ACS Applied Nano Materials
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2024
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IF 5.3
Xiaodi Li,Yantao Zhang,Yaying Dou,Zhiyi Zhao,Xiaoyun Fan,Haichao Jiang
Lithium metal is widely utilized due to its high theoretical capacity and low electrochemical potential. However, the growth of uncontrollable lithium dendrites and increased voltage polarization during lithium stripping and plating can severely impact cycling stability. In this study, we propose a nitrogen-rich triazinyl nanoporous organic polymer (DCP-CTF) as an artificial solid–electrolyte interphase (SEI) for a lithium-metal anode. The spatial distribution of the porous layered array structure enables the gradient migration of Li+. Meanwhile, the rigid nanochannels can also restrict the excessive growth of Li depositions through the steric confinement effect and reduce the generation of lithium dendrites. By combining density functional theory calculations with Fourier transform infrared spectroscopy, we demonstrate the functional lithiophilic coordination of DCP-CTF. The electron-rich triazine ring acts as a donor to attract Li+, and the pyridine nitrogen group serves as an effective lithium anchoring site. The abundant distribution of these lithiophilic sites can regulate Li+ transfer, thereby ensuring smooth lithium deposition and inhibiting dendrite formation. As a result, the DCP-CTF-modified lithium-metal anode exhibits exceptional electrochemical stability of more than 2500 h of cycling in an ether-based electrolyte at a high current density of 20 mA cm–2.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 29
·18127-18136
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IF 10.7
Jing Tao,Can Zhang,Xueyang Li,Xinlong Chen,Chenzhen Ji,Wang Wan,Chao Wang
Lithium metal anodes tend to form non-uniform Li deposition that causes dendrite growth during cycling. Meanwhile, the deposition and dissolution of lithium metal often results in the continuous formation and breakdown of the SEI. Additionally, the use of thick lithium metal often results in an excessive inventory of lithium, which diminishes the energy advantage of lithium metal. Fabricating thin lithium foils is challenging owing to the low mechanical strength of lithium metal. To address these issues, we employed an in situ structural regulation strategy to prepare high-performance lithium metal batteries. The mechanical strength of the prepared LiF@LiZn10/Li foil was significantly enhanced, allowing it to be thinned down to a thickness of 5 μm, accompanied with great air stability. Moreover, the in situ formation of LiZn alloys improved Li-deposition behavior. Furthermore, we demonstrated the participation of LiF particles in the in situ formation of the SEI, which facilitated Li+-transport kinetics. The LiF@LiZn10/Li electrode demonstrated significantly enhanced cycling performance by synergistically improving Li-deposition behavior and optimizing the SEI layer in situ. The LiF@LiZn10/Li foil electrode exhibited a long cycling life of over 1300 h at 1 mA cm−2 and 1 mA h cm−2. When coupled with a commercial LiFePO4 cathode (3.3 mA h cm−2), the LiFePO4‖LiF@LiZn10/Li cell exhibited a cycle life approximately thrice that of the cells with LMBs. This work provides a novel strategy to optimize LMAs for next-generation LMBs.
研究领域:
材料科学
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电化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yali Liu,Youlong Xu
The application of solid polymer electrolytes (SPEs) has been impeded by the low ionic conductivity, narrow oxidation potential and poor mechanical strength. Herein, we designed a novel in-situ PVDF-HFP/Poly 1,3-dioxolane (PDOL) polymer electrolyte with dual-salts and functional plasticizers of succinonitrile (SN)/fluoroethylene carbonate (FEC). One of the dual-salts, Lithium difloro(oxalato)borate (LiDFOB), could initiate the polymerization of DOL in-situ in the porous PVDF-HFP host to improve the interfacial compatibility. SN is beneficial to the improvement of ionic conductivity and the stability of high voltage cathodes, while the FEC can generate the LiF-rich SEI on Li metal anode. The PVDF-HFP host can further restrict the motion of anion and increase the strength of the SPE. Therefore, the as-obtained SPE exhibits a thin thickness of ∼ 32 μm, high ionic conductivity of 1.06 × 10 −4 S cm −1 at room temperature, an enlarged electrochemical window of 5.86 V versus Li/Li + and high lithium-ion transference number t Li+ of 0.72. Benefited from the synergetic effect, the Li/LiFePO 4 cell delivers a high initial capacity of 141.7 mAh g −1 at 2C with a capacity retention of 94.99% after 1000 cycles. This three-dimensional porous film-derived in-situ polymer electrolytes provide a new sight and simple strategy for designing polymer electrolytes, exhibiting attractive potential in flexible and high-energy–density solid-state batteries.
