Nanoscale
·
2025
·
IF 5.1
Luo Zhang,Haodong Zhao,Donglai Xiao,Haibo Tian,Haibo Zhang,Xinghua Zhu,Dingyu Yang
Lithium-ion batteries (LIBs) have been widely applied in electric vehicles, smart grids, and other fields due to their high energy density and long cycle life. However, the flammability of conventional carbonate-based electrolytes poses significant safety risks and hinders the large-scale deployment of high-energy-density batteries. Herein, we propose a nonflammable carbonate-based local high-concentration electrolyte (LHCE) composed of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)/fluorinated ethylene carbonate (FEC)/1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE). This formulation replaces highly flammable conventional solvents with FEC and highly fluorinated TTE, substantially reducing fire hazards. The electrolyte exhibits an electrochemical window up to 5.5 V. Synergistic interactions between TFSI⁻ anions and FEC facilitate the formation of a robust, LiF-rich solid electrolyte interphase (SEI) on the graphite (Gr) anode and an effective cathode electrolyte interphase (CEI) on the high-voltage LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode, suppressing structural degradation and transition metal dissolution. Consequently, the NCM811||Gr full battery using LHCE demonstrates superior cyclability, with a capacity loss below 8% over 200 cycles at a high cutoff voltage of 4.5 V and an average coulombic efficiency (CE) of 99.9%. This work provides a promising electrolyte design for stable and safe high-voltage LIBs, offering potential guidance for advanced battery systems.
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IONICS
·
2025
·
IF 2.6
Gu Bonwun,Kang Chankyu
In this study, the flash points and ionic conductivity of three ternary electrolyte solvents (ethylene carbonate (EC); diethyl carbonate (DEC); and dimethyl carbonate (DMC)) were investigated in lithium-ion batteries. The flash points of the solvent mixtures were experimentally measured and compared with predictions using Raoult’s law and multiple regression analysis. These results indicate that EC increases flash point temperature and ionic conductivity owing to its high dielectric constant and boiling point. In contrast, DMC has a lower flash point because of its low boiling point and high reactivity. The coefficient of determination ( R 2 ) and mean absolute error (MAE) suggest that Raoult’s law better predicts overall trends in flash points. Simultaneously, multiple regression analysis provided higher accuracy for specific mixture compositions. Additionally, the ionic conductivities of the ternary electrolyte mixtures were analyzed, demonstrating that DMC maintained high conductivity through polar conformers despite its low dielectric constant. The optimal mixture ratio of EC: DEC: DMC at 7:2:1 achieved a balance with a high flash point (55.5 °C) and high ionic conductivity (9.0 mS cm⁻ 1 ), enhancing battery safety and ionic conductivity. This study highlights the critical role of solvent composition in optimizing lithium-ion battery electrolytes for improved safety and ionic conductivity. Graphical
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Journal of Energy Storage
·
2026
·
IF 9.8
Mingdong Du,Yanxia Liu,Chenxing Wang,Fulai Qi,Mingyu Shi,Wenjing Liu,Shengnan He,Zhijun Wu,Zhenglong Li,Chenchen Li,Hongge Pan
Lithium (Li) metal is the ideal anode material for building future large-scale energy storage batteries. Nevertheless, Li metal anodes suffer from incompatibility with conventional carbonate-based electrolytes, which possibly leads to severe Li dendrite growth, undesirable electrolyte decomposition, and rapid deterioration of the cycling performance. To address these challenges, the traditional commercial electrolyte is doped with cerium bis(trifluoromethanesulfonyl)imide (Ce(TFSI) 3 ) for enhanced Li anode stability. The low migration rate of Ce 3+ leads to formation of a Ce-enriched corrosion resistant solid electrolyte interphase (SEI), while the TFSI − anion enables a significant enhancement of inorganic components within the SEI, thus facilitating uniform Li + deposition and mitigation of detrimental electrolyte decomposition. The resulting electrolyte exhibits superior electrochemical stability against Li anodes. This is evidenced by a Li||Li symmetric cell that cycles steadily for over 1300 h at a current density of 1 mA cm −2 and a capacity of 1 mAh cm −2 , along with a exchange current density of 1.3183 mA cm −2 . Additionally, Li||LiFePO 4 full cell demonstrates 76.8% capacity retention (110.39 mA cm −2 ) after 900 cycles at 1 C. This work illustrates the significant impact of a corrosion-resistant interface on Li anode performance and offers a valuable idea for constructing high-durability SEI layers.
