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ACS Applied Energy Materials · 2021 · IF 6.024

Interfacial Enhancement of Silicon-Based Anode by a Lactam-Type Electrolyte Additive

Gaopan Liu,Tianpeng Jiao,Yong Cheng,Ke Zhou,Yue Zou,Mingsheng Wang,Yong Yang,Jianming Zheng

A silicon-based anode is being developed for industrial application in lithium-ion batteries (LIBs) because of its extremely high theoretical specific capacity. However, the large volume variation during de/lithiation and poor interfacial stability issues cause rapid capacity decay, hindering its practical application. Herein, from the interfacial stabilization point of view, a lactam-based electrolyte additive, namely, N-acetylcaprolactam (donated as NACA), is explored to construct a flexible, robust, and protecting solid electrode interphase (SEI) on the SiOx/C electrode surface. On one hand, due to a stronger complexation with PF5/HF/H2O, NACA functions well in stabilizing the LiPF6 salt, thereby mitigating the corrosion of HF toward the SiOx/C electrode. On the other hand, the NACA-derived interphase could be well adapted to the huge volume change of the silicon electrode. As a consequence, the Li||SiOx/C battery with 2% NACA shows an increase in capacity retention by 15.6% at 30 °C and by 20.8% at 45 °C at 0.5C compared to the baseline. Meanwhile, the cycling performance of the NCM90 cathode is also improved with the NACA additive. Our work provides valuable understanding for seeking more effective amide-based additives for a silicon-based electrode and for the development of functional electrolytes for high-energy-density LIBs.

CAS / MDL: 1888-91-1
研究领域: 材料科学 · 电化学 · 能源存储
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-13 · IF 15.7

Air-stable Li5FeO4 additive enabled by carbon coating for energy-dense lithium-ion batteries

Liu Canshang,Zhang Hao,Zhou Weiwei,Tian Xu,Zhang Tiantian,Niu Sicheng,Li Jianing,Cao Minglei,Wang Qin,Lv Fei,Peng Tangping,Tao Lijuan,Rang Xiaodong,Chen Zhicheng,Su Xin

Li 5 FeO 4 is a promising pre-lithiation additive for the positive electrode in lithium-ion batteries, offering the potential to enhance energy density. However, its susceptibility to air degradation presents a significant challenge for commercialization. In this study, we develop an effective carbon coating strategy utilizing pitch to improve the air stability of Li 5 FeO 4 . The coating process results in the formation of a compact carbon layer on the surface of Li 5 FeO 4 particles, enabling the coated Li 5 FeO 4 to retain a high specific capacity of 743.4 mAh g −1 after 72 h of exposure to air with 20% relative humidity. This retention represents 92.3% of its initial capacity and 85.7% of its theoretical maximum capacity. In contrast, uncoated Li 5 FeO 4 undergoes rapid degradation, losing most of its electrochemical activity within just 4 h under identical conditions. Beyond improving air stability, the carbon coating enhances Li 5 FeO 4 ’s specific capacity, rate capability, and cycling stability. To substantiate the practical application of carbon-coated Li 5 FeO 4 , we construct a pouch-type cell, which exhibits a 13.7% increase in energy density compared to the cell without the prelithiation additive. These findings collectively suggest that the carbon-coated Li 5 FeO 4 represents a viable strategy for advancing the commercial deployment of this material in lithium-ion batteries.

CAS / MDL: 24937-79-9 872-50-4
研究领域: 材料科学 · 电化学 · 储能
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CERAMICS INTERNATIONAL · 2019 ·Vol. 45 ·期 8 ·10633-10639 · IF 3.45

Improved cycling performance of CeO2-inlaid Li-rich cathode materials for lithium-ion battery

Guorong Hu,Zhichen Xue,Zhongyuan Luo,Zhongdong Peng,Yanbing Cao,Weigang Wang,Yuexi Zeng,Yong Huang,Yong Tao,Tianfan Li,Zhiyong Zhang,Ke Du

The Li-rich cathode material for long cycle performance and long-term storage performance is a challenge for next-generation lithium-ion batteries due to the rapid capacity degradation over cycling and the formation of residual lithium on the surface during long-term storage. Herein, an elevated performance of Li 1.2 Mn 0.54 Ni 0.13 Co 0.13 O 2 materials via CeO 2 inlay is reported, which was prepared from Li 1.2 Mn 0.54 Ni 0.13 Co 0.13 O 2 by sol-gel inlay with CeO 2 . It was proved by scanning electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy that cerium oxide cladding not only covered the surface of the material but also diffused into the interior of the material change crystal structure. Cerium oxide on the cladding not only reduces the material's contact with water and carbon dioxide in the air, but also prevents the material from being corroded by electrolyte during electrochemical test. The position of the transition metal atom is replaced Ce atoms, which increases the unit cell volume and the stability of the Li-rich material during the cycling. The results show that the storage property and the electrochemical cycling property of the material have been improved obviously. The CeO 2 inlaid lithium rich material discharged 204.6 mAh/g for the first time at the current of 1C, and 164.4 mAh/g after 150 charge and discharge cycles with corresponding capacity retention rate of 80.35%, compared with the retention rate of 57.26% for pristine Li-rich material capacity. After being stored in humid air for 40 days, the CeO 2 inlaid lithium-rich material showed better electrochemical performance than the pristine one. It is powerfully demonstrated that the CeO 2 inlay strategy here holds huge promise for surface modification of electrode materials for lithium-ion batteries.