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
JOURNAL OF NON-CRYSTALLINE SOLIDS
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2022
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IF 4.458
Li Gao,Dujiang Lu,Yinghui Yang,Rongzhang Guan,Dongmei Zhang,Chenyi Sun,Shuai Liu,Xiufang Bian
A simple synthesis has been proposed for seaweed-like amorphous TiO 2-x modified Sb (a-TiO 2-x /Sb) composite nanowires as sodium-ion battery (SIBs) anodes by a dealloying method of Al-Sb-Ti alloys. Compared with other conventional methods, this method has the advantages of simple preparation, high yield and easy large-scale synthesis. It is excitingly discovered that a-TiO 2-x /Sb effectively alleviates volume changes and stabilizes the solid electrolyte interface (SEI). The a-TiO 2-x /Sb nanowires electrodes deliver outstanding electrochemical performance based on the synergistic effects, exhibiting a high reversible capacity of 591.9 mA h g −1 at 100 mA g −1 , stable cycling performance with a high capacity retention of 96.4% after 200 cycles and superior rate capability 382.2 mA h g −1 at 10,000 mA g −1 , which is very competitive among the reported Sb-based anodes.
研究领域:
材料科学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Fujuan Han,Zenghua Chang,Rennian Wang,Fengling Yun,Jing Wang,Chenxi Ma,Yi Zhang,Ling Tang,Haiyang Ding,Shigang Lu
LiNi0.8Mn0.1Co0.1O2||SiOx@graphite (NCM811||SiOx@G)-based lithium-ion batteries (LIBs) exhibit high energy density and have found wide applications in various fields, including electric vehicles. Nonetheless, its low-temperature performance remains a challenge. One of the most efficacious strategies to enhance the low-temperature functionality of battery is the development of appropriate electrolytes with low-temperature suitability. Herein, p-tolyl isocyanate (PTI) and 4-fluorophenyl isocyanate (4-FI) are used as additive substances to integrate into the electrolytes to improve the low-temperature performance of the battery. Theoretical calculations and experimental results indicate that PTI and 4-FI can both preferentially generate a stable SEI on the electrode surface, which is beneficial to reduce the interfacial impedance. As a result, the additive, i.e. 4-FI, is superior to PTI in improving the low-temperature performance of the battery due to the optimization of F in the SEI membrane components. At room temperature, the cyclic stability of the NCM811/SiOx@G pouch cell increases from 92.5% (without additive) to 94.2% (with 1% 4-FI) after 200 cycles at 0.5 C. Under the operating temperature of −20 °C, the cyclic stability of the NCM811/SiOx@G pouch cell increases from 83.2% (without additive) to 88.6% (with 1% 4-FI) after 100 cycles at 0.33 C. Therefore, a rational interphase design involving the modification of the additive structure is a cost-effective way to improve the performance of LIBs.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
PubMed
高影响因子
POLYMER
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2025
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IF 4.5
Xiuling Dong,Xinyi Ge,Wei Chen,Shuangqing Li,Zheng Xing,Qingguo Zhang,Zhong-Xia Wang
The interface problem between Li anode and gel polymer electrolytes (GPEs) hinder the performance improvement and application of Li metal batteries (LMBs). Herein, a GPE showcasing high ionic conductivity (3.91 mS cm −1 ) and elastic modulus (6.04 MPa) as GPE based on poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) was devised by introducing ionic liquids (ILs). The reconfiguration of Li ion solvation environment and the formation of LiF-rich solid electrolyte interface (SEI) protective layer have improved the interface problem. The LMB assembled from an optimized GPE- ET0.25 has stable Li deposition and excellent electrochemical properties , making the Li||LiFePO 4 (LFP) battery attaining an impressive long-cycle capacity retention rate of 96.0 %. This study emphasizes the advantages of IL aligned GPEs design, and the significance of forming stable SEI to improve battery performance, and provides ideas for the design of flexible LMBs with high safety and high performance.
