Small
·
2023
·Vol. 19
·期 39
·2302691
·
IF 13.3
Jing Yu,Guodong Zhou,Yueqing Li,Yuhao Wang,Dengjie Chen,Francesco Ciucci
Composite polymer-ceramic electrolytes have shown considerable potential for high-energy-density Li-metal batteries as they combine the benefits of both polymers and ceramics. However, low ionic conductivity and poor contact with electrodes limit their practical usage. In this study, a highly conductive and stable composite electrolyte with a high ceramic loading is developed for high-energy-density Li-metal batteries. The electrolyte, produced through in situ polymerization and composed of a polymer called poly-1,3-dioxolane in a poly(vinylidene fluoride)/ceramic matrix, exhibits excellent room-temperature ionic conductivity of 1.2 mS cm −1 and high stability with Li metal over 1500 h. When tested in a Li|electrolyte|LiFePO 4 battery, the electrolyte delivers excellent cycling performance and rate capability at room temperature, with a discharge capacity of 137 mAh g −1 over 500 cycles at 1 C. Furthermore, the electrolyte not only exhibits a high Li + transference number of 0.76 but also significantly lowers contact resistance (from 157.8 to 2.1 Ω) relative to electrodes. When used in a battery with a high-voltage LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode, a discharge capacity of 140 mAh g −1 is achieved. These results show the potential of composite polymer-ceramic electrolytes in room-temperature solid-state Li-metal batteries and provide a strategy for designing highly conductive polymer-in-ceramic electrolytes with electrode-compatible interfaces.
研究领域:
材料科学
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电化学
·
能源存储
·
固态电池
·
高分子化学
·
无机非金属材料
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Jinhai You,Haotian Deng,Xiaomei Zheng,Hao Yan,Li Deng,Yao Zhou,Juntao Li,Miaogen Chen,Qiong Wu,Pengyue Zhang,Hui Sun,Jie Xu
Li metal anodes (LMAs) are promising candidates for the anodes of high-energy-density batteries due to their lower reduction potential and high specific capacity. Unfortunately, LMAs usually suffer from uncontrollable Li plating and insecure solid electrolyte interphase layers, especially when used in conjunction with carbonate-based electrolytes. Herein, we proposed using metal alkoxides of titanium butyrate to react with hydroxyl groups on Li metal. A composite protective layer containing TiO2 and ROLi was generated to modify Li (designated as treated Li), leading to dendrite-free LMAs and achieving significantly enhanced cycling stability. Notably, symmetric cells using treated Li electrodes can deliver over 1500 h of stable cycling under a current density of 2 mA cm–2 in an ether-based electrolyte. Moreover, under extreme conditions of 5 mA cm–2 using a carbonate-based electrolyte, symmetric cells employing a treated Li electrode demonstrated stable cycling for over 80 h, as compared to the fluctuating voltage seen after only 10 h of cycling when using a bare Li electrode. Furthermore, full cells using a treated Li anode coupled with a high loading of LiCoO2 cathode (≈15 mg cm–2) displayed excellent cycling stability at 0.2 C over 150 cycles with a high capacity retention of 98.1% and an enhanced average Coulombic efficiency above 99.6%. By comparison, full cells using the bare Li anode drop to 125.4 mA h g–1 with a capacity retention of just 83.3%. The treated Li exhibited superior rate performance and delivered 132.7 mA h g–1 even at 5 C. This strategy provided a facile and effective option for the construction of advanced LMAs.
