JOURNAL OF MEMBRANE SCIENCE
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2024
·
IF 8.4
Lin-Pei Guo,Zhi-Yuan Guo,Jing Wang,Pan-Pan Zhang,Zhi-Hui Huang,Zhi-Yong Ji
Monovalent selective ion-exchange membranes have been widely used for lithium extraction from brine with a high Mg/Li ratio. However, extracting Li + directly from raw brine with high Na/Li ratio remains a significant challenge. This study introduces a flexible lithium selective composite membrane by incorporating lithium-ion conductor with a quaternized polymer. The lithium-ion conductor provides pathways for lithium transmission, while the quaternized polymer effectively hinders the leakage of impurity cations. As a result, with the applied voltage of 2.0 V, the membrane achieved a high Li + /Na + separation coefficient of 35.48 with a Li + flux of 8.33 × 10 −10 mol cm −2 s −1 in the simulated Yiliping brine, which are 56.3 and 2.8 times higher than that of commercial monovalent selective cation exchange membrane (CIMS). We proposed a lithium transport mechanism involving an adsorption-dehydration-diffusion process through the membrane. Theoretical calculations indicate that the combined effects of significant adsorption energy (−0.47 eV), low dehydration energy (515 kJ mol −1 ), and low diffusion barrier (0.37 eV) leads to the high selectivity for lithium. These findings provide promising prospects for the large-scale preparation of lithium ion-selective membranes, enabling the direct lithium extraction from raw brine.
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Seokyoung Choi,Wuliang Feng,Yongyao Xia
High nickel and Co-free layered cathodes (LiNi0.9Mn0.1O2, NM) for lithium-ion batteries (LIBs) have gained researchers’ interest recently because of their high energy density and being free of toxic elements, but they still suffer from inferior electrochemical performance due to the lattice instability during cycling. Herein, we successfully improved the electrochemical performance of NM using a high-entropy strategy. A high nickel Co-free multidoped high-entropy LiNi0.9Mn0.05Zr0.01Nb0.01Ti0.01Al0.01Mg0.01O2 (HE-NM, where HE represents high entropy with Zr, Nb, Ti, Al, and Mg dopants) cathode with five dopants was successfully synthesized. Owing to the effect of the multidopant, parasitic reactions and the accumulation of rock-salt phase were successfully suppressed, which led to uniformized interior stress and effectively inhibited microcracks during cycling. Consequently, HE-NM showed high thermal and structural stability with an initial discharge capacity of 206.35 mAh g–1 at 0.1 C and a retention of 76% after 100 cycles at 1 C, which showed a great advantage over the pristine NM (63%). This work provided a strategy for the stabilization of the NM cathode, which provided insight for the development of high-performance LIBs.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Xiaomin Ren,Yingying Chen,Yu Wang,Hongyan Fu,Dan Hu,Xudong Feng
The positively charged nanofiltration membrane (NF) has a strong repulsive effect on divalent magnesium ions, thus could be applied for the separation of Mg 2+ /Li + . Chemical grafting modification is an effective way to prepare positively charged membranes. However, it is difficult to achieve chemical modification on the surface of polyamide membrane as the chemical stability of polyamide. By introducing hydroxyl rich monomers (3-[n-tris(hydroxymethyl)methylamino]−2-hydroxypropanesulfonic, HMAH) as active sites in the interfacial polymerization process, the olefin monomers containing quaternary ammonium salt functional groups (acryloxyethyl trimethyl ammonium chloride, ATA) were reacted onto the surface of NF membrane through radical polymerization initiated by cerium ions to obtain positively charged NF membrane. The successful grafting reaction of quaternary ammonium salt monomer onto the surface of NF membrane was verified by Fourier-transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and scanning electron microscope (SEM). The membrane with dense and smooth surface layer showed C-N + characteristic peak in XPS N1s spectra and high isoelectric point. Meanwhile, the as-prepared membrane achieved high MgCl 2 rejection of 95.74% and low LiCl rejection of 18.1%, with pure water permeance of 9.43 L·m −2 ·h −1 ·bar −1 . After 60 hours of mixture filtration experiment, the membrane exhibited good long-term stability, maintaining the ionic separation selectivity over 30, which indicated that the positively charged membrane prepared by grafting method has potential application in the separation of Mg 2+ /Li + .
