Advanced Energy Materials
·
2025
·Vol. 15
·期 35
·2501255
·
IF 26
Mingyi Tang,Jianqi Sun,Caohua He,Chengyi Hou,Qinghong Zhang,Yaogang Li,Zongyi Qin,Kerui Li,Hongzhi Wang
Halide solid electrolytes (SEs) have emerged as promising candidates for all-solid-state batteries (ASSBs) owing to their considerable ionic conductivity, mechanical deformability, and compatibility with high-voltage cathodes. However, the conventional equimolar substitution strategy for developing halide SEs has limitations, as it fails to simultaneously ensure the presence of abundant vacancies and mobile Li-ions, which are two critical factors governing ionic conductivity. Herein, a non-equimolar substitution strategy is adopted to design a Li and vacancy co-enriched Li 2 Zr 0.75 Ta 0.2 Cl 6 with high ionic conductivity (1.74 mS cm −1 ) and compatibility with high-voltage Ni-rich cathode. Specifically, more Zr 4+ is substituted with less Ta 5+ to generate Zr-vacancies without depleting Li-ion content while maintaining charge neutrality. Under the Li-rich state, abundant Zr-vacancies provide additional Li-ion migration pathways within the non-Li-centered octahedral framework and promote uniform and efficient Li-ion transport. ASSBs assembled with single-crystalline LiNi 0.8 Co 0.1 Mn 0.1 O 2 (scNCM811) cathode demonstrate exceptional cycling stability with high-capacity retention (80.0% over 7800 cycles) and maintain stable cycling over 12 000 cycles at a high rate of 5 C. Notably, even under high loading conditions (20.62 mg cm −2 scNCM811), the ASSBs maintained a capacity retention of 80.8% over 800 cycles and 70.1% over 2300 cycles at a high rate of 1 C.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 41
·2103049
·
IF 18.808
Hao Li,Yunfei Du,Xiaomeng Wu,Jingying Xie,Fang Lian
The stringent demands for lithium salts make the design of “polymer-in-salt” type solid electrolyte restricted since it was proposed in 1993. Herein, a novel polymer-in-salt solid electrolyte is developed via a supramolecular strategy based on poly(methyl vinyl ether-alt-maleic anhydride) (PME) and novel single-ion lithiated polyvinyl formal (LiPVFM)/lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) composite salts (Dual-Li). Hydroxyl of LiPVFM in Dual-Li forms a strong hydrogen bond with the carboxylic acid group generated by the partial ring-opening reaction of maleic anhydride in PME. Meanwhile, PME with abundant carbonyl enables the improved LiTFSI coordination in the polymer/salt composites. As a result, the greatly enhanced mutual solubility of PME and Dual-Li is of importance to build a “polymer-in-salt” solid electrolyte (PISE), which exhibits high ionic conductivity of 3.57 × 10 –4 S cm –1 , wide electrochemical window beyond 5 V, and superior lithium-ion transference number of 0.62 at 25 °C as well as excellent interfacial compatibility with electrodes. The as-assembled LiCoO 2 ||Li solid batteries present prominent high-voltage cyclability with 89.2% capacity retention in 225 cycles. Furthermore, LiNi 0.7 Mn 0.2 Co 0.1 O 2 ||Li pouch cells exhibit remarkable safety even under harsh conditions. The study offers a promising strategy to address the high voltage compatibility and interfacial issues using PISE in solid-state batteries.
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高影响因子
Nano Energy
·
2021
·
IF 17.881
Yaoyao Li,Yuanpeng Liu,Lanxin Xue,Wei Chen,Tianyu Lei,Anjun Hu,Jianwen Huang,Xuepeng Wang,Xianfu Wang,Bo Chen,Yin Hu,Chengtao Yang,Jie Xiong
Lithium metal batteries (LMBs) have great potential for next-generation rechargeable batteries due to the high theoretical capacity and ideal compatibility coupled with diverse cathode materials . However, the random Li deposition associated with the large local space charge caused by the anion depletion near the surface of anode, as well as the insufficient reduction of Li + related to the suppressed Li + solvation process induced by the electrostatic force between anion and cation hinder the development of high-energy-density LMBs. Herein, as evidenced theoretically and experimentally, we simultaneously eliminate the anion depletion region and promote the lithium salt dissociation by employing ZIF-67 with unsaturated metal sites as anionphilic additive to regulate anion distribution and weaken its bond with Li + . As a result, the short-circuit hazard is remitted in symmetrical cell with modified electrolyte at 3 mA cm −2 under capacity of 3 mAh cm −2 for more than 2000 h. As employed for the lithium-sulfur battery with high sulfur loading of 4.5 mg cm −2 , the modulated electrolyte enables the battery delivering an initial capacity of 713 mAh g −1 with decay rate of 0.05% per cycle over 100 cycles at 3 mA cm −2 . This work demonstrates an efficient and scalable strategy for constructing dendrite-free LMBs via eliminating the anion depletion region and facilitating the Li + solvation process.
