JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
·
IF 14.3
Xianzhun Huang,Haojie Liu,Wenyi Xiang,Lihan Chen,Xinran Li,Bangzhuang Xue,Jian Ma,Yueyue Wu,Chengwei Wang,Yinhua Bao,Weiwei Ping
Oxide-based electrolytes are promising with high ion conductivity and a wide electrochemical window (0–5 V). However, the brittleness and poor compressibility severely inhibit their application. Here, inspired by the “flexible eggshell membrane”, we fabricated a 20 µm, flexible and compressible Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 thin film by in-situ healing the LLZTO crystal chips with poly(di(ethylene glycol) ethyl ether acrylate) electrolytes. Fracture mechanics analysis demonstrates the superior mechanical properties of the flexible LLZTO films. With the package pressure increasing from 0.6 to 1.4 t, the Li metal symmetric cell displays a decreasing internal resistance from ∼281 to ∼156 Ω cm 2 , corresponding to the low limit of ion conductivity from ∼0.6 × 10 −4 to ∼2.1 × 10 −4 S/cm. The symmetric cell can be a stable cycle for ∼220 h at 0.4 mA/cm 2 and ∼300 h at 0.1 mA/cm 2 with a bending angle of 30°. The full cell LiFePO 4 /LLZTO/Li shows a superior rate performance of 150 mA/g and a long cycle life of ∼200 cycles. Pairing with the LiNi 0.8 Co 0.1 Mn 0.1 O 2 , the cell displays a Coulombic efficiency of ∼99.7 % for ∼150 cycles. These results indicate that we have successfully fabricated flexible and compressible LLZTO films, and this will open an avenue for the application of high-energy-density thin film batteries.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-14
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IF 15.7
Zou Zhijuan,Liu Pengfei,Dou Ruiyang,Liu Kaijun,Wang Yunlong,Song Lixian,Tong Liping,Yin Guolu,Kang Wenbin,Cai Wenlong,Zhang Yaping,Chen Hongbing,Song Yingze
Binders are essential for maintaining positive electrode integrity in Li||S batteries and significantly affect their performance. However, commercial linear binders often have disordered networks, poor binding efficiency, and insufficient mechanical strength. To address these challenges, three-dimensional covalent binders offer a promising solution. Traditional methods for producing cross-linked binders require additives and result in poorly controlled polymer networks due to the stochastic nature of liquid-phase polymerization. Moreover, the mechanisms by which reticulated binders stabilize the positive electrode remain unclear, requiring investigation under operando conditions. Herein, we present an approach to tailor cross-linked polyacrylamide networks using solid-state operando γ-ray irradiation chemistry, which eliminates additives and produces a pure, ordered network with remarkable binding capabilities. By integrating in situ high-resolution optical frequency domain reflectometry, multiscale synchrotron radiation characterization, and virtual simulations, this study reveals the role of binders in dynamically encaging and confining sulfur. Specifically, γ-ray-enabled polyacrylamide networks enhance battery performance through mechanical strengthening, optimized sulfur regeneration, and improved re-occupancy. Consequently, the well-designed composite positive electrode structure with only 5.0 wt% binder improves soft-packaged Li||S battery performance across various scenarios. Notably, a 1.2-Ah pouch cell achieves 410.1 Wh kg −1 specific energy with a low electrolyte/sulfur ratio of 3.0 µL mg –1 .
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Functional Materials Letters
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2025
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IF 1.1
Hanchen Xu,Zhiyong Yu,Lujia Tian,Suni Du,Yichun Zhao,Jingsai Cheng,Hanxing Liu,Zhongzhi Yuan
Copper fluoride (CuF 2 ) has demonstrated great potential as a cathode material for LIBs owing to its high energy density. In this study, a two-step synthesis method was proposed to prepare porous CuF 2 by using Cu-based metal-organic frameworks (MOFs). N 2 adsorption-desorption isotherms, along with SEM and TEM analyses, proved that the intermediates CuO exerted a certain influence on the pore structure of the final CuF 2 products. The porous CuF 2 achieved a first discharge capacity of 554 mAh ⋅ g − 1 at 0.1C. At a high current density of 5C, it delivered a rate capacity of 413 mAh ⋅ g − 1 within 1.5–4.2 V. The results of electrochemical impedance spectroscopy show that varying degrees of porosity influence the lithium-ion diffusion coefficient, leading to differences in electrochemical performances.
