Hybrid polymer network cathode-enabled soluble-polysulfide-free lithium–sulfur batteries

Meng Liao, Yaobin Xu, Muhammad Mominur Rahman, Sha Tan, Daiwei Wang, Ke Wang, Naveen K. Dandu, Qian Lu, Guoxing Li, Linh Le, Rong Kou, Heng Jiang, Au Nguyen, Pei Shi, Lei Ye, Anh T. Ngo, Enyuan Hu, Chongmin Wang and Donghai Wang ()
Additional contact information
Meng Liao: The Pennsylvania State University
Yaobin Xu: Pacific Northwest National Laboratory
Muhammad Mominur Rahman: Brookhaven National Laboratory
Sha Tan: Brookhaven National Laboratory
Daiwei Wang: The Pennsylvania State University
Ke Wang: The Pennsylvania State University
Naveen K. Dandu: University of Illinois at Chicago
Qian Lu: The Pennsylvania State University
Guoxing Li: The Pennsylvania State University
Linh Le: The Pennsylvania State University
Rong Kou: The Pennsylvania State University
Heng Jiang: The Pennsylvania State University
Au Nguyen: The Pennsylvania State University
Pei Shi: The Pennsylvania State University
Lei Ye: The Pennsylvania State University
Anh T. Ngo: University of Illinois at Chicago
Enyuan Hu: Brookhaven National Laboratory
Chongmin Wang: Pacific Northwest National Laboratory
Donghai Wang: The Pennsylvania State University

Nature Sustainability, 2024, vol. 7, issue 12, 1709-1718

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41893-024-01453-0

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