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Batteries & Supercaps
·
2026
·Vol. 9
·期 8
·e70437
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IF 4.5
Enyong Wang,Haoming Wang,Shengxiang Kang,Xiaohui Liu,Jing Zhang,Lan Xia,Yuejin Zhu,Like Huang
Hybrid halide perovskites (HPs) exhibit soft lattice frameworks and intrinsic ion-migration characteristics, suggesting potential tolerance toward foreign-ion insertion beyond their established optoelectronic applications. However, their structural evolution and electrochemical reaction pathways under lithium insertion remain largely unexplored. In this work, CH 3 NH 3 PbI 3 films were fabricated on Cu foil via a facile drop-casting method and systematically investigated as model electrodes for lithium-ion storage. The initial discharge capacity reaches 310.4 mA h g −1 and stabilizes at approximately 120 mA h g −1 after 160 cycles at moderate current density. Detailed electrochemical and structural analyses reveal a multistep lithiation process involving Li + insertion, partial reduction of Pb(II) species, and interfacial alloying reactions accompanied by progressive lattice degradation. The results provide insights into ion-induced structural transformation and interfacial chemistry in HPs under electrochemical environments. Considering their compositional tunability and structural flexibility, HPs may serve as a versatile platform for exploring functional electrochemical layers. Graphical Electrochemical characterization shows that MAPbI 3 halide perovskite is not merely electrochemically active for lithium storage, but undergoes coupled bulk and interfacial evolution during cycling. Materials characterization and schematic analysis reveal that lithium-ion insertion drives lattice distortion in the soft perovskite framework, while near the Cu current collector, the perovskite gains electrons and is reduced to metallic Pb.
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Nanomaterials
·
2026
·Vol. 16
·期 15
·969
·
IF 4.8
Junaid Aslam,Muhammad Arif Khan,Weiwei Sun,Chao Yang
Germanium (Ge) is a promising high-capacity anode material for lithium-ion batteries; however, its practical application remains limited by substantial volume variation, unstable interfacial reactions, and rapid capacity degradation during repeated lithiation/delithiation. In this work, a binder-free Ge/C/MXene@NF hybrid electrode was developed through a sequential fabrication process, where Ge nanoparticles were immobilized within a PVP-derived carbon matrix supported on a three-dimensional nickel-foam scaffold and subsequently integrated with a Ti3C2TxMXene conductive network to construct a hierarchical Ge/C/MXene hybrid architecture. The nickel foam provides a continuous current-collecting framework and mechanical support, while the MXene network improves electrical connectivity, electrolyte accessibility, and interfacial charge-transfer kinetics. Structural and compositional analyses further indicate the presence of PVP-derived carbon and a possible minor NiGe interfacial phase formed during annealing. Comparison with Ge@NF and the individual component electrodes provides insight into the respective contributions of MXene, Ge, and the PVP-derived carbon framework to the electrochemical behaviour of the composite electrode. Using the total deposited active-material mass as the normalisation basis, the MXene@Ge@NF electrode retains a reversible specific capacity of 789.8 mAh g−1after 100 cycles at an effective current density of 76.2 mA g−1. The observed electrochemical behaviour originates from the integrated contributions of Ge nanoparticles, the PVP-derived carbon matrix, the conductive Ti3C2TxMXene network, the three-dimensional nickel-foam scaffold, and possible Ni–Ge interfacial interactions. Rather than representing a Ge-dominated electrode, this architecture demonstrates the advantages of integrating multiple functional components within a binder-free Ge/C/MXene hybrid architecture.
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Nature Sustainability
·
2026
·
IF 32.1
Zhao Chang-Xin,Li Zheng,Zhang Daoning,Zhang Nan,Zhang Qiu,Wang Zeyi,Li Yue,Chen Yawei,Wang Chunsheng
Fast charging and low-temperature operation are essential for next-generation energy storage. However, high-energy batteries struggle to meet these demands as existing electrolytes cannot simultaneously deliver fast interfacial kinetics, high ionic conductivity and favourable interphase formation. Prevailing strategies focus on weakening thermodynamic solvation, yet this approach does not directly address the kinetic bottleneck, that is, the desolvation barrier governing interfacial charge transfer. Here we reveal that the desolvation kinetics are dictated by dynamic solvent exchange rather than thermodynamic solvation energy. Guided by this mechanistic insight, we have formulated an electrolyte in which two anions carry distinct anionic potentials: high-anionic-potential anions form contact ion pairs that accelerate solvation-exchange kinetics, while low-anionic-potential anions form solvent-separated ion pairs that sustain high bulk ionic conductivity. The electrolyte enables fast charging and low-temperature operation in high-loading lithium-ion batteries. The design principle was further validated in aqueous aluminium-ion electrochemical systems, underscoring its broader relevance to sustainable, resource-abundant battery chemistries beyond the lithium ion. Together, our findings establish a new electrolyte design paradigm that decouples interfacial and bulk transport properties and expands the design space of battery electrolyte systems.
