EUROPEAN POLYMER JOURNAL
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2025
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IF 6.3
Shanshan Gao,Wenshuo Wang,Dayang Yu,Pengju Pan,Yongzhong Bao
All-solid-state lithium metal batteries (ASSLMBs) are considered as next-generation energy storage devices due to their high specific energy density and safety, and solid polymer electrolytes (SPEs) are an important component of ASSLMBs. Poly(ethylene oxide) (PEO) is the most prevalent matrix of SPE but is criticized for its poor mechanical properties and a narrow electrochemical stability window. To address this issue, poly(vinylidene fluoride)- b- poly(poly(ethylene glycol) methyl ether methacrylate (PVDF- b- PPEGMA) copolymer fibers with an ivy-like morphology were prepared by electrospinning and used to support PEO/lithium salt electrolytes. The electrospun PVDF- b- PPEGMA copolymer fiber membrane provides an uncial hierarchical structure with large pore size, good compatibility and adhesion with PEO due to side ethylene oxide units in the PPEGMA segment. The ivy-like fibers supported SPE exhibited good thermal stability and high mechanical strength. Furthermore, ASSLMBs assembled using the above SPE, LiFePO 4 cathode, and lithium metal anode possessed a wide electrochemical stable window (5.58 V vs. Li/Li + ) and good initial discharge capabilities at 60 °C.
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高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Bin He,Yujie Dai,Shuai Jiang,Dawei Chen,Xilong Wang,Jie Song,Dan Xiao,Qian Zhao,Yan Meng,Wei Feng
Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structural degradation of high energy-density Li-rich layered oxide (LLO), leading to voltage and capacity fading. Herein, the dual-strategy of Cr x B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature. Density functional theory (DFT) calculations prove that stable B–O and Cr–O bonds through the local gradient doping can significantly reduce the high-energy O 2 p states of interfacial lattice O, which is also effective for the near-surface lattice O, thus greatly stabilizing the LLO surface. Besides, differential electrochemical mass spectrometry (DEMS) indicates that the Cr x B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions, including allowing speedy Li + migration. The voltage and capacity fading of the modified cathode (LLO-CrB) are adequately suppressed, which are benefited from the uniformly dense cathode electrolyte interface (CEI) composed of balanced organic/inorganic composition. Therefore, the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g −1 (with a retention rate of 95.1%). This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.
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JOURNAL OF POWER SOURCES
·
2024
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IF 8.1
Lu Sai,Zhongsheng Dai,Zhenbo Wang,Huiling Zhao,Ying Bai
Li-rich layered oxides with high energy densities have become one kind of promising cathode for advanced lithium-ion batteries, however some issues are severely hindering their practical applications. To address these challenges, fast ion conductive LiTi 2 (PO 4 ) 3 (LTPO) is employed to modify the typical Li-rich cathode Li 1 · 2 Mn 0 · 56 Ni 0 · 17 Co 0 · 07 O 2 (LMNCO) via a sol-gel process combined with a two-step annealing treatment in this work. Serving as a physical separator, LTPO coating effectively depresses the side reactions at cathode-electrolyte interface and the transition-metal dissolution from LMNCO active material under harsh electrochemical environment. Meanwhile, LTPO layer with high ion conductivity could facilitate the interfacial Li + diffusion during charge/discharge process. In addition, partial Ti 4+ ions doped into LMNCO effectively elevate the oxygen electronegativity and restrain the excessive oxidization of lattice oxygen, thus stabilizing the crystal structure and alleviating the stress-strain propagation upon cycling. Electrochemical characterization results demonstrate that the LTPO-modified LMNCO cathode exhibits a superior capacity retention of 86.5 % after 400 cycles at room temperature and that of 73.7 % even under an elevated temperature of 45 °C after 250 cycles under 1C. This study provides a facile strategy for the surface modification of Li-rich layered-structure oxides, which also sheds light in enhancing electrochemical performances for various cathode materials .