研究领域:
材料科学
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电化学
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储能技术
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高分子科学
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锂离子电池
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Mengyue Yu,Jian Ma,Lei Dong,Minghao Huang,Bangzhuang Xue,Yi Sun,Hongfa Xiang
Silicon monoxide (SiOx, x ≈ 1) has been a promising candidate of anode materials for next-generation lithium-ion batteries due to its high specific capacity (∼2600 mA h g–1). However, huge volume expansion and the resultant repeated destruction of the solid electrolyte interphase (SEI) are key challenges to the practical application of the SiOx anode. In this work, a highly elastic quasi-solid polymer electrolyte (QSPE) is demonstrated for batteries employing an SiOx anode, which is prepared via in situ cationic ring-opening polymerization employing 1,3,5-trioxane (TXE) as the monomer, 1,3,2-dioxathiolane 2,2-dioxide (DTD) as both the initiator and film-forming additive, and fluoroethylene carbonate as the plasticizer. This TXE-based QSPE possesses excellent ionic conductvity properties, including an extremely low glass-transition temperature of −94.3 °C, a high ionic conductivity of 1.36 mS cm–1 at 25 °C, and a high Li+ transference number of 0.66. The long poly-TXE skeleton endows the polymer electrolyte with a high elastic modulus of 42 MPa, helping to effectively suppress the volume expansion of the SiOx anode during cycling. DTD participates in the construction of a robust SEI containing Li2SOx species, mitigating the structural collapse of SiOx particles. As a result, the cyclic stability of the SiOx anode has been remarkably enhanced─the Li||SiOx half-battery with the in situ TXE-based QSPE achieves 81.9% capacity retention after 200 cycles at 0.5C, exhibiting significant improvement over its liquid-state counterparts and showing promising application potential.
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
Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Zhang Shuoqing,Li Ruhong,Hu Nan,Deng Tao,Weng Suting,Wu Zunchun,Lu Di,Zhang Haikuo,Zhang Junbo,Wang Xuefeng,Chen Lixin,Fan Liwu,Fan Xiulin
Electrolyte engineering advances Li metal batteries (LMBs) with high Coulombic efficiency (CE) by constructing LiF-rich solid electrolyte interphase (SEI). However, the low conductivity of LiF disturbs Li + diffusion across SEI, thus inducing Li + transfer-driven dendritic deposition. In this work, we establish a mechanistic model to decipher how the SEI affects Li plating in high-fluorine electrolytes. The presented theory depicts a linear correlation between the capacity loss and current density to identify the slope k (determined by Li + mobility of SEI components) as an indicator for describing the homogeneity of Li + flux across SEI, while the intercept dictates the maximum CE that electrolytes can achieve. This model inspires the design of an efficient electrolyte that generates dual-halide SEI to homogenize Li + distribution and Li deposition. The model-driven protocol offers a promising energetic analysis to evaluate the compatibility of electrolytes to Li anode, thus guiding the design of promising electrolytes for LMBs.
