JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Haofan Wang,Zhifei Wu,Xu Zhang,Li Liu,Deqing Liu,Jin Ran,Dawei Zhang
Conventional polymer anion exchange membranes (AEMs) suffer from the permeability-selectivity trade-off in diffusion dialysis (DD), limiting their efficiency in critical resource recovery scenarios (e.g., acid recycling and Li + extraction). To overcome this, this study incorporated polyaniline-modified MXene (PANI-Ti 3 C 2 T X ) nanosheets as transformative fillers into quaternized polyphenylene oxide (QPPO). The resulting PANI-Ti 3 C 2 T X -QPPO membranes enable dual-function DD for H + /metal cations and Li + /Mg 2+ separation. First, the as-prepared membranes exhibited enhanced microphase separation, yielding expanded hydrophilic domains (13.95–14.8 nm vs. 12.5 nm in pristine QPPO). Moreover, the 1.0 %-PANI-Ti 3 C 2 T X -QPPO membrane (with 1.0 wt% filler loading) achieved a peak ion exchange capacity of 1.75 mmol g −1 . For H + /metal cations separation: in HCl/FeCl 2 mixture, the H + dialysis coefficient ( U H ) reached 1.39–1.50 × 10 −2 m h −1 (2.7–2.9 times higher than the commercial TWDDA3S, 0.52 × 10 −2 m h −1 ); in HCl/AlCl 3 mixture, U H reached 1.50–1.53 × 10 −2 m h −1 , combined with exceptional selectivity ( S H/Al = 1568.4–1805.8), outperforming both TWDDA3S ( U H = 0.94 × 10 −2 m h −1 , S H/Al = 1423.8) and pristine QPPO ( U H = 1.27 × 10 −2 m h −1 , S H/Al = 1117). Finally, for Li + /Mg 2+ separation, the membranes delivered enhanced Li + flux with competitive S Li/Mg (11.4–12.4) against TWDDA3S (11.4) and QPPO (11.8). This study demonstrates that PANI-Ti 3 C 2 T X and QPPO synergistically overcome the permeability-selectivity trade-off in polymer membranes.
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高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Jintao Du,Haihua Luo,Qing Zhang,Chao Wang,Wei Chen,Shufen Wu,Xinyuan Yin,Jingjing Fu,Heng Cao,Xiaosong Liu,Wenhua Zhang
The strong coupling between Li+ transport and polymer segmental motion is considered to inherently limit the low-temperature performance of all-solid-state polymer electrolytes (ASPEs). Breaking the symmetric coordination environment of Li+ to promote its hopping transport mechanism offers a promising strategy to address this issue. In this work, we incorporate ∼60 wt % succinonitrile (SN) into a polypropylene (PP)-reinforced poly(ethylene oxide) (PEO)–(lithium bis(trifluoromethanesulfonyl)imide) LiTFSI (PPLS) electrolyte to disrupt the Li+ coordination symmetry. Multiple spectroscopies and theoretical calculations reveal that SN competitively coordinates with Li+ against PEO chains, resulting in an asymmetric and weakened Li+ solvation structure. Electrochemical impedance spectroscopy (EIS) and distribution of relaxation times (DRT) analyses demonstrate the decoupled dynamics of the Li+ transport from segmental relaxation. The PPLS electrolyte achieves a high ionic conductivity of (5.98 ± 0.585) × 10–5 S/cm at 0 °C and stable Li plating/stripping for >700 h at 0.1 mA/cm2 (25 °C). All-solid-state lithium batteries exhibit exceptional cycling performance at both room temperature and 0 °C. This work reveals the plasticizer-mediated formation of asymmetric Li+ coordination structures and their critical role in decoupling Li+ transport, offering a design paradigm for ASPEs that synergistically enhances ionic conductivity, mechanical robustness, and low-temperature adaptability.
