Nanoscale Research Letters
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2014
·Vol. 9
·期 1
·1-5
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IF 2.481
Wang Yanming,Wang Yajing,Wang Fei
Well-crystallized Li 2 NiTiO 4 nanoparticles are rapidly synthesized by a molten salt method using a mixture of NaCl and KCl salts. X-ray diffraction pattern and scanning electron microscopic image show that Li 2 NiTiO 4 has a cubic rock salt structure with an average particle size of ca. 50 nm. Conductive carbon-coated Li 2 NiTiO 4 is obtained by a facile ball milling method. As a novel 4 V positive cathode material for Li-ion batteries, the Li 2 NiTiO 4 /C delivers high discharge capacities of 115 mAh g -1 at room temperature and 138 mAh g -1 and 50°C, along with a superior cyclability.
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ACS Applied Materials & Interfaces
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2014
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IF 5.9
Xiaofei Wang,Ding Zhu,Ming Song,Shengrong Cai,Lei Zhang,Yungui Chen
The “(−) lithium (Li) anode|organic anolyte + inorganic catholyte|solid-state cathode (+)” Li–O2/air battery based on an inorganic solid-state air cathode was fabricated with a simple method. The electrochemical performance and reaction products of the Li–O2/air batteries under pure O2 and ambient air were investigated, respectively. The inorganic Li-ion conductive solid-state electrolyte Li1.3Al0.3Ti1.7(PO4)3 was stable during cycling and avoided the decomposition and volatilization problems that conventional organic electrolytes faced. Moreover, the porous air cathode provided a sufficient gas-phase O2-transport channel, facilitating the achievement of a high capacity of 14192 or 7869 mA h g–1 under pure O2 or ambient air, respectively. Our results demonstrate that the Li–O2/air battery using an inorganic porous air cathode has a great potential for practical application.
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Journal of Energy Chemistry
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2024
·
IF 14
Jinpeng Jian,Qian Chen,Hao Sun,Rui Li,Yaolin Hou,Yulong Liu,Jia Liu,Haiming Xie,Jiefang Zhu
The commercialization of lithium-sulfur (Li-S) batteries faces several challenges, including poor conductivity, unexpected volume expansion, and continuous sulfur loss from the cathode due to redox shuttling. In this study, we introduce a novel polymer via a simple cross-linking between poly(ether-thioureas) (PETU) and poly(3,4-ethylenedioxythiophene)- poly(styrenesulfonate) (PEDOT:PSS) as a bifunctional binder for Li-S batteries (devotes as “PPTU”). Compared to polyvinylidene fluoride (PVDF), as-prepared PPTU exhibits significantly higher electrical conductivity, facilitating electrochemical reactions. Additionally, PPTU demonstrates effective adsorption of lithium polysulfides, leading to improved cycling stability by suppressing the shuttling effect. We investigate this behavior by monitoring morphological changes at the cell interface using synchrotron X-ray tomography. Cells with PPTU binders exhibit remarkable rate performance, desired reversibility, and excellent cycling stability even under stringent bending and twisting conditions. Our work represents promising progress in functional polymer binder development for Li-S batteries.
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JOURNAL OF SOLID STATE CHEMISTRY
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2024
·
IF 3.2
Zezhen Yin,Yun Zhang,Shihua Ding,Tianxiu Song,Xiaoning Li,Jiaying Dan
Low permittivity LiAl 1- x Li x O 2- x ( x = 0–0.02) ceramics were prepared by conventional solid-state reaction method. XRD analysis indicated that the system remained single phase solid solution in the whole range of x examined. Li + heterovalent substitution for Al 3+ generated oxygen vacancy O vac , and enhanced the relative density from 94.33% to 97.13%. The dielectric constant ε r showed near linear variations versus sintering temperature and x value. Their relations mainly depended on the combined effects of relative density and dielectric polarizability . The quality factor Q×f was more than doubled from 15,647 GHz to 31,627 GHz, due to the packing fraction enlargement and covalent bond strengthening. The variation of temperature coefficient of resonance frequency τ f was explained from the view of oxygen bond valence. When x = 0.01, the ceramic exhibited the best microwave dielectric properties with ε r = 5.37, Q×f = 31,627 GHz and τ f = −104.2 ppm/°C when sintered at 1300 °C for 5 h.
