ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chenran Hao,Huichao Lu,Jiqiong Liu,Huiming Zhang,Xirui Kong,Jun Yang,Yanna Nuli,Jiulin Wang
As one of the most promising battery systems, the lithium sulfur battery is expected to be widely used in fields of high energy density demands. Owing to the unique solid–solid conversion mechanism, there is no shuttle effect for the Li-SPAN (sulfurized polyacrylonitrile) battery. However, the compatibility between Li anode and carbonate electrolyte has not been resolved, which prevents the SPAN from practical applications. Herein, an organic–inorganic gel carbonate electrolyte is proposed to stabilize interphases and structures of both the anode and cathode, where polyimide (PI) is used for electrolyte gelation, which can assist in the uniform distribution of inorganic components at the electrolyte interface. Furthermore, ZnS nanodots loaded on two-dimensional MoS2 flakes provide abundant Li-ion diffusion paths, improve the transfer kinetic of Li ions, and induce uniform nucleation and deposition of Li. This gel electrolyte ensures Li symmetric cells a long-term cycle life of more than 900 h under the condition of deep lithium plating/stripping at 5 mAh cm–1. Li∥Cu cells exhibit a prolonged lifespan of 800 h with a CE of 98.3%. Furthermore, the Li-SPAN battery shows stability of more than 850 cycles, with the capacity retention of 85.1%. This work provides an approach for high-energy Li-SPAN batteries with carbonate-based electrolytes.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·Vol. 35
·期 44
·2509658
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IF 19
Chaoqiang Tan,Zeyu Shen,Shichao Zhang,Zhijun Wu,Shengnan He,Hongge Pan,Hao Cheng,Yingying Lu
Sulfurized polyacrylonitrile (SPAN) recently emerges as a prospective cathode for lithium–sulfur (Li–S) batteries owing to its high S utilization, remarkable cycling stability, and liberty from shuttle effect. Despite weakly solvating ether electrolytes exhibiting simultaneously compatibility for SPAN cathode and lithium (Li) anode, they universally suffer from low ionic conductivity and narrow liquid-phase temperature range. However, conventional ether-based electrolytes with excellent ionic conductivity cannot realize reversible solid–solid conversion of SPAN cathode due to Li polysulfide intermediates (LiPSs) dissolving and shuttling. Here, a series of weakly solvating ethers are evaluated by selectively methylating dimethoxymethane (DMM) to fine-tune their solvation capability and liquid-phase temperature range. Enlightened from weakly solvating ether electrolytes, the contact ion pair (CIP)-dominated electrolyte is designed for satisfactory ionic conductivity of electrolyte and reversible solid–solid conversion of SPAN cathode over wide temperature range. The reinforcement mechanisms of the CIP-dominated electrolyte for the Li anode and SPAN cathode are comprehensively elucidated through experimental characterizations and molecular dynamics simulations. Based on the optimized electrolyte, Li||SPAN full cells can steadily operate over wide temperature range from −20 to 60 °C. Furthermore, the 120 mAh Li||SPAN pouch cell can exhibit 85.5% capacity retention after 45 cycles at 0.2 C.
研究领域:
电化学
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能源材料
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锂离子电池
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电极界面化学
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电解质工程
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分子动力学模拟
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2025
·
IF 14.1
Runhe He,Hao Liu,Qing Gao,Dong Cai,Kuikui Xiao,Yinhang Zhang,Xinmin Zhang,Xianyang Cheng,Yuhui Wang,Lixing Kang,Huagui Nie,Yatao Liu,Zhi Yang
Sulfurized polyacrylonitrile (SPAN) represents a highly promising cathode material for lithium–sulfur (Li–S) batteries, leveraging a solid-solid sulfur conversion mechanism. However, persistent interfacial side reactions and sluggish redox kinetics in SPAN cathodes compromise the electrochemical performance. Here, quaternized chitosan (QCS) is employed as a functional agent to stabilize the SPAN cathode electrolyte interphase (CEI). The positively charged quaternary ammonium groups selectively adsorb PF 6 – anions, modifying the Helmholtz layer structure and facilitating the formation of an anion-derived CEI enriched with LiF. Consequently, the SPAN@QCS-1.0% cathode delivers a high discharge capacity of 1499 mAh g −1 at 0.2 C, an outstanding rate capability of 902 mAh g −1 at 10 C, and a prolonged cycle life exceeding 1500 cycles at 1 C. Under practical conditions of high sulfur loading (12.0 mg cm −2 ) and lean electrolyte (E/S ratio = 5 µL mg −1 ), the SPAN cell achieves a high areal capacity of 17.1 mAh cm −2 , surpassing that of conventional lithium–ion batteries (≈4 mAh cm −2 ) by more than fourfold. Furthermore, a 0.9 Ah pouch-cell prototype demonstrates stable cycling for over 30 cycles. The interface strategy provides a facile and effective approach to developing high-performance SPAN-based Li–S batteries.
