Journal of Materials Chemistry A
·
2025
·
IF 9.5
Junyu Chen,Xuedong Zhang,Feixiang Wu,Long Xie,Feng Li,Nina Wu,Zixuan Cao,Jinwen Zhao,Yuxuan Zhang,Xin He,Hongxia Gu,Jianyu Huang,Qiao Huang
Integrating conversion-type cathodes (such as iron-based fluorides (IBFs)) into sulfide all-solid-state batteries (ASSBs) significantly enhances energy density but faces challenges including unstable cathode/electrolyte interfaces. To mitigate these issues, a near-amorphous Li1.26Mg0.12Zr1.86(PO4)3 (LMZP) coating technology is developed to protect nano-sized FeF2 (n-FeF2) and micro-sized FeF3 (m-FeF3) cathodes from reacting with the sulfide electrolyte for the first time. The LMZP coating approach offers simplicity, low energy consumption and scalability. With the LMZP-coated cathodes and lithium–indium (Li–In) anode, the ASSBs achieve a discharge capacity of 310 mAh g−1 after 600 cycles and a maximum areal capacity of 2 mAh cm−2 for n-FeF2, and 301 mAh g−1 after 700 cycles with a maximum areal capacity of 3.1 mAh cm−2 for m-FeF3. When using a lithium (Li) metal anode, the ASSBs maintain a discharge capacity of 310 mAh g−1 after 300 cycles for n-FeF2 and 300 mAh g−1 after 600 cycles for m-FeF3, demonstrating excellent cycling stability and capacity retention. Notably, a discharge capacity of 280 mAh g−1 is sustained after 200 cycles for n-FeF2 and 301 mAh g−1 after 180 cycles for m-FeF3, with a reduced stack pressure (10 MPa). These results are unprecedented in IBF-based ASSBs, highlighting the potential of advanced coating strategies to enable scalable, high-performance metal fluoride cathodes in ASSBs with higher energy densities.
研究领域:
储能材料
·
电化学
·
固态电池技术
·
表面涂层工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Haolong Tan,Tongwei Gao,Wensheng Yang,Yue Gao,Quan Xie,Yunjun Ruan,Qian Chen,Tinghong Gao
The rapid development of microelectronic devices has increased the demand for miniature energy storage systems that are highly safe and exhibit long cycling life and excellent energy density. However, the lack of low-cost and high-performance fabrication methods presents a significant challenge to thin-film electrode fabrication. This study reports a strategy combining controllable pre-curing treatment with rapid thermal annealing (RTA), which enables in situ fabrication of high-quality sodium vanadium phosphate [Na 3 V 2 (PO 4 ) 3 ] thin films. RTA facilitates the cleavage of weak metal–O bonds in the precursor film, whereas optimisation of the pre-curing duration (0–100 s) effectively eliminates organic residues and strengthens the carbon framework, suppressing particle agglomeration. This synergistic control substantially improves crystallization uniformity and film densification, resulting in a refined grain structure and highly oriented crystal facets. Under optimal conditions, the thin film demonstrates a high specific capacity of 85.6 mAh g −1 at a current density of 1 A g −1 , retains 72.5 mAh g −1 even at 20 A g −1 , and demonstrates 90.3 % capacity retention after 200 cycles. Moreover, the assembled full sodium-ion cell exhibits an average operating voltage of 1.3 V while maintaining 94.2 % capacity retention after 500 cycles. This study elucidates for the first time the synergistic regulation pathway of the pre-curing–RTA coupling mechanism in Na 3 V 2 (PO 4 ) 3 thin-film fabrication and proposes an advanced preparation strategy for cost-effective, highly integrated, high-power sodium-ion thin-film devices, providing critical theoretical foundations and robust technical support for next-generation all–solid state sodium microbattery design and development.
