COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Xianyu Liu,Jing Li,Yingchun Xiao,Xiangcheng Dong,Lei Tao,Zhiyuan Liu,Zheng Liu,Jia Zhang,Shengjie Xu
The Li metal anode is regarded as the most potential electrode material in the next-generation energy storage system, because of the high energy density and specific capacity. However, the advancement of Li metal anode is restricted by the volume changing and dendrite growth. In this paper, the Co and Zn co-doped porous carbon framework (CF-CZ) derived from MOF structure was designed and produced to realize the dendrite-free Li metal anode. The porous structure could accommodate the deposited Li metal, which relaxes the pressure of electrode structure and relieves the volume changes. Meanwhile, the Co, Zn co-doping effectively improves the lithiophilicity of framework, which attracts Li + and decreases the nucleation barrier. Besides, numerous micropores of MOF structure could divide the Li + flux to reduce the local current density for dense sedimentation. With the synergies of co-doping and porous structure, the symmetric cell of CF-CZ shows better electrochemical performance (the overvoltage can be stable at 14 mV after 1200 cycles) than pure Cu foil, and the LFP cells deliver 116.4 mAh g −1 at 1 C after 200 cycles. As a consequence, the CF-CZ possesses the potential to be applied in Li metal anodes.
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ENERGY & FUELS
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2024
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IF 5.2
Aonan Wang,Yiming Guo,Fanghua Ning,Xiaoyu Liu,Fujun Li,Jiujun Zhang,Shigang Lu,Jin Yi
The lithium carbon dioxide (Li-CO2) battery is regarded as an attractive electrochemical energy storage system on account of its high energy density (∼1876 Wh kg–1) and utilization of “greenhouse gas” CO2. The main discharge product lithium carbonate (Li2CO3) is decomposed along with the inevitable formation of superoxide radicals (O2•–), and it results in irreversible side reactions, such as the deterioration of electrolytes and oxidation of the carbon cathode, which lead to unfavorable cycle life. Herein, sodium lignosulfonate (LSS) is introduced as a radical capture agent to reduce the reactivity of generated O2•– in the Li-CO2 battery. Combined with the results of adsorption energy calculation, it is found that O2•– can be preferentially adsorbed with LSS. It favors suppression of the side reactions between O2•– and the carbon cathode/electrolyte during charge. The discharge/charge voltage gap of the Li-CO2 battery is significantly reduced by 0.23 V with a long lifespan of over 200 cycles. This investigation demonstrates that the reactivity manipulation of the O2•– is essential to construct a stable and efficient Li-CO2 battery.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Cai-Yun Zhang,Chen-Yang Wang,En-Zhu Zhao,Guowei Yu,Hui-Ling Deng,Rui Huang,Zhao-Yun Wang,Pu Hu,Min Yan,Zhitian Liu
Lithium‑sulfur batteries demonstrate substantial promises for evolving into next-generation energy storage systems, but sluggish kinetics of LiPSs conversion and poor interfacial stability at the cathode-electrolyte interface remain critical challenges. Biowaste carbon as hosts is a cost-effective strategy to improve the electrical conductivity of Li-S batteries. However, limited polar sites in raw biowaste carbon restrict the capacity to anchor LiPSs. Herein, we propose a bio-derived hybrid host (PANI@GC) synthesized from waste grapefruit peels and polyaniline to address the rate-determining steps in sulfur electrochemistry. The grapefruit-derived carbon establishes an excellent conductive network that enables rapid electron transfer, while the PANI-integrated numerous polar sites (aromatic amine groups, conjugated π-π stacking) create a catalytically active interface to anchor and accelerate LiPSs conversion kinetics. Due to the conductive-catalytic network, the PANI@GC/S cathode delivers exceptional performance of 1190 mAh g −1 at 0.2C and maintains 779.8 mAh g −1 under stringent conditions (5 mg cm −2 sulfur loading, 8 μL mg −1 E/S ratio). Remarkably, the catalytic interface minimizes capacity fading, exhibiting only 28.9 mAh g −1 loss after 7-day rest, compared to Pure S (152.83 mAh g −1 ). This research pioneers a sustainable strategy to engineer conductive-catalytic networks at cathode-electrolyte interfaces, providing fundamental insights into biowaste utilization for high-energy-density battery systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yinghong Wang,Ping Xiong,Wei Yang,Zhitong Zhang,Xiaoling Xu,Liming Yang,Huiji Xiao,Kai Zhang,Zhenzhou Wang,Wei Zhang,Xubiao Luo
Highly selective Mg 2+ /Li + separation membranes hold significant application prospects in extraction of lithium. However, the high Mg 2+ /Li + concentration ratio commonly found in brines and the very close hydrated ionic radii of the two ions limit the separation efficiency of conventional membranes. This study proposes a dual-phase supramolecular synergistic sieving nanofiltration membrane design strategy. Leveraging the unique molecular recognition unit and hydrophilic external interface characteristics of γ -cyclodextrin ( γ -CD), combined with the multifunctional positively charged groups of histidine, the strategy achieves the directional construction of highly efficient Mg 2+ /Li + sieving channels within the membrane. The strategy is accomplished through the synergistic action of γ -CD’s selective capture of high-valent Mg 2 + and histidine’s electrostatic repulsion effect. During the Mg 2 + /Li + separation process, the fabricated γ -CD-histidine composite membrane (HCF membrane) demonstrates outstanding comprehensive performance. It achieves a remarkably high Li + /Mg 2+ separation factor of 28.98 and maintains excellent separation performance across a wide Mg 2+ /Li + ratio range (1:1–100:1). The enhanced hydrophilicity of the HCF membrane significantly boosts permeate flux, while also exhibiting long-term operational stability and biofouling resistance during continuous operation under high Mg 2+ /Li + ratios. This research enables the high-selectivity separation of Mg 2+ and Li + with concurrent Li + enrichment, demonstrating significant potential for lithium extraction from salt-lake.
