Crystals
·
2024
·Vol. 15
·期 1
·31
·
IF 2.4
Zhongran Yao,Fen Qi,Qiang Sun,Lin Ye,Xiaowei Yang,Guojie Chao,Pei Tang,Kongjun Zhu
Lithium-conducting NASICON materials have emerged as a promising alternative to organic liquid electrolytes for high-energy-density Li-metal batteries, owing to their superior ionic conductivity and excellent air stability. However, their practical application is hindered by poor sintering characteristics and high grain boundary resistance. In this investigation, Li1.3Al0.3−xYxTi1.7(PO4)3(LAYTP-x,x= 0.00, 0.01, 0.03, 0.05, and 0.07) were successfully synthesized via conventional solid-state reaction to explore the impact of Y3+on both ionic conductivity and chemical stability. The structural, morphological, and transport properties of the samples were comprehensively characterized in order to identify the optimal doping concentration. All samples exhibited a NASICON structure with a uniform distribution of Y elements within the electrolyte. Due to its highest relative density (95.8%), the LAYTP-0.03 electrolyte demonstrated the highest total conductivity of 2.03 × 10−4S cm−1with a relatively low activation energy of 0.33 eV, making it suitable for solid-state batteries. When paired with the NCM811 cathode, the Li/LAYTP-0.03/NCM811 cell exhibited outstanding electrochemical performance: a high capacity of 155 mAh/g was achieved at 0.2C after 50 cycles with a Coulombic efficiency of approximately 100%, indicating highly reversible lithium plating/stripping facilitated by the LAYTP-0.03 electrolyte. These results suggest that the LAYTP-0.03 ceramic electrolyte could be a promising alternative for developing safe solid-state Li-metal batteries.
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2025
·Vol. 31
·期 12
·e202403915
·
IF 3.7
Qi Pan,Wanliang Yang,Chen Wu,Dongjia Xie,Yuan Wang
Graphical A ploy(1,3-dioxolane) (PDOL) layer was constructed by a Al(OTf) 3 -induced in-situ solidification process between the interface of LATP and anode/cathode. The as-prepared PDOL as an “interfacial adhesive” can fill the gap between the LATP and the electrode, providing a better interfacial contact and reduced interfacial impedance. Such interfacial adhesive layer not only effectively prevents Li metal from reducing LATP but also provides intimate interface contact and limits unnecessary electron transport. Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) as the solid-electrolyte has attracted much attention for Li-ion batteries. However, the unstable LATP/Li interface and the insufficient contact between the anode/cathode and LATP usually lead to the structural collapse of LATP and the large solid–solid interfacial resistance for Li+ transport. Herein, a poly(1,3-dioxolane) (PDOL) adhesive layer was constructed by a Al(OTf) 3 -induced in-situ solidification process between the interface of LATP and anode/cathode. Such PDOL interfacial adhesive layer alleviates adverse reduction reactions at the LATP/Li interface and provides stable and well-contacted bilateral electrode interfaces. Benefitting from the PDOL interfacial adhesive, the Li|adhesive-LATP|Li symmetric cells achieve a current density up to 0.7 mA cm −2 and exhibit a good cycling stability for more than 2750 h at 0.1 mA cm −2 , and the Li|adhesive-LATP|LiFePO4 solid-state batteries with interface modification exhibit a capacity of 158 mAh g −1 at 0.2 C with a retention of 94 % after 100 cycles.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Houlin Cheng,Jingxuan Li,Pengcheng Wang,Youzu Xu,Zhiyang Zhang,Qian Feng,Hurong Yao,Zhigao Huang,Jiaxin Li
This work utilized Y 2 O 3 and rGO as additives, and systematically regulated their spatial distribution and composite ratio with Na 3 V 2 (PO 4 ) 3 (NVP) to overcome the bottlenecks faced by NVP, such as intrinsically low electronic conductivity, severe interfacial side reactions, and structural instability during cycling. The modified NVP cathode can significantly enhance its electrochemical performance, and improve its sodium storage and thermal safety performance in the pouch-type full cell. The as-prepared NVP@Y 2 O 3 @rGO material achieves an 84 % capacity retention rate after 1000 cycles at 1C&27 °C, while still delivering a specific capacity of 49.6 mAh g −1 at an ultra-high rate of 30C. Under elevated temperature of 45 °C, it maintains 91.5 % capacity retention after 400 cycles at 1C. In contrast, the pristine NVP retains only 38.2 %. Moreover, it exhibits a reversible capacity of 63.6 mAh g −1 even at an ultra-high rate of 40C. More importantly, pouch-type full cell testing further confirms its superior cycling stability (60.8 % capacity retention after 100 cycles, representing a 30.5 % improvement over the unmodified sample). Mechanistic studies reveal that the combined effects of Y 2 O 3 and rGO effectively facilitate electron/ion transport, suppress electrode-electrolyte interfacial side reactions, mitigate volume change stress, and enhance structural integrity. This work offers new insights for designing high-stability cathode materials for sodium-ion batteries.
