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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-12 · IF 15.7

Electronic structure formed by Y2O3-doping in lithium position assists improvement of charging-voltage for high-nickel cathodes

Wang Shijie,Liang Kang,Zhao Hongshun,Wu Min,He Junfeng,Wei Peng,Ding Zhengping,Li Jianbin,Huang Xiaobing,Ren Yurong

High-capacity power battery can be attained through the elevation of the cut-off voltage for LiNi 0.83 Co 0.12 Mn 0.05 O 2 high-nickel material. Nevertheless, unstable lattice oxygen would be released during the lithium deep extraction. To solve the above issues, the electronic structure is reconstructed by substituting Li + ions with Y 3+ ions. The dopant within the Li layer could transfer electrons to the adjacent lattice oxygen. Subsequently, the accumulated electrons in the oxygen site are transferred to nickel of highly valence state under the action of the reduction coupling mechanism. The modified strategy suppresses the generation of oxygen defects by regulating the local electronic structure, but more importantly, it reduces the concentration of highly reactive Ni 4+ species during the charging state, thus avoiding the evolution of an unexpected phase transition. Strengthening the coupling strength between the lithium layers and transition metal layers finally realizes the fast-charging performance improvement and the cycling stability enhancement under high voltage.

CAS / MDL: 1310-65-2
研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

High voltage electrochemical performance of ultrahigh-Ni cathode via in situ constructed nano-LiF and CNT composite cathode electrolyte interphase layer

Yunchao Liao,Na Wang,Xinyi Dai,Wenwen Zhou,Fuzhong Wu,Jiexi Wang,Haijun Chen,Yi Mai

Ultrahigh-nickel LiNi x Co y Mn 1-x-y O 2 cathode material (Ni content ≥ 0.9) is of great significance for the development of high energy density of lithium-ion batteries. However, its high surface activity leads to more surface residual lithium formation and deterioration of electrochemical performance, especially at high voltage. Here we add NH 4 F and nitrogen-doped carbon nanotubes (CNT) during the dimethyl carbonate (DMC) washing process, and constructed in situ the nano-LiF and CNT composite cathode electrolyte interphase (CEI) layer while removing part of residual lithium, effectively optimizing the surface environment of LiNi 0.9 Co 0.05 Mn 0.05 O 2 . The modified LiNi 0.9 Co 0.05 Mn 0.05 O 2 has a capacity retention rate of 61.3 % after 200 cycles between 2.8 and 4.5 V at 1C, significantly higher than the 46.7 % of the unwashed sample, and a specific discharge capacity of 146.9 mAh g −1 at 5C, compared to 127.5 mAh g −1 for the unwashed sample. Benefit from the alleviation of polarization and the increase of Li + diffusion coefficient, the stable CEI layer provides effective protection for LiNi 0.9 Co 0.05 Mn 0.05 O 2 under 4.5 V, alleviating surface side reactions. In this paper, a simple and effective strategy is developed to optimize the surface of Ni-rich cathode material, which provides a new insight for the treatment of surface residual lithium.

CAS / MDL: 308068-56-6 616-38-6
研究领域: 材料科学 · 电化学
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Materials Today Communications · 2025 · IF 4.5

Synergistic effect of Na and B co-doping on the electrochemical properties of LiNi0.865Co0.095Al0.04O2 cathode materials for Li-ion batteries

Wujie Ge,Yuanxiang Fu,Chaonan Wang,Lirong Yan,Qi Feng,Bing Yan,Xiang Li

The high-nickel cathode material LiNi 0.865 Co 0.095 Al 0.04 O 2 (NCA) has garnered significant attention due to its high energy density and cost-effectiveness in production. However, this material is also prone to rapid capacity degradation, primarily due to phase transitions occurring during the redox process. In this paper, the co-modification with Na and B cations is employed to stabilize the lattice structure and enhance the electrochemical performance of the NCA material. It can be found that the incorporation of Na and B cations in the lattice can reduce cation mixing, expand the Li-layer spacing and improve crystal stability, thereby increasing the specific capacity and cyclic stability of the NCA material. Specifically, the co-doped NCA-2 sample exhibits a specific capacity of 202.1 mAh/g at 0.1 C and maintains a capacity retention of 78.75 % at 1 C after 300 cycles, representing a substantial improvement over the pristine material (187.2 mAh/g and 61.68 % capacity retention). Moreover, at a current density of 10 C, the co-doped NCA-2 sample demonstrates a high specific capacity of 133.9 mAh/g, compared to 110.1 mAh/g for the pristine material. The Na/B co-doping strategy presented in this study offers a straightforward method to improve the cyclability and rate behavior of cathode materials, highlighting its potential for commercial applications.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 电化学
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Nano-Micro Letters · 2025 ·Vol. 17 ·期 1 ·1-15 · IF 36.3