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ACS Nano
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2025
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IF 16
Yuying Qin,Jing Gao,Junze Lu,Yafei Li,Danni Du,Zhiwei Zhang,Chengxiang Wang,Jiafeng Li,Peng Xiao,Longwei Yin,Rutao Wang
Lithium-rich disordered rock-salt (DRS) materials exhibit potential for fast-charging Li-ion batteries and capacitors, primarily arising from their pseudocapacitive Li+ charge-storage behavior in a low-potential region (<1.0 V versus Li/Li+). This behavior originates from a three-dimensional (3D) Li+-percolation diffusion network, a mechanism defined as percolation pseudocapacitance. However, the relationship between the structural characteristics and pseudocapacitive behaviors remains unclear. Here, we design a series of DRS-Li3V2O5 with different degrees of crystallinity through adjusting the crystallization of V2O5 precursors. We show that DRS-Li3V2O5 with a lower degree of crystallinity exhibits quasi-rectangular cyclic voltammetry (CV) curves and sloped galvanostatic charge/discharge (GCD) profiles, characteristic of surface redox pseudocapacitance. On the contrary, DRS-Li3V2O5 with a higher degree of crystallinity shows a couple of redox peaks with a small voltage offset observed in CV curves and approximately plateau-like GCD profiles, which are characteristic of intercalation pseudocapacitance. Besides, a lower degree of crystallinity leads to a higher specific capacity at a low rate but a poorer rate capability at a high rate, whereas a higher degree of crystallinity leads to a higher pseudocapacitive contribution and a longer cycling lifespan. We propose that a higher degree of crystallinity can promote the formation of a more integrated percolation network on DRS electrodes, which provides faster 3D Li+ transport pathways.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Fei Zhou,Jiangmin Jiang,Gaoyu Zhou,Lingbang Qiu,Wenxuan Fu,Chencheng Xu,Yanhua Cui,Quanchao Zhuang
Lithium/fluorinated carbon (Li/CF x ) batteries have garnered substantial interest from researchers due to their superior energy density and low self-discharge characteristics. However, the strong covalent C F bond in the CF x cathode limits its discharge kinetics, affecting the actual power density and operating voltage. In this work, N -methylpyrrolidone (NMP) with high donor number has proposed as the main solvent of the electrolyte to facilitate the breaking of the C F bond through a bimolecular nucleophilic substitution (S N 2) reaction. This strategy effectively reduces the energy barrier for Li + embedding and improves interfacial reaction potential. Notably, NMP forms a nitrogen-rich cathode-electrolyte interface (CEI) membrane during the discharge process, which enhances interfacial ionic conductivity and stabilizes the electrode-electrolyte interface. The optimized electrolyte system achieves a discharge plateau of 2.7 V and an energy density of 2128 Wh kg −1 at 50 mA g −1 , significantly surpassing that of the conventional electrolyte (COE). This study provides a low-cost electrolyte optimization strategy, offering a promising approach to maintaining the high energy density and discharge voltage of Li/CF x batteries.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Hao Feng,Zhenxi Li,Shilun Gao,Youjia Zhang,Ruijie Guo,Peng-Fei Cao,Huabin Yang
The increasing demand for safe, high-energy-density batteries drives the development of solid-state electrolytes. Organic/inorganic hybrid electrolytes, integrating the benefits of polymer and inorganic electrolytes, exhibit flexibility, high mechanical strength, and superior ionic conductivity. However, interfacial incompatibility between organic/inorganic components and high electrolyte/electrode interfacial resistance restricts their practical applications. Herein, a flexible and high ionic conductive organic/inorganic electrolyte is prepared via the simple electrospinning of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 @polyacrylonitrile (LAGP@PAN) and then in-situ polymerization of vinylene carbonate (VC). The LAGP fillers are homogenously distributed in PAN fibers, contributing to the compatible interface