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高影响因子
DESALINATION
·
2024
·
IF 8.3
Li Wang,Jianfeng Zhang,Shixin Meng,Huiyong Wu,Yunze Zhao,Zhen Meng,Lei Feng,Huanting Wang,Yuan Cheng,Liangrong Yang,Huizhou Liu
The dissolution loss of extractant into aqueous solution during lithium solvent extraction from salt lakes poses a significant issue. We found that branched chains of neutral organophosphorus extractants provide suitable steric hindrance, enhancing lithium extraction efficiency and Li/Mg selectivity. Additionally, increasing the number of alkyl chains in organophosphorus extractants increases their hydrophobicity, thereby reducing extractant dissolution loss during the extraction process. Based on these findings, a novel extraction system comprising tri(2-ethylhexyl) phosphate (TOP), FeCl 3 , and 4-methyl-2-pentanone (MIBK) was explored. The extraction conditions, including the Fe/Li molar ratio, diluents, phase ratio, and stripping conditions, were thoroughly investigated and optimized. The extraction mechanism was elucidated at the molecular level using FT-IR, Raman, NMR, and density functional theory (DFT) calculations. The results demonstrated that the TOP-FeCl 3 -MIBK system achieved an 85 % extraction efficiency for Li + in a single stage, with a Li + /Mg 2+ separation factor reaching 5842, surpassing previously reported data in the literature. 31 P NMR and 7 Li NMR analyses revealed that the TOP and tributyl phosphate (TBP) complexes existed in different forms within the organic phase. Slope analysis indicated that the stoichiometric ratio of the extraction complex involving Li + , TOP, and MIBK was LiFeCl 4 ·TOP·MIBK. Furthermore, DFT calculations indicated that the TOP complex was more stable than the TBP complex after extraction. We anticipate that our findings will pave the way for the development of a series of novel extractants with higher Li/Mg selectivity by enhancing steric hindrance and incorporating longer alkyl chains to minimize dissolution loss. We expect this research to inspire the development of similar neutral organophosphorus extractants.
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高影响因子
DESALINATION
·
2024
·
IF 8.3
Xunshuang Zhang,Junxiang Wu,Yu He,Chenhao Zhao,Minfang An,Liangbin Li
Lithium (Li) reserves in liquid resources are significantly higher than solid lithium ores and can fully meet the growing demand for Li. Lithium-ion sieves (LIS) adsorption of Li from liquid resources is one of the most promising methods. However, conventional polymeric adsorption materials encapsulate most LIS in dense structures, leading to low adsorption capacity and slow adsorption rate. Therefore, HTO-PVA/PAAm hydrogel was synthesized from titanium-type lithium-ion sieves (HTO), acrylamide, and polyvinyl alcohol by free radical polymerization. The HTO-PVA/PAAm hydrogel is characterized by a soft three-dimensional (3D) network, continuously adjustable pore structure, high specific surface area, and excellent hydrophilicity. Accordingly, the HTO-PVA/PAAm owns an excellent Li + adsorption capacity (22.16 and 31.31 mg·g −1 in pH 7.2 and 12 of LiCl solutions, respectively) among reported advanced adsorbents. 90 % of Li + is desorbed within 60 min, indicating the efficient and rapid Li + desorption response of the hydrogel. Meanwhile, this hydrogel still maintains a Li + adsorption capacity of 90 % after eight adsorption-desorption cycles, during which Ti loss is <0.42 % in each cycle. In this work, HTO-PVA/PAAm hydrogel synthesized by an environmentally friendly and low-cost approach shows great application potential as a new strategy for Li + adsorption from liquid resources.