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Nature Communications
·
2026
·
IF 18.1
Hong Xufeng,Wang Xizhe,Harris Stephen J.,Zhao Hongbo,Meng Jiashen,Jia Qingshan,Zhao Qianchuan,Xu Kang,Pang Quanquan,Jiang Benben
Designing electrolyte materials for high-energy lithium metal batteries requires navigating vast, discrete chemical spaces, where intricate interphasial and electrolyte chemistries render component interactions largely unclear. Traditional trial-and-error methods struggle with discontinuous electrolyte-performance relationships and inefficient adaptation to new molecular candidates, hindering discovery. Here, we propose a two-stage deep active learning framework with knowledge transfer for rapid electrolyte design. In stage one, deep active learning with deep kernel learning selects informative experiments and models discontinuous relationships between formulation and performance, improving sample efficiency and reducing experimental cost. In stage two, target statistic coding quantifies what was learned and transfers it to new design settings, such as expanded formulation spaces and newly introduced components, using only a small number of additional measurements. Using this framework, we found electrolytes that increase the average lifetime of lithium metal symmetric cells by threefold after three learning iterations, and we rapidly identified improved formulations for Li 0 | |LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells in expanded chemical spaces. This work provides an experiment-driven, sample-efficient route to explore complex electrolyte formulation spaces and quantify inter-component correlations, as well as a realistic, high-cost, small-data benchmark for probabilistic surrogate modeling and sequential decision-making in discrete chemical spaces.
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Nature Communications
·
2026
·
IF 18.1
Chen Yunyi,Qian Xitang,Lyu Yuxiang,Qiu Yican,Zhou Siyu,Lan Xinyi,Lu Siqi,Shao Minhua
Initial-anode-free lithium metal batteries offer the potential for high energy density and simplified manufacturing, positioning as a transformative platform for sustainable energy storage. However, their implementation is hindered by the low reversibility of lithium plating/stripping. Herein, we propose a dynamic integrated interface engineering strategy that incorporates an Ag-based multifunctional initiator into the electrolyte. This additive consists of Ag + paired with anions capable of generating Lewis acids, enabling electrode-electrolyte interfacial coupling through in situ polymerization, while simultaneously enhancing the lithiophilicity of current collectors via Ag + -driven in situ deposition. The controlled release of the additive regulates the solvation structure, leading to the solid electrolyte interphase with an inverted organic-rich inner/inorganic-rich outer architecture, which represents a deliberate departure from conventional models. The anion anchoring effect reinforces the self-healing capability of the interphase, ensuring the construction of fast Li-ion transport pathways and a durable protective barrier, realizing highly stable operation of initially anode-free quasi-solid-state batteries. Specifically, the Cu | |LiFePO 4 cell exhibits 90% capacity retention after 200 cycles at 0.1 C, and a 2 Ah-level pouch cell delivers a specific energy of 467 Wh kg −1 based on total cell weight. This work provides an effective unified approach to address multiple interfacial challenges in initially anode-free lithium batteries.
