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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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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COMBUSTION AND FLAME
·
2026
·
IF 5.9
Yushen Yu,Bin Dong,Jiabiao Zou,Bingzhi Liu,Long Zhu,Shuyao Chen,Zhihong Hu,Jiwen Guan,Aamir Farooq,Zhandong Wang
Ethyl methyl carbonate (EMC, C 4 H 8 O 3 ), a solvent in lithium-ion batteries, poses fire risks due to thermal instability, but existing combustion models fail to accurately predict species concentrations and ignition delays. In this study, we conducted EMC pyrolysis experiment in a jet-stirred reactor (JSR) at 620−1010 K and 1.0 bar and quantitively measured the decomposition products by the synchrotron VUV photoionization mass spectrometry and gas chromatography. The pyrolysis at higher temperature of 981–1476 K were examined by employing shock tube (ST) and laser absorption diagnostics. We found EMC mainly decomposing through the retro-ene reaction pathway in JSR and we obtained the rate constants of EMC retro-ene reaction at 710–830 K derived from the mole fraction change of EMC assuming the first order reaction rate. At higher temperature of 981–1476 K in ST, the rate constants are obtained by the measured CO 2 time-histories. The overall best-fit Arrhenius expression of EMC decomposition is found to be: k ( T ) = 2.74×10 13 (s –1 )∙exp[-49.057(kcal∙mol -1 )/ RT ]. By incorporating the determined rate constant into the previous models, the updated kinetic models yield notably improved predictions of mole fraction of EMC and its reaction products, while maintaining good agreement with experimental data on global combustion properties of EMC.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhaojun Liu,Jiaxuan Feng,Rui Yang,Shen-ao Wang,Xiaochen Wu,Xiangyu Zhang,Sujuan Cheng,Ning Liu,Teng Long,Pengchao Si
Overcoming the trade-off between high-voltage stability and wide-temperature performance, especially at low temperatures, in lithium-ion batteries (LIBs) requires innovative electrolyte design. While carbonate-based electrolytes dominate commercial applications for their graphite compatibility, their strong solvent-ion interactions and elevated viscosity below −20 °C significantly compromise low-temperature performance. They also lead to unstable reactions at the electrode surfaces under high voltage. We report a LiNO 3 -tailored electrolyte system that simultaneously achieves an unprecedented 5.54 V electrochemical window and stable operation down to −40 °C. By coupling low-melting carboxylate esters with fluoroethylene carbonate and LiNO 3 additives, the formulation constructs anion-dominated solvation structures. The designed electrolyte suppresses solvent decomposition at high voltage while maintaining ionic conductivity at ultra-low temperatures. The high-loading full cells (G/NCM811, 12.68 mg cm −2 ) achieve 70 % capacity retention at −40 °C relative to room temperature performance, sustaining 89 % capacity after 350 cycles at 1C at 25 °C. Moreover, the novel electrolyte enables G/NCM811 pouch batteries to charge and discharge at a high voltage of 5.1 V, achieving a second-cycle coulombic efficiency of 91.22 %. Furthermore, the new electrolyte enables the Li/NCM811 cell to operate at high temperatures of 75 °C and supports rapid charging and discharging of the high-loading G/NCM811 full cell at 70 °C. This work provides a promising design principle for extreme-condition electrolytes through synergistic nitrate chemistry and solvation engineering.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
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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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Small
·
2026
·
IF 12.1
Haojie Wan,Shaoqing Liu,Ying Zhang,Xue Liu,Rong Zeng,Jiashen Meng,Jean-Jacques Gaumet,Wen Luo,Jianwen Liu
For sodium-ion batteries, addressing the issue of limited cycle life is crucial for their widespread industrial application, and the electrolyte plays a pivotal role in this context. In this study, a practically viable electrolyte with industrial potential is proposed, introducing sulfone and borate as cooperative electrolyte additives to improve cycling stability. The optimized electrolyte formulation is composed of NaPF 6 (sodium hexafluorophosphate) dissolved in a mixed solvent of PC (propylene carbonate)/EMC (ethyl methyl carbonate), supplemented with PES (prop-1-ene-1,3-sultone) and NaODFB (sodium difluoro(oxalato)borate). In this system, the decomposition of PES generates S-O x species, which modify the interfacial chemical environment and promote a more complete decomposition of ODFB − . As a result, B- and S-containing organic intermediates are further transformed into oxygen-coordinated inorganic species (e.g., B-O x and S-O x ), which subsequently reconstruct into a crosslinked inorganic interphase. This cooperative interfacial evolution leads to the formation of more uniform, compact, and chemically stable CEI/SEI layers, thereby enabling superior cycling stability. As a demonstration, the Na||NVP (sodium vanadium phosphate) half-cell retains a specific capacity of 109.8 mAh·g −1 after 5000 cycles, corresponding to a capacity retention of 96.7%. This work offers valuable insights and experimental support for the large-scale industrialization of long-life sodium-ion battery electrolytes.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Pengbing He,Qionghua Xie,Jinyu Wang,Guocheng Yao,Liangshi Wang
