Key Takeaways & Executive Findings
- •• • Capacity decay in SPAN||Gr pouch cells is driven by active lithium loss and increased resistance, with active lithium loss becoming dominant at higher temperatures (25–55 °C). • • The accelerated aging model based on the Arrhenius equation (y = 0.9x + a) accurately predicts cycling performance, reducing testing time by 50% when extrapolating from 55 °C to 25 °C. • • Active lithium loss is mainly due to dead lithium formation and SEI/CEI thickening, while resistance increase is predominantly from SEI/CEI thickening. • • The decay mechanism remains consistent across 25–55 °C, validating the use of accelerated aging models for this battery chemistry.
Abstract
Sulfur-based lithium-ion batteries, particularly those employing sulfurized poly(acrylonitrile) (SPAN) cathodes and graphite (Gr) anodes, offer high theoretical capacity and low cost but suffer from temperature-dependent capacity decay. This study systematically investigates the electrochemical dynamics and capacity decay mechanism of SPAN||Gr pouch cells cycled at 25–55 °C. Multiscale analyses reveal that capacity fade arises from active lithium loss and increased resistance, both accelerated by higher temperatures. Active lithium loss is primarily attributed to dead lithium formation and thickening of the solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI), while resistance increase is predominantly due to SEI/CEI thickening. As temperature rises, active lithium loss becomes the dominant decay factor. Leveraging the consistent decay mechanism across temperatures, an accelerated aging model based on the Arrhenius equation is developed: y = 0.9x + a. This model accurately predicts cycling parameters at specific temperatures and reduces testing time by 50% when extrapolating from 55 °C to 25 °C. These insights provide critical guidance for developing long-life sulfur-based batteries for practical energy storage applications.
1. Introduction
Conventional lithium–sulfur batteries, while offering high theoretical capacity (1675 mAh g−1), suffer from rapid capacity decay due to polysulfide dissolution and lithium metal anode instability. Sulfurized poly(acrylonitrile) (SPAN) chemically anchors sulfur within its polymer matrix, effectively suppressing polysulfide dissolution in carbonate electrolytes. Pairing SPAN with a graphite (Gr) anode circumvents lithium metal challenges, achieving 99% capacity retention over 1000 cycles in pouch cells. However, temperature-dependent capacity decay mechanisms remain poorly understood, impeding real-world deployment where thermal fluctuations are inevitable.
This study addresses the critical bottleneck of temperature sensitivity by systematically investigating SPAN||Gr pouch cells cycled at 25–55 °C. Through multiscale analyses, we identify consistent decay mechanisms—active lithium loss and increased resistance—across temperatures, enabling the construction of an Arrhenius-based accelerated aging model. This model accurately predicts cycling performance and reduces testing time by 50%, offering a practical pathway for rapid evaluation and optimization of long-life sulfur-based batteries.
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Huangwei Zhang, Xiaoyu Ge, Yidan Zhang, Kai Huang, Qihang Wang, Xin Deng, Yue Shen, Feng Ryan Wang, Jiulin Wang, Yunhui Huang, Zhen Li (2026). Cycling Decay Mechanism and Accelerated Aging Model of Sulfur-Based Lithium-Ion Batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3695-8
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Frequently Asked Questions
What are the primary degradation mechanisms in SPAN||Gr pouch cells at elevated temperatures?
At 25–55 °C, capacity decay is driven by active lithium loss (from dead lithium formation and SEI/CEI thickening) and increased resistance (mainly from SEI/CEI thickening). As temperature rises, active lithium loss becomes the dominant factor.
How does the accelerated aging model reduce testing time?
The model, based on the Arrhenius equation (y = 0.9x + a), allows prediction of cycling performance at 25 °C from data at 55 °C, cutting testing time by 50%.
What is the role of active lithium inventory in cycle life?
Active lithium loss is a critical factor; introducing additional lithium during pre-lithiation or replenishing during cycling could extend cycle life.
Is the decay mechanism consistent across the tested temperature range?
Yes, the decay mechanism remains unchanged from 25 °C to 55 °C, validating the use of accelerated aging models for this system.
What are the practical implications for battery design?
The findings suggest that managing active lithium inventory and minimizing SEI/CEI growth are key to improving cycle life, and the accelerated model enables faster evaluation of design optimizations.
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