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LiNi0.8Co0.1Mn0.1O2
Nano Energy · 2019 · IF 15.548

A special enabler for boosting cyclic life and rate capability of LiNi0.8Co0.1Mn0.1O2: Green and simple additive

Chen-Guang Shi,Chong-Heng Shen,Xin-Xing Peng,Chen-Xu Luo,Lin-Fan Shen,Wen-Jia Sheng,Jing-Jing Fan,Qiong Wang,Shao-Jian Zhang,Bin-Bin Xu,Jiang-Jun Xian,Yi-Min Wei,Ling Huang,Jun-Tao Li,Shi-Gang Sun

LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) is widely known for its extremely high specific capacity and relatively low cost, which draws extensive attention worldwide. However, poor cycling performance and rate capability impose restrictions on its large-scale practical application. Here we report that succinic anhydride (SA) as an additive in carbonate electrolyte significantly enhances the cycling performance and rate capability of Li/NCM811 cells. Capacity retention can reach 93.8% after 400 cycles at 1C rate by adding 3 wt% SA, while the pristine one cannot even endure 100 cycles. Moreover, rate capability can also be optimized to 82.4% of 5C/0.5C capacity ratio. The improvement of electrochemical performance was attributed to the formation of a uniform conductive cathode electrolyte interphase (CEI) layer upon particles. Our results confirm that firstly, the CEI formed by SA can protect active sites on the surface of NCM811 from side reactions. Secondly, the uniform conductive CEI plays a part in inhibiting severe polarization and local overcharge during long cycles. Moreover, the robust CEI layer can suppress the internal cracks, prohibit the irreversible phase transformation and nickel element migration of NCM811.

CAS / MDL: 108-30-5
研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Tailoring electrode-electrolyte interphases to enable the cycling stability of lithium metal batteries with LiNi0.8Co0.1Mn0.1O2 cathode

Sen Jiang,Xin Xu,Junying Yin,Xuequan Zhu,Lai Wei,Kang Xi,Linghao Zhang,Yuelang Lan,Haihua Wu,Yunfang Gao

Rechargeable lithium metal batteries (LMBs) coupling with Ni-rich cathodes are promising high-energy-density electrochemical energy storage devices. However, the growth of Li dendrites and structural degradation of Ni-rich materials, associated with the erratic electrode-electrolyte interphase (EEI) and corrosion of harmful acidic species from the hydrolysis of LiPF 6 , seriously deteriorate the cycling performance of LMBs with Ni-rich cathodes. Herein, glutaric anhydride (GA) as a multifunctional electrolyte additive is proposed to achieve satisfactory lifespan of LMBs by in situ constructing LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode/Li anode-electrolyte interphases (CEI/AEI), and scavenging corrosive acidic species. The GA-derived CEI/AEI layers are rich in C O species, which can strongly coordinate with the Li anode and delithiated Ni-rich cathode surface . Thus, parasitic reactions of the electrolyte on the aggressive surface of the Ni-rich cathode and Li anode are notably reduced. Furthermore, the problems such as the inner microcrack evolution of NCM811 particles, the growth of Li dendrites and the corrosion of acidic species are well addressed. Consequently, the capacity retention of Li/NCM811 cell is increased from 59.4% to 90.7% after 300 cycles at 1C in the presence of GA, and the Li/Li symmetrical cell with GA exhibits the super-stable cyclic performance of 1400 h at 0.2 mA cm −2 .

研究领域: 材料科学 · 电化学能源存储
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

LiF-Rich Interfaces and HF Elimination Achieved by a Multifunctional Additive Enable High-Performance Li/LiNi0.8Co0.1Mn0.1O2 Batteries

Yue Lei,Xin Xu,Junying Yin,Sen Jiang,Kang Xi,Lai Wei,Yunfang Gao

Li-metal batteries (LMBs), especially in combination with high-energy-density Ni-rich materials, exhibit great potential for next-generation rechargeable Li batteries. Nevertheless, poor cathode–/anode–electrolyte interfaces (CEI/SEI) and hydrofluoric acid (HF) attack pose a threat to the electrochemical and safety performances of LMBs due to aggressive chemical and electrochemical reactivities of high-Ni materials, metallic Li, and carbonate-based electrolytes with the LiPF6 salt. Herein, the carbonate electrolyte based on LiPF6 is formulated by a multifunctional electrolyte additive pentafluorophenyl trifluoroacetate (PFTF) to adapt the Li/LiNi0.8Co0.1Mn0.1O2 (NCM811) battery. It is theoretically illustrated and experimentally revealed that HF elimination and the LiF-rich CEI/SEI films are successfully achieved via the chemical and electrochemical reactions of the PFTF additive. Significantly, the LiF-rich SEI film with high electrochemical kinetics facilitates Li homogeneous deposition and prevents dendritic Li from forming and growing. Benefiting from the collaborative protection of PFTF on the interfacial modification and HF capture, the capacity ratio of the Li/NCM811 battery is boosted by 22.4%, and the cycling stability of the symmetrical Li cell is expanded over 500 h. This provided strategy is conducive to the achievement of high-performance LMBs with Ni-rich materials by optimizing the electrolyte formula.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