研究领域: 材料科学 · 电化学 · 锂离子电池 · 能源存储 · 无机非金属材料
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 12 ·120535 · IF 4.316

Reactivating Dead Li by Shuttle Effect for High-Performance Anode-Free Li Metal Batteries

Jie Chen,Bin He,Zexiao Cheng,Zhixiang Rao,Danqi He,Dezhong Liu,Xiang Li,Lixia Yuan,Yunhui Huang,Zhen Li

Anode-free Li metal batteries are considered the ultimate configuration for next-generation high energy-density Li-based batteries due to the elimination of excess Li metal. However, the limited Li source aggravates issues such as dendrite growth and “dead” Li formation. Any Li loss caused by the SEI formation and dead Li has a great influence on the performance of the full cell. Here, we introduce LiI with shuttle effect to suppress the Li dendrites and reactivate the dead Li in the anode-free LiFePO4 (LFP) ∣Cu full cells. During cycling, the iodine transforms between I− and I3−, and a chemical reactions occur spontaneously between I3− and Li dendrites or dead Li. The generated Li+ in the electrolyte remains active in the following cycling. The anode-free LFP∣Cu cells deliver an initial discharge capacity of 139 mAh g−1 and maintain capacities of 100 mAh g−1 with a capacity retention of 72% after 100 cycles. Both the anode-free LFP∣Cu coin cells and pouch cells with LiI additive show much-improved performances. This work provides a new strategy for high-performance anode-free Li metal batteries.

研究领域: 电化学储能 · 材料科学 · 能源化学 · 电池技术
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IONICS · 2018 ·Vol. 25 ·期 6 ·2563-2574 · IF 2.347

Effects of functional binders on electrochemical performance of graphite anode in potassium-ion batteries

Wu Xuan,Xing Zheng,Hu Yi,Zhang Ya,Sun Yongwen,Ju Zhicheng,Liu Jinlong,Zhuang Quanchao

Electrochemical properties of the graphite electrode in potassium-ion batteries (KIBs) depend on the selection of the proper binder. The results in our experiment show that compared with the conventional binders of poly(vinylidene fluoride) (PVDF) and carboxymethylcellulose sodium (CMCNa), the polyacrylate sodium (PAANa) binder can greatly improve the electrochemical performance during the potassiation and depotassiation. Specifically, the initial discharge and charge capacity of the graphite-PAANa electrode are 415.4 and 238.5 mAh g −1 , respectively. Even after 50 cycles, it still has a high charge capacity retention of 96.9 % . Considering the good swelling property of the PAANa binder, the adhesive and mechanical strength of composite electrodes are obviously enhanced. In addition, the graphite-PAANa electrode can also decrease the electrolyte decomposition on the graphite particle surface and restrain the capacity fading resulted from the repeatedly volume expansion.

研究领域: 电化学 · 能源材料 · 电池技术 · 材料科学 · 应用物理
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Journal of Energy Chemistry · 2016 ·Vol. 26 ·期 3 ·481-487 · IF 2.322

Amorphous Zr(OH)4 coated LiNi0.915Co0.075Al0.01O2 cathode material with enhanced electrochemical performance for lithium ion batteries

Zhen Zhang,Pengfei Zhou,Huanju Meng,Chengcheng Chen,Fangyi Cheng,Zhanliang Tao,Jun Chen

LiNi 0.915 Co 0.075 Al 0.01 O 2 (NCA) with Zr(OH) 4 coating is demonstrated as high performance cathode material for lithium ion batteries (LIBs). The coated materials are synthesized via a simple dry coating method of NCA with Zr(OH) 4 powders, and then characterized with scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Experimental results show that amorphous Zr(OH) 4 powders have been successfully coated on the surface of spherical NCA particles, exhibiting improved electrochemical performance . 0.50   wt% Zr(OH) 4 coated NCA delivers a capacity of 197.6   mAh/g at the first cycle and 154.3   mAh/g after 100 cycles with a capacity retention of 78.1% at 1 C rate. In comparison, the pure NCA shows a capacity of 194.6   mAh/g at the first cycle and 142.5   mAh/g after 100 cycles with a capacity retention of 73.2% at 1 C rate. Electrochemical impedance spectroscopy (EIS) results show that the coated material exhibits a lower resistance, indicating that the coating layer can efficiently suppress transition metals dissolution and decrease the side reactions at the surface between the electrode and electrolyte. Therefore, surface coating with amorphous Zr(OH) 4 is a simple and useful method to enhance the electrochemical performance of NCA-based materials for the cathode of LIBs.

