Materials Today Energy
·
2023
·
IF 9.3
Nanrui Li,Tianqi Jia,Yanru Liu,Yunfei Ouyang,Yao Lv,Geng Zhong,Yufeng Wang,Bo Sun,Sirong Lu,Shifei Huang,Feiyu Kang,Yidan Cao
The formation of Li dendrites and dead Li, which causes short circuits, continuous side reactions, low Coulombic efficiency (CE) and thermal runaway, severely hinders the development of anode-free lithium metal batteries . Here, Cu-based current collector with super-three-dimensional lithiophilic modification layer is developed by the pyrolysis of resorcinol formaldehyde on 3D engineered copper mesh (a-RF@3D CM). The modification layer, consisting of highly dispersed CuO x sites in the O-containing defective carbon, together with the super-three-dimensional microstructure exhibits excellent lithiophilicity and capability to effectively reduce the nucleation overpotential, accommodate the uniform dendrite-free lithium deposition, promote stable and inorganic-rich solid electrolyte interphase formation, and improve the cycle stability. As a result, the a-RF@3D CM current collector exhibits reduced nucleation overpotential of 14.2 mV and prolonged cycling life over 400 cycles with average CE >98.5%. In the LiFePO 4 ||a-RF@3D CM anode-free cell, average CE of 99.50% and capacity retention of 60.66% are successfully achieved after 100 cycles. Meanwhile, average CE 99.78% and capacity retention of 64.43% are successfully achieved in LiFePO 4 ||Li@a-RF@3D CM cell (N/P = 1.6) after 200 cycles. The work provides feasible way to realize the fabrication of anode-free lithium metal batteries and also enhance the understanding of solid electrolyte interface evolution and regulation strategy of Li plating–stripping in advanced Li metal-based batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Advanced Energy Materials
·
2022
·Vol. 12
·期 40
·2201800
·
IF 29.698
Jie Chen,Zexiao Cheng,Yaqi Liao,Lixia Yuan,Zhen Li,Yunhui Huang
Li metal batteries have suffered from dendrite growth and its derived dead Li formation for a long time. A new lithium restoration method through the shuttling of redox mediators has been proposed recently. However, the side reaction of severe self-discharge often occurs when some redox mediators are used. Here, a selection principle of redox mediators for reactivating dead Li in lithium metal batteries is put forward, which is able to reactivate the dead Li effectively and reduce the self-discharge at the same time. Three redox mediators of ferrocene (Fc), 10-methylphenothiazine (MPT), and thianthrene (Th) with different redox potentials are tested in LiFePO 4 |Cu anode-free Li metal batteries to clarify the selection principle. Furthermore, 2,2,6,6-tetramethylpiperidinooxy (TEMPO), which is speculated to be a suitable one for reactivating dead Li in lithium metal batteries, is verified. This work provides a universal selection principle of redox mediators and may boost its practical application in Li metal batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Yan Liu,Yuan Li,Long Chen,Fang Yan,Zhihong Lin,Junmou Wang,Jingyi Qiu,Gaoping Cao,Biyan Wang,Hao Zhang
For high-specific energy Li batteries, hybrid anodes with graphite and Li metal are promising. However, the degradation of graphite-Li metal hybrid anodes during long cycles has been significantly fastened by dendritic Li growth and dead Li accumulation ascribed to the inferior solid electrolyte interphase (SEI). Efficient material construction strategies are highly demanded to inhibit the deactivation of graphite intercalation compounds (GICs: LiC 12 , LiC 6 , etc.) in graphite-Li metal hybrid anodes. Here, we introduced a physical-chemical modification strategy. Which is acted by a combination of a LiF-rich and elastic SEI and preset void in the composite electrodes, which was realized by Cu mesh current collectors, resulting in the retardant of the accumulation of dead Li and side reaction sediments on graphite surface and the retaining of the Li + insertion channels. The strategy ensured the long-term activity of both GICs and Li metal in graphite-Li metal hybrid anodes. Thus, the hybrid anodes obtain higher reversibility of both the lithium-ion insertion/deintercalation and Li metal deposition/dissolution processes. The batteries can maintain a specific capacity of up to 500 mAh/g, with an average CE of 98.5% for 85 cycles. This work presents a novel and effective methodology to realize the high reversibility of the high-capacity graphite-Li metal hybrid anodes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Xiao-Ru Chen,Chong Yan,Jun-Fan Ding,Hong-Jie Peng,Qiang Zhang