研究领域:
材料科学
·
电化学
·
储能
·
电池技术
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Depeng Song,Zewen Yang,Qing Zhao,Xiaolin Sun,Yue Wu,Yuan Zhang,Jing Gao,Cheng Wang,Li Yang,Takeo Ohsaka,Futoshi Matsumoto,Jianfei Wu
Li-rich cathodes have potential for use in next-generation Li-ion batteries (LIBs) owing to their high specific capacity and low cost. However, their intrinsic cycling decay and voltage fading limit practical applications. In addition, these cathodes contain Co, which is nonrenewable, scarce, and expensive. This situation severely limits the rapid and sustainable development of low-cost LIBs. This paper introduces a novel dilute electrolyte to overcome these limitations based on the Co-free Li-rich Li1.2Mn0.54Ni0.26O2 (LMNO) cathode. An even and robust cathode-electrolyte interface (CEI) formed on the surface of LMNO further protects it from side reactions in the dilute electrolyte. This Co-free Li-rich cathode exhibits the best electrochemical performance reported to date among Li-rich cathodes in terms of outstanding cycling stability (capacity retention of 99.8% at 0.5 C) and dramatically suppressed voltage fading (only 0.3% after 100 cycles). This study demonstrates the potential of Co-free Li-rich cathodes for applications in next-generation LIBs.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
DESALINATION
·
2026
·
IF 9.9
Yaoxian Hu,Binbin Zhou,Xinyu Xiao,Hui Su,Wensen Liu,Zhaowu Zhu,Tao Qi
Dual roles of electronic effect and steric hindrance in NOPs are decoupled. • A structure-performance paradox in linear and branched NOPs is revealed. • The intrinsic Li + /Mg 2+ micro-solvation divergence (CIP vs. SSIP) is uncovered. • A dual-parameter model is established to predict extraction capacity and selectivity. This study proposes a synergistic electronic effect and steric hindrance regulation mechanism in neutral organophosphate-extraction systems targeting efficient Li and Mg extraction from salt lake brines. Using tributyl phosphate (TBP), tripentyl phosphate (TAP), and triisoamyl phosphate (TIAP) as model extractants, we decoupled the dual roles of linear-chain elongation and branching in alkyl chain structures. The former enhances the P O electron density and intrinsic Li + affinity via the positive inductive effect, whereas branched structures govern the selectivity via steric hindrance. Combined molecular dynamics (MD) simulations and density functional theory (DFT) calculations revealed that Li + forms a compact four-coordinate contact-ion pair (CIP, [Li·2L·H 2 O·TFSI]), whereas Mg 2+ exists as a bulky six-coordinate solvent-separated ion pair (SSIP, [Mg·4L·2H 2 O] 2+ ). This difference considerably amplifies steric sieving. Specifically, the bulky branched chains of TIAP impose a severe conformational energy penalty (97.5 kJ/mol) on the crowded Mg 2+ shell, strongly suppressing Mg 2+ coordination. Consequently, the extraction efficiency of TIAP is comparatively low in pure Li + systems (60.5%) but surges to 83% in high-Mg backgrounds under the synergistic action of steric Mg 2+ rejection and the Hofmeister effect, achieving a superior separation factor of 215.0. Finally, a quantitative dual-parameter model that accurately explains the extraction capacity (TAP > TBP > TIAP) and selectivity (TIAP > TAP > TBP) trends was established. This study provides deep molecular insights into Li + /Mg 2+ separation along with a robust theoretical framework for rational design of selective ligands for complex brines. Download: Download high-res image (94KB) Download: Download full-size image
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Le Shi,Li Ding,Sihua Liu,Haifu Gao,Jingguo She,Jianhua Zhang,Xiaolong Lu,Chunrui Wu
To achieve efficient separation of Li + /Mg 2+ , nanofiltration membranes (NFMs) with intensified positive charge density were fabricated by surface grafting of guanazole (GAZ) on the surface of piperazine (PIP)/trimesoyl chloride (TMC) NFMs. GAZ is rich in amino groups with smaller molecular size, could contact and react more sufficiently with reaction sites on membrane surface, and give less potential blockage of surface pores, compared to traditional surface grafting molecules. The influence of the chargeability and pore size of pristine PIP/TMC NFMs and surface grafting reaction on the structure and performance of GAZ grafted NFMs was investigated. Simulated brine with Mg 2+ /Li + ratio of 150 was utilized to evaluate the feasibility of GAZ grafted NFMs in treating salt-lake brine with high Mg 2+ /Li + ratios. The results showed that the positive charge density on the NFMs surface was improved and the percentage of larger pores was reduced with the successful grafting of GAZ. The optimal GAZ grafted NFMs exhibited higher MgCl 2 rejection (94.2%) than that of PIP/TMC NFMs (64.2%) and maintained a stable pure water permeance. It was worth noting that the Li + /Mg 2+ separation factor for simulated brine of 2000 mg·L -1 (Mg 2+ /Li + ratio of 150) reached 25.7, which was potentially applicable for treating salt-lake brine with high Mg 2+ /Li + ratios.
