期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 15, 期 2, 页码 843-854出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ee03103a
关键词
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资金
- Office of Vehicle Technologies of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program (Battery500 Consortium) [DE-EE0007762]
- DOE Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
Advanced electrolytes can improve the electrochemical performance of anode-free lithium-metal batteries by forming denser and better-packed lithium morphologies, enabling uniform lithium plating over the electrode area and reducing capacity fade. However, the mechanisms by which electrolytes improve performance are still not well understood.
Anode-free lithium-metal batteries (LMBs) are ideal candidates for high-capacity energy storage as they eliminate the need for a conventional graphite electrode or excess lithium-metal anode. Current anode-free LMBs suffer from low Coulombic efficiency (CE) due to poor lithium stripping efficiency. Advanced electrolyte development is a promising route to maximize lithium plating and stripping CE and minimize capacity fade. However, a poor understanding of the mechanisms by which advanced electrolytes improve performance hampers progress in the practical development of anode-free LMBs. Here, we use synchrotron techniques and other tools to analyze the influence of three commercially available electrolytes on the composition, heterogeneity, kinetics, morphology, and electrochemistry of anode-free LMBs. Advanced electrolytes improve the electrochemical performance of anode-free LMBs by forming much denser and better-packed Li morphologies on a Cu current collector than on the conventional electrolyte. Li plates uniformly over the electrode area with the advanced electrolytes rather than in a few active sites. Inactive crystalline Li with heterogeneous distribution dominates the capacity degradation of anode-free cells, especially with the conventional electrolyte, indicating that reducing the amount of dead crystalline Li will significantly improve the cycling stability of anode-free cells. The understanding of the Li plating and stripping process obtained from this work will accelerate the development of anode-free LMBs with high efficiency.
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