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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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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Multifunctional High-Efficiency Additive with Synergistic Anion and Cation Coordination for High-Performance LiNi0.8Co0.1Mn0.1O2 Lithium Metal Batteries

Can Liao,Longfei Han,Xiaowei Mu,Yulu Zhu,Na Wu,Jingyi Lu,Yonghui Zhao,Xingjun Li,Yuan Hu,Yongchun Kan,Lei Song

Safety and high energy density have long restricted the large-scale practical application of lithium metal batteries because of the unbridled growth of lithium dendrites and the rapid deteriorating cycle performance of the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode. Herein, an additive of RbNO3 with multiple functions is proposed for dendrite-free NCM811 lithium metal batteries. Benefiting from the electrostatic shielding effect formed by Rb+ during the Li+ deposition process and the solvation effect of NO3– to regulate lithium deposition, a high Coulombic efficiency of 95.02% (compared with the low Coulombic efficiency of 89.37% in the blank electrolyte) is acquired in Li//Cu cells, and the uniform growth of the lithium metal deposition with a large strawberry-like morphology is achieved. Moreover, when a cathode of NCM811 matches with a lithium metal anode, an extraordinary capacity retention of 93.67% after 200 cycles with a high Coulombic efficiency of 99.7% in the electrolyte with the RbNO3 system (a capacity retention of 80.1% with a Coulombic efficiency of 98.0% for the blank electrolyte) is achieved at 1C. This work provides guidance for the development of high-efficiency additives with dual synergistic regulation effects of anions and cations for lithium metal batteries in the future.

CAS / MDL: 13126-12-0
研究领域: 材料科学 · 电化学 · 电池技术
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ADVANCED MATERIALS · 2024 ·Vol. 36 ·期 33 ·2406451 · IF 27.4

Quantifying Asymmetric Zinc Deposition: A Guide Factor for Designing Durable Zinc Anodes

Shixun Wang,Zhaodong Huang,Jiaxiong Zhu,Yiqiao Wang,Dedi Li,Zhiquan Wei,Hu Hong,Dechao Zhang,Qi Xiong,Shimei Li,Ze Chen,Nan Li,Chunyi Zhi

Zinc metal is recognized as the most promising anode for aqueous energy storage but suffers from severe dendrite growth and poor reversibility. However, the coulombic efficiency lacks specificity for zinc dendrite growth, particularly in Zn||Zn symmetric cells. Herein, a novel indicator ( f D ) based on the characteristic crystallization peaks is proposed to evaluate the growth and distribution of zinc dendrites. As a proof of concept, triethylenetetramine (TETA) is adopted as an electrolyte additive to manipulate the zinc flux for uniform deposition, with a corroborating low f D value. A highly durable zinc symmetric cell is achieved, lasting over 2500 h at 10 mA cm −2 and 400 h at a large discharge of depth (10 mA cm −2 , 10 mAh cm −2 ). Supported by the low f D value, the Zn||TETA-ZnSO 4 ||MnO 2 batteries overcome the sudden short circuit and fast capacity fading. The study provides a feasible method to evaluate zinc dendrites and sheds light on the design of highly reversible zinc anodes.

研究领域: 材料科学 · 电化学
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ADVANCED MATERIALS · 2020 ·Vol. 32 ·期 24 ·2001740 · IF 27.398

Colossal Granular Lithium Deposits Enabled by the Grain-Coarsening Effect for High-Efficiency Lithium Metal Full Batteries

Weidong Zhang,Qiang Wu,Jinxin Huang,Lei Fan,Zeyu Shen,Yi He,Qi Feng,Guannan Zhu,Yingying Lu

The low Coulombic efficiency of the lithium metal anode is recognized as the real bottleneck to practical high-efficiency lithium metal batteries with limited Li excess. The grain size and microstructure of deposited lithium strongly influences the lithium plating/stripping efficiency. Here, a solubilizer-mediated carbonate electrolyte that can realize grain coarsening of lithium deposits (>20 µm in width) with oriented columnar morphology, which is in sharp contrast with conventional nanoscale dendrite-like lithium deposits in carbonate electrolytes, is reported. It exhibits improved Li Coulombic efficiency to 98.14% at a high capacity of 3 mAh cm −2 over 150 cycles, because the colossal lithium deposition with minimal tortuosity can maintain the bulk Li with continuous electron conducting pathway during the stripping process, thus enabling efficient Li utilization. Li/NMC811 full batteries, composed of thin Li anode (45 µm) and a high-capacity NMC811 cathode (16.7 mg cm −2 ), can achieve at least 12 times longer lifespan (200 cycles).

CAS / MDL: 7790-69-4 62086-04-8
研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2023 · IF 6.4

ZnO/Carbon Shell/Carbon Cloth as a Stable Host for High Li-Content Anodes

Junqin Xie,Kangning Liu,Sha Fu,Xian-Xiang Zeng,Congshan Zhou,Tong-Tong Zuo,Xiongwei Wu

Among all energy storage systems, lithium metal batteries (LMBs) show great advantages in terms of energy density. Nevertheless, the challenges of lithium metal anodes, namely, dendrite formation and low Coulombic efficiency, hinder the practical application of LMBs. In this work, we used the ZnO/carbon shell/carbon cloth as a host for the lithium metal anode. The introduction of ZnO sites reduces the nucleation barrier of lithium deposition, and the existence of a 3D current collector alleviates the volume change during lithium plating/stripping. In addition, the combination of ZnO/C and 3D carbon cloth decreases the local current density and contributes to uniform lithium plating/stripping. The half cells assembled with modified carbon cloth electrodes cycle for more than 125 cycles with a high Coulombic efficiency of 99.34%, even under a high areal capacity of 6 mA h cm–2. By and large, our work provides a simple and effective strategy to modify the current collector for high Li-content anodes.

