ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Yu Duan,Zihan Ma,Jiaxuan He,Yingying Huang,Shuo Bao,Jinlin Lu
P2-type layered cathode materials have low energy density due to low initial Na content. In this research, high sodium content P2-type cathode material Na0.8Li0.08Ni0.23Mn0.67Cu0.1O1.92F0.08 (NMC-LF), was synthesized by a simple high-temperature solid-phase method. The strong electronegativity of F allows the local TM-O bond to be transformed into a TM-F bond, and the TMO6 octahedron becomes more stable. The doping of Li+ not only maintains structural stability but also transforms the two-phase reaction in the high-voltage range into a solid-solution reaction. This leads to an effective suppression of the irreversible P2–O2 phase transition in the high-voltage region. At 20 mA·g–1, the initial discharge capacity of NMC-LF reaches 131.05 mAh·g–1. At a high current density of 200 mA·g–1, the discharge capacity reaches 101.9 mAh·g–1 and remains at 99.31% after 150 cycles. The diffusion coefficient of NMC-LF is as high as 8.67 × 10–13 cm2·s–1. Furthermore, the structural evolution during material formation is elaborated by high-temperature XRD, and it is determined that there are no impurities at 900 °C. Under the joint synergy of Li/F/Cu and the design of high sodium content, the long-cyclic and high-rate performance has been significantly improved. In-situ XRD tests show that Li/F/Cu codoping inhibits the P2–O2 phase transition and enhances structural reversibility. This provides a new idea for the research of layered cathode materials.
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DOI
高影响因子
IONICS
·
2026
·
IF 3.4
Wu Keying,Xie Wenda,Liu Xingjian,Chen Jing,Pu Haitao,Luo Bing
Separator design can improve electrolyte wetting, ion transport and dimensional stability in lithium metal cells with LiFePO 4 cathodes. Here, an Fe–Ti metal–organic framework (MOF) was prepared by a solvothermal route and incorporated into poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) nanofiber membranes by electrospinning. The effects of filler loading were evaluated against pristine PVDF-HFP and a commercial Celgard separator. Among the investigated compositions, PVDF-HFP/MOF-10 exhibited an electrolyte contact angle of 18°, an ionic conductivity of 1.7 × 10⁻ 3 S cm⁻ 1 at 30 °C, and an apparent Li⁺ transference number of 0.56 under the Bruce–Vincent measurement protocol. The composite also showed improved thermal dimensional stability. Li‖Li cells operated for over 500 h at 1 mA cm⁻ 2 and 1 mAh cm⁻ 2 , while LiFePO 4 ‖Li cells retained 92.3% of their initial discharge capacity after 500 cycles at 1 C. These observations support the use of the composite separator for improving performance under the tested conditions. Adsorption calculations provide a possible molecular explanation for electrolyte affinity, but do not establish ion desolvation, selective anion immobilization or a unique bimetallic synergy in the operating electrolyte. The contribution is the integration and loading optimization of an Fe–Ti MOF within a porous PVDF-HFP separator, with the microscopic transport mechanism remaining to be resolved.
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高影响因子
DESALINATION
·
2025
·
IF 9.8
Xinyue Zhang,Shichen Xiao,Zerong Miao,Xudong Wang,Jin Wang,Jiajin Hao,Junwei Xin,Huihui Zhang,Lei Wang
The selective recovery of lithium from salt-lake brines using functionalized polyamide nanofiltration (NF) membranes offers a promising strategy to alleviate the global lithium resource shortage. However, the structural controllability of functional fillers and their interfacial compatibility remain critical challenges in constructing high-performance NF membranes. In this study, a polyamide NF membrane was modified with defect-engineered and gel-state UiO-66-NH 2 nanoparticles, combined with an external electric field, to achieve efficient Li + /Mg 2+ separation. By tuning the HCl/HAc ratio, the nucleation and growth of UiO-66-NH 2 were regulated, yielding gel-state nanoparticles with abundant defects (defect coordination number ~ 0.73), excellent dispersibility, and high protonation, facilitating interfacial integration with the polyamide matrix. In situ characterization revealed that defect-engineered and gel-state UiO-66-NH 2 enhanced the membrane's positive surface charge and formed a “spinal-like” microstructure. Under the optimal acid ratio, the nanoparticles promoted higher polyamide cross-linking, reducing the average effective pore size from 0.54 to 0.46 nm, enabling synergistic control of both physical and chemical membrane properties. With an applied electric field, monovalent ion dehydration and migration were accelerated, enhancing ion decoupling and achieving a separation factor of 83.87 for Li + /Mg 2+ at an applied current of 6 mA. This work demonstrates a triple synergistic mechanism involving interface regulation, structural optimization, and electric-field coupling, highlighting the pivotal role of gel-state defect-engineered MOFs in tuning membrane microstructure and surface charge. This finding provides new theoretical guidance and design strategies for efficient lithium recovery using electric-field assisted functional nanofiber membranes.
