AICHE JOURNAL
·
2025
·
IF 4
Hai Zhang,Yixuan Meng,Fan Wang,Ze Zhang,Zhenyu Yang
This work introduces nickel (II) tetraphenylporphyrin (NiTPP) as a multifunctional electrolyte additive to simultaneously address polysulfide shuttle and uncontrolled lithium dendrite growth in lithium–sulfur (Li–S) batteries. Mobile NiTPP species act as homogeneous catalysts with Ni–N 4 centers for rapid polysulfide redox mediation to suppress migration, while planar molecules featuring lithium-affinity capability migrate to the lithium metal surfaces, enabling uniform lithium flux and anode protection. NiTPP-modified electrolytes significantly enhance Li–S battery performance, demonstrated by 634.9 mAh g −1 at 4C, 758.3 mAh g −1 after 100 cycles at 0.2 C (83.4% retention), and 757.5 mAh g −1 under high sulfur loading (2.9 mg cm −2 ) with lean electrolyte ( E / S = 5 μL mg −1 ), all with high Coulombic efficiency. Crucially, NiTPP, acting as a soluble dual-functional mediator enabling homogeneous operation in electrolytes, simplifies Li–S battery fabrication while demonstrating the commercial viability of molecularly engineered mobile active sites for stabilizing both electrodes in high-energy-density Li–S batteries.
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高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 42
·24251-24261
·
IF 10.733
Yunyun Zhong,Lei Zhong,Shuanjin Wang,Jiaxiang Qin,Dongmei Han,Shan Ren,Min Xiao,Luyi Sun,Yuezhong Meng
With the rapid development of electronic devices and electric vehicles, the requirements for their safety issues and service stabilities have become more and more strict. Single-ion gel polymer electrolytes exhibit outstanding ion conduction, high safety, good flexibility and a lithium transference number close to unity, leading to extensive research. In this work, a flexible fluorinated polysulfonamide based single-ion polymer electrolyte (SIPE) was synthesized using lithium [(4-styrenesulfonyl)(fluorosulfonyl)imide] (LiSFSI), pentaerythritol tetrakis(3-mercaptopropionate) (PETMP) and pentaerythritol tetraacrylate (PET4A) via one-step in situ photoinitiated thiol–ene click reaction in plasticizers, with electrospun poly(vinylidene fluoride) (PVDF) as the standing membrane. The influence of plasticizer content was investigated and the optimized electrolyte exhibits ultra-high ionic conductivity (5.81 × 10−3 S cm−1 at 28 °C) and a high lithium transference number of 0.91, near to unity. This ionic conductivity is among the highest ionic conductivities exhibited by SIPEs reported to date. Its electrochemical stability window is up to 5.2 V. More importantly, Li/LiFePO4 cells using the prepared SIPE as both the electrolyte and separator displayed high reversible capacity at room temperature. It also exhibits excellent long-term stability and reliability as it maintains a capacity of 140 mA h g−1 at 0.2C rate even after 230 cycles without obvious decay at room temperature.
研究领域:
材料科学
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电化学
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能源存储
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高分子化学
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电池技术
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qianxiao Fan,Wendi Zhang,Yilong Jin,Dongmei Zhang,Xianglong Meng,Wanxiong Peng,Jinhui Wang,Jinshan Mo,Kai Liu,Lehao Liu,Meicheng Li
All-solid-state lithium batteries employing sulfide solid electrolyte are promising candidates for next generation lithium batteries. Nevertheless, the unstable interface of sulfide solid electrolyte and Li metal has limited the lifespan of sulfide solid state lithium metal batteries. Herein, a composite protection layer composed of Li-Ag/LiF (LAF) is formed on Li metal surface by the in-situ reaction of silver-fluoride (AgF) and Li metal to solve the instability issue of the Li 6 PS 5 Cl/Lithium interface. The Li-Ag particles act as nucleation sites for Li deposition and LiF can avoid the growth of lithium dendrites. The density function theory (DFT) calculation results show the lithiophilic of Li-Ag alloys and high interfacial energy of LiF/Li 6 PS 5 Cl interface, proving the superiority of the LAF protection layer. The critical current density of the Li-LAF/ Li 6 PS 5 Cl/ LAF-Li symmetric battery is 1.6 mA cm −2 and the battery achieved a long lifespan of over 3000 h at 0.1 mA cm −2 and 0.1mAh cm −2 at room temperature. In addition, a high discharge capacity of 139.1mAh/g is obtained in the LiNbO3@LiCoO2/ Li6PS5Cl/ LAF-Li full cell. This work provides a feasible strategy for the interface modification of sulfide all-solid-state Li metal batteries.
