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Rice U team develops new class of quasi-solid-state electrolytes; stable performance at high temperatures

Researchers at Rice University, with colleagues at Wayne State University, report the development of a new class of quasi-solid-state Li-ion battery electrolytes which have the structural stability of a solid and the wettability of a liquid.

Micro flakes of clay particles drenched in a solution of lithiated Room Temperature Ionic Liquid (RTIL) form a quasi-solid system with structural stability until 355 ˚C. With an ionic conductivity of ~3.35mS cm-1, the composite electrolyte delivers stable electrochemical performance at 120 ˚C. As reported in a paper in ACS Applied Materials & Interfaces, a rechargeable lithium battery with LTO electrodes and the clay-based electrolyte delivered reliable capacity for over 120 charge/discharge cycles.

This discovery, like earlier work on supercapacitors by the lab, depends on the malleable qualities of bentonite clay and room-temperature ionic liquids that serve as both a separator and an electrolyte system and provide a conductive path between a battery’s anode and cathode.

A schematic representation of the components employed for synthesis of clay-RTIL quasi-solid-state electrolyte, along with the envisioned structure of lithium-ion battery. Credit: ACS, Kalaga et al. Click to enlarge.

Clay naturally has a lot of moisture in it, and that’s not a problem when you’re doing supercapacitors. But a battery has to have a lithium-ion conductive species in the electrolyte to conduct lithium ions from the cathode or anode, or vice versa, when you charge and discharge. Lithium is very reactive with water, so our first challenge was to eliminate water from the clay while keeping its structure intact.

—Kaushik Kalaga, lead author of the study

Kalaga and his team started by baking commercial clay particles at 650 C for an hour to dry them out. They then combined a room-temperature ionic liquid and lithium salt and mixed them into the clay in an oxygen-free glove box. The liquefied salt acts as a source of lithium ions that conduct through the electrolyte to the electrodes.

The researchers spread the resulting peanut butter-like slurry between lithium metal electrodes and encapsulated them in coin-shaped batteries for testing at various temperatures.

Conventional organic electrolytes cannot be used in batteries over 60 ˚C, due to their low boiling temperature; the vapors that form beyond 80 ˚C can lead to an explosion, Kalaga said. Batteries that have solid-state electrolytes work in high temperatures, but the electrolytes don’t connect as well with electrodes, which hurts performance.

The researchers built their composite electrolyte to be tough and conductive and still present the maximum surface area to electrodes to provide a solid path for current.

The units proved able to deliver current at high temperatures with a stable voltage window of 3 volts over 120 charge-discharge cycles and featured both the thermal stability of solid-state electrolytes and the wetting properties of liquid electrolytes, assuring good contact with the electrodes. The voltage window is the range between which the electrolyte is stable and is not chemically degraded.

It’s able to produce pretty good performance at room temperature, but it gets better at higher temperatures. The clay-based electrolyte gets less viscous but still retains its consistency at least to 150 C. The next step is to push the limits further.

—Kaushik Kalaga

The nature of the material makes it suitable for forming into many types of batteries, from thin films to commercial-scale units, the researchers wrote.

The Advanced Energy Consortium supported the research.


  • Kaushik Kalaga, Marco-Tulio F Rodrigues, Hemtej Gullapalli, Ganguli Babu, Leela Mohana Reddy Arava, and Pulickel M Ajayan (2015) “Quasi-Solid Electrolytes for High Temperature Lithium Ion Batteries” ACS Applied Materials & Interfaces doi: 10.1021/acsami.5b07636



This may be a good first step towards improved, more rugged, lower cost, solid states batteries?

Wish them the best.

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