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Tao Huanga,Lifeng Guan,Shuai Jin,Dehui Zhang,Wangwen Liao,Xiangyang Zhou,Xingxing Liu,Chen Wu,Wei Zeng
The low electrical conductivity of Li 3 V 2 (PO 4 ) 3 (LVP) impedes its practical application. To address this issue, this study enhances its conductivity by introducing nitrogen-doped carbon nanoframes into LVP. Using phytic acid as a carbon and phosphorus source, and polyvinylpyrrolidone (PVP) as a nitrogen source, nitrogen-doped nanoframe-modified LVP material (LVP@NC) was successfully synthesized. Importantly, the carbon nanoframes of LVP@NC are entirely derived from the precursor’s thermal decomposition, simplifying the synthesis process and reducing production costs. By optimizing the process parameters, significant improvements were achieved in key performance indicators, including the initial discharge capacity at 1C (132.85 mAh·g −1 ), long cycling life at 10C (98.98 % capacity retention after 1000 cycles), and rate capability at 50C (99.65 mAh·g −1 ). These improvements are attributed to the introduction of nitrogen-doped nanoframes, where the high-temperature decomposition of PVP leads to the formation of porous honeycomb-like structures, and nitrogen doping in the nanocarbon framework introduces defects and active sites, thereby promoting lithium-ion migration and facilitating electrolyte penetration. This simple, novel, and energy-efficient method demonstrates significant potential for the large-scale preparation of high-performance cathode materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Yipeng Yang,Yanting Ma,Kaineng Feng,Songsheng Zheng,Zhaolin Wang
Semi-solid electrolytes tend to inherit the advantages of both solid-state electrolytes and liquid electrolytes. However, the challenge is to simultaneously enhance both ionic conductivity, transference number and long cycle performance of batteries. In this study, a semi-solid electrolyte was successfully synthesized with a hollow structured metal organic framework (HMOF) and a polymer binder (PVDF). The hollow structure of HMOF serves as a framework to encapsulate a large amount of lithium salt and electrolyte, reducing concentration polarization in lithium metal batteries. Its unique pore structure and abundant hydroxyl functional groups can restrict anion movement, thereby increasing the Li-ion transference number. On the other hand, the PVDF acts as a binder, making the electrolyte thinner, more flexible, and easier to process for broader applications. Furthermore, a Li@HMOF semi-solid electrolyte (LHMSSE) was fabricated by adding Bis (trifluoromethane) sulfonimide lithium salt (LiTFSI) into the HMOF(Li@HMOF), which exhibits a high ionic conductivity of 0.89 mS cm −1 at 30 °C and a high Li-ion transference number of 0.75 at 30 °C. Notably, the Lithium symmetric battery of Li||LHMSSE ||Li can operate stably for over 1200 h at a current density of 0.2 mA cm −2 , and the lithium metal full battery of Li||LHMSSE||LFP (LiFePO 4 ) retains a capacity of 127.7 mAh g −1 after 2000 cycles at 1C, with a capacity retention rate of 89.1 % and an average coulombic efficiency of 99.9 %. When paired with high-load LFP (10 mg cm −2 ) or NCM811 (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ) (10 mg cm −2 ) cathodes, a stable cycling performance can be achieved at a rate of 0.2C.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Xingwen Lu,Yue He,Zebiao Huang,Jiating Li,Zenghua Qi,Jianqiao Qin,Fei Wang
Addressing the escalating volume of retired lithium-ion batteries (LIBs) is crucial for protecting the environment and minimizing resource wastage. In this study, Li 2 CO 3 and NCM 111 carbonate precursor ((Ni 1/3 Co 1/3 Mn 1/3 )CO 3 ) were successfully generated from the retired ternary LIBs through a combined process of thermal reduction and carbonate precipitation. During the thermal reduction process, graphite interacted with the cathode material (LiNi 0.5 Co 0.2 Mn 0.3 O 2 ) from used LIBs, facilitating the conversion of Li from its LiO x polyhedral structure into Li 2 CO 3 . Simultaneously, the transition metals within LiNi 0.5 Co 0.2 Mn 0.3 O 2 were transformed into Ni (0) , Co (0) , and MnO. Under optimal conditions, a graphite/LiNi 0.5 Co 0.2 Mn 0.3 O 2 mass ratio of 0.15/1 was sintered at 750 °C for 120 min, resulting in the recovery of 98.7% Li as Li 2 CO 3 with a purity of 99.65% through water leaching and evaporation. After isolating Li as Li 2 CO 3 from spent NCM, the residue was dissolved and co-precipitated as NCM111 carbonate precursor ((Ni 1/3 Co 1/3 Mn 1/3 )CO 3 ) using ammonium complexing agents, with recovery ratios of 98.4%, 99.4%, and 99.7% for Ni, Co and Mn, respectively. The recovered precursors exhibited spherical morphology and rhodochrosite crystal structure. These results offer valuable insights into recycling valuable metals from used NCM batteries, thereby promoting the sustainability of the new energy industry.