研究领域:
材料科学
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储能技术
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电化学
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固态电池
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纳米材料
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高影响因子
Advanced Energy Materials
·
2019
·Vol. 9
·期 38
·1902125
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IF 24.884
Jianwen Liang,Xiaona Li,Yang Zhao,Lyudmila V. Goncharova,Weihan Li,Keegan R. Adair,Mohammad Norouzi Banis,Yongfeng Hu,Tsun-Kong Sham,Huan Huang,Li Zhang,Shangqian Zhao,Shigang Lu,Ruying Li,Xueliang Sun
Li metal is a promising anode material for all-solid-state batteries, owing to its high specific capacity and low electrochemical potential. However, direct contact of Li metal with most solid-state electrolytes induces severe side reactions that can lead to dendrite formation and short circuits. Moreover, Li metal is unstable when exposed to air, leading to stringent processing requirements. Herein, it is reported that the Li 3 PS 4 /Li interface in all-solid-state batteries can be stabilized by an air-stable Li x SiS y protection layer that is formed in situ on the surface of Li metal through a solution-based method. Highly stable Li cycling for over 2000 h in symmetrical cells and a lifetime of over 100 cycles can be achieved for an all-solid-state LiCoO 2 /Li 3 PS 4 /Li cell. Synchrotron-based high energy X-ray photoelectron spectroscopy in-depth analysis demonstrates the distribution of different components within the protection layer. The in situ formation of an electronically insulating Li x SiS y protection layer with highly ionic conductivity provides an effective way to prevent Li dendrite formation in high-energy all-solid-state Li metal batteries.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2018
·Vol. 165
·期 9
·D321
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IF 3.662
Baoguo Zhang,Zhongning Shi,Lingling Shen,Aimin Liu,Junli Xu,Xianwei Hu
Herein, inspired by previous reports on the electrochemical reduction of Al in diverse electrolyte systems, we describe a novel Al-containing solvate ionic liquid (2:1 (mol/mol) mixture of ethylene carbonate (EC) and AlCl3) that allows low-temperature electrochemical deposition of Al and features the advantages of low cost, ease of preparation, and high electrochemical stability. Electrodeposition of Al-Li alloy and Li can also be realized in this system. Additionally, the above ionic liquid exhibited a saturated vapor pressure of 0.0012 kPa and a conductivity of 1.32 mS/cm at 298 K, which was acceptable for practical applications. To elucidate the electrochemical deposition mechanism, the ionic components of the 2:1 EC/AlCl3 system were characterized by a range of instrumental analysis techniques and theoretical calculations, and Lewis-acidic cations were identified as the electroactive species for Al electrodeposition. Notably, an Al-Li alloy could be obtained by co-deposition in the new solvate ionic liquid, and Li metal could also be electrodeposited on a high-purity Al plate in the form of Al4Li9 and Li3Al2 under ambient conditions using LiCl as a Li source. Al-containing solvate ionic liquids, which to an extent evolved from organic-salts, are of increasing interest. They are expected to gain more attention in the field of electrochemical metallurgy of active metals, due to their higher tunability and lower price.
研究领域:
材料科学
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电化学
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高影响因子
Advanced Energy Materials
·
2023
·Vol. 13
·期 20
·2204272
·
IF 27.8
Kanglong Guo,Chunlei Zhu,Huaping Wang,Shihan Qi,Junda Huang,Daxiong Wu,Jianmin Ma
Increasing the cut-off voltage of cathodes can improve the energy density of Li||LiCoO 2 batteries. However, the electrolyte and cathode suffer from oxidation and deterioration at high voltage, respectively, which lead to rapid battery degradation. Herein, a uniform, highly Li + conductive cathode electrolyte interphase (CEI) is constructed by using bis-(benzenesulfonyl)imide (BBSI) as an additive to stabilize Li||LiCoO 2 batteries at 4.6 cut-off voltage with superior cycling and high-rate performance. Such a CEI is comprised of LiF and conductive Li + moieties (e.g., Li 2 S and Li 3 N), which can improve the Li + migration, alleviate cathode degradation, and other secondary degradation factors caused by uneven local Li + intercalation/deintercalation. As expected, Li||LiCoO 2 batteries with a 1% BBSI-containing electrolyte sustain 81.30% of initial capacity after 300 cycles at 0.5C, and 88.27% of initial capacity even after 500 cycles at 2C/3C.
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高影响因子
Journal of Energy Storage
·
2023
·
IF 9.4
Xuhui Wang,Xufeng Dong,Xinyi Song,Fangyuan Hu,Hao Huang,Min Qi
All solid-state battery (ASSB) as the breakthrough of the advanced lithium-ions battery owing to its superior energy density and safety. Solid electrolytes are required to possess excellent electrochemical and safety. However, the low ionic conductivity and the poor interfacial compatibility, respectively, limits the progress of polymer and ceramic electrolyte , which accelerate the development of composite solid electrolyte (CSE). Therefore, we demonstrate a hierarchy structure that PEO(polyethylene)-LLZO@NFPAN-SiO 2 , which consists of SiO 2 particles encapsulated nanofibers (in-situ hydrolyzed by TEOS) and flexible membrane of PEO-LLZO to synergistically elevate the performance of CSE. This CSE exhibits broad electrochemical window (6 V vs. Li) and strong ionic conductivity (3.3 × 10 −4 S cm −1 , 30 °C), and also shows robust strength (5.1 MPa). The assembled Li-symmetric cells exhibit superior cycling life of 1000 h, with an extremely modest over potential of 45 mV. The full cell exhibits excellent cycle stability, 102 mA h g −1 after 100 cycles at 0.5C, and a high initial Coulomb efficiency of 68 %. Skeleton-flesh structure is constructed by in-situ particle-embedded nanofiber and covered polymer, which strengthened mechanical capability, compatibility, inhibition of lithium dendrites , and introduced multi-Li + transport pathways, ensuring high safety and superior electrochemical performance for the applications of ASSBs.