研究领域:
材料科学
·
环境工程
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产品关联
DOI
高影响因子
Journal of Magnesium and Alloys
·
2025
·
IF 13.8
Fanfan Liu,Xiaomeng Fan,Xinyue Gao,Jinjin Ban,Guoqin Cao,Shilin Zhang,Junhua Hu
Rechargeable Mg/Li hybrid ion batteries with Mg 2+ /Li + double-salt electrolytes and safe Mg anodes are a viable option for large-scale energy storage. Nevertheless, achieving the desired reasonable electrochemical performance remains a great challenge due to the capacity limitations of conventional Li-intercalation cathodes. To mitigate this limitation, the 3D oxygenated MXene Ti 3 C 2 @CoS 2 /FeS 2 (denoted as o-Ti 3 C 2 @CoS 2 , o-Ti 3 C 2 @FeS 2 ) with both dual-storage mechanism and multidimensional structure to achieve the desirable storage capacity is engineered. Benefiting from the formation of special structure and interfacial chemical bonds Ti–O–Co/Ti–O–Fe, as well as the electronegative o-Ti 3 C 2 weaken the Co–S/Fe–S bonds, the o-Ti 3 C 2 @CoS 2 cathode exhibits superior capacity up to 425 mAh g −1 at 100 mA g −1 and overwhelming advantageous ultra-long life over 2,400 cycles at 500 mA g −1 . Simultaneously, the o-Ti 3 C 2 @FeS 2 also displays a high-rate capability, outstanding cycling stability, and fast diffusion kinetics. Furthermore, the conversion reaction of Mg 2+ /Li + co-intercalation and the charge storage mechanism during cycling are thoroughly clarified by systematic ex-situ characterizations and theoretical computations. This study reveals the influence of MXene electrode structure on the importance of electrochemical performance and provides guidance for the future design of high-performance MXene materials for energy storage applications.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 41
·2205998
·
IF 19.924
Yu Ni,Chao Huang,Hong Liu,Yuhao Liang,Li-Zhen Fan
All-solid-state batteries are one of the most promising lithium–ion batteries as they are safe with high energy density and applicable to different occasions. Sulfide solid electrolytes (SSEs) are welcoming due to their good ionic conductivity and processability. However, as the SSE conductor is unstable when exposed to air, its development and application are limited. A series of new Li 3+2x P 1−x Bi x S 4−1.5x O 1.5x (X = 0.02, 0.04, 0.06, 0.08) solid electrolytes are synthesized by co-doping Li 3 PS 4 with Bi and O, and the new electrolytes have better ionic conductivity and air-stability than Li 3 PS 4 . The lithium ionic conductivity of Li 3.12 P 0.94 Bi 0.06 S 3.91 O 0.09 solid electrolytes reached up to 2.8 mS cm –1 at room temperature, the highest and 9 times as high as that of Li 3 PS 4 . The doped solid electrolytes are compatible with lithium anode, and the cycling performance is improved. Importantly, the critical current density of Li 3.12 P 0.94 Bi 0.06 S 3.91 O 0.09 electrolytes can reach to 1.2 mA cm –2 . In particular, the Li|Li 3.12 P 0.94 Bi 0.06 S 3.91 O 0.09 |Li symmetric cells are stable even after 400 h running at 1 mA cm –2 and 25 °C. Bi 2 O 3 doping SSEs are expected to be the next generation of all-solid-state lithium batteries due to their good ionic conductivity and air-stability.
研究领域:
材料科学
·
能源存储与转换
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DOI
高影响因子
Advanced Energy Materials
·
2024
·
IF 24.4
Wenjie Ren,Xinchao Shang,Yan Lin,Hao Ren,Linchen Zhang,Hang Su,Qi Li,Linjie Zhi,Mingbo Wu,Zhongtao Li
Polymer electrolytes-based batteries are suffering great degradation due to the irreversible lithium deposition and increased impedance at sub-zero temperature, which is related with Li + conductivity of bulk electrolyte (σBulk) and ionic conductivity of solid electrolyte interface (σSEI). Thereby, an artificial SEI layer has coated on Li anode through in situ polymerizing polyester with fluorinated porphyrin, which could accelerate Li + desolvation and conductivity of SEI. Then, the dual-salt eutectic polymer electrolyte tolerate is employed to accelerate Li + transfer through optimize their solvation structure. The matching factor is calculated to evaluate the synergistic effect of σBulk and σSEI on low-temperature Li + mobility. Thus, homogenize the Li + flux during Li-plating is achieved by marching the Li + diffusion rate ( δ = 1.92), which significantly mitigate overpotential aggravation and suppress dendrite nucleation. Overall, such marching factor could provide a theoretical parameter for evaluating the low-temperature tolerability of solid-state lithium batteries (SSBs), which would useful for improving batteries’ durability, safety and flexibility.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2023
·Vol. 27
·期 6
·1399-1409
·
IF 2.5
Zhang Ruixin,Xie Binxuan,Rong Junfeng,Liu Lili,Hou Guolin,Chen Shimou
Polymer electrolytes with high safety and high performance are considered to be one of the most promising candidates to upgrade the traditional organic-solvent-based lithium-ion batteries. However, unlimited thermal runaway and incompatibility between electrolyte and electrode greatly limit the development of advanced polymer electrolytes. In this work, we fabricated bilayer polymer electrolytes (DLMs) with a multilevel heterostructure to achieve high-temperature self-shutdown functionality and uniform Li-ion flux. The double-layer heterostructure consists of a self-shutdown layer in contact with the cathode and an ionic liquid composite polymer layer in contact with the anode, which can achieve effective electrode–electrolyte interface contact, fast self-shutdown, and more than 900 h of stable lithium plating/stripping. In addition, the NCM523/DLM/Li battery exhibits a high reversible capacity of 129.7 mAh g −1 at 0.5 C and maintains high-capacity retention (> 89%) after 200 charge–discharge cycles. This study shows a great advantage in handling thermal abuse and a stable lithium anode, suggesting a promising approach to the high-safety lithium metal batteries.
