ACS Applied Energy Materials
·
2021
·
IF 6.024
Kaibin Fang,Qian Xie,Chengyun Wang,Xiulian Qiu,Yali Wang,Wei Yang,Xin-wei Yu
LiNi0.8Co0.15Al0.05O2 (LNCA) cathode materials have an extremely high energy density, which can greatly enhance the driving range of pure electric vehicles if they are used in on-board batteries. However, the development of the LNCA cathode material is restricted by the expensive transition metal cobalt (Co). Therefore, researchers are devoted to finding other metals to replace Co to synthesize nickel (Ni)-rich Co-free materials to reduce the cost. To investigate the feasibility of replacing Co with manganese (Mn) as a transition metal, this paper reports the synthesis and compares the properties of four Ni-rich materials with different Co–Mn contents by gradually adding Mn to LNCA materials and reducing the Co content in equal amounts using an oxalic acid coprecipitation method. The results show that Mn can compensate the effect of Co deficiency to a certain extent; it is feasible to use Mn to completely replace Co in the synthesis of Ni-rich ternary Co-free materials under the premise of sacrificing a certain initial specific capacity. The tetrameric material LiNi0.8Co0.1Mn0.05Al0.05O2 substituted with trace amounts of Mn exhibited the most excellent electrochemical properties among the four synthesized materials. Therefore, to synthesize satisfactory Ni-rich Co-free materials, it is suggested to develop and synthesize quaternary Co-free materials on the basis of LiNi0.8Co0.1Mn0.05Al0.05O2.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Qi Liu,Zhenqian Wu,Jingying Sun,Ruimei Xu,Xianwei Li,Xiao Yu,Yong Liu
Co-free, Ni-rich cathode materials have aroused enormous attentions for the low cost, sustainable development of lithium-ion batteries. However, it is not easy to fabricate single-crystalline Ni-rich cathode materials from the hierarchical structured precursors via coprecipitation method. Furthermore, it is difficult to introduce Al dopant during the coprecipitation process to obtain high quality Ni-rich cathode material owing to the rapid sediment of Al 3+ . Herein, we developed a one-step stirring-assisted cation chelation and reassembly route for fabricating crack-free single-crystalline, Al-doped Co-free Ni-rich cathode material. The fabricated LiNi 0.8 Mn 0.16 Al 0.04 O 2 shows a high capacity of 204 mAh g −1 at 0.1C, excellent rate capability (143 mAh g −1 at 10C), and good cycling stability (an initial specific capacity of 178 mAh g −1 with capacity retention of 82.2% at 1C over 200 cycles). Furthermore, when tested at a raised temperature of 55 °C, it exhibited an initial capacity of 194.7 mAh g −1 with capacity retention of 82.1% at 1C over 100 cycles. The outstanding electrochemical performance can be ascribed to the synergistic effect of single crystalline structure and successful doping of Al element in the cathode, which enable fast ion and electron transport , suppress Li/Ni mixing and maintain the structural stability.
研究领域:
材料科学
·
电化学
·
能源存储技术
✓ 已验证
DOI
高影响因子
Nano Energy
·
2024
·
IF 16.8
Yu Tang,Zhiyong Huang,Wei Wang,Yali Wen,Shuoxiao Zhang,Xi Chen,Zhibo Zhang,Zijia Yin,Tingting Yang,Tianyi Li,Leighanne C. Gallington,He Zhu,Si Lan,Steven Wang,Yang Ren,Zhenduo Wu,Qi Liu
The sluggish Li-ion kinetics restrict the rapid charging capabilities and contribute to the structural deterioration of Ni-rich cathode materials . Notably, crack propagation during repeated charging cycles deteriorates the electrochemical stability, which hinders the further development of high-energy-density batteries for electric vehicles (EVs). In this paper, we proposed a simple yet effective method to enhance the Li-ion diffusion and mechanical properties of Ni-rich cathodes via straightforward Zr doping. In-situ high-rate XRD reveals that the detrimental uneven delithiation under the fast-charging process has been largely alleviated. Particularly, a robust structure with higher modulus and fracture strength is constructed owing to the higher Zr-O bond. By mitigating the kinetic hindrance and increasing the particle’s stiffness, the proposed Ni-rich cathode shows an impressive 97.6 % capacity retention under a 5 C rate current. This work provides a facile and efficient strategy for large-scale production of fast-charging Ni-rich cathode materials.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Shouyi Yin,Hongyi Chen,Jun Chen,Abouzar Massoudi,Wentao Deng,Xu Gao,Shu Zhang,Ying Wang,Tsung-Wu Lin,Craig E. Banks,Shi-zhang Qiao,Guoqiang Zou,Hongshuai Hou,Xiaobo Ji