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Hanmeng Yuan,Zhimin Zhao,Chenguang Wang,Hongshuai Gao,Yi Nie
With the rising prevalence of lithium-ion batteries, efficient recovery of metal ions, particularly those potentially released from LiFePO 4 anodes, has become critical. Given that both Fe 3+ and Li + ions can form electrostatic adsorptive interactions, achieving effective separation of conventional adsorbent materials becomes challenging. This study presents an amino acid-functionalized nanocellulose hydrogel (ANH) synthesized by incorporating L-threonine, which significantly enhances the selective adsorption of Fe 3+ in a mixed-ion environment by leveraging coordination differences between Li + and Fe 3+ . The morphology, functional groups, and pore structure of ANH were extensively characterized using scanning electron microscopy, Fourier transform infrared spectroscopy, and mercury intrusion porosimetry techniques. Through batch experiments, the adsorption thermodynamics and isotherms of ANH for Fe 3+ were examined. Furthermore, the adsorption selectivity of ANH for Li + and Fe 3+ was evaluated in a mixed-ion system, revealing that the adsorption capacity for Fe 3+ was four times higher than for Li + at elevated concentrations. The adsorption mechanism of Li + /Fe 3+ was elucidated through multi-scale simulations, and the influence of varying amino acid grafting degree on adsorption metrics, such as solvent-accessible area and hydrogen bonding numbers, was investigated. The combination of experimental and theoretical results demonstrates the potential of ANH to inform the development of high-performance, selective adsorbents.
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WATER RESEARCH
·
2025
·
IF 12.4
Xiongrui Jiang,Lingjie Zhang,Yanhui Miao,Licai Chen,Jiaoyan Liu,Tingting Zhang,Shuai Cheng,Yuhan Song,Yunliang Zhao
Stacking two-dimensional (2D) nanosheets into lamellar membranes holds great promise in the selective separation of Li + and Mg 2+ from salt-lake brines, but revealing the intrinsic effect of nanosheet properties on the ion transport remains a great challenge. The primary reasons are inevitable emerging defects and changes in surface functional groups during nanosheet preparation. Here, we successfully demonstrated the intrinsic dependence of ion separation on the size and layer charge density of 2D building blocks using defect-free and inherently permanent charged clay nanosheets. The smaller-sized nanosheets readily assembled into lamellar membranes with narrower nanochannel dimension, which facilitated the steric hindrance effect to improve the Li + /Mg 2+ selectivity. Experiments and calculations demonstrated the layer charge density-dependent ion separation as well, for which a novel mechanism of intrinsic selective separation driven from the energy barrier difference of ions transport was proposed. Based on the “internal” regulation of the intrinsic nanosheet properties, MMT membranes realized stable and efficient Li + /Mg 2+ separation under extreme conditions, multi-cycle and long-term experiments, with an optimal S Li/Mg of 38.9, superior to most of the reported state-of-the-art membranes. This work reveals the intrinsic interplay of nanosheet properties tuning the ion transport and separation, which will inspire the design and development of advanced 2D lamellar membranes, particularly for sustainable and environmental energy exploitation.