研究领域:
材料科学
·
电化学
·
能源存储
·
薄膜制备
·
固态电池
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Kai Chen,Yanping Tang,Shuqing Zhang,Xuxia Hao,Xiaoning Zhao,Li-Qian Cheng,Youxuan Xiao,Zhaoyin Wen
Sulfide all-solid-state lithium battery (ASSLB) with nickel-rich layered oxide as the cathode is promising for next-generation energy storage system. However, the Li+ transport dynamic and stability in ASSLB are hindered by the structural mismatches and the instabilities especially at the oxide cathode/sulfide solid electrolyte (SE) interface. In this work, we have demonstrated a simple and highly effective solid-state mechanofusion method (1500 rpm for 10 min) to combine lithium conductive NASICON-type LiZr2(PO4)3 nanocrystals (∼20 nm) uniformly and compactly onto the surface of the single crystallized LiNi0.8Co0.1Mn0.1O2, which can also attractively achieve Zr4+ doping in NCM811 and oxygen vacancies in the LZPO coating without solvent and annealing. Benefiting from the alleviated interface mismatches, sufficient Li+ ion flux through the LZPO coating, promoted structural stabilities for both NCM811 and sulfide SE, strong electronic coupling effect between the LZPO and NCM811, and enlarged (003) d-spacing with enriched Li+ migration channels in NCM811, the obtained LZPO-NCM811 exhibits superior stability (185 mAh/g at 0.1C for 200 cycles) and rate performance (105 mAh/g at 1C for 1300 cycles) with high mass loading of 27 mgNCM/cm2 in sulfide ASSLB. Even with a pronounced 54 mgNCM/cm2, LZPO-NCM811 manifests a high areal capacity of 9.85 mAh/cm2. The convenient and highly effective interface engineering strategy paves the way to large-scale production of various coated cathode materials with synergistic effects for high performance ASSLBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shiqi Sun,Yanjun Chen,Qiang Bai,Zhen Tian,Que Huang,Changcheng Liu,Shengnan He,Yaxiong Yang,Yanzhong Wang,Li Guo
Researchers are accustomed to utilizing traditional solid-state and sol–gel routes to synthesize Na 3 V 2 (PO 4 ) 3 (NVP). No regulation mechanism is proposed to illustrate the growth process of NVP in solvothermal environment. In current work, uniform spherical particles with positive charge are synthesized by molecular self-assembly of nanosphere micelles using structural guiding agent polyethylene glycol (PEG) and surfactant Cetyltrimethylammonium bromide (CTAB). Nanoflower-shaped NVP sample is successfully prepared in the 100 % methyl alcohol medium, derived from the plate V 2 O 5 (negative charge) combining with the nuclear nanospheres (positive charge) with the induction of electrostatic attraction. Based on the multi-dimensional tests and molecular dynamic calculation, the protective mechanism of polar solution for NVP system is proposed for the first time, that is, methanol solvent system can better protect the morphological features of NVP than water environment to maintain the original special nanoflower morphology. Due to the distinctive and stabilized nanoflower construction, the optimized NVP60 sample can provide more extra active sites for the efficient de-intercalation of Na + and possess a large contacting area with electrolyte, resulting in the facilitated kinetic characteristics and superior electrochemical performance. The optimized NVP60 cathode possesses superior sodium storage property in both half cell and full cell. This work proposes a synergetic strategy combining theory and experiment to design and synthesize the modified NVP-based cathode materials from the molecular bonding aspect, further promoting the development of high performance cathode for SIBs.
研究领域:
材料科学
·
电化学
·
纳米材料
·
能源存储
·
无机化学
·
计算材料学
·
电池技术
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Yingmin Jin,Xin Zong,Xuebai Zhang,Chaojun Liu,Dong Li,Zhenggang Jia,Gen Li,Xuanguang Zhou,Junhua Wei,Yueping Xiong
Composite solid electrolyte (CSE) consisting of Li + conductive fillers and polymer matrix has become attractive for high energy-density lithium batteries . Current researches focus on the “ceramic in polymer”-type CSE due to the severe agglomeration of ceramic particles. Consequently, the destroyed percolation network impedes the further improvement in ionic conductivity . In this work, we report a novel structural design of ceramic-enriched CSE consisting of three-dimensional (3D) interconnected Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP), polyvinylidene fluoride (PVDF) and LiN(SO 2 ) 2 (CF 3 ) 2 (LiTFSI). The 3D LATP network is constructed through the surface functionalization of LATP particles by polymethyl methacrylate (PMMA). Owing to the intermolecular interaction between PMMA and PVDF, the incorporation of PMMA-coated LATP (denoted as LATP@PMMA) enables the uniform distribution of ceramic phase and generates interconnected LATP network. Noticeably, such an electrolyte maximizes the utilization of inorganic fillers through the facile treatment of zero-dimensional materials, which is comparable to those 3D template-derived fillers. Furthermore, continuous Li + conduction pathways through LATP framework and LATP/PVDF interphase are guaranteed by the enhanced affinity of LATP towards PVDF matrix and the intrinsic Li + complexation capability of PMMA. Remarkable cycling performances of the LiNi 0.5 Co 0.2 Mn 0.3 O 2 /LATP@PMMA-PVDF/Li batteries confirm the feasibility of 3D ceramic-enriched composite electrolyte in the application of solid-state lithium batteries.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 19
·10625-10637
·
IF 14.511
Kun Wang,Xiaobing Huang,Tao Zhou,Dan Sun,Haiyan Wang,Zhi Zhang
