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Science China-Chemistry · 2025 · IF 9.7

Controllably elevating the initial Coulombic efficiency of Li3VO4 anode via a facile electrode pre-lithiation technique for lithium-ion batteries

Liang Haoyue,Zhong Xingguo,Huang Guxin,Liu Wenpan,Liu Yao,Wang Shuhao,Wang Deyu,Liu Hao,Wang Hao,Zhai Tianyou,Li Huiqiao

Li 3 VO 4 has been a promising insertion anode material for Li-ion batteries, which has high theoretical capacity (up to ∼600 mAh g −1 ) and safe Li insertion voltage (0.5–1 V vs. Li/Li + ). However, the low initial Coulombic efficiency (ICE) has always been the bottleneck limiting its commercialisation. Here, we propose a facile pre-lithiation method to controllably elevate the ICE by the post-treatment of the prepared Li 3 VO 4 composite electrode based on an immersion reaction. In this process, the whole electrode was immersed in the liquid Li source, via which the ICE of the Li 3 VO 4 electrode can be controllably elevated from 80% to over 100% within 5 min of pre-lithiation. Rather than the traditional powder treatment for pre-lithiation, this process we proposed minimizes the impact of pre-lithiation on the battery assembly process. Moreover, we further investigated the effect of this pre-lithiation process on the functional components in the electrode. For the first time the ICE of Li 3 VO 4 electrode was elevated to 100%. As a result, the initial reversible capacity of LiFePO 4 ∥Li 3 VO 4 full cell was improved from 44.0 to 146.3 mAh g −1 , demonstrating the feasibility and great potential of the process.

CAS / MDL: 9004-32-4 9085-26-1
研究领域: 材料科学 · 电化学 · 能源存储
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CHEMISTRY OF MATERIALS · 2015 · IF 8.354

Hierarchically Designed Germanium Microcubes with High Initial Coulombic Efficiency toward Highly Reversible Lithium Storage

Chuanjian Zhang,Zhou Lin,Zhenzhong Yang,Dongdong Xiao,Pu Hu,Hongxia Xu,Yulong Duan,Shuping Pang,Lin Gu,Guanglei Cui

Germanium has been investigated intensively for its high specific capacity and tough nature, which make it a promising candidate anode for high energy lithium-ion batteries. However, the rational design of a germanium electrode with enhanced electrochemical performances is still a big challenge. Herein, we designed and synthesized germanium microcubes with a hierarchical structure directly on titanium foil via a simple hydrogen reduction method. An ultrahigh initial Coulombic efficiency of 91.8% was acquired due to the high crystallinity of germanium for reversible lithium insertion and extraction, less adverse side reaction for irreversible lithium loss, and unique hierarchical structure for easier electrolyte penetration. In addition, the Li2CO3-predominated solid electrolyte interface contributes significantly to the excellent cycling and rate performances of the anode. Both half and full cell performances demonstrate that germanium has potential applications in high-performance lithium-ion batteries.

CAS / MDL: 1310-53-8
研究领域: 材料科学 · 电化学
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Carbon Energy · 2022 ·Vol. 5 ·期 2 ·e257 · IF 21.556

Highly N-doped carbon with low graphitic-N content as anode material for enhanced initial Coulombic efficiency of lithium-ion batteries

Yihua Tang,Jingjing Chen,Zhiyong Mao,Christina Roth,Dajian Wang

N-doped carbons as one of the most prominent anode materials to replace standard graphite exhibit outstanding Li + storage performance. However, N-doped carbon anodes still suffer from low N-doping levels and low initial Coulombic efficiency (ICE). In this study, high N-doped and low graphitic-N carbons (LGNCs) with enhanced ICE were synthesized by taking advantage of a denitrification strategy for graphitic carbon nitride (g-C 3 N 4 ). In brief, more than 14.5 at% of N from g-C 3 N 4 (55.1 at% N) was retained by reacting graphitic-N with lithium, which was subsequently removed. As graphitic-N is largely responsible for the irreversible capacity, the anode's performance was significantly increased. Compared to general N-doped carbons with high graphitic-N proportion (>50%) and low N content (<15 at%), LGNCs delivered a low proportion of 10.8%–17.2% within the high N-doping content of 14.5–42.7 at%, leading to an enhanced specific capacity of 1499.9 mAh g −1 at an ICE of 93.7% for the optimal sample of LGNC (4:1). This study provides a facile strategy to control the N content and speciation, achieving both high Li + storage capacity and high ICE, and thus promoting research and application of N-doped carbon materials.

