ACS Nano
·
2025
·
IF 16
Muhammad Imran,Zhongsheng Dai,Fiaz Hussain,Renjie Chen,Feng Wu,Li Li
Applying higher operating voltage (≥4.6 V) to elevate the energy density of LiCoO2 (LCO) is essential for achieving high-energy lithium-ion batteries (LIBs). However, a higher working voltage would induce lattice oxygen release, resulting in the surface structure transition from the initial layered to a disordered phase. Furthermore, direct contact between the electrolyte and LCO material could lead to serious surface side reactions, resulting in severely enhanced interfacial resistance. Herein, by regulating the annealing temperature, we first introduced La2Mo2O9 (LMO) with sufficient oxygen vacancies (41%) to engineer the LCO surface. Specially, the La and Mo ions with high bonding energy with oxygen could form robust La–O and Mo–O bonds with LCO surface oxygen, acting as an “oxygen anchor” to stabilize the oxygen. Furthermore, the abundant oxygen vacancies in the LMO buffer could in situ capture and reserve the possible released oxygen from bulk LCO. Therefore, the reaction involving oxygen species with the electrolyte is effectively mitigated, thus validly alleviating the structure degradation and elevating the electrochemical performance, enabling the half-cell to showcase 86.2% capacity retention after 100 cycles under 4.6 V and 1C, and a full cell could also achieve excellent capacity retention (90%) after 450 cycles.
研究领域:
材料科学
·
电化学
·
储能
·
锂离子电池
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产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 32
·2405519
·
IF 27.4
Weiyuan Huang,Jianyuan Li,Qinghe Zhao,Shunning Li,Mingyuan Ge,Jianjun Fang,Zhefeng Chen,Lei Yu,Xiaozhou Huang,Wenguang Zhao,Xiaojing Huang,Guoxi Ren,Nian Zhang,Lunhua He,Jianguo Wen,Wanli Yang,Mingjian Zhang,Tongchao Liu,Khalil Amine,Feng Pan
Pushing intercalation-type cathode materials to their theoretical capacity often suffers from fragile Li-deficient frameworks and severe lattice strain, leading to mechanical failure issues within the crystal structure and fast capacity fading. This is particularly pronounced in layered oxide cathodes because the intrinsic nature of their structures is susceptible to structural degradation with excessive Li extraction, which remains unsolved yet despite attempts involving elemental doping and surface coating strategies. Herein, a mechanochemical strengthening strategy is developed through a gradient disordering structure to address these challenges and push the LiCoO 2 (LCO) layered cathode approaching the capacity limit (256 mAh g −1 , up to 93% of Li utilization). This innovative approach also demonstrates exceptional cyclability and rate capability, as validated in practical Ah-level pouch full cells, surpassing the current performance benchmarks. Comprehensive characterizations with multiscale X-ray, electron diffraction, and imaging techniques unveil that the gradient disordering structure notably diminishes the anisotropic lattice strain and exhibits high fatigue resistance, even under extreme delithiation states and harsh operating voltages. Consequently, this designed LCO cathode impedes the growth and propagation of particle cracks, and mitigates irreversible phase transitions. This work sheds light on promising directions toward next-generation high-energy-density battery materials through structural chemistry design.
