JOURNAL OF POWER SOURCES
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2025
·
IF 7.9
Chuanwei Gao,Guohong Kang,Zengqi Zhang,Zheng Chen,Chuanchuan Li,Jianjun Zhang,Bingqian Zhang,Jie Lu,Yifan Gong,Qingfu Wang,Guanglei Cui
Uncontrollable lithium dendrites caused by the kinetic mismatch between the rapid Li + deposition and the sluggish Li + diffusion, exacerbating capacity degradation and safety risks in lithium metal batteries. The commercially available separator hardly regulates Li + migration due to its heterogeneous pores and inferior electrolyte affinity. Herein, a polypropylene separator modified by lithiophilic sulfonated aramid fibers is proposed to suppress lithium dendrites by accelerating Li + transport kinetics. Specifically, the sulfonate group in the functionalized separator displays superior Li + affinity and effective suppresses anion migration. This enhances the Li + transference number to 0.72, which is two times of the unmodified separator. Additionally, the functionalized separator achieves an increased ionic conductivity of 4.45 × 10 −4 S cm −1 and a high critical current density of 7.7 mA cm −2 . The improved Li + transport kinetics effectively alleviates Li + depletion near lithium electrodes caused by the rapid Li + deposition on electrodes, ultimately suppressing the growth of lithium dendrites. Consequently, the Li||Li cells with as-prepared separators show superior cycling performances for 6000 h, and the 1.2 Ah LiCoO 2 pouch cell remains a capacity of 1.13 Ah after 100 cycles. This work provides a novel paradigm to promote the practical implementation of high-safety lithium metal batteries.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Guoke Zhao,Jie Sun,Gongqing Tang,Yang Zhang,Guoyuan Pan,Yiqun Liu
To address the critical challenge of lithium extraction from high Mg 2+ /Li + ratio brines, this study develops a high-performance separation membrane through synergistic regulation of binary and ternary acyl chloride monomers combined with a bis-quaternary ammonium salt surface modification strategy. Optimizing the ratio of terephthaloyl chloride (TPC) to trimesoyl chloride (TMC) facilitates the formation of a periodic stripe Turing structure on the piperazine-based polyamide membrane's surface, markedly increasing the effective permeation area and water flux. The study reveals that adjusting the TPC ratio finely tunes the polyamide network's crosslinking density, thereby affecting the size exclusion effect. Additionally, TPC incorporation, by diminishing surface carboxyl density, enhances the membrane's surface positive charge, significantly improving its Li + permeability and Mg 2+ rejection capabilities. The optimized TPC-20 membrane demonstrates exceptional ion selectivity, achieving a MgCl 2 rejection of 91.3 %, a LiCl rejection of 11.3 %, and a water flux of 61 LMH. Further enhancement via amino-terminated bis-quaternary ammonium salt (ATBAS) grafting achieves 98.7 % Mg 2+ rejection, a record Li + negative rejection of -37.3 %, and a Mg 2+ /Li + selectivity of 105.1. Extended testing for 120 h verifies the membrane's reliable performance, highlighting its potential for industrial application. This research provides an efficient and energy-saving membrane separation solution for lithium extraction from brines.
