ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chenxi Gao,Xiao Xu,Tiansheng Bai,Jun Cheng,Zhen Zeng,Hongqiang Zhang,Naixuan Ci,Wei Zhai,Qing Ma,Jingyu Lu,Jun Ma,Lijie Ci,Deping Li
Nickel-rich layered oxide with high reversible capacity and high working potentials is a prevailing cathode for high-energy-density all-solid-state lithium batteries (ASSLBs). However, compared to the liquid battery system, ASSLBs suffer from poor Li-ion migration kinetics, severe side reactions, and undesired formation of space charge layers, which result in restricted capacity release and limited rate capability. In this work, we reveal that the capacity loss lies in the H2–H3 phase transition period, and we propose that the inconsistent interfacial Li-ion migration is the arch-criminal. We introduce Si doping to stabilize the bulk structure and Li4SiO4 fast ionic conductor coating to regulate the interfacial behaviors between the Ni-rich cathode and sulfide-based solid electrolyte Li6PS5Cl. The modified NCM@LSO-2||LPSCl||Li–In ASSLBs deliver a high reversible capacity of 183.5 mA h g–1 at 0.1C, 30.3% higher than the bare NCM811 electrode. Besides, the interfacial regulation strategy enables the operation at a high rate of 5.0C and achieves a high capacity retention ratio of ∼85.8% after 500 cycles at 1.0C. Furthermore, the underlying mechanisms are well investigated through kinetic analyses and theoretical simulations. This work provides an in-depth understanding on the interfacial degradations between Ni-rich cathodes and sulfide-based all-solid-state electrolytes from the view of kinetic limitations and offers potential solutions.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qiao Zhang,Chunxi Hai,Yanxia Sun,Yunyun Gao,Shengde Dong,Luxiang Ma,Xin He,Qi Xu,Yuan Zhou
How to effectively recover Li + from liquid mineral brines with high Mg 2+ /Li + ratio and low Li + concentration is very significant and important for promoting the carbon peak and carbon neutrality plan valid. Therefore, taking the application merits and formation scheme into consideration, well-crystallized β-Li 2 TiO 3 precursors for obtaining TiO 2 ⋅H 2 O adsorbents were prepared through a classical solid-phase method under the optimized conditions. Interestingly, both Li + desorption and titanium dissolution loss ratio of TiO 2 ⋅H 2 O adsorbents depend on the HCl concentration and delithiation temperature. The Li + escaping routes from LTO precursors to TiO 2 ⋅H 2 O adsorbents is dramatically distinctive with that in the next adsorption/desorption cycles. Accordingly, as-prepared TiO 2 ⋅H 2 O adsorbents owns the high adsorption capacity up to 51.25 mg/g at 60 °C and low Ti-dissolution loss ratio around 1.08 %. The initial adsorption capacity of TiO 2 ⋅H 2 O adsorbents in real original oil–gas field brines containing 100 ppm Li + is 20.14 mg/g. According to the structure–property relationship, formation and working mechanisms of TiO 2 ⋅H 2 O adsorbents was proposed.
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ACS Nano
·
2024
·
IF 15.8
De-Hui Guan,Xiao-Xue Wang,Cheng-Lin Miao,Jia-Xin Li,Jian-You Li,Xin-Yuan Yuan,Xin-Yue Ma,Ji-Jing Xu
High-energy lithium (Li)-based batteries, especially rechargeable Li–CO2 batteries with CO2 fixation capability and high energy density, are desirable for electrified transportation and other applications. However, the challenges of poor stability, low energy efficiency, and leakage of liquid electrolytes hinder the development of Li–CO2 batteries. Herein, a highly conductive and stable metal–organic framework-encapsulated ionic liquid (IL@MOF) electrolyte system is developed for quasi-solid-state Li–CO2 batteries. Benefiting from the host–guest interaction of MOFs with open micromesopores and internal IL, the optimized IL@MOF electrolytes exhibit a high ionic conductivity of 1.03 mS cm–1 and a high transference number of 0.80 at room temperature. The IL@MOF electrolytes also feature a wide electrochemical stability window (4.71 V versus Li+/Li) and a wide working temperature (−60 °C ∼ 150 °C). The IL@MOF electrolytes also enable Li+ and electrons transport in the carbon nanotubes-IL@MOF (CNT-IL@MOF) solid cathodes in quasi-solid-state Li–CO2 batteries, delivering a high specific capacity of 13,978 mAh g–1 (50 mA g–1), a long cycle life of 441 cycles (500 mA g–1 and 1000 mAh g–1), and a wide operation temperature of −60 to 150 °C. The proposed MOF-encapsulated IL electrolyte system presents a powerful strategy for developing high-energy and highly safe quasi-solid-state batteries.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Chengdong Fang,Yuhang Zhang,Yixuan Li,Pengfei Sun,Liping Cui,Jiajia Chen
Polymer electrolyte is an attractive material for constructing high-performance solid-state batteries. However, the overall low room-temperature ionic conductivity and low transference number impede the practical application of polymer electrolyte. Ion-dipole interaction, as non-covalent interactions, has the potential to regulate Li + coordination. It will contribute to the selectivity filter of ion conduction and improve overall ion conduction performance. Herein, we introduced benzene sulfonamide (BS) and N-methylbenzenesulfonamide (NBS) into PEO-LiTFSI complexes, respectively. The ion-dipole interactions of Li···-N-H might be provided by the organic molecules. Due to the difference in the molecular structure between BS and NBS, the stronger ion-dipole interactions between NBS and Li + could significantly improve the coordination of Li + . As a result, PEO-LiTFSI-NBS delivers an extraordinary ionic conductivity of 1.08 × 10 −4 S cm −1 at 30 °Ϲ and a high lithium ion transference number of 0.77. When employed in assembling LiFePO 4 |Li solid-state battery, the specific discharge capacity could reach 151.90 mAh g −1 with a high coulombic efficiency of around 99.92 % at 50 μA cm −2 (35 °Ϲ).
