ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Lin Lin,Wei Han,Guang Li,Jingjing Zhang
The widespread adoption of composite solid electrolytes (CSEs) in solid-state lithium metal batteries has been significantly impeded by insufficient room-temperature ionic conductivity, primarily due to high energy barriers for Li-ion transport across ceramic/polymer interfaces. While interfacial modification has emerged as a key strategy, the structural and mechanistic principles governing efficient ion transport remain poorly understood. Here, we address this challenge through an innovative interface engineering approach, constructing a molecular bridge between Li7La3Zr2O12 nanofibers (LLZO NFs) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) using a 3-(methacryloyloxy)propyltrimethoxysilane (MPS) linker. This design achieves multiple synergistic effects: (1) robust chemical bonding enables uniform dispersion of ceramic nanofibers even at high loadings (60 wt %); (2) polar MPS moieties effectively adsorb and reorganize solvated species at the ceramic/polymer interface; and (3) optimized Li+ coordination via dual bonding configurations (Li···O═C with MPS and Li···F–C with PVDF-HFP) drastically reduces the interfacial energy barrier (−0.456 eV), creating continuous ion transport highways across the interface. Systematic investigation of the linker’s structure–property relationship reveals key design principles for interfacial chemistry. The resulting composite electrolyte (CLPH–OH) with 60 wt % of functionalized LLZO NFs delivers an exceptional ionic conductivity of 8.3 × 10–4 S cm–1 at room temperature. Remarkably, Li//CLPH–OH//Li symmetric cells achieve stable cycling for 2000 h at 0.1 mA cm–2, and LiFePO4 full cells retain 93.6% capacity after 300 cycles at 0.5 C. This study provides both fundamental insights into interfacial ion transport mechanisms and a strategy for designing high-performance solid-state electrolytes through precise molecular-level interface engineering.
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高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
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
·
2025
·Vol. 16
·期 1
·1-14
·
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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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yushuang Lin,Nan Li,Weihao Xue,Hong Chen,Zhiruo Zhang,Zhao Dai
Achieving precise pore size tuning in nanofiltration membranes for Mg 2+ /Li + separation remains challenging due to the similar hydrated radii of the ions and the lack of real-time monitoring for dynamic adjustments. In this study, we developed a novel pH-responsive color-changing nanofiltration membrane with tunable pore sizes, enabling real-time monitoring and enhanced separation efficiency. By incorporating γ-cyclodextrin during interfacial polymerization, we achieved angstrom-level pore size tuning and reduced pH sensitivity. The color response of the membrane enables dynamic adjustments to the feed solution pH, optimizing pore radii to ∼0.41 nm, leading to a separation factor of 35.5. Molecular dynamics simulations and weight cut-off experiments confirmed that γ-cyclodextrin enhanced pore uniformity, resulting in a denser, more efficient membrane. This innovative approach offers a flexible and precise solution for Mg 2+ /Li + separation, demonstrating high permeance (15.5 L m −2 h −1 bar −1 ) and potential for applications in seawater desalination, resource recovery, and industrial ion separation.
研究领域:
膜科学
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分离技术
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材料科学
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化学工程
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环境科学
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Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 41
·35727-35735
·
IF 9.5
Xiaoyu Wang,Ben Ma,Xuehui Shangguan,Qinglei Wang,Ping Li,Li Su,Yi Zhao,Yufei Wei,Haixin Zhang,Jie Gao,Faqiang Li
Lithium–aluminum layered double hydroxides (Li/Al-LDHs) have achieved successful industrial-scale application in lithium extraction from salt lakes due to their excellent structural stability, high selectivity and environmental friendliness. However, they suffer from limited adsorption capacity. Herein, this issue can be effectively resolved by precise regulation of the LDH nucleation strategy, thereby controlling oxygen species content. The Li/Al-LDHs are synthesized via a one-pot precipitation method, and the nucleation conditions, including Al/Li ratio, crystallization temperature and terminal pH, are systematically optimized through crystal growth analysis, adsorption performance evaluation, and structural stability characterization. The results confirm that the adsorption capacity of Li/Al-LDHs is critically dependent on the pH value attained at equilibrium. Notably, the terminal pH simultaneously governs Al(OH)3 nucleation and Li+ intercalation through oxygen speciation control. The elevated active oxygen content (38.65%) enhances hydrophilicity (contact angle 22.5°) and strengthens lithium-ion diffusion kinetics. The density functional theory (DFT) calculation further indicates that high levels of active oxygen (37.5%) facilitate low formation energy (−3.527 eV) and adsorption energies (−0.739 eV), confirming the correlation between the structure and Li active sites. What's more, the prepared Li/Al-LDHs show outstanding lithium adsorption performance with a maximum adsorption capacity of 13.42 mg g−1 in East Taijinar salt-lake brine. The separation coefficients of Na+, K+, and Mg2+ are 395.86, 140.89, and 121.69, respectively. This study provides vital insights for advancing high-performance aluminum-based lithium adsorbents.
