Journal of Energy Storage
·
2025
·
IF 9.8
Shaoxiang Su,Gaoyang Liang,Meizhen Qu,Zhengwei Xie,Wenjing Liu
Compared to nano‑silicon, micron-sized silicon offers broader raw material availability, can be derived from industrial-grade silicon powder, features simplified fabrication processes, lower costs and avoids the agglomeration issues associated with nanoparticles, demonstrating greater potential for large-scale applications. However, its severe volume expansion during cycling triggers structural instability and cycling performance degradation, severely hindering commercialization. Therefore, this study utilizes the Si-OH groups on the surface of micron-sized silicon to form hydrogen bonds and covalent bonds with polyacrylic acid binders to improve cycling performance. Vacuum high-temperature treatment is employed to promote the formation of Si–O–C(O)– covalent bonds between the Si-OH on the silicon surface and polyacrylic acid. The influence of surface Si-OH density on cycling performance was investigated, as this density needs to balance the long-cycle stability of micron-sized silicon with the parasitic side reactions caused by Si-OH groups. The appropriate quantity of Si-OH will enhance the structural stability of the electrode, promote the formation of more Li 2 CO 3 /LiF, and mitigate the electrical contact and capacity loss caused by the volume expansion of micron-sized silicon. Si-OH-10-180 electrode prepared under vacuum high temperature exhibits a high reversible capacity of 1264 mAh g −1 at 0.5 A g −1 after 200 cycles. Compared to the Si-105 electrode, which has a capacity of 63 mAh g −1 after 45 cycles at 2 A g −1 , the Si-OH-10-180 electrode maintains a reversible capacity of 453 mAh g −1 after 300 cycles. This work provides a direct approach to enhance the cycling performance of high-capacity micrometer-sized silicon-based anodes.
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DOI
高影响因子
RARE METALS
·
2023
·Vol. 43
·期 3
·1017-1029
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IF 8.8
Han Xiang,Xu Min,Gu Lan-Hui,Lan Chao-Fei,Chen Min-Feng,Lu Jun-Jie,Sheng Bi-Fu,Wang Peng,Chen Song-Yan,Chen Ji-Zhang
Silicon has ultrahigh capacity, dendrite-free alloy lithiation mechanism and low cost and has been regarded as a promising anode candidate for solid-state battery. Owing to the low infiltration of solid-state electrolyte (SSE), not the unstable solid–electrolyte interphase (SEI), but the huge stress during lithiation- and delithiation-induced particle fracture and conductivity lost tend to be the main issues. In this study, starting with micron-Si, a novel monothetic carbon conductive framework and a MgO coating layer are designed, which serve as electron pathway across the whole electrode and stress releasing layer, respectively. In addition, the in situ reaction between Si and SSE helps to form a LiF-rich and mechanically stable SEI layer. As a result, the mechanical stability and charge transfer kinetics of the uniquely designed Si anode are significantly improved. Consequently, high initial Coulombic efficiency, high capacity and durable cycling stability can be achieved by applying the Si@MgO@C anode in SSB. For example, high specific capacity of 3224.6 mAh·g −1 and long cycling durability of 200 cycles are achieved. This work provides a new concept for designing alloy-type anode that combines surface coating on particle and electrode structure design. Graphical abstract
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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固态离子学
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纳米材料
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电池技术
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DOI
高影响因子
Energy & Environmental Materials
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2025
·
IF 14.1
Wenjian Wang,Changyi Zheng,Shengjie Zhang,Yao Liu,Linjuan Zhang,Jianqiang Wang,Yonggang Wang
Micro-sized silicon (mSi) anodes offer high capacity for next-generation lithium-ion batteries but suffer from severe volume changes, causing unstable interphases and poor cycling. Traditional electrolytes derive unstable electrolyte/electrolyte interphases, and flammable solvents pose safety risks. Here, we introduce a non-flammable molten salt electrolyte, which consists of lithium bis(fluorosulfonyl)imide, potassium bis(fluorosulfonyl)amide, and cesium bis(fluorosulfonyl)imide in a mole ratio of 0.3:0.35:0.35 (noted as Li 0.3 K 0.35 Cs 0.35 FSA), that forms an inorganic interphase on mSi, stabilizing the electrode/electrolyte interface. Computational and experimental insights elucidate the FSA − anion decomposition-derived SEI predominantly of LiF, Li 3 N, Li 2 O, and Li 2 S, which exhibits mechanical resilience and low interfacial resistance, effectively accommodating the significant volume expansion of silicon during lithiation/delithiation. As a result, the Li||mSi half-cell achieves 60.7% capacity retention after 100 cycles with 99.5% average Coulombic efficiency. Overall, the Li 0.3 K 0.35 Cs 0.35 FSA electrolyte eliminates flammability concerns while enabling robust cycling performance. This work demonstrates a safe, high-energy battery system by coupling mSi anodes with stable molten salt electrolytes, addressing both interfacial instability and safety challenges in mSi-based lithium-ion batteries.