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Materials Today Chemistry
·
2025
·
IF 6.7
Yuan Wang,DouDou Zhang,Hao song,Xiuxia Yang,Zhichao Liu,Yuankang Wang,Jie Yu,Xu Tian
X-ray scintillators are crucial for medical, industrial, and security imaging systems. However, achieving dual-mode of real-time and delayed imaging within a single matrix still faces challenges. Herein, LiGa 5 O 8 : Tb 3+ was successfully synthesized by the high-temperature solid-phase method. By controlling the atmosphere and optimizing the Li + /Ga 3+ ratio, the trap structure of LiGa 5 O 8 : Tb 3+ spinel phosphors is effectively adjusted, which achieved excellent dual-mode imaging. The air-synthesized Li 1.6 Ga 5 O 8 :4 %Tb 3+ exhibits intense X-ray excited persistent luminescence (X-PersL, 595 nm), while the sample of LiGa 5 O 8 :Tb 3+ reduced in H 2 /N 2 shows enhanced radioluminescence (RL) without X-PersL. This precise manipulation of anti-occupancy defects controls the charge trapping/detrapping dynamics, enabling switchable RL (real-time imaging) and X-PersL (delayed imaging) modes through the single Tb 3+ ions emission. The result resolves the incompatibility between prompt and persistent X-ray responses in conventional scintillators. The defect-regulation method establishes a universal strategy for developing scintillators compatible with complex operational demands, advancing high-performance X-ray imaging technologies.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Qiyue Fan,Jie Lin,Yue Sun,Xiangting Hu,Hang Yu,Zhenda Lu
Lithium manganese oxide (LMO) ion sieves are promising for lithium extraction due to their high adsorption capacity. However, their practical application is often limited by structural degradation from manganese leakage, reduced lithium uptake, and poor Li + /Mg 2+ selectivity, especially in brines with high Mg/Li ratios. To overcome these challenges, we in-situ synthesized polyamide (PA) nanofiltration membranes on the surface of LMO using two distinct amine monomers, polyethyleneimine (PEI) and piperazine (PIP), to create novel composite adsorbents LMO@PA(PEI) and LMO@PA(PIP). Both the coated materials demonstrated improved lithium uptake capacity and cyclic stability in adsorption-desorption cycles in simulated brine. More importantly, under a challenging Li/Mg ratio of 1:50 in binary ion solutions, the separation factors (α) of HMO@PA(PEI) and HMO@PA(PIP) were 2.23 and 4.55 times higher than that of uncoated HMO, showcasing excellent Li + /Mg 2+ selectivity. These findings highlight that polyamide nanofiltration layers successfully endow LMO with enhanced capacity, selectivity, and long-term stability, presenting a promising and scalable approach for direct lithium extraction from high‑magnesium salt lakes.
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DESALINATION
·
2025
·
IF 9.8
Shuwei Jia,Jun Wei,Xinyu Ma,Zhi Wang
High-efficiency lithium extraction from salt lakes is pivotal to meet escalating lithium demand driven by energy storage and electric vehicle industries. In this study, the small-molecule aminoacetonitrile (AAN) was introduced as an aqueous-phase co -monomer to modulate the interfacial polymerization process between polyethyleneimine (PEI) and trimesoyl chloride (TMC). Specifically, the primary amine in AAN molecules reacted with acyl chloride moieties in TMC, occupying reaction sites and thereby preserving a larger fraction of unreacted primary amine groups on the PEI chains within the separation layer, which significantly enhanced the membrane's surface positive charge. Simultaneously, the nitrile groups of AAN preferentially coordinated with Li + ions to effectively counteract the repulsive effect of the strongly positively charged membrane surface on Li + . This “charge-coordination” synergistic mechanism enabled precise control over the separation process. When treating mixed salt solution with a Mg 2+ /Li + mass ratio of 100, the optimized membrane achieved a separation factor of 74.7, along with enhanced MgCl 2 rejection of 99.3 % compared to virgin membrane's 93.9 %, and reduced LiCl rejection from 56.3 % to 49.3 %. Notably, upon treatment of simulated salt lake brine, the membrane manifested a pronounced Li + enrichment effect, with a LiCl rejection rate of −8.8 % while retaining a high MgCl 2 rejection capacity. This study employed a simple preparation process with industrialization potential, providing a guiding strategy for constructing high-selectivity membranes for Mg 2+ /Li + separation.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Ting Qi,Xiaona Wei,Xianfu Chen,Tiandan Lu,Dongliang Jin,Jing Zhong
Nanofiltration (NF) membranes are emerging as promising candidates for lithium extraction. However, their performance is challenged by the comparable physicochemical characteristics of Li + and Mg 2+ . In this work, a dual-reinforcement strategy is proposed to simultaneously enhance both selectivity and permeability by combining the densification of the polyamide (PA) network and the construction of Li + -selective transport channels. During the interfacial polymerization of piperazine (PIP) and trimesoyl chloride (TMC), the cross-linking density of the PA layer is increased by adding sodium dodecyl sulfate (SDS), while Li + -selective transport nanochannels are constructed by incorporating 15-crown-5 ether (CE). This synergistic modification enhances Mg 2+ rejection via intensified size exclusion and facilitates Li + permeation through ion-specific recognition. The resulting PIP/SDS/CE-PA membrane exhibits a high cross-linking degree of 91.26 %, a reduced pore size of 0.70 nm, and a narrow pore size distribution (σ = 1.22). Molecular dynamics simulations confirm the preferential complexation of CE with Li + , and that Li + exhibits faster and more favourable translocation in the PIP/SDS/CE-PA membranes, thereby facilitating its selective transport. Experimentally, the membrane achieves a high MgCl 2 rejection of 97.1 % and a low LiCl rejection of 56.7 %, yielding an exceptional Li + /Mg 2+ selectivity of 30 in a MgCl 2 /LiCl binary system, while maintaining a water permeance of 5 L m −2 h −1 bar −1 . These findings demonstrate the strong potential of the PIP/SDS/CE-PA membrane for the direct treatment of high Mg 2+ /Li + ratio salt-lake brines and offer a versatile strategy for designing next-generation NF membranes for selective ion separations.