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MATERIALS LETTERS
·
2025
·
IF 2.7
Caili He,Jinying Guo,Zhen Guo,Mengqi Ding,Hao Tang,Renjie Wang,Meifang Zhang
Layered oxide LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) is one of the promising cathode materials for high energy lithium ion batteries , which offering enhanced energy density and battery capacity. However, as the reaction progresses, a series of adverse effects arises. In this paper, the dual-additive electrolyte synergistic effect are ingeniously introduced to the traditional electrolyte LiPF 6 to form a low impedance and stable cathode electrolyte interface on the cathode surface. The specific discharge capacity of the battery at 5C was 154 mAh g −1 , while of the base electrolyte was only 106 mAh g −1 . The battery demonstrated over 82 % capacity retention after 200 cycles at 1C, while the base electrolyte was only 62 %.
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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锂离子电池
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电极界面
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电解液工程
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Chen Zheng,Liu Peng,Cao Yu-Long,Xie Yu-Long
The manganese-based ion sieve H 1.6 Mn 1.6 O 4 shows significant advantages in lithium adsorption. Its prominent features include high adsorption capacity and low pollution characteristics of the preparation process. These combined advantages make this material important in the lithium extraction technology in salt lakes. However, problems such as high manganese dissolution loss rate, poor cyclic stability, and difficulty in powder recycling seriously restrict the industrialized application. In this paper, we propose to optimize the structure of spinel-type manganese lithium ion-sieves with a 2% Co 3+ doping strategy, which can effectively inhibit the lattice collapse triggered by Jahn–Teller aberration during the pickling cycle by replacing part of the Mn 3+ active sites with Co 3+ . After doping, the relative Mn 4+ content on the surface of the material increased from 58%–61% according to the XPS test, confirming that the introduction of Co 3+ facilitated the transition of Mn 3+ to the higher valence state Mn 4+ through the charge compensation effect. Reducing the disproportionation activity of Mn 3+ reduces the dissolution loss of Mn 2+ during the pickling process. The experimental results showed that the adsorption of doped HMCO-2 material increased from 28.8–34.9 mg/g. The adsorption capacity retention rate was 77% after five cycles, there was a high selective adsorption of Li + , and the manganese dissolving loss rate was decreased to 2.3%.
研究领域:
材料科学
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化学工程
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环境科学
·
无机化学
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高影响因子
Joule
·
2023
·
IF 39.8
Yatao Liu,Linhan Xu,Yongquan Yu,MengXue He,Han Zhang,Yanqun Tang,Feng Xiong,Song Gao,Aijun Li,Jianhui Wang,Shenzhen Xu,Doron Aurbach,Ruqiang Zou,Quanquan Pang
The transition from dissolution-precipitation to quasi-solid-state sulfur reaction promises restricted polysulfide shuttle and lean electrolyte operation of Li-S batteries but incurs poor reaction kinetics. We here demonstrate that structural reorganization of sparingly solvating electrolytes (SSEs)—which is uniquely afforded by using low-density and low-cost aromatic anti-solvents—is vital for taming the quasi-solid-state sulfur reaction. Aromatic anti-solvents disrupt the interconnected structure of concentrated tetrahydrofuran (THF) electrolyte, uniquely creating subdomains that act to dissolve elemental sulfur, thus accelerating its consumption and re-formation while maintaining ultralow polysulfides solubility. The altered subdomains further result in robust solid electrolyte interphase (SEI) on lithium metal. As a result, the Li-S cell with a 3 mg sulfur cm −2 sulfur cathode can cycle steadily for ∼160 cycles with a lean electrolyte of 5 μL mg sulfur −1 . Our work provides new insights into fine-tuning the electrolyte microstructure through solvent innovations for developing sulfur-based batteries that are high energy, cheap, and durable.
研究领域:
材料科学
·
电化学
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NATURE
·
2025
·Vol. 637
·期 8047
·846-853
·
IF 48.5
Song Huimin,Münch Konrad,Liu Xu,Shen Kaier,Zhang Ruizhuo,Weintraut Timo,Yusim Yuriy,Jiang Dequan,Hong Xufeng,Meng Jiashen,Liu Yatao,He Mengxue,Li Yitao,Henkel Philip,Brezesinski Torsten,Janek Jürgen,Pang Quanquan
With promises for high specific energy, high safety and low cost, the all-solid-state lithium–sulfur battery (ASSLSB) is ideal for next-generation energy storage 1 , 2 , 3 , 4 , 5 . However, the poor rate performance and short cycle life caused by the sluggish solid–solid sulfur redox reaction (SSSRR) at the three-phase boundaries remain to be solved. Here we demonstrate a fast SSSRR enabled by lithium thioborophosphate iodide (LBPSI) glass-phase solid electrolytes (GSEs). On the basis of the reversible redox between I − and I 2 /I 3 − , the solid electrolyte (SE)—as well as serving as a superionic conductor—functions as a surficial redox mediator that facilitates the sluggish reactions at the solid–solid two-phase boundaries, thereby substantially increasing the density of active sites. Through this mechanism, the ASSLSB exhibits ultrafast charging capability, showing a high specific capacity of 1,497 mAh g −1 sulfur on charging at 2C (30 °C), while still maintaining 784 mAh g −1 sulfur at 20C. Notably, a specific capacity of 432 mAh g −1 sulfur is achieved on charging at an extreme rate of 150C at 60 °C. Furthermore, the cell demonstrates superior cycling stability over 25,000 cycles with 80.2% capacity retention at 5C (25 °C). We expect that our work on redox-mediated SSSRR will pave the way for developing advanced ASSLSBs that are high energy and safe.
