Towards high energy density sodium ion batteries through electrolyte optimization

A comprehensive study is reported entailing optimization of sodium ion electrolyte formulation and compatibility studies with positive and negative electrode materials. EC:PC:DMC and EC:PC:DME were found to exhibit optimum ionic conductivities and lower viscosities. Yet, hard carbon negative electrode materials tested in such electrolytes exhibit significant differences in performance, rooted in the different resistivity of the SEI, which results in too large polarization and concomitant loss of capacity at low potentials when DME is used as a co-solvent. EC0.45:PC0.45:DMC0.1 was found to be the optimum composition resulting in good rate capability and high capacity upon sustained cycling for hard carbon electrodes. Its compatibility with positive Na3V2(PO4)2F3 (NVPF) electrodes was also confirmed, which led to the assembly of full Na-ion cells displaying an operation voltage of 3.65 V, very low polarisation and excellent capacity retention upon cycling with ca. 97 mA h g−1 of NVPF after more than 120 cycles together with satisfactory coulombic efficiency (>98.5%) and very good power performance. Such values lead to energy densities comparable to those of the current state-of-the-art lithium-ion technology.

[1]  D. Aurbach,et al.  The Correlation Between Surface Chemistry, Surface Morphology, and Cycling Efficiency of Lithium Electrodes in a Few Polar Aprotic Systems , 1989 .

[2]  M. Doeff,et al.  Thin Film Solid State Sodium Batteries for Electric Vehicles , 1995 .

[3]  P. Johansson,et al.  Mixed Solvent and Polymer Coordination in PAN and PMMA Gel Polymer Electrolytes Studied by Ab Initio Calculations and Raman Spectroscopy , 2003 .

[4]  D. C. Johnston,et al.  Phase separation and frustrated square lattice magnetism of Na1.5VOPO4F0.5 , 2011, 1104.4017.

[5]  Kazuma Gotoh,et al.  Electrochemical Na Insertion and Solid Electrolyte Interphase for Hard‐Carbon Electrodes and Application to Na‐Ion Batteries , 2011 .

[6]  M. Wohlfahrt‐Mehrens,et al.  Ageing mechanisms in lithium-ion batteries , 2005 .

[7]  Huilin Pan,et al.  Carbon coated Na3V2(PO4)3 as novel electrode material for sodium ion batteries , 2012 .

[8]  Jeff Dahn,et al.  Studies of Lithium Intercalation into Carbons Using Nonaqueous Electrochemical Cells , 1990 .

[9]  Emanuel Peled,et al.  The Electrochemical Behavior of Alkali and Alkaline Earth Metals in Nonaqueous Battery Systems—The Solid Electrolyte Interphase Model , 1979 .

[10]  Jean-Marie Tarascon,et al.  In search of an optimized electrolyte for Na-ion batteries , 2012 .

[11]  A. Hémon-Ribaud,et al.  Phase Transitions in the Na3M2(PO4)2F3 Family (M=Al3+, V3+, Cr3+, Fe3+, Ga3+): Synthesis, Thermal, Structural, and Magnetic Studies , 1999 .

[12]  D. Talaga,et al.  Lithium solvation in bis(trifluoromethanesulfonyl)imide-based ionic liquids. , 2006, Physical chemistry chemical physics : PCCP.

[13]  Sylvie Grugeon,et al.  XPS Identification of the Organic and Inorganic Components of the Electrode/Electrolyte Interface Formed on a Metallic Cathode , 2005 .

[14]  S. Okada,et al.  Cathode properties of Na3M2(PO4) 2F3 [M = Ti, Fe, V] for sodium-ion batteries , 2013 .

[15]  A. Goñi,et al.  High capacity hard carbon anodes for sodium ion batteries in additive free electrolyte , 2013 .

[16]  Jean-Marie Tarascon,et al.  Is lithium the new gold? , 2010, Nature chemistry.

[17]  Marca M. Doeff,et al.  Rechargeable Na/Na[sub x]CoO[sub 2] and Na[sub 15]Pb[sub 4]/Na[sub x]CoO[sub 2] polymer electrolyte cells , 1993 .

[18]  Doron Aurbach,et al.  Identification of Surface Films Formed on Lithium in Propylene Carbonate Solutions , 1987 .

[19]  Gerbrand Ceder,et al.  Electrode Materials for Rechargeable Sodium‐Ion Batteries: Potential Alternatives to Current Lithium‐Ion Batteries , 2012 .

[20]  Pierre Kubiak,et al.  High voltage cathode materials for Na-ion batteries of general formula Na3V2O2x(PO4)2F3−2x , 2012 .

[21]  F. Hensel,et al.  Synthetic and thermodynamic investigations in the polymerization of ethylene carbonate , 1990 .

[22]  Kristina Edström,et al.  Characterisation of the SEI formed on natural graphite in PC-based electrolytes , 2004 .

[23]  Philipp Adelhelm,et al.  Room-temperature sodium-ion batteries: Improving the rate capability of carbon anode materials by templating strategies , 2011 .

[24]  Doron Aurbach,et al.  Challenges in the development of advanced Li-ion batteries: a review , 2011 .

[25]  D. Stevens,et al.  An In Situ Small‐Angle X‐Ray Scattering Study of Sodium Insertion into a Nanoporous Carbon Anode Material within an Operating Electrochemical Cell , 2000 .

[26]  Donghan Kim,et al.  Sodium‐Ion Batteries , 2013 .

[27]  P. Johansson,et al.  Spectroscopic characterization of the conformational states of the bis(trifluoromethanesulfonyl)imide anion (TFSI , 2005 .

[28]  Teófilo Rojo,et al.  Na-ion batteries, recent advances and present challenges to become low cost energy storage systems , 2012 .

[29]  Doron Aurbach,et al.  On the correlation between surface chemistry and performance of graphite negative electrodes for Li ion batteries , 1999 .

[30]  Diana Golodnitsky,et al.  Composition, depth profiles and lateral distribution of materials in the SEI built on HOPG-TOF SIMS and XPS studies , 2001 .

[31]  D. Stevens,et al.  High Capacity Anode Materials for Rechargeable Sodium‐Ion Batteries , 2000 .

[32]  J. Tarascon,et al.  Li Metal‐Free Rechargeable LiMn2 O 4 / Carbon Cells: Their Understanding and Optimization , 1992 .

[33]  M. R. Palacín,et al.  Optimisation of performance through electrode formulation in conversion materials for lithium ion batteries: Co3O4 as a case example , 2012 .

[34]  Katsuaki Okabayashi,et al.  Raman intensity study of local structure in non-aqueous electrolyte solutions—II. Cation—solvent interaction in mixed solvent systems and selective solvation , 1989 .

[35]  Rémi Dedryvère,et al.  Surface film formation on a graphite electrode in Li‐ion batteries: AFM and XPS study , 2005 .

[36]  D. Devlin,et al.  Thermal decomposition and dehydration of sodium perchlorate monohydrate , 1987 .