ACS Nano
·
2024
·
IF 15.8
Jieqing Shen,Wensheng Tian,Shuohan Liu,Hui Pan,Cheng Yang,Hengdao Quan,Shenmin Zhu
The low ionic conductivity of poly(ethylene oxide) (PEO)-based polymer electrolytes at room temperature impedes their practical applications. The addition of a plasticizer into polymer electrolytes could significantly promote ion transport while inevitably decreasing their mechanical strength. Herein, we report a supramolecular plasticizer (SMP) to break the trade-off effect between ionic conductivity and mechanical properties in PEO-based polymer electrolytes. Accordingly, the SMP is constructed by tetraethylene glycol dimethyl ether (G4) and SbF3 through halogen bonds. The SMP-plasticized PEO electrolyte (PEO/SMP) presents a simultaneously enhanced ionic conductivity of 2.4 × 10–4 S cm–1 (25 °C) and a high mechanical strength of 8.1 MPa, compared to those of pristine PEO-based electrolytes. Benefiting from the halogen bonds between G4 and SbF3, the Li–O coordination in PEO/SMP is evidently weakened, and thus rapid Li+ transport is achieved. Furthermore, the PEO/SMP electrolyte possesses a wide electrochemical stability window of 4.5 V and, importantly, derives an inorganic-rich SEI with a low interfacial resistance on a lithium metal surface. By using PEO/SMP, the lithium-metal battery with the LiNi0.5Co0.2Mn0.3O2 cathode exhibits a good rate and long-term cycling performance with a capacity retention of 75.3% (500 cycles). This work offers a rational guideline for the design of polymer electrolytes suitable for high-performance lithium-metal batteries.
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高影响因子
Small
·
2024
·
IF 13
Nan Wang,Tingxue Fang,Tinghui An,Yuhao Wang,Jiaqi Li,Shuming Yu,Honghai Sun,Dong Xiang,Xiangjie Bo,Kedi Cai
Li-O 2 batteries urgently needs high discharge capacity and stable cycling performance, requiring effective and reliable bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, Hovenia acerba Lindl -like heterostructure composed of cobalt sulfide and tin dioxide supported on carbon substrate (CoS/SnO 2 @C) is prepared via CO 2 laser irradiation technology. The half-wave potential of CoS/SnO 2 @C for the ORR is 0.88 V, while the overpotential of the OER at 10 mA cm −2 is as low as 270 mV. The Li-O 2 batteries employing the bifunctional CoS/SnO 2 @C catalyst displays a high discharge specific capacity of 3332.25 mAh g −1 and long cycling life of 226 cycles. Additionally, theory calculations demonstrate that the construction of heterostructure decreases energy barrier of the rate-determining step (RDS) for both ORR and OER. Notably, SnO 2 behaves as the electronic promoter to optimize the electronic structure of heterostructure interface and triggers charge redistribution of CoS, which weakens the adsorption strength of the * O-intermediates and allows to break the linear scaling relationship, thus further enhancing the catalytic performance of CoS/SnO 2 @C. This research furnishes directions for the design of heterogeneous catalysts, highlighting its great potential for application in rechargeable Li-O 2 batteries.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yaozhi Zhang,Bingru Wang,Fang Wang,Yasen Dai,Shuhang Ren,Yucui Hou,Weize Wu
This work designs a new method for recovering spent LiFePO 4 cathode materials, aiming to address issues with traditional hydrometallurgy processes such as complex operations, low lithium recovery rates, and high wastewater discharge. The method involves using a deep eutectic solvent (DES) composed of chloroacetic acid and ethanol, and oxygen as an oxidant, for the cooperative leaching of LiFePO 4 powders. Based on the acidic nature of the DES and the oxidizing properties of oxygen, LiFePO 4 was undergone an in-situ transformation into solid FePO 4 , while 100% of lithium was dissolved in the DES with high selectivity. The FePO 4 product can be recovered by filtration, and the addition of oxalic acid to the filtrate allows for lithium recovery. Importantly, the structure of the DES remained unchanged after use, allowing for three recycling cycles without a significant decrease in LiFePO 4 recovery efficiency. This process is environmentally friendly, with no generation of acidic or alkaline wastewater, and boasts high metal recovery rates, showcasing its huge potential for application.
