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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

A low cost single-crystalline LiNi0.60Co0.10Mn0.30O2 layered cathode enables remarkable cycling performance of lithium-ion batteries at elevated temperature

Zhi Zhang,Maohui Bai,Xinming Fan,Maoyi Yi,Yufeng Zhao,Jiujun Zhang,Bo Hong,Zhian Zhang,Guorong Hu,Yanqing Lai

Nickel-rich and low-cobalt content in layered ternary cathodes (NCM) is considered as a promising candidate for commercial lithium-ion batteries (LIBs). Nevertheless, the traditional poly-crystalline NCM (PC-NCM) will inevitably go through intergranular cracks and structural collapse of the secondary spheres upon charge/discharge and thus result in serious performance degradation , limiting its practical application. Herein, we report a novel single-crystalline LiNi 0.6 Co 0.1 Mn 0.3 O 2 (SC-NCM) with by far the lowest fabricating cost, and a remarkable long cycling performance under harsh conditions. Such a unique design can withstand 900 cycles at high compaction density (~3.0 g cm −3 ) without any cracks observed. Therefore, it exhibits a superior capacity retention of 87.4% after 150 cycles at an extremely elevated temperature (55 °C) and a high charging-voltage (4.4 V). A 10 Ah LiNi 0.6 Co 0.1 Mn 0.3 O 2 ||graphite full cell delivers superior capacity retention of 73.9% after 900 cycles at 45 °C, where the highest cathode loading level (40.5 mg cm −2 ) and area capacity (6.48 mAh cm −2 ), outperforming the state-of-the-art SC-NCMs reported in literatures. This work provides a promising strategy for the development of high-energy and long-term cycle stability LIBs through controlling micron-sized single crystal particles as well as the Ni/or Co content in SC-NCM.

研究领域: 材料科学 · 能源存储技术
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RSC Advances · 2020 ·Vol. 10 ·期 17 ·9917-9923 · IF 3.119

Synthesis of a fine LiNi0.88Co0.09Al0.03O2 cathode material for lithium-ion batteries via a solvothermal route and its improved high-temperature cyclic performance

Guolin Cao,Jie Zhu,Yunjiao Li,Yuan Zhou,Zhuomin Jin,Bin Xu,Chunxi Hai,Jinbo Zeng

Nickel–Cobalt–Aluminum (NCA) cathode materials for lithium-ion batteries (LIBs) are conventionally synthesized by chemical co-precipitation. However, the co-precipitation of Ni2+, Co2+, and Al3+ is difficult to control because the three ions have different solubility product constants. This study proposes a new synthetic route of NCA, which allows fabrication of fine and well-constructed NCA cathode materials by a high temperature solid-state reaction assisted by a fast solvothermal process. The capacity of the LiNi0.88Co0.09Al0.03O2 as-synthesized by the solvothermal method was 154.6 mA h g−1 at 55 °C after 100 cycles, corresponding to 75.93% retention. In comparison, NCA prepared by the co-precipitation method delivered only 130.3 mA h g−1 after 100 cycles, with a retention of 63.31%. Therefore, the fast solvothermal process-assisted high temperature solid-state method is a promising candidate for synthesizing high-performance NCA cathode materials.

研究领域: 材料科学 · 能源存储
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LANGMUIR · 2017 · IF 3.833

LiF as an Artificial SEI Layer to Enhance the High-Temperature Cycle Performance of Li4Ti5O12

Lan Zhang,Kaihang Zhang,Zhaohui Shi,Suojiang Zhang

Li4Ti5O12 (LTO) is a promising anode material for electric vehicles (EVs) and electrochemical energy storage applications because of its safety, good rate capability, and long cycle life. At elevated temperature, such as 60 °C, it always shows poor cycle performance because of the instability between the electrode material and electrolyte, which may also lead to a serious gassing issue. In this article, a facile hydrothermal method is adopted to coat the LTO powder with a thin LiF layer, in which the LiF acts as an artificial solid electrolyte interface (SEI) layer to prevent the direct contact of LTO and electrolyte, thus improving the high-temperature cycle performance. Electrochemical tests prove that the LiF coating layer has no influence on the kinetics at ambient temperature and greatly enhances the high-temperature cycle stability, and the LTO@LiF composite material keeps 87% of its initial discharge capacity in 300 1C cycles at 60 °C. Moreover, the LiF coating layer exhibits a special self-driven reforming process during the initial cycles, which makes it uniform and more effective at enhancing the stability between electrode/electrolyte interfaces.