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高影响因子
Sustainable Energy & Fuels
·
2025
·
IF 4.1
Yitao Hui,Xianhe Meng,Aobo Yue,Qi Shen,Bingyu Liu,Nengjun Yu,Qiaoling Kang,Lijing Yan,Chubin Wan,Tingli Ma
Na superionic conductors (NASICONs) have attracted much attention due to their unique framework structure and high capacity. However, the poor intrinsic electron conductivity severely limits further development. This work develops a soft-hard carbon composite modified Na3V2(PO4)3 (NVP) cathode with excellent rate performance and long-term cycling stability. The optimized sample exhibits excellent electrochemical performance and can release a specific discharge capacity of 102.7 mAh g-1 at 1 C rate. At the same time, after 5000 cycles at 20 C rate, the discharge capacity can reach 82.3 mAh g-1, and the capacity retention rate is 100.1 %. The morphological characteristics of the NVP/C samples were investigated, Meanwhile, combined with Raman spectroscopy and electrochemical analysis, these results revealed that the synergistic interaction between soft and hard carbon components significantly enhances electronic conductivity and facilitates rapid ionic transport. This work provides a unique idea for the surface modification and synthesis of NASICON cathode materials for sodium-ion batteries.
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 45
·期 2
·906-914
·
IF 3.288
Hong-bo Huang,Cai-ling Liu,Yue Yang,Shao-hua Luo
A series of lanthanum-doped Na3V2−xLax(PO4)3/C (0 ≤ x ≤ 0.03) composites have been fabricated via a simple sol–gel approach. The influences of La3+ substitution on the structure, morphology and electrochemical properties are systematically studied. Rietveld refinement is applied to explore the actual substitution site of La, which proves that La3+ ions successfully occupy the octahedral V sites. It is suggested that appropriate La doping will reduce the particle size and enhance the reversible capacity and rate capability. Among all the samples, the as-prepared Na3V1.99La0.01(PO4)3/C compound shows the highest electrochemical capability. It delivers a high initial specific capacity of 111.3 mA h g−1 at 0.2C and maintains a capacity of 108.1 mA h g−1 over 100 cycles, exhibiting much better electrochemical performance than the original Na3V2(PO4)3/C. In addition, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) experiments suggest that low-level La doping can greatly decrease the polarization and increase electrical conductivity with fast reaction kinetics and a higher Na+ diffusion coefficient. The study presented here will provide considerable insights into rare earth element-doping tactics, which will facilitate the commercialization of sodium-ion batteries.
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2020
·Vol. 31
·期 21
·18360-18369
·
IF 2.22
Wang Mengmeng,Tao Yueming,Zhang Dongyun,Sun Guanghan,Feng Ping,Chang Chengkang
Na 3–2 x Mg x V 2 (PO 4 ) 3 /C (0 ≤ x ≤ 0.2) were synthesized by a sol–gel method. According to X-ray diffraction (XRD) Rietveld refinement and energy dispersive spectroscopy (EDS) mapping results, Mg ions were approved to occupy the Na2 (18e) site in Na 3–2 x Mg x V 2 (PO 4 ) 3 /C for the first time. The amount of Mg substitution in Na 3–2 x Mg x V 2 (PO 4 ) 3 /C was optimized. The specific discharge capacities of Na 2.9 Mg 0.05 V 2 (PO 4 ) 3 /C at 10 C, 20 C, and 30 C were 98.9%, 91.5%, and 76.2% of the value obtained at 1 C, respectively. Na 2.9 Mg 0.05 V 2 (PO 4 ) 3 /C exhibited the highest capacity retention of 80.3% with a discharge capacity of 77.3 mAh·g −1 after 1200 cycles at 10 C. Na 2.9 Mg 0.05 V 2 (PO 4 ) 3 /C exhibited superior rate performance, resulting from a high sodium diffusion coefficient ( D Na ) of 3.91 × 10 –12 cm 2 ·s −1 and the excellent electrical conductivity (5.7 × 10 –2 s·cm −1 ). Combining the X-ray photoelectron spectroscopy (XPS) and Electrochemical impedance spectroscopy (EIS) results, the mechanism of Mg substitution was investigated. Since two Na + were replaced by one Mg 2+ , \({\mathrm{V}}_{\text{Na}}^{^{\prime}}\) was produced to maintain valence equilibrium. This phenomenon benefited Na + migration by broadening the diffusion channel in the structure of Na 3 V 2 (PO 4 ) 3 . According to the EPR results, the signal intensity of Na 2.9 Mg 0.05 V 2 (PO 4 ) 3 /C was much stronger than that of Na 3 V 2 (PO 4 ) 2 /C, thus confirming the existence of \({\mathrm{V}}_{\text{Na}}^{\mathrm{^{\prime}}}\) after Mg substitution. When the amount of Mg substitution was further increased to 0.1, the D Na decreased because of the small radius of Mg 2+ , which led to severe lattice distortion and volumetric shrinkage of the unit cell.