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Journal of Energy Chemistry
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2025
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IF 14.9
Xingxing Zhang,Weihao Shi,Qingmei Su,Zemin He,Liming Wang,Xinglong Deng,Dequn Zhao,Rui Yan,Jinqi Chen,Hongli Chen,Zongcheng Miao,Wenhuan Huang
Solid-state lithium metal batteries (SSLMBs) face critical challenges from dendrite growth and unstable interfaces. While composite polymer electrolytes (CPEs) offer promise, poor ionic conductivity (<10 −5 S cm −1 ), low Li + transference numbers ( t Li+ < 0.5), and inadequate interfacial stability limit practical application. Herein, we design a dual-channel metal-organic framework (MOF)-based CPEs that simultaneously regulate ion transport and construct a high-conductivity interphase. This MOF features two distinct channels. The one imposes spatial confinement (0.57 nm in pore size) to suppress anion migration (TFSI − ), while the other facilitates immobilizing TFSI − through iodine-mediated nucleophilic substitution. More importantly, the liberated I − reacts with Li + to in situ generate lithium iodide (LiI)-enhanced solid-electrolyte interphase (SEI), replacing insulating LiF-rich counterparts. This LiI-SEI exhibits superior ionic conductivity and homogenizes Li + flux to suppress dendrites. Integrated into a poly(vinylidene fluoride)-cohexafluoropropylene (PVDF-HFP) matrix, the MOF CPE achieves exceptional ionic conductivity (2.13×10 −4 S cm −1 ) and a high t Li+ of 0.95 (25 °C). Density functional theory and molecular dynamics calculations verify ion-regulation mechanisms. As a result, LiFePO 4 //Li cells retain 94.99% capacity after 800 cycles (1 C), while NCM811//Li cells demonstrate sustained stability over 200 cycles. This work provides valuable insights into the design of multifunctional MOF ionic conductors for high-performance SSLMBs.
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Energy Storage Materials
·
2022
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IF 20.831
Jiaqi Zhu,Dan Cai,Jingru Li,Xiuli Wang,Xinhui Xia,Changdong Gu,Jiangping Tu
Optimization of lithium metal anode is a pivotal part in facilitating the evolution of next-generation high energy density solid-state lithium metal batteries (LMBs). However, the practical application of lithium anode in solid-state LMBs is limited by uncontrollable dendrite growth and the poor interfacial contact with solid electrolyte. Herein, a 40 µm thin lithium composite anode based on the AlN-embedded reduced graphene oxide (rGO) scaffold synthesized via one-step molten lithium infusion is proposed. The resulting lithiophilic Li-Al alloy and high ion-conductive Li 3 N in situ constructed the lithium ion diffusing highways inside electrode, enabling a well-oriented Li deposition and effectively inhibiting the dendrite growth. Combined with in-situ polymerization and Li 3 N-modified solid electrolyte interphase (SEI), the composite anodes can prolong the lifespan of symmetric cell to 2100 h at 0.2 mA cm −2 /0.2 mAh cm −2 in carbonate-based solid polymer electrolytes. Moreover, LAG||LiFePO 4 full cells also excelled in cycling capability and rate performance. This modified electrode offers a promising synergistic solution for designing high-performance solid-state LMBs.
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Advanced Science
·
2024
·Vol. 11
·期 30
·2404307
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IF 14.3
Shiyuan Guo,Yuefeng Su,Kang Yan,Chenying Zhao,Yun Lu,Haoyu Wang,Jinyang Dong,Ning Li,Yun Liu,Yibiao Guan,Feng Wu,Lai Chen
Constructing composite solid electrolytes (CSEs) integrating the merits of inorganic and organic components is a promising approach to developing high-performance all-solid-state lithium metal batteries (ASSLMBs). CSEs are now capable of achieving homogeneous and fast Li-ion flux, but how to escape the trade-off between mechanical modulus and adhesion is still a challenge. Herein, a strategy to address this issue is proposed, that is, intercalating highly conductive, homogeneous, and viscous-fluid ionic conductors into robust coordination laminar framework to construct laminar solid electrolyte with homogeneous and fast Li-ion conduction (LSE-HFC). A 9 µm-thick LSH-HFC, in which poly(ethylene oxide)/succinonitrile is adsorbed by coordination laminar framework with metal–organic framework nanosheets as building blocks, is used here as an example to determine the validity. The Li-ion transfer mechanism is verified and works across the entire LSE-HFC, which facilitates homogeneous Li-ion flux and low migration energy barriers, endowing LSE-HFC with high ionic conductivity of 5.62 × 10 −4 S cm −1 and Li-ion transference number of 0.78 at 25 °C. Combining the outstanding mechanical strength against punctures and the enhanced adhesion force with electrodes, LSE-HFC harvests uniform Li plating/stripping behavior. These enable the realization of high-energy-density ASSLMBs with excellent cycling stability when being assembled as LiFePO 4 /Li and LiNi 0.6 Mn 0.2 Co 0.2 O 2 /Li cells.