CAS / MDL: 108-78-1
研究领域: 材料科学 · 能源存储
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2024 ·Vol. 35 ·期 14 ·1-13 · IF 2.8

The facile preparation and performances of prelithiated silicon oxide anode materials

Hou Chunping,Yue Zeyu,Sun Hehang,Zhai Lidong,Xie Haidong,Tian Hui,Qu Yuqing,Wang Xinwei,Hou Jiao

Silicon oxide (SiO x ) anode materials have gained significant attention in lithium-ion batteries due to their high theoretical specific capacity (above 1965 mAh g −1 ), relatively stable cycling performance, and lower production costs. However, SiO x anode materials tend to form a solid electrolyte interphase (SEI) film and generate inert substances like Li 2 O and Li 4 SiO 4 during the initial charge and discharge processes, leading to the consumption of active lithium ions and low initial coulombic efficiency. To address these issues effectively, prelithiation of SiO x anode materials is explored in this study. A lithium powder suspension is prepared by dispersing lithium powder and carbon nanotubes (CNTs) in the electrolyte, served as the prelithiation agent. The SiO/G@C@A anode material is then prelithiated with this agent. The lithium powder suspension prelithiation agent enables effective prelithiation of the anode material. The SiO@C@A-1 anode exhibits improved electrochemical performances. At a current density of 0.1 A g −1 , the initial specific capacity reaches 981.3 mAh g −1 with an initial coulombic efficiency of 95.65%, which is approximately 25% higher than that of the untreated sample. After 100 cycles and at a current density of 0.5 A g −1 , the prelithiated sample retains a discharge specific capacity of 648 mAh g −1 , with a capacity retention rate of 83.27%, around 10% higher than that of the untreated sample, demonstrating excellent cycling performances.

研究领域: 材料科学 · 电化学
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MATERIALS CHEMISTRY AND PHYSICS · 2019 · IF 2.781

Effect of pyrolysis temperature on lithium storage performance of pyrolitic-PVDF coated hard carbon derived from cellulose

Lingfang Li,Changling Fan,Bin Zeng,Muchu Tan

The effect of pyrolysis temperature on the electrochemical performance of cellulose-derived hard carbon as anode material for lithium ion batteries was discussed in detail. Because of the presence of more oxygen-containing groups, the hard carbon pyrolyzed below 700 °C has larger irreversible capacity. The initial coulombic efficiency is low and the capacity decreases rapidly. X-ray photoelectron spectroscopy (XPS)results show that the ratio of C O to C–O bond becomes very small when higher than 800 °C, most of the oxygen-containing groups and hydrogen disappears. Hard carbon obtained at 1100 °C has higher initial coulombic efficiency and better cycle performance, no voltage hysteresis exists. The number of micropores of HC-1100 is much larger than that of mesopores, which reduces the irreversible deposition of lithium ions in mesopores. However, due to the decrease of interlayer space, lithium storage sites become less and the capacity is a bit lower than HC-800 and HC-950. The hard carbon obtained in 800–1000 °C range has the best comprehensive performance in charge-discharge capacity, initial coulombic efficiency and cycle performance.

CAS / MDL: 9004-34-6
研究领域: 材料科学 · 电化学
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ChemSusChem · 2019 ·Vol. 12 ·期 14 ·3377-3382 · IF 7.804

Reactivating Li2O with Nano-Sn to Achieve Ultrahigh Initial Coulombic Efficiency SiO Anodes for Li-Ion Batteries

Rusheng Fu,Yongkang Wu,Chongzhao Fan,Zuxin Long,Guangjie Shao,Zhaoping Liu

Graphical Breaking the ICE : The SiO anode in Li-ion batteries has low initial coulombic efficiency (ICE) because of the irreversible formation of Li 2 O and lithium silicates. Sn-mixed SiO shows great promise to address these issues by reactivating Li 2 O, in the inverse reaction to that occurring at the metal oxide anodes. Sn is shown to form an outstanding conductive phase, which boosts the reaction kinetics and also reactivates Li 2 O. The application of SiO anodes in Li-ion batteries is greatly restricted by its low initial coulombic efficiency (ICE). Usually, a pre-lithiation procedure is necessary to improve the ICE, but the available technologies are associated with safety issues. Metal (M)-mixed SiO shows great promise to address these issues by reactivating Li 2 O through the reaction M+Li 2 O→MO x +Li + , which is the inverse reaction to that occurring at MO x anodes. Sn is found to be a good choice of metal for this concept. Nanoscale Sn-mixed SiO composites are prepared by mechanical milling. Sn forms an outstanding conductive phase, which boosts the reaction kinetics and also reactivates the Li 2 O byproduct. Sn/SiO (1:2 w/w) delivers a significant improvement in ICE from 66.5 % to 85.5 %. A higher ICE value of >90 % is obtained when the Sn content is ≥50 wt %. However, additional electrolyte decomposition occurs, which is catalyzed by Sn. In addition, coarsening of the nano-Sn material reduces the inverse conversion reactivity of Sn/Li 2 O and subsequently results in rapid capacity fading. The quantitative analysis indicates that, in contrast to transition metals, the alloying and dealloying nature of Sn gives a 50 % improvement in reversible capacity, attributed to Sn/Li 2 O. This work gives a general strategy to choose metals for increasing the ICE of SiO x and metal oxides.