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Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Yufei Yan,Jin Wang,Wubin Wang,Chao Han,Kaili Huo,Qingyun Zhang,Ning Wang
Positively charged nanofiltration (NF) membranes are widely used to separate Li + and Mg 2+ , which play an important role in extracting lithium from salt lakes. Despite its widespread use, the polyethyleneimine-trimesoyl chloride (PEI-TMC) membrane has attracted attention due to its limited permeance and separation efficiency. To address these challenges, we introduced amine-functionalized titanium dioxide (TiO 2 -NH 2 ) nanoparticles into the interfacial polymerization (IP) reaction. The introduction of TiO 2 -NH 2 reduced the diffusion rate of PEI and formed nanoscale water channels in the polyamide (PA) layer. This modification effectively modulated the structure of the NF membrane. The NF membrane exhibited high water permeance (9.65 L·m −2 ·h −1 ·bar −1 ) and Li + /Mg 2+ selectivity ( S Li, Mg = 16.31) when 0.03 wt% TiO 2 -NH 2 was used. The DLVO theory and transition state theory showed that the introduction of TiO 2 -NH 2 improved the rejection of Li + and Mg 2+ by the membrane. Furthermore, the optimized NF membranes demonstrated excellent stability during long-term filtration and in the mixed salt solutions with varying Mg 2+ /Li + mass ratios. This work is of great significance for designing and advancing membrane materials that facilitate the efficient separation of lithium from salt lakes with high Mg 2+ /Li + mass ratios.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Jia-Shuai Chen,Jing Wang,Ji-Hong Zhang,Zhi-Yuan Guo,Pan-Pan Zhang,Xiao-Fu Guo,Jie Liu,Zhi-Yong Ji
Achieving separation of lithium and magnesium with similar radii is crucial for the current lithium extraction technology from salt lakes, which usually possess a high lithium-to-magnesium ratio. Herein, we proposed the facile sequential interfacial polymerization (SIP) approach to construct electronanofiltration membranes (ENFMs) with a bilayer charged structure consisting of a high positively charged surface and a negatively charged sublayer. The trimesoyl chloride (TMC) concentration was adjusted to enhance the −COOH content and negative charge of the polyamide sublayer to promote Li+ migration, and then the quaternized polyethylenimine was introduced to the membrane surface by the SIP process to increase the positive charge density on the surface of the ENFMs, which would block the migration of Mg2+ and enhance the Li+/Mg2+ selectivity of the ENFMs. The optimal quaternary-modified ENFMs achieved outstanding selectivity for Li+/Mg2+ (49.85) and high Li+ flux (4.10 × 10–8 mol cm–2 s–1) at a current density of 10 mA cm–2. Moreover, in simulated brines with low lithium concentration and high Mg2+/Li+ ratio, the optimal ENFMs also displayed elevated Li+/Mg2+ selectivity (>45), highlighting the substantial promise of the membranes for practical applications.