Developing High-Energy, Stable All-Solid-State Lithium Batteries Using Aluminum-Based Anodes and High-Nickel Cathodes

Wu Xin,Wang Meiyu,Pan Hui,Sun Xinyi,Tang Shaochun,Zhou Haoshen,He Ping

Aluminum (Al) exhibits excellent electrical conductivity, mechanical ductility, and good chemical compatibility with high-ionic-conductivity electrolytes. This makes it more suitable as an anode material for all-solid-state lithium batteries (ASSLBs) compared to the overly reactive metallic lithium anode and the mechanically weak silicon anode. This study finds that the pre-lithiated Al anode demonstrates outstanding interfacial stability with the Li 6 PS 5 Cl (LPSCl) electrolyte, maintaining stable cycling for over 1200 h under conditions of deep charge–discharge. This paper combines the pre-lithiated Al anode with a high-nickel cathode, LiNi 0.8 Co 0.1 Mn 0.1 O 2 , paired with the highly ionic conductive LPSCl electrolyte, to design an ASSLB with high energy density and stability. Using anode pre-lithiation techniques, along with dual-reinforcement technology between the electrolyte and the cathode active material, the ASSLB achieves stable cycling for 1000 cycles at a 0.2C rate, with a capacity retention rate of up to 82.2%. At a critical negative-to-positive ratio of 1.1, the battery’s specific energy reaches up to 375 Wh kg −1 , and it maintains over 85.9% of its capacity after 100 charge–discharge cycles. This work provides a new approach and an excellent solution for developing low-cost, high-stability all-solid-state batteries.

CAS / MDL: 546-89-4 409071-16-5
研究领域: 材料科学 · 能源技术
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Self-repaired cathode electrolyte interphase to stabilize the high-nickel cathode interface by a sustained-release multifunctional electrolyte additive

Yue Zou,Qizheng Zheng,Yonglin Tang,Yawen Yan,Shiyuan Zhou,Hong-Gang Liao,Yu Qiao,Jun Bao,Shi-Gang Sun

Increasing the nickel content in high-nickel LiNi x Co y Mn 1-x-y O 2 cathode materials (NCM) can boost their energy density. However, the consequence of rising Ni content in NCM consists in the heightened stress buildup, intensified irreversible phase transition and severe electrolyte decomposition, and consequently accelerating the battery’s degradation. In the current study, we have revealed that the 4-fluoro-N, N dimethylbenzenesulfonamide (FBSN) as an electrolyte additive can refrain the typical dehydrogenation of EC. Furthermore, a continuously repaired cathode electrolyte interphase (CEI) is designed elaborately on LiNi 0.9 Co 0.05 Mn 0.05 O 2 (NCM90) surface by employing the FBSN as a sustained-release electrolyte additive to enhance cycling stability of NCM90||Li cells. This CEI, composed of high mechanical strength LiF and benzene ring skeleton, along with conductive Li + moieties (S-rich and N-rich species), can be effectively self-repaired in time when damaged, reduce the interaction between the NCM90 and sensitive electrolyte, and mitigate the devastation to the NCM90 cathode surface. As a result, the NCM90||Li cells with 2 % FBSN-containing electrolyte delivers a capacity retention of 90.2 % after 200 cycles at 1C, and 83.1 % after 200 cycles even at higher voltage of 4.5 V, superior than that of Base electrolyte (70.0 % at 4.3 V and 68.0 % at 4.5 V). This study provides an engaging approach to design electrolytes for high-nickel cathodes by autonomously interfacial repair.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

Wrinkled and flexible N-doped MXene additive for improving the mechanical and electrochemical properties of the nickel-rich LiNi0.8Co0.1Mn0.1O2 cathode

Song-Yi Liao,Shuai-Fu Cui,Yue-Zhu Li,Wei-Xiang Cheng,Xing-Wen Huang,Jing Zhang,Ting-Ting Cui,Xu-Gang Shu,Yong-Gang Min