Efficient separation of lithium isotopes is crucial for nuclear energy, isotope geochemistry, and advanced energy storage. This study developed an electromigration system that uses organic solvents as the separation medium. The system investigated the effects of solvent type, lithium salt species, and migration path length. The EMC-based system demonstrated superior isotopic selectivity, achieving a separation factor exceeding the industrial benchmark of 1.050 under conditions of 16 V, 0.1 mol∙L −1 LiTFSI anolyte, a 10 cm path length, and 3 h of operation. In contrast, the DMA-based system exhibited significantly higher Li + flux due to weaker coordination, albeit with lower isotope selectivity. Molecular dynamics simulations revealed distinct solvation behaviors. EMC formed dense LiTFSI clusters that enhanced isotope selectivity but impeded ion transport, whereas DMA formed looser complexes that facilitated faster ion migration. Radial distribution functions and coordination numbers confirmed stronger Li + interactions with EMC compared to DMA. These findings establish a mechanistic understanding of the trade-off between isotopic separation efficiency and ion flux, providing both theoretical and experimental guidance for designing high-performance lithium isotope separation systems.
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MOLECULES
·
2025
·Vol. 30
·期 11
·2474
·
IF 4.6
Yuqing Gao,Yankui Mo,Shengguang Qi,Mianrui Li,Tongmei Ma,Li Du
Polymer electrolytes (PEs) provide enhanced safety for high–energy–density lithium metal batteries (LMBs), yet their practical application is hampered by intrinsically low ionic conductivity and insufficient electrochemical stability, primarily stemming from suboptimal Li+solvation environments and transport pathways coupled with slow polymer dynamics. Herein, we demonstrate a molecular design strategy to overcome these limitations by regulating the Li+solvation structure through the synergistic interplay of conventional Lewis acid–base coordination and engineered hydrogen bond (H–bond) networks, achieved by incorporating specific H–bond donor functionalities (N,N′–methylenebis(acrylamide), MBA) into the polymer architecture. Computational modeling confirms that the introduced H–bonds effectively modulate the Li+coordination environment, promote salt dissociation, and create favorable pathways for faster ion transport decoupled from polymer chain motion. Experimentally, the resultant polymer electrolyte (MFE, based on MBA) enables exceptionally stable Li metal cycling in symmetric cells (>4000 h at 0.1 mA cm−2), endows LFP|MFE|Li cells with long–term stability, achieving 81.0% capacity retention after 1400 cycles, and confers NCM622|MFE|Li cells with cycling endurance, maintaining 81.0% capacity retention after 800 cycles under a high voltage of 4.3 V at room temperature. This study underscores a potent molecular engineering strategy, leveraging synergistic hydrogen bonding and Lewis acid–base interactions to rationally tailor the Li+solvation structure and unlock efficient ion transport in polymer electrolytes, paving a promising path towards high–performance solid–state lithium metal batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Nanjie Chen,Dongchu Chen,Jingshu Wu,Yuekun Lai,Dongyang Chen
Redox flow batteries (RFBs) are highly promising electrochemical systems for large-scale energy storage. To develop high energy density non-aqueous catholyte for RFBs, herein, two polar and bulky polyethylene glycol tails have been attached to the tetrathiafulvalene (TTF) core by ester exchange reactions. Such modification turns scarcely soluble TTF particles into viscous oils, which are totally miscible with the conventional organic electrolytes. The 4,4′(5′)-bis(2-(2-methoxyethoxy)ethyl)carboxylate -tetrathiafulvalene (TTF-BMEEC) with a mass-based specific capacity of 107.84 mAh g −1 is systematically evaluated in a hybrid RFB. When paired with a Li foil electrode and a permselective separator, the catholyte consisting of 1.0 M of TTF-BMEEC delivers two high discharge voltage plateaus of 3.55 and 3.88 V, a large volumetric capacity of 49.6 Ah L −1 , an outstanding energy density of 178.0 Wh L −1 , and a high cycling capacity retention of 91.5% after 100 cycles at the current density of 10 mA cm −2 . The excellent electrochemical stability of TTF-BMEEC is confirmed by UV–vis and 1 H NMR investigations and supported by density functional theory (DFT) calculations. These results demonstrate that molecular engineering has great potential for the development of high performance organic redox-active materials for RFBs.