研究领域:
材料科学
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电化学
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能源存储
·
结构化学
·
电池技术
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DOI
高影响因子
MATERIALS LETTERS
·
2021
·
IF 3.423
Hong Guo,Fei Shen,Weichang Guo,Dingyuan Zeng,Yuting Yin,Xiaogang Han
All-solid-state batteries with garnet-type solid electrolytes are expected to achieve high safety. However, poor contact between the cathode and the solid-state electrolyte remains a bottleneck in improving electrochemical performance. We propose an interface modification strategy by adopting nano γ-Al 2 O 3 as a co-sintering additive to address the interfacial issue. The Li|Li 6.75 La 3 Zr 1.75 Nb 0.25 O 12 |LiCoO 2 all-solid-state battery exhibits promoted capacities due to intimate interfacial contact between the cathode and the electrolyte after modification. This work provides a low-cost and convenient strategy to overcome the interfacial issue in all-solid-state batteries.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Xiaoye Liu,Xiangkun Kong,Wenyi Xiang,Yining Jiang,Bingqinq Xiong,Weiwei Ping,Changrong Xia,Daoming Huan,Chengwei Wang
Garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) has high ionic conductivity and good compatibility with lithium metal. High-temperature processing has been proven an effective method to decrease the interface resistance of cathode|LLZO. However, its application is still hindered by the interlayer co-diffusion with the cathode and high sintering temperature (>1200 °C). In this work, a new garnet-type composite solid-state electrolyte (SSE) Li 6.54 La 2.96 Ba 0.04 Zr 1.5 Nb 0.5 O 12 -LiCoO 2 (LLBZNO-LCO) is firstly proposed to improve the chemical stability and electrochemical properties of garnet with high-temperature processing. Small doses of LCO (3%) can significantly decrease the LCO|SSE interface resistance from 121.2 to 10.1 Ω cm 2 , while the sintering temperature of garnet-type LLBZNO decreases from 1230 to 1000 °C. The all-solid-state battery based on the sintered LLBZNO-LCO SSE exhibits excellent cycling stability. Our approach achieves an enhanced LCO|SSE interface and an improved sintering activity of garnet SSE, which provides a new strategy for optimizing the comprehensive performance of garnet SSE.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Zhe Gao,Zhuoxi Wu,Yangyang Liu,Mohamed H. Helal,Ahmad Aljabr,Zeinhom M. El-Bahy,Junwei Han,Jiang Zhou
Sustainable battery recycling increasingly requires approaches that can restore electrochemical performance rather than simply recover individual elements. In this work, a regeneration strategy is developed for degraded LiCoO 2 (D-LCO) cathodes by utilizing lithium (Li) vacancies formed during long-term cycling as effective sites for structural modification. By taking advantage of these defects in degraded LiCoO 2 , a small amount of lanthanum (La) is incorporated into the layered lattice through a short thermal regeneration process, leading to simultaneous improvements in both structure and kinetics. Expansion of the c -axis spacing stabilizes the layered framework by suppressing Li/Co cation mixing and mitigating irreversible phase transitions during cycling. At the same time, the widened interlayer pathways facilitate Li + transport and reduce charge-transfer resistance. Together, these effects account for the enhanced electrochemical behavior of the regenerated cathode. As a result, the regenerated LiCoO 2 (R-LCO) delivers a reversible capacity of 145.35 mA h g −1 and retains 82.64% of its initial capacity after 500 cycles, exceeding the performance of commercial LiCoO 2 under identical conditions. This study demonstrates a practical route for regenerating layered cathode materials with improved functionality and provides a viable direction for high-value battery recycling. This work achieves direct upcycling of degraded LiCoO 2 cathodes via utilizing lithium (Li) vacancies formed during long-term cycling as effective sites for structural modification and provides a promising pathway for high-value battery recycling. Download: Download high-res image (185KB) Download: Download full-size image
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shiyou Wu,Tongxing Lei,Zhiyu Ding,Jun Wei,Junwei Wu