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高影响因子
Carbon Neutralization
·
2022
·Vol. 1
·期 1
·49-58
·
IF 0
Xiao-Hao Liu,Wei-Hong Lai,Jian Peng,Yun Gao,Hang Zhang,Zhuo Yang,Xiang-Xi He,Zhe Hu,Li Li,Yun Qiao,Ming-Hong Wu,Hua-Kun Liu
Developing low-cost and high-voltage manganese (Mn)-based Na superionic conductor (NASICON) cathode materials have attracted extensive interest. The low capacity and cycling instability of Na 4 MnAl(PO 4 ) 3 (NMAP), however, limits its performance in sodium-ion batteries (SIBs). Herein, a binary Na 4 Mn 0.5 Fe 0.5 Al(PO 4 ) 3 (MNFAP) is fabricated to ease the structural instability and, in turn, deliver an improved reversible capacity of 102 mAh g −1 at 0.1 C and a high energy density of 287.7 Wh kg −1 . The synergistic interaction of Fe and Mn in Na 4 Mn 0.5 Fe 0.5 Al(PO 4 ) 3 /C composite leads to a one-phase solid-solution reaction mechanism with high structural reversibility. Theoretical calculations have also been performed to explain the upshifted voltage platform of both Fe 2+ /Fe 3+ and Mn 3+ /Mn 4+ redox potentials. The rational design of NASICON-type cathodes by regulating their composition with dual metal ions provides new perspectives for developing high-performance SIBs.
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DOI
IONICS
·
2016
·Vol. 23
·期 3
·575-583
·
IF 2.119
He Zhangxing,Jiang Yifan,Sun Dan,Dai Lei,Wang Haiyan
Inferior rate capability is a big challenge for LiTi 2 (PO 4 ) 3 anode for aqueous lithium-ion batteries. Herein, to address such issue, we synthesized a high-performance LiTi 2 (PO 4 ) 3 /carbon/carbon nanotube (LTP/C/CNT) composite by virtue of high-quality carbon coating and incorporation of good conductive network. The as-prepared LTP/C/CNT composite exhibits excellent rate performance with discharge capacity of 80.1 and 59.1 mAh g −1 at 10 C and 20 C (based on the mass of anode, 1 C = 150 mA g −1 ), much larger than that of the LTP/C composite (53.4 mAh g −1 at 10 C, and 31.7 mAh g −1 at 20 C). LTP/C/CNT also demonstrates outstanding cycling stability with capacity retention of 83.3 % after 1000 cycles at 5 C, superior to LTP/C without incorporation of CNTs (60.1 %). As verified, the excellent electrochemical performance of the LTP/C/CNT composite is attributed to the enhanced electrical conductivity, rapid charge transfer, and Li-ion diffusion because of the incorporation of CNTs.
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高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Bangqian Wang,Jianjun He,Congcong Zhu,Bangcai Huang,Haijun Chen,Shan Guo,Fuzhong Wu,Guanghui Liu,Yong Deng,Xinyi Dai
The monoclinic Li 3 V 2 (PO 4 ) 3 cathode demonstrates significant promise for high-performance lithium-ion batteries (LIBs) technologies, primarily due to its outstanding energy density and enhanced safety performance. However, its practical application was hindered by inherent limitations, particularly, intrinsically restricted electron mobility and pronounced capacity fading during cycling at voltages exceeding 4.6 V. To overcome these challenges, this study employs a facile sol-gel method to synthesize carbon-coated Li 3 V 2 (PO 4 ) 3 materials while introducing In 3+ substitution for partial V 3+ sites. Electrochemical evaluations substantiate that the optimal In 3+ doping level of Li 3 V 2 (PO 4 ) 3 (LVP/C-In0.09) exhibits significantly enhanced performance. Specifically, the LVP/C-In0.09 sample delivers remarkable capability, sustaining 131.4 mAh g −1 at 10 C while maintaining 88.4 % of initial capacity after 500 cycles, surpassing the undoped LVP/C sample (initial capacity: 106.5 mAh g −1 ; retention: 75.7 %). XRD analysis indicates that incorporating In 3+ effectively broadens Li + diffusion channels. XAFS characterization reveals that the unit cell expansion is attributed to an increased V-V interatomic distance. Additionally, the controlled In 3+ doping effectively decreases the electrochemical resistance while substantially improving Li + diffusion kinetics. This study proposes a potential strategy to boost the practical application of Li 3 V 2 (PO 4 ) 3 in LIBs.