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高影响因子
Small
·
2022
·Vol. 18
·期 26
·2201996
·
IF 15.153
Tengfei Zhang,Hong Xiao,Xiao Liang,Fanchao Zhang,Huifeng Zhuang,Qiuming Gao,Lirong Zheng
A universal strategy is established for preparing the carbonaceous matrix-based atomically distributed metal catalysts M-BPC (M=Ni, Co, Fe, Cu, and Mn, and biomass-derived porous carbon (BPC)) by one-step pyrolysis of mixed metal salts and biomass alfalfa. The optimized Ni-BPC has dual-atom Ni(II) 2 N 4 (µ 2 -N) 2 moieties, which are chemically anchored on the alfalfa-derived developed porous N-doped carbon BPC matrix. An ultrahigh specific surface area of 3133 m 2 g −1 with huge total pore volume of 3.02 cm 3 g −1 is obtained for Ni-BPC. The Ni-BPC could greatly promote the redox kinetics and effectively prevent the shuttle effect of lithium polysulfides in a Li–S battery. The Li–S battery assembled with the Ni-BPC modified separator exhibits prominent rate performance with the reversible specific capacities of 1279, 1119, 1037, 948 and 787 mAh g −1 at the current densities of 0.1, 0.2, 0.5, 1 and 2 C, respectively. The battery presents an ultra-long life with low capacity decay of 0.028% per cycle up to 2100 cycles at 1 C. Even under high areal S loadings of 3.9 mg cm −2 , the high discharge capacity of 976.6 mAh g −1 is obtained at 0.2 C and excellent cycling stability with 61.1% capacity retention is achieved after 490 cycles.
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高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yu Yan,Mengmeng Shang,Shuai Huang,Yining Wang,Yixin Sun,Peipei Dang,Jun Lin
Near-infrared (NIR) phosphors are fascinating photoluminescence materials with applications in phosphor-converted light-emitting diodes (pc-LEDs) for night vision lighting, which are still restricted by low efficiency and thermal stability in the current research stage. In this work, AScSi2O6 (A = Na/Li) are chosen as hosts due to a larger band gap and a single octahedral site for Cr3+ doping. The NIR-emitting Cr3+-activated AScSi2O6:Cr3+ phosphors were successfully prepared by a common high-temperature solid-state method. X-ray diffraction and Rietveld refinement confirm that the Cr3+ prefers to enter the Sc3+-octahedral lattice site in the AScSi2O6 structure. Under blue light excitation, AScSi2O6:Cr3+ phosphors exhibit broadband NIR emission from 700 to 1100 nm with a full width at half-maximum of ∼150 nm owing to the 4T2 → 4A2 electron transition of Cr3+. The photoluminescence properties were enhanced by adjusting the fluxes and sintering conditions, and highly efficient LiScSi2O6:Cr3+ NIR phosphors with external quantum efficiencies of 33.4% were obtained. Moreover, the optimized LiScSi2O6:Cr3+ exhibits excellent thermal stability (75% at 150 °C) with an activation energy of 0.33 eV. Importantly, the fabricated NIR pc-LED with the highly efficient LiScSi2O6:Cr3+ phosphor demonstrates brighter NIR light and a higher luminous efficacy than the NaScSi2O6:Cr3+ phosphor in night vision.
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高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Zhong Xu,Tao Yang,Xiang Chu,Hai Su,Zixing Wang,Ningjun Chen,Bingni Gu,Hepeng Zhang,Weili Deng,Haitao Zhang,Weiqing Yang
Solid-state composite polymer electrolytes (CPEs) usually suffer from intrinsic low ionic conductivity and a solid–solid interface, badly inhibiting their widespread commercial application in all-solid-state Li-metal battery (ASSLMB) energy storage. Herein, a synergetic strategy using strong Lewis acid–base and weak hydrogen bonds was employed for self-assembly in situ construction of three-dimensional (3D) network-structured poly(ethylene oxide) (PEO) and SiO2 CPEs (PEO@SiO2). Ascribed to this synergistically rigid–flexible coupling dynamic strategy, a harmonious incorporation of monodispersed SiO2 nanoparticles into PEO could remarkably reduce crystallinity of PEO, significantly enhancing the ionic conductivity (∼1.1 × 10–4 S cm–1 at 30 °C) and dramatically facilitating solid electrolyte interface stabilization (electrochemical stability window > 4.8 V at 90 °C). Moreover, the PEO@SiO2-based ASSLMBs possess excellent rate capability over a wide temperature range (∼105 mA h g–1 under 2 C at 90 °C), high temperature cycling capacity (retaining 90 mA h g–1 after 100 cycles at 90 °C), and high specific capacity (146 mA h g–1 under 0.3 C at 90 °C). Unambiguously, these high ionic conductivity CPEs along with excellent flexibility and safety can be one of the most promising candidates for high-performance ASSLMBs, evidently revealing that this synergistically rigid–flexible coupling dynamic strategy will open up a way to exploit the novel high ionic conductivity solid-state electrolytes.