Cathode-anode reaction products interplay enabling high performance of LiNi0.8Co0.1Mn0.1O2/artificial graphite pouch batteries at elevated temperature

Huajun Zhao,Yunxian Qian,Guangfu Luo,Jian Chang,Chaoyang Wang,Jun Wang,Huaiyu Shao,Yonghong Deng

LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode coupling with artificial graphite (AG) is a promising tendency for high-energy-density batteries . However, realization of long-term lifespan under current realistic conditions remains a “Gordian knot” for large-scale commercialization-oriented realm owing to the aggressive and highly reactive Ni 4+ sites on the delithiated cathodes and electrolyte exhaustion. Vinylene carbonate (VC) is commonly employed as the additive for graphite anode in carbonate electrolytes. However, VC has limited protection ability for NCM811/AG, especially for high-temperature cycling, showing conspicuous gas generation and large interfacial resistance . Herein, advanced carbonate-based electrolytes containing vinylene carbonate (VC) and phosphate compounds like triallyl phosphate (TPPC2) and tripropargyl phosphate (TPPC3) as electrolyte additives are reported to improve the performance of NCM811/AG pouch cells at elevated temperature. Theoretical calculations and comprehensive characterizations reveal that these two electrolytes well regulate the electrodes interface with more robust and homogenous films. Moreover, the TPPC2 and TPPC3 additives exhibit stronger tendency to eliminate the corrosive active oxygen ( 1 O 2 ) released from NCM811. These merits mitigate the electrolyte decomposition, decrease the gas generation, inhibit the dissolution of transition metals from cathode, and protect the structure stability of NCM811. Such outstanding electrochemical performance reveals promising prospects in the commercialized application of NCM811/AG batteries .

研究领域: 电化学 · 材料科学 · 能源存储 · 锂离子电池 · 界面化学 · 电极材料 · 电解质工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2020 · IF 4.65

Pretreated precursor to realize dual modification that improves the high voltage electrochemical performance of LiNi0.8Co0.1Mn0.1O2 cathode materials

Jiandong Zhang,Fuzhong Wu,Xinyi Dai,Yi Mai,Yijing Gu

Ni-rich cathodes have been increasingly studied due to their satisfactory capacity and low cost. However, the rapid attenuation of capacity during charging and discharging Ni-rich cathodes limits their practical use. In this work, a KMnO 4 -pretreated precursor is used to synthesize LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) in air. The product shows various morphological and structural characterizations, thereby verifying that the pretreatment can successfully achieve the dual modification of a MnO 2 coating and Mn 4+ doping. Electrochemical tests indicate that the 1.0 wt% KMnO 4 -pretreated sample exhibits superior cycling performance from 3.0 to 4.5 V. Additionally, the capacity retention rate after 100 cycles reaches 79.15% at 0.2 C, which shows that the pretreated sample has better cycling stability compared with the pure sample calcined in air (59.22%) and the pure sample calcined in oxygen (71.17%). In addition, the capacity retention reaches 82.27% at a high current density of 1 C while suppressing the potential polarization. Cyclic voltammetry and electrochemical impedance spectroscopy tests show that the pretreatment decreases the resistance and suppresses the irreversible phase transition. The protective MnO 2 coating inhibits the interfacial reactions between the active substance and electrolyte, while the Mn 4+ dopant improves the crystal structure. Therefore, it is concluded that LiNi 0.8 Co 0.1 Mn 0.1 O 2 , with a superior electrochemical performance at a high of 4.5 V, can be prepared through a KMnO 4 -pretreated precursor in air.

研究领域: 材料科学 · 电化学 · 储能技术 · 锂离子电池 · 正极材料
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

High-performance Li/LiNi0.8Co0.1Mn0.1O2 batteries enabled by optimizing carbonate-based electrolyte and electrode interphases via triallylamine additive