研究领域: 电化学 · 材料科学 · 能源存储 · 电池技术 · 无机非金属材料 · 固态化学
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CHEMICAL COMMUNICATIONS · 2017 ·Vol. 53 ·期 11 ·1805-1808 · IF 6.319

Investigation of K3V2(PO4)3/C nanocomposites as high-potential cathode materials for potassium-ion batteries

Jin Han,Guan-Nan Li,Feng Liu,Minqiang Wang,Yan Zhang,Linyu Hu,Chunlong Dai,Maowen Xu

Novel K3V2(PO4)3 and three-dimensional conductive network K3V2(PO4)3/C nanocomposites are successfully fabricated and further evaluated as cathode materials for potassium-ion batteries for the first time. The K3V2(PO4)3/C nanocomposite exhibits a high-potential platform of 3.6–3.9 V and a good capacity retention of at least 100 cycles. This work may provide new insight into developing cathode materials for potassium-ion batteries.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Sustainable Cathodic Performances of VS4 in Rechargeable Magnesium Batteries by Cobalt Substitution

Muhammad Kashif Naseem,Mian Azmat,Changliang Du,Muhammad Ismail,Hajra Baig,Rong Jiang,Asif Ali,Meishuai Zou,Youqi Zhu,Chuanbao Cao

Vanadium tetrasulfide (VS4) is one of the most promising cathodic materials for rechargeable magnesium battery systems (RMBSs). Elemental substitution to expand layers, creation of sulfur vacancies, and reduction of particle sizes of VS4 are undoubtedly effective strategies to enhance cathodic performances. Experimental and DFT analysis revealed that valence states of vanadium and cobalt have been elevated from V2+ to V3+ and Co2+ to Co3+ in VS4 and that the Co–S bond length shortened due to cobalt substitution, which resulted in enhanced overall internal polarization in the layered atomic structure of VS4 by increasing cobalt concentrations. This phenomenon of charge accumulation contributes toward regulated magnesiation and accommodated volume expansion while cycling, resulting in the enormous structural stability of VS4 and sustainable battery performance during a long and stable cycling at a cost of 20% capacity diminution as compared to pristine VS4 in RMBS. Hence, 9% CoVS4 demonstrated a capacity of 158 mAh g–1 at a current density of 500 mA g–1 with approximately 98% capacity retention after 1000 cycles. Sustainable cathodic performance is the most desirous feature for commercialization. This work provides insight realization regarding structural limitations and opportunities of VS4 for sustainable cathodic performances in RMBS with non-nucleophilic 0.25 mol/L (R-PhOMgCI)2-A1Cl3/THF (PMC) electrolyte and has laid a theoretical plus experimental foundation for future developments.

CAS / MDL: 2386-64-3 62-55-5
研究领域: 材料科学 · 电化学 · 电池技术
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Journal of Energy Chemistry · 2024 · IF 14

Achievable dual-strategy to stabilize Li-rich layered oxide interface by a one-step wet chemical reaction towards long oxygen redox reversibility

Bin He,Yujie Dai,Shuai Jiang,Dawei Chen,Xilong Wang,Jie Song,Dan Xiao,Qian Zhao,Yan Meng,Wei Feng

Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structural degradation of high energy-density Li-rich layered oxide (LLO), leading to voltage and capacity fading. Herein, the dual-strategy of Cr x B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature. Density functional theory (DFT) calculations prove that stable B–O and Cr–O bonds through the local gradient doping can significantly reduce the high-energy O 2 p states of interfacial lattice O, which is also effective for the near-surface lattice O, thus greatly stabilizing the LLO surface. Besides, differential electrochemical mass spectrometry (DEMS) indicates that the Cr x B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions, including allowing speedy Li + migration. The voltage and capacity fading of the modified cathode (LLO-CrB) are adequately suppressed, which are benefited from the uniformly dense cathode electrolyte interface (CEI) composed of balanced organic/inorganic composition. Therefore, the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g −1 (with a retention rate of 95.1%). This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.

