JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 12
·120535
·
IF 4.316
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
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yun Zhu,Fanping Meng,Nannan Sun,Liyuan Huai,Muqin Wang,Feihong Ren,Zhendong Li,Zhe Peng,Feng Huang,Hui Gu,Deyu Wang
Sponge-like lithium (Li) deposition results in high-surface-area morphology that harmfully accelerates the side reactions between Li and electrolyte, arousing serious safety issues of next high energy density Li metal batteries (LMBs). Herein, we propose a strategy to suppress the sponge-like Li deposition by plating Li metal on aluminum nitride (AlN)-modified substrates. For a practical Li deposition of 4 mAh cm–2 on a AlN-modified copper (Cu) electrode, the roughness and thickness of the as-deposited Li layer are only ∼10% and ∼50% of those for the Li layer deposited on bare Cu. Only based on the compacted Li deposition layer without any other protective remedies, the AlN-modified Cu electrode could provide a Li cycling life of 5 times longer than that on bare Cu, and an AlN-modified carbon felt was proved as an efficient interlayer to boost the cycling stability of Li||LiFePO4 batteries. These results demonstrate the high importance of suppressing the sponge-like Li deposition for high energy density LMBs.
研究领域:
材料科学
·
储能
·
电化学
·
锂金属电池
✓ 已验证
DOI
高影响因子
Microstructures
·
2024
·Vol. 4
·期 4
·N
·
IF 0
Zhendong Li,George Z. Chen,Di Hu,Xiayin Yao,Zhe Peng
Dendritic lithium (Li) deposition is a critical issue hindering the development of next-generation high-energy-density Li metal batteries (LMBs). Confining Li deposition within a three-dimensional host is a general strategy to suppress the volume expansion of the Li electrode. However, precise control of continuous Li growth in the pore space of the host is rarely investigated, which is a crucial issue to enable a high utilization ratio of the hosted Li for practical LMBs. Herein, a novel hierarchical host structure possessing a multifunctional secondary porous structure to regulate the continuous Li growth with high uniformity and reversibility is proposed. The secondary porous structure consisting of carbon nanotubes, nickel and Li2O-enriched solid electrolyte interphase is in-situ generated via lithiation reaction of a modified nickel foam scaffold, exhibiting high lithiophilicity, fast Li+ transportation and charge transfer. The LMB utilizing Li metal electrodes hosted by this rational structure achieved a stable cycling over 300 cycles with a practical LiFePO4 positive electrode (~2.5 mAh cm-2) at 0.5C/0.5C in the voltage window of 2.5-4.4 V. This work provides a novel approach to designing the host microstructure for constructing more stable Li metal electrode in practical LMBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Mingli Lu,Jie Sheng,Limiao Lin,Rongfu Zhou,Wucheng Xie,Junjun Shi,Xueyi Lu,Xia Lu
Essentially, rapid Li + accumulation in the anode region triggers a strong space charge layer and significant Li + concentration gradient, which ultimately leads to Li dendrites and interface issues. Herein, a mechanically robust layer consisting of lithiated-palygorskite (Li-Pal) and thermoplastic polyurethane elastomer (TPU) is employed to regulate the Li electrochemistry. The negatively charged Li-Pal surface demonstrates an exceptional lithiopholicity, which can leverage Li + supplement function to mitigate the concentration gradient. Meanwhile, the high elasticity of TPU can suppress Li dendrite growth and penetration during cycling. Enabled by such a hybrid layer, a high Coulombic efficiency (CE) of 99.1% over 300 cycles is delivered in Li/Cu half cells, and a long cycling life over 1400 h is achieved in a symmetric cell. The corresponding LiFePO 4 full cells present a high capacity retention of 90.6% over 1000 cycles at 5 C. This interfacial engineering highlights the synergetic design of a protective layer with high mechanical stability and Li + affinity for dendrite-free Li metal batteries.