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Energy Storage Materials
·
2024
·
IF 18.9
Dengxu Wu,Jian Peng,Zhiwen Jiang,Lei Zhu,Yujing Wu,Chang Xu,Zhixuan Wang,Ming Yang,Hong Li,Liquan Chen,Fan Wu
Lithium-metal batteries with solid electrolytes (SEs) have emerged as promising electrochemical energy storage devices due to high energy density and safety. However , inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their practical application. Herein , a new type of room-temperature liquidous Li metal arene complex—Li-Phenanthrene (Phen)-Ether is explored to enable a 3D LiSi@Li-Phen-Ether (3D LSLL) anode with low cost, high safety and high ion/electron-conductivity. Symmetric cells with sulfide SE and 3D LSLL anode deliver an ultra-high critical current density (> 13 mA cm −2 ) and long cycle life (> 1000 h, 0.25 mA cm −2 ). Moreover, full battery (LFP/sulfide SE/3D LSLL) can operate at low-external pressure (0.5 MPa) and ambient temperature by introducing a flexible cathode/sulfide interlayer with high ion conductivity (2 mS cm −1 ). This unprecedented battery configuration demonstrates high-rate (2C) performance and long cycle life (over 300 cycles), which exceeds preciously-reported sulfide SE/lithium batteries at low stack pressures, and may open up a promising route for high-energy-density, cost-effective and safe rechargeable lithium batteries.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2024
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IF 4.1
Yunqin Yang,QiuMing Liang,Tianwei Lei,Huan He,Tianquan Liang
The capacity of Co-free Li-rich Mn-based layered oxide decreases rapidly due to the irreversible lattice oxygen lose and the crystal structure change. The sodium modified cathode materials are synthesized via the sol–gel method and the electrochemical properties are investigated. Specifically, the first discharge capacity of Li 1.18 Na 0.02 Mn 0.54 Ni 0.26 O 2 is 150.5 mAh·g −1 at 2C, demonstrating a capacity preservation rate of 94.1 % after 100 cycles. And the diffusion coefficient of Li 1.18 Na 0.02 Mn 0.54 Ni 0.26 O 2 is 1.2152 × 10 -15 , which is better than 1.3798 × 10 -16 of the undoped material. This work demonstrates that appropriate Na + doping can stabilize the crystal structure, increase the lithium layer spacing and reduce the irrevocable escape of lattice oxygen within material.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 12
·5592-5600
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IF 3.5
Yunchun Zha,Yuyun Li,Zitong Fei,Changyi Fan,Qi Meng,Xingyi Peng,Peng Dong
The use of a carbon thermal reduction roasting method to recover lithium resources from spent lithium-ion batteries (S-LIBs) provides an important opportunity for recycling S-LIBs. The preferential extraction of Li via reduction roasting has been widely studied; however, the extraction of Li from mixed cathode materials has been rarely reported. Herein, we propose a method based on carbon thermal reduction to preferentially extract Li from mixed cathode materials. It was confirmed that there are differences in carbon thermal reduction products at 700 °C–850 °C by the thermodynamic analysis of the carbon thermal reduction process. At the same time, the effects of factors such as roasting temperature, roasting time, and material ratio on Li leaching efficiency were investigated. The Li recovery rate reached 98.86% under the optimal conditions of holding at 750 °C for 4 h with a molar ratio of mixed cathode materials to graphite of 1 : 0.25. Recovered Li2CO3 can be directly used as a lithium source for the regeneration of cathode materials. This study will provide new opportunities for the efficient recycling of spent lithium-ion batteries (S-LIB) mixtures.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Shuzeng Zhang,Yang Ding,Teng Zhang,Kangrui Qiang,Pengcheng Wu,Xiaoqian Zhang,Jiasong Zhong
The utilization of phosphors for information storage, data encryption, temperature sensing, etc. has been becoming a research hotspot. However, modulating dynamic and pluralistic phosphor emissions is still a huge challenge. Herein, we developed a Li + -induced site occupation engineering in Bi 3+ activated Mg 2 SnO 4 (MSO) phosphor with multiple emissions and dynamic afterglow for versatile applications. Experiments and first-principles calculations demonstrated that Bi 3+ would simultaneously enter [MgO 4 ] tetrahedron and [SnO 6 ] octahedron to present red and blue emissions, respectively. As Li + ions were introduced into Mg 2 SnO 4 :Bi 3+ , the preferably generated [LiO 4 ] could hinder the Bi 3+ from entering [MgO 4 ] units, so as to force Bi 3+ to substitute Sn 4+ in [SnO 6 ], thereby leading to strengthened blue emission. Due to the distinct luminescence decay of Bi 3+ in tetrahedron and octahedron units, the luminescence colors were regulated from blue to purple and red with enhancing temperature upon UV light excitation, being suitable for luminescence intensity ratio (LIR) thermometer. Moreover, by virtue of the afterglow properties originating from the inherent oxygen vacancies of Mg 2 SnO 4 , the dynamic information encryption and anti-counterfeiting by Mg 2 SnO 4 :Bi 3+ , Li + were achieved. The proposed site occupation engineering can certainly spur several innovative ideas in manufacturing high-performance phosphors for versatile applications.