CAS / MDL: 693-98-1 10196-18-6
研究领域: 材料科学 · 能源存储
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INORGANIC CHEMISTRY · 2025 · IF 4.7

In Situ Assembly Engineering-Induced 3D MOF-Driven MXene Framework for Highly Stable Na Metal Anodes

Yiming Zhang,Zhipeng Li,Baihua Qu,Xing Shen,Le Tong,Jin Wang,Jingqin Cui,Xin Li,Qingshui Xie,Jingfeng Wang

Sodium metal, with its high theoretical capacity, low redox potential, and cost-effectiveness, presents a promising anode candidate for next-generation high-energy-density batteries. However, the development of Na metal anodes is significantly challenged by issues such as uncontrolled dendrite growth, uncontrolled volume expansion, and associated safety concerns. Designing and developing advanced materials to enhance the conductivity of sodium metal anodes and promote uniform sodium ion deposition are of urgent importance. Herein, a MXene-based hybrid material was developed by integrating MOF-derived Zn, Co, N, and C dopants with Ti3C2Tx MXene to serve as a hosting substrate for the Na metal anode. The MXene provided a conductive framework, while the MOF-derived dopants introduced sodiophilic sites, promoting uniform Na deposition and mitigating volume expansion. The optimized material demonstrated an average Coulombic efficiency of 99.99% over 3000 cycles and stable cycling for over 5000 h in symmetrical cells and maintained over 80% capacity retention at 3 C after 500 cycles in full-cell tests, highlighting its potential as a robust Na metal anode material.

CAS / MDL: 7722-76-1
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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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Redox mediator-regulated microbial electrolysis cell to boost coulombic efficiency and degradation activity during gaseous chlorobenzene abatement

Zanyun Ying,Han Chen,Zheng He,Yutao Hu,Zhipeng Huang,Jialing Gao,Xinya Wang,Jiexu Ye,Jingkai Zhao,Shihan Zhang,Jianmeng Chen

Microbial electrolysis cell (MEC), a promising technology, is being developed for volatile organic compounds (VOCs) abatement. One of the critical issues to limit its industrial application is the poor electron transfer . In this work, anthraquinone-2,6-disulfonate (AQDS) and flavin mononucleotide (FMN) are dosed to MECs for the chlorobenzene (CB) removal, which are denoted as MEC-AQDS and MEC-FMN, respectively. The MEC performance is significantly promoted due to that RMs lower down the internal resistance. The CB removal efficiency in MEC-AQDS and MEC-FMN are increased by 40% and 20%, respectively, compared with neat MEC. Moreover, EC max and K s of MEC-AQDS are 26% and 75% higher than that of neat MEC, respectively. AQDS is a more suitable RM with 66% and 50% higher in dechlorination efficiency and coulombic efficiency, respectively, compared with FMN. The enhancement of dechlorination process in MEC-AQDS is ascribed to two reasons. The lower resistance accelerates the electron transfer rate during dechlorination; and the enhancing growth of dechlorinating bacterium leads to an abundant excretion of dechlorination enzymes. Additionally, electrochemical analysis and intermediate detection imply that RMs affect the electron transfer pathways but not the degradation mechanism , that is, CB converts into 2-chlorophenol and 3-chlorocatechol successively, then ring-opens and dechlorinates for mineralization .

研究领域: 环境科学 · 微生物学
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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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Research · 2019 · IF 0

Synergistic Effects of Salt Concentration and Working Temperature towards Dendrite-Free Lithium Deposition

Panlong Li,Chao Li,Yang Yang,Chanyuan Zhang,Renhe Wang,Yao Liu,Yonggang Wang,Jiayan Luo,Xiaoli Dong,Yongyao Xia

The lithium- (Li-) metal anode is crucial for developing high-energy-density batteries, while its dendritic growth and the low charge/discharge Coulombic efficiency in organic electrolytes hinder its practical application. Herein, we employed an in situ optical microscope to investigate the effect of the electrolyte concentration and the working temperature on the Li-plating/-stripping process. It is found that a higher concentration electrolyte can suppress its side reaction to improve the charge/discharge Coulombic efficiency, and a higher temperature can help lithium plate/strip uniformly with less lithium dendritic growth. An average Coulombic efficiency was obtained as high as 99.2% for over 150 cycles with a fixed plating capacity of 2 mAh cm-2 on copper foil in a 3 mol/kg ether-based electrolyte under 60°C, which provides an efficient and facile strategy for developing high-performance Li-metal batteries.

研究领域: 材料科学 · 电化学
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IONICS · 2020 ·Vol. 26 ·期 8 ·3841-3851 · IF 2.394

Morphosynthesis of SnO2 nanocrystal networks as high-capacity anodes for lithium ion batteries

Sun Xiaolei

Tin dioxide (SnO 2 ) is of interest as an alternative anode material for lithium ion batteries. However, the major concern is the significant volume expansion during lithiation process, resulting in poor capacity retention and rate capability. Here, a facile morphosynthesis route is adapted for the fabrication of hierarchical SnO 2 nanocrystal networks with interwoven fibers, by immersing sacrificial eggshell membrane in a Sn-based sol followed by a calcination process in air. With both structural and compositional advantages, the synthesized SnO 2 networks electrode manifests superior reversible capacities of 938, 802, 736, 636, and 506 mAh g −1 even at high current densities of 0.2, 0.5, 1, 2, and 5 A g −1 , respectively. Besides, its initial Coulombic efficiency (72.6%) is also much enhanced compared with that of bare SnO 2 nanoparticles (59.6%) and commercial SnO 2 nanopowders (46.8%). The finding highlights the probable potential application of the SnO 2 networks for next-generation lithium ion batteries.

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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