Large-scale virtual high-throughput screening for the identification of new battery electrolyte solvents: computing infrastructure and collective properties.

A volunteer computing approach is presented for the purpose of screening a large number of molecular structures with respect to their suitability as new battery electrolyte solvents. Collective properties like melting, boiling and flash points are evaluated using COSMOtherm and quantitative structure-property relationship (QSPR) based methods, while electronic structure theory methods are used for the computation of electrochemical stability window estimators. Two application examples are presented: first, the results of a previous large-scale screening test (PCCP, 2014, 16, 7919) are re-evaluated with respect to the mentioned collective properties. As a second application example, all reasonable nitrile solvents up to 12 heavy atoms are generated and used to illustrate a suitable filter protocol for picking Pareto-optimal candidates.

[1]  J. Perdew,et al.  Density-functional approximation for the correlation energy of the inhomogeneous electron gas. , 1986, Physical review. B, Condensed matter.

[2]  A. Becke,et al.  Density-functional exchange-energy approximation with correct asymptotic behavior. , 1988, Physical review. A, General physics.

[3]  Hans W. Horn,et al.  ELECTRONIC STRUCTURE CALCULATIONS ON WORKSTATION COMPUTERS: THE PROGRAM SYSTEM TURBOMOLE , 1989 .

[4]  A. Schäfer,et al.  Fully optimized contracted Gaussian basis sets of triple zeta valence quality for atoms Li to Kr , 1994 .

[5]  Marco Häser,et al.  Auxiliary basis sets to approximate Coulomb potentials (Chem. Phys. Letters 240 (1995) 283-290) , 1995 .

[6]  Florian Weigend,et al.  Auxiliary basis sets for main row atoms and transition metals and their use to approximate Coulomb potentials , 1997 .

[7]  P. Balbuena,et al.  Lithium-ion batteries : solid-electrolyte interphase , 2004 .

[8]  Kang Xu,et al.  Nonaqueous liquid electrolytes for lithium-based rechargeable batteries. , 2004, Chemical reviews.

[9]  M. Winter,et al.  What are batteries, fuel cells, and supercapacitors? , 2004, Chemical reviews.

[10]  Stefan Grimme,et al.  Semiempirical GGA‐type density functional constructed with a long‐range dispersion correction , 2006, J. Comput. Chem..

[11]  Stefan Grimme,et al.  Toward the exact solution of the electronic Schrödinger equation for noncovalent molecular interactions: worldwide distributed quantum monte carlo calculations. , 2008, The journal of physical chemistry. A.

[12]  Y. Abu-Lebdeh,et al.  High-Voltage Electrolytes Based on Adiponitrile for Li-Ion Batteries , 2009 .

[13]  Y. Abu-Lebdeh,et al.  New electrolytes based on glutaronitrile for high energy/power Li-ion batteries , 2009 .

[14]  Frank Neese,et al.  Accurate theoretical chemistry with coupled pair models. , 2009, Accounts of chemical research.

[15]  J-M Tarascon,et al.  Key challenges in future Li-battery research , 2010, Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences.

[16]  J. Goodenough.  Challenges for Rechargeable Li Batteries , 2010 .

[17]  K. Xu.  Electrolytes and Interphasial Chemistry in Li Ion Devices , 2010 .

[18]  Martin Korth,et al.  Third-Generation Hydrogen-Bonding Corrections for Semiempirical QM Methods and Force Fields , 2010 .

[19]  P. Novák,et al.  A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries , 2010 .

[20]  B. Scrosati,et al.  Lithium batteries: Status, prospects and future , 2010 .

[21]  Svetoslav H. Slavov,et al.  Quantitative correlation of physical and chemical properties with chemical structure: utility for prediction. , 2010, Chemical reviews.

[22]  Pavel Hobza,et al.  A Transferable H-Bonding Correction for Semiempirical Quantum-Chemical Methods. , 2010, Journal of chemical theory and computation.

[23]  Mark F. Mathias,et al.  Electrochemistry and the Future of the Automobile , 2010 .

[24]  Yang‐Kook Sun,et al.  Lithium-ion batteries. A look into the future , 2011 .

[25]  M. Winter,et al.  High flash point electrolyte for use in lithium-ion batteries , 2011 .

[26]  Alán Aspuru-Guzik,et al.  The Harvard Clean Energy Project: Large-Scale Computational Screening and Design of Organic Photovoltaics on the World Community Grid , 2011 .

[27]  A. Klamt.  The COSMO and COSMO‐RS solvation models , 2011 .

[28]  Chris Morley,et al.  Open Babel: An open chemical toolbox , 2011, J. Cheminformatics.

[29]  Anubhav Jain,et al.  Phosphates as Lithium-Ion Battery Cathodes: An Evaluation Based on High-Throughput ab Initio Calculations , 2011 .

[30]  Martin Korth,et al.  Empirical hydrogen-bond potential functions--an old hat reconditioned. , 2011, Chemphyschem : a European journal of chemical physics and physical chemistry.

[31]  D. Aurbach,et al.  A review of advanced and practical lithium battery materials , 2011 .

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

[33]  S. Grimme,et al.  The lithium-thiophene riddle revisited. , 2011, The journal of physical chemistry. A.

[34]  G Marcou,et al.  In silico design of new ionic liquids based on quantitative structure-property relationship models of ionic liquid viscosity. , 2011, The journal of physical chemistry. B.

[35]  Anubhav Jain,et al.  Novel mixed polyanions lithium-ion battery cathode materials predicted by high-throughput ab initio computations , 2011 .

[36]  Kang Xu,et al.  Interfacing electrolytes with electrodes in Li ion batteries , 2011 .

[37]  Andrea Balducci,et al.  Adiponitrile-based electrochemical double layer capacitor , 2012 .

[38]  Kang Xu,et al.  Li^+-solvation/desolvation dictates interphasial processes on graphitic anode in Li ion cells , 2012 .

[39]  Lars Ruddigkeit,et al.  The enumeration of chemical space , 2012 .

[40]  K. Leung.  Electronic Structure Modeling of Electrochemical Reactions at Electrode/Electrolyte Interfaces in Lithium Ion Batteries , 2012, 1304.5976.

[41]  Frank Neese,et al.  The ORCA program system , 2012 .

[42]  L. Curtiss,et al.  Atomic-level modeling of organic electrolytes in lithium-ion batteries , 2013 .

[43]  K. Leung.  Two-electron reduction of ethylene carbonate: A quantum chemistry re-examination of mechanisms , 2013, 1307.3165.

[44]  John B Goodenough,et al.  The Li-ion rechargeable battery: a perspective. , 2013, Journal of the American Chemical Society.

[45]  John B Goodenough,et al.  Evolution of strategies for modern rechargeable batteries. , 2013, Accounts of chemical research.

[46]  Jens Leker,et al.  Current research trends and prospects among the various materials and designs used in lithium-based batteries , 2013, Journal of Applied Electrochemistry.

[47]  J. Dearden,et al.  QSPR prediction of physico-chemical properties for REACH , 2013, SAR and QSAR in environmental research.

[48]  Martin Korth,et al.  Large-scale virtual high-throughput screening for the identification of new battery electrolyte solvents: evaluation of electronic structure theory methods. , 2014, Physical chemistry chemical physics : PCCP.

[49]  John B. Goodenough,et al.  Electrochemical energy storage in a sustainable modern society , 2014 .

[50]  Martin Korth.  Computational studies of solid electrolyte interphase formation , 2014 .