ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Binyu Lu,Liuyi Hu,Wenkui Zhang,Jun Zhang,Yang Xia,Yongping Gan,Xinping He,Xinhui Xia,Ruyi Fang,Hui Huang
Construction of quasi-solid-state lithium metal batteries (LMBs) by in situ polymerization is considered a key strategy for the next generation of energy storage systems with high specific energy and safety. Poly(1,3-dioxolane) (PDOL)-based electrolytes have attracted wide attention among researchers, benefiting from the low cost and high ionic conductivity. However, interfacial deterioration and uncontrollable growth of lithium dendrites easily appeared in LMBs due to the high reactivity of lithium metal, resulting in the failure of LMBs. In this work, a strategy is developed of using Ga(OTF)3 as the initiator to obtain a PDOL-based gel electrolyte (GaPD). In addition, a hybrid stable solid electrolyte interphase (SEI) of lithium fluoride/Li2O/Li–Ga alloys is observed on the surface of lithium metal. Combined with density functional theory calculations, the hybrid SEI shows high affinity toward Li+, indicating that a uniform deposition of Li+ could be achieved. Therefore, the Li/GaPD/Li cell operates stably for 1600 h at room temperature. In addition, the LiFePO4/GaPD/Li cell retains a capacity retention rate of 90.2% over 200 cycles at 1 C. This work provides a reference for the practical application of in situ polymerization technology in high-performance and safe LMBs.
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高影响因子
ChemElectroChem
·
2020
·Vol. 7
·期 11
·2389-2394
·
IF 4.154
Xiang Peng,Kai Huang,Shipai Song,Fang Wu,Yong Xiang,Xiaokun Zhang
A garnet-polymer composite electrolyte with high Li + conductivity and transference number is developed using microporous Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) framework as the matrix. The LLZTO framework, fabricated by a template-assisted gel-casting process, possesses micron-sized grains and well-fused grain boundaries, eliminating the low-conductive bottleneck at the interfaces between the ceramic blocks, and providing conductive and continuous networks for Li + transport. As a result, the garnet-polymer composite electrolyte displays a high ionic conductivity (2.61×10 −4 S cm −1 at 25 °C), an ultrahigh Li + transference number of 0.71, as well as excellent thermal, structural, and electrochemical stabilities. Benefiting from the desired physical and chemical properties, the presented composite electrolyte enables a Li−Li cell to be cycled for more than 600 h at 25 °C. In addition, the integrated LiFePO 4 /CPCE/Li cells also show excellent cycling stability with a specific capacity of 133.2 mAh g −1 after 100 cycles under 50 °C. This study demonstrates a significant optimization on the microstructure of composite electrolytes that can be utilized for all-solid-state lithium batteries. Graphical Continuous paths : We demonstrated a garnet-polymer composite electrolyte exhibiting excellent Li+ conductivity and transference number, by applying a microporous Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) framework with well-fused grain boundary
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Small
·
2025
·
IF 12.1
Xiangxiang Chen,Junru Wu,Wentao Zhang,Ji Li,Ziyao Gao,Xu Zhao,Kuang Yu,Yan-Bing He,Baohua Li,Feiyu Kang,Lele Peng
Constructing robust solid-electrolyte interphase (SEI) on electrodes is crucial for achieving stable lithium metal batteries in liquid electrolytes. However, intrinsic issues associated with liquid electrolytes remain unavoidable, such as the continuous corrosion of SEI and the high costs involved. Herein, a novel lithium salt-free solid-state polymer electrolyte (SPE) is introduced enabled by in situ polymerization of 1,3-dioxolane and 1,3,5-trioxane with the addition of ionic liquid to eliminate the drawbacks of liquid electrolyte. The homogeneous interaction between the polymer and ionic liquid constructs a synergistic Li + conduction pathway, promoting the extraction of Li + out of the cathode/anode and the smooth transport throughout the polymer network to endow a higher Li + transference number (0.63) and a comparable ionic conductivity (1.21 mS cm −1 ) to the conventional liquid electrolyte (0.45 and 5.51 mS cm −1 ). The absence of lithium salt prevents the oxidative decomposition of lithium salts in electrolytes to generate hazardous and corrosive acidic species. More intriguingly, an anion-dominated solvation configuration can be realized by the incorporation of ionic liquid with the polymer matrix, inducing the formation of an inorganic-rich and anti-corrosive SEI on the electrodes. The resulting salt-free SPE enables superior cycling stability in lithium||LiFePO 4 battery with a high capacity retention of over 92% after 780 cycles.
