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protective films through vapor and liquid-phase chemical modification of lithium prior to introduction to the cell have demonstrated improvement in cell performance82,83 and lithium anode stability with cycling.84-86 However, further gains could be made with flexible, mechanically adaptable interfaces. Preformed Li+ cation transmissive membranes87,88 as well as membranes formed in situ by jamming of nanoparticle salts89 and their integration with Li anodes have been proposed, where select examples have demonstrated dimensional control of the anode with electrodeposition and dissolution. These and related approaches designed to overcome the underlying electroconvective instabilities, which are known to be the source of unstable, dendritic deposition, must also solve the underlying anode reactivity/coulombic efficiency problem before ultimate success can be achieved. Management of the local volume change within a cell that employs a metal anode must also be addressed. Discharge of the anode produces local volume loss and threatens gaining the ability to maintain a coherent, low impedance interface with the artificial SEI membranes and films integrated with the anode. One solution to this problem is to design for volume change through an appropriately sized host scaffold, where the scaffold material mass and volume are minimal relative to the metal. It may be that heterostructuring of the reconfigurable interphases with the anode is the key to success to amplify threshold behavior around phase transitions so that the system evolves toward optimal ion-transporting properties even when operating conditions fluctuate, such as inhomogeneities in mechanical stress, ion current, or electric field. The interplay between electrons, ions, phonons, and chemical bonds in interphases could be used to create ion transduction behaviors that can be controllably damped, focused, and distributed, or made to be oscillatory as needed. Surface structure, reaction products, potential profiles, and interfacial chemistry all contribute to the nature of the interface. Deliberate design of mechanistic aspects could enable active (rather than passive) control of chemical structure and composition at interfaces, which may facilitate new electrode development and the establishment of more resilient interfaces. Harnessing the powerful tools of synthetic chemistry to create designer interphases that offer explicit control of function will lead to significant progress in the design and synthesis of dynamic interfaces that are able to respond to electrical, chemical, or physical cues to self-repair or to trigger a change in interface structure and transport properties, resulting in increased safety and enhanced lifetime for EES systems. 2.3.3 REFERENCES 1. Nie, M.; Chalasani, D.; Abraham, D.P.; Chen, Y.; Bose, A.; Lucht, B.L., Lithium ion battery graphite solid electrolyte interphase revealed by microscopy and spectroscopy. J. Phys. Chem. C, 2013, 117, 1257-1267. 2. Aurbach, D., Review of selected electrode–solution interactions which determine the performance of Li and Li ion batteries. J. Power Sources, 2000, 89, 206. 3. Peled, E., The electrochemical behavior of alkali and alkaline earth metals in nonaqueous battery systems—The solid electrolyte interphase model. J. Electrochem. Soc., 1979, 126, 2047. 4. Verma, P.; Maire, P.; Novák, P.A., review of the features and analyses of the solid electrolyte interphase in Li-ion batteries. Electrochim. Acta, 2010, 55, 6332. 5. Suo, L.; Borodin, O.; Gao, T.; Olguin, M.; Ho, J.; Fan, X.; Luo, C.; Wang, C.; Xu, K., “Water-in-salt” electrolyte enables high-voltage aqueous lithium- ion chemistries. Science, 2015, 350, 938. 6. Yamada, Y.; Furukawa, K.; Sodeyama, K.; Kikuchi, K.; Yaegashi, M.; Tateyama, Y; Yamada, A., Unusual stability of acetonitrile-based superconcentrated electrolytes for fast-charging lithium-ion batteries. J. Amer. Chem. Soc., 2014, 136, 5039. 7. Qian, J.F.; Henderson; W.A.; Xu, W.; Bhattacharya, P.; Engelhard; M., Borodin, O.; Zhang, J.G., High rate and stable cycling of lithium metal anode. Nat. Commun. 2015, 6, 6362, DOI;10.1038/ncomms7362. 8. Xu, K.; Wang, C., Batteries: Widening voltage windows. Nature Energy, 2016, 1, 16161. 9. Wei, S.; Xu, S.; Agrawal, A.; Choudhury, S.; Lu, Y.; Tu, Z.; Ma, L.; Archer, L.A., A stable room-temperature sodium-sulfur battery. Nat. Commun., 2016, 7, 11722 (2016). 10. Choudhury, S.; Agrawal, A.; Wei, S.; Jeng, E.; Archer, L.A., Hybrid hairy nanoparticle electrolytes stabilizing lithium metal batteries. Chem. Mater., 2016, 28, 2147. 11. Ding, M.S.; von Cresce, A.; Xu, K., Conductivity, viscosity, and their correlation of a super-concentrated aqueous electrolyte. J. Phys. Chem. C 2017, 121 (4), 2149-2153. 12. Black, J.M.; Baris Okatan, M.; Feng, G.; Cummings, P.T.; Kalinin, S.V.; Balke, N., Topological defects in electric double layers of ionic liquids at carbon interfaces. Nano Energy, 2015, 15, 737. 13. Borodin, O.; Zhuang, G.V.; Ross, P.N.; Xu, K., Molecular dynamics simulations and experimental study of lithium ion transport in dilithium ethylene dicarbonate. J. Phys. Chem. C, 2013, 117, 7433. 14. Sacci, R.L.; Lehmann, Michelle L.; Diallo, Souleymane O.; Cheng, Yongqiang Q.; Daemen, Luke L.; Browning, James F.; Doucet, Mathieu; Dudney, Nancy J.; Veith, Gabriel M., Lithium transport in amorphous LixSi anode materials investigated by quasi-elastic neutron scattering. J. Phys. Chem. C, in press (2017). 15. Uysal, A.; Zhou, H.; Feng, G.; Lee, S.S.; Li, S.; Fenter, P.; Cummings, P.T.; Fulvio, P.F.; Dai, S.; McDonough, J.K., Structural origins of potential dependent hysteresis at the electrified graphene/ionic liquid interface. J. Phys. Chem. C, 2013, 118, 569. NEXT GENERATION ELECTRICAL ENERGY STORAGE PRIORITY RESEARCH DIRECTION – 3 51PDF Image | Next Generation Electrical Energy Storage
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