CAS / MDL: 7789-24-4
研究领域: 材料科学 · 电化学
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SOLID STATE IONICS · 2019 · IF 2.886

A facile strategy to improve the cycle stability of 4.45 V LiCoO2 cathode in gel electrolyte system via succinonitrile additive under elevated temperature

Ning Xu,Hebing Zhou,Youhao Liao,Guanjie Li,Mengqing Xu,Weishan Li

The rapid capacity fading of LiCoO 2 cathodes under high temperature limits its further development in high energy density of lithium ion batteries , caused by the unmatched liquid electrolyte that tends to decompose when the working potential exceeds 4.2 V (vs. Li + /Li). Gel polymer membrane blended with PEO (poly(ethylene oxide)) and P(VdF-HFP) (poly(vinylidene fluoride- co -hexafluoropropylene)) is used to enhance the oxidative stability of liquid electrolyte in the polymer matrix . In order to maximize the capacity of LiCoO 2 cathode, proper amount of SN (succinonitrile) that helps to construct a stable CEI (cathode electrolyte interface) film is added into the electrolyte. The SN-contained GPE (gel polymer electrolyte) has the highest oxidative decomposition potential of 5.2 V and the lowest interfacial resistance . At 55 °C, the LiCoO 2 /GPE/Li coin-cell keeps 82% of capacity after 350 cycles in 3.0 V ~ 4.45 V at 1 C rate, compared with that of 9% capacity retention using the polyethylene separator saturated with liquid electrolyte. The enhancement in the cyclic stability under elevated temperature attributes to the dual strategies: the GPE guarantees the better oxidative stability by suppressing the further oxidative decomposition of liquid electrolyte, while the high quality CEI film formed by the SN additive protects the structural integrity of LiCoO 2 cathode.

研究领域: 材料科学 · 电化学
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Energy Technology · 2022 ·Vol. 10 ·期 9 ·2200163 · IF 4.149

Achieving the Interface Stability of LiMn2O4 Cathode Using Aqueous Polyacrylic Acid/acrylate Copolymer and Nanoscale CaCO3 to Improve the High-Temperature Cycling and Storage Performance of Lithium-Ion Batteries

Yan Cui,Jiahui Chen,Jingyang Zhao,Zhen Ma,Yuming Tan,Jianjun Xue,Hanliang Xu,Junmin Nan

Based on a strategy of stabilizing the LiMn 2 O 4 (LMO) cathode interface, the high-temperature cycling and storage performance of 18 650-type LMO/graphite lithium-ion batteries (LIBs) is effectively improved. The LMO cathode is prepared using lithium carboxymethyl cellulose (CMCLi)–polyacrylic acid/acrylate copolymer composite binder and nanoscale CaCO 3 functional component (marked as binder C). Compared with the traditional oily binder, the dissolution of Mn 2+ from LMO cathode into the electrolyte can effectively decrease, and the structure stability of LMO cathode can increase. The batteries exhibit retention capacity of 80.3% at 1 C after 600 cycles at room temperature and 76.7% at 1 C after 200 cycles at temperature of 45 °C. The high-temperature storage performance is also improved and there are 81.1% and 73.5% residual capacities when the fully charged batteries are stored in 60 °C for 14 and 28 days. The enhanced performance is mainly attributed to the interfacial stability of LMO cathode due to the bonding ability of composite binders and the elimination of HF by CaCO 3 . These results reveal the application prospect of as-developed aqueous binders and provide a way to improve the performance of LMO-based LIBs through stable interface strategy.

CAS / MDL: 471-34-1
研究领域: 材料科学 · 电化学 · 电池技术
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Aminoalkyldisiloxane as effective electrolyte additive for improving high temperature cycle life of nickel-rich LiNi0.6Co0.2Mn0.2O2/graphite batteries

Xiaodan Yan,Cheng Chen,Xuequan Zhu,Lining Pan,Xinyue Zhao,Lingzhi Zhang

A novel aminoakyldisiloxane compound, (3-( N, N -dimethylamino)diethoxypropyl) pentamethyldisiloxane (DSON), is reported as an effective electrolyte additive for improving the electrochemical performances of high energy density power batteries of nickel-rich LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622)/graphite. The NCM622/graphite cells using DSON addition in the carbonate-based reference electrolyte exhibit enhanced electrochemical performances, especially high temperature performances including long cycle life and high temperature storage. The pouch cell (1 Ah) with 0.2 wt% DSON retained a capacity of 88% as compared with 84% for that without DSON in electrolyte after 200 cycles at 45 °C. The mechanism investigation reveals that DSON acts as a film-forming additive for constructing uniform conductive cathode electrolyte interphase (CEI) layer upon NCM622 particles, which suppresses the internal cracks and prohibits the irreversible phase transformation of NCM622. DSON also serves as an effective water/acid scavenger and inhibits the hydrolysis of LiPF 6 , thus effectively blocking the occurrence of side reactions and the dissolution of transition metal ions from cathode. Therefore, NCM622 cathode sheet maintains a better integrity surface morphology after 100 cycles. This work demonstrates that aminoakyldisiloxane is promising for practical use as effective electrolyte additive for high energy density power batteries of nickel-rich NCM/graphite.