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高影响因子
Interdisciplinary Materials
·
2025
·Vol. 4
·期 6
·914-926
·
IF 31.6
Wanqing Ren,Yang Li,Xingyi Peng,Meng Wu,Xiang Qi,Peng Lei,Changyi Fan,Ce-Wen Nan,Li-Zhen Fan
Zirconium-based halide electrolytes were created as prospective candidates for all-solid-state lithium batteries (ASSLBs) because of their low cost, wide electrochemical window, and superior compatibility with oxide cathodes. However, practical implementation is hindered by limitations such as suboptimal room-temperature (RT) ionic conductivity (< 1 mS cm −1 ) and poor interfacial compatibility with lithium metal. Herein, we report a new class of zirconium-based chlorides, Li 2− x Zr 1− x Nb x Cl 6 , synthesized by a high-valent Nb 5+ doping method. The introduction of Nb 5+ induces local lattice decrease, which simultaneously weakens the binding intensity of Li─Zr and optimizes ion migration pathways and defect concentrations. Therefore, the optimal composition, Li 1.75 Zr 0.75 Nb 0.25 Cl 6 (denoted as LZC-Nb), achieves a high RT ionic conductivity of 1.82 mS cm −1 and exceptional moisture resistance. Furthermore, the dynamic interfacial modulation of LZC-Nb forms a low-impedance passivation layer, enhancing Li + transport kinetics. This improvement in interfacial stability enables symmetric batteries to exceed a critical current density of 1.3 mA cm −2 . Combined with a LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode, the resultant ASSLB retains 81.8% of its initial capacity (157.5 mAh g −1 ) after 600 cycles at 0.3 C. This study provides a proven strategy for developing inorganic ionic conductors with superior ionic transport and interfacial compatibility, offering a viable pathway toward high-performance ASSLBs.
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高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Hao Wang,Wujie Ge,Wen Li,Feng Wang,Wenjing Liu,Mei-Zhen Qu,Gongchang Peng
Dealing with the water molecule on the surface of LiNi0.6Co0.2Mn0.2O2 (NCM) cathode and hydrogen fluoride in the electrolyte is one of the most difficult challenges in Li-ion battery research. In this paper, the surface polymerization of tetraethyl orthosilicate (TEOS) on NCM to generate ethoxy-functional polysiloxane (EPS) wrapped NCM (E-NCM) cathode under mild conditions and without any additions is utilized to solve this intractable problem. The differential scanning calorimetry, transmission electron microscopy, and X-ray photoelectron spectroscopy results show that the formed amorphous coating can provide a protective shell to improve the NCM thermal stability, suppress the thickening of the solid electrolyte interphase (SEI) layer, and scavenge HF in the electrolyte. The E-NCM composite with 2 mol % EPS delivers a high discharge capacity retention of 84.9% after 100 cycles at a 1 C discharge rate in the 2.8–4.3 V potential range at 55 °C. Moreover, electrochemical impedance spectroscopy measurements reveal that the EPS coating could alleviate the impedance rise during cycling especially at an elevated temperature. Therefore, the fabricated E-NCM cathode with long-term cycling and thermal stability is a promising candidate for use in a high-energy Li-ion battery.
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PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Yunhao Li,Shuhao Wang,Wenyuan Wu,Haijun Yu,Ruxin Che,Guodong Kang,Yiming Cao
Nanofiltration is considered a promising technology for separation of multivalent/monovalent ions such as extracting lithium from Salt Lake brine with high Mg 2+ /Li + ratio. However, the nanofiltration membranes fabricated via conventional interfacial polymerization process generally possess negatively charged surface and have low Mg 2+ /Li + selectivity. Herein, we proposed a new and facile method, i.e., reversed interfacial polymerization (RIP), to prepare nanofiltration membranes with positively charged surface and uniform charge distribution. The sequence of amine (polyethyleneimine, PEI) and acyl chloride (trimesoyl chloride, TMC) monomers on polysulfone support was reversed compared to the conventional interfacial polymerization (IP) process. Moreover, the solvent of amine monomer was acetone instead of water. The nanofiltration membranes fabricated by this method exhibited higher water flux (from 4.88 to 22.25 Lm −2 h −1 ) and MgCl 2 rejection (from 84.36% to 97.71%). Meanwhile, LiCl/MgCl 2 separation factor in single salt solution reached up to 13.93, which was almost quadruple compared to the conventional control membrane. In addition, the developed nanofiltration membrane also exhibited an excellent separation selectivity ( S Li, Mg = 9.22) in mixture system (Mg 2+ /Li + mass ratio of 20), which had good application potential in extracting lithium resources from Salt Lake brine.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2017
·
IF 3.133
Zhongdong Peng,Ying Li,Ke Du,Yanbin Cao,Guorong Hu
In order to improve the electrochemical performance of LiMn 2 O 4 at elevated temperatures, a series of Li 1.2 Ni 0.2 Mn 0.6 O 2 -modified LiMn 2 O 4 samples have been synthesized by a facile sol-gel method. The structure and morphology of pristine and modified LiMn 2 O 4 are investigated by X-ray diffraction (XRD) and scanning electron microscopy (SEM), respectively. The Li 1.2 Ni 0.2 Mn 0.6 O 2 coating layer is identified by transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS), which plays an important role in reducing the dissolution of manganese, thereby improving the cycle performance and rate capability of the material. The 2 wt% Li 1.2 Ni 0.2 Mn 0.6 O 2 -modified LiMn 2 O 4 sample exhibits a higher capacity retention of 95.88% than that of the pristine one (81.2%) after 200 cycles at 1C and 25 °C. Furthermore, a capacity retention of 89.74% is obtained for the 2 wt%-modified LiMn 2 O 4 sample after 200 cycles at 1C and 55 °C, compared to 66.34% for the pristine one. Surface modification with a Li-rich Li 1.2 Ni 0.2 Mn 0.6 O 2 material is a good way to improve the elevated temperature performance of LiMn 2 O 4 .