between the polymer matrix and inorganic reinforcement. The in-situ polymerization of VC to poly(vinylene carbonate) (PVCA) further improves the intimate electrolyte/electrode contact. As a result, the LAGP@PAN/PVCA electrolyte exhibits a high ionic conductivity of 2.05 × 10 −4 S cm −1 at 30 °C. The Li|LAGP@PAN/PVCA|Li symmetric cell can stably cycle for over 2300 h. The Li|LAGP@PAN/PVCA|LiFePO 4 cell exhibits excellent cycling performance with a capacity retention of 88 % after 700 cycles at 1C. Even combined with commercial LiFePO 4 cathode and thin Li foil anode (N/ P = 2), the full cell also shows stable cycling performance. This study presents a promising approach to mitigate interfacial challenges in solid electrolytes, facilitating the development of Li metal with high-safety and high-energy density.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Tingting Liu,Zhian Dou,Zhen Li,Yiran Sun,Chunyi Wang,Longchen Li,Hao Yin,Jiwen Li,Xiaozhong Wu,Jinglin Mu,Pengfei Zhou,Jin Zhou
Li/CF x primary batteries are renowned for their exceptional energy density, yet their practical deployment is hindered by the inherently sluggish kinetics of the CF x cathode. This study addresses this limitation by incorporating selenium (Se) into CF x (denoted as CF x /Se) via a facile low-temperature thermal treatment, significantly enhancing its electrochemical performance. Comprehensive spectroscopic and electrochemical analyses reveal that Se doping induces the formation of C Se bonds, which promote semi-ionic C F bonding, thereby accelerating Li + diffusion and reducing charge transfer resistance. Density functional theory calculations further demonstrate that Se doping modulates the electronic structure of CF x , narrowing its bandgap to establish an efficient conductive network and markedly improving electronic conductivity. The optimized CF x /Se-1 composite (Se:CF x = 1:9) delivers outstanding performance, achieving a discharge capacity of 383.9 mAh g −1 at a high current density of 20 A g −1 with an energy density of 765.7 Wh kg −1 and a power density of 3.99 × 10 4 W kg −1 . Moreover, CF x /Se-1 exhibits remarkable wide-temperature operability (−35 to 60 °C), retaining a capacity of 485.3 mAh g −1 at 0.5 A g −1 with a stable 2.0 V plateau even at −35 °C. This work underscores the pivotal role of Se doping in tailoring the band structure of CF x , unlocking its potential for high-power and extreme-temperature Li/CF x batteries.
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Journal of Material Cycles and Waste Management
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2025
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IF 3
Lou Wen-bo,Liu Dong-yan,Zhao Da,Wang Yun,Sun Zi-cheng,Zou Yi,Niu Xiao-wei,Cheng Quan-guo,Li Jian-zhong,Liu Hong-hui
The recovery of NCM (LiNi x Co y Mn 1-x-y O 2 , abbreviated as NCM) cathode materials from retired lithium-ion batteries is a research hotspot in resource recycling field. Nevertheless, due to aluminum impurities mixed in raw materials, Li(I) and Al(III) ions are easy to combine to form water-insoluble LiAlO 2 during reduction, affecting Li(I) ions’ water-leaching efficiency. In this study, the LiAlO 2 formation environment is analyzed. Thermodynamic analysis reveals that there is generally less spontaneity in the reaction of Li (I) ions with aluminum monomers compared to Al 2 O 3 , and the introduction of CO 2 can inhibit Li-Al-O substance production. Li-Al binding experiments show that there is almost no direct reaction between Li 2 CO 3 and aluminum monomers, but under Ar atmosphere, Li 2 CO 3 and Al 2 O 3 can easily lead to Li-Al binding, a kinetic analysis considers that binding is controlled by chemical reaction, with an activation energy of 57.78 kJ/mol, and the activation energy increases to 88.028 kJ/mol with CO 2 atmosphere. Under reduced optimization conditions (reduction temperature: 500 °C, time: 6 h, and m NCM : m Al = 1: 0.25), the carbonation water-leaching efficiency can reach 95.1% for Li(I) ions and less than 1% for Ni(II), Co(II), Mn(II), and Al(III) ions. Thus, this work offers a theoretical basis for the industrial Li(I) ions’ recovery from aluminum-containing NCM materials.
