Accelerated discovery of cathode materials with prolonged cycle life for lithium-ion battery

Large-scale battery systems are essential for efficiently utilizing renewable energy power sources from solar and wind, which can generate electricity only intermittently. The use of lithium-ion batteries to store the generated energy is one solution. A long cycle life is critical for lithium-ion battery when used in these applications; this is different from portable devices which require 1,000 cycles at most. Here we demonstrate a novel co-substituted lithium iron phosphate cathode with estimated 70%-capacity retention of 25,000 cycles. This is found by exploring a wide chemical compositional space using density functional theory calculations. Relative volume change of a compound between fully lithiated and delithiated conditions is used as the descriptor for the cycle life. On the basis of the results of the screening, synthesis of selected materials is targeted. Single-phase samples with the required chemical composition are successfully made by an epoxide-mediated sol-gel method. The optimized materials show excellent cycle-life performance as lithium-ion battery cathodes.

[1]  N. Okazaki,et al.  Preparation of SiO2-Al2O3 Gels from Tetraethoxysilane and Aluminum Chloride , 1993 .

[2]  K. Fujimura,et al.  Accelerated Materials Design of Lithium Superionic Conductors Based on First‐Principles Calculations and Machine Learning Algorithms , 2013 .

[3]  J. Satcher,et al.  Aerogel Synthesis of Yttria-Stabilized Zirconia by a Non-Alkoxide Sol−Gel Route , 2005 .

[4]  K. S. Nanjundaswamy,et al.  Phospho‐olivines as Positive‐Electrode Materials for Rechargeable Lithium Batteries , 1997 .

[5]  C. Delmas,et al.  Lithium deintercalation in LiFePO4 nanoparticles via a domino-cascade model. , 2008, Nature materials.

[6]  Gerbrand Ceder,et al.  Opportunities and challenges for first-principles materials design and applications to Li battery materials , 2010 .

[7]  Marco Buongiorno Nardelli,et al.  The high-throughput highway to computational materials design. , 2013, Nature materials.

[8]  F. Izumi,et al.  Three-Dimensional Visualization in Powder Diffraction , 2007 .

[9]  Kresse,et al.  Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. , 1996, Physical review. B, Condensed matter.

[10]  Sai-Cheong Chung,et al.  Optimized LiFePO4 for Lithium Battery Cathodes , 2001 .

[11]  Yet-Ming Chiang,et al.  Electronically conductive phospho-olivines as lithium storage electrodes , 2002, Nature materials.

[12]  Yasuaki Tokudome,et al.  Sol-gel Synthesis of Macroporous YAG from Ionic Precursors via Phase Separation Route , 2007 .

[13]  Krishna Rajan,et al.  Identifying the ‘inorganic gene’ for high-temperature piezoelectric perovskites through statistical learning , 2011, Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences.

[14]  C. Humphreys,et al.  Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study , 1998 .

[15]  Yuki Yamada,et al.  Facile Preparation of Monolithic LiFePO4/Carbon Composites with Well-Defined Macropores for a Lithium-Ion Battery , 2011 .

[16]  R. Service.  Computational science. Materials scientists look to a data-intensive future. , 2012, Science.

[17]  Stefano Curtarolo,et al.  Finding Unprecedentedly Low-Thermal-Conductivity Half-Heusler Semiconductors via High-Throughput Materials Modeling , 2014, 1401.2439.

[18]  Kristin A. Persson,et al.  Commentary: The Materials Project: A materials genome approach to accelerating materials innovation , 2013 .

[19]  Yet-Ming Chiang,et al.  Aliovalent Substitutions in Olivine Lithium Iron Phosphate and Impact on Structure and Properties , 2009 .

[20]  Yasuaki Tokudome,et al.  Synthesis of hierarchical macro/mesoporous dicalcium phosphate monolith via epoxide-mediated sol–gel reaction from ionic precursors , 2011 .

[21]  Burke,et al.  Generalized Gradient Approximation Made Simple. , 1996, Physical review letters.

[22]  Xiaodong Wu,et al.  Cracking causing cyclic instability of LiFePO4 cathode material , 2005 .

[23]  R. Simpson,et al.  Use of Epoxides in the Sol−Gel Synthesis of Porous Iron(III) Oxide Monoliths from Fe(III) Salts , 2001 .