研究领域:
电化学
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材料科学
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能源存储
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界面化学
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锂电池技术
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Mei Liu,Yiting Hao,Jingde Li,Guihua Liu
The integration of micro-sized silicon (μm-Si) with high theoretical capacity and structurally stable graphite (Gr) has great potential in promoting the next generation of lithium-ion battery anodes. However, the application of Gr/μm-Si anodes is impeded by the excessive solid electrolyte interphase (SEI) accumulation and electrical disconnection caused by μm-Si swelling and fracturing. Herein, a multifunctional carbon layer (MCL) composed of in situ grown carbon nanotubes (CNTs) and pyrolytic carbon derived from polyacrylonitrile is prepared to optimize Gr/μm-Si anode material. The pyrolytic carbon serves to anchor the CNTs and isolate the μm-Si surface from the electrolyte, mitigating side reactions and ensuring stable SEI formation. The CNTs create a robust three-dimensional conductive network, providing mechanical buffering for μm-Si volume expansion while enhancing electron and ion transport. Accordingly, the Gr/Si@MCL anode exhibits a discharge specific capacity of 503.6 mAh g −1 , maintaining an exceptionally low capacity decay of just 0.031% per cycle after 500 cycles at a current density of 1 A g −1 . Furthermore, the Gr/Si@MCL||LiFePO 4 full-cell demonstrates excellent performance, particularly with a high energy density of 347 Wh kg −1 . These results highlight the potential of the proposed structure design for advancing the practical deployment of Gr/μm-Si anodes in next-generation energy storage devices.
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Jianshun Feng,Mingxiu Hou,Qian Zhang,Dong Wang,Zhenjiang Li,Jie Liu,Yumin Wu,Lei Wang
Designing robust binders has been demonstrated to be an effective and facile strategy to stabilize Si anodes. However, the binders that performed well for Si nanoparticles are not applicable for low-cost and accessible Si micron-powders. Hence, a novel binder design strategy is still greatly required for practical micron-Si anodes. Herein, a robust water-based network binder (named as c-PTP-Alg) has been designed via coupling potassium tripolyphosphate (PTP) inorganic oligomer with alginic acid (Alg) organic macromolecule. Owing to the unique structure of PTP, a network with high mechanical resistance can be constructed in c-PTP-Alg binder via strong ion-dipole interactions. Moreover, the highly soluble and dispersed PTP inorganic oligomer in water prevents the organic macromolecule from aggregation. This induces a homogeneous texture in the c-PTP-Alg binder, which enables the polar groups in the composite binder to anchor micron-Si particles efficiently. Therefore, by simply applying the c-PTP-Alg binder, a significantly improved electrochemical performance of micron-Si anode with a high reversible capacity of 1599.9 mAh g −1 after 100 cycles at 3000 mA g −1 has been obtained. More specially, the high-energy-density Si||S-PAN full cells have also been constructed, showing the practical application prospect of the c-PTP-Alg binder.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Yiye Guo,Mouren Miao,Yun-Xiao Wang,Chunxing Yan,Jin Liu,Yuliang Cao,Hanxi Yang,Xinping Ai,Fu-Sheng Ke
A full cell via pairing high-capacity silicon anode with high-voltage NMC cathode (Li(Ni 0.83 Co 0.12 Mn 0.05 )O 2 ) holds great promise as a high-energy battery system for practical applications. Nevertheless, this potential has been hindered by challenges in terms of the pulverization of Si particles, unstable electrode/electrolyte interface, and severe dissolution of transition metals at high voltage. Herein, we present a novel high-voltage and weakly solvating electrolyte, consisted of lithium bis(fluorosulfonyl)imide in mixed solvent of diethyl carbonate and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether, which effectively enables the remarkable cycling stability of both micron silicon anode (a high reversible capacity of 1667 mAh g −1 after 200 cycles) and Ni-rich cathode (a notable capacity retention of 83% after 140 cycles at an ultrahigh cut-off voltage of 4.9 V). It is revealed that the tailored electrolyte leads to the formation of a robust and reinforced concrete-like solid electrolyte interphase, characterized by a distinctive vertical side-by-side columnar structure comprised of LiF and sulfide on the micro-silicon anode. Meanwhile, a uniform and thin cathode-electrolyte interphase is observed on the surface of NMC particles when cycled in the designed electrolyte. Furthermore, coupled with high-capacity micro-Si and high-voltage NMC, this designed electrolyte endows a remarkable full-cell with high energy density (475 Wh kg −1 ), excellent rate capability, and high-voltage cycling stability. This research contributes a pioneering approach to enabling the utilization of micron-sized silicon anodes and Ni-rich cathodes for next-generation high-energy lithium-ion 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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DOI
高影响因子
Energy Technology
·
2020
·Vol. 8
·期 7
·2000278
·
IF 3.404
Xiang Guan,Yuanxing Yong,Qingping Wu,Xiaowan Zhang,Xuhong Guo,Chilin Li,Jun Xu
High-capacity silicon anodes have attracted tremendous interest for next-generation lithium-ion batteries (LIBs). However, its further application is limited by the large volume expansion during cycling. Designing nanostructured silicon is an effective strategy to acquire high-performance anodes, but it will face problems of high cost and poor coulombic efficiency. As a comparison, surface modification of micron silicon is more economically viable. Herein, a novel route is proposed to synthesize metal-chelated biomimetic polyelectrolyte as a powerful binder, which wraps micron silicon particles in a thin Fe 3+ –polydopamine (PDA) layer with a thickness of 2–5 nm. The introduced Fe 3+ can form powerful metal-chelated bonds with PDA at appropriate hydrothermal temperature (160 °C). As a result, the mechanical strength of the protective layer is enhanced and the electrochemical activity of micron silicon is improved. Meanwhile, the 3D crosslinking structure formed through the esterification between the elastic polymer layer and polyacrylic acid (PAA) further guarantees the structural stability of anodes. Batteries using Si@Fe 3+ –PDA–160/PAA anode exhibit excellent cycling performance with stable capacity of 2000 mAh g −1 over 200 cycles at 0.5 C and high capacity retention ratio of 80% after 100 cycles at 0.1 C.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
危险品化学品经营许可证（带存储）