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CHEMPHYSCHEM
·
2025
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IF 2.2
Yu Chen,Zhenghui Liu,Zheng Li,Yanlong Wang,Qi Liu,Minghui Feng
Achieving high metal leaching efficiency via regulation strategy is essential for minimizing raw material waste and reducing waste generation in hydrometallurgy. However, conventional approaches of tuning temperature and time frequently result in increased equipment corrosion and increased industrial costs. Therefore, recycling waste solid-state battery relies on the development of new tuning strategies. Here, a new strategy is developed to tune the leaching efficiency of metals by amino acid-based low-melting mixture solvents from lithium aluminum titanium phosphate Li 1.3 Al 0.3 Ti 1.7 P 3 O 12 (LATP) in all-solid-state lithium-ion batteries. This novel strategy demonstrates a more pronounced metal leaching efficiency, resulting in an increase in the highest Li leaching efficiency from 48.0% to 78.2%. In comparison, tunability by solvent types, temperature, and time on Li efficiency is less efficient, with Li efficiency only varying from 44.9% to 52.3%, 37.7% to 51.0%, and 36.8% to 56.3%, respectively. Graphical A new and sustainable strategy is developed to tune the recycling of solid electrolyte LATP by adjusting ternary components in the biodegradable and biocompatible amino acid-based low-melting mixture solvents, achieving a significant increase in Li leaching efficiency from 48.0% to 78.2%, indicating a 1.6-fold enhancement.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Jie Zhou,Keying Cai,Tianci Zhou,Xiangfei Li,Yawen Li,Can Zhang,Zhuoyuan Zheng,Yusong Zhu
Li-dendrite growth and polysulfides shuttle are two core problems that restrict the applications of lithium-sulfur batteries (LSBs). Here, a double-layer-modified gel separator (DMS) is proposed to enable a shuttle-inhibition and dendrite-free quasi-solid-state LSB, where the polypropylene separator is sandwiched between an ultra-thin VS 2 layer (3 um) and a ceramic/polymer layer (6 um). On the cathode side, VS 2 layer can inhibit the polysulfides shuttle and boost their conversion kinetics. Meanwhile, on the anode side, the Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP)/PMMA/PVDF gel polymer electrolyte with the high-elastic-modulus and the homogenized Li-ion flux could effectively avoid dendrite growth. Last but not least, the quasi-solid-state LSB effectively prevents the evaporation of flammable ether-based electrolyte. Consequently, the quasi-solid-state-LSBs assembled with DMS show a high-capacity of 1197 mA h g −1 at 0.2 C and ultra-stable cycling performance over 800 cycles at 2 C with the decay rate of just 0.032% per cycle. Even with the high-sulfur-loading of 2.5 mg cm −2 , the LSB still delivers the high-capacity of 640.5 mA h g −1 at 2 C with stable cycling over 500 cycles. What's more, the assembled pouch cells still function properly even on the nail penetration and folding test, verifying the gel layer's integrity, and retention of electrochemical function under realistic conditions.
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Nanoscale
·
2020
·Vol. 12
·期 26
·14037-14046
·
IF 6.895
Shenghui Zheng,Junpeng Shi,Xiaoyan Fu,Chengcheng Wang,Xia Sun,Changjian Chen,Yixi Zhuang,Xiaoyan Zou,Yuechan Li,Hongwu Zhang
In this paper, we have designed long afterglow luminescent MgGeO3:Mn2+,Yb3+,Li+ (MGO) nanoparticles in the first (NIR-I) and second (NIR-II) biological windows. Yb3+ ions served not only as the trap center to enhance the NIR-I long afterglow emission of Mn2+ at 680 nm, but also as an emitting center to produce a NIR-II long afterglow emission at ∼1000 nm. Furthermore, we have found the addition of Li+ can greatly increase the NIR-II afterglow emission of Yb3+ and the optimal amount of Mn2+, Yb3+ and Li+ was found to be 0.1, 0.5 and 0.5 mol%, respectively. The MGO nanoparticles synthesized using sol–gel methods showed a uniform morphology with a diameter of 50–100 nm, which were suitable for applications in bioimaging. More importantly, we have found MGO nanoparticles can be effectively excited to produce long persistent NIR-I and II luminescence using soft X-rays, suggesting that low dosage soft X-rays can also serve as a more powerful and deep tissue excitation source to recharge MGO nanoparticles. Furthermore, the MGO nanoparticles can also be re-excited to produce photo-stimulated emission under the irradiation of 650 and 808 nm NIR lasers. The in vivo imaging results have shown that MGO nanoparticles modified with folic acid (FA) can effectively realize super long-term targeted in vivo imaging of inflammation with a high sensitivity via recharging using soft X-rays and NIR lasers, which can provide not only an accurate diagnosis of inflammation, but also long-term monitoring of possible changes in the focus of inflammation in real time.
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