ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yin Xie,Yongcheng Jin,Lan Xiang
The nontoxicity and low cost make LiMn2O4 a competitive cathode material for lithium-ion batteries. LiMn2O4 has a high theoretical capacity (296 mAh g–1) when cycled in the 3 and 4 V regions. However, it displays a low practical capacity (∼120 mAh g–1) because of the unavailability of the 3 V region caused by severe Jahn–Teller distortion. The present work investigated the full utilization of LiMn2O4 in both 3 and 4 V by tuning the nanoscale interfacial properties. Li-rich structures at the surface and interface of the spinel material and nanograin strain were introduced to improve the performances and were achieved by grinding LiMn2O4 and Li2O at 700 rpm for 10 h under an argon atmosphere. The product shows a high initial discharge capacity of 287.9 mAh g–1 at 0.05 C between 1.2 and 4.6 V and retains 83.2% of the capacity after 50 cycles. The nanoscale interfacial structure was clarified by spherical aberration-corrected microscopy and XRD refinement, and complex occupancies of Li and Mn were found at the interface. A correlation between the interfacial properties and electrochemical performance was established, and the improved performance could be attributed to the polycrystalline nature of the material, the unique Li-rich interfacial structure, and the slightly elevated valence state of Mn. The present results may provide insight for further evaluating the complex mechanism of controlling the electrochemical performance of LiMn2O4.
研究领域:
材料科学
·
电化学
·
储能
·
锂离子电池
·
纳米材料
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2020
·
IF 3.83
Mengying Cai,Zhixiong Huang,Yiling Huang,Jian Zou,Shaojun Shi,Fei Geng
Lithium-rich, manganese-based cathode materials with high specific capacity have become a research focus in recent years; however, the transformation to the spinel phase and the dislocations of the material lead to inferior electrochemical performances. In this work, a lanthanum heterosphere was constructed on the surface of a Li-rich manganese-based material without distinct phase interface and lattice mismatch to address these problems. Such a surface heterosphere can prevent the migration of metal ions and enhance the diffusion of Li + and transference of electrons. By virtue of the surface heterosphere, which can also preserve the oxygen vacancies , high initial discharge/charge capacities of La-LLO (359.6/293.4 mA h g −1 ) can also be achieved. The La-LLO cathode also exhibits outstanding cycle performance (236.7 mA h g −1 at 0.1 A g −1 during 100 cycles) and rate capability (59.3 mA h g −1 and the capacity retention of 76.9% for 500 cycles at 5 A g −1 ). It has been proven that such a melting impregnation method is effective in constructing a surface heterosphere on the surface of a Li-rich manganese-based material for improving Li storage properties.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Chen Wu,Jieming Hu,Hanxian Chen,Chengyi Zhang,Mingli Xu,Lin Zhuang,Xinping Ai,Jiangfeng Qian
Prussian blue analogues (PBAs) have been attracting intense attention owing to its two-electron storage capability and considerable cost advantage, especially in Na-ion and K-ion batteries. However, things are quite different when it comes to Li-ion batteries, because lithium-containing Li 4 Fe(CN) 6 precursor is not commercially available and thus the traditionally prepared Li-deficient FeFe(CN) 6 products fail to couple with commercial graphite anode for full cells. Herein, we put forward a potential matching principle to guide the chemical pre-lithiation of FeFe(CN) 6 into a Li-rich Li x FeFe(CN) 6 ( x varies from 0 to 2) cathode. The potential matching principle was convincingly confirmed by theoretical analysis and over-lithiation experiments. Perylene-Li reagent was elaborately screened to serve as both Li + and electron donor for controllable chemical lithiation reaction while preserving the host framework stable. Our work provided a general guiding principle and effective methodology for controllable synthesis of Prussian blue analogues in gradient lithiation depth, which could be served as a platform for in-depth, systematic and comprehensive research on the properties of PBAs materials.