The NASICON-type Na4MnV(PO4)3 (NMVP) possesses potential as a cathode material in SIBs, and is known for its stable 3D Na+ superconductive framework, high voltage platform, and relatively low cost and toxicity. Nevertheless, the intrinsic poor electronic conductivity and Jahn–Teller effect from Mn3+ during cycling limit its further application. Herein, to address such issues, a well-designed 3D porous spheroidal Ce3+-doped NMVP@CeO2/C cathode was constructed via a simple spraying drying-assisted route. As proved, the synergistic effect of Ce3+ doping in the crystal framework and CeO2 surface coating was achieved simultaneously, which greatly improved the electronic conductivity, facilitated the ion diffusion transfer and stabilized the crystalline structure. As a result, the as-prepared sample delivered superior discharge performance (50.3 mA h g−1 at 50C) and long circular life (91.0 mA h g−1 after 2000 cycles at 5C with 86.7% capacity retention). Furthermore, the reversible biphasic reaction for cathodes was confirmed by Galvanostatic intermittent titration technique (GITT) and ex situ XRD. The DFT calculation revealed the influence of Ce3+-doping on the crystalline framework and electrochemical properties. Finally, the optimized NMVP cathode also showed great potential for practical utilization through the successful assembly of full cells.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Mengyue Liu,Kexin Wan,Xinmiao Zhang,Mingkun Wang,Dawei Yang,Jishi Wei,Kun Chang,Hongwei Tang
NASICON-type cathodes as promising candidates have attracted more and more attention, and Na 3 V 2 (PO 4 ) 3 is one of the outstanding representatives. In particular, it can tolerate complex interface reaction processes during the Zn 2+ insertion/desertion in the aqueous environment. However, existing three-dimensional channels in the intrinsic Na 3 V 2 (PO 4 ) 3 always hardly play to their advantages as narrow pathways and some other defects. This work has considered both the conductivity and capacity of this vanadium-based NASICON cathode at the same time, where a sodium-rich cathode material Na 3.2 V 1.8 Mn 0.15 Mg 0.05 (PO 4 ) 3 (NVMMP) with Mn 2+ and Mg 2+ dual-substituents has been designed considering the low cost and environmentally friendly characteristics. The synergistic effects introduced by Mn 2+ and Mg 2+ substitution led to a significant increase in the capacity and cycle life of the optimized NVMMP cathode material (with a capacity retention rate of 90.6 % after 2500 cycles at 2 A g −1 ). Furthermore, the reversible storage mechanism of Zn 2+ in NVMMP cathode materials and the theoretical study of such synergistic substitution on intrinsic electronic conductivity have been revealed by different in/ex-situ characterization techniques and theoretical calculations, where redox processes generated by Mn 3+ /Mn 4+ , enhanced ionic/electron pathway, and the pinning effect caused by injecting inert MgO 6 octahedra into the NASICON framework are key points to high capacity and long-life span.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2024
·
IF 6.1
Yongquan Zhang,Hongchang Gao,Jingshun Wang,Qingguo Chi,Tiandong Zhang,Changhai Zhang,Yu Feng,Yue Zhang,Dianxue Cao,Kai Zhu
All-solid-state lithium metal batteries (ASSLMBs) are considered the most competitive next-generation energy storage batteries due to their high energy density and high safety. Polyethylene oxide (PEO) is an ideal solid-state electrolyte due to its high chain flexibility, high dielectric constant, and strong dissociation ability towards lithium salts. However, the application of PEO is severely hindered by drawbacks such as low ion conductivity at room temperature and low electrochemical window. In this work, we constructed a Li1.25Al0.25Zr1.75(PO4)3 (LAZP)/PEO composite solid-state electrolyte (CSSE) with improved ion conductivity, enlarged electrochemical window, and stable charge–discharge cycle performance. The CSSE leads to an obvious LiF layer and Li2CO3 formation at the interface of lithium metal. Meanwhile, the addition of LAZP reduces the side reaction between PEO and the lithium metal significantly and suppresses the deterioration of ion conductivity. In addition, we modified LiFePO4 (M-LFP), the cathode sheet of the ASSLMBs, by adding an appropriate proportion of multi-walled carbon nanotubes (MWCNTs), PEO and lithium bis(trifluoromethane sulfonimide) (LiTFSI) to improve the ionic and electronic conductivity inside the cathode of the ASSLMBs. The Li/CSSE/M-LFP full cell exhibits a specific discharge capacity of 152 mA h g−1 at 60 °C and 2 C rate and a capacity retention rate of 93.5% after 200 cycles at 1 C. This work demonstrates an effective strategy for increasing the specific capacity, rate ability and long-cycle performance of ASSLMBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2019
·Vol. 45
·期 8
·11068-11072
·
IF 3.45
Yanqing Lai,Zhen Sun,Liangxing Jiang,Xiaojing Hao,Ming Jia,Li Wang,Fangyang Liu
NASICON-type LiZr 2 (PO 4 ) 3 (LZP) has a high bulk ionic conductivity (∼10 −4 S cm −1 ) and a wide electrochemical stability window between 0 and 5.5 V. However, LZP suffers from a problem in which its desirable rhombohedral phase transforms to the triclinic phase (∼10 −8 S cm −1 ) below 50 °C. In this work, we reported a rhombohedral-structured LiZr 2 (PO 4 ) 3 (α-LZP) at room temperature with a high total Li-ion conductivity (2.8 × 10 −6 S cm −1 ) by a microwave sintering process. Moreover, this approach realized a drastic reduction in the sintering temperature from the typical 1200 °C–900 °C with only a 4 h holding time. Using this approach, we also demonstrated the successful synthesis of Ca-incorporated Li 1.2 Ca 0.1 Zr 1.9 (PO 4 ) 3 (LCZP) with an ionic conductivity of 1.7 × 10 −5 S cm −1 .