CAS / MDL: 18282-10-5
研究领域: 材料科学 · 电化学
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Energy & Environmental Materials · 2021 ·Vol. 5 ·期 1 ·353-359 · IF 15.122

Sn Alloy and Graphite Addition to Enhance Initial Coulombic Efficiency and Cycling Stability of SiO Anodes for Li-Ion Batteries

Xingyang Du,Hanying Zhang,Xuexia Lan,Bin Yuan,Renzong Hu

Silicon monoxide (SiO) has aroused increased attention as one of the most promising anodes for high-energy density Li-ion batteries. To enhance the initial Coulombic efficiencies (ICE) and cycle stability of SiO-based anodes, a new facile composition and electrode design strategy have been adapted to fabricate a SiO–Sn–Co/graphite (G) anode. It achieves a unique structure where tiny milled SiO–Sn–Co particles are dispersed among two graphite layers. In this hybrid electrode, Sn–Co alloys promoted Li + extraction kinetics, and the holistic reversibility of SiO and graphite enhanced the electrical conductivity. The SiO–Sn–Co/G electrode delivered an average ICE of 77.6% and a reversible capacity of 640 mAh g −1 at 800 mA g −1 , and the capacity retention was above 98% after 100 cycles, which was much higher than that of the SiO with an ICE of 55.3% and a capacity retention of 50%. These results indicated that this was reliable method to improve the reversibility and cycle ability of the SiO anode. Furthermore, based on its easy and feasible fabrication process, it may provide a suitable choice to combine other alloy anodes with the graphite anode.

研究领域: 材料科学 · 电化学
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CARBON · 2025 · IF 11.6

LiCl modified graphene by wet ball-milling strategy for high performance lithium-ion battery

Wei Wu,Ranlu Zheng,Yixuan Bai,Qingyi Feng,Bo Li,Yongliang Tang,Hongxiang Deng,Xiaotao Zu,Shuangyue Wang,Xia Xiang

Graphene-based lithium-ion batteries suffer from the poor initial coulombic efficiency and low mass loading. A convenient method is proposed to replenish the Li loss in the first cycle and improve the cycling stability of high mass loading batteries simultaneously in this work. Graphene is modified by introducing LiCl (G/LC) through a wet ball-milling process, which leads to the formation of hybrid solid electrolyte interface. As a result, the half-cells based on high mass loading G/LC electrodes exhibit obviously improved initial coulombic efficiency (>90 %) and high areal specific capacity of 2.53 mAh cm −2 at high current density of 0.55 mA cm −2 . Furthermore, the full-cells based on G/LC anode paired with LiNi 6 Mn 2 Co 2 O 2 cathode deliver a high initial coulombic efficiency of 76.7 %, as well as a high-capacity retention of 97.52 % after 200 cycles, suggesting the potential application of this extend strategy for rechargeable batteries.

CAS / MDL: 64-17-5 7447-41-8
研究领域: 材料科学 · 能源存储
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Chemistry-An Asian Journal · 2025 · IF 3.3

Exploration into the Synthesis and Sodium Storage Characteristics of Hard Carbon Derived from Plastics

Shuai Ruan,Xinping He,Hui Huang,Yongping Gan,Yang Xia,Jun Zhang,Fangfang Tu,Jiayuan Xiang,Wangjun Wan,Chen Wang,Xinhui Xia,Wenkui Zhang