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RARE METALS
·
2024
·Vol. 43
·期 8
·3634-3646
·
IF 9.6
He Pu-Qiang,Guo Jun,Huang Hui,Guo Zhong-Cheng
Bismuth-based anode materials have been regarded as promising Li-ion batteries due to their high theoretical capacity. However, their low conductivity and associated volume expansion inhabited their commercialization. In this work, Bi 2 O 2 CO 3 @C composites were successfully synthesized by in situ anchoring of flower-like Bi 2 O 2 CO 3 nanosheets on a carbon-based substrate via hydrothermal. The unique composited structure of Bi 2 O 2 CO 3 @C leads to a stable specific capacity of 547 mAh·g −1 after 100 cycles at a current density of 0.1 A·g −1 . Notably, it demonstrates excellent rate capability with a specific capacity of 210 mAh·g −1 at 5 A·g −1 . After 550 cycles at a current density of 0.5 A·g −1 , a high reversible capacity of nearly 400 mAh·g −1 was observed. Additionally, in situ X-ray diffraction measurements clearly demonstrate the conversion between Bi and Li 3 Bi during alloying/dealloying, confirming the good electrochemical reversibility of the materials for Li storage. The reaction kinetics of Bi 2 O 2 CO 3 @C were further investigated using galvanostatic intermittent titration technique. Furthermore, Bi 2 O 2 CO 3 @C exhibited excellent long-term stability, maintaining its high reversible capacity for over 200 cycles at a current density of 0.5 A·g −1 in a full cell configuration using Li 1.20 Mn 0.54 Ni 0.13 Co 0.13 O 2 as the cathode material. This result further underscores its promising potential for lithium-ion batteries. This work may provide inspiration for the design of alloy-type negative electrode materials for high-performance rechargeable batteries. Graphical abstract
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Processes
·
2025
·Vol. 13
·期 1
·232
·
IF 2.8
Jiulong Che,Jian Zhang,Qing Lang,Jiayuan Yu,Yixiao Yang,Longqi Luo,Zhiyi Liu,Jiahui Ye,Gang Wang
Dual-ion batteries (DIBs) were demonstrated as a promising technology for large-scale energy storage due to their low cost, recyclability, and impressively fast charge capability. Graphite as a commonly used cathode material in DIBs, however, suffers from poor compatibility with commercial Li-ion electrolytes and graphite anodes, making it difficult to directly utilize the well-established infrastructure for Li-ion batteries. Herein, we report a small aromatic amine molecule 4,4′,4″-tris(diphenylamino)triphenylamine (N4) functioning as a compatible anion host in the EC-containing Li-ion electrolyte. With an average discharge voltage of 3.6 V (vs. Li+/Li), the N4 electrode delivers a reversible specific capacity of 108 mAh/g, which is much higher than 29 mAh/g for the graphite cathode at the same condition. The high capacity retention of 91.3% was achieved after 500 cycles at 1 A/g. The N4 electrode also exhibited good rate performance. Via different characterization techniques like Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy, the energy storage mechanism of N4 was revealed as a conversion between amine and quaternary amine cations, accompanied by PF6−(de-)insertion. As consequences, the assembled N4||graphite DIB w showed a high discharge capacity of 90 mAh/g within 1.5–4.1 V, and good cycling stability with a 98% capacity retention after 40 cycles. Decent rate performance was achieved in the N4||graphite DIB as well. This work provides new insights into designing a compatible anion host for affordable DIBs.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Li Qin,Haifeng Yu,Hujun Zhang,Qilin Cheng,Ling Chen,Hao Jiang
All-dry solid-phase synthesis (ADSPS) is considered an eco-friendly and cost-effective method for preparing Ni-rich Co-poor cathodes, yet slow ion diffusion during the solid-phase sintering process results in agglomerate particles with severe Li/Ni mixing. Herein, a Mg/Sr-codoped and ZrO2-coated single-crystalline LiNi0.73Co0.05Mn0.22O2 cathode with a well-layered structure is fabricated through the ADSPS method. The Sr ions effectively accelerate the ion migration at the grain boundary to facilitate particle coarsening, while the Mg ions act as “pillar ions” to decrease the Li/Ni mixing and improve the structural stability. Moreover, the ZrO2 coating layer can further alleviate the interfacial side reactions to hinder the structure degradation and enhance the particle integrity. Therefore, the resultant single-crystalline cathodes deliver a high reversible capacity of 192.4 mAh g–1 and display an impressive retention of 87.5% after 300 cycles at 0.5 C in a pouch-type full cell. The ADSPS strategy in this work shows great potential for the synthesis of single-crystalline Ni-rich ternary cathodes for Li-ion batteries.