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高影响因子
ACS Nano
·
2025
·
IF 16
Hualong Wu,Jiahao Dong,Jiantao Li,Guiyang Gao,Liang Lin,Ailin Liu,Hongfei Zheng,Guanyi Wang,Junxiang Liu,Laisen Wang,Jie Lin,Khalil Amine,Dong-Liang Peng,Qingshui Xie,Jun Lu
Low initial Coulombic efficiency and severe capacity/voltage fading during cycling caused by serious irreversible oxygen release, especially in the initial cycle, and resultantly induced unstable electrode/electrolyte interfacial chemistry, largely prohibit the commercial application of high-capacity Li-rich layered oxide cathodes (LLOs). In this work, a dual reductive gas interface cotreatment strategy is applied to regulate the lattice oxygen redox activity and reversibility with a multiple defective structure design including Li/O/TM (TM = transition metal) vacancies and the intrinsic TM doping as well as a full-surface protective layer, which can suppress the irreversible TM migration and then undesirable phase transformation, resisting the corrosion of electrolyte during cycling effectively. Importantly, the introduced reversible SO32–/SO42– redox couple that provides extra capacity compensation could alleviate the distortion of oxygen-central octahedral structure and structural collapse caused by immoderate oxygen oxidation. Thus, the lattice oxygen redox chemistry is optimized, with negligible oxygen loss during the initial cycle. And the designed AS-LLO cathode with greatly enhanced structure stability shows high-capacity retentions of 99.2% at 0.3C after 100 cycles and 82.4% even after 1000 cycles at 5C. This work provides a guideline for manipulating the oxygen redox chemistry to achieve long-lifespan Li-rich layered oxide cathodes for high-energy-density lithium batteries.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Lanhua Ma,Jiwei Zhao,Mengjie Li,Hai Su,Yong Li,Yuansheng Liu,Hang Liu,Ewa Zygadło-Monikowska,Yunhua Xu
Quasi-solid electrolytes are poised to revolutionize the next generation of high-energy-density lithium metal batteries. However, they face considerable challenges in operating at high temperatures due to severe side reactions, particularly with high-voltage cathodes. Here, we fabricated a nonflammable quasi-solid electrolyte (QSE) using an in situ copolymerization method. This electrolyte features a copolymer host with both flexible branches and a rigid skeleton, along with fire-retardant fluorine- and phosphorus-based plasticizers. The flexible branches reduce crystallinity and facilitate lithium-ion migration, while the rigid skeleton provides excellent high-temperature stability. The optimized fluorine–phosphorus mixed plasticizer provides effective sequestration of highly reactive oxygen/hydroxide radicals, along with a wide electrochemical window (up to 4.7 V vs Li+/Li), thereby ensuring excellent interface stability and safety characteristics. Consequently, the resulting quasi-solid electrolyte demonstrates remarkable physicochemical and electrochemical properties, enabling highly reversible lithium plating-stripping processes and good compatibility with cathodes. Using the nonflammable QSE, a high capacity retention of 82.3% is achieved for LiFePO4 after 1000 cycles at a high current density of 5 C and 80 °C. The good compatibility with high-voltage cathodes was demonstrated by the stable cycling of LiCoO2 over 400 cycles at a high cutoff voltage of 4.5 V and an elevated temperature of 60 °C.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiaohui Song,Rui Huang,Xin Liang,Yang Wang,Qian Hou,Binghui Ge,Qiaobao Zhang,Febri Baskoro,Afriyanti Sumboja,Rong Xiang,Hongfa Xiang,Zhimei Huang
The commercialization of Li-S batteries is constrained by the unstable interface, severe shuttle of polysulfides, and sluggish kinetic conversion reactions. Electrolyte regulation is a straightforward and efficient way to tackle those mentioned issues. Herein, a multifunctional electrolyte additive of 2,5-Dimercapto-1,3,4-thiadiazole (DMTD) is introduced in the ether-based electrolyte, which can be lithiated into Li 2 -DMTD when contacted with the Li or Li 2 S during the discharge process. The generated Li 2 -DMTD can operate as a highly ionic-conducting protective coating on the Li surface, inhibiting the formation of Li dendrites, and increasing interface stability. Then, it is reversibly oligomerized with Li 2 S, forming two organosulfur oligomers during the ensuing electrochemical process. Such a modified reaction routine can reduce the shuttle effect and speed up the reaction kinetics of Li 2 S at the cathode, preventing cathode passivation and boosting active material utilization. As a result, The Li||Li symmetric cells with DMTD exhibit about 5-fold cycle life than the reference cell under 5 mA cm −2 current density. Meanwhile, the initial charge voltage of Li||Li 2 S battery is greatly decreased from 3.7 V to 3.0 V with DMTD, and the assembled Li-S cell shows an improved capacity retention from 45.7 % to 81.2 % after 320 cycles. Therefore, this work successfully tackled the critical issues by designing functional organosulfur electrolyte additives in LSBs, which provides theoretical guidance for the electrolyte design in LSBs.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Zheyi Zhang,Qian Wei,Fen Jiao
The efficient recovery of fine-grained lepidolite remains a critical challenge in lithium resource extraction. This study proposes a flotation method leveraging mineral dissolution, focusing on the action mechanisms of Li⁺, Al³⁺, and Si⁴⁺ ions released from lepidolite and feldspar surfaces in alkaline environments. Flotation tests confirm that dissolved ions increase the flotation recovery of lepidolite from 45.24 % to 81.34 %. Inductively Coupled Plasma (ICP), Zeta potential, laser particle size measurement, and high-speed photography demonstrate that selectively released ions induce selective particle aggregation by regulating mineral surface potentials, thereby increasing the apparent particle size. Surface tension and foam property tests show that dissolved ions reduce the surface tension of the collector solution, optimize foam stability, and enhance mineralization efficiency. This study elucidates the pivotal role of dissolved ions in fine-grained lepidolite flotation and provides new insights into interface regulation strategies for the flotation of fine silicate minerals.