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ENVIRONMENTAL TECHNOLOGY
·
2023
·
IF 2.8
Juan Xu,Kai Li,Lanxiang Liu,Jinju Ma,Hong Zhang
Lithium cobalt oxide (LCO) has been employed as cathode material for 40 years. However, the low solubility of LCOs in water and strong electrostatic force and H-bonding between the LCOs particles limited the use of the aqueous binders in the LCO system. We report a feasible and universal approach to fabricating a complex cathode of LCO and reduced graphene oxide (RGO). Tannic acid (TA) could simultaneously disperse LCO and RGO particles. Meanwhile, the branched polyphenol TA acts as a ‘bridge’ molecule for connecting the LCO and RGO, confirmed by the SEM test. The rheology properties of the PVDF slurry of cathode materials (LCO, LCO/, RGO, and TA/LCO/RGO) were also determined. It could be found that the TA could act as a crosslinking agent for the LCO and RGO particles, increasing the viscosity and storage modulus of the slurry. The cell employed the TA/LCO/RGO slurry as the cathode material, have a higher areal capacity, and had a higher redox potential than employed LCO/RGO and LCO as cathode materials, all of which could be attributed to the addition of the TA. This green molecule can be used to fabricate environmentally friendly and possibly biodegradable electrochemical energy storage devices.
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LANGMUIR
·
2023
·
IF 3.9
Zhuo Wang,Quanbing Pei,Mengmeng Wang,Junjun Tan,Shuji Ye
Silicon is reported to be a promising anode material due to its high storage capacity and excellent energy conversion rate. Molecular-level insight into the interaction between silicon electrodes and electrolyte solutions is essential for understanding the formation of a stable solid electrolyte interphase (SEI), but it is yet to be explored. In this study, we apply femtosecond sum frequency generation vibrational spectroscopy to investigate the initial adsorption of various pure and mixed electrolyte molecules on the silicon anode surface by monitoring the SFG signals from the carbonyl group of electrolyte molecules. When the silicon comes in contact with a pure carbonate solution, the linear carbonates of diethyl carbonate and ethyl methyl carbonate adopt two conformations with opposite C═O orientations on the silicon interface while the cyclic carbonates of ethylene carbonate and propylene carbonate almost adopt one conformation with C═O bonds pointing toward the silicon electrode. When the silicon comes in contact with the mixed linear and cyclic carbonate solutions, the total SFG intensity from the mixed solutions is approximately 2∼5 times weaker than those of pure cyclic carbonates. The C═O bonds of cyclic carbonates point toward the silicon electrode, while the C═O bonds of linear carbonates face toward the bulk solution at the silicon/mixed solution interface. No preferential absorption behaviors of the linear and cyclic carbonate electrolytes on the silicon electrode are observed. Such findings may help to understand the mechanism by which the SEI formed on the silicon anode is unstable.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Hao Wu,Wenfang Feng,Michel Armand,Zhibin Zhou,Heng Zhang
Carbonyl-based negative electrodes have received considerable interest in the domain of rechargeable lithium batteries, owing to their superior feasibility in structural design, enhanced energy density, and good environmental sustainability. Among which, lithium terephthalate (LiTPA) has been intensively investigated as a negative electrode material in the past years, in light of its relatively stable discharge plateau at low potentials (ca. 1.0 V vs Li/Li+) and high specific capacity (ca. 290 mAh g–1). However, its cell performances are severely limited owing to the poor quality of the solid-electrolyte-interphase (SEI) layer generated therein. Here, we report the utilization of lithium bis(fluorosulfonyl)imide (LiFSI) as an electrolyte salt for forming a Li-ion permeable SEI layer on the LiTPA electrode and subsequently improving the cyclability and rate performance of the LiTPA-based cells. Our results show that, differing from the reference electrolyte containing the lithium hexafluorophosphate (LiPF6) salt, the electrochemical reductions of the FSI– anions occur prior to the lithiation processes of LiTPA electrode, which is capable of building an inorganic-rich SEI layer containing lithium fluoride (LiF) and lithium sulfate (Li2SO4). Consequently, the lithium metal (Li°)||LiTPA cell shows significantly improved cycling performance than the LiPF6-based reference cell. This work provides useful insight into the reductive processes of the FSI– anions on negative electrodes, which could spur the deployment of highly sustainable and high-energy rechargeable lithium batteries.
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