研究领域:
材料科学
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电化学
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储能
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
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IF 16.6
Xie Yuxiang,Huang Yixin,Zhang Yinggan,Wu Tairui,Liu Shishi,Sun Miaolan,Lee Bruce,Lin Zhen,Chen Hui,Dai Peng,Huang Zheng,Yang Jian,Shi Chenguang,Wu Deyin,Huang Ling,Hua Yingjie,Wang Chongtai,Sun Shigang
The Li metal is an ideal anode material owing to its high theoretical specific capacity and low electrode potential. However, its high reactivity and dendritic growth in carbonate-based electrolytes limit its application. To address these issues, we propose a novel surface modification technique using heptafluorobutyric acid. In-situ spontaneous reaction between Li and the organic acid generates a lithiophilic interface of lithium heptafluorobutyrate for dendrite-free uniform Li deposition, which significantly improves the cycle stability (Li/Li symmetric cells >1200 h at 1.0 mA cm −2 ) and Coulombic efficiency (>99.3%) in conventional carbonate-based electrolytes. This lithiophilic interface also enables full batteries to achieve 83.2% capacity retention over 300 cycles under realistic testing condition. Lithium heptafluorobutyrate interface acts as an electrical bridge for uniform lithium-ion flux between Li anode and plating Li, which minimizes the occurrence of tortuous lithium dendrites and lowers interface impedance.
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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JOURNAL OF POWER SOURCES
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2022
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IF 9.794
Yi-Xuan Li,Xiang Ding,Fei Chen,Kuo Cao,Chun-Hua Chen
NaClO 4 is utilized as a salt-type electrolyte additive to improve the electrochemical performance in both Li-rich/graphite full cells and Li-rich/Li half cells. The corresponding characterizations such as scanning electron microscopy and X-ray photoelectron spectroscopy reveal that the NaClO 4 -added electrolyte can suppress the transition metal dissolution from Li-rich cathode and form a stable conductive cathode electrolyte interface layer to protect Li-rich cathode and promote Li + ions transfer. A small amount (0.1 wt%) of NaClO 4 additive enables Li-rich/graphite full cells to maintain 86% capacity after 50 cycles and Li-rich/Li half cells to maintain 95% capacity after 100 cycles, showing a great application potential.
研究领域:
电化学
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材料科学
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能源存储
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电池技术
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功能材料
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Cai Qi,Shu Zu,Xukun Zhu,Tong Zhang,Longyan Li,Li Song,Yachao Jin,Mingdao Zhang
Functional and active carbon material is of great concern in facilitating the performance of lithium-sulfur (Li-S) battery . In this work, we develop a bamboo-like nitrogen-doped carbon nanotubes (Co@NCNTs-2) with low cobalt metal content, which acts as not only the host matrix for sulfur loading but also an efficient catalyst for the adsorption and conversion of lithium polysulfides (LiPSs). The characterization results show that the Co particles are mainly encapsulated inside the Co@NCNTs-2, and the N species are mainly distributed on the outer surface of Co@NCNTs-2. The Co particles are the growth sites of carbon nanotubes and are wrapped by carbon to form Co@NCNTs-2. It is confirmed that the uniform graphitized structure contributes to charge transfer, while the enriched N species assist the trap and catalytic conversion of the polysulfides, thus helping to restrain the shuttle effect. As a result, the resultant Co@NCNTs-2-S cathode presents high reversible capacity at different current densities and exhibits superior cycling stability for 300 cycles at 0.5 C.