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高影响因子
ChemSusChem
·
2022
·Vol. 15
·期 11
·e202200313
·
IF 9.14
Gaoli Guo,Xiaoping Tan,Kaidi Wang,Huang Zhang
Aqueous zinc batteries have been regarded as a promising energy storage technology due to their high energy, high material abundance, low toxicity, and intrinsic safety. NASICON-type materials have been proposed as efficient cathodes for rechargeable batteries, yet they suffer from fast degradation and low Coulombic efficiency in aqueous batteries. Here we demonstrate that a rationally designed aqueous electrolyte containing a supporting Na salt and polymer additive can efficiently suppress the water activity through hydrogen bonding and facilitate the anion involvement in interfacial reactions, thus enabling the stable operation of sodium superionic conductor (NASICON) cathodes in aqueous zinc batteries. As exemplified by a Na 3 V 2 (PO 4 ) 3 cathode, the cell with zinc metal anode exhibits high cycling Coulombic efficiencies (around 99.9 % in average) with a steady output voltage and capacity retention for 300 cycles. This work addresses the potential issues with NASICON-type cathodes in aqueous zinc batteries and proposes an effective solution via fundamental interphasial chemistry to design efficient and sustainable aqueous electrolytes. Graphical Engineering electrode-electrolyte interphase : A rationally designed aqueous electrolyte with bi-cation and polymer additive is reported for aqueous zinc batteries with NASICON cathodes. As exemplified by a Na 3 V 2 (PO 4 ) 3 cathode, the full cells exhibited remarkable cycling stability and efficiency, benefiting from the well-suppressed material dissolution by electrolyte-induced interfacial engineering.
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高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Binggong Yan,Yongchao Wang,Hongliang Ren,Xizhao Lu,Masashi Kotobuki,Bin Liu,Kaiyong Jiang
NASICON-structured solid-state electrolyte, namely Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) possesses high ionic conductivity and good compatibility with lithium metal that make it an ideal electrolyte for next-generation lithium battery. However, high interfacial impedance and possible dendrite limit its practical applications. To reduce interfacial impedance, herein, surface texturing on the LAGP is conducted using a femtosecond laser, and further wetted by ionic liquids. The femtosecond laser-modified surface can effectively increase wettability and improve the interfacial contacts. Low area specific impedance of 81.4Ω cm -2 is obtained and the full battery demonstrates good electrochemical performances.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Peng Wei,Yanxiang Liu,Yarui Su,Ling Miao,Yangyang Huang,Yi Liu,Yuegang Qiu,Yuyu Li,Xiaoyu Zhang,Yue Xu,Xueping Sun,Chun Fang,Qing Li,Jiantao Han,Yunhui Huang
We are presenting a sol–gel method for building novel nanostructures made of nanosized F-doped Na1–2xTi2(PO4)3–xFx (NTP-Fx, x = 0, 0.02, 0.05, and 0.10) particles embedded in three-dimensional (3D) carbon matrices (NTP-Fx/C). This technique combines advantages of both zero-dimensional materials and 3D-carbon networks. Proper fluorine doping stabilizes the NTP structure and greatly enhances ion/electron transportation, leading to superhigh-rate electrochemical performance and ultralong cycle life. The composite electrode delivers high specific capacities of 121, 115, 112.2, 110.1, 107.7, 103.1, 85.8, and 62.5 mA h g–1 at 0.2, 0.5, 1, 2, 5, 10, 20, and 30 C, respectively. It retains an unbelievable ∼70% capacity after a thousand cycles at a rate as high as 10 C. Electroanalytical results reveal that fluorine doping significantly enhances Na+ diffusion kinetics. Meanwhile, density functional theory calculations demonstrate F-doped NTPs’ own outstanding electrochemical properties, which is due to the enhanced intrinsic ionic/electronic conductivity. The results show that anion doping is an efficient way to make high-performance NTP anodes for sodium-ion batteries.
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高影响因子
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