In this work, the wrinkled, flexible, and layered nitrogen-doped Ti 3 C 2 T x (shorten as N-MXene) is synthesized by using cyanamide as N-dopants. The changeable (002) plane spacing and the attached functional groups of N-MXene are detected by XRD and XPS analyses in details, respectively. The microscopic morphology of N-MXene is characterized by SEM and TEM, which demonstrates its wrinkled and flexible characteristics. When the wrinkled N-MXene being added into the LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) as conductive additive, the attained electrodes obtain enhanced electrochemical performances at the appropriate weight ratio (namely 2.5-N-MXene with 2.5 wt.%). The 2.5-N-MXene delivers “extra” capacity of 226.9 mAh/g at 0.1 C (20 mA/g) current density. The “extra” capacity is assigned to Li ions intercalation/extraction from the wrinkled/flexible/layered N-MXene. Moreover, based on the analyses of CV and dQ/dV curves, the wrinkled/flexible N-MXene additive could effectively inhibit the phase transition of M↔H2 of NCM811 and alleviate the volume change of the particles in the circulation. From DFT simulation, the N-MXene is more capable of preventing Ni/Co/Mn from dissolving and migrating to the negative electrode to form dendrites through adsorption. Therefore, the N-MXene should be a very competitive conductive agent to improve the mechanical and electrochemical properties of high nickel cathode materials.

研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Enhancement in the electrochemical stability at high voltage of high nickel cathode through constructing ultrathin LiCoPO4 coating

Jian Wei,Houfei Xiong,Hao Zhang,Xueting Li,Yanyi Liu,Zongmo Shi

The challenge of commercial layered-structure nickel-rich cathodes in lithium-ion batteries (LIBs) are the rapid capacity/voltage degradation at high rate capability and thermal runaway. The wide operational voltage range and excellent electrochemical stability of the coating material are key points to improve electrochemical performance and thermal stability at high voltage and high rate conditions. The uniformly olivine-type LiCoPO 4 (LCP) coatings were successfully prepared on the surface of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode combining sol–gel method and heat treatment. The capacity retention and operating voltage stability of the cathode at high cutoff voltage of 4.6 V were dramatically improved due to the ultrathin and stable interface is designed. The modified NCM811 exhibited a high cycling capacity of 157.7 mAh·g −1 at 5 C with a capacity loss of only 12.1 %. In high nickel cathode coating modification, LCP as the thinnest phosphate coating effectively improves the capacity decay of the cathode at high rate. The interface reconstruction provided a stable channel of Li + transport, which suppressed the cathode/electrolyte interface reaction to enhance the stability. The formation of strong covalent P O bonds at the interface significantly reduced the oxidizing activity on the NCM811 surface, further inhibiting the oxygen release and irreversible phase transition.

研究领域: 材料科学 · 能源存储与转换
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Sacrificial Additive C60-Assisted Catholyte Buffer Layer for Li1+xAlxTi2–x(PO4)3-Based All-Solid-State High-Voltage Batteries

Xuan Wang,Shuo Huang,Benben Wei,Min Liu,Bo Yang,Ruoqing Liu,Hongyun Jin

All-solid-state batteries with oxide electrolytes and high-nickel layered oxide cathodes (LiNixCoyMnzO2 and LiNixCoyAlzO2, x + y + z = 1, x ≥ 60%) have received widespread attention owing to their high energy density and high safety. However, they generally suffer from interfacial structural instability when coupled with solid-state electrolytes, which strongly diminishes the longevity of the battery. In this work, we propose adding a sacrificial additive C60 to the catholyte buffer layer between Li1.4Al0.4Ti1.6(PO4)3 (LATP) and LiNi0.8Co0.1Mn0.1O2 (NCM811) to enhance the electrochemical stability under high-voltage operating conditions. A uniform and robust cathode–electrolyte interphase (CEI) film enriched with LixPOyFz, LiPxFy, and C60Fn is spontaneously formed on the surface of the cathode particles. In addition, the NCM811/Li solid-state battery delivers a discharge capacity of 150.3 mAh g–1 with a retention of 85% after 200 charge–discharge cycles at 0.5 C. This study offers a practical approach toward realizing LATP-based all-solid-state high-voltage batteries characterized by exceptional cycling stability.

