Volume 1, Issue 2, Pages (October 2017)

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Volume 1, Issue 2, Pages 344-358 (October 2017) Patternable, Solution-Processed Ionogels for Thin-Film Lithium-Ion Electrolytes  David S. Ashby, Ryan H. DeBlock, Chun-Han Lai, Christopher S. Choi, Bruce S. Dunn  Joule  Volume 1, Issue 2, Pages 344-358 (October 2017) DOI: 10.1016/j.joule.2017.08.012 Copyright © 2017 Elsevier Inc. Terms and Conditions

Joule 2017 1, 344-358DOI: (10.1016/j.joule.2017.08.012) Copyright © 2017 Elsevier Inc. Terms and Conditions

Figure 1 The Sol-Gel Process Schematic of ionogel synthesis for spin coating. Joule 2017 1, 344-358DOI: (10.1016/j.joule.2017.08.012) Copyright © 2017 Elsevier Inc. Terms and Conditions

Figure 2 Physical Structure and Bonding of Ionogels (A and B) N2 adsorption isotherm for (A) gel 1 and (B) gel 2. Inset is the calculated BJH pore size distribution from the adsorption isotherms. See also Figure S1. (C) FTIR spectrum for gel 1 and the silica matrix gelled in the absence of ILE. (D) FTIR spectrum of gel 2 with an overlay of the ILE spectrum. Peaks associated with Si-O-Si (asterisk), =CH2 (circle), and the VC (square) are indicated. See also Figure S2. Joule 2017 1, 344-358DOI: (10.1016/j.joule.2017.08.012) Copyright © 2017 Elsevier Inc. Terms and Conditions

Figure 3 Confinement Effect on the ILE Properties (A) TGA showing the thermal stability of the ILE, gel 1, gel 2, and the silica matrix without ILE. (B) Temperature dependence of the ionic conductivity for spin-coated gel 1 and gel 2. Data are presented as the mean with error bars. These ionogels are compared with neat ILE and LiPON. The activation energies are shown. (C) Electrochemical window of gel 1 in a cell with a stainless steel working electrode and lithium metal as the counter and reference electrode. (D) Temperature dependence of the ionic conductivity for drop-cast gel 1 and gel 2. Data are presented as the mean with error bars. These ionogels are compared with neat ILE and LiPON. The activation energies are shown. LiPON ionic conductivity was obtained from published data.46 Joule 2017 1, 344-358DOI: (10.1016/j.joule.2017.08.012) Copyright © 2017 Elsevier Inc. Terms and Conditions

Figure 4 Topographical and Penetration Ability of Ionogels (A) Scanning EM cross-section of gel 1 spun on an Si wafer. Scale bar, 1 μm. See also Figure S3. (B) Gel 1 spun on an LFP cathode. EDS mapping shows the penetration of the ILE and SiO2 components N, Si, F, S, and O. Scale bar, 25 μm. (C) Scanning EM planar view of gel 3 spun on Si wafer. The diameter of the patterned circles is 250 μm. Scale bar, 200 μm. (D) Cross-sectional scanning EM image of photo-patterned gel 3 spun on an Si wafer. Scale bar, 200 μm. See also Figure S4. Joule 2017 1, 344-358DOI: (10.1016/j.joule.2017.08.012) Copyright © 2017 Elsevier Inc. Terms and Conditions

Figure 5 Electrochemical Properties of Thin-Film Ionogels (A) GV measurements of different electrolytes on LFP at C/10. Results are shown for gel 1 and gel 2, with the ILE serving as a comparison. The inset shows the dQ/dV versus V curves extrapolated from the GV measurements. (B) Capacity variation with cycling for gel 1. Majority of the 150 cycles were at C/2. (C) Capacity variation with cycling for gel 2. Majority of the 80 cycles were at C/2. Joule 2017 1, 344-358DOI: (10.1016/j.joule.2017.08.012) Copyright © 2017 Elsevier Inc. Terms and Conditions