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高影响因子
ACS Nano
·
2025
·
IF 16
Yu Cheng,Lulu Du,Xiaowei Liu,Hong Zhang,Xidan Xiao,Xinkuan Hu,Guangyao Dong,Yingkui Yang,Lin Xu
Rapid Li+ transport channels in composite solid electrolytes (CSEs) are often attributed to organic–inorganic interfaces. However, slow Li+ transport through polymer chains is still dominant due to inefficient interface construction and weak interface interactions. In this study, interface-dominated Li+ transport was achieved in ultracompatible CSEs by modifying sub-1 nm inorganic cluster chains (ICCs) with polyether amine (PEA). The abundant amino groups in PEA made ICCs monodisperse in the PVDF-HFP matrix and form hydrogen bonds with polymer chains. The distribution of organic–inorganic interfaces and interfacial hydrogen bonds was amplified by the multidimensional optimized interfaces. Moreover, the direction of −CF2– groups was regulated by the hydrogen bonds to provide rich and continuous interface interaction sites and local charge accumulation regions for more free Li+ and more Li+ transport pathways, thereby making the Li+ interface transport dominant (52%) for the overall Li+ transport in CSEs. Consequently, the as-obtained composite solid electrolyte exhibits exceptional room temperature ionic conductivity (0.53 mS cm–1), a substantial Li+ transference number (0.65), and a stable cycling performance (95% capacity retention of NCM/Li batteries after 500 cycles at 0.5 C). This work introduces key concepts for the practical application of ICCs and outlines core design principles for composite solid electrolytes.
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PubMed
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Xiaoke Zhi,Jiahao Xu,Li Wang,Guangchuan Liang
The practical application of lithium manganese iron phosphate (LMFP) is hampered by its low electrical conductivity and poor Li+ diffusion kinetics. Herein, high-rate Li0.98Na0.02Mn0.6Fe0.4PO4/C cathode material has been prepared through ball milling, spray drying, and carbothermal reduction methods using glucose and PEG as carbon sources, along with a water-soluble dispersant maleic acid acrylic acid copolymer (MA-AA) and a zwitterionic surfactant dodecyl dimethyl betaine (BS-12). It is found that the addition of MA-AA can improve the grinding efficiency and reduce the viscosity of the ball-milled slurry, thereby leading to a smaller primary particle size with enhanced homogeneity. The unique structure of BS-12 makes its hydrophobic hydrocarbon chains adsorb and encapsulate raw material particles, increasing the compactness between particles. Meanwhile, the hydrophilic groups are oriented toward water, thereby enhancing the wettability between raw material particles and water-soluble carbon sources, which finally leads to the formation of a thin and uniform carbon coating layer. Therefore, the synergistic effect of MA-AA and BS-12 significantly reduces the primary particle size and improves the uniformity of the carbon layer, thereby enhancing the Li+ diffusion rate and electrical conductivity of the cathode material. The as-prepared sample exhibits discharge capacities of 159.1, 131.1, and 117.9 mAh g–1 at 0.2, 5, and 10 C rates, respectively, and a capacity retention rate of 97.02% after 200 cycles at 1 C. The cooperative use of a dispersant and a surfactant during the ball-milling process is an effective approach to enhance the high-rate capability and cycling stability of olivine-based cathode materials.