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Materials Today Communications
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2025
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IF 4.5
Jiaqi Wang,Xiqiang Huang,Xingbao Zhu,Yuanguo Wu,Zining Man,Xiangyu Wen,Weiting Qi,Xing Tang,Zhe Lü
Despite their potential to enhance safety and design flexibility in next-generation lithium batteries, particularly lithium-oxygen (Li-O 2 ) systems, solid polymer electrolytes (SPEs) face persistent challenges of insufficient ionic conductivity and high interfacial resistance. To address these limitations, we developed a novel PEGDA-based quasi-solid-state electrolytes (QSEs) through in situ polymerization, strategically incorporating three functional additives: cellulose acetate (CA), N-methyl-2-pyrrolidone (NMP), and fluoroethylene carbonate (FEC). The electrolyte design leverages multiple synergistic mechanisms: hydrogen bonding between CA and NMP optimizes microstructural organization for efficient Li⁺ transport pathways; carbonyl groups in NMP coordinate with Li⁺ to facilitate LiTFSI dissociation, while oxygen-rich functional groups in CA provide supplementary Li⁺ coordination sites; FEC is introduced to further improve interfacial stability. This molecular engineering approach achieves an impressive room-temperature ionic conductivity of 8.54 × 10 −4 S cm −1 and a high lithium-ion transference number of 0.78. The QSE demonstrated excellent cycling stability (>900 h) in lithium symmetrical batteries and significantly improved the discharge capacity (12243 mAh g −1 ) and long-term cycling performance (590 h) of Li-O 2 batteries. These results highlight the efficacy of our multi-functional additive strategy in overcoming fundamental limitations in solid electrolytes, offering important insights for the rational design of high-performance energy storage systems.
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ACS Sensors
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2025
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IF 9.1
Chaoqi Zhu,Kechen Zhou,Huiyu Su,Yazhou Yang,Jiahong Tang,Xiaoxia Wang,Wulin Song,Dawen Zeng
The development of highly sensitive electrolyte leakage monitoring sensors is critical for enabling early fault detection and ensuring the safe operation of lithium-ion battery (LIBs) systems. In this study, perovskite LaFeO3 hollow microspheres with an average diameter of 850 nm were synthesized via a hydrothermal method. Gas-sensing tests demonstrated that the LaFeO3 hollow microsphere sensor exhibited exceptional responsiveness to dimethyl carbonate (DMC) gas, achieving a remarkable response value of 67.9 toward 10 ppm DMC at an operating temperature of 150 °C. The sensor also showed a fast response/recovery rate (170/90 s), excellent selectivity, long-term stability, and a low detection limit of 20 ppb. This excellent gas-sensing performance may be attributed to the high specific surface area and well-developed mesoporous structure of the hollow structure. Moreover, it demonstrated rapid response capabilities in simulated leakage detection scenarios. This work presents a novel perovskite LaFeO3-based sensor that can effectively detect DMC gas leakage and provide an effective strategy for enhancing safety monitoring in LIB applications.
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Energy & Environmental Materials
·
2025
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IF 14.1
Yuanxin Gao,Xinyi Wang,Dong Lv,Zhang Zhang,Jiangpeng Li,Xiaoyan Feng,Jingchao Chai,Yun Zheng,Yu Peng,Yanqing Wang,Yingying Wang,Lingyu Zhu,Zhihong Liu
Fluorinated amide electrolytes represent a promising solution for high-energy density lithium metal batteries, yet their application in Ni-rich layered oxide cathodes is hindered by interfacial instability. This study develops a non-flammable fluorinated amide-based deep eutectic electrolyte modified with fluoroethylene carbonate, which simultaneously enhances ionic conductivity (1.5 × 10 −4 S cm −1 ) and anodic stability (>4.4 V vs Li + /Li). Applied in Li/NCM811 batteries, the fluoroethylene carbonate-based electrolyte enables 83.2% capacity retention after 200 cycles at 0.5 C, significantly outperforming conventional counterparts. ToF-SMIS and XPS tests reveal that fluoroethylene carbonate facilitates the formation of a LiF-rich cathode-electrolyte interphase, suppressing parasitic reactions and improving Li + transport kinetics. Furthermore, the electrolyte demonstrates superior lithium metal compatibility, inhibiting dendrite growth while enhancing thermal safety. These findings underscore the critical role of fluorinated amide electrolytes in stabilizing Ni-rich cathodes and highlight their potential for next-generation high-voltage lithium metal batteries.
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