研究领域:
储能
·
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
Batteries-Basel
·
2024
·Vol. 10
·期 6
·189
·
IF 4.6
Libo Song,Yuanyue He,Zhendong Li,Zhe Peng,Xiayin Yao
Sluggish transfer kinetics caused by solid–solid contact at the lithium (Li)/solid-state electrolyte (SE) interface is an inherent drawback of all-solid-state Li metal batteries (ASSLMBs) that not only limits the cell power density but also induces uneven Li deposition as well as high levels of interfacial stress that deteriorates the internal structure and cycling stability of ASSLMBs. Herein, a fast Li+transfer scaffold is proposed to overcome the sluggish kinetics at the Li/SE interface in ASSLMBs using an α-MnO2-decorated carbon paper (CP) structure (α-MnO2@CP). At an atomic scale, the tunnel structure of α-MnO2exhibits a great ability to facilitate Li+adsorption and transportation across the inter-structure of α-MnO2@CP, leading to a high critical current density of 3.95 mA cm−2at the Li/SE interface. Meanwhile, uniform Li deposition can be guided along the skeletons of α-MnO2@CP with minimized volume expansion, significantly improving the structural stability of the Li/SE interface. Based on these advantages, the ASSLMBs using α-MnO2@CP protected the Li anode and can stably cycle up to very high charge/discharge rates of 10C/10C, paving the way for developing high-power ASSLMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Jiaru Wei,Beichen Sun,Wenbiao Ma,Fengfeng Gao,Xiaowei An,Xiao Du,Xiaogang Hao
Spinel LiMn 2 O 4 is a promising electrode for electrochemically switched ion exchange (ESIX) lithium extraction, but its sluggish solid-phase diffusion and severe Mn dissolution limit its application in high-Mg 2+ /Li + salt lake brines. Herein, we report a clear size effect that regulates Li + intercalation kinetics and Mg 2+ /Li + separation by comparing hydrothermally synthesized nano-sized N-LiMn 2 O 4 (20–100 nm) and commercial micron-sized LiMn 2 O 4 (∼10 μm). Nanosizing induces preferential exposure of thermodynamically stable (111) facets, effectively suppressing surface reconstruction and Mn dissolution. In-situ distribution of relaxation time (DRT) reveals that the rate-limiting step changes from pure solid-phase diffusion in micron LiMn 2 O 4 to surface-diffusion co-control in N-LiMn 2 O 4 , reducing solid-phase diffusion resistance by 75% and charge-transfer resistance by 78.6%. Benefiting from kinetic optimization, the N-LiMn 2 O 4 /C/PVDF electrode maintains a Li + /Mg 2+ separation factor > 100 even at an ultrahigh Mg 2+ /Li + ratio of 500, far exceeding the micron counterpart. After optimization (wet film thickness = 200 μm, adsorption potential = 1.0 V), the electrode retains >90% capacity after 10 cycles in 200 mg·L −1 LiCl solution. This work clarifies the size-dependent kinetic transition mechanism and provides a rational design strategy for high-selectivity electrodes toward efficient lithium extraction from high-Mg/Li brines.
✓ 已验证
DOI
高影响因子
SOLID STATE IONICS
·
2022
·
IF 3.699
Tianxiang Ning,Yanzhi Zhang,Qian Zhang,Xuefeng Shen,Yinyi Luo,Taoyong Liu,Piao Liu,Zhiwei Luo,Anxian Lu
In this study, Ta single-doped Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (Ta 0.6 ) and a series of Ta, Sr co-doped Li 6.4+x La 3-x Sr x Zr 1.4 Ta 0.6 O 12 (Ta 0.6 Sr x , x = 0.1, 0.2, 0.3, and 0.4) electrolytes are synthesized via a two-step process. The XRD result reveals that all samples have a pure cubic phase, which indicates that Ta 5+ and Sr 2+ can enter the lattice of LLZO and stabilize the cubic phase. The SEM images exhibit that all samples have a dense microstructure and tight grain boundary without obvious holes. The excellent properties are achieved when the doping amount of Sr reaches 0.2 mol. Among all designed samples, the Ta 0.6 Sr 0.2 has the highest Li + conductivity and relative density of 8.54 × 10 −4 S cm −1 and 98.79%, respectively, as well as the lowest activation energy roughly 0.302 eV. Additionally, the symmetrical cell's galvanostatic cycling data show that it has excellent cycling performance and extremely low overpotentials even after 350 cycles, indicating that it can be successfully applied to next-generation all-solid-state lithium-ion batteries (ASSLIBs).