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Journal of Energy Chemistry
·
2026
·
IF 15.6
Wenrong Lv,Fei Pei,Minna Mao,Zhenyu Huang,Gaoce Han,Yi Zhang,Yu Huang,Aiqi He,Wenjie Lin,Qiang Gao,Yue Guo,Yunhui Huang,Yifei Yu
Understanding the structural evolution and failure mechanisms of electrodes is vital for advancing high-energy-density lithium batteries. However, real-time visualization of internal degradation processes under realistic conditions remains a major challenge. Here, we report an operando distributed strain imaging approach based on intrinsic Rayleigh backscattering to reveal the distinct stress evolution of Li-metal batteries (LMBs) with PVDF-based solid polymer electrolyte (SPE) and carbonate-based liquid electrolyte (LE). Distinct from conventional fiber Bragg grating (FBG)-based point strain monitoring, this distributed imaging method provides high spatiotemporal resolution and stress sensitivity, enabling non-destructive, full-area detection of interfacial inhomogeneity in lithium deposition beyond the reach of conventional electrochemical signals. Using this technique, we achieve continuous stress imaging over the full life cycle (>1600 h) in pouch-type LMBs, enabling life-cycle tracking of degradation evolution and uncovering an anomalous “V-shaped” stress trajectory during lithium deposition. Notably, NCM811|LE|Li batteries exhibit a maximum local strain of 441 µε after 120 h, more than twice that of NCM811|SPE|Li (164 µε). Large-area mapping further reveals that the PVDF-based SPE facilitates homogeneous Li + flux and uniform deposition. This Rayleigh-backscattering-enabled imaging offers a powerful diagnostic method for quantifying interfacial stress dynamics and real-time assessment of state of health in high-energy-density lithium batteries. Distributed Rayleigh-optical frequency domain reflectometry (OFDR) strain imaging reveals distinct chemo-mechanical degradation between NCM811|LE|Li and NCM811|SPE|Li pouch cells under industrial low stack pressure. Download: Download high-res image (201KB) Download: Download full-size image
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Fengqian Wang,Qigao Han,Shuaijing Ji,Junwei Wang,Baoshuai Du,Keyao Li,Liquan Tian,Weixin Zhang,Shun Tang,Shijie Cheng,Yuan-cheng Cao
The process of solvent-free binder fibrillation is a promising technology in the field of increasing electrode density and green economy. However, the electron conduction and homogeneity of thick electrodes are limited, resulting in poor battery performance and mechanical properties. Herein, we compare the effect of three different forms of conductive materials on the cathode, and design a “point-line” combined conductive carbon-binder network with polytetrafluoroethylene fiber embedded in carbon nanotubes and super P by air mill. We illustrate that the performance enhancement of the optimized cathode originates from the combined factors of excellent electronic conductivity, low surface energy and special nested structure. Furthermore, the embedded binder has the ability to protect the cathode and maintain structural stability. These characteristics result in superior cycling stability for the optimized cathode, with a capacity retention rate of 91.4 % after 150 cycles at 1C and a better rate capability (158.6 and 142.2 mAh g −1 at 1 and 2C, respectively). Consequently, it provides a valuable strategy to combine the functions of different materials to develop high energy density lithium-ion batteries.
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Nano Research
·
2022
·Vol. 16
·期 6
·8368-8376
·
IF 10.269
Zhou Ge,Zhao Yulin,Hu Chuan,Ren Zhenzhen,Li Hong,Wang Liping
Lithium (Li) metal is an ideal anode for the next generation high-energy-density batteries. However, it suffers from dendrite growth, side reactions, and infinite relative volume change. Effective strategies are using porous carbons or surface modification carbons to guide Li deposition into their pores. While the Li deposition behavior is still ambiguous. Here, we systematically determine their deposition behavior in various surface-modified carbons and in different electrolytes via optical microscopy and scanning electron microscopy study. It is found that Li will not spontaneously deposit into the carbon pores, which is significantly dependent on the carbon surface, current density, areal capacity, and electrolyte. Thus, a “lithiophilic” modified commercial hard carbon with Ag is developed as a stable “host” and efficient surface protection derived from the localized high-concentration electrolyte exhibits a pretty low volume change (5.3%) during cycling at a current density of 2 mA·cm −2 and an areal capacity of 2 mAh·cm −2 . This strategy addresses the volume change and dendrite problems by rationally designed host and electrolyte, providing a broad perspective for realizing Li-metal anode.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Zhaoxin Lu,Zhenlian Chen,Muqin Wang,Yi Wan,Jingkun Yan,Shuaishuai Chen,Yan Shen,Zhao Yan,Deyu Wang
Lithium aluminum titanium phosphate, abbreviated as LATP, is an important Li+ solid-state electrolyte thanks to its high ionic conductivity and good stability in the ambient atmosphere. Extensive efforts have been devoted to understanding its advanced electrochemical properties. However, the strategy to use it in practical cell is rarely available. In this work, we demonstrate LATP’s working behavior via LATP that is coated on a separator facing the cathode and anode, respectively, in both graphite|LiNi0.8Co0.1Mn0.1O2 and Li|LiNi0.8Co0.1Mn0.1O2 cells. With the LATP contact with LiNi0.8Co0.1Mn0.1O2, the cells deliver slightly lower reversible capacity owing to a large Li+ diffusion impedance originated from the space charge layer formed between LATP and cathode and show better durability due to the synergetic Li+ transportation via LATP and organic electrolyte. As for LATP facing graphite, the cells deliver a higher discharge capacity and better cyclic stability. It is ascribed to the buffering and protecting effect of the solid electrolyte interphase (SEI) that reduces the interfacial impedance and precludes the interfacial reaction between LATP and lithiated graphite. When directly in contact with lithium, LATP is decomposed quickly and the cells’ performance varies with the recipe of organic electrolytes. This work clearly indicated that LATP could improve the cells’ performance when appropriate technologies are utilized to address the associated challenges.
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