Abstract
Among the emerging ‘beyond lithium-ion’ technologies for maximized sustainability, lithium–sulfur (Li–S) is a favoured chemistry because of its exceptional energy density from the conversion of sulfur, an element in abundant supply. However, the dissolution of several intermediate polysulfides formed during conversion leads to rapid performance degradation over cycling. Here we address this issue by sulfurizing a hybrid polymer network with polyphosphazene and carbon as a cathode for Li–S batteries. With rich sites to re-bond and adsorb dissociative sulfur species, this hybrid polymer network circumvents the formation of soluble polysulfides and enables a unique, reversible inserting conversion reaction. Thus, our cathode delivers both high capacity (~900 mAh g−1cathode) and excellent cycling stability in Li–S coin cells, with a pouch cell demonstration of projected energy density of ~300 Wh kg−1 and 84.9% capacity retention after 150 cycles. The strategy can be extended to other cost-effective, recyclable polymers, advancing sulfur-based batteries towards practical energy storage application.
| Original language | English |
|---|---|
| Article number | 2003666 |
| Pages (from-to) | 1709-1718 |
| Number of pages | 10 |
| Journal | Nature Sustainability |
| Volume | 7 |
| Issue number | 12 |
| DOIs | |
| State | Published - Dec 2024 |
| Externally published | Yes |
Funding
This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy (DOE), through an Advanced Battery Materials Research (BMR) Program award no. DE-EE0009650. C.W. thanks the support of Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US DOE under the Advanced BMR Program and the United States-Germany Cooperation on Energy Storage under contract no. DE-LC-000L072. The in situ TEM was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the US DOE\u2019s Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory. The Pacific Northwest National Laboratory is operated by Battelle for the US DOE under contract no. DE-AC05-76RL01830. The work at Brookhaven National Laboratory is supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the US DOE through the Advanced BMR Program under contract no. DE-SC0012704. This research used the 8-BM and 28-ID-2 beamlines of the National Synchrotron Light Source II, US DOE Office of Science User Facilities, operated for the DOE\u2019s Office of Science by the Brookhaven National Laboratory under contract no. DE-SC0012704. We thank the computing resources provided by the Laboratory Computing Resource Center at Argonne National Laboratory for performing the density functional theory calculations.