研究领域:
材料科学
·
电化学
·
能量存储
✓ 已验证
DOI
高影响因子
COMPOSITES SCIENCE AND TECHNOLOGY
·
2019
·
IF 6.309
Xuelian Fu,Yuchao Li,Chengzhu Liao,Weiping Gong,Mingyang Yang,Robert Kwok Yiu Li,Sie Chin Tjong,Zhouguang Lu
Low ionic conductivity and large interfacial impedance between the electrode and electrolyte are the main bottleneck issues of the current solid electrolytes . In this study, a novel 3D hierarchical solid electrolyte was developed to tackle the large interfacial impedance problem. A flexible polyethylene oxide/lithium chlorate (PEO/LiClO 4 ) was in-situ formed inside the 3D porous Li 6.28 La 3 Zr 2 Al 0.24 O 12 (LLZAO) network by simply using a cleanroom wiper as the template. The obtained 3D LLZAO-PEO/LiClO 4 composite solid electrolyte exhibited a high ionic conductivity of 2.25 × 10 −5 S cm −1 at 30 °C, being 30.7 times higher than that of pristine PEO/LiClO 4 electrolyte. The improved ionic conductivity was attributed to the 3D porous LLZAO structure with continuous fast ion transport pathways. In addition, the 3D LLZAO network can effectively inhibited the growth of lithium dendrite , leading to excellent stability and desirable safety during lithium stripping/plating cycling. Furthermore, the all-solid-state LiFePO 4 /Li battery system based on the obtained 3D LLZAO-PEO/LiClO 4 electrolyte showed a high initial discharge specific capacity of 143.8 mAh·g −1 and a high capacity retention of 86% after 200 cycles at 60 °C. This 3D composite solid electrolyte design is very effective in reducing the interfacial impedance and provides a solution for the further development of high-performance solid electrolyte for all-solid-state rechargeable batteries.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Minsong Huang,Zhenguo Yao,Qingping Wu,Yongjian Zheng,Jianjun Liu,Chilin Li
Anode interface modification is crucial for the stabilization of Li–metal batteries (LMBs), which have been considered as the most promising system for the electric vehicle market owing to their high energy density (500 W h kg–1). However, the biggest challenge for LMBs lies in the preservation of anode reversibility, including plated Li morphology control and dendritic Li inhibition during cycling. Here, we propose a nanostructure modulation strategy of Li grains and plating to activate the anode kinetics of LMBs without the compromise of anode stability. This modulation is triggered by the rapid deposition of ultrathin polydopamine coating on the Cu foil (PDA@Cu), which results in an unusual interlaced growth of vertical or lie-down two-dimensional Li nanoflakes on PDA. The high binding energy (>3 eV) between Li atoms and rich imino/carbonyl groups enables a superior lithiophilicity of PDA to homogenize the Li-ion flowing and Li-mass electroplating with negligible nucleation overpotential. The high Coulombic efficiency (98%) and low voltage hysteresis (∼20 mV) are stabilized for at least 300 cycles in the Li–PDA@Cu cell architecture. This PDA@Cu electrode can even tolerate much higher current densities of 5 and 10 mA cm–2 for 170 and 100 cycles, respectively. The interlaced network of Li nanosheets reinforces the electric contact and therefore charge transfer at the anode–electrolyte interface characterized by small interfacial resistance (<3 Ω cm2) and activation energy (0.28 eV). A viewpoint of robustness loss or mechanical heterogeneity in Li plating is discussed to disclose the evolution from column-like Li grains to porous Li sponges and then to compactly stacked Li nanoflakes with porosity shrinkage.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Yue Chen,Minghui He,Ning Zhao,Jingming Fu,Hanyu Huo,Tao Zhang,Yiqi Li,Fangfang Xu,Xiangxin Guo
Garnets are promising solid electrolytes for developing solid state Li batteries , owing to their features of relatively high conductivity and stability against lithium metal. However, they show shortcoming of Li penetration through garnets during Li plating and stripping, which limits their practice application. Herein, we present a strategy to solve such problem by coating SnO 2 films on the surfaces of the Li 6 · 4 La 3 Zr 1 · 4 Ta 0 · 6 O 12 pellets. Through conversion reaction of SnO 2 with Li at 200 °C, the nanocomposite layers consisting of crosslinked Li x Sn and Li 2 O are formed between the Li and the Li 6 · 4 La 3 Zr 1 · 4 Ta 0 · 6 O 12 electrolytes. This leads to transition from lithiophobicity to lithiophilicity, thus greatly reducing interfacial resistance from 1100 Ω cm 2 to 25 Ω cm 2 . Furthermore, taking advantage of suppressing volume change of Li x Sn alloy which is about 260%, the intermediate layers maintain integrity under the current densities of 0.2 mA cm −2 for 650 h cycles. In addition, the critical current density of Li/SnO 2 -Li 6.4 La 3 Zr 1 · 4 Ta 0 · 6 O 12 -SnO 2 /Li can be as high as 1.15 mA cm −2 . As a proof-of-concept, this effective interface modification based on conversion reaction method contributes to a useful way of solving the Li/garnet interface problem and promoting the solid state Li batteries development.