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高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Qian Zhao,Weizong Wang,Cheng Ruan,Zhengping Ding,Yurong Ren
Chloride-based solid-state electrolytes (SSEs) have attracted significant attention due to their favorable combination of ionic conductivity and electrochemical stability. However, chloride SSEs exhibit lower ionic conductivity than sulfides and liquid electrolytes, along with Li metal instability, hindering their high-rate all-solid-state battery (ASSB) applications. Previous studies have emphasized a cation substitution strategy, particularly high-entropy design, to enhance ionic conductivity, while anion substitution remains an underexplored yet promising alternative. Herein, through low-content Br substitution, Li3InCl5.9Br0.1 is synthesized via mechanical ball milling and achieves a room-temperature ionic conductivity of 1.30 mS cm–1, which represents a 48% enhancement over pristine Li3InCl6 (0.88 mS cm–1). Combined experimental and theoretical analyses reveal that the enhanced ionic conductivity stems from moderate local lattice distortion and optimized Li–Cl/Br bond lengths that facilitate Li+ conduction. The assembled LiCoO2|Li3InCl5.9Br0.1|Li6PS5Cl|Li–In ASSBs significantly demonstrate 81.89% capacity retention after 100 cycles at 0.2C (vs 70.55% for ASSBs with pristine Li3InCl6), along with improved rate performance. This work provides a reliable strategy of low-content Br– substitution to develop advanced chloride SSEs for application in ASSBs.
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高影响因子
RSC Advances
·
2017
·Vol. 7
·期 39
·24305-24311
·
IF 3.108
Keli Zhang,Yonggao Xia,Zhengdong Yang,Rusheng Fu,Chengxu Shen,Zhaoping Liu
Three dimensional (3D) porous silicon/reduced graphene oxide (Si/rGO) composites with typical networks have suffered damage during electrode preparation, which evidently affects the cycle and rate capabilities of Si/rGO anodes. Here, a controllable evaporation dry method is proposed to fabricate structure-preserved 3D porous Si/rGO anode materials by tuning the pore size distribution of the networks. As a result, after evaporation drying for 3.5 h, the optimal sample of 3D porous Si/rGO anode (denoted as Si–G-3.5) with a pore size of ∼500 nm could preserve its 3D network during the electrode preparation process. While the structures of Si/rGO composites with different drying times (denoted as Si–G-0, Si–G-2.5 and Si–G-4) failed to be preserved. Consequently, The Si–G-3.5 anode exhibits a high reversible specific capacity of 1563 mA h g−1 at 50 mA g−1, 90% capacity retention after 100 cycles and superior rate capability (955 mA h g−1 at 2 A g−1).
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高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 5
·1232-1238
·
IF 2.726
Chen Weijie,Xia Huicong,Guo Kai,Jin Wangzhe,Du Yu,Yan Wenfu,Qu Gan,Zhang Jianan
Lithium-sulfur(Li-S) batteries have been puzzled by the “shuttle effect”. In the recent years, catalytic materials present a huge potential for solving this problem. However, the exploitation for catalytic activity was still challenging in Li-S batteries. In this article, we put forward a single atom catalyst (SAC) of FeN 4 coupled with Fe 3 C on the N-doped carbon (FeN 4 /Fe 3 C@NC) by one-step pyrolysis method. The FeN 4 and Fe 3 C synergistically catalyze the polysulfides conversion when the N-doped carbon provides the high conductive three-dimensional skeleton in Li-S batteries. As a result, the FeN 4 /Fe 3 C@NC shows a specific capacity of 1100 mA·h/g at 0.2 C(1 C=1675 mA/g). In addition, the FeN 4 /Fe 3 C@NC maintains 99.01% of the pristine specific capacity after 100 cycles at 0.5 C, indicating the improved electrochemical performance in Li-S batteries. This work sheds new lights on the design of engineering catalysts for developing high-performance Li-S batteries.
