2020
Study of oxygen vacancies′ influence on the lattice parameter in ZnO thin film journal October 2012
Fluorine and Lithium: Ideal Partners for High‐Performance Rechargeable Battery Electrolytes journal November 2019
A New Type of Protective Surface Layer for High-Capacity Ni-Based Cathode Materials: Nanoscaled Surface Pillaring Layer journal February 2013
On the behavior of the LixNiO2 system: an electrochemical and structural overview journal September 1997
Characterization of high-power lithium-ion batteries by electrochemical impedance spectroscopy. I. Experimental investigation journal June 2011
Use of Ce to Reinforce the Interface of Ni-Rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 Cathode Materials for Lithium-Ion Batteries under High Operating Voltage journal January 2019
Lithium malonatoborate additives enabled stable cycling of 5 V lithium metal and lithium ion batteries journal October 2017
Oxygen Vacancy Diffusion and Condensation in Lithium‐Ion Battery Cathode Materials journal June 2019
Li‐Rich Li 2 [Ni 0.8 Co 0.1 Mn 0.1 ]O 2 for Anode‐Free Lithium Metal Batteries journal March 2021
Facile Fabrication of Ethoxy-Functional Polysiloxane Wrapped LiNi 0.6 Co 0.2 Mn 0.2 O 2 Cathode with Improved Cycling Performance for Rechargeable Li-Ion Battery journal July 2016
Improvement of the optical properties of ZnO nanorods by Fe doping journal November 2007
Molybdate flux growth of idiomorphic Li(Ni 1/3 Co 1/3 Mn 1/3 )O 2 single crystals and characterization of their capabilities as cathode materials for lithium-ion batteries journal January 2016
The effect of excimer laser annealing on ZnO nanowires and their field effect transistors journal February 2009
Phase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy journal February 2017
A High‐Performance Li–Mn–O Li‐rich Cathode Material with Rhombohedral Symmetry via Intralayer Li/Mn Disordering journal March 2020
A highly stabilized nickel-rich cathode material by nanoscale epitaxy control for high-energy lithium-ion batteries journal January 2018
Electrochemical Evaluation and Structural Characterization of Commercial LiCoO[sub 2] Surfaces Modified with MgO for Lithium-Ion Batteries journal January 2002
Synergistic Effect of F Doping and LiF Coating on Improving the High-Voltage Cycling Stability and Rate Capacity of LiNi 0.5 Co 0.2 Mn 0.3 O 2 Cathode Materials for Lithium-Ion Batteries journal September 2018
Dynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries journal April 2017
Effect of fluorine on the electrochemical performance of spherical LiNi0.8Co0.1Mn0.1O2 cathode materials via a low temperature method journal March 2013
Renovating the electrode-electrolyte interphase for layered lithium- & manganese-rich oxides journal June 2020