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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Tris(pentafluoro)phenylborane electrolyte additive regulates the highly stable and uniform CEI membrane components to improve the high-voltage behaviors of NCM811 lithium-ion batteries

Lucheng Li,Meiling Liu,Peng Yang,Wenfeng Yuan,Jun Chen

Broadening the charging and discharging voltage window of high nickel cathode material NCM811 is the most expected method to improve the high specific energy density of batteries currently, yet the cathode-electrolyte interface (CEI) formed by the oxidized and decomposed products of carbonate-based electrolyte under high voltage are always so unsatisfied. Therefore, a voltage-stabilizer, TPFPB (Tris(pentafluoro)phenylborane), added into baseline electrolyte (1 M LiPF 6 in EC:EMC:DMC=1:1:1 vol%) to promote the electrochemical performance of the battery at 4.5 V. The results interpret that the TPFPB-contained NCM811-Li half-cells exhibit high specific capacity (167.10 mAh/g), excellent capacity retention rate (CRR) (75.37 %), and high rate performance (173.3 mAh/g at 5C) during 4.5 V. Meanwhile, through the analysis of the physical characterization techniques. the B- and F-rich interfacial layer, named as CEI film, existing at the interface between the cathode and the electrolyte, produced under 4.5 V, is superior, resulting in impeding the structural collapse of the cathode material and the continued dissolution of transition metal ions (TM n + ) from the cathode material, as well as, ameliorate the electrochemical polarization of the battery, ultimately, it can stabilize the electrochemical performance of the battery under high voltage. Therein, the present work elucidate a new and substantial approach to enhance the high-voltage performances of rich-Ni cathode materials.

CAS / MDL: 1109-15-5
研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Multifunctional carbonyl-rich compounds for constructing “corrosion-resistant electrodes and electrolyte interface” in high-voltage sodium-metal batteries

Qiang Wang,Qian Wang,Xinming Fan,Chaofan Tang,Lu Zhou,Shan Liu,Hui Tang,Runjin Liu,Linka Zhu,Lei Zhang,Qinghua Tian,Xueyi Guo

In recent years, there has been notable advancement in the development of high-performance materials for sodium-ion batteries, particularly in layered oxide cathodes. However, research on enhancing the interface between electrolytes and cathodes remains nascent. One promising approach involves the addition of electrolyte additives, recognized for their cost-effectiveness and efficiency in bolstering the electrode/electrolyte interface to enhance material stability during high-voltage cycling. In this work, we investigate the use of glutaric anhydride (GA) as an electrolyte additive to improve the cycling stability of NaNi 1/3 F 1/3 M 1/3 O 2 /Na (NFM/Na) high-voltage sodium-metal batteries. Batteries using GA-containing electrolytes demonstrate impressive capacity retention: 80.51 % after 200 cycles at 4.0 V and 76.01 % after 150 cycles at 4.1 V. The research delves into the mechanistic insights behind GA’s effectiveness in enhancing cyclic stability. Theoretical calculations reveal that GA plays a crucial role in modifying the structure of the first solvation shells, promoting the formation of an elastic cathode-electrolyte interface (CEI) film enriched with O C O groups. This uniform and stable CEI film effectively preserves the material’s crystal structure and mitigates the dissolution of transition metals, thereby prolonging battery lifespan under demanding extremely cycling conditions.

CAS / MDL: 108-55-4
研究领域: 材料科学 · 电化学
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ENERGY & FUELS · 2024 · IF 5.2

Improve High Voltage Resistance Performance of LiNi0.8Co0.1Mn0.1O2 Lithium Metal Batteries by Two Novel Aromatic Compound Electrolyte Additives

Jian Lv,Yiwen Wang,Zhuyu Wang,Danni Shen,Qinggong Jia

Ternary high-nickel oxide exhibits a relatively high working voltage compared with traditional lithium battery cathodes (LiFePO4, etc.). Consequently, it has been widely studied in recent years and is at the forefront of research on positive electrodes for power batteries. To achieve higher reversible capacity, it is often necessary to increase the battery operating voltage. However, there are many drawbacks to this method, such as surface cracking of the working electrode and serious side reactions with the electrolyte. The novel dual-additive combination in this work has the potential to significantly address the aforementioned issues. A composite polymer cathode–electrolyte interface (CEI) film is formed on the surface of the cathode due to two aromatic compound additives preoxidation. The stable CEI film not only improves the stability of the electrode but also suppresses solvent and hydrofluoric acid (HF) to effectively inhibit the side reaction on the cathode surface. Furthermore, these two additives can be readily reduced at the anode to form a solid electrolyte interface (SEI) membrane containing rich LiN&LiF, which effectively suppresses the formation of lithium dendrites. The battery capacity retention could be up to nearly 83% on the dual-additive electrolyte compared to the baseline electrolyte after 300 cycles. This work may provide more possibilities for future research on high-voltage lithium batteries.