研究领域:
材料科学
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能源存储技术
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ACS Applied Materials & Interfaces
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2021
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IF 9.229
Zhao Jiang,Zhongxu Li,Xiuli Wang,Changdong Gu,Xinhui Xia,Jiangping Tu
All-solid-state lithium-metal batteries (ASSLMBs) with sulfide electrolytes have attracted attention owing to their superior safety and high energy density. However, interfacial instability of sulfide electrolytes against Li metal still hinders their applications. Herein, F-doping is adopted to optimize the structure of Li10SnP2S12. It is demonstrated that the Li9.95SnP2S11.95F0.05 (LSPSF) electrolyte exhibits a high ionic conductivity of 6.4 mS cm–1 because of F-doping, which can reduce the impurity Li2SnS3 and generate Li+ vacancies. In addition, the Li6PS5I (LPSI) glass–ceramic interlayer is employed to enhance the interfacial stability between the sulfide electrolyte and Li metal by restraining the reduction of Sn4+ cations, as indicated by X-ray photoelectron spectroscopy (XPS). As a result, the assembled ASSLMBs with the LPSI interlayer deliver high initial discharge capacity and remarkable cycling stability. This work provides a new design route for manufacturing high-performance ASSLMBs.
研究领域:
材料科学
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电化学
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JOURNAL OF NON-CRYSTALLINE SOLIDS
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2026
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IF 3.6
Beibei Pan,Yuanhao Ma,Jiawei Zhao,Caiyan Chen,Shuaishuai Liu,Yang Shen,Qiuju Zheng,Yuebo Hu
Li 0.5 La 0.5 TiO 3 (LLTO) is a promising solid-state electrolyte material due to its excellent chemical stability, wide electrochemical window, and relatively high ionic conductivity. This work aims to further improve the ionic conductivity of LLTO via modification with borophosphate glasses containing lithium halides. The underlying rationale is that the unique mixed network structure of borophosphate glass can provide additional pathways for lithium ion (Li + ) transport. Furthermore, the incorporation of halogenated borosilicate glass (especially LiI) is expected not only to supply extra Li + , but also to improve the solid electrolyte interface by filling the voids among LLTO pellets, thus enhancing the overall electrochemical performance. The results demonstrate that the sample with 2 wt.% Li 2 O-B 2 O 3 -P 2 O 5 -LiI (LBPI) glass achieves a favorable room temperature ionic conductivity of 1.03 × 10 –3 S·cm –1 , which is approximately double that of the pristine LLTO. Our findings confirm the synergistic modification effect of borophosphate glass and lithium halides in improving Li + transport and present a strategic approach for developing advanced solid-state electrolytes with satisfactory electrochemical performance.
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CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Yingchao Wang,Zhen Wang,Qiyang Lu,Qingxian Miao,Yonghao Ni,Liulian Huang,Lihui Chen,Zhiwei Lin,Yuxin Liu,Jianguo Li
Charged cellulose in nonwoven leads to nano-sized pores and high charged density of CNW. • Donnan exclusion and Debye-length-related electrostatic regulation facilitate Li+ transport and suppress Mg2+ in CNW. • CNW in FO delivers Li + permeation of 920 g·h −1 ·m −2 with Li + /Mg 2+ selectivity of 3.24. • CNW remains stable at wide pH, high salinity, and long-term operation. With the rapid growth of the lithium battery industry, global lithium demand continues to increase, making efficient and selective lithium extraction from salt lake brines increasingly important. In this context, the performance of ion-selective separation membranes is crucial, with surface charge and porous transport structure being widely recognized as key factors influencing separation efficiency. Herein, this study develops a scalable charged cellulose-inserted nonwoven composite membrane (CNW) by embedding charged cellulose molecules into a nonwoven fabric through a simple vacuum-assisted impregnation process. The CNW possesses interconnected porous transport pathways (porosity of 66%) and a negatively charged interface (zeta potential of −49 mV), which support the selective ion transport through the synergistic effects of Donnan exclusion and Debye-length-related electrostatic regulation. Under the optimal conditions, the permeation rates of Li + and Mg 2+ reach 920 and 284 g·h −1 ·m −2 , respectively, while the Li + /Mg 2+ selectivity of 3.24, approximately 3 times higher than that of the original cellulose membrane, under osmotically driven FO operation. Moreover, the membrane maintains stable separation performance and structural integrity during long-term operation. These findings demonstrate that the synergistic regulation of charged interfaces and porous transport pathways provides a promising strategy for scalable and sustainable lithium extraction from salt-lake brines. Download: Download high-res image (187KB) Download: Download full-size image