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产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2021
·Vol. 8
·期 9
·2003887
·
IF 16.806
Yiyuan Yan,Jiangwei Ju,Shanmu Dong,Yantao Wang,Lang Huang,Longfei Cui,Feng Jiang,Qinglei Wang,Yanfen Zhang,Guanglei Cui
Solid-state lithium battery promises highly safe electrochemical energy storage. Conductivity of solid electrolyte and compatibility of electrolyte/electrode interface are two keys to dominate the electrochemical performance of all solid-state battery. By in situ polymerizing poly(ethylene glycol) methyl ether acrylate within self-supported three-dimensional porous Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 framework, the as-assembled solid-state battery employing 4.5 V LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode and Li metal anode demonstrates a high Coulombic efficiency exceeding 99% at room temperature. Solid-state nuclear magnetic resonance results reveal that Li + migrates fast along the continuous Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 phase and Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 /polymer interfacial phase to generate a fantastic conductivity of 2.0 × 10 −4 S cm −1 at room temperature, which is 56 times higher than that of pristine poly(ethylene glycol) methyl ether acrylate. Meanwhile, the in situ polymerized poly(ethylene glycol) methyl ether acrylate can not only integrate the loose interfacial contact but also protect Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 from being reduced by lithium metal. As a consequence of the compatible solid-solid contact, the interfacial resistance decreases significantly by a factor of 40 times, resolving the notorious interfacial issue effectively. The integrated strategy proposed by this work can thereby guide both the preparation of highly conductive solid electrolyte and compatible interface design to boost practical high energy density all solid-state lithium metal battery.
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高影响因子
Energy Materials
·
2025
·Vol. 5
·期 4
·N
·
IF 11.2
Dongwei Zhou,Guiyang Gao,Zhanlin Yang,Weibin Guo,Liang Lin,Yinggan Zhang,Chengkun Zhang,Saichao Li,Yuanyuan Liu,Baisheng Sa,Guoying Wei,Dong-Liang Peng,Jie Lin,Qingshui Xie
Li-rich Mn-based cathode materials (LRM) have received great attention owing to their high capacity and low cost. However, the mismatch between the widely used carbonate electrolyte and the LRM cathode and lithium metal anode causes a series of problems, such as electrolyte continuous oxidation, cathode structure degradation, and Li dendritic growth. Herein, inorganic oxide B2O3 is introduced as a dual-functional high-voltage electrolyte additive to construct stable cathode electrolyte interphase and solid electrolyte interphase for Li||LRM batteries. The modified interface derived from the additive can induce dendrite-free Li deposition, stabilize cathode structure, and inhibit transition metal dissolution. Moreover, the adverse side reactions are mitigated, thus enhancing Li+ transport rate and reducing interface impedance. With the addition of B2O3 into the carbonate electrolyte, the Li||LRM battery exhibits an enhanced discharge capacity of 221 mAh g-1 after 200 cycles, equaling a capacity retention of 92.1%. When the upper cut-off voltage is increased to 5 V, a superior capacity retention of > 85% can still be achieved after 150 cycles at 1 C. In addition, the low cost of B2O3 benefits for commercial application. This work offers new guidance for the research of low-cost, high-voltage dual-functional additives for advanced lithium metal batteries.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Hui Yang,Baozhong Ma,Shuyang Shi,Jiancheng Yu,Yubo Liu,Zhihe Cao,Chengyan Wang
The alkali method has been proven to be an effective approach for lithium (Li) and rubidium (Rb) extraction; however, the significant dissolution of silicon (Si) remains a challenging issue. A high Si concentration in the leachate can cause filtration difficulties and pipeline blockages, while also negatively affecting phase separation during the subsequent extraction of Rb. Additionally, since the leachate needs to be recycled, the removal of Si from the leach liquor is essential. This study introduces an innovative approach of adding Al(OH) 3 for Si removal during the alkali leaching of lithium concentrate. Preliminary single-factor experiments demonstrate that Al(OH) 3 effectively reduces the Si concentration in leach liquor but also consumes NaOH, leading to a decline in Li and Rb leaching efficiency. Given the interaction between Al(OH) 3 addition and NaOH concentration on element leaching, Response Surface Methodology was employed to predict and optimize the parameters of the leaching process. Under the optimal parameters of 290 g/L NaOH concentration, 39 % Al(OH) 3 addition, and 120 °C leaching temperature, the experimental leaching efficiencies of Li, Rb, and Si were 99.8 %, 87.9 %, and 4.1 %, respectively. Subsequently, Rb was separated with Li via solvent extraction under high alkaline conditions. The single-stage extraction efficiency of Rb was 82.8 % at optimized conditions, and after four-stage countercurrent extraction, the overall Rb recovery could reach 99.2 %. The innovative alkali method proposed not only enables the synergistic extraction and separation of Li and Rb but also achieves effective Si removal and its utilization.