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PubMed
高影响因子
RUSSIAN JOURNAL OF ELECTROCHEMISTRY
·
2019
·Vol. 55
·期 10
·998-1008
·
IF 1.043
Chuanzhang Ge,Fan Zhenghua,Shen Long,Qiao Yongmin,Ling Licheng,Wang Jianming
A scalable synthesis of unique pyrolysis carbons from phosphorus-doped epoxyphenolics (EPN) through a facile curing and pyrolysis process is reported. The obtained carbons with a high pyrolysis yield of ca. 48% are investigated by SEM, TEM, XRD, Raman and nitrogen adsorption, and evaluated as anode for LIBs. The results show that the nanocrystal structure, proportion of defect sites and porosity (nanovoids) of the obtained carbons are highly dependent on pyrolysis temperature, thus affecting their electrochemical properties. The EPN carbon pyrolyzed at 900°C (EPN900) delivers the largest reversible capacity of nearly 420 mA h g –1 at 0.1 C, which is higher than the theoretical capacity of graphite, mainly resulting from lithium-ions insertion into the turbostratic nanosheets and absorption on defect sites. While the EPN carbon pyrolyzed at 2800°C (EPN2800) exhibits a balanced lithium storage performance with relatively large reversible capacity of 343 mA h g –1 , high initial coulombic efficiency (~86%), and superior cycling performance (299 mA h g –1 after 100 cycles at 0.3 C). This work provides a feasible solution for the large-scale preparation of high performance anode material and deepens the high-value utilization of the staple epoxy product.
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高影响因子
Science China-Materials
·
2017
·Vol. 60
·期 4
·304-314
·
IF 3.956
Zhu Kunlei,Sun Yinghui,Wang Rongming,Shan Zhongqiang,Liu Kai
High-tap density electrode materials are greatly desired for Li-ion batteries with high volumetric capacities to fulfill the growing demands of electric vehicles and portable smart devices. TiO 2 , which is one of the most attractive anode materials, is limited in their application for Li-ion batteries because of its low tap density (usually <1 g cm −3 ) and volumetric capacity. Herein, we report uniform mesoporous TiO 2 submicrospheres with a tap density as high as 1.62 g cm −3 as a promising anode material. Even with a high mass loading of 24 mg cm −2 , the TiO 2 submicrospheres have impressive volumetric capacities that are more than double those of their counterparts. Moreover, they can be synthesized with ~100% yield and within a reaction time of ~6 h by optimizing the experimental conditions and formation mechanism, exhibiting potential for large-scale production for industrial applications. Other mesoporous anode materials, i.e., high-tap density mesoporous Li 4 Ti 5 O 12 submicrospheres, are fabricated using the generalizedmethod. We believe that our work provides a significant reference for the industrial production of mesoporous materials for Li-ion batteries with a high volumetric performance.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2016
·Vol. 26
·期 37
·6797-6806
·
IF 11.382
Yue Ma,Reza Younesi,Ruijun Pan,Chenjuan Liu,Jiefang Zhu,Bingqing Wei,Kristina Edström
Pulverization of electrode materials and loss of electrical contact have been identified as the major causes for the performance deterioration of alloy anodes in Li-ion batteries. This study presents the hierarchical arrangement of spatially confining silicon nanoparticles (Si NPs) within graphene foam (GF) for alleviating these issues. Through a freeze-drying method, the highly oriented GF monolith is engineered to fully encapsulate the Si NPs, serving not only as a robust framework with the well-accessible thoroughfares for electrolyte percolation but also a physical blocking layer to restrain Si from direct exposure to the electrolyte. In return, the pillar effect of Si NPs prevents the graphene sheets from restacking while preserving the highly efficient electron/Li + transport channels. When evaluated as a binder-free anode, impressive cycle performance is realized in both half-cell and full-cell configurations. Operando X-ray diffraction and in-house X-ray photoelectron spectroscopy confirm the pivotal protection of GF to sheathe the most volume-expanded lithiated phase (Li 15 Si 4 ) at room temperature. Furthermore, a free-standing composite film is developed through readjusting the pore size in GF/Si monolith and directly integrated with nanocellulose membrane (NCM) separator. Because of the good electrical conductivity and structural integrity of the GF monolith as well as the flexibility of the NCM separator, the as-developed GF/Si-NCM electrode showcases the potential use in the flexible electronic devices.