研究领域:
材料科学
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电化学
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电池技术
✓ 已验证
DOI
高影响因子
ACS Nano
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2025
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IF 16
Ao Li,Jing Hao,Kai Wu,CaiYun Chang,XiangYong Zhang,He Gan,Jin Tan,Ting Xie,Fu Zhou,PengCheng Wang,CuiPing Han,HongDa Du,BaoHua Li,Qi Liu
Due to the inherent redox potential of the zinc metal anode (ZMA), it is susceptible to corrosion and dendrite formation in aqueous electrolytes. These issues compromise the electroplating-stripping process at the electrolyte–electrode interface, adversely affecting the reversibility of aqueous zinc-ion batteries (AZIBs). Here, we propose a chelating-ligand additive (i.e., DS) strategy to construct in situ an inorganic/organic hybrid bilayer interface. The organic molecule enriched in -PO3 groups is calculated to preferentially adsorb onto the surface of ZMA. During subsequent reactions, these adsorbed molecules decompose preferentially due to their low lowest unoccupied molecular orbital energy level (0.34 eV), forming a Zn(PO3)2-enriched inorganic solid electrolyte interphase (SEI) layer. Simultaneously, the intermediate carbon skeleton cross-links, creating an organic layer atop the SEI, thereby forming an inorganic/organic hybrid SEI bilayer interface. This bilayer SEI interface effectively inhibits corrosion and hydrogen evolution reactions (HERs) while regulating the Zn2+ ion flux at the interface, inducing uniform Zn depositions. Consequently, the Zn||Zn symmetric battery demonstrates a long-term cycling lifespan exceeding 1700 h at 5 mA cm–2. The Zn||I2 pouch battery yielded a capacity retention of 71.3% after 1100 cycles. This synergistic modulation strategy offers insights into the development of ZMA stabilizer additives, potentially advancing the performance and durability of AZIBs.
研究领域:
材料科学
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电化学
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储能技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
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2021
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IF 9.127
Linze Lv,Yan Wang,Weibo Huang,Yueyue Wang,Zhang Cao,Yuchen Li,Qiang Shi,Honghe Zheng
The commercialization of silicon (Si) anodes is sluggish due to the poor electrochemical performance of Si-based full cells (FCs). In order to break this limitation, this work investigates the effect of cathode type on the electrochemical performance of Si-based FCs and its mechanism. Based on electrochemical and spectral characterization , NCM523 is more suitable for assembling Si-based FCs to achieve high-rate and long-cycle. This is mainly because that the cathode type has an impact on the distribution of electrolyte decomposition products, while NCM523 is beneficial to the formation of more conductive organic components in the Si anode, and more LiF in the FC that can prevent electrolyte erosion. This work contributes to a basic comprehension of the electrochemical performance and SEI formation of Si-based FCs, and the results are helpful to the development and application of Si anodes.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
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IF 4.175
Jishen Hao,Zhiyong Yu,Hanxing Liu,Wei Song,Jun Liu,Linghua Kong,Chuanhua Li
Herein, NiF 2 artificial interface was proposed for the first time to enhance the electrochemical performances of LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) under 4.5 V. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images verify NiF 2 layer is successfully constructed on the surface of NCM523. The 1.0 wt% NiF 2 -modified NCM523 delivers a much higher capacity retention (86.9%) than pristine sample (69.0%) after 100 cycles under 4.5 V at 30 °C, even exceeding pristine NCM523 under 4.2 V (82.2%). Beyond that, the cycling stability of NCM523 under 4.5 V at 55 °C is also visibly improved due to the NiF 2 protective layer. Electrochemical impedance spectroscopy analyses confirm that NiF 2 suppresses the increase of interface resistance and therefore makes for the interface kinetics behaviors during cycling. In addition, the measurements of SEM, TEM and XPS support that the inhibition of the SEI (solid electrolyte interphase) growth can be attributed to the restrained side reactions between electrolyte and NCM523 by NiF 2 artificial layer at 4.5 V.
研究领域:
材料科学
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电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Fuyang Jiang,Yi Sun,Kuanxin Zhang,Yongchao Liu,Xuyong Feng,Hongfa Xiang
SiO x is considered to be a promising anode material for lithium-ion batteries (LIBs) due to the high lithium storage capacity. However, the large initial irreversible capacity loss and intensive volume change during cycling hinder its commercial applications. Prelithiation is an effective and convenient strategy to improve the initial Coulombic efficiency (ICE) of SiO x , while incomplete and unstable SEI on the prelithiated anode still results in rapid capacity decay. Herein, through the synergy effect of chemical pre-lithiation process and fluoroethylene carbonate reduction, a compact and stable LiF-rich SEI layer is in-situ formed on the surface of prelithiated SiO x anode. The modified SiO x anode exhibits a high ICE of 90.7% with good cycling performance. When paired with the commercial LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) cathode, the assemble pre-Li-SiO x /C||NCM622 full cell exhibit a high ICE of 85.7% and stable cycling stability. This work provides a new insight in constructing favorable SEI in pre-lithiation process.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）