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Zhichen Xue,Xianyue Qi,Luyu Li,Wei li,Lian Xu,Yongqiang Xie,Xiangwan Lai,Guorong Hu,Zhongdong Peng,Yanbing Cao,Ke Du
Overlithiated oxide cathode materials show high capacity but poor cycle stability and voltage attenuation. In this work, a concentration difference driven molten salt ion exchange strategy is used to replace a small quantity of lithium ions by sodium ions. With the entry of sodium ions, the interplanar spacing is increased and the structure is stabilized. The electrochemical properties of materials have been improved obviously. The powder X-ray diffraction, inductively coupled plasma atomic emission spectroscopy, scanning electron microscopy, and transmission electron microscopy are used to detect the entry of sodium ions and structural changes. The modified materials display high discharge specific capacity, excellent cycling performance, and reduced voltage attenuation.
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产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 18
·2213702
·
IF 19
Meng Yao,Qinqin Ruan,Yangyang Wang,Liyu Du,Qiongguang Li,Lv Xu,Ruji Wang,Haitao Zhang
Composite polymer electrolytes (CSEs) that simultaneously possess superior electrochemical performances with robust mechanical properties are highly desired to the application of high-energy lithium metal batteries. Herein, a novel dual-polymer@inorganic network CSE (DNSE@IN) through a sequential nonhydrolytic sol-gel reaction of tetraethoxysilane (TEOS) and the semi-interpenetration of poly(vinylidene fluoride-co-hexafluoropropene)-hexafluoropropylene (P(VDF-HFP)) with poly(ionic liquid) (PIL) is proposed. DNSE@IN, which has a robust dual-polymer@inorganic networks, not only has high ionic conductivity (0.53 mS cm −1 at 20 °C), but also exhibits an outstanding Young's modulus of 723.2 MPa. As a result, the DNSE@IN based Li/LiFePO 4 and Li/Li 1.17 Ni 0.27 Co 0.05 Mn 0.52 O 2 (Li-rich) cells exhibit remarkable cycling stability from room temperature (RT) to 100 °C. As-assembled Li/Li-rich battery shows superior cyclability of 194.3 mAh g −1 after 70 cycles at 4.3 V under RT. Additionally, the scale-up high-voltage Li/Li-rich pouch cells exhibit excellent cyclability (nearly 100% capacity retention after 93 cycles) and superior flexibility, safety at RT for potential practical applications. As such, the work of decoupling ionic conductivity and mechanical properties opens a novel route to develop novel CSEs for the construction of high-energy lithium metal batteries.
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高影响因子
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS
·
2020
·Vol. 235
·期 4
·451-466
·
IF 2.03
Yuli Xue,Yan Zhang,Xiaoling Tan,Wenqing Li,Zhongshu Li,Shaonan Xu,Peng Zhang,Jian Wang,Peiping Zhang,Shiding Miao
It is of importance to reclaim single-salt of potash from Li + -type brines of low concentration. In this work the potassium salts KHCO 3 was efficiently separated from the lithium carbonate-type brines with the aid of CO 2 carbonation. The phase field was provided in which the precipitation of KHCO 3 occurs and single-salt of potassium can be obtained. The low concentration of [Li + ] was also successfully concentrated to a high level (8.1 g/L), and this concentration can be used as sources for Li + -salts production using pre-developed strategies, which looks forward wider applications of the lithium resources of natural brine. This state-of-art was traced via isotherm evaporation on the quaternary system of Li + –K + –CO 3 2− –H 2 O at 298.15 K in which the carbonation steps were performed by CO 2 . Metastable phase diagram was found to consist of three invariant points, seven univariant curves, and four crystallization fields corresponding to Li 2 CO 3 , KHCO 3 , potassium carbonate sesquihydrate (K 2 CO 3 ⋅ 3/2H 2 O), and a potassium carbonate and potassium bicarbonate double salt (K 2 CO 3 ⋅ 2 KHCO 3 ⋅ 1.5H 2 O). There was no crystallization field corresponding to LiHCO 3 . The pH-composition diagram and density-composition diagram were also plotted. This work was carried out in aim of extracting/separating single salts of alkali metals from carbonate-type brines of west China.
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高影响因子
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