研究领域:
材料科学
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电化学
·
能源存储
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高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Tiancheng Na,Yang Liu,Xiangcun Li,Wenji Zheng,Yan Dai,Zhijun Yan,Wei Kou,Gaohong He
We report a method based on 2,4-dihydroxybenzoic acid-formaldehyde (RF-COOH) microsphere hard templates to prepare core-shelled Fe 2 O 3 microspheres , which were then added to graphene oxide to obtain hierarchical reduced graphene oxide, ultimately dropping Fe 2 O 3 (Fe 2 O 3 @rGO) by Vitamin C reduction and freeze drying. When used as cathode materials for lithium-sulfur batteries, Fe 2 O 3 @rGO shows a high specific capacity of 400.5 mAh g −1 at 2 C after 500 cycles. The prominent performance is due to the collaborative assembly of rGO , which provides stable structural support and favourable conductivity, and core-shelled Fe 2 O 3 microspheres, which are certified to have a strong interaction with polysulfides. The loose and stable skeletons of highly electroconductive rGO can offer a conductive framework for rapid ion/electron transport. Meanwhile, the unique core-shelled structure of Fe 2 O 3 with the ample void space can anchor polysulfides through the strong chemical adsorption and buffer the mechanical stresses caused by volume expansion during the charge and discharge processes. Moreover, Fe 2 O 3 promotes the transformation of polysulfides to insoluble LiPSs during the discharging process, effectively alleviating the shuttling of the polysulfides.
研究领域:
材料科学
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能源存储
·
电化学
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高影响因子
DESALINATION
·
2026
·
IF 9.9
Chun-Xu Zhang,Yan-Yan Chen,Ren-Jie Fan,Yu-Xuan Sun,Xiaohu Wang,Fujun Xiong,Yong Wang,Mei-Ling Liu,Shi-Peng Sun,Weihong Xing
Electric field-assisted nanofiltration (ENF) has emerged as a promising technology for Mg 2+ /Li + separation from salt lake brines. However, integrating ENF process with widely used negatively charged membranes induces a non-uniform distribution of reconstructed positive charge. This leads to reduced separation efficiency under high feed concentrations due to charge shielding effects. To overcome this limitation, we developed a strategy employing a positively charged nanofiltration (NF) membrane under an applied electric field. This configuration facilitates both the dehydration of hydrated Li + and a more uniform distribution of positive charges on the membrane surface. The optimized system demonstrated a remarkable separation performance, achieving nearly 100% rejection of Mg 2+ and − 176% rejection of Li + . The separation factor ( S Li, Mg ) represents a 162-fold improvement over the system without an electric field. The ENF process successfully separated Mg 2+ and Li + even in real Yiliping salt lake brine. Furthermore, the permeate stream containing high-purity Li + enabled the production of battery-grade Li₂CO₃ with 99.9% purity. This study demonstrates a pragmatic and efficient approach for Mg 2+ /Li + separation, showcasing considerable promise for high-purity Li + extraction from salt lakes.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 12
·3112-3118
·
IF 5.16
Zhipeng Lin,Hao Zhang,Guofeng Liang,Yanqi Jin,Hongbin Zeng,Jiawang Li,Jian Chen,Weihong Zhang,Fangyan Xie,Yanshuo Jin,Hui Meng
Graphical Composite nanostructured cathode : FeOOH nanocubes with a core–shell structure and anchored on carbon ribbons have been prepared. The carbon ribbons improve the conductivity of the system and make more of the FeOOH surface available for electrochemical reaction. An Li/O 2 battery with FeOOH as the cathode material shows a specific capacity of 14816 mAh g −1 cathode and a long-term stability of 67 cycles over 400 h (see figure). A composite of FeOOH nanocubes anchored on carbon ribbons has been synthesized and used as a cathode material for Li/O 2 batteries. Fe 2+ ion-exchanged resin serves as a precursor for both FeOOH nanocubes and carbon ribbons, which are formed simultaneously. The as-prepared FeOOH cubes are proposed to have a core–shell structure, with FeOOH as the shell and Prussian blue as the core, based on information from XPS, TEM, and EDS mapping. As a cathode material for Li/O 2 batteries, FeOOH delivers a specific capacity of 14816 mA h g −1 cathode with a cycling stability of 67 cycles over 400 h. The high performance is related to the low overpotential of the oxygen reduction/evolution reaction on FeOOH. The cube structure, the supporting carbon ribbons, and the -OOH moieties all contribute to the low overpotential. The discharge product Li 2 O 2 can be efficiently decomposed in the FeOOH cathode after a charging process, leading to higher cycling stability. Its high activity and stability make FeOOH a good candidate for use in non-aqueous Li/O 2 batteries.
研究领域:
材料科学
·
能源存储与转换
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高影响因子
危险品化学品经营许可证（带存储）