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MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Shimei Xu,Song Liu,Yanlin Zhou,Rengui Xiao,Xiang Ke
Organic materials have garnered significant attention due to abundant resources, recyclability, and ease of design. However, they are hampered in practical applications by poor conductivity and high solubility. Herein, a lithium metal battery is developed in this work, utilizing the cathode material polyanthraquinonyl sulfide (PAQS) doped with a trace of NaCl. Additionally, the ionic liquid lithium bis-trifluoromethanesulfonimide and lithium metal as the anode. Physicochemical characterizations utilizing Raman spectroscopy and X-photoelectron spectroscopy indicate that both Na + and Li + migrate within the cell, forming a dual-cation battery. In addition, the battery displays exceptional rate performance with a capacity of 86 mAh·g −1 at 20 C, which is more than triples the capacity without NaCl, and has excellent cycling performance. Moreover, it retains 98 % capacity after 1000 cycles at 2 C with no significant degradation. This research offers an innovative strategy for developing a high-performance double-cation battery.
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Materials
·
2024
·Vol. 17
·期 19
·4682
·
IF 3.1
Duo Wang,Zhaomin Wang,Chunli Wang,Dongming Yin,Yao Liang,Limin Wang,Yong Cheng,Ming Feng
Polyanionic structures, (MO4)n−,can be beneficial to the transport of lithium ions by virtue of the open three-dimensional frame structure. However, an unstable interface suppresses the life of the (MO4)n−-based anode. In this study, MnWO4@C nanorods with dense nanocavities have been synthesized through a hydrothermal route, followed by a chemical deposition method. As a result, the MnWO4@C anode exhibits better cycle and rate performance than MnWO4as a Li-ion battery; the capacity is maintained at 718 mAh g−1at 1000 mA g−1after 400 cycles because the transport of lithium ions and the contribution of pseudo-capacitance are increased. Generally, benefiting from the carbon shell and electrolyte additive (e.g., FEC), the cycle performance of the MnWO4@C electrode is also effectively improved for lithium storage.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Liyuan Wang,Lingli Dong,Liyuan Xie,Zhitao Wang,Linpo Li,Enbo Shangguan,Jing Li
Regulating metal nodes to innovate the metal–organic framework (MOF) structure is of great interest to boost the performance of MOFs-incorporated composite solid electrolytes. Herein, Ce4+ with a low-lying 4f orbital is selected as metal center to coordinate with organic ligand to prepare MOF of Ce-UiO-66. The unsaturated open metal sites and defected oxygen vacancies furnish Ce-UiO-66 with strengthened Lewis acidity, which promotes Ce-UiO-66 interacting effectively with both poly(ethylene oxide) (PEO) and Li salt anions. Accordingly, Ce-UiO-66 as additive fillers can be uniformly dispersed in PEO matrix to form an advanced composite solid-state electrolyte (Ce-UiO@PEO) with accelerated Li+ transport. The optimized Ce-UiO@PEO displays a boosted ionic conductivity of 4.20 × 10–4 S cm–1 and an improved Li+ transference number of 0.39 at 60 °C, which are highly comparable to those of other MOFs@PEO electrolytes. Combined with the mechanical and thermal stabilities, such a Ce-UiO@PEO electrolyte enables Li/Li symmetric and Li/LiFePO4 full cells with superior cycling stability and rate performance. The Ce-UiO@PEO electrolytes are of great potential to be applied in high-performance lithium metal batteries.