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Nano Energy
·
2024
·
IF 16.8
Shuwei Wang,Jianxun Zhang,Lihan Zhang,Xia Hu,Xianying Qin,Xinping Yan,Zile Wang,Xuewei Lu,Yan Xin,Feiyu Kang,Huajun Tian,Baohua Li
Three-dimensional (3D) porous hosts play pivotal roles in realizing dendrite-free lithium metal anodes (LMAs) owing to their high specific area. However, uneven local electric field and lack of lithiophilic sites on the reactive interface cause nonuniform lithium ion (Li + ) deposition, leading to Li dendrite growth and parasitic reactions. These issues will inevitably incur short cycling life and severe safety hazards of lithium metal batteries . Herein, a 3D self-supporting host composed of hollow carbon nanofibers incorporated with silicon (Si) nanoparticles inside (Si-HCF) is constructed as Li metal host by a scalable coaxial electrospinning technique . During the first cycle, the Si nanoparticles is alloyed with Li + to form lithiophilic Li-Si alloy, contributing to deliver a low nucleation overpotential and homogeneous surface potential confirmed by Kelvin probe force microscopy, finally guiding Li + flux homogeneously throughout the fibrous mat. As expected, the Li metal can percolate through Si-HCF host reversibly without uncontrollable Li dendrites and the Si-HCF exhibits a stable cycle life of Li plating/stripping over 1400 h. Additionally, the full cell combined with LiFePO 4 cathodes presents steady cycling over 400 cycles with a high average coulombic efficiency of 99.4 %. This work provides new insights for the synthesis of 3D hosts with controllable nucleation sites to homogenize Li + deposition in LMAs.
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NEW JOURNAL OF CHEMISTRY
·
2025
·Vol. 49
·期 7
·2962-2972
·
IF 2.5
Jiahe Li,Fang Du,Changsheng Tang,Luyang Wang,Yulin Yang,Debin Xia,Jian Zhang,Bowen Tao,Ping Wang,Kaifeng Lin
Al–Li alloys are considered promising materials in solid propellants owing to their higher combustion efficiency than Al particles, which exhibit incomplete combustion. However, Al–Li alloy particles cannot be directly applied in propellant systems owing to their poor compatibility. Thus, in this work, an in situ polymerized film was formed via the pretreatment of Al–Li alloy followed by polymerization with trifluoroethyl methacrylate (TFEMA) and N,N′-methylene-bis-acrylamide (MBA). The hydrothermal stability of the coated samples was improved with a mass variation rate of 5.82% on treatment with TFEMA (30%) and MBA (10%), corresponding to 116.62% of Al–Li at 60 °C and 75% humidity for 30 days. Besides, the thermostability increased based on the 19° backward skewing of the high temperature exothermic peak. Meanwhile, there were no pores and cracks in the HTPB propellant, which proved the possibility of its practical application with the compatibility of level 1 with HTPB in solid rocket motors. In addition, the Al–Li propellant exhibited a better combustion performance of 0.53 s and 1309.33 °C than the Q3 Al propellant, with 1.34 s ignition delay time and 990.24 °C burning temperature. The combustion efficiency was also improved based on the observation of combustion phenomena and residue size. Besides, the combustion mechanism was analyzed based on the characteristics of Al–Li with the micro-explosion effect. Therefore, Al–Li alloy has the potential to be used as a new generation solid propellant.