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高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Xingtao Qi,Ze Zhang,Chuanbao Tu,Chao Zhu,Junchao Wei,Zhenyu Yang
Due to the deficiency of low melting point and poor wettability of commercial polyolefin separators, the design and development of ceramic coating separators have been received more and more attention in Li-ion batteries recently. However, it is challenging to solve the disadvantageous exfoliation issue of ceramic coating during charge/discharge cycles and needs to be addressed urgently. Herein, a covalent grafting interface engineering strategy has been proposed to prepare a highly efficient and stable polypropylene/mSiO 2 separator (PP-g-mSiO 2 ) by the nanoscale mSiO 2 layer anchoring on the surface of PP separator with covalent bonding. As expected, the covalent bonding force increase the interfacial stability of PP-g-mSiO 2 separator and the mSiO 2 NPs facilitate more storage of electrolyte, which results in high thermal stability, high electrolyte affinity and swift lithium-ion diffusion . When used as the separator in LIBs, the Li/LiFePO 4 cell with PP-g-mSiO 2 separator exhibits excellent rate capability with a discharge capacity of 101 mA h/g at 5 C and remains high capacity retention of 93% after 1000 continuous charge–discharge cycles, which suggests that the PP-g-mSiO 2 separator possesses a stable and covalent grafting ceramic surface and have greater affinity to electrolyte, resulting in quicker lithium-ion diffusion and excellent cycling stability. Therefore, the covalent grafting interface modification has confirmed an effective strategy to block exfoliation issues of ceramic coating and developed the high-performance ceramic separators for LIBs.
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高影响因子
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION A-A JOURNAL OF PHYSICAL SCIENCES
·
2023
·Vol. 78
·期 10
·921-926
·
IF 1.8
Cong Liu,Junshen Xing,Zheng Liu,Wenlin Feng
BaSr 2 (PO 4 ) 2 : 4 %Eu 3+ , 4 % A ( A = Li + , Na + , K + ) phosphors were prepared by high-temperature solid-phase method. The crystal structure, photoluminescence properties, thermal stability, chromaticity coordinates, and fluorescence lifetime of the samples were investigated. The excitation and emission spectra of the samples are broadbands and the maximum peak of the emission spectrum is located at 619 nm. Among three charge compensators, the luminescence intensity is optimal for Li + co-doping case, and the quenching temperature of the typical sample is about 500 K. the fluorescence lifetime
τ
is 1469.6 ns, and the chromaticity coordinates exhibit a strong red emission. The present phosphor has a potential application for white light-emitting diodes (LEDs) under the near-ultra violet (n-UV) light excitation.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Yifan Wang,Weisen Yang,Chunmei Zhang,Xiaoshuai Han,Jingquan Han,Shuijian He,Jiapeng Hu,Shaohua Jiang
Herein, balsa wood, poplar wood, and birch wood were selected to systematically study precursors on the structure and Li-storage properties of wood-based hard carbon thick electrodes (WHCTEs). After carbonization, the densities of balsa, poplar, and birch carbon (Bal-W, Pop-W, and Bir-W) reach 99.29, 279.13, and 608.14 mg cm⁻ 3 , respectively. The specific surface areas of Bal-W, Pop-W, and Bir-W are 798, 729, and 609 m 2 g⁻ 1 , respectively. Bal-W is rich in mesopores at 2–4 nm; Pop-W also has a certain amount of mesopores; while Bir-W has almost no mesopores but large numbers of micropores concentrated at 1.2 and 1.6 nm. In the battery test, due to the highest mass loading, Bir-W retained the largest remaining capacity among the three samples after 200 cycles at 1 mA cm⁻ 2 . The remaining capacities of Bal-W, Pop-W, and Bir-W are 12.27, 34.15, and 41.03 Ah L⁻ 1 , respectively. It is found that mass loading, specific surface area, and pore size distribution have a greater influence on the electrode capacity performance. In addition, the kinetic features of the Li-ion storage of WHCTEs were studied. This work may provide an important reference for the field of WHCTEs for alkali metal ion batteries and can promote its practical application.
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高影响因子
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