Advanced Energy Materials
·
2022
·Vol. 13
·期 3
·2203703
·
IF 29.698
Wei He,Niaz Ahmad,Shaorui Sun,Xiao Zhang,Leguan Ran,Ruiwen Shao,Xuefeng Wang,Wen Yang
To implement the growing requirement for higher energy density all-solid-state lithium batteries (ASSLBs), further increasing the working voltage of LiCoO 2 (LCO) is a key to breaking through the bottleneck. However, LiCoO 2 severe structural degradation and side reactions at the cathode interface obstruct the development of high-voltage sulfide-based ASSLBs (≥4.5 V). Herein, a nano-metric Li 1.175 Nb 0.645 Ti 0.4 O 3 (LNTO) coated LCO cathode where microscopic Ti and Nb segregation at the interface during cycling potentially stabilizes the cathode lattice, and minimizes side reactions, simultaneously, is designed. Advanced transmission electron microscopy reveals that the stable spinel phase minimizes the micro stress at the cathode interface, avoids structure fragmentation, and hence significantly enhances the long-term cyclic stability of LNTO@LCO @ 4.5 V. Moreover, the differential phase contrast scanning transmission electron microscopy (DPC-STEM) visualizes the nano-interlayer LNTO to boost Li + migration at the cathode interface. Electrochemical impedance spectroscopy (EIS) reveals that sulfide-based cells with the LNTO nano-layer effectively reduce the interfacial resistance to 140 Ω compared to LiNbO 3 (235 Ω) over 100 cycles. Therefore, 4.5 V sulfide-based ASSLBs offer gratifying long-cycle stability (0.5 C for 1000 cycles, 88.6%), better specific capacity, and rate performance (179.8 mAh g –1 at 0.1 C, 97 mAh g –1 at 2 C).
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xue Ye,Jianneng Liang,Jiangtao Hu,Dazhuan Wu,Yongliang Li,Xiaoping Ouyang,Qianling Zhang,Xiangzhong Ren,Jianhong Liu
To achieve safe and high energy density solid-state batteries (SSBs), the weight of solid-state electrolyte (SSE) should be minimized and a high voltage and high specific capacity cathode should be used. Polyethylene oxide (PEO)-based polymer electrolytes (PEs) has been identified as the optimal SSE for SSBs owing to their versatile advantages. However, fabricating ultra-thin and high voltage stable PEO-based PEs is still challenging. Herein, an ultra-thin (8.1 µm) blending polymer electrolyte (BPE) is designed through blending PEO, Polymethyl methacrylate (PMMA) and Poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP), and complexing with Succinonitrile (SN), Fluoroethylene carbonate (FEC) and LiTFSI plasticizers. Based on this design, Li|BPE|LiFePO 4 quasi-solid-state battery (QSSB) can operate for 250 cycles with a capacity retention of 92.8%, 4.5 V high voltage Li|BPE|LiCoO 2 QSSB exhibits 87% capacity retention after 80 cycles, with an average Coulombic efficiency ≥99.8%, which is much superior than 4.5 V Li|PEO|LiCoO 2 SSB, whose capacity rapidly decays to 0 mAh/g after a dezen of cycles. DFT calculation suggests that blending PEO, PMMA and PVDF-HFP increase the electrochemical oxidation tolerance. Interface study by TEM and XPS discloses PEO-LiTFSI/LiCoO 2 interface is unstable with a big amount of decomposed products from PEO-LiTFSI and from LiCoO 2 , while BPE/LiCoO 2 interface is more stable without obvious decomposition, indicating the promising application of BPE for high energy density QSSBs.