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Micromachines
·
2024
·Vol. 15
·期 7
·828
·
IF 3
Ji Li,Yu Wang,Xinyuan Pei,Chunhe Zhou,Qing Zhao,Ming Lu,Wenjuan Han,Li Wang
The ZnMn2O4/V2CTxcomposites with a lamellar rod-like bond structure were successfully synthesized through high-temperature calcination at 300 °C, aiming to enhance the Li storage properties of spinel-type ZnMn2O4anode materials for lithium-ion batteries. Moreover, even though the electrode of the composites obtained at 300 °C had a nominal specific capacity of 100 mAh g−1, it exhibited an impressive specific discharge capacity of 163 mAh g−1after undergoing 100 cycles. This represents an approximate increase of 64% compared to that observed in the pure ZnMn2O4electrode (99.5 mAh g−1). The remarkable performance of the composite can be credited to the collaborative impact between ZnMn2O4and V2CTx, leading to a substantial improvement in its lithium ion storage capacity. Therefore, this study offers valuable insights into developing cost-effective, safe, and easily prepared anode materials.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jianjun Zhao,Jun Chen,Miaomiao Zhou,Qian Zhang,Xiaocheng Li,Junqing Pan
The enormous volume change of silicon (Si) leads to pulverization of Si electrodes and continuous growth of solid-electrolyte-interphase (SEI) layers on the Si surface, for which we report a new Si anode material (PMDA-NiPc@Si) with a homogeneous and tetragonal covalent organic frameworks (COFs) coating on the surface of nano-Si particles. COFs with tetragonal structures have higher stability than other structures, which helps to increase the long cycle life of the electrodes. The strong constraining buffering effect of the coating layer can fully inhibit and buffer the volume change of Si nanoparticles during charging-discharging, reduce the consumption of electrolytes and form a homogeneous, stable and robust, LiF- and LiN-rich SEI film, and ultimately improve the rate performance and long-cycle performance. The pre-lithiation of PMDA-NiPc@Si shows a superior lithium ion conductivity that can enhance the lithium ion transport kinetics of silicon electrodes and significantly improve the initial coulomb efficiency (ICE). PMDA-NiPc@Si exhibits excellent specific capacity and cycling performance, with a capacity retention rate of 93.8 % after 100 cycles, which is 2.7 times higher than that of nano-Si. It also offers a high reversible capacity of 654 mAh/g and a capacity retention rate of 80.4 % after 2000 cycles at 5 A/g. The assembled full battery with PMDA-NiPc@Si anode and NCM811 cathode displayed a specific capacity of 175.8 mAh/g with a retention rate of 85.8 % after 100 cycles at 0.2C. The PMDA-NiPc@Si electrode shows only about 44 % of the expansion rate (21.6 to 31.1 μm), which is only 27.3 % of that of the Si electrode . PMDA-NiPc@Si anodes show significantly enhanced electrochemical performance, which will provide novel ideas for the development of high-performance Li-ion batteries.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Wubin Wang,Jin Wang,Yufei Yan,Kaili Huo,Chao Han,Qingyun Zhang
The positively charged nanofiltration (NF) membrane prepared via interfacial polymerization (IP) of polyethyleneimine (PEI) and trimesoyl chloride (TMC) has drawn considerable attention for lithium-magnesium separation, particularly crucial for lithium recovery from salt lakes with high Mg 2+ /Li + mass ratios. However, NF membranes prepared solely from amine monomers have not achieved efficient Li + and Mg 2+ separation. In this study, PEI-g-C 3 N 5 /TMC composite NF membranes were successfully fabricated by mixing amino-rich graphitic carbon nitride (g-C 3 N 5 ) with PEI, followed by the IP reaction of the mixed solution with TMC. Molecular dynamics (MD) simulation results showed that g-C 3 N 5 had an attractive effect on PEI, which led to a decrease in the diffusion rate of PEI, thereby resulting in a thinner separation layer. Density functional theory (DFT) revealed that g-C 3 N 5 competed with PEI, leading to a reduction in the crosslinking within the polyamide (PA) layer and subsequently causing an increase in the surface pore size of the membrane. Besides, the hydrophilicity and positive charge of the modified membrane were both improved. MD simulations, transition state theory, and DLVO principles indicated that the modification of the PA layer by g-C 3 N 5 enhanced the repulsion of Mg 2+ and the transport of Li + during the NF process. This breakthrough effectively overcame the trade-off effect between membrane separation and permeability, especially at a g-C 3 N 5 content of 0.06 wt%, where the lithium-magnesium selectivity coefficient ( S Li, Mg = 18.18) and pure water flux (Flux = 58.59 L m −2 h −1 ) reached the optimum values. Meanwhile, the PEI-g-C 3 N 5 /TMC membrane demonstrated stable separation performance during prolonged filtration and in solutions with varying Mg 2+ /Li + mass ratios. This study not only provides an effective strategy for the design of NF membranes but also expands the application prospects of nanomaterials in the field of membrane separation.
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