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JOURNAL OF MEMBRANE SCIENCE
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2025
·
IF 9
Yufei Yan,Jin Wang,Wubin Wang,Chao Han
Positively charged polyethyleneimine (PEI) nanofiltration (NF) membranes exhibit great potential for Li + /Mg 2+ separation. However, the dense nature of the polyamide (PA) layer presents a challenge in breaking through the permeance bottleneck, significantly hindering its further application. In this study, 1-(2-aminoethyl)piperazine (AEP) was first incorporated into the PEI solution as a structural regulator to adjust the microstructure of the PA separation layer. The structure of the PA selective layer was fine-tuned with the incorporation of AEP, enlarging the spacing between the long-chain molecules of PEI, and established hydrogen bonding interactions with PEI. This led to the generation of Turing structures on the membrane surface, which enhanced permeance. Meanwhile, the primary amine groups in AEP were protonated in water, aiding in boosting positive membrane charge and subsequently elevating its rejection capability for divalent cations. The ingenious combination of large molecule PEI and small molecule AEP served a dual purpose in promoting the membrane construction and performance. The optimized PEI/AEP-TMC NF membrane exhibited high pure water permeance (11.24 L m −2 h −1 bar −1 ) and excellent Li + /Mg 2+ selectivity ( S Li, Mg = 24.59), while also achieving higher Li purity and Li recovery. Insights into the remarkable performance of the modified membranes were gained through the transition state theory. Additionally, the internal stress generated in the NF process was determined by utilizing the principles of thin plate theory, revealing that the NF membrane possesses good pressure resistance and maintains stable operation at pressures up to 9 bar. This study demonstrates the capability of PEI/AEP-TMC NF membranes for Li + /Mg 2+ separation and offers a novel aqueous phase monomer for the preparation of NF membranes specifically for Li + /Mg 2+ separation.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Mengke Li,Han Wang,Gaojie Yan,Zongjie Hu,Yi Feng,Xiaojie Zhang
Sulfhydryl-based polyimides were synthesized by the nucleophilic ring-opening reaction of thiolactone monomers (BPDA-T, ODPA-T, BTDA-T) with polyethylenimine (PEI), and they were coated on carbon nanotubes as host materials (BPTP@CNT, ODTP@CNT, and BTTP@CNT) of the sulfur cathode. BPTP@CNT/S, ODTP@CNT/S, and BTTP@CNT/S as cathode materials not only promote the covalent bonding of sulfur and polysulfide with sulfhydryl-based polyimides but also reduce the shuttle effect of soluble polysulfide in the redox process. Moreover, sulfhydryl-based polyimides can help improve the compatibility and interfacial contact between sulfur and conductive carbon while alleviating the volume expansion of the cathode. In addition, the conductive network of carbon nanotubes improves the electronic conductivity of the cathode materials. The BTTP@CNT/S cathode showed superior stability (the initial capacity was 902 mAh g–1 at 1C, and the capacity retention rate was 88.58% after 500 cycles) and the initial capacity could reach 718 mAh g–1 when the sulfur loading was 4.8 mg cm–2 (electrolyte/sulfur ratio: 10 μL mg–1), which fully proves the feasibility of the large-scale application of sulfhydryl-based polyimide materials.
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JOURNAL OF POWER SOURCES
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2025
·
IF 7.9
Xiaolong Liang,Yunxiao Zhou,Dongqing Liu,Haiming Wang,Jing Sun,Xingke Cai
Separator play a crucial role in the performance of lithium metal batteries (LMBs). However, the commonly utilized polyolefin separators exhibit significant drawbacks, including poor thermal stability, low electrolyte affinity, and limited effectiveness in suppressing lithium dendrite growth, which restricts their practical application in LMBs. In this study, we developed an ultra-thin (∼700 nm) Ti 0.6 Fe 0.4 O 2 nanosheet coating on the surface of polypropylene (PP) separators using a spray coating process. The resulting Ti 0.6 Fe 0.4 O 2 nanosheet-modified composite separator demonstrates superior electrolyte affinity, thermal stability, and mechanical properties compared to the unmodified PP separator. Furthermore, the Ti 0.6 Fe 0.4 O 2 nanosheet coating facilitates the regulation of homogeneous electrolyte distribution, thereby promoting uniform and rapid ionic transport. Li//Li symmetric cells employing the modified composite separators exhibit lower polarization values and more stable voltage fluctuations over extended cycling periods, specifically after 500, 200, and 100 cycles at current densities of 1.0, 2.0, and 5.0 mA cm −2 , respectively, when compared to those utilizing pristine PP separators. Additionally, full cells incorporating the modified composite separator exhibit enhanced cycling stability and rate capability at 1C, 2C, and 5C rates. The straightforward and efficient method presented in this study offers promising potential for the mass production of metal oxide-modified composite separators.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jian Lu,Chenye Dai,Shilong Li,Dong Zou,Yuqing Sun,Wenheng Jing