Lithium (Li) metal attributes to the promising anode but endures the low Columbic efficiency (CE) and safety issues from the inactive Li accumulation. The metallic Li which is isolated from the lithium anode (named dead Li 0 ) consists the major component of the inactive Li. We systematically and meticulously investigated the formation and evaluation of dead Li 0 during stripping process from electron transfer, the oxidation of Li 0 to Li + and the diffusion of Li + through solid electrolyte interphase (SEI). The above-mentioned processes were regulated by adjusting the contact sites of electron channels , the dynamic rate of conversion from Li 0 to Li + , and the structure as well as components of SEI. The design principles for achieving less dead Li 0 and higher CE are proposed as a proof of concept in lithium metal batteries . This new insight sheds a comprehensive light on dead Li 0 formation and guides the next-generation safe batteries for future application.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
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
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 39
·2003800
·
IF 16.836
Weidong Zhang,Zeyu Shen,Siyuan Li,Lei Fan,Xinyang Wang,Fang Chen,Xiaoxian Zang,Tian Wu,Fuyuan Ma,Yingying Lu
Fast Li-metal depletion and severe anode pulverization are the most critical obstacles for the energy-dense Li-metal full batteries using thin Li-metal anodes (<50 µm). Here, a wavy-nanostructured solid electrolyte interphase (SEI) with fast ion transfer kinetics is reported, which can promote high-efficiency Li-metal plating/stripping (>98% at 4 mAh cm −2 ) in conventional carbonate electrolyte. Cryogenic transmission electron microscopy (cryo-TEM) further reveals the fundamental relationship between wavy-nanostructured SEI, function, and the electrochemical performance. The wavy SEI with greatly decreased surface diffusion resistance can realize grain coarsening of Li-metal deposition and exhaustive dissolution of active Li-metal during the stripping process, which can effectively alleviate “dead Li” accumulation and anode pulverization problems in practical full cells. Under highly challenging conditions (45 µm Li-metal anodes, 4.3 mAh cm −2 high capacity LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathodes), full cells exhibit significantly improved cycling lifespan (170 cycles; 20 cycles for control cells) via the application of wavy SEI.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Shen Huasen,Li Zhaohuai,Li Jiantao,He Qiu,Li Mengjun,Tian Yunan,Wu Guoning,Zhao Yan,Zhang Xuanxuan,Xiao Jingjing,Amine Khalil,Li Yuyu,Xie Ming,Lu Jun
The growth of lithium (Li) dendrites and the accumulation of dead Li (i.e., Li metal regions which are electronically disconnected from the current collector) significantly undermine the safety and performance of Li metal batteries. This study employs kilogram–scale atomic layer deposition technology to construct zinc oxide with a preferential (002) crystal orientation, which homogeneously forms on commercial carbon nanotube papers. Our approach emphasizes the importance of achieving a moderate Li adsorption energy and low Li migration energy barriers to suppress Li dendrite growth. In this work, we introduce the concept of “catalytic” effect for dead Li reconversion, as validated through time–of–flight secondary ion mass spectrometry, leading to a Li plating/stripping efficiency of 99.89%. The Ah–level Li metal pouch cells with high–nickel positive electrodes achieve a specific energy of 380 Wh kg −1 (based on the mass of the whole pouch cell) and demonstrate stable cycling under demanding conditions. Analysis of the cycled pouch cells confirms the structural integrity and provides insights into the mechanism of the dead Li “catalytic” conversion.