The implementation of Ni-rich cathodes with high energy density has been critically restrained by stress corrosion. Herein, crack-free LiNbO3-coated LiNi0.88Co0.10Mn0.02O2, as theoretically predicted, demonstrates highly reversible lithiation/delithiation. Mechanically, the phase transition (H1 → H2 → H3) is significantly alleviated by the excogitation of the interfacial force invoked by the LiNbO3 coating layer, as verified by X-ray absorption spectroscopy and extended X-ray absorption near-edge structure spectroscopy. Meanwhile, the stabilities of the crystal structure are remarkably strengthened by the strong Nb–O bond activated by Nb5+ doping that is confirmed by Rietveld refinement of X-ray diffraction and differential capacitance curves. Chemically, the interface shielding effect is conducive to protecting the electrode against electrolyte corrosion along with subsequent transition-metal dissolution, ultimately rendering a faster/highly convertible lithium-ion diffusion. Greatly, the excellent electrochemical properties (74% capacity retention after 300 cycles at 2 C within 2.5–4.3 V) and structural stability (the morphology remains intact after 500 cycles at 5 C within 2.5–4.3 V) are successfully achieved. Given this, this elaborate work might inaugurate a potential avenue for rationally tuning the structure/interface evolution toward Ni-rich materials.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Tong Gao,Shu-Yu Zhou,Pengpeng Dai,Jidong Song,Junhong Liao,Yuxuan Sun,Chenglong Yu,Shi-Xi Zhao,Guozhong Cao
Single-crystal Ni-rich ternary cathode materials (811), with their comprehensive advantage of high energy density and low manufacturing cost, have been considered the most promising materials for Li-ion batteries. Due to strong O-p/TM-d covalent hybridization, the complete oxidation of Ni ions during electrochemical cycling is often accompanied by inevitable oxygen loss, resulting in an irreversible surface phase transition, accumulated lattice stress, and poor thermal stability. Considering the fact that introducing heteroatoms into traditional doping systems can alter the electron density distribution around coordinated oxygen, compositionally complex systems based on high-entropy doping may have a more significant effect on stabilizing lattice oxygen. Herein, the high-entropy doping strategy was applied to design and synthesize single-crystal NCM811 cathodes (HE811) through the molten salt method. Compared to 811, HE811 cathodes show an excellent initial Coulombic efficiency of 90.74% at 0.2C and deliver a higher capacity retention of 80.79% after 300 cycles at 1C between 2.8 and 4.3 V. Owing to high-entropy doping, the oxygen electron densities around multidopants are increased, inhibiting the excessive oxidation of lattice oxygen and improving the stability of TMO6 coordination structures. This work could provide insights into the high-entropy doping effects in modulating oxygen charge distribution to design high-energy-density Ni-rich ternary cathode materials with long-term cycling.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
Small
·
2020
·Vol. 16
·期 13
·1906025
·
IF 11.459
Lecai Wang,Li Li,Hanyong Wang,Jingbo Yang,Yitian Ma,Jiawei Wu,Feng Wu,Renjie Chen
Ni-rich Li-ion cathode materials promise high energy density, but are limited in power density and cycle life, resulting from their poor dynamic characteristics and quick degradation. On the other hand, capacitor electrode materials promise high power density and long cycle life but limited capacities. A joint energy storage mechanism of these two kinds is performed in the material-compositional level in this paper. A valence coupling between carbon π-electrons and O 2− is identified in the as-prepared composite material, using a tracking X-ray photoelectron spectroscopy strategy. Besides delivering capacity simultaneously from its LiNi 0.8 Co 0.1 Mn 0.1 O 2 and capacitive carbon components with impressive amount and speed, this material shows robust cycling stability by preventing oxygen emission and phase transformation via the discovered valence coupling effect. Structural evolution of the composite shows a more flattened path compared to that of the pure LiNi 0.8 Co 0.1 Mn 0.1 O 2 , revealed by the in situ X-ray diffraction strategy. Without obvious phase transformation and losing active contents in this composite material, long cycling can be achieved.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Lifan Wang,Rui Wang,Jingyue Wang,Rui Xu,Xindong Wang,Chun Zhan