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 33
·17056-17064
·
IF 11.301
Xin-Yu Hu,Pan Xu,Shengwen Deng,Jie Lei,Xiaodong Lin,Qi-Hui Wu,Mingsen Zheng,Quanfeng Dong
Lithium (Li) is a metallic element possessing the most negative electrode potential and the lowest electrochemical equivalent, which make it one of the key materials for the development of the next-generation Li batteries with high specific energy. However, the heterogeneous deposition, volume expansion, solid-electrolyte interphase (SEI) fracture, and high reactivity of metallic Li make its commercialized development difficult. Herein, a novel polyaniline (PANI) decorated three-dimensional (3D) copper mesh (3DCMP) skeleton for a Li metal anode is proposed, which was prepared by in situ polymerizing aniline on the surface of a copper mesh (3DCM). The lithiophilic PANI micro-sheets could induce ordered Li deposition on the mesh and facilitate the formation of a more available SEI film, which could effectively alleviate the formation of Li dendrites and highly promote the utilization of Li during long-term cycling. The symmetrical-cell displayed an excellent Li plating/stripping performance, in which it maintained an overpotential of less than 20 mV at a current density of 2 mA cm−2 over 4000 h. Furthermore, the full-cell coupled with the LiFePO4 cathode exhibited a high capacity retention of 84.8% at 4C after 550 cycles and when coupled with the rGO/S cathode exhibited a capacity retention of 94.4% at 1C after 100 cycles. Hence, it demonstrates a promising potential to be applied in large-scale manufacturing.
研究领域:
材料科学
·
电化学
·
储能技术
·
纳米材料
·
电池化学
✓ 已验证
DOI
高影响因子
Chemistry-An Asian Journal
·
2024
·Vol. 19
·期 14
·e202400181
·
IF 3.5
Xingguang Lu,Yuanyuan Ren,Daming Chen,Xiaolong Guo,De Li,Yong Chen
In Li-ion batteries, the origin of memory effect in Al-doped Li 4 Ti 5 O 12 has been revealed as the reversible Al-ion switching between 8a and 16c sites in the spinel structure, but it is still not clear about that for olivine LiFePO 4 , which is one of the most important cathode materials. In this work, a series of Na-doped and Ti-doped LiFePO 4 are prepared in a high-temperature solid-state method, electrochemically investigated in Li-ion batteries and characterized by X-Ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR) and Magic-Angle-Spinning Nuclear Magnetic Resonance (MAS NMR). Compared with non-doped LiFePO 4 , the Ti doping can simultaneously suppress the memory effect and the Li−Fe anti-site, while they are simultaneously enhanced by the Na doping. Meanwhile, the Ti doping improves the electrochemical performance of LiFePO 4 , opposite to the Na doping. Accordingly, a schematic diagram of phase transition is proposed to interpret the memory effect of LiFePO 4 , in which the memory effect is attributed to the defect of Li−Fe anti-site.
研究领域:
材料科学
·
电化学
·
储能
·
电池技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）