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Title: Metal segregation in hierarchically structured cathode materials for high-energy lithium batteries

Journal Article · · Nature Energy
 [1];  [2];  [3];  [1];  [1];  [4];  [3];  [3];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
+ Show Author Affiliations

Controlling surface and interfacial properties of battery materials is key to improving performance in rechargeable Li-ion devices. Surface reconstruction from a layered to a rock salt structure in metal oxide cathode materials is commonly observed and results in poor high-voltage cycling performance, impeding attempts to improve energy density. Hierarchically structured LiNi0.4Mn0.4Co0.2O2 (NMC-442) spherical powders, made by spray pyrolysis, exhibit local elemental distribution gradients that deviate from the global NMC-442 composition; specifically, they are Ni-rich and Mn-poor at particle surfaces. These materials demonstrate improved Coulombic efficiencies, discharge capacities, and high-voltage capacity retention in lithium half-cell configurations. The subject powders show superior resistance against surface reconstruction due to the tailored surface chemistry, compared to conventional NMC-442 materials. This paves the way towards the development of a new generation of robust and stable high-energy NMC cathodes for Li-ion batteries.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC00112704
OSTI ID:
1224767
Report Number(s):
BNL-108492-2015-JA; KC0403020
Journal Information:
Nature Energy, Vol. 1, Issue 1; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 202 works
Citation information provided by
Web of Science

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Cited By (40)

Multifunctional NiTiO 3 nanocoating fabrication based on the dual-Kirkendall effect enabling a stable cathode/electrolyte interface for nickel-rich layered oxides journal January 2018
Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities journal January 2018
Structural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides. text January 2019
In Situ Carbon-Coated NCM622 through CF x for Lithium-Ion Batteries with High Cycling Stability journal January 2019
Trace doping of multiple elements enables stable battery cycling of LiCoO2 at 4.6 V journal June 2019
Charge distribution guided by grain crystallographic orientations in polycrystalline battery materials journal January 2020
Structural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides journal November 2019
A highly stabilized nickel-rich cathode material by nanoscale epitaxy control for high-energy lithium-ion batteries journal January 2018
Synthesis and Electrochemical Property of LiMn2O4 Porous Hollow Nanofiber as Cathode for Lithium-Ion Batteries journal February 2017
Selective TiO 2 Nanolayer Coating by Polydopamine Modification for Highly Stable Ni‐Rich Layered Oxides journal October 2019
Reviving lithium cobalt oxide-based lithium secondary batteries-toward a higher energy density journal January 2018
Anomalous metal segregation in lithium-rich material provides design rules for stable cathode in lithium-ion battery journal April 2019
Thermally driven mesoscale chemomechanical interplay in Li 0.5 Ni 0.6 Mn 0.2 Co 0.2 O 2 cathode materials journal January 2018
In Situ Probing and Synthetic Control of Cationic Ordering in Ni-Rich Layered Oxide Cathodes journal October 2016
Structural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides text January 2019
Atomic-Scale Observation of LiFePO 4 and LiCoO 2 Dissolution Behavior in Aqueous Solutions journal September 2018
Elucidating the Mechanism Involved in the Performance Improvement of Lithium‐Ion Transition Metal Oxide Battery by Conducting Polymer journal February 2019
Intragranular cracking as a critical barrier for high-voltage usage of layer-structured cathode for lithium-ion batteries journal January 2017
Depth-Dependent Redox Behavior of LiNi 0.6 Mn 0.2 Co 0.2 O 2 journal January 2018
Degradation and Aging Routes of Ni-Rich Cathode Based Li-Ion Batteries text January 2020
Radially Oriented Single‐Crystal Primary Nanosheets Enable Ultrahigh Rate and Cycling Properties of LiNi 0.8 Co 0.1 Mn 0.1 O 2 Cathode Material for Lithium‐Ion Batteries journal February 2019
Lithium-Graphite Paste: An Interface Compatible Anode for Solid-State Batteries journal January 2019
High capacity vanadium oxide electrodes: effective recycling through thermal treatment journal January 2019
Synchrotron-Based X-ray Absorption Fine Structures, X-ray Diffraction, and X-ray Microscopy Techniques Applied in the Study of Lithium Secondary Batteries journal April 2018
Unsupervised Data Mining in nanoscale X-ray Spectro-Microscopic Study of NdFeB Magnet journal September 2016
High-Capacity Cathode Material with High Voltage for Li-Ion Batteries journal January 2018
Degradation and Aging Routes of Ni-Rich Cathode Based Li-Ion Batteries journal January 2020
Revisiting the charge compensation mechanisms in LiNi 0.8 Co 0.2−y Al y O 2 systems journal January 2019
High-voltage positive electrode materials for lithium-ion batteries journal January 2017
Surface Chemistry Dependence on Aluminum Doping in Ni-rich LiNi0.8Co0.2-yAlyO2 Cathodes. journalarticle January 2019
A review of Ni-based layered oxides for rechargeable Li-ion batteries journal January 2017
Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies journal December 2019
Degradation Mechanisms and Mitigation Strategies of Nickel-Rich NMC-Based Lithium-Ion Batteries journal October 2019
Revealing the chemistry of an anode-passivating electrolyte salt for high rate and stable sodium metal batteries journal January 2018
Pb-Doped Lithium-Rich Cathode Material for High Energy Density Lithium-Ion Full Batteries journal January 2019
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High‐Voltage Performance of Ni‐Rich NCA Cathodes: Linking Operating Voltage with Cathode Degradation journal August 2019
Structural insights into the formation and voltage degradation of lithium- and manganese-rich layered oxides text January 2019

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