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Advanced Energy Materials
·
2024
·Vol. 14
·期 11
·2303458
·
IF 24.4
Wei Li,Huwei Wang,Jinkai Zhang,Haodong Zhang,Ming Chen,Jiali Wang,Yueteng Gao,Rongyi Zhao,Junyang Hu,Guang Feng,Dengyun Zhai,Feiyu Kang
Various electrolyte additives are developed to construct a cathode electrolyte interphase (CEI) layer for high-voltage LiCoO 2 since the cathode suffers severe interfacial degradation when increasing the cut-off voltage over 4.55 V. However, the CEI derived from the additive sacrificial reaction faces the risk of rupture due to the corrosion reaction and the volumetric variation of the cathode. Herein, a non-passivating cathode interface is realized for 4.6 V LiCoO 2 with a non-sacrificial electrolyte additive (TBAClO 4 ) by regulating the solvent environment at the interface rather than the preferential decomposition for CEI formation. Owing to the novel protection mechanism, the cell performance shows little dependence on the CEI-formation process. Therefore, an ultra-high initial coulombic efficiency (96.63%) and excellent cycling stability (81% capacity retention after 300 cycles) are achieved in Li||LiCoO 2 batteries. Moreover, even with the electrolyte containing 1000 ppm H 2 O, the remarkable water capture ability of the additive together with its interfacial regulation enables the 4.6 V Li||LiCoO 2 battery to retain 80% capacity after 200 cycles. This non-sacrificial strategy provides new insights into high-voltage electrolyte additive design for high-energy-density lithium metal batteries.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Kai Zong,Xiaojun Bao,Kejie Jiang,Mei Zhang,Dongshun Deng
Gaseous ammonia (NH 3 ) pollution is harmful to human health and the environment. Developing adsorbents with excellent performance are in demand for NH 3 capture and separation. In this work, hyper-crosslinked polymer (HCP) with abundant pore and suitable surface property was prepared by one-step cross-linking reaction and applied to support various Li salts. The as-obtained Li salts@ HCPs were systematically characterized and evaluated for NH 3 adsorption at different composition and experimental conditions. The preferred [email protected] displayed reversible and outstanding NH 3 adsorption capacity of 37.33 mmol/g at 25℃ and 1.0 bar. Furthermore, kinetic and thermodynamics analysis revealed that the weak chemisorption of NH 3 on [email protected] was mainly controlled by adsorption equilibrium on the inner surface. The adsorption mechanism was elucidated using spectroscopic analysis and DFT calculations. Present work could provide more understanding of the gas–solid adsorption behavior and offer guidance for designing advanced materials for NH 3 capture and separation.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chenran Hao,Huichao Lu,Jiqiong Liu,Huiming Zhang,Xirui Kong,Jun Yang,Yanna Nuli,Jiulin Wang
As one of the most promising battery systems, the lithium sulfur battery is expected to be widely used in fields of high energy density demands. Owing to the unique solid–solid conversion mechanism, there is no shuttle effect for the Li-SPAN (sulfurized polyacrylonitrile) battery. However, the compatibility between Li anode and carbonate electrolyte has not been resolved, which prevents the SPAN from practical applications. Herein, an organic–inorganic gel carbonate electrolyte is proposed to stabilize interphases and structures of both the anode and cathode, where polyimide (PI) is used for electrolyte gelation, which can assist in the uniform distribution of inorganic components at the electrolyte interface. Furthermore, ZnS nanodots loaded on two-dimensional MoS2 flakes provide abundant Li-ion diffusion paths, improve the transfer kinetic of Li ions, and induce uniform nucleation and deposition of Li. This gel electrolyte ensures Li symmetric cells a long-term cycle life of more than 900 h under the condition of deep lithium plating/stripping at 5 mAh cm–1. Li∥Cu cells exhibit a prolonged lifespan of 800 h with a CE of 98.3%. Furthermore, the Li-SPAN battery shows stability of more than 850 cycles, with the capacity retention of 85.1%. This work provides an approach for high-energy Li-SPAN batteries with carbonate-based electrolytes.
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