CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
YuFei Zhang,QiuHong Zhang,Yang Zhao,Di Wang,XinYue Wang,BaoNing Wang,Xu Yang,YuHang Jia,LiLi Wu,XiTian Zhang,Qi Jin
Stoichiometry engineering expands electronic tunability in Li S catalysts. • Composition tuning regulates charge redistribution and d-band centers in HEAs. • CF/HEA-1 enables Sabatier-balanced LiPSs adsorption and conversion. • CF/HEA-1 lowers polarization and accelerates bidirectional sulfur redox. • CF/HEA-1 enables 2000-cycle Li S cells with only 0.022% decay per cycle. Most existing studies on high-entropy alloy (HEA) sulfur electrocatalysts rely on changing elemental species to adjust their affinity for lithium polysulfides (LiPSs) and matching redox catalytic activity, so as to alleviate the intrinsic trade-off between LiPS adsorption and desorption. In this work, interconnected carbon fibers (CF) modified with CrMnFeCoNi HEA nanoparticles of tunable atomic ratios are synthesized to uncover the correlation between catalytic activity and surface electronic configuration toward efficient sulfur electrocatalysis. Combining density functional theory (DFT) calculations and systematic experimental characterizations, we demonstrate that tuning the atomic ratios of metallic elements within CrMnFeCoNi HEA can redistribute their surface charge, shift the positions of the d-band center, and ultimately regulate their adsorption affinity toward LiPSs. The optimized HEA catalyst achieves a favorable balance between adsorption and desorption, which drastically boosts the catalytic efficiency of LiPS conversion. Consequently, the cell based on the optimized CF/HEA-1 interlayer delivers a high reversible capacity of 938 mAh g −1 and maintains stable long-term cycling over 2000 cycles at 1.0C, corresponding to an ultralow capacity decay rate of 0.022% per cycle. This work proposes a feasible electronic modulation strategy to optimize HEA catalytic behavior, providing valuable guidance for the design of advanced lithium‑sulfur battery electrocatalysts. Download: Download high-res image (129KB) Download: Download full-size image
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Zehao Shi,Tiancheng Wang,Zeyuan Shi,Shengrui Cui,Zengqi Zhang,Wei Liu,Yongcheng Jin
“Shuttle effect” is a serious obstacle in the development of high-performance lithium-sulfur batteries and modified separator is considered an effective strategy to prevent the shuttle effect of soluble polysulfides (LiPSs). Herein, we demonstrate a modified polypropylene (PP) separator composed of nitrogen-doped carbon coated LiFePO 4 (NC-LFP), Ketjen black carbon (KB) and polyvinylidene fluoride (PVDF) (NC-LFP interlayer), which can improve adsorption and catalytic conversion toward LiPSs. The analysis shows that NC-LFP interlayer could effectively adsorb LiPSs and therefore suppress its shuttle effects due to the Fe N C functional groups in the nitrogen-doped carbon coated on LFP polar particles. The DFT analysis and the electrochemical performance test demonstrate the Fe N C functional groups in NC-LFP interlayer provide lower activation barrier for catalytic conversion reaction of LiPSs to Li 2 S and vice versa. The coin cells with NC-LFP modified separator exhibit an initial discharge specific capacity of 907 mAh/g at 1C. After 500 cycles, the specific capacity is 702 mAh/g with a retention rate of 79.5 %. Moreover, at 8C rate, the discharge-specific capacity of 667.5 mAh/g is achieved. The use of NC-LFP interlayer modified separators realizes lithium-sulfur batteries with long-cycle life and high-rate performance, providing an emerging strategy for high-performance Li-S batteries.
研究领域:
材料科学
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电化学
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储能
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电池技术
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DOI
高影响因子
ELECTROCHIMICA ACTA
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2022
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IF 7.336
Pengqian Guo,Pengfeng Jiang,Weixin Chen,Guoyu Qian,Deyan He,Xia Lu
Interfacial engineering plays an important role in dynamically stabilizing the electrochemical performance of lithium-sulfur batteries (LSBs). Constructing a robust interface, e.g., using a multifunctional membrane, benefits not only for the suppression of lithium polysulfides (LiPSs) shuttling, but also for the inhibition of uncontrollable Li dendrite growth. Herein, a bifunctional membrane is fabricated with the Al 2 O 3 nanoparticle-embedded polyacrylonitrile nanofibers (Al 2 O 3 /PAN) in a facile way as separator, which are found effective in blocking the growth of Li dendrite and the shuttling of LiPSs in LSBs. The exposed Al 2 O 3 nanoparticles work in a responsible way to physiochemically capture the LiPSs and simultaneously let the Li ions shuttle through the PAN nanofiber network as the simulation indicated. The 3D cross-linked membrane can also block the oriented Li deposition and growth to make the symmetric Li||Li cell cycle over 1500 h without short circuit at 0.5 mA cm −2 . Moreover, the LSB exhibits a reversible capacity of 2.08 mAh cm −2 at 500 mA g −1 under the sulfur loading of 3.6 mg cm −2 . These results provide a doable and economy way to fabricate the robust membrane to deal effectively with the tough issues, which sheds new light on the design and optimization of high-energy-density sulfur prevailed rechargeable batteries.
研究领域:
材料科学
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电化学
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能源存储
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电池技术
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DOI
高影响因子
Green Energy & Environment
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2020
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IF 6.395
Hongtai Li,Yanxiao Chen,Quan Jin,Wei Xiang,Benhe Zhong,Xiaodong Guo,Bao Wang
Serious shuttle effect and sluggish conversion kinetics of lithium polysulfides (LiPSs) have a massive impact on obstructing the practical application of lithium-sulfur (Li–S) batteries. To address such issues, Fe-Nx sites enriched microporous nanoflowers planted with tangled bamboo-like carbon nanotubes (Fe-Nx-C/Fe 3 C-CNTs NFs) are found to be effective catalytic mediators with strong anchoring capabilities for LiPSs. The bamboo-like carbon nanotubes catalyzed by Fe 3 C/Fe entangled each other to form a conductive network, which encloses a flower-like microporous carbon core with embedded well-dispersed Fe-Nx active sites. As expected, electrons smoothly transfer along the dense conductive bamboo-like carbon network while the flower-like carbon core consisting of micropores induces the homogeneous distribution of tiny sulfur and favors the lithium ions migration with all directions. Meanwhile, Fe-Nx sites strongly trap long-chain LiPSs with chemical anchoring, and catalyze the redox conversion of LiPSs. Due to the aforementioned synergistic effects, the [email protected] /Fe 3 C-CNTs NFs cathode exhibited a remarkable specific capacity (635 mAh g s −1 ) at 3 C and a favorable capacity decay with 0.04% per cycle even after 400 cycles at 1 C.
研究领域:
材料科学
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能源存储
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电化学
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纳米技术
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DOI
高影响因子
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