To satisfy the increasing energy density requirements for electric vehicles and grid-scale energy storage systems, Ni-rich layered oxide cathode materials are often fabricated as micron-sized secondary spherical particles consisting of nanosized single crystals. Unfortunately, the hierarchical structure inevitably induces intergranular cracks and parasitic reactions at the cathode–electrolyte interphase, aggravating chemomechanical instability and seriously hindering their practical application. Here, we propose a nanowelding strategy to build consolidation points at the grain boundary of the primary particles, which dramatically enhances the capacity retention and chemomechanical stability. Meanwhile, the oxygen vacancies in the ceria-based solid electrolyte possessing oxygen adsorbing and storage capability can restrain the active oxygenates in the surficial lattice to avoid oxygen evolution. Experimental characterization further confirms that this unique architecture can effectively prevent the liquid electrolyte from penetrating into the active material along the grain boundary and consequently eliminate the adverse effects, including intergranular cracks, cathode electrolyte interface formation and growth, and the layered structure-rock salt phase irreversible transition. This finding provides a promising approach to realize the rapid commercialization of highly stabilized nickel-rich cathode materials for high-performance lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储技术
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Haocheng Ji,Junxiong Wang,Haotian Qu,Junfeng Li,Wenhai Ji,Xiao Qiu,Yanfei Zhu,Hengyu Ren,Ruyu Shi,Guanjun Ji,Wenguang Zhao,Guangmin Zhou
Facing the resource and environmental pressures brought by the retiring wave of lithium-ion batteries (LIBs), direct recycling methods are considered to be the next generation's solution. However, the contradiction between limited battery life and the demand for rapidly iterating technology forces the direct recovery paradigm to shift toward “direct upcycling.” Herein, a closed-loop direct upcycling strategy that converts waste current collector debris into dopants is proposed, and a highly inclusive eutectic molten salt system is utilized to repair structural defects in degraded polycrystalline LiNi 0.83 Co 0.12 Mn 0.05 O 2 cathodes while achieving single-crystallization transformation and introducing Al/Cu dual-doping. Upcycled materials can effectively overcome the two key challenges at high voltages: strain accumulation and lattice oxygen evolution. It exhibits comprehensive electrochemical performance far superior to commercial materials at 4.6 V, especially its fast charging capability at 15 C, and an impressive 91.1% capacity retention after 200 cycles in a 1.2 Ah pouch cell. Importantly, this approach demonstrates broad applicability to various spent layered cathodes, particularly showcasing its value in the recycling of mixed spent cathodes. This work effectively bridges the gap between waste management and material performance enhancement, offering a sustainable path for the recycling of spent LIBs and the production of next-generation high-voltage cathodes.
研究领域:
材料科学
·
环境科学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chenxi Gao,Xiao Xu,Tiansheng Bai,Jun Cheng,Zhen Zeng,Hongqiang Zhang,Naixuan Ci,Wei Zhai,Qing Ma,Jingyu Lu,Jun Ma,Lijie Ci,Deping Li
Nickel-rich layered oxide with high reversible capacity and high working potentials is a prevailing cathode for high-energy-density all-solid-state lithium batteries (ASSLBs). However, compared to the liquid battery system, ASSLBs suffer from poor Li-ion migration kinetics, severe side reactions, and undesired formation of space charge layers, which result in restricted capacity release and limited rate capability. In this work, we reveal that the capacity loss lies in the H2–H3 phase transition period, and we propose that the inconsistent interfacial Li-ion migration is the arch-criminal. We introduce Si doping to stabilize the bulk structure and Li4SiO4 fast ionic conductor coating to regulate the interfacial behaviors between the Ni-rich cathode and sulfide-based solid electrolyte Li6PS5Cl. The modified NCM@LSO-2||LPSCl||Li–In ASSLBs deliver a high reversible capacity of 183.5 mA h g–1 at 0.1C, 30.3% higher than the bare NCM811 electrode. Besides, the interfacial regulation strategy enables the operation at a high rate of 5.0C and achieves a high capacity retention ratio of ∼85.8% after 500 cycles at 1.0C. Furthermore, the underlying mechanisms are well investigated through kinetic analyses and theoretical simulations. This work provides an in-depth understanding on the interfacial degradations between Ni-rich cathodes and sulfide-based all-solid-state electrolytes from the view of kinetic limitations and offers potential solutions.