Similar physicochemical properties render the separation of Li + /Mg 2+ from salt lake brine difficult for two-dimensional (2D) membranes. Herein, ultraefficient Li + /Mg 2+ separation was achieved under the influence of an electric field using MXene/carbon nanotube (CNT) membranes developed on tubular ceramic substrates via thermal crosslinking. Crosslinking reactions between CNTs and MXene yielded well–intercalated CNTs between MXene nanosheets, forming antiswelling MXene/CNT membranes (MCMs) (interlayer spacing: 8.04 Å) suitable for Li + /Mg 2+ separation. At 2.8 V applied voltage, the MCMs exhibited Li + flux of 0.0491 mol m −2 h −1 and high Li + /Mg 2+ selectivity of 54.5, which outperform existing state–of–the–art 2D membranes. Specifically, under a positive electric field, Li + with a small hydration diameter and low hydration energy permeated through the membrane nanochannels more easily than Mg 2+ , increasing and decreasing Li + and Mg 2+ flux, respectively. Additionally, Mg 2+ retention was enhanced via the complexation of enriched Mg 2+ with –OH and –COOH on the membrane surface. The MXene membrane surface was thus reconfigured to be positively charged, inducing effective Mg 2+ rejection. This study offers a novel and practical approach for efficiently separating Li + /Mg 2+ as well as monovalent/multivalent ions.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Zhen Wang,Li Deng,Xue-Rui Yang,Jin-Xia Lin,De-Quan Cao,Jun-Ke Liu,Zhen Tong,Jing Zhang,Gao-Yang Bai,Yu-Xi Luo,Zu-Wei Yin,Yao Zhou,Juntao Li
The production of Li 2 CO 3 /C through CO 2 reduction reaction in nonaqueous systems is a complex four-electron, multi-step process, and the short existence time of intermediate monomers is not conducive to observation, which causes great difficulties in clarifying and regulating the CO 2 reduction path. Herein, ferrocene (Fc) as a functional additive into the electrolyte can stabilize the discharge intermediates and favor the occurrence of the two-electron reaction path during CO 2 RR, which leads to more stable operation of the Li-CO 2 battery; with the assistance of Fc, the CO 2 reduction pathway in Li-CO 2 battery is also clarified. Theoretical calculation analysis combined with experimental characterization observation confirms that Fc can shorten the CO 2 reduction distance through interaction with CO 2 and affecting the solvent environment around Li + , stabilize intermediate products to clarify the discharge path. The existence time of intermediates and discharge depth of the battery are key factors affecting the CO 2 reduction pathway. The Li 2 C 2 O 4 formed by CO 2 reduction through the 2-electron pathway is more favorable for the reversible operation of the Li-CO 2 battery than Li 2 CO 3 /C through the 4-electron pathway. This work provides inspiration for clarifying the reaction mechanism and regulating the CO 2 reduction pathway to improve the electrochemical performance of Li-CO 2 battery in the future.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
·
IF 4.1
Hu Fu,Weigang Zhu,Wenhua Xu,Zhongwei Zhao
Lithium-ion detection is necessary for extraction of lithium. Electrochemical sensors based on spinel LiMn 2 O 4 /λ-MnO 2 are expected to enable low-cost detection of lithium ions. Many studies demonstrate preferential intercalation of lithium ions, but little research has been done on how the differences in intercalation between lithium and other ions arise. Here, the differences in intercalation were identified by electrochemical impedance spectroscopy. Lithium ions were preferentially intercalated into λ-MnO 2 because of low charge transfer impedance. The apparent diffusion coefficient of sodium or potassium ions was one order of magnitude lower than that of lithium ions, while that of magnesium or calcium ions was two orders of magnitude lower. Therefore, insignificant intercalation of sodium, magnesium, potassium, and calcium ions slowed down diffusion of lithium ions through the channel and obstructed lithium-ion intercalation. The concentration of lithium ions was detected in brine of Baqiancuo Salt Lake by stripping voltammetry using λ-MnO 2 and an average recovery of 95.0 % was achieved. This study gives insights into ion intercalation of LiMn 2 O 4 in brine, which favors improvement of lithium-ion sensor based on LiMn 2 O 4 . In addition, the investigation facilitates understanding of the selectivity of similar materials (e.g., LiFePO 4 and Prussian blue analogous) in intercalation process.
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