研究领域:
材料科学
·
电化学
·
固体离子学
·
储能技术
·
陶瓷工艺
✓ 已验证
DOI
高影响因子
CHEMICAL COMMUNICATIONS
·
2016
·Vol. 52
·期 78
·11661-11664
·
IF 6.567
Jin Han,Yubin Niu,Shu-juan Bao,Ya-Nan Yu,Shi-Yu Lu,Maowen Xu
Novel nanocubic KTi2(PO4)3 was successfully fabricated via a facile hydrothermal method combined with a subsequent annealing treatment and further evaluated as an electrode material for potassium-ion batteries for the first time. For comparison, carbon-coated KTi2(PO4)3 obtained by a normal cane sugar-assisted method reveals improved electrochemical performances in potassium-ion batteries. This work may give a new insight into developing electrode materials for potassium-ion batteries.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiaoyi Li,Yongjian Zhou,Jiawen Tang,Siliang Zhao,Jingyong Zhang,Xiao Huang,Bingbing Tian
NASICON-type Li1.3Al0.3Ti1.7(PO4)3 (LATP) has attracted a lot of attention because of its high ionic conductivity and stability to air and moisture. However, the size effect of LATP primary particles on ionic conductivity is ignored. In this study, different sizes of LATP particles are prepared to investigate the morphology, relative density, and ionic conductivity of the LATP solid electrolyte. The influences of particle size and sintering temperature on the microstructure, phase composition, and electrical properties of LATP ceramics were systematically studied. The medium-sized LATP particle (2 μm) presents a great microstructure with a high relative density of over 97%, the highest ionic conductivity of 6.7 × 10–4 S cm–1, and an activation energy of 0.418 eV. The Li–Li symmetric cells and Li–LFP batteries delivering good electrochemical performance were fabricated with highly conductive LATP ceramics. These results make significant strides in elucidating the relationship between the particle sizes of LATP and its electrochemical performance.
研究领域:
材料科学
·
固体离子学
·
储能
·
陶瓷材料
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2015
·
IF 2.999
Jian Liu,Xiulan Duan,Yang Zhang,Ziqing Li,Fapeng Yu,Huaidong Jiang
Rb 2 Ti 1.95 Yb 0.05 (PO 4 ) 3 crystals with langbeinite-type structure were grown by high-temperature solution method. The chemical composition and electronic structure were analyzed using inductive coupled plasma atomic emission spectroscopy (ICP-AES) and X-ray photoelectron spectroscopy (XPS). The deconvolution of Ti 2p 3/2 photoemission line reveals two peaks at 459.3 eV and 458.1 eV, indicating titanium existence in two valence states: Ti 4+ (459.3 eV) and Ti 3+ (458.1 eV). The reduced BE difference ΔBE (O 1s-Ti 2p 3/2 ) shows stronger ionicity of Ti–O bonds in Rb 2 Ti 1.95 Yb 0.05 (PO 4 ) 3 compared with RbTiOPO 4 . Additionally, UV absorption, specific heat, and second harmonic generation (SHG) efficiency were studied. The UV absorption edge of the Rb 2 Ti 1.95 Yb 0.05 (PO 4 ) 3 crystal was observed at 368 nm. The SHG intensity of Rb 2 Ti 1.95 Yb 0.05 (PO 4 ) 3 is 5–6 times greater than that of KDP crystal when the particle size is between 38 and 74 μm.
研究领域:
材料科学
·
物理学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）