Sen Jiang,Xin Xu,Junying Yin,Yue Lei,Hongtao Guan,Yunfang Gao

Lithium (Li) metal batteries (LMBs), paired with high-energy–density cathode materials , are promising to meet the ever-increasing demand for electric energy storage. Unfortunately, the inferior electrode–electrolyte interfaces and hydrogen fluoride (HF) corrosion in the state-of-art carbonate-based electrolytes lead to dendritic Li growth and unsatisfactory cyclability of LMBs. Herein, a multifunctional electrolyte additive triallylamine (TAA) is proposed to circumvent those issues. The TAA molecule exhibits strong nucleophilicity and contains three unsaturated carbon–carbon double bonds , the former for HF elimination, the later for in-situ passivation of aggressive electrodes. As evidenced theoretically and experimentally, the preferential oxidation and reduction of carbon–carbon double bonds enable the successful regulation of components and morphologies of electrode interfaces, as well as the binding affinity to HF effectively blocks HF corrosion. In particular, the TAA-derived electrode interfaces are packed with abundant lithium-containing inorganics and oligomers , which diminishes undesired parasitic reactions of electrolyte and detrimental degradation of electrode materials . When using the TAA-containing electrolyte, the cell configuration with Li anode and nickel-rich layered oxide cathode and symmetrical Li cell deliver remarkably enhanced electrochemical performance with regard to the additive-free cell. The TAA additive shows great potential in advancing the development of carbonate-based electrolytes in LMBs.

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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ACS Applied Energy Materials · 2022 · IF 6.959

Nonflammable Dual-Salt Electrolytes for Graphite/LiNi0.8Co0.1Mn0.1O2 Lithium-Ion Batteries: Li+ Solvation Structure and Electrode/Eelectrolyte Interphase

Fanjue Wen,Shuai Cao,Xin Ren,Yuliang Cao,Xinping Ai,Fei Xu

Trimethyl phosphate (TMP) is the most promising safe solvent for lithium-ion battery (LIB) electrolyte because of the nonflammability, oxidation stability, and low cost, but its application is hindered by incompatibility with the graphite anode. Herein, nonflammable electrolytes with ordinary concentration (1 mol L–1) are designed for graphite/LiNi0.8Co0.1Mn0.1O2 (Gr/NCM811) LIBs with TMP/2,2,2-trifluoroethyl methyl carbonate (FEMC) binary solvents. Stable cycling of the Li/Gr half cells with high capacity is achieved via modulation of the Li+ solvation structure. A dual-salt strategy of lithium hexafluorophosphate/lithium difluoro(oxalato)borate is further used to realize the high performance of the Gr/NCM811 full cells. More significantly, the functions and relationship of Li+ solvation structure and electrode/electrolyte interphase are elucidated. Li+ solvation structure and interphase are respectively the thermodynamic and kinetic factors for the side reactions of the electrolyte occurring at the electrode/electrolyte interphase, which should be considered comprehensively in the design of electrolytes for high-energy density LIBs.

研究领域: 材料科学 · 能源化学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Slurry-Coated LiNi0.8Co0.1Mn0.1O2–Li3InCl6 Composite Cathode with Enhanced Interfacial Stability for Sulfide-Based All-Solid-State Batteries

Qing Ye,Xiaohan Li,Wenkui Zhang,Yang Xia,Xinping He,Hui Huang,Yongping Gan,Xinhui Xia,Jun Zhang

The implementation of all-solid-state lithium batteries (ASSLBs) is regarded as an important step toward the next-generation energy storage systems. The sulfide solid-state electrolyte (SSE) is a promising candidate for ASSLBs due to its high ionic conductivity and easy processability. However, the interface stability of sulfide SSEs toward high-capacity cathodes like nickel-rich layered cathodes is limited by the interfacial side reaction and narrow electrochemical window of the electrolyte. Herein, we propose introducing the halide SSE Li3InCl6 (LIC) with high (electro)chemical stability and superior Li+ conductivity to act as an ionic conductive additive in the Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM) cathode mixture through a slurry coating, aiming to build a stable cathode–electrolyte interface. This work demonstrates that the sulfide SSE Li5.5PS4.5Cl1.5 (LPSCl) is chemically incompatible with the NCM cathode, and the indispensable role of the substitution of LPSCl with LIC in enhancing the interfacial compatibility and oxidation stability of the electrolyte is highlighted. Accordingly, this new configuration shows superior electrochemical performance at room temperature. It shows a high initial discharge capacity (136.3 mA h g–1 at 0.1C), cycling performance (77.4% capacity retention at the 100th cycle), and rate capability (79.3 mA h g–1 at 0.5C). This work paves the way for investigating interfacial challenges regarding high-voltage cathodes and provides new insights into possible interface engineering strategies.

