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Title: Transition-Metal Carbodiimides as Molecular Negative Electrode Materials for Lithium- and Sodium-Ion Batteries with Excellent Cycling Properties

Journal Article · · Angewandte Chemie (International Edition)
ORCiD logo [1]; ORCiD logo [1];  [2];  [3]; ORCiD logo [4];  [5];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Inst. Charles Gerhardt de Montpellier, Montpellier (France); Electrochemical Energy Network Storage, Amiens (France)
  2. RWTH Aachen Univ. (Germany). Inst. of Inorganic Chemistry (IPC)
  3. Forschungszentrum Julich (Germany). Peter Grunberg Institute (PGI), Julich Centre for Neutron Science (JCNS); Univ. of Liege, (Belgium). Inst. of Chemistry
  4. Forschungszentrum Julich (Germany). Peter Grunberg Institute (PGI), Julich Centre for Neutron Science (JCNS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  5. Normandie Univ., Rouvray (France)
+ Show Author Affiliations

Abstract We report evidence for the electrochemical activity of transition‐metal carbodiimides versus lithium and sodium. In particular, iron carbodiimide, FeNCN, can be efficiently used as negative electrode material for alkali‐metal‐ion batteries, similar to its oxide analogue FeO. Based on 57 Fe Mössbauer and infrared spectroscopy (IR) data, the electrochemical reaction mechanism can be explained by the reversible transformation of the Fe−NCN into Li/Na−NCN bonds during discharge and charge. These new electrode materials exhibit higher capacity compared to well‐established negative electrode references such as graphite or hard carbon. Contrary to its oxide analogue, iron carbodiimide does not require heavy treatments (such as nanoscale tailoring, sophisticated textures, or coating) to obtain long cycle life with current density as high as 9 A g −1 for hundreds of charge–discharge cycles. Similar to the iron compound, several other transition‐metal carbodiimides M x (NCN) y with M=Mn, Cr, Zn can cycle successfully versus lithium and sodium. Their electrochemical activity and performance open the way to the design of a novel family of anode materials.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1261390
Alternate ID(s):
OSTI ID: 1401420
Journal Information:
Angewandte Chemie (International Edition), Vol. 55, Issue 16; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 70 works
Citation information provided by
Web of Science

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Cited By (22)

2D Nanospace Confined Synthesis of Pseudocapacitance-Dominated MoS 2 -in-Ti 3 C 2 Superstructure for Ultrafast and Stable Li/Na-Ion Batteries journal August 2018
Na-Ion Batteries for Large Scale Applications: A Review on Anode Materials and Solid Electrolyte Interphase Formation journal July 2017
Schwefel‐basierte Elektroden mit Mehrelektronenreaktionen für Raumtemperatur‐Natriumionenspeicherung journal July 2019
Quantum‐Chemical Study of the FeNCN Conversion‐Reaction Mechanism in Lithium‐ and Sodium‐Ion Batteries journal January 2020
Sulfur-Based Electrodes that Function via Multielectron Reactions for Room-Temperature Sodium-Ion Storage journal July 2019
Quantum‐Chemical Study of the FeNCN Conversion‐Reaction Mechanism in Lithium‐ and Sodium‐Ion Batteries journal January 2020
Cobalt Carbodiimide as Negative Electrode for Li‐Ion Batteries: Electrochemical Mechanism and Performance journal August 2019
Layered Carbodiimides A 2 M(CN 2 ) 3 with Tetravalent Cations M = Sn, Zr, and Hf : Layered Carbodiimides A journal April 2018
Reversible High Capacity and Reaction Mechanism of Cr 2 (NCN) 3 Negative Electrodes for Li‐Ion Batteries journal December 2019
Understanding Fundamentals and Reaction Mechanisms of Electrode Materials for Na-Ion Batteries journal January 2018
The Ternary Post-transition Metal Carbodiimide SrZn(NCN) 2 : The Ternary Post-transition Metal Carbodiimide SrZn(NCN) journal September 2017
Ammonothermal Synthesis of Alkali-Alkaline Earth Metal and Alkali-Rare Earth Metal Carbodiimides: K 5- x M x (CN 2 ) 2 +x (HCN 2 ) 1- x ( M = Sr, Eu) and Na 4.32 Sr 0.68 (CN 2 ) 2.68 (HCN 2 ) 0.32 : Ammonothermal Synthesis of Alkali-Alkaline Earth Metal and Alkali-Rare Earth Metal Carbodiimides: K5-xMx(CN2)2+x(HCN2)1-x (M = Sr, Eu) and Na4.32Sr0.6 journal October 2017
Nonaqueous synthesis of metal cyanamide semiconductor nanocrystals for photocatalytic water oxidation journal January 2018
Self-templated synthesis of heavily nitrogen-doped hollow carbon spheres journal January 2018
Carbodiimides as energy materials: which directions for a reasonable future? journal January 2018
Dual anode materials for lithium- and sodium-ion batteries journal January 2018
A new tilt and an old twist on the nickel arsenide structure-type: synthesis and characterisation of the quaternary transition-metal cyanamides A 2 MnSn 2 (NCN) 6 (A = Li and Na) journal January 2019
Synthesis, Crystal Structure, and Chemical-Bonding Analysis of BaZn(NCN)2 journal December 2017
Quantum-Chemical Study of the FeNCN Conversion-Reaction Mechanism in Lithium- and Sodium-Ion Batteries text January 2020
Quantum‐Chemical Study of the FeNCN Conversion‐Reaction Mechanism in Lithium‐ and Sodium‐Ion Batteries text January 2020
Reversible High Capacity and Reaction Mechanism of Cr 2 (NCN) 3 Negative Electrodes for Li-Ion Batteries text January 2020
Electrochemical Evaluation of Pb, Ag, and Zn Cyanamides/Carbodiimides journal February 2019

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Related Subjects

25 ENERGY STORAGE
batteries
carbodiimide
lithium ions
sodium ions