CAS / MDL: 13762-51-1
研究领域: 材料科学 · 电化学 · 能源存储
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Advanced Composites and Hybrid Materials · 2022 ·Vol. 5 ·期 4 ·2988-3001 · IF 11.806

Synergistic effect of tailored 3D/2D Ti3C2Tx/CoS2/C nanostructured composite anode for significantly enhanced Li-ion storage

Zhao Xiaoyu,Zhang Yingbing,Hou Yongdan,Zhao Zijian,Gong Yaxin,Wang Yanfei,Wei Huige,Pol Vilas G.

A beneficial strategy for enhancing the electronic conductivity of transition metal chalcogenides (TMCs) as lithium-ion battery anode material is through shortening the charge transfer path between the sulfide particles. However, the combination between the carbon-based matrix and electroactive materials is sometimes weak, which hinders the cycling stability. In this paper, the Ti-based MXene, T 3 C 2 T x , was used as a conductive frame, combined with the ZIF-67-based CoS 2 /C grains yielding Ti 3 C 2 T x /CoS 2 /C composite electrode through one-step and two-step synthesis methods, which displayed significantly enhanced capacity, rate performancem, and cycling stability. The compsoite reached a capacity retention of 82.6% after 100 cycles with a significantly higher capacity of 1020.5 mAh/g at 0.2 A/g current density. After 100 discharge–charge cycles, the Ti 3 C 2 T x /CoS 2 /C composite revealed a low volume expansion of 9.5%, suggesting superior structural integrity and stability with the synergistic effect of both MXene 2D and CoS 2 /C 3D nanostructures. Graphical abstract

研究领域: 材料科学 · 电化学 · 能源存储
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IONICS · 2022 ·Vol. 28 ·期 7 ·3269-3276 · IF 2.961

High-performance lithium-ion batteries with gel polymer electrolyte based on ultra-thin PVDF film

Shi Tianze,Kang Shuai,Zhang Kun,Xue Fengjuan,Lu Wenqiang

Both reducing the liquid electrolyte and solid electrolyte have been acting as novelty strategy for commercial lithium-ion batteries avoiding safety problems such as fires and explosion which is mostly caused by the liquid organic electrolyte flammability. However, reducing the liquid electrolyte leads to capacity loss and energy fade of batteries. Here, we synthesized ultra-thin film of polyvinylidene fluoride (PVDF)-based gel polymer electrolyte (GPE), which also act as the separator, with trace amount electrolyte solution as a whole system to explore the optimized balance between safety and capacity of these new batteries. Both battery rate performance and cyclic stability are significantly improved when the thickness of the polymer electrolytes decrease to 20 μm. Furthermore, the batteries exhibit excellent cyclic stability when a minimum of 5 μl liquid electrolytes was added to the surface of the thin PVDF film (110.9 mAh·g −1 with a capacity retention of 78.6% at 0.5C after 150 cycles). It should be noted that the maximum discharge-specific capacity and discharge-specific capacity after 150 cycles of 5 μl-LFP/GPE-20/GC cell is 1.29 and 1.44 times larger than that of commercial cells. All the experiment results above might provide an optimization technical route and process for real applications in future lithium-ion batteries.

研究领域: 材料科学 · 能源技术 · 电化学
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Nanoscale · 2025 ·Vol. 17 ·期 10 ·6049-6057 · IF 5.1

Facile synthesis of Si/C composites for high-performance lithium-ion battery anodes

Jiasheng Chen,Xuanliang Wang,Zhaoping Deng,Eun Mi Kim,Sang Mun Jeong

Nanotization and surface coating of silicon (Si) particles are effective methods to mitigate volume expansion and protect the solid electrolyte interphase (SEI) film during charge and discharge cycles. We utilized a magnesium-thermal reduction process to form nano-sized Si particles and applied a simple spray solidification and calcination technique to coat the surface with carbon (Si/C). The resulting carbon-coated core-structured Si/0.01C composite, with an optimal carbon layer, exhibits outstanding electrochemical performance. Specifically, it demonstrates a discharge capacity of 3119 mA h g−1 at a current density of 0.2 A g−1 and 1010 mA h g−1 at 2 A g−1. When employed in lithium-ion batteries (LIBs), the Si/0.01C electrode maintains a discharge capacity of 1159 mA h g−1 after 173 cycles, with an impressive capacity retention of 85.8% between cycles 73 and 173, measured at 1 A g−1. This assessment of its continuous cycling performance at 1 A g−1 followed initial C-rate characterization (0.2 → 0.4 → 0.6 → 0.8 → 1 → 2 → 0.2 → 1 A g−1). The enhanced capacity and cycling stability of the carbon-coated Si/C composite compared to those of pure Si nanoparticles are attributed to the encapsulation of Si nanoparticles within the carbon layer, which mitigates volume expansion.

CAS / MDL: 25014-41-9
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