研究领域:
电化学
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储能
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材料科学
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电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE CHEMICAL LETTERS
·
2023
·
IF 9.1
Zhenqiang Guo,Huicong Yang,Qian Wei,Shengjun Xu,Guangjian Hu,Shuo Bai,Feng Li
ABSTRACT Sulfurized polyacrylonitrile (SPAN) is proposed as a promising cathode material for lithium sulfur batteries. However, the continuous side reactions at the electrolyte-electrode interfaces as well as the slow redox kinetics of SPAN cathode deteriorate the electrochemical performance. In this study, an electrolyte with dual-additives comprising 2-fluoropyridine (2-FP) and lithium difluorobis (oxalato) phosphate (LiDFBOP) was used to improve the performance of Li||SPAN cells. 2-FP has a lower lowest occupied molecular orbital energy than that of the solvents in the electrolyte, leading to its prior reduction. A LiF-rich film can be formed on the electrode, effectively improving the stability of the electrolyte-electrode interfaces and prolonging the life. Simultaneously, LiDFBOP could form an electrolyte-electrode interface film containing a large amount of Li x PO y F z species, compensating for the kinetic deterioration caused by the lower ionic conductive of LiF formed at the electrolyte-electrode interface. Hence, an electrode-interface film with good chemical stability and high Li + transport was established by LiF and Li x PO y F z -rich species. The Li||SPAN cell with the electrolyte containing dual-additives demonstrates an excellent capacity retention of 97.5% after 200 cycles at 1.0 C, 25 °C, comparing to 56.2% capacity retention without additives. Moreover, the rate capacities of cells with dual-additives can reach 1128.1 mAh/g at 5 C, comparing to only 813.5 mAh/g using electrolyte without additives. Our results shown that the dual-additives in electrolyte provide a promising strategy for practical application of lithium sulfur batteries with SPAN cathodes.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2021
·Vol. 17
·期 47
·2103778
·
IF 13.281
Huajin He,Ying Liao,Wenhua Zuo,Guochang Li,Jiabao Gu,Yixiao Li,Zheng Hu,Yong Yang
Reducing SF 6 (as gas cathode) in Li batteries is a promising concept for the double benefit of mildly converting greenhouse SF 6 and providing a high theoretical energy density of 3922 Wh kg −1 . However, the reduction process is hampered by its sluggish kinetics. Here, cobalt phthalocyanine (CoPc) molecules immobilized on porous carbon matrix are, for the first time, introduced to the Li SF 6 chemistry to deliver an enhanced energy density. It is revealed that the high redox potential of Co(II)Pc/[Co(I)Pc] − (≈2.85 V) facilitates the formation of Co(I) N 4 sites to catalyze the SF 6 electrochemical reduction. By using highly porous holey nitrogen-doped carbon nanocages as carbon matrix, the Li SF 6 cells deliver a high discharge voltage of 2.82 V at 50 mA g C+CoPc −1 and an unprecedented areal capacity of 25 mAh cm −2 at 0.1 mA cm −2 , much superior to previous results. This work opens up new possibilities for high-efficiency conversion of SF 6 in lithium batteries.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）