研究领域:
材料科学
·
电化学
·
能源存储技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 31
·17941-17949
·
IF 3.049
Xinxin Li,Hebang Shi,Bo Wang,Na Li,Liqiang Zhang,Pengpeng Lv
Surface coating of metal oxides is an effective approach for enhancing the capacity retention of a nickel-rich layered cathode. Current conventional coating techniques including wet chemistry methods and atomic layer deposition are restricted by the difficulty in perfectly balancing the coating quality and scale-up production. Herein, a highly efficient TiO2 coating route through fluidized bed chemical vapor deposition (FBCVD) was proposed to enable scalable and high yield synthesis of a TiO2 coated nickel-rich cathode. The technological parameters including coating time and TiCl4 supply rate were systematically studied, and thus a utility TiO2 deposition rate model was deduced, promoting the controllable TiO2 coating. The FBCVD TiO2 deposition mechanism was fundamentally analyzed based on the TiCl4 hydrolysis principle. The amorphous and uniform TiO2 coating layer is compactly attached on the particle surface, forming a classical core–shell structure. Electrochemical evaluations reveal that the TiO2 coating by FBCVD route indeed improves the capacity retention from 89.08% to 95.89% after 50 cycles.
研究领域:
材料科学
·
化学工程
·
能源技术
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Weili Sun,Qingqing Zhang,Xiao-Guang Sun,Cheng Li,Yongsheng Huang,Wenyu Mu,Junbin Tan,Jianlin Li,Kai Liu,Shijian Zheng,Sheng Dai
Nickel-rich (Ni ≥ 90%) layered oxides materials have emerged as a promising candidate for next-generation high-energy-density lithium-ion batteries (LIBs). However, their widespread application is hindered by structural fatigue and lattice oxygen loss. In this work, an epitaxial surface rock-salt nanolayer is successfully developed on the LiNi 0.9 Co 0.1 O 2 sub-surface via heteroatom anchoring utilizing high-valence element molybdenum modification. This in-situ formed conformal buffer phase with a thickness of 1.2 nm effectively suppresses the continuous interphase side-reactions, and thus maintains the excellent structure integrity at high voltage. Furthermore, theoretical calculations indicate that the lattice oxygen reversibility in the anion framework of the optimized sample is obviously enhanced due to the higher content of O 2 p states near the Fermi level than that of the pristine one. Meanwhile, the stronger Mo–O bond further reduces cell volume alteration, which improves the bulk structure stability of modified materials. Besides, the detailed charge compensation mechanism suggests that the average oxidation state of Ni is reduced, which induces more active Li + participating in the redox reactions, boosting the cell energy density. As a result, the uniquely designed cathode materials exhibit an extraordinary discharge capacity of 245.4 mAh g −1 at 0.1 C, remarkable rate performance of 169.3 mAh g −1 at 10 C at 4.5 V, and a high capacity retention of 70.5% after 1000 cycles in full cells at a high cut-off voltage of 4.4 V. This strategy provides an valuable insight into constructing distinctive heterostructure on high-performance Ni-rich layered cathodes for LIBs.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Peng He,Maolin Zhang,Saijing Wang,Limin Yuwen,Yuan Wang,Yangxi Yan,Dongyan Zhang,Xiaofei Sun
Co-free and Ni-rich LiNi 0.95 Mn 0.05 O 2 (NM95) cathodes are expected to be widely employed in power batteries due to their high capacity and low cost. However, the loss of Co and increase in Ni compromise cyclic stability and high-rate performance. Herein, PPy coating layer with excellent flexibility and conductivity is introduced on NM95 surface to enhance the structural stability and charge transfer properties. X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray spectroscopy, electrochemical impedance spectroscopy and cyclic voltammetry are utilized to elaborate on positive influence of PPy on electrochemical performance. PPy coating alleviates volumetric changes of cathode caused by charge/discharge process, suppressing mechanical fragmentation. Moreover, PPy provides protective layer to suppress side reactions and isolate the corrosion of electrolytes. Besides, PPy is widely recognized excellent electronic conductor that can promote electronic conduction. It is revealed that PPy-coated NM95 cathode exhibits excellent capacity retention of 90.1 % (4.3 V) and 84.4 % (4.5 V) after 100 charge/discharge cycles at 1 C. Moreover, capacity retention is 91.1 % after 100 cycles and initial capacity is as high as 153.4 mAh/g at 5 C. These results indicate that flexible and electronically conductive coating is effective strategy to enhance cyclic stability of NM95 cathodes.
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）