The crux for the advancement of high-performance sodium-ion batteries resides in the development of low-cost, high-performance hard carbon anode materials. In this study, waste plastics are utilized as precursors to prepare plastic-derived hard carbon materials through a simple high-temperature one-step carbonization method, which is particularly suitable for new energy storage devices such as sodium-ion batteries and supercapacitors. Through in-depth exploration, we discover that the initial coulombic efficiency of hard carbon is intimately associated with its structure, within which the PU material exhibits the attributes of high capacity, initial coulombic efficiency and excellent cycle performance, meriting further optimization of hard carbon precursor materials. In this study, a novel idea of preparing high-performance hard carbon anode by a low-carbon and environmentally friendly method is proposed, and the key factors influencing the electrochemical performance of hard carbon materials are revealed, providing a valuable experimental basis for the further development of sodium anodes.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 能源存储
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CARBON · 2024 · IF 10.5

Iron-decorated N/S co-doped porous carbon for sodium-ion battery anode to achieve high initial coulombic efficiency

Tie Ma,Dan Li,ChenQi Wang,Ning Liu,Chao Wang,GuangPing Wu,Li Guo

Hard carbon materials are preferred as anode materials for sodium-ion batteries due to their abundance, low price, and environmental friendliness. However, doping-based modification usually induces low initial coulombic efficiency (ICE), which seriously affects the practical application of carbon materials. In this work, Fe-modified N/S co-doped porous carbon is prepared using the salt template method. Fe, N, and S are uniformly distributed on the porous carbon to form an interwoven network structure, providing abundant active sites. Moreover, during the electrochemical reaction, FeN x effectively catalyzes the generation of solid electrolyte interface (SEI) film, which reduces the consumption of Na + in the side reaction, leading to a high initial coulombic efficiency, and at the same time, the stabilized SEI film accelerates the diffusion of electrons and ions, effectively enhancing the multiplication rate performance. The NFSC exhibits a high specific capacity (371.3 mAh/g) by the co-coordination strategy and a high ICE (85.9 %). This study provides new ideas for research based on the modification of carbon materials.

研究领域: 材料科学 · 电化学
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IONICS · 2023 ·Vol. 29 ·期 6 ·2241-2248 · IF 2.8

Dual function high efficiency silicon electrode prelithiation strategy

Deng Rongfeng,Wang Zhilong,Chen Kanghua

The Si anode holds the most potential among anode materials, however, its low initial coulombic efficiency has been a serious impediment to commercial progress. In this study, we immersed Si electrode in the prelithiation reagent of lithium-biphenyl(Li-Bp)/2-methyltetrahydrofuran(2-Me-THF) for 5 min, resulting in an initial coulomb efficiency was increased to 135%. The full cell assembled with LiFePO 4 has a coulomb efficiency of 89.1% for the first turn and the capacity retention rate of 87.2% after 100 cycles. Prelithiation reagent after drying can form a protective layer on the surface of the Si electrode, and the prelithiated Si electrode can stably exist for more than 9 h at the dew point (DP) of -25 ℃, which provides a strategy for industrial production.

研究领域: 材料科学 · 电化学 · 能源技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Chemical prepotassiation enabling high-efficiency and long-life alloy anodes for potassium-ion batteries

Xinyuan Xiang,Dan Liu,Jiangping Song,Xinxin Zhu,Zhizhong Xie,Haolin Tang,Hua Zheng,Deyu Qu

Using high-capacity alloy anodes can grandly advance potassium-ion batteries. However, one common issue plaguing these anodes is the loss of active K + ions associated with persistent side reactions on unstable electrode-electrolyte interfaces, resulting in low initial Coulombic efficiency (ICE) and shortened cycling life. Herein, we first explore the potential of a solution-based potassiation reagent (potassium-biphenyl in dimethoxyethane, K-Bp/DME) for chemical prepotassiation. With a low redox potential of 0.45 V vs . K + /K, the K-Bp/DME solution can readily pre-storing K + ions into various alloy-type anodes by a simple immersion operation in a few minutes. Taking nanostructured Bi/P/CNT composite as an example, we demonstrate that the K-Bp/DME prepotassiation simultaneously enables the notable ICE improvement (from 51.9% to 96.2%) and long-life cycling (running 700 cycles at 1.5 A g −1 with a tiny capacity attenuation rate of 0.031% per cycle) by forming a KF-rich SEI film. Furthermore, the full cell assembled by coupling the prepotassiated Bi/P/CNT anode with a potassium Prussian blue cathode delivers a desirable ICE of 88.6% and superior capacity retention of 75.3% after 450 cycles at 0.3 A g −1 . Besides, this prepotassiation method is also successfully extended to other anodes (Sb and Sn), indicating its general applicability.

研究领域: 材料科学 · 电化学
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