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
CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Xingrui Pu,Xing Cheng,Qiaohong Yan,Yueming Lin,Rentai Yan,Ruize Yang,Xiaohong Zhu
The need to develop safe solid-state lithium batteries has stimulated intense research efforts for Li + solid electrolytes. However, the low conductivity limits the development of NASICON LiZr 2 (PO 4 ) 3 (LZP) electrolyte. Here, the doping effects of Ta on the structure, surface morphologies and electrochemical properties of Li 1- x Zr 2- x Ta x (PO 4 ) 3 (LZTP, x = 0, 0.01, 0.02, 0.04, 0.06 and 0.08) solid electrolyte were analyzed. LZTP was prepared using a simple solid-state reaction route, followed by sintering at 1200 °C for 12 h. A proper content of Ta 5+ substitution for Zr 4+ is beneficial to stabilize the high conductive rhombohedral (α) phase of LZP at room temperature. Doping Ta 5+ is conducive to unblocking of Li + at the M1 site and facilitates the occupation of Li + at the M2 site, thereby expanding the pathway for Li + conduction. Rietveld refinement data demonstrated that the Zr–O and P–O bond lengths ( d Zr-O and d P-O ) increased with a decrease in Zr–O–P bond angles ( θ Zr-O-P ) as x rose. The distortions in the ZrO 6 octahedron may weaken the coulomb attraction in Li + -O 2- , resulting in a lower activation energy ( E a ) and a higher Li + conductivity. The highest room-temperature conductivity (6.06 × 10 −5 S cm −1 ) was obtained at x = 0.06, which reached 1.5 × 10 −4 S cm −1 at 50 °C. The E a was found to decrease from 0.388 eV ( x = 0) to 0.306 eV ( x = 0.06). In addition, Ta doping resulted in improved connectivity and reduced pore formation, which also contributed to the decrease in resistance. The Raman spectrum demonstrated that some phonon modes of bending vibration in PO 4 were degenerate and external modes became too weak to be observed or even disappeared as Ta content increased. This change in the modes also had an impact on the Li + conductivity. Overall, the LZTP-0.06 appears to be a promising candidate for the solid electrolyte.
研究领域:
材料科学
·
电化学
·
固态电池
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Jiaxin Wu,Yuhan Ma,Haichang Zhang,Haonan Xie,Jin Hu,Chunsheng Shi,Biao Chen,Chunnian He,Naiqin Zhao
Poly(ethylene oxide) (PEO)-based electrolytes have been extensively studied for all-solid-state lithium-metal batteries due to their excellent film-forming capabilities and low cost. However, the limited ionic conductivity and poor mechanical strength of the PEO-based electrolytes cannot prevent the growth of undesirable lithium dendrites, leading to the failure of batteries. Metal–organic frameworks (MOFs) are functional materials with a periodic porous structure that can improve the electrochemical performance of PEO-based electrolytes. However, the enhancement effect of MOFs with different metal centers and the interaction mechanism with PEO remain unclear. Herein, MOF-74s with Cu or Ni centers are prepared and used as fillers of PEO-based electrolytes. Adding 15 wt % of Cu-MOF-74 to the PEO-based electrolyte (15%Cu-MOF/P–Li) effectively improves the ionic conductivity, lithium transference number, and mechanical strength of the PEO-based electrolyte simultaneously. Furthermore, the ordered pore channels of Cu-MOF-74 provide uniform Li-ion transport pathways, facilitating homogeneous Li+ deposition. As a result, the lithium symmetric cell with 15%Cu-MOF/P–Li shows stable cycles for 1080 h at 0.1 mA cm–2 and 0.1 mAh cm–2, and the Li | 15% Cu-MOF/P–Li | LFP full cell exhibits a long cycle life up to 200 cycles at 60 °C and 0.5 C, with a capacity retention rate of 89.7%.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Su Han,Zhong Yu,Wang Changhong,Liu Yu,Hu Yang,Li Jingru,Wang Minkang,Jiao Longan,Zhou Ningning,Xiao Bing,Wang Xiuli,Sun Xueliang,Tu Jiangping
Sulfide electrolytes represent a crucial category of superionic conductors for all-solid-state lithium metal batteries. Among sulfide electrolytes, glassy sulfide is highly promising due to its long-range disorder and grain-boundary-free nature. However, the lack of comprehension regarding glass formation chemistry has hindered their progress. Herein, we propose interstitial volume as the decisive factor influencing halogen dopant solubility within a glass matrix. We engineer a Li 3 PS 4 -Li 4 SiS 4 complex structure within the sulfide glassy network to facilitate the release of interstitial volume. Consequently, we increase the dissolution capacity of LiI to 40 mol% in 75Li 2 S-25P 2 S 5 glass. The synthesized glass exhibits one of the highest ionic conductivities among reported glass sulfides. Furthermore, we develop a glassy/crystalline composite electrolyte to mitigate the shortcomings of argyrodite-type sulfides by utilizing our synthesized glass as the filler. The composite electrolytes effectively mitigate Li intrusion. This work unveils a protocol for the dissolution of halogen dopants in glass electrolytes.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 35