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Zhitang Fang,Wanyun Li,Bangchuan Zhao,Jin Bai,Kunzhen Li,Hongyang Ma,Xuebin Zhu,Yuping Sun
A series of Li-rich Mn-based layered material Li1.2Ni0.13Co0.13Mn0.54O2 (LMR) with different particle sizes and particle-size distributions (PSDs) have been successfully synthesized via a combustion method using different manganese sources. The particle size of the N-LMR material prepared using Mn(NO3)2·4H2O as the manganese source is the smallest, and its PSD range is the narrowest among all of the samples. The unique particle size and PSD have a great influence on the electrochemical kinetics of Li-ion extraction/insertion reactions, leading to enhanced electrochemical performance when used as a cathode material for both the half and full Li-ion cells, especially the specific charge capacity at high current rates. The value of the charge specific capacity will determine the state of charge at the initial discharge stage and then influence the discharge process of these Li-rich Mn-based oxides. The N-LMR electrode delivers an initial discharge capacity of 309.2 mA h g–1 at 0.1C, and the specific capacity can reach up to 208.1 mA h g–1 at 1C. After 140 cycles, the electrode can still maintain 95.6% of its initial specific capacity at 1C. Moreover, the material displays a superior high-temperature lithium storage property at 55 °C and the full cells using N-LMR as the cathode material also show a much better electrochemical performance.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Qihang Yu,Wu Tang,Yang Hu,Jian Gao,Ming Wang,Sihong Liu,Huanhuan Lai,Liang Xu,Cong Fan
For the first time, two novel air-sensitive Li-rich organic cathodes ( m -TP4OLi and p -TP4OLi) are designed and reported. The structure-performance relationship for the two organic cathodes is comparatively studied. Using organic anode of lithium terephthalate (Li 2 TP), the resulting Li 2 TP II p -TP4OLi all-organic Li-ion batteries can deliver the peak discharge capacity of 330 mAh g −1 cathode in 1–3.4 V, corresponding to the high energy density of ~574 Wh kg −1 cathode using the median voltage of 1.74 V. Furthermore, the fabricated graphite II p -TP4OLi Li-ion batteries can show the peak discharge capacity of 305 mAh g −1 cathode in 1.5–3.4 V with a high median voltage of 2.4 V, resulting in the peak energy density of ~732 Wh kg −1 cathode (2.4 V × 305 mAh g −1 ). Meanwhile, the graphite II p -TP4OLi Li-ion batteries exhibit impressive device stability over 20,000 cycles. To the best of our knowledge, the peak energy density of our p -TP4OLi is currently the world record among Li-rich organic cathodes in lab conditions, outperforms the energy density of inorganic LiFePO 4 (~476 Wh kg −1 ), comparable with that of inorganic LiCoO 2 (~760 Wh kg -1 ) under the same lab conditions.
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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
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电化学
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能源存储
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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
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电化学
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电池技术
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DOI
高影响因子
DESALINATION
·
2024
·
IF 8.3
Peng Zhao,Fei Guo,Lingfeng Wang,Huange Zhen,Ning Zhang,Shaohua Yin,Guoli Zhou,Xuehua Ruan,Gaohong He,Xiaobin Jiang
Nanofiltration membranes with high selectivity and long-term stability for magnesium and lithium ions are crucial to efficiently enriching lithium resources in salt lake brines. Herein, a nano-gradient-structured nanofiltration membrane was fabricated, in which PEI with different molecular weights and TMC were utilized in a gradient interfacial polymerization process to construct the target active layer. Via this facile strategy, the grafting density of PEI and the amino group introduced were properly adjusted, and the pore size distribution and surface charge of the active layer were optimized. The fabricated active layer simultaneously possesses sub-nanometer pore size with a modified gradient structure and high interfacial positive charges, which can accurately screen lithium and magnesium. The successful grafting of secondary PEI and the high positive charge and continuity of the active layer have been demonstrated. After 150 hour operation (Mg/Li ratio of 50), PEI-70000/PA/PES nanofiltration membrane achieved a lithium‑magnesium separation factor (S Li/Mg ) as high as 150 while maintaining the stable permeation flux of approximately 20 L·m −2 ·h −1 ·MPa −1 , and the terminal Mg/Li ratio on the permeable side falls to 0.32, which exhibits significant potential for extracting Li from salt lake brines with high Mg/Li ratio with promising long-term stability.
研究领域:
材料科学
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环境工程
·
化学工程
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高影响因子
危险品化学品经营许可证（带存储）