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ACS Omega
·
2023
·
IF 4.1
Zhixin Wang,Zhipeng Cai,Meinan Liu,Fuliang Xu,Fangmin Ye
High-potential lithium metal batteries (LMBs) are still facing many challenges, such as the growth of lithium (Li) dendrites and resultant safety hazards, low-rate capabilities, etc. To this end, electrolyte engineering is believed to be a feasible strategy and interests many researchers. In this work, a novel gel polymer electrolyte membrane, which is composed of polyethyleneimine (PEI)/poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) cross-linked membrane and electrolyte (PPCM GPE), is prepared successfully. Due to the fact that the amine groups on PEI molecular chains can provide the rich anion receptors and strongly pin the anions of electrolytes and thus confine the movement of anions, our designed PPCM GPE owns a high Li+ transference number (0.70) and finally contributes to the uniform Li+ deposition and inhibits the growth of Li dendrites. In addition, the cells with PPCM GPE as a separator behave the impressive electrochemical performances, i.e., a low overpotential and an ultralong and stable cycling performance in Li∥Li cells, a low overvoltage of about 34 mV after a stable cycling for 400 h even at a high current density of 5 mA/cm2, and, in Li∥LFP full batteries, a specific capacity of 78 mAh/g after 250 cycles at a 5 C rate. These excellent results suggest a potential application of our PPCM GPE in developing high-energy-density LMBs.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Mingran Zhou,Wenda Dong,Ao Xu,Zhiwen Yin,Zhi-Yi Hu,Xinling Wang,Liang Wu,Lihua Chen,Yu Li,Bao-Lian Su
Lithium-selenium batteries (LSeBs) have attracted increasing attention due to their excellent electronic conductivity and high theoretical specific capacity. However, there are still difficult problems such as low utilization rate and fast capacity decay in the actual application process. Herein, a surface iodine modified three-dimensional (3D) nano hollow carbon fiber (I-NHCF) network is designed and synthesized as Se host (Se@I-NHCF) for highly stable LSeBs. The surface iodine species induce the formation of robust cathode electrolyte interface (CEI), thus preventing the transformation of amorphous selenium to low-activity crystalline selenium and enabling stable electrochemical performance. Moreover, the surface iodine species promote rapid charge transfer, enhancing the chemical reaction kinetics and improving the utilization of the active Se species. As a result, the Se@I-NHCF cathode exhibits superior specific capacity of 581.8 mAh g −1 with a high stability (0.0054% capacity decay per cycle) after 500 cycles at 1C, and an excellent rate performance of 567.6 mAh g −1 at 2C. This work addresses the problem of rapid capacity decay by the formation of uniform and robust CEI to conserve highly reactive amorphous Se species, improve Se utilization, and achieve ultra-stable Li-Se batteries with high energy and long cycle life.
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Materials
·
2023
·Vol. 16
·期 16
·5511
·
IF 3.4
Anyu Yue,Yong Cao,Yi Zhang,Shenggang Zhou
The Mg-Li alloy stands as the lightest metallic structural material known to date, finding a wide range of applications. However, its development has been hindered by its susceptibility to oxidation and corrosion. In this study, we aimed to address this issue by employing electroless deposition to form a protective zinc layer on the surface of a magnesium–lithium alloy. The optimization of the zinc layer was achieved through varying parameters such as the zinc dipping time (1~10 min), temperature (20~70 °C), and zinc content (20~200 g/L). Surface characterization was performed using scanning electron microscopy (SEM) and X-ray diffraction, while electrochemical tests and scratch tests were conducted to evaluate corrosion resistance and coating adhesion. The results demonstrated the successful formation of a uniform and dense pure zinc layer on the surface of the Mg-Li alloy when the zinc-dipping time was set at 5 min, the temperature was at 30 °C, and the zinc content was at 50 g/L. Under these conditions, the corrosion potential of the Mg-Li alloy experienced the greatest positive shift, reaching as high as −1.38 V. Additionally, the corrosion current was minimized, measuring at 2.78 × 10−6A/cm2. Furthermore, the maximum arc tolerance radius was observed. Consequently, the electroless deposition of zinc onto Mg-Li alloys significantly improves their corrosion resistance and bonding, opening up new prospects for the application of zinc-plated Mg-Li alloys.Keywords:Mg-Li alloy;electroless-deposited;zinc coating;corrosion resistance
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