·2401100
·
IF 13
Xingkai Wang,He Huang,Hong Zhang,Qiujiang Dong,Wanxing Zhang,Meng Gao,Jinyang Li,Biao Chen,Hao Guo,Xiaopeng Han
The increasing need for energy storage devices with high energy density has led to significant interest in Li-metal batteries (LMBs). However, the use of commercial electrolytes in LMBs is problematic due to their flammability, inadequate performance at low temperatures, and tendency to promote the growth of lithium dendrites and other flaws. This study introduces a localized high-concentration electrolyte (LHCE) that addresses these issues by employing non-flammable electrolyte components and incorporating carefully designed additives to enhance flame retardancy and low-temperature performance. By incorporating additives to optimize the electrolyte, it is possible to attain inorganic-dominated solid electrolyte interphases on both the cathode and anode. This achievement results in a uniform deposition of lithium, as well as the suppression of electrolyte decomposition and cathode deterioration. Consequently, this LHCE achieve over 300 stable cycles for both LiNi 0.9 Mn 0.05 Co 0.05 O 2 ||Li cells and LiCoO 2 ||Li cells, as well as 50 cycles for LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811||Li) pouch cells. Furthermore, NCM811||Li cells maintain 84% discharge capacity at −20 °C, in comparison to the capacity at room temperature. The utilization of this electrolyte presents novel perspectives for the safe implementation of LMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shu-Ya Lei,Lin-Bo Liu,Subiao Liu,Wei Sun,Yue Yang,Jing-Li Luo
The recycling of spent LiCoO 2 batteries has attracted numerous attentions in view of their environmental and economic values. However, conventional hydrometallurgy strategies for spent LiCoO 2 recycling still undergo complicated processes that involve multiple steps, resulting in a high-value metal loss and a low value-added product. Herein, a facile method was developed to recycle lithium and repurpose oxygen vacancy-rich cobalt-based catalysts toward oxygen evolution reaction (OER). By roasting LiCoO 2 with ammonium sulfate salt at 975 °C for 120 min, lithium was converted into soluble Li 2 SO 4 and 99.2 % of Li could be preferentially leached by H 2 O, while cobalt was recycled in the form of highly pure cobalt oxide (M−CoO). Importantly, the M−CoO exhibited an excellent OER activity, superior to the spent LiCoO 2 , the prepared Co 3 O 4 , the commercial RuO 2 , and most of the reported cobalt-based catalysts. The results confirmed that the outstanding OER activity of M−CoO was originated from the rich surface oxygen vacancy, which facilitated the surface reconstruction to form a highly active layer of short-range order species during OER. This study showcased a novel approach to achieving a priority lithium recovery, coupled with an advanced route for catalyst regeneration, from spent lithium-ion batteries for energy conversion and storage devices.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Yanhua Zhang,Jiadong Deng,Dongwei Hu,Fei Chen,Qiang Shen,Lianmeng Zhang,Shijie Dong
The Li + concentration and Li + transport channel size of garnet-type solid electrolyte Li 7 La 3 Zr 2 O 12 are the two key factors associated with the improvement of Li ionic conductivity . Through precise control of the Li + concentration and the Li + transport channel size by Ta-doping (Li 7-X La 3 Zr 2-X Ta X O 12 , X = 0.2–1.0), synergistic regulation of the two factors is achieved. Results show that the optimum Li + concentration seems to be at about 6.31 where the Li + occupancy in LiO 6 is high and the Li + arrangement in LiO 4 is disordering. With the Li + concentration higher than 6.31, the occupancy in LiO 4 sites remains constant but the Li + arrangement in LiO 4 becomes more and more ordering. At higher Li + concentration of 6.52, Li + arrangement becomes certain of ordering which should have reduced the grain conductivity, however, the grain conductivity is still as high as 9.84 × 10 −4 S cm −1 . This indicates that LLZO with this Li + concentration have favorable Li + transport channel size. The optimum Li + transport channel size is about 12.95 ± 0.01 Å. At Li + concentration of 6.31, the proper Li + concentration is the main factor for the high grain ionic conductivity of 10.1 × 10 −4 S cm −1 . While at Li + concentration of 6.52, the suitable Li + transport channel size is the main factor for the high grain ionic conductivity. In conclusion, the high grain ionic conductivity at Li + concentration of 6.31–6.52 is due to the synergistic regulation of Li + concentration and Li + transport channel size.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Ji-Wei Zhang,Wen-Hao Wang,Meng-Xiang Xie,Hou-Ran Wu,Yan-Pei Wang,Hao-Tian Bao,Bo-Qun Cao,Gang-Qin Shao