Lithium cobalt oxide (LCO) cathode materials could deliver about 220 mAh/g when operated at 4.6 V. However, high-voltage LCO materials still endure detrimental interfacial side reactions and serious structural degradation, leading to severe performance deterioration. Herein, we have proposed a facile strategy that utilizes good-wettability LiPO 3 and ionically conductive Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) to successfully construct a highly stable Li 3 PO 4 layer and a well-matched transition layer (such as Co 2 TiO 4 and LiCoPO 4 ) on the surface of LCO material. The designed multifunctional coating can not only suppress the oxygen release and electrolyte decomposition but also facilitate Li + diffusion kinetics. As a result, the modified LCO exhibits superior cycling stability over 200 cycles at 4.6 V, with excellent capacity retentions of 79.24 % at room temperature and 79.45 % at high temperature of 45 ℃. Besides, the modified LCO realizes a reversible discharge capacity of 178.42 mAh/g at 3C (1C = 200 mA/g) over 300 cycles. This work provides a practical reference for mass-production of high-voltage LCO with long lifespan and high-rate capability.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Linjun Zhong,Ziqiang Fan,Zhe Wang,Xinyue Wu,Jingan Liu,Junjun Liu,Junyang Zheng,Qing Chen,Lidan Xing,Jianhui Li,Yu Ying,Ronghua Zeng
Almost all commercial lithium-ion batteries (LIBs) with LiCoO 2 (LCO) as cathode material are cycled from 3.0 to 4.2 V and their actual specific capacity just ranges from 140 to 160 mA h g −1 , which is much lower than the theoretical specific capacity of LCO of 274 mA h g −1 . To further improve the actual specific capacity of LCO, elevating the upper limit of its working voltage is necessary. However, as the upper limit of its working voltage is elevated to 4.5 V or higher, the LCO crystal will undergo severe irreversible phase transition, and the oxidization decomposition of electrolyte on the cathode’s surface will exacerbate, which will severely reduce the cycling lifespan of batteries, hindering the actual application of high voltage LCO. In this work, we find that 3,5-difluorophenylboronic acid pinacol ester (35-DAPE) is an effective cathode electrolyte interphase (CEI)-forming additive, which can form a robust and stable CEI layer rich in fluorophenyl-groups and B–F/B–O bonds on the surface of LCO cathode, inhibiting the dissolution of cobalt ions and maintain the structural stability of LCO crystal over cycles. The graphite||LCO pouch cells in a voltage range of 3.0–4.5 V with 35-DAPE display a capacity retention rate of 91.1% after 150 cycles at room temperature, compared to that of 2.4% in baseline electrolyte. Besides, rate performance at room temperature and discharging performance at low temperatures of graphite||LCO pouch cells can also be observed with an improvement after the introduction of 35-DAPE. In addition, this work has explained the decomposition mechanism of 35-DAPE and how its products improve the electrochemical performance of graphite||LCO pouch cells in detail, which not only advances the actual application of fluorophenylboronic acid pinacol ester additive in high voltage LIBs but also provides valuable insights for the design of functional electrolyte additives.
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DOI
高影响因子
Magnetic Resonance Letters
·
2022
·Vol. 3
·期 1
·61-66
·
IF 0
Bei Hu,Fushan Geng,Ming Shen,Bingwen Hu
Dual-mode electron paramagnetic resonance (EPR) spectroscopy was employed to analyze redox mechanisms in lithium cobalt oxide LiCoO 2 (LCO) cathode material during delithiation and lithiation. It was found that the O3-II could not fully convert back to the pristine O3–I phase while oxygen vacancies quickly generate and accumulate during the cycling. Our study paves the way for better understanding the doping effects of different elements on LiCoO 2 in the future.
研究领域:
材料科学
·
电化学
·
储能
·
光谱学
✓ 已验证
DOI
ACS Nano
·
2025
·
IF 16
Yuhao Du,Wenguang Zhao,Zijian Li,Hengyu Ren,Haocong Yi,Shengyu Wu,Jun Wang,Feng Pan,Qinghe Zhao
The applied cathodes in lithium-ion batteries usually suffer from severe structural degradation upon fast charging, and the correlated mechanism still remains vague. Here, we reveal the surface structural evolution of LiCoO2 (LCO) during cycling at 4.6 V vs Li/Li+ with an extreme high fast-charging current of 10 C. Fast charging induces surface heterogeneous delithiation, promoting nonuniform surface phase transitions and resulting in the formation of a triphase hybrid on the charged surface. The triphase hybrid consists of the layered, spinel, and rock-salt (RS) phases. As cycling proceeds, this triphase hybrid propagates gradually toward the bulk, accompanied by a progressive thickening of the surface RS phase, leading to deteriorated Li+ transport kinetics and accelerated capacity fading. Thus, suppressing the heterogeneous Li+ delithiation of LCO is crucial for enhancing fast-charging durability. By applying a uniform and robust surface coating, the surface delithiation homogeneity upon extreme fast charging is significantly improved, and the thickening of the surface Li+-blocking RS phase is greatly reduced, thereby achieving enhanced cycling stability of LCO. This work benefits the development of more advanced LCO cathodes tailored for fast-charging applications.