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高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Gangning Zhang,Shigang Lu,Shangqian Zhao,Li Zhang,Haobo Sun
Due to the theoretical ultrahigh energy density of the Li–O2 battery chemistry, it has been hailed as the ultimate battery technology. Yet, practical Li–O2 batteries usually need to be designed in a large-sized pattern to actualize a high specific energy density, and such batteries often cannot be cycled effectively. To understand the inherent reasons, we specially prepared large-sized (13 cm × 13 cm) Li–O2 model batteries with practical energy output (6.9 Ah and 667.4 Wh/kgcell) for investigations. By subregional and postmortem analysis, the cathode interface was found to have severe local inhomogeneity after discharge, which was highly associated with the electrolyte and O2 maldistribution. The quantitative results by X-ray photoelectron spectroscopy (XPS) evidenced that this local inhomogeneity can exacerbate the generation of lithium acetate during charge, where the locally higher ratio of unutilized carbon surface and less Li2O2 after discharge would result in increased lithium acetate formation for a subsequent local overcharge. Moreover, verification experiments proved that the byproduct lithium acetate, which had been of less concern, was recalcitrant and triggered much larger polarization compared with the commonly reported byproduct Li2CO3 during battery operations, further revealing the key limiting factors leading to the poor rechargeability of batteries by its accumulation at a pouch-type cell level.
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高影响因子
IONICS
·
2021
·Vol. 28
·期 2
·767-777
·
IF 2.817
Zang Guojing,He Min,Liao Youhao,Li Minsui,Hong Mingyao,Li Weishan
To improve the comprehensive performance of fibrous membrane based on poly(methyl vinyl ether-alt-maleic anhydride) P(MVE-MA)- and poly(vinylidene fluoride-co-hexafluoropropylene) P(VdF-HFP)-blended copolymers, a small amount of nano-Al 2 O 3 was doped by electrospinning technique to apply for high-energy-density cathode material of nickel-rich LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA) based Li-ion battery. The results indicated that the electrospinning membrane and corresponding gel polymer electrolyte (GPE) only doped with 3.0 wt.% nano-Al 2 O 3 presented the proper structure and delivered the best electrochemical characterization. Due to the uniform distribution of nanoparticles on the fibers with higher density, the specific surface area and porosity of the fiber membrane were increased, leading to the improved fracture stress of 172.0 MPa for the membrane and ionic conductivity of 2.1 × 10 −3 S cm −1 for the GPE at room temperature. Contributed from the proper pore structure and the enhanced interfacial stability, the capacity retention of 89.4% was achieved for the Li/GPE/NCA coin cell after 200 cycles in the voltage range of 3.0 V and 4.3 V under room temperature using the GPE doped with 3 wt.% Al 2 O 3 , compared with that of 63.6% for the GPE without nanoparticles. Similarly, the discharge capacity of the coin cell under 7 C rate (123.2 mAh g −1 ) maintained 65% of that at 0.3 C (189.4 mAh g −1 ), showing good rate performance of the developed GPE. Therefore, the significant improvement in electrochemical stability of the GPE achieved by doping a small number of nanoparticles provided a simple and feasible solution for the development of high-energy-density Li-ion batteries.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zheng Zhang,Jinfeng Zhang,Zhihua Zhang,Xiao Du,Xiaogang Hao,Xiaowei An,Guoqing Guan,Jun Li,Zhong Liu
A novel physically blended polyvinylidene fluoride (PVDF) and polyacrylic acid (PAA) composite binder enhanced LiMn 2 O 4 /C (carbon black) film based electrode was successfully fabricated, and applied in an electrochemically switched ion exchange (ESIX) process for selective extraction of Li + from high Mg/Li ratio brine. The multifunctional composite binder system enabled the obtained LiMn 2 O 4 /C/PVDF- b -PAA film coated electrode to exhibit superior mechanical, hydrophilic and electrochemical properties compared with the LiMn 2 O 4 /C/PVDF film coated electrode. Based on the density functional theory (DFT) calculations, the ion exchange interaction between H + of –COOH groups in PAA and Li + facilitated the transport of Li + at the electrode interface, which enhanced lithium extraction performance of the film coated electrode. For treating the simulated brine (Mg/Li: ∼500), the intercalation capacity of Li + was about 15.1 mg g −1 , and the total extraction efficiency of lithium reached up to 62.8% after two electrochemical intercalation tests. Moreover, the film coated electrode displayed excellent selectivity towards Li + ions even in pre-treated actual brine (Mg/Li: ∼292.2). The Mg/Li mass ratio in the recovery solution could decrease to 0.46, and the calculated Li + /Mg 2+ separation coefficient reached as high as 631.08. In particular, the highly stable and scalable electroactive film could be prepared effectively, thus increasing its applicability. It is expected that such a LiMn 2 O 4 /C/PVDF- b -PAA film coated electrode could be a promising candidate for the selective extraction of Li + from high Mg/Li mass ratio brines.