研究领域:
材料科学
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电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Cheng Chen,Jiali Guo,Chunlei Wu,Xianjian Duan,Lingzhi Zhang
Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) is considered the most prominent cathode material to establish a practical high energy density of lithium-ion batteries (LIBs) for future electric vehicles. The energy density of LIBs is greatly determined by the capacity of electrode materials and the operating voltage of the cells. To further improve the cycle lifespan of NCM811 batteries to meet the requirement of driving range for the electric vehicle market, it is vital to design a novel electrolyte additive that can enhance the stability of the cathode/electrolyte interface at a wide range of voltage. Herein, a novel borate functionalized disiloxane compound, 1,1,1,3,3-pentamethyl-3-(3-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)propyl) disiloxane (PMBPDS), is synthesized as cathode electrolyte interphase (CEI) film-forming additive to improve the cycling performance of NCM811 batteries. Systematic studies reveal that PMBPDS can construct a stable CEI film on the NCM811 surface and efficiently scavenge hydrofluoric acid (HF). The PMBPDS-derived CEI prevents the dissolution of transmission metals in the NCM811 cathode and enhances the capacity retention of NCM811/graphite cells from 68.3 to 70.6% after 200 cycles at 1 C in the voltage window of 3–4.5 V. This work provides more understanding on designing the molecular structure of additive compounds for improving the electrochemical performance of LIBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Min Li,Said Amzil,Cancan Peng,Xuan Ting Wu,Junwei Feng,Xingchen Liu,Jie Gao,Peter Müller-Buschbaum,Ya-Jun Cheng,Yonggao Xia
Lithium cobalt oxide (LCO) remains the predominant cathode for consumer electronics, owing to its superior volumetric energy density and theoretical capacity. However, extending its operating voltage beyond 4.5 V triggers aggressive electrolyte decomposition, leading to structural deterioration and rapid performance decay. To address this challenge, we propose a functionalized polyester-diacrylate-polydimethylsiloxane (PAPDMS) as a slurry additive, forming a protective layer. This layer plays a crucial role in improving electronic conductivity, enhancing mechanical flexibility, and facilitating electrolyte uptake of LCO. In particular, this protective layer not only modulates the solvation structure, thereby promoting the formation of an inorganic-rich CEI, but also effectively suppresses the dissolution of transition metals. The dual-effect synergy of the PAPDMS layer on both the electrode and electrolyte significantly enhances LCO stability at 4.5 V. Compared with the original LCO, the modified LCO shows an increase in capacity retention rate from 62.3% to 85.2% after 200 cycles at 4.5 V. Moreover, in a practical graphite||LCO pouch cell, the PAPDMS-modified LCO demonstrates superior long-term stability with 78.2% capacity retention after 500 cycles, dramatically outperforming pristine LCO electrodes (46.8%). This strategy presents a scalable approach to stabilizing high-voltage LCO in next-generation lithium-ion batteries.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 19
·2212150
·
IF 19
Zhongsheng Wang,Chunlei Zhu,Jiandong Liu,Xinhong Hu,Yulu Yang,Shihan Qi,Huaping Wang,Daxiong Wu,Junda Huang,Pengbin He,Jianmin Ma
Tailoring inorganic components of cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) is critical to improving the cycling performance of lithium metal batteries. However, it is challenging due to complicated electrolyte reactions on cathode/anode surfaces. Herein, the species and inorganic component content of the CEI/SEI is enriched with an objectively gradient distribution through employing pentafluorophenyl 4-nitrobenzenesulfonate (PFBNBS) as electrolyte additive guided by engineering bond order with functional groups. In addition, a catalytic effect of LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NCM622) cathode is proposed on the decomposition of PFBNBS. PFBNBS with lower highest occupied molecular orbital can be preferentially oxidized on the NCM622 surface with the help of the catalytic effect to induce an inorganic-rich CEI for superior electrochemical performance at high voltage. Moreover, PFBNBS can be reduced on the Li surface due to its lower lowest unoccupied molecular orbital , increasing inorganic moieties in SEI for inhibiting Li dendrite generation. Thus, 4.5 V Li||NCM622 batteries with such electrolyte can retain 70.4% of initial capacity after 500 cycles at 0.2 C, which is attributed to the protective effect of the excellent CEI on NCM622 and the inhibitory effect of its derived CEI/SEI on continuous electrolyte decomposition.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2013
·
IF 3.777
Qin Hao,Caixia Xu,Suzhen Jia,Xiaoyun Zhao
Fe 2 O 3 nanoparticles are employed as a coating material to optimize the electrochemical performance of LiCoO 2 at high voltage. When the current rate is 1 C with the cutoff potential at 4.5 V, the 5 wt.% Fe 2 O 3 -coated LiCoO 2 delivers an initial capacity of 168.7 mAh g −1 . More importantly, its capacity retention after 50 cycles reaches up to 92.6%, whereas the value for pristine LiCoO 2 is only 58.5%. The electrochemistry impedance spectroscopy analysis demonstrates that Fe 2 O 3 coating plays an important role in decreasing the charge transfer resistance of cell. Compared with the performance of the Fe 2 O 3 -mixed and Fe-doped LiCoO 2 samples, it is found that the role of Fe 2 O 3 coating is unique, which may change the characteristic of the surface of LiCoO 2 particles. This technique may provide an effective and convenient way for optimizing other electrode materials .
