Designing Artificial Solid-Electrolyte Interphases for Single-Ion and High-Efficiency Transport in Batteries

Substrates able to rectify transport of ions based on charge and/or size are ubiquitous in biological systems. Electrolytes and interphases that selectively transport electrochemically active ions are likewise of broad interest in all electrical energy storage technologies. In lithium-ion batteries, electrolytes with single- or near-single-ion conductivity reduce losses caused by ion polarization. In emergent lithium or sodium metal batteries, they maintain high conductivity at the anode and stabilize metal deposition by fundamental mechanisms. We report that 20- to 300-nm-thick, single-ion-conducting membranes deposited at the anode enable electrolytes with the highest combination of cation transference number, ionic conductivity, and electrochemical stability reported. By means of direct visualization we find that single-ion membranes also reduce dendritic deposition of Li in liquids. Galvanostatic measurements further show that the electrolytes facilitate long (3 mAh) recharge of full Li/LiNi0.8Co0.15Al0.05O2 (NCA) cells with high cathode loadings (3 mAh cm−2/19.9 mg cm−2) and at high current densities (3 mA cm−2).

Citation

Tu Z, Choudhury S, Zachman MJ, Wei S, Zhang K, et al. (2017) Designing Artificial Solid-Electrolyte Interphases for Single-Ion and High-Efficiency Transport in Batteries. Joule 1: 394–406. Available: http://dx.doi.org/10.1016/j.joule.2017.06.002.

Sponsors

This work was supported by the Department of Energy, Advanced Research Projects Agency – Energy (ARPA-E) through award #DE-AR0000750. M.J.Z. and L.F.K. acknowledge support by the NSF (DMR-1654596). The work made use of electrochemical characterization facilities in the KAUST-CU Center for Energy and Sustainability, supported by the King Abdullah University of Science and Technology (KAUST) through award #KUS-C1-018-02. Electron microscopy facilities at the Cornell Center for Materials Research (CCMR), an NSF-supported MRSEC through grant DMR-1120296, were also used for the study. Additional support for the FIB/SEM cryo-stage and transfer system was provided by the Kavli Institute at Cornell and the Energy Materials Center at Cornell, DOE EFRC BES (DE-SC0001086). Z.T. thanks Bryant Polzin for kindly providing NCA cathode materials from the Cell Analysis, Modeling, and Prototyping (CAMP) Facility at Argonne National Laboratories.