研究领域:
储能技术
·
材料科学
·
电化学
·
纳米技术
·
表面工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Rongfeng Yang,Fan Wang,Wan-er Cui,Wei Chen,Tianyu Lei,Dongjiang Chen,Dongxu Chen,Li Xia,Chi Zhang,Kaijun Cheng,Runyi Dai,Yichao Yan,Xiaobin Niu,Yin Hu
Lithium sulfur batteries are persistently investigated by the research community due to their high energy density property. However, in order to get such performance, based on the current pouch cell strategy, less electrolyte and more stacking electrodes need be applied, leading to the aggravated dendrite growth, dead lithium accumulation and electrolyte depletion. In this context, we report a regenerative redox mediator strategy, targeting the operation window of the lithium sulfur batteries. The redox mediator can spontaneously consume the dead lithium on the anode, then be re-oxidized on the cathode through electrochemical process. Based on this design, the lithium sulfur pouch cell can be fully charged at 1C for more than 140 cycles. Moreover, the regeneration mechanism is studied by in situ UV–vis spectroscopy. This work not only validates the effectiveness of redox mediator for improving the high rate charging and cycling of lithium sulfur pouch cells, but also excludes the invalid mediator type and provides the design concept, guiding the future development of high rate charging strategy for lithium sulfur batteries.
研究领域:
储能
·
电化学
·
材料科学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Peng Du,Xinming Fan,Bao Zhang,Liang Cao,Jiancan Ren,Xing Ou,Xueyi Guo,Qi Liu
The extensive use of electric vehicles has raised the requirement of fast-charging for lithium-ion batteries. However, conventional graphite anode suffers from lithium dendrites and unacceptable capacity fade during fast charging. The limited ion channels and lithiophobic nature hinder the application of graphite in fast charging. Besides, the formation and accumulation of “dead lithium” accelerate the capacity decay during long-term cycling at high current density . Here, lithiophilic hard carbon-riveted graphite (HCRG) anode is delicately designed and fabricated to overcome the influence of “dead lithium” and meet the requirement of fast charging. The riveted heterostructure plays a crucial role in the lithiophobic-to-lithiophilic transition of graphite surface and the lithiophilic surface of HCRG can attract more Li-ions and facilitate re-intercalation of Li-ions into graphite bulk in relaxation time at low potential rather than plating on the surface, which effectively decreases the polarization and increases the proportion of reversible lithium at high current density. As a result, it exhibits excellent rate performance with 98.2% capacity retention when rate increasesing from 1 C to 15 C and fast-charging performance with 90.1% energy retention after 4000 cycles at an ultrahigh rate of 10 C in LiFePO 4 /HCRG full-cell. This strategy of constructing riveted heterostructure efficiently boosts the lithium intercalation reaction. It achieves fast-charging performance, highlighting the comprehensive understanding of interfacial kinetics and structure optimization for other fast-charging anodes.
研究领域:
储能
·
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Changyong Mo,Lijiao Quan,Weiya Zhu,Guanjie Li,Xianshu Wang,Youhao Liao,Weishan Li
As an ideal anode material of lithium metal for high-energy-density batteries, the development of lithium metal batteries (LMBs) has been limited by the Li dendrite’s growth and accumulation of dead Li. To solve this problem, a highly elastic artificial polymer layer coated on the surface Li anode by rapid ultraviolet radical polymerization is developed. The clad poly(methyl methacrylate-acrylic acid-sulfobetaine methacrylate) (P(MMA-AA-SBMA)) terpolymer not only shows good interfacial compatibility with Li metal due to the surface formation process by in situ light solidification but also contains functional anion groups of −COO– and −SO3–, contributing the convenient channels to regulate the transport of Li ions. Ascribed from the stable interface of clad Li and the suppressed decomposition reaction of the liquid electrolyte in the later cycle stage, the Li||LiCoO2 full cell exhibits good cycle stability, maintaining 96% of initial capacity after 100 cycles in 1C rate between 3 and 4.35 V, compared with that of 67% for bare Li. Thus, the artificial polymer cladding promotes the electrochemical stability of Li metal, providing a facile way for application in high-energy-density LMBs.
研究领域:
材料科学
·
电化学
·
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）