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Jiayi Wang,Yichen Hao,Jinping Li,Jiangfeng Yang
The shortage of lithium resources and the accumulation of retired batteries are strategic issues that need to be addressed urgently. Here, we propose an innovative and efficient strategy for the preferential extraction of Li+, followed by the sequential recovery of Mn2+ and Co2+, utilizing GIS zeolite from battery leachate. Li+ ions were preferentially exchanged, achieving a 95% recovery rate at 0 °C; subsequently, 94% of Mn2+ and 97% of Co2+ were recovered by increasing the temperature to 40 and 60 °C; meanwhile, 90% of Ni2+ remains in solution. The fastest kinetic rate of Li+ in GIS zeolite and its efficient extraction at low temperatures were verified through ion exchange processes; at higher temperatures, the adsorption capacity and selectivity of GIS zeolite for Co2+ and Mn2+ increased. We found the diffusion rate of Li+ in GIS zeolite to be over 2.5 times faster than that of Mn2+, Co2+, and Ni2+, which all have the same rate by molecular dynamics simulations. The ion exchange of Mn2+, Co2+, and Ni2+ was an endothermic reaction, with the ΔH0 and ΔG0 following the order Mn2+ < Co2+ < Ni2+ by thermodynamic calculations. The regeneration ability of GIS zeolite indicated its promising industrial application prospects.
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Peng Zeng,Hao Yu,Hong Liu,Yongfang Li,Ziyi Zhou,Xi Zhou,Changmeng Guo,Bin Li,Manfang Chen,Zhigao Luo,Ying Wang,Baobao Chang,Xianyou Wang
The application of Li-S batteries is hampered by some unresolved issues, including the severe polysulfides shuttle effects and sluggish reaction kinetics. Hence, we designed and prepared tin oxide hydroxide quantum dots (TOH) anchored on a honeycomb porous carbon (HPC) matrix as multifunctional sulfur hosts, and deeply studied the enhancement of TOH on the reaction kinetics of Li-S battery referred to as the apparent activation energy, Li+ ion diffusion coefficient, and reaction barrier. It is proved by density functional theory that the HPC@TOH hosts have a higher binding energy to polysulfides than the simplex carbon matrix. Meanwhile, the catalytic TOH can decrease the surface active energy of the redox reaction and accelerate the conversion of sulfur-containing species. Consequently, by means of the synergistic effects of physical capture and chemical adsorption together with catalytic conversion, the comprehensive performances of Li-S batteries are distinctly promoted. In particular, a Li-S battery using HPC@TOH as a host delivers a good reversible specific capacity of 1342.95 mAh g–1 at 0.1 C. Moreover, with the current increased to 1 C, it shows a relatively satisfactory specific capacity of 918.05 mAh g–1. After 400 cycles, a competitive specific capacity of 688.54 mAh g–1 can still be maintained with a very low fading rate of 0.06% per cycle. Most importantly, when the sulfur areal loading reaches as high as 4.25 mg cm–2 and electrolyte/sulfur ratio is controlled to be as low as 7 μL mg–1, and the Li-S battery using HPC @TOH as a host can still cycle steadily more than 50 cycles at 0.2 C. Therefore, this work provides an effective manner to boost the comprehensive performance of Li-S batteries by virtue of optimizing and designing the host material with synergistic effects of physical capture, chemical adsorption, and catalytic conversion.