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高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Ling Meng,Zhaoxia Sun,Guanghang Sun,Xiting Zhang,Meng Dan,Jin Long,Jian Hu
Herein, we reported that KOH impregnation can generate a large number of porous structures with fruitful nitrogen self-doped groups during the carbonized process for poly (p-phenylene terephthalamide) fiber and poly (p-phenylene benzobisoxazole) fiber (denoted as PPTA and PBO, respectively). The intrinsical insulation, volume change, and shuttle effect of polysulfides then can be more significantly improved for the PBO-coated separator than the PPTA case. The discharge capacity primary achieves 1,322 mA h/g, which retains 827 mA h/g even after 200 cycles at 0.2 C for the cell with PBO-coated separator. The reversible specific discharge capacity maintains 841 mA h/g with a Coulomb efficiency of 99.7% at 5 C. The nitrogen self-doped nanocarbon particles are etched by KOH with the simple one-step preparation, which has promising application as Li-S battery cathode.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 6
·2907-2916
·
IF 12.732
Qiyu Wang,Xiangqun Xu,Bo Hong,Maohui Bai,Jie Li,Zhian Zhang,Yanqing Lai
Quasi-solid-state lithium metal batteries hold great potential for use in next generation energy systems due to their high energy capacity and safety. However, these systems still suffer from incompatible interphases and limited cycling performance due to Li dendrite growth. Considering this, nonpolar triallyl cyanurate with a ring-centred –CN coupled structure with pentaerythritol tetraacrylate as a cross-linking agents was applied in the in situ synthesis of gel polymer electrolyte (GPE). The GPE displays high ionic conductivity (7.93 mS cm−1) at room temperature and high stability towards a Li metal anode. Furthermore, the micro-electric field created by triallyl cyanurate (TAC) after polymerization provides uniform adsorption sites for Li+ flow and induces even distribution, which ensures a long cycling life (700 cycles) with a capacity retention of 80.6% for a LiFePO4|GPE|Li battery at 1C. The design of the polymer skeleton provides new insights into solid-state battery optimization different from the intrinsic properties of the electrolyte. This polymeric electrolyte also allows for new opportunities to practically manufacture lithium metal batteries.
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高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.7
Zunqiu Xiao,Huaying Wang,Ningyuan Cai,Yutong Li,Kejia Xiang,Wei Wei,Tao Ye,Zhongtai Zhang,Shitong Wang,Zilong Tang
Anti-perovskite materials such as Li 2 (OH)Cl have garnered considerable interest as solid electrolytes due to their numerous advantages. However, the low ionic conductivity of the orthorhombic Li 2 (OH)Cl near room temperature presents a significant challenge for the application. In this study, we intricately modulate the −OH content in Li 2 (OH)Cl through a controlled heat treatment process. This method effectively increases the cubic phase content and lowers the phase transition temperature, thereby enhancing the ionic conductivity at 30 °C by more than an order of magnitude. Theoretical calculations illustrate that the removal of −OH content significantly reduces the barrier for phase transition, leading to substantial alterations in the Li-ion transport pathway and migration barrier. Furthermore, LiHClO-600 demonstrates exceptional resistance to lithium reduction and is compatible with lithium metal and LiFePO 4 , rendering it a viable solid electrolyte for batteries. Both experimental findings and theoretical calculations cohesively highlight the pivotal role of −OH content in driving phase transition and facilitating Li-ion transport in anti-perovskite solid electrolytes, paving the way for their potential utilization in all-solid-state batteries.
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高影响因子
Small
·
2023
·Vol. 20
·期 14
·2308279
·
IF 13.3
Weishang Jia,Junxian Chen,Zihao Wang,Aijun Zhou,Yong-Sheng Hu,Jingze Li
The development and application of lithium (Li) anode is hindered by volumetric variation, dendritic Li growth, and parasitic reactions. Herein, a dual-phase Li-barium (Ba) alloy with self-assembled microchannels array is synthesized through a one-step thermal fusion method to investigate the inhibition effect of lithiophilic composite porous array on Li dendrites. The Li-rich Li-Ba alloy (BaLi24) as composite Li electrode exhibits an ordered porous structure of BaLi 4 intermetallic compound after delithiation, which acts as a built-in 3D current collector during Li plating/striping process. Furthermore, the lithiophilic BaLi 4 alloy scaffold is a mixed conductor, featuring with Li + ions diffusion capability, which can efficiently transport the reduced Li to the interior of the electrode structure. This unique top-down growth mode can effectively prohibit Li dendrites growth and improve the space utilization of 3D electrode structure. The spin-polarized density functional theory (DFT) calculations suggest that the absorption capability of BaLi 4 benefits the deposition of Li metal. As a result, the cell performance with the dual-phase Li-Ba alloy anode is significantly improved.
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高影响因子
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