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高影响因子
Journal of the American Chemical Society
·
2023
·
IF 15
Guodong Chen,Wenda Li,Xiaofan Du,Chen Wang,Xuelian Qu,Xiangyu Gao,Shanmu Dong,Guanglei Cui,Liquan Chen
Li-SOCl2 batteries possess ultrahigh energy densities and superior safety features at a wide range of operating temperatures. However, the Li-SOCl2 battery system suffers from poor reversibility due to the sluggish kinetics of SOCl2 reduction during discharging and the oxidation of the insulating discharge products during charging. To achieve a high-power rechargeable Li-SOCl2 battery, herein we introduce the molecular catalyst I2 into the electrolyte to tailor the charging and discharging reaction pathways. The as-assembled rechargeable cell exhibits superior power density, sustaining an ultrahigh current density of 100 mA cm–2 during discharging and delivering a reversible capacity of 1 mAh cm–2 for 200 cycles at a current density of 2 mA cm–2 and 6 mAh cm–2 for 50 cycles at a current density of 5 mA cm–2. Our results reveal the molecular catalyst-mediated reaction mechanisms that fundamentally alter the rate-determining steps of discharging and charging in Li-SOCl2 batteries and highlight the viability of transforming a primary high-energy battery into a high-power rechargeable system, which has great potential to meet the ever-increasing demand of energy-storage systems.
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高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 14
·5862-5869
·
IF 9.931
Ming Li,Chao Wang,Lixiao Miao,Jingwei Xiang,Tanyuan Wang,Kai Yuan,Jitao Chen,Yunhui Huang
Lithium–sulfur (Li–S) batteries are promising for the next-generation energy storage devices due to their high theoretical energy density and low cost. However, the shuttle effect and the passive layer between the separator and electrode still affect the cycling stability and coulombic efficiency seriously. Herein, we develop a 10 μm-thick rGO (reduced graphene oxide) and molybdenum phosphide (MoP) composite coating layer on a Celgard separator to improve the electrochemical performance of Li–S batteries. The introduction of such a MoP/rGO coating layer on the separator not only impedes the diffusion of polysulfides to the anode but also improves the sulfur utilization. In particular, the 10 nm MoP nanoparticles are very efficient for the polysulfide adsorption. Compared to the pristine Celgard separator, superior electrochemical performance is obtained in both coin cells and pouch cells with the MoP/rGO coated separator. High areal capacity (∼3 mA h cm−2), good rate performance, and long cycle life (300 cycles) are attained under a sulfur loading of 3.88 mg cm−2. The capacity decay rate is as low as 0.045% per cycle over 300 cycles. In addition, the pouch cells made by the modified separator with a high sulfur loading of 4.6 mg cm−2 achieve good electrochemical performance. At 0.1C, the initial discharge capacity is 1083 mA h g−1, and still remains at 759 mA h g−1 after 120 cycles. The result reveals the potential practical use of this MoP/rGO coated separator for Li–S batteries.
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高影响因子
SOLID STATE SCIENCES
·
2020
·
IF 2.434
Xinshu Luo,Yingying Li,Kun Liu,Jingbo Zhang
BaTiO 3 is used to fabricate the electron transport layer of perovskite solar cells due to its spontaneous polarization . Li + ions were doped into BaTiO 3 by the hydrothermal synthesis to increase the spontaneous polarization. The particle size of the as-prepared BaTiO 3 nanoparticles becomes smaller and more uniform for doping of Li + ions with a molar ratio of 1.0 during the synthesis processes. The absorption edge shifts towards the short wavelength with the increase in the doping amount. Further, TiO 2 nanocrystalline thin film was deposited on the Li-doped BaTiO 3 thin film , the double layer was used as an electron transport layer of perovskite solar cell to indirectly demonstrate the effect of doping on the spontaneous polarization of BaTiO 3 . The perovskite solar cell based on BaTiO 3 with 1.0 doping molar ratio of Li + ions shows the highest light-to-electric conversion efficiency of 14.3% accompanying with the highest short-circuit photocurrent density. The measurements of impedance spectra and intensity modulating photocurrent spectra indicate that the photocurrent enhancement of perovskite solar cells is attributed to the spontaneous polarization enhancement of Li-doped BaTiO 3 thin films. The enhanced internal electric field in the BaTiO 3 thin layer accelerates the photogenerated electron transport in the electron transport layer of perovskite solar cell.
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高影响因子
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