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Fang Fu,Jianfei Lin,Shiyuan Zhang,Ying Liu,Tianzong Ma,Ruonan Jing,Liqun Sun,Haiming Xie
The inadequate room-temperature ionic conductivity and unstable electrode-electrolyte interfaces have encumbered the widespread adoption of high-voltage solid-state Li metal batteries (SSLMBs). Here, we report a molecularly engineered polymer electrolyte synthesized by grafting poly(ethylene glycol) diacrylate (PEGDA) and 2,2,2-trifluoroethyl methacrylate (TFEMA) onto a tri(2-hydroxyethyl) isocyanurate triacrylate (THEICTA) framework, coupled with interface engineering strategies. The hierarchical coordination competition within the polymer matrix facilitates rapid Li⁺ transport, achieving an ionic conductivity of 0.95 mS cm⁻¹ at room temperature. Advanced characterization techniques including X-ray photoelectron spectroscopy (XPS), in situ X-ray diffraction (XRD), and high-resolution transmission electron microscopy (HRTEM) reveal the formation of a robust, nitrided and boronized cathode electrolyte interphase (CEI) on LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622), effectively suppressing oxidative decomposition and mitigating structural degradation at high voltages (≥4.5 V). As a result, the Li||NCM622 cell delivers a high initial discharge capacity of 188.6 mAh g⁻¹ with 70.4 % capacity retention after 700 cycles. Furthermore, a Li metal pouch cell featuring an energy density of 456 Wh kg⁻¹ demonstrates excellent cycling stability, maintaining a capacity retention rate of 87.8 % after 130 cycles. This study provides a scalable molecular design strategy for polymer electrolytes, advancing the development of high-voltage SSLMBs for next-generation energy storage.
研究领域:
材料科学
·
电化学
·
储能技术
·
聚合物化学
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电池技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chong Ni,Zhen Li,Kai Wang,Yongchao Liu,Yuanyun Dou,Wentao Wu,Hongyu Wang,Yu Yao,Hongfa Xiang,Xuyong Feng
Surface modification is a highly effective strategy to suppress side reactions between electrode materials and electrolytes. The preparation of coated electrode materials generally involves two steps: the synthesis of electrode materials and subsequent surface coating, which is a long and costly process. Here, we report a novel solid-state reaction method to prepare Li 2 ZrO 3 -coated LiCoO 2 in a single step. By controlling the cooling rate, the solid solubility of Zr in LiCoO 2 decreases, resulting in the precipitation of Zr 4+ on the surface and the formation of a Li 2 ZrO 3 coating layer. X-ray photoelectron spectroscopy, combined with a focused ion beam and high-resolution transmission electron microscopy, confirms the uniform Li 2 ZrO 3 coating on the surface of LiCoO 2 . Electrochemical performance testing shows that Li 2 ZrO 3 -coated LiCoO 2 exhibits enhanced cycle stability, even when charged to 4.5 V. After cycling at 1C for 200 cycles, Li 2 ZrO 3 -coated LiCoO 2 maintains a capacity of about 180 mAh g −1 , which is 94 % of the initial 193 mAh g −1 .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Leshuai Qiao,Yang Chen,Xuanxuan Zhang,Xiangxin Cheng,Wanfu Liang,Yuyu Li,Jingchao Chai,Ming Xie,Dianbo Ruan,Zhihong Liu
Water-based binders in lithium-ion batteries have garnered increasing attention owing to their environmental benignity and cost effectiveness. In this research, a waterborne poly(lithium acrylate-co-acrylonitrile) copolymer, P(LiAA-AN), was prepared and utilized as a high-performance binder for 4.5 V LiCoO2 in a lithium-ion battery. This copolymer binder integrates characteristics of both polyacrylic lithium and polyacrylonitrile. It has the ability to compensate for additional Li ions and engage in the formation of a stable cathode solid electrolyte interface (CEI) on the surface of 4.5 V LiCoO2. Consequently, in comparison with poly(vinylidene fluoride) (PVDF) and LiPAA binders, the water-based P(LiAA-AN) binder leads the 4.5 V LCO/Li battery to superior rate performance and high cycle stability. When the cell was cycled under a current density of 0.5 C (1 C = 185 mAh g–1) and a cutoff voltage of 3.0–4.5 V (vs Li+/Li), a high capacity retention ratio of 91.5% was achieved after 200 cycles. In addition, the P(LiAA-AN) binder demonstrates an excellent electrolyte absorption and a reduced charge transfer impedance. These results substantiate the effectiveness of the P(LiAA-AN) water-based binder in enhancing the electrochemical performance of the high-voltage LiCoO2 cathode.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2015