研究领域: 材料科学 · 电化学 · 储能技术 · 固态电池 · 界面工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Nickel-rich layered cathode LiNi0.8Co0.1Mn0.1O2 mediated by a selective lattice doping towards high-performance lithium ion battery

Jue Zhang,Tangzhe Cao,Ying Lei,Jianying Li,Weifeng Fan,Bin Zhang,Xingyong Liu,Yujun Si,Honghui Wang

Rapid capacity loss and voltage fading pose a significant barrier to the commercialization of nickel-rich materials with layered structures due to particle cracking and structure degradation. Double element selective lattice modification strategy that can balance multiple performance requirements is gaining attention. Here, we proposed a selective lattice doping strategy to enhance the lattice stability of LiNi 0.8 Co 0.1 Mn 0.1 O 2 via a double element co-doping of Mg and W. Impressively, the Mg/W co-doping improved electrochemical reaction kinetics and discharge capacity, and largely suppressed structure degradation simultaneously. In situ X-ray diffraction (XRD) results demonstrated that W/Mg co-doping can tune H2−H3 phase transition, relieving the lattice stress and mechanical degradation . These improvements can be attributed to a synergistic effect of W and Mg, in which high valence state W 6+ induced the formation of Ni 2+ and strong W−O bonds increased layer structure stability, meanwhile Mg 2+ as a pillar inhibited Li + /Ni 2+ mixing and maintained structural stability. This work provides selective lattice dual-doping strategic guidelines for the use of high energy efficiency and robust stability high-nickel low-cobalt cathodes in lithium-ion batteries.

研究领域: 材料科学 · 能源存储
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Enhanced Long-Term Stability and Safety of LiNi0.8Co0.1Mn0.1O2 Cathode via Nanoscale Surface Modification with Sulfonyl-Functionalized Polyimide Layer

Changchao Sun,Yongjun Kang,Bingxue Liu,Daolei Lin,Guofeng Tian,Shengli Qi,Dezhen Wu

Nickel-rich layered oxide cathodes (LiNi0.8Co0.1Mn0.1O2, NCM811) have shown great promise in high-energy-density lithium-ion batteries due to their high specific capacity. However, their practical application is severely hampered by structural instability, interfacial side reactions, and transition metal dissolution. To address this issue, in the present work, a highly polar polyimide containing sulfonyl moiety (named PI (6FOS)) is designed and utilized as a functional interfacial coating layer on NCM811 by copolymerizing 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA) with 4,4′-oxidianiline (ODA) and 4,4′-diaminodiphenyl sulfone (DDS). The combination of high polar constant and superior interfacial stability of PI (6FOS) contributes to effective suppression of electrolyte decomposition and transition metal dissolution. The strong interactions between polar trifluoromethyl and sulfonyl groups in the molecular chain and NCM811 particles enhance interfacial stability and facilitate lithium-ion transport. As expected, the PI (6FOS)/NCM811 electrode exhibits excellent long-term cycling performance with a remarkable capacity retention of 94% over 100 cycles at 0.2 C and 83% over 300 cycles at 1 C within 2.5–4.3 V. Even under high-voltage conditions (4.7 V), it maintains 59% capacity retention after 300 cycles at 1 C. The PI (6FOS)/NCM811 electrode shows outstanding rate capability, with a discharge specific capacity of 140.3 mAh g–1 at 5 C. Meanwhile, the presence of the polyimide coating layer increases the thermal decomposition temperature of the cathode material and reduces heat generation. The perspective of the coating design strategy based on sulfonyl-containing polyimide modification offers a novel path toward high-stability cathodes for high-energy-density and high-safety lithium-ion batteries.

研究领域: 材料科学 · 电化学 · 储能 · 电池技术
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Adiponitrile (ADN): A Stabilizer for the LiNi0.8Co0.1Mn0.1O2 (NCM811) Electrode/Electrolyte Interface of a Graphite/NCM811 Li-Ion Cell

Yijing Qiu,Dongsheng Lu,Yunyan Gai,Yuepeng Cai

Adiponitrile (ADN) is studied as an additive of commercial carbonate electrolyte for a graphite/NCM811 Li-ion cell in this work. Compared with the cell using a baseline electrolyte, the cycling stability of the cells using 0.2, 0.5, 1, and 2 wt % ADN-added electrolytes is significantly improved. Among them, the effect is most prominent when the ADN content is 0.5 wt %, and the capacity retention rate of the cell after 200 cycles at 0.3 C is increased by 17.6%. Scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy analyses confirm that ADN can make the coating layer formed on the cathode and anode surfaces of the cell denser and uniform. The formation of the cathodic coating layer does not obey the usual mechanism of adsorption between the nitrile group and metal ions, but it may be due to the polymerization of ADN initiated by carbocations from the oxidation of solvent molecules (ethylene carbonate/ethyl methyl carbonate) in the electrolyte. The cathodic coating layer greatly decreases the oxidation of the electrolyte so that a stable coating layer (also called solid electrolyte interface/SEI) can be formed on the anode, which is the reason for improvement of the cycling performance of the cell. However, the formation of the anode SEI layer is almost independent of ADN, and it still depends on the common reduction reaction of the electrolyte.

研究领域: 材料科学 · 电化学
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