CAS / MDL: 13463-67-7 554-13-2
研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Stabilizing the Interphase in an Ultra-High-Nickel Cathode Enabling High-Performance Lithium-Ion Batteries

Qing Zhao,Zhibin Zhang,Depeng Song,Xiaolin Sun,Yuan Zhang,Jing Gao,Ohsaka Takeo,Matsumoto Futoshi,Jianfei Wu

High-nickel (Ni ≥ 90%) cathodes which have a high specific capacity hold great potential for next-generation lithium-ion batteries (LIBs). However, their practical application is restricted by their high interfacial reactivity because of the presence of residual lithium (Li) compounds on the surface. Herein, the LiNi0.9Co0.06Mn0.04O2 (NCM90) cathode is surface-modified with sulfur (S) via a simple and feasible dry mixing and low-temperature heat treatment, converting the residual lithium compound on the surface into inactive lithium sulfate (Li2SO4). This induces the formation of a stable inorganic enriched electrode–electrolyte interface on the cathode surface and inhibits the occurrence of side reactions, ultimately inhibiting lattice collapse and the dissolution of transition metal ions. After modifying, the capacity retention rates of NCM90/Li and NCM90/graphite cells are both greatly enhanced after long cycling. This work provides a new idea for the rational design of the electrode–electrolyte interface of high-nickel cathodes.

CAS / MDL: 7704-34-9
研究领域: 材料科学 · 能源存储技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Enhanced mechanical and surface chemical stability in cobalt-free, high-nickel cathode materials for lithium-ion batteries

Zhenping Qiu,Zhiwen Wang,Shun Yuan,Chaojie Zhao

Cobalt-free, high-nickel cathode materials are essential for the sustainable evolution of energy storage technologies, reducing the dependence on resources with significant environmental and social implications and simultaneously improving the efficiency and cost effectiveness of batteries. This paper introduces a cobalt-free, high-nickel cathode material called 0.01B-LiNi 0.98 Mg 0.01 Zr 0.01 O 2 (NMZB) developed using a novel blend of elements to enhance mechanical and surface chemical stability. Detailed evaluations confirmed the successful integration of Mg, Zr, and B into the particles, with Mg and Zr primarily located within the particle interior and B predominantly on the surface. This unique elemental configuration significantly improves the stability of the bulk phase and surface structure of the material. In addition, the refinement of primary particles within NMZB further enhances its mechanical stability. As a result, NMZB exhibits exceptional electrochemical stability, achieving 90.5 % capacity retention after 200 cycles at a 1C rate. This compositional strategy incorporates a high nickel content into layered materials while eliminating cobalt, which is crucial for advancing the development of cost effective and high-performance lithium-ion battery technology.

研究领域: 材料科学 · 能源技术
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Small · 2025 · IF 12.1

Multifunctional Siloxane Additive Enabling Ultrahigh-Nickel Lithium Battery with Long Cycle Life at 30  and 60 °C

Xilong Chen,Zhili Yu,Xiangjie Li,Zhaoyu Sun,Guozheng Ma,Qiyun Li,Yingchun Ou,Yuxuan Liu,Renzong Hu

Ultrahigh-nickel layered oxide cathodes (≥90% nickel) possess exceptionally high discharge capacities, which can significantly improve the energy density of lithium-ion batteries and alleviate the driving range anxiety of electric vehicles. However, the high interfacial reactivity of ultrahigh-nickel cathodes, especially the detrimental side reactions with harmful acidic species like HF in the electrolyte, can deteriorate the battery interface and reduce the cycle life, hindering their practical application. In this study, 3-isocyanatopropyltrimethoxysilane (PTTS-NCO) is introduced as the electrolyte additive, which can effectively scavenge the harmful acidic species in the electrolyte and form a protective surface layer at the electrode/electrolyte interface, thereby enhancing the electrochemical performance of the battery (NCM90/Li). Specifically, the most effective battery based on the PTTS-NCO additive can maintain 70.3% of its capacity after 500 cycles at 30 °C. Even under a high cathode loading (3.0 mAh cm −2 ), it can retain 86.2% of its capacity after 300 cycles, far exceeding the base battery. Furthermore, it exhibits good performance under the harsh high-temperature environment, maintaining over 70.3% capacity retention in the NCM90/Li battery up to 350 cycles at 60 °C. This work demonstrates the great potential of multifunctional siloxane additive in lithium batteries based on ultrahigh-nickel cathode.

CAS / MDL: 15396-00-6 1067-25-0
研究领域: 材料科学 · 电化学 · 能源存储
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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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