·Vol. 41
·期 5
·7133-7139
·
IF 2.605
Rui Du,Yujing Bi,Wenchao Yang,Zhe Peng,Meng Liu,Yang Liu,Baoming Wu,Bangcheng Yang,Fei Ding,Deyu Wang
To improve the cyclic stability of LiNi 0.8 Co 0.1 Mn 0.1 O 2 cycled between 2.8 and 4.5 V vs. Li/Li + , titanium was incorporated into LiNi 0.8 Co 0.1 Mn 0.1 O 2 at various molar concentrations of 1, 2, 3 and 5% during the synthesis. The XRD , EDS and XPS analyses indicated that the titanium ions were effectively incorporated into the lattice of ternary oxides by occupying the transitional metal positions. Among the investigated molar concentrations, 2% Ti-substituted LiNi 0.8 Co 0.1 Mn 0.1 O 2 exhibited the best multifaceted performances with a relatively high capacity (205.7 mA h g −1 at 0.1 C), good rate capability (178.2 mA h g −1 at 1 C, 155.3 mA h g −1 at 5 C) and acceptable cyclic stability (86.9% at the 200th). The post-mortem analysis indicated that Ti substitution alleviates cracking from secondary particles to primary ones. This behavior is most likely due to the decreased ratio of volumetric deformation ( i.e. , 4.82% for the 2% Ti-substituted sample, which is 19.8% lower than that of the pristine one). Our results demonstrate that mechanical properties may play a crucial role in its long cyclability for use as a high-capacity ternary cathode.
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Zhengping Ding,Ran Song,Yu Shen,Huahui Lin,Peng Wei,Xiangqun Zhuge,Ke Qu,Zhenzhong Yang,Yurong Ren
Combining a high cut-off voltage cathode with a high specific-capacity lithium metal anode offers a promising path toward ultra-high-energy-density batteries (> 400 Wh kg -1 ). However, the practical application of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)||Li batteries with a 4.5 V cut-off voltage is challenged by severe interface deterioration. This study introduces a novel bifunctional electrolyte additive called 2,2,2-Trifluoroethyl Nonafluorobutanesulfonate (TNS), designed to form a thin, robust electrolyte interface layer on both cathode and anode surfaces. Detailed analysis reveals that TNS decomposes and modifies the solid-electrolyte-interface layer. Through the synergistic effects of fluoride and sulfonate functional groups, the resulting cathode-electrolyte-interface (CEI) enhances the structural stability of NCM811 while providing a high-efficiency lithium-ion transport channel to accelerate Li + insertion and extraction. At a cut-off voltage of 4.5 V, NCM811||Li batteries with 1 % TNS (by weight) exhibit high discharge capacity retention of 74.2 % after 150 cycles at a 1C rate and 60.1 % after 150 cycles at a 2C rate. This study offers valuable insights for designing high-voltage electrolyte additives in ultra-high-energy-density lithium metal batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Yang Chen,Shujian Liu,Shaokai Cheng,Shuyu Gao,Jingchao Chai,Qiuyue Jiang,Zhihong Liu,Xueqing Liu,Jiyan Liu,Ming Xie,Wubin Dai
The polyvinylidene fluoride (PVdF) binder is the classic binder for cathodes because of its excellent electrochemical stability and superior adhesion property. However, PVdF is very expensive and sensitive to moisture. Therefore, pursuit of a cost-effective binder is highly desirable, especially for high-voltage cathode application. Polyacrylonitrile (PAN) possesses strong polar C≡N groups, endowing it with oxidation resistance and strong binding properties. Herein, the PAN binder was systematically investigated for the electrochemical performance of the 4.5 V high-voltage LiCoO2 (HV-LCO) electrode. The results showed that the HV-LCO-PAN electrode delivered superior rate capability and cycling stability to the corresponding HV-LCO-PVdF. The PAN binder was highly tolerant of moisture and was capable of forming uniform coating on the cathode materials. Moreover, the PAN binder had ultrahigh mechanical modulus (8.01 GPa) and hardness (381.45 MPa) in a liquid electrolyte, thereby improving cycling stability and rate capability. X-ray photoelectron spectroscopy analysis further demonstrated that PAN formed uniform coating on the surface of LiCoO2 and played a role of an artificial cathode–electrolyte interphase layer, suppressing decomposition of the liquid electrolyte under high cutoff voltage.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 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）