Abstract
Lithium-ion batteries are the leading energy storage technology for portable electronics and vehicle electrification. However, demands for enhanced energy density, safety, and scalability necessitate solid-state alternatives to traditional liquid electrolytes. Moreover, the rapidly increasing utilization of lithium-ion batteries further requires that next-generation electrolytes are derived from earth-abundant raw materials in order to minimize supply chain and environmental concerns. Toward these ends, clay-based nanocomposite electrolytes hold significant promise since they utilize earth-abundant materials that possess superlative mechanical, thermal, and electrochemical stability, which suggests their compatibility with energy-dense lithium metal anodes. Despite these advantages, nanocomposite electrolytes rarely employ kaolinite, the most abundant variety of clay, due to strong interlayer interactions that have historically precluded efficient exfoliation of kaolinite. Overcoming this limitation, here we demonstrate a scalable liquid-phase exfoliation process that produces kaolinite nanoplatelets (KNPs) with high gravimetric surface area, thus enabling the formation of mechanically robust nanocomposites. In particular, KNPs are combined with a succinonitrile (SN) liquid electrolyte to form a nanocomposite gel electrolyte with high room-temperature ionic conductivity (1 mS cm-1), stiff storage modulus (>10 MPa), wide electrochemical stability window (4.5 V vs Li/Li+), and excellent thermal stability (>100 °C). The resulting KNP-SN nanocomposite gel electrolyte is shown to be suitable for high-rate rechargeable lithium metal batteries that employ high-voltage LiNi0.8Co0.15Al0.05O2 (NCA) cathodes. While the primary focus here is on solid-state batteries, our strategy for kaolinite liquid-phase exfoliation can serve as a scalable manufacturing platform for a wide variety of other kaolinite-based nanocomposite applications.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 34913-34922 |
| Number of pages | 10 |
| Journal | ACS Applied Materials and Interfaces |
| Volume | 16 |
| Issue number | 27 |
| DOIs | |
| State | Published - Jul 10 2024 |
Funding
This work was supported by the National Science Foundation Future Manufacturing Program (NSF CMMI-2037026), the Northwestern University Materials Research Science and Engineering Center (NSF DMR-2308691), and the Trienens Institute for Sustainability and Energy at Northwestern University. In addition, C.M.T. was supported by the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1842165. D.Z. was supported by the Northwestern University McCormick Summer Undergraduate Research Award and the Meister Undergraduate Research Fund. Scanning and transmission electron microscopy, EDS, XPS, and FTIR analysis were performed in the NU ANCE facility at Northwestern University, which is supported by the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633), the Materials Research Science and Engineering Center (MRSEC) (NSF DMR-2308691), the State of Illinois, and Northwestern University. Rheometry and TGA were performed in the MatCI facility, which receives support from the Materials Research Science and Engineering Center (MRSEC) (NSF DMR-2308691). Physisorption measurements (BET) were performed in the React Engineering and Catalyst Testing (REACT) core facility at Northwestern University. XRD was performed in the Jerome B. Cohen X-Ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-2308691)
Keywords
- clay nanocomposite
- liquid-phase exfoliation
- solid-state battery
- succinonitrile
- sustainability
ASJC Scopus subject areas
- General Materials Science