研究领域:
材料科学
·
电化学
·
储能
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2016
·
IF 4.803
Bihe Wu,Jing Wang,Jiyang Li,Weiqing Lin,Huining Hu,Feng Wang,Shiyong Zhao,Chaolun Gan,Jinbao Zhao
In this work, morphology-controlled lithium cobalt oxides (LCO) were obtained by a simple two-step method that involves a Co 3 O 4 synthetic process, in which cubic and spherical Co 3 O 4 were prepared by a hydrothermal method and a subsequent lithiation process with Li 2 CO 3 . The structures and morphologies of two materials were investigated by XRD, SEM and TEM. In contrast with the LCO prepared by using commercial Co 3 O 4 precursor, the cubic and spherical LCO materials have an excellent performance in cyclic stability and rate capacity which is attributed to the better fluidity and less agglomeration with specific morphology of LCO materials.
研究领域:
材料科学
·
电化学
·
储能
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Jun Cheng,Wenjie Lin,Jingrong Hou,Yaqi Liao,Yunhui Huang
As the classic cathode material, lithium cobalt oxide (LiCoO2, LCO) suffers from severe structural and interfacial degradation at voltage >4.5 V, which induces fast capacity decay of the cells. Herein, we adopt a simple and effective method, doping aluminum (Al) cations in precursors, to improve the structural stability of LCO and systematically investigate the effect of Al doping on the electrochemical performances. Doping in precursors rather than bulk particles is beneficial to realize uniform Al ions distribution. Even at 4.5 V charging voltage, the LCO/graphite pouch cells with high Al doping levels (8500 ppm) deliver initial and reversible discharge capacities of 386 and 369 mAh after 500 cycles, respectively. The capacity retention is as high as 95.5%. When the cutoff voltage reaches 4.55 V, the pouch cell maintains 79.0% of the first-cycle discharge capacity after 500 cycles. With optimized electrolyte, the pouch cell realizes 87.3% of the initial discharge capacity after 500 cycles at 45 °C. Moreover, the thermal safety performance of the pouch cells with Al doping is promising. Our work displays an excellent inspiration for developing high-voltage, long-cycle, and safe LCO cathode for commercial lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Qiaoyi Yan,Zhengzheng Liu,Feng Wu,Renjie Chen,Li Li
Sustainable recycling of degraded LiCoO 2 (LCO) cathode is critical for minimizing the environmental footprint of lithium-ion batteries. Herein, we propose an upcycling method that converts degraded LCO into high-voltage cathodes by constructing a compositional and structural dual-gradient structure, guided by the effective ionic potential (EIP, Φ* ), a descriptor for foreign dopant diffusivity in degraded LCO lattices. Specifically, low- Φ* dopants tend to exhibit high bulk diffusivity, whereas high- Φ* dopants are retained near the surface, which promotes the formation of the compositional gradient and leads to a structural transition in LCO from a fully disordered, dense surface to an ordered layered structure in the bulk. This structure endows the upcycled cathode with a stabilized surface and low-strain bulk structure, enabling its superior electrochemical performance over the commercial counterpart at cut-off potentials of 4.6 and 4.65 V. Comprehensive kinetic and thermodynamic analyses reveal the critical role of vacancies in spent LCO for this structural engineering: Bulk vacancies facilitate the formation of deeper dopant concentration gradients within particles, while vacancies near the surface promote the development of a continuous and dense surface disordered structure. Multiscale characterizations and theoretical calculations elucidate the relationship between the engineered structure and the electrochemical stability of the upcycled cathode.
研究领域:
材料科学
·
电化学
·
可持续能源
·
电池回收
·
固态化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）