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Energy & Environmental Science
·
2024
·Vol. 17
·期 11
·3807-3818
·
IF 32.4
Shenyang Xu,Zhefeng Chen,Wenguang Zhao,Wenju Ren,Chenxin Hou,Jiajie Liu,Wu Wang,Chong Yin,Xinghua Tan,Xiaobing Lou,Xiangming Yao,Zhihai Gao,Hao Liu,Lu Wang,Zuwei Yin,Bao Qiu,Bingwen Hu,Tianyi Li,Cheng Dong,Feng Pan,Mingjian Zhang
As commercial cathodes with the highest practical capacity, the structural nature of Li-rich Mn-based (LMR) cathodes, composite or solid solution, is still under debate. Due to the extreme structural similarity of two layered-phase components, namely, the monoclinic phase (C2/m) and rhombohedral phase (Rm), no single tool can resolve this concern alone. Herein, we combined multiple advanced techniques to comprehensively study the structural changes during synthesis of LMR cathodes from different aspects such as the elemental distribution, local structure, long-range structure, and short-range structure, revealing a clear process from the formation of two phases to the gradual phase fusion and eventually to a nearly solid solution. Particularly, X-ray pair distribution function (PDF) analysis combined with theoretical simulations reveals for the first time that the transition metal (TM)–TM distance increases with the progress of the phase fusion, which makes the short-range structural change in TM–TM atomic pairs an effective parameter for judging the extent of phase fusion. Eventually, excellent electrochemical performance was achieved by balancing capacity and cycling stability through adjusting the phase fusion to a medium extent in lithium and sodium two layered-phase components. This study establishes an approach to investigate the structural evolution in the complicated multiple-phase system and provides valuable insights into the design and optimization of cathodes by tuning the phase fusion extent.
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Energy Storage Materials
·
2022
·
IF 20.831
Shuixin Xia,Lingli Luo,Xun Zhang,Liangfei Shen,Junhe Yang,Wei Liu,Shiyou Zheng
The practical implementation of Li metal has been severely obstructed by the uncontrolled dendritic Li growth and poor cycling efficiency. Herein, highly lithiophilic, ultrathin (∼60 nm) and conformal bismuth-oxygen-carbon layer-modified carbon fibers (CF@BOC) first prepared from the bismuth-based MOF membrane self-assembly were rationally adopted to stabilize Li metal. Highly efficient ultrasmall (∼1.8 nm) bismuth seeds and in-situ generated Li 2 O-enriched interphase can cooperatively enable the homogeneous Li nucleation/growth and extraordinarily high Li utilization efficiency. Consequently, the modified Li metal exhibits ultrahigh rate capability (10 mA cm −2 ) and ultralong lifespan stability (6900 cycles). Impressively, the Li|LiFePO 4 full cell delivers an exceptional long-term cycling over 200 cycles under the rather harsh condition of low negative-to-positive-capacity (N/P) ratio (∼0.44) and electrolyte-to-capacity (E/C) ratio (5 g Ah −1 ). And the Li|LiCoO 2 full cell also reveals a prolonged cycling performance even at the ultralow N/P ratio (∼0.26) with a remarkable energy density of 361.3 Wh kg −1 . Furthermore, the pouch cell with a high loading cathode (3.6 mAh cm −2 ) still demonstrates prolonged cycling lifespan under the practical condition of extremely limited Li metal and lean electrolyte. This work enlightens a significant stride toward highly stable Li metal anode for practicability.
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Energy Storage Materials
·
2025
·
IF 20.2
Yiping Liu,Yuxin Huang,Qiang Zhang,Rouyan Guo,Guangqi Zhang,Jie Dong,Liancheng Zhao,Liming Gao
Ideal solid electrolyte interphase (SEI) is required for non-dendrite lithium (Li) deposition of lithium metal batteries (LMBs). However, the spontaneously-formed SEI is non-homogenous in the composition and structure and thus cause oriented distribution of Li + flux, which leads to the detrimental formation of lithium dendrites and poor cyclability of batteries. Here we propose a vertical & lateral ion-flux modulated ion-conductive SEI for high-voltage Li-metal batteries. A fluorinated MCM-41 (FMCM-41) modified LiPF 6 electrolyte is designed to construct the SEI film, which consists of homogenously distributed LiF and Li x SiO y , to regulate Li + transport paths in the lateral and the vertical direction, respectively, achieving uniform lithium plating. With the FMCM-41 modified electrolyte, the prepared Li||Li cell presents a long-term stability over 1000 h, and the Li||NCM622 full cell exhibits outstanding cycling performance with a high specific capacity of 169.9 mAh g -1 and a high-capacity retention of 93.3 % over 100 cycles at 0.5 C. This lateral-vertical concept provides a promising strategy for designing a desired SEI with uniform Li + transport paths to achieve ultra-long and high-rates lithium metal batteries.
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