Journal of Materials Chemistry A
·
2013
·Vol. 1
·期 47
·15016-15021
·
IF 0
Qianru Shi,Lixin Xue,Zengbin Wei,Fu Liu,Xudong Du,Darryl D. DesMarteau
Lithiated poly(perfluoroalkylsulfonyl)imide (PFSILi) ionene is synthesized and blended with poly(vinylidene) difluoride (PVDF) to serve as binder for the electrode of a lithium ion battery. The incorporation of the PFSILi ionene adds ionic conducting channels inside the electrodes and prevents electrolyte depletion during rapid charging–discharging. The small composition change results in an increase in the battery performance, including a better reversibility, lower polarization or internal resistance and an improved discharge capacity, as well as a higher energy density at high rates or elevated temperatures. At the rate of 2 C and 60 °C, the discharge plateau potential for the cell with the ionene based binder is 0.29 V higher than that for the cell with a PVDF only cathode binder. At a 4 C rate, the discharge capacity and energy density of a LiFePO4–Li half-cell with the ionic binder are 50% and 66%, respectively, higher than those of the cell using the nonionic PVDF binder at room temperature. Thus, the ionene polymer offers a new route, rather than just altering the active materials, to overcome the limitations of capacity and power density for rechargeable lithium batteries.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2024
·
IF 3.5
Ziyong Li,Mengnan Qin,Yanzhou Lei,Shuang Gao
Due to the depletion of fossil fuels, extensive CO 2 emissions, and growing demand for electrochemical energy, it is important to develop further utilization of renewable energy, as well as advanced energy storage techniques. To this end, the optically chargeable supercapacitor, which can convert the photon energy of solar light into electrochemical energy and store it for long-term usage, attracts extensive investigations. Among these, heterojunction construction was revealed as an effective method to enhance capacity. Recent works have reported the implementations of precipitation in ceramics, where the introduced matrix-precipitate two-phase structure is inspiring for constructing heterojunction, whereas it was seldom reported. In this work, Li-doped NaNbO 3 electrode material was prepared by adopting a multi-step solid reaction to precipitate LiNbO 3 and construct LiNbO 3 /NaNbO 3 heterojunctions. The electrochemical measurement demonstrates an enhanced optically chargeable capacity of roughly 85% increase at a scan rate of 1 mV/s and a four-fold increase at a charging–discharging current density of 1 A/g, as well as outstanding stability by introducing precipitates and constructing heterojunctions. This finding proposes a novel methodology design of heterojunction construction via precipitation to enhance the optically chargeable capacity of supercapacitor electrode materials and, therefore, may open up a potentially new application field for precipitate-tuned functionality in functional ceramics.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Yingyao He,Guiliang Li,Haibo Lin,Qiu Han,Yinlu Ye,Jianqiang Wang,Fu Liu
Selective separation property enhancement is quite important for membranes separations, especially for high mass ratio Mg 2+ /Li + separations. Low selectivity and unclear separation mechanism are the challenges for current membranes. In this study, we designed 4-aminophenyl-15-crown-5 incorporated polyamide nanofiltration membranes through interfacial polymerization for Li + enrichment. The electrochemical tests and energy barrier calculations using transition state theory confirmed that the crown ether in nanofiltration membrane is responsible for governing Mg 2+ transportation, resulting in a substantial energy barrier impeding its transport. Furthermore, a two-stage nanofiltration process was employed to enhance Li + enrichment in simulated brine and achieved 35-fold increase in Li + enrichment using as-fabricated membranes. These results demonstrate the substantial potential for Li + extraction from brine with a high Mg 2+ /Li + mass ratio using the crown ether incorporated membrane. Meanwhile, the proposed strategy incorporating transport barriers presents a novel approach for designing ion-selective channels within membranes.
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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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JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Lang Bai,Jiangmin Jiang,Xingchen Li,Yuqing Zhang,Lei Zhang,Lingbang Qiu,Libo Wang,Yanhua Cui,Quanchao Zhuang
Fluorinated carbon (CF x ) is considered to be a promising cathode material for lithium primary batteries, which has an ultra-high theoretical energy density of 2180 Wh kg −1 . However, the C-F bonds in CF x materials are strongly covalent, leading to a low intrinsic conductivity and poor electrochenical performance. In this work, a high entropy electrolyte (HE) has proposed to maintain the original discharge platform and exhibit a second discharge voltage platform that appeared around 1.7 V, which effectively improves the specific capacity of Li/CF x batteries (1035 mAh g −1 ). This significant improvement can be attributed to the chelation of the dioxygen atoms in the solvent with the Li + , resulting in the solvated Li + being co-intercalated into the lamellar structure of the graphite. Notably, the Li/CF x batteries in the HE electrolyte exhibit higher specific capacity than the single lithium salt at −40 °C and 80 °C (539 mAh g −1 , 1132 mAh g −1 ). This is mainly due to high entropy changes the point of the electrolyte solidifies, thus avoiding capacity loss caused by solid-phase electrolyte clogging the electrode holes. This work provides an efficient and reliable method for the design of Li/CF x batteries with high specific capacity.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zejun Song,Zhenggong Wang,Yanshao Yang,Jiaqi Zhang,Wangxi Fang,Jian Jin
Lithium, a highly sought-after element for various industries, is primarily sourced from salt-lake brines, where its extraction faces the critical challenge of separating Li + from high concentrations of Mg 2+ . In this work, we present a crown ether functionalized polymer membrane with a hierarchical pore structure, designed for highly selective Li + /Mg 2+ separation. By grafting 12-crown-4-ether onto a microporous polyimide, ether rings matching the size of Li + are incorporated within the interconnected intrinsic micropores, facilitating Li + permeation while restricting Mg 2+ transport. The addition of PEG4000 during membrane formation creates unconnected macropores, reducing effective membrane thickness while preventing pore linkages that could lead to Mg 2+ leakage. Consequently, the Li + permeation rate significantly increases from 0.0095nmol cm −1 s −1 to 0.257 nmol cm −1 s −1 , while Mg 2+ permeation remains low at 0.0014 nmol cm −1 s −1 , achieving a remarkable Li + /Mg 2+ selectivity of up to 184. This study offers a straightforward and efficient approach for developing Li + selective membranes for efficient lithium extraction.
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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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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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JOURNAL OF MEMBRANE SCIENCE
·
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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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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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 12
·5592-5600
·
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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