The lithium silicon phosphor sulfo-chloride (LiSiPSCl) with a Li 10 GeP 2 S 12 -type structure is one of the most promising solid electrolytes (SEs) for all-solid-state lithium-ion batteries (ASSLIBs) due to its currently highest ionic conductivity at RT. In this work, three kinds of LiSiPSCl electrolytes, i.e. Li 7.59(10) Si 1.95(9) P 1.65(7) S 11.64(1) Cl 0.36(1) (SE-450), Li 7.67(12) Si 1.90(1) P 1.67(1) S 11.61(2) Cl 0.39(2) (SE-475) and Li 7.58(5) Si 1.75(4) P 1.79(2) S 11.54(4) Cl 0.46(4) (SE-500), were prepared at 450 / 475 / 500 °C for 8 h through a solid-state method. The assembling of blocking / symmetrical / semi-blocking cells and ASSLIBs, and electrochemical measurements were carried out by coupling the three SEs with two kinds of anodes (Li metal and Li-In alloy) and one cathode of LiNbO 3 -coated LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM@LNO). Studies were focused on the relationship among chemical compositions, phase structures and electrochemical properties, as well as the electrolyte/electrode interfacial stability. Results show that LiSiPSCl electrolytes had favorable interfacial stability with Li-In anode and exhibited low polarization voltage (< 20 mV) and decomposition current (< 0.01 mA). The optimized NCM@LNO//SE-475//Li-In of ASSLIBs exhibited a stable long-term cycle performance with a capacity retention of 97.0% (128.4 mAh g − 1 ) after 50 cycles and 81.1% (107.4 mAh g −1 ) after 100 cycles at 0.1 C. In addition, it exhibited a good rate performance while its capacity retention remained 99.3% (140.6 mAh g −1 ) after 39 cycles at 0.05 / 0.1 / 0.2 / 0.5 / 0.05 C.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Wang Ke,Shaobo Cai,Runlin Ma,Jingge Shi,Manman Wu,Menggai Jiao,Yongzheng Fang,Yiyang Liu,Zhen Zhou
With the increasing application of electric vehicles, the surging of lithium-ion batteries (LIBs) may foreshadow potential environmental disruptions stemming from mishandling spent LIBs and greenhouse gas emissions from recycling. Urgent advancements are needed in the current recycling technologies for dead LIBs. Herein, we propose a solution to address the challenge of industrial LIB waste recycling by repurposing it into environmentally friendly functional materials. Specifically, unitary and ternary transition metal organic frameworks (TT-MOFs) were successfully synthesized for use in the separator for high-performance lithium-sulfur (Li-S) batteries. The unique ternary MOFs demonstrate the capability to mitigate the shuttle effect and enhance the adsorption and conversion of lithium polysulfides during cycling. Notably, we achieved an initial discharge capacity of 1008.7 mA h g–1 at 0.5 C, with a decay rate of only 0.054% after 500 cycles. This research reuses waste solutions from the wet metallurgy process of LIB recycling and unveils a promising approach for the development of sustainable energy-storage materials in the future.
研究领域:
材料科学
·
储能技术
·
电池技术
·
环境科学
·
回收技术
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Huanhuan Gao,Jianzhong Liu,Peihui Xu,Haiou Wang,Jianren Fan
Aluminum-lithium (Al–Li) alloys are crafted by incorporating minute quantities of Li into Al, thereby alleviating the passivation effect of dense alumina. This strategic blend elevates the energy release potential of Al-based fuels by enhancing reactivity and facilitating efficient combustion reactions. The effects of Li content and particle size on the combustion characteristics of Al–Li alloys are systematically investigated, with a particular focus on several pivotal aspects: thermal oxidation behavior, ignition delay time, combustion time, combustion intensity, temperature, and the condensed-phase products. The results show that, upon heating to 1500°C, the oxidation weight gain of Al–Li alloys reaches 6.5 times that of raw Al. This indicates that adding Li significantly enhances the extent of the oxidation reaction. Increased Li content and particle size reduction further accelerate the oxidation reaction. The ignition delay time and combustion time are effectively shortened, showing a more intense combustion process, higher flame temperature and more significant micro-explosion effect. Ultimately, these factors lead to a significant reduction in the size of condensed-phase products. Based on these insights, a comprehensive impact mechanism for the energy release of Al–Li alloys has been proposed, providing theoretical guidance for applying Al–Li alloys in related fields.
研究领域:
材料科学
·
燃烧学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）