CAS / MDL: 86-74-8 1072-63-5
研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 9 ·090554 · IF 4.316

Bis(neopentyl glycolato)diboron as A Cathode Stabilizer Additive for High-Voltage Lithium-ion Batteries

Donghai Huang,Zhiqiang Ge,Changfu Yuan,Ao Mei,Zhiyong Fu,Zhiping Le

Bis(neopentyl glycolato)diboron (BNGDB) is used as a electrolyte additive to improve the stability of commercialized lithium ion batteries operating at a high charging-cutoff voltage. Adding of BNGDB lowers the oxidation potential of the electrolyte, which will lead to the formation of a uniform, stable, and low resistance cathode solid electrolyte interphase (CEI) on the cathode surface. This CEI film can suppress the loss of electrolyte by preventing further reaction between electrolyte and cathode material (LiNi0.6Co0.2Mn0.2O2), which improves cyclic stability and discharge capability of LiNi0.6Co0.2Mn0.2O2/graphite pouch cells. With 0.5 wt% BNGDB addition, the pouch cell demonstrate a discharge capacity retention of 83.2% after 200 cycles in base electrolyte. This work brings new insight into the role of additives in electrolytes and can guide the design of more versatile electrolytes for commercialized lithium-ion batteries.

研究领域: 材料科学 · 电化学
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Journal of Energy Storage · 2025 · IF 9.8

Development of stable electrode-electrolyte interfaces with multifunctional flame-retardant microspheres for safe, high-voltage, and high-energy-density lithium batteries

Hao Yu,Guoqing Liu,Hao Jia,Tao Zhu,Xinxin Dong,Wei Liu,Xiaoyu Gu,Shuheng Wang,Sheng Zhang

Polyethylene oxide (PEO) organic solid electrolyte is regarded as one of the important research directions of next-generation battery technology due to its good electrode interface compatibility, mechanical flexibility, and economic processability. However, the low ionic conductivity, limited electrochemical stability, and flammability of PEO have restricted its large-scale application. This work reports the synthesis of multifunctional flame-retardant microspheres (HCCP-THEIC, HT) using hexachlorocyclotriphosphazene (HCCP) and 1,3,5-tris(2-hydroxyethyl) isocyanurate (THEIC), and subsequently incorporation into PEO. It has been demonstrated that the crystallinity of PEO is reduced under the synergistic effect of physical hindrance from HT and the weak intermolecular hydrogen-bond interactions between HT and PEO. This promotes the dissociation of lithium salts, leading to an increase in the mobility and concentration of free Li + , thereby expanding the electrochemical window to 4.7 V. More importantly, HT stabilizes the electrode-electrolyte interface, promotes the formation of stabilized constituents in both the SEI (solid electrolyte interphase) and CEI (cathode electrolyte interphase) layers, and effectively suppresses lithium dendrites growth. The LiNi₀.₈Mn₀.₁Co₀.₁O₂ (NCM811)//Li cell retains 77.4 % of its capacity after 100 cycles at 4.3 V and 0.5C. Additionally, HT enhances fire safety through free radical scavenging and condensed-phase carbonization, reducing the heat release of pouch batteries by approximately 10 %. This simple and scalable HT synthesis offers a promising approach for producing safe, high-performance, and stable all-solid-state lithium metal batteries.

CAS / MDL: 839-90-7
研究领域: 电化学 · 材料科学 · 能源存储 · 高分子化学 · 界面化学 · 电池技术
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ACS Nano · 2025 · IF 16

Regulating Interfacial Nucleophilic Chemistry via Hybrid Electrolyte Enables Stable 4.8 V-Class Li-Rich||Li-Metal Batteries

Chenyang Jiao,Qizheng Zheng,Kang Zhang,Jiyuan Xue,Na Liu,Baodan Zhang,Yueli Lin,Xuequan Zhu,Changhao Wang,Hong-Gang Liao,Chong-Heng Shen,Yeguo Zou,Yu Qiao,Shi-Gang Sun

High-energy-density Li-rich layered oxide-based Li-metal batteries depend critically on the unique anionic redox. However, severe electrolyte decomposition and interfacial structural degradation hinder the longevity and stability of Li-rich||Li-metal batteries. Here, we show that a rational hybrid electrolyte design strategy can regulate interfacial chemistry through precise manipulation of cathode surface-exposed nucleophilic species. As a proof of concept, ethyl methyl sulfone is employed as the primary solvent due to its oxidative stability and resistance to nucleophilic attack, simultaneously strategically fabricating a fluorinated ether as a cosolvent that directs nucleophilic reaction toward its targeted functionality. Furthermore, this hybrid electrolyte design simultaneously facilitates the formation of a LiF-rich cathode electrolyte interphase (CEI) and reorganizes the solid electrolyte interphase on the Li metal from the preferential decomposition of cosolvents and anions. As a result, ultrahigh Coulombic efficiency (CE) (>99.4%) for Li-rich cathodes and enhanced Li-metal plating/stripping reversibility are achieved. Consequently, the optimized electrolyte demonstrates exceptional cycling stability, retaining 92% capacity over 100 cycles with ultrahigh average CE (>99.3%) under demanding conditions (limited Li supply, N/P = 2). Remarkably, this hybrid electrolyte enabled superior operation with anode-free cell architectures and enabled extreme temperatures (−30 to 55 °C) cycling. By effectively transforming detrimental nucleophilic attack into interfacial enhancement, this work establishes a new paradigm for electrolyte design in utilizing anionic redox chemistry.

CAS / MDL: 1318-02-1
研究领域: 电化学 · 能源材料 · 固态离子学 · 电池技术 · 界面科学 · 材料化学
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