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高影响因子
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Kang-Ning Gao,Hao-Ran Wang,Ming-Hui He,Yi-Qiu Li,Zhong-Hui Cui,Ya Mao,Tao Zhang
The development of solid-state lithium-oxygen batteries is currently limited primarily by the high solid-solid interfacial resistance and the lack of efficient assembly of electrolyte and electrode. In this work, noncovalent interactions between the cations of an ammonium ionic liquid and both solid electrolytes and carbon air cathodes are introduced. The ionic liquid-based electrolytes (ILE) are solidified on Li 6·40 La 3 Zr 1·40 Ta 0·60 O 12 (LLZTO) nanoparticles and gelated by multi-wall carbon nanotubes (MWCNTs), respectively, to construct LLZTO@ILE quasi-solid-state electrolyte (QSSE) and MWCNTs-LLZTO/ILE gel cathode (GC). The QSSE exhibits a high ionic conductivity of 1.71 × 10 −3 S cm −1 at 60 °C, high Li-ion transference number of 0.56, broad electrochemical window of ~4.8 V and good thermal stability . The GC shows outstanding compatibility with QSSE. Quasi-solid-state Li–O 2 batteries are assembled by integrating QSSE and GC films with a facile roll forming method, showing a low total interfacial resistance (~87 Ω cm 2 ), and excellent reversible cycles (70 cycles) with low charge overpotential (<0.44 V) and quite high electrical energy efficiency (>70%) at 60 °C and 200 mA g −1 . A 0.12 Ah pouch-type Li–O 2 battery was achieved by this method. These results suggest that the noncovalent interactions initiated by IL cations could be an effective approach to solve the solid-solid interface issue and achieve high discharge capacity in solid-state energy storage devices.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 47
·27095-27101
·
IF 12.732
Zilong Zhuang,Chang Liu,Yiyang Yan,Pengcheng Ma,Daniel Q. Tan
Lithium metal anode (LMA) possesses the largest energy density among all anode candidates, while dendrite growth is a huge barrier in the direct application of LMA in batteries. Herein, metal–organic framework (MOF) derived Zn–CxNy nanoparticle arrays are newly grown onto carbon cloth as an effective host toward lithium metal anode. The N and Zn species are lithiophilic to Li-ions, resulting in a stable Li plating/stripping process of up to 2300 h without running into a dendrite issue when operating at a current density of 10 mA cm−2. The newly developed ZNCC-Li anode also exhibits an ultralow voltage hysteresis of only 6.4 mV at the end of the operating process. This work creates an effective design of MOF-derived lithium metal anode suitable for high-energy batteries.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Pengfei Wan,Siyang Dong,Jing Xiong,Xuanyang Jin,Shengjun Lu,Yufei Zhang,Haosen Fan
Lithium sulfur batteries (LSBs) have been considered as one of the most promising options for next generation high-performance batteries. However, the heavy shuttle effect and inferior redox conversion during the charge/discharge processes of the batteries have greatly hindered their further applications. In this study, to address these disadvantages of LSBs, Fe/Fe 3 C/FeN 0.0324 heterostructured nanocubes were designed and prepared through high temperature carbonization process using Prussian blue precursor. Then the Fe/Fe 3 C/FeN 0.0324 nanocubes were used to modify the commercial polypropylene (PP) separator, which can greatly catalyze the redox transformation of polysulfides and provide sufficient active sites for chemisorption . As result, the modified separator endowed LSBs with excellent rate capacity and cycle stability, delivering a high-capacity of 1025 mAh/g at 0.5 C with nearly 100% coulombic efficiency. It also displayed a superb cycling performance with a per-cycle capacity attenuation rate of 0.09% after 300 cycles. When the current density increased to 1 C with the S loading of 1.73 mg cm −2 , Fe/Fe 3 C/FeN 0.0324 -PP separator presented a satisfactory capacity decay rate of 0.05% per cycle after 1000 cycles. Besides, it also presented outstanding electrochemical performance even at high sulfur loading of 4.5 mg cm −2 . This work has provided a new avenue for the design of nanomaterials with synergistic effect of catalytic conversion and chemisorption of polysulfides for the promotion of high-performance Li-S batteries.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jie Cui,Yunfei Du,Long Zhao,Xiaocheng Li,Zixu Sun,Dong Li,Hao Li
Rechargeable batteries paired with polyether-based solid-state electrolytes is a promising system to solve the safety problem of lithium metal (Li-metal) batteries, and stable solid electrolyte interface (SEI) layer between electrolyte and anode is highly required for their long-term stability. Here we propose a novel thermal-stable polymerized 1,3-dioxolane electrolyte (PSiDOL), which is in situ formed via a multifunctional 1,3-bis(3-glycidoxypropyl) tetramethyl disiloxane crosslinker. This network structural PSiDOL not only achieves good flame retardancy, significantly increased operating temperature and improved oxidative stability, but also induces the formation of stable and robust SEI layer with rich Li x SiO y /LiF on the surface of Li-metal anode. Moreover, the three-dimensional polymer skeleton with abundant polar groups is beneficial to improve the ionic conductance and cationic transference number. As a result, the PSiDOL electrolyte enable ultralong-term (over 4000 h) reversible and stable lithium plating/stripping in Li symmetrical cell for lithium anode. In addition, the assembled full cells based on such electrolyte display desirable cycling stability at high temperature and high voltage with suppressed electrolyte degradation. This work affords a facile and practical approach to develop advanced electrolytes for solid-state Li-metal batteries with high safety and durability.
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高影响因子
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