Abstract
New electrolytes are critical for high-energy lithium (Li)–sulfur (S) batteries (LSBs) to ensure their stability against Li metal anode and polysulfides (PSs) shuttling which hinder the large-scale application of LSBs. In this study, the design principle of moderately solvating electrolytes (MSEs) for LSBs is demonstrated by using a multiple-solvent system comprising of a highly solvating solvent, a weakly solvating solvent, and a non-solvating solvent to create a well-balanced electrolyte system. This resulting electrolyte significantly improves the cycle life of LSBs, achieving 300 cycles, which is twice as long as that of similar cells with the conventional electrolyte and it also ensures stable calendar life for at least seven months. The optimal MSE forms robust passivation layers enhancing the structural integrity of both S and Li metal electrodes after cycling. These virtues effectively hinder parasitic side reactions and self-discharge behavior of LSBs. This electrolyte design principle is versatile and can be applied to other battery chemistries, providing a potential path toward the development of a more efficient and stable battery system. By addressing key challenges such as the instability of electrodes and shuttling of polysulfides, this electrolyte approach offers promising solutions for advancing LSB technology.
| Original language | English |
|---|---|
| Article number | 2503365 |
| Journal | Advanced Materials |
| Volume | 37 |
| Issue number | 33 |
| DOIs | |
| State | Published - Aug 21 2025 |
| Externally published | Yes |
Funding
This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (VTO), of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under the contract no. DE-AC05-76RL01830. 3-D slicing work was carried out by using the dual beam system that was funded by a grant from the Washington State Department of Commerce's Clean Energy Fund. The XPS characterization was supported under a partial grant from the Washington State Department of Commerce's Clean Energy Fund and performed at the Environmental Molecular Sciences Laboratory, a DOE Office of Science User Facility sponsored by the Office of Biological and Environmental Research located at Pacific Northwest National Laboratory (PNNL). PNNL is operated by Battelle for the DOE under contract DE-AC05-76RL01830. The XRD work was performed at the National Synchrotron Light Source II, a US DOE Office of Science user facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. The authors thank Brian Callaghan of PNNL for running Raman experiments. This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (VTO), of the U.S. Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) program (Battery500 Consortium) under the contract no. DE‐AC05‐76RL01830. 3‐D slicing work was carried out by using the dual beam system that was funded by a grant from the Washington State Department of Commerce's Clean Energy Fund. The XPS characterization was supported under a partial grant from the Washington State Department of Commerce's Clean Energy Fund and performed at the Environmental Molecular Sciences Laboratory, a DOE Office of Science User Facility sponsored by the Office of Biological and Environmental Research located at Pacific Northwest National Laboratory (PNNL). PNNL is operated by Battelle for the DOE under contract DE‐AC05‐76RL01830. The XRD work was performed at the National Synchrotron Light Source II, a US DOE Office of Science user facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE‐SC0012704. The authors thank Brian Callaghan of PNNL for running Raman experiments.
Keywords
- cycle and calendar life
- lithium-sulfur battery
- moderately solvating electrolyte
- polysulfide
- self-discharge