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高影响因子
Small
·
2025
·Vol. 21
·期 19
·2501524
·
IF 12.1
Si Yi,Zhilin Yan,Yiming Xiao,Cuicui Ye,Huangjie Qiu,Jingwen Zhang,Pengpeng Ning,Deren Yang,Ning Du
Silicon monoxide (SiO) has garnered significant attention as a promising anode material for high-energy-density lithium-ion batteries due to its lower volume expansion relative to pure silicon (Si) and its higher capacity compared to graphite. Nevertheless, the poor intrinsic electronic/ionic conductivity and the low initial Coulombic efficiency (ICE) of SiO result in inferior rate capability and inadequate practical energy density, hindering its commercial viability. Here, a simultaneous prelithiation and in situ nitrogen (N) doping approach for SiO utilizing lithium nitride (Li 3 N), which significantly enhances both the ICE and lithium-ion (Li + ) diffusion kinetics, is proposed. N atoms are not only incorporated into the carbon layer on the surface of SiO but also form a uniformly distributed amorphous Li 2 SiN 2 phase within the SiO, facilitating Li + transport. Molecular dynamics simulations demonstrate that the Li + diffusion coefficient of amorphous Li 2 SiN 2 is significantly higher than that of other crystalline phases present in the prelithiated SiO matrix. The 1.5 Ah pouch cells further validate that the SiON-0.175/graphite||NCM811 exhibits a high ICE of 88.06%, and it retains 51.5% of its capacity even under 4C fast charging conditions. This study offers new insights into the development of next-generation SiO anode materials with high ICE and high-rate performance.
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高影响因子
Advanced Energy Materials
·
2022
·Vol. 12
·期 29
·2200656
·
IF 29.698
Wenze Wang,Qian Zhang,Tian Jiang,Songjie Li,Jiazhe Gao,Xuehua Liu,Chunfu Lin
Li 4 Ti 5 O 12 (LTO) is the most famous Li + -storage anode material with fast- and stable-charging capability, but suffers from several disadvantages, such as poor electron conduction, low energy density, and disappointing high-temperature performance. Here, LaCeNb 6 O 18 (LCNO) micrometer-sized particles are explored as a fast- and stable-charging anode material superior to LTO sub-micrometer-sized particles in terms of the working potential, rate capability, and high-temperature performance. The conductive Ce 3+ and Nb 5+ ↔ Nb 3+ reactions in LCNO, respectively, enable its significantly larger electronic conductivity and lower working potential than those of LTO. LCNO owns a very open A-site-cation-deficient perovskite structure, in which (vacancy/La/Ce)O 12 layers with electrochemical inactivity and superior volume-buffering capability locate between active NbO 6 layers, leading to not only fast Li + diffusivity but also low- and negative-strain behavior at different temperatures. At 25 ° C, LCNO exhibits higher rate capability (50 vs 0.1 C capacity ratio of 67.9%) than that of LTO, and excellent cyclability. At 60 ° C, LCNO maintains excellent cyclability, and achieves larger reversible capacity and even higher rate capability, whereas the high temperature lowers all the electrochemical properties of LTO. Therefore, LCNO holds great promise for fast- and stable-charging applications in a wide temperature range, even when its particle sizes are on the order of micrometers.
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高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 21
·9906-9914
·
IF 9.931
Sheng Liang,Yang Xia,Chu Liang,Yongping Gan,Hui Huang,Jun Zhang,Xinyong Tao,Wei Sun,Weiqiang Han,Wenkui Zhang
Lithium sulfide (Li2S) is considered as a promising lithium storage material because of its high theoretical specific capacity of 1166 mA h g−1. The electrochemical performance of Li2S can be remarkably improved by introducing carbon to form Li2S–carbon composites. However, the complex preparation process of Li2S–carbon composites limits their large-scale applications. Herein, we present a green and facile strategy to synthesize porous carbon-coated Li2S–carbon nanotube composites (Li2S@PC–CNT) by heating carbon disulfide (CS2) and the lithium hydride–CNT mixture at a temperature below 250 °C, which is the lowest temperature for in situ synthesis of Li2S–carbon composites reported till date. For the Li2S@PC–CNT composites, Li2S@PC particles are connected with neighboring particles through the 3D CNTs network skeleton. This unique nanoarchitecture not only prevents the loss of active materials and diffusion of polysulfides, but also significantly facilitates fast electron and ion transport. As a result, a high specific capacity (820 mA h g−1 at 0.1 A g−1 after 10 cycles) and a remarkable cycle life (502 mA h g−1 at 0.5 A g−1 after 300 cycles) are achieved. The rationally designed structure and superior electrochemical performance of the Li2S@PC–CNT composites will pave a new avenue for realizing high energy density of Li–S batteries.
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高影响因子
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