CAS / MDL: 872-50-4
研究领域: 电化学 · 材料科学
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Journal of Energy Storage · 2025 · IF 9.8

Suppression elevated-temperature transition metal dissolution in LiNi0.5Mn1.5O4 cathode via a HF-resistant bis[3-(trimethoxysilyl)propyl]amine coating

Liqin Xiong,Zheng Cheng,Guorong Hu,Yanbing Cao,Zhongdong Peng,Bin Zhang,Ke Du

High-voltage spinel LiNi 0.5 Mn 1.5 O 4 (LNMO) emerges as an ideal cathode for high energy density lithium-ion batteries due to its 4.7 V operating voltage and low-cost manganese-rich composition. However, the severe interfacial degradation caused by transition metal dissolution and pervasive electrolyte decomposition compromises practical viability in commercial lithium-ion batteries, critically under elevated-temperature operation. To address this problem, we constructed a covalently anchored bis[3-(trimethoxysilyl)propyl]amine (BTPA) coating layer on the LNMO surface through atomic-scale grafting. The BTPA-coated LNMO confers exceptional cyclic stability and rate capability, representing a transformative advancement in cathode performance. At 50 °C, BTPA-coated LNMO cathode maintains 96.10 % capacity retention after 100 cycles at 1C, significantly outperforming pristine LNMO (58.92 % retention), while demonstrating exceptional rate capability with 109.42 mAh·g −1 delivered at 10C compared to 92.71 mAh·g −1 for the pristine LNMO. The synergistic suppression of Mn 3+ formation and parasitic reactions underpins unprecedented high-temperature cyclability, establishing a paradigm for extreme-condition energy storage.

CAS / MDL: 2530-85-0
研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 界面化学 · 锂离子电池
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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 POWER SOURCES · 2020 · IF 8.247

1,4-Phenylene diisocyanate (PPDI)-containing low H2O/HF and multi-functional electrolyte for LiNi0·6Co0·2Mn0·2O2/graphite batteries with enhanced performances

Wenlian Wang,Tianxiang Yang,Shuai Li,Jing Lu,Xiaoyang Zhao,Weizhen Fan,Chaojun Fan,Xiaoxi Zuo,Shaolong Tie,Junmin Nan

Lithium-ion batteries (LIBs) with high-nickel ternary material cathode can provide a high specific capacity but are more sensitive to the H 2 O/HF contents and functional additives in the electrolyte. In this work, 1,4-phenylene diisocyanate (PPDI) is developed as an H 2 O/HF scavenger and film-forming electrolyte additive to enhance the performances of pouch LiNi 0 · 6 Co 0 · 2 Mn 0 · 2 O 2 (NCM622)/graphite batteries. Compared with batteries containing the blank electrolyte, the electrochemical performances of batteries with the PPDI-containing electrolyte can be significantly improved. Thereinto, after 600 cycles at room temperature (25 °C) and 300 cycles at high temperature (45 °C), the capacity retentions for the batteries with the PPDI-containing electrolyte are 84.9% and 81.3% at 1C, while the rates for the batteries with the blank electrolyte are only 29.3% and 14.4%, respectively. With the aid of theory calculations and spectroscopic characterization, the reasons behind the performance enhancement are elucidated, and the reaction mechanism of PPDI and H 2 O/HF is proposed. It is demonstrated that PPDI can scavenge H 2 O/HF in the electrolyte and form stable and highly conductive films on two electrodes to stabilize NCM622 and improve battery performances. Besides the functionalized electrolyte, this work can also inspire new ideas to develop functionalized electrolytes for high-performance NCM622-based LIBs.

CAS / MDL: 104-49-4
研究领域: 材料科学 · 电化学 · 能源存储 · 电池技术
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SOLAR ENERGY MATERIALS AND SOLAR CELLS · 2025 · IF 6.3

Mn/al/Ce ternary-doped CaO composites for ultra-stable and solar-enhanced calcium looping thermochemical energy storage: Synergistic effects and atomic-level insights

Qingyang Mei,Hui Liu,Jinjia Wei

To address the challenges of structural degradation and low solar absorptivity in calcium-based thermochemical energy storage systems under high-temperature cycling, we propose a novel Mn/Al/Ce ternary-doped CaO composite (Ca10Mn1Al1Ce1) optimized for solar-driven calcium looping applications. Through a sol-gel synthesis strategy, the co-doping strategy synergistically integrates structural stabilization mediated by Ca 2 MnO 4 /Ca 3 Al 2 O 6 frameworks, carbonation kinetics enhancement through CeO 2 -induced oxygen vacancies, and Mn element doping, significantly improving the material's solar energy absorption performance. The optimized material demonstrates unprecedented cycling stability with only 5.6 % energy density decay over 200 cycles, outperforming pure CaO (73.5 % degradation after 100 cycles). Kinetic analysis reveals accelerated calcination rates enabled by Mn doping, while DFT calculations confirm an 18.3 % reduction in CaCO 3 decomposition energy barriers. Remarkably, the composite achieves a 3.9-fold enhancement in solar absorptivity through synergistic full-spectrum light harvesting. This work establishes a multifunctional doping strategy that simultaneously addresses sintering resistance, solar absorptance, and reaction kinetics, offering a promising pathway for next-generation concentrated solar power plants requiring high-temperature, long-cycle thermochemical energy storage.

研究领域: 储能材料 · 太阳能转换 · 热化学 · 固态化学 · 材料科学 · 化学工程
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