Small
·
2025
·Vol. 21
·期 42
·e05135
·
IF 12.1
Jinwei Zhang,Xiaolin Zhang,Junmin Xu,Xinyue Li,Dezhi Xiao,Zhixia Duan,Han Zhou,Xinchang Wang,Paul K. Chu
A porous KVPO 4 F/reduced graphene oxide (KVPF/rGO) microgrid aerogel electrode is designed and fabricated using direct ink writing 3D printing for high-performance potassium-ion battery cathodes. This 3D-printed KVPF/rGO aerogel electrode, which integrates well-dispersed KVPO 4 F microspheres in the reduced graphene oxide matrix, shows enhanced structural integrity and electrical conductivity, thereby facilitating efficient ion and electron transport. The KVPF/rGO electrode achieves a reversible discharge capacity of 99.0 mAh g −1 at a current density of 50 mA g −1 in the voltage range between 2.0 and 5.0 V. It retains 93.9% of its capacity after 100 cycles and delivers a discharge capacity of 72.6 mAh g −1 at a high current density of 500 mA g −1 , demonstrating good rate capability. The role of rGO in improving charge transfer and minimizing polarization is demonstrated. The flexibility of the 3D-printed electrodes is validated by fabricating soft-pack batteries, which maintain stable performance under mechanical stress, an essential requirement for wearable electronics. The results highlight the large potential of 3D printing technology to enhance the properties and flexibility of potassium-ion batteries and pave the way for future advancements in energy storage devices.
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PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Jimin Qiu,Yuchen Ji,Wenfang Li,Yuhang Li,Wenguang Zhao,Yunxing Zuo,Weiyuan Huang,Chen Zhu,Mingjian Zhang,Guorui Zheng,Luyi Yang,Feng Pan,Zu-Wei Yin
Lithium cobalt oxide (LiCoO2) cathodes suffer serious structure instability when charged to high voltage (>4.5 V), including H1-3 phase transition, cobalt dissolution, and interfacial side reactions, which are closely related to the instability of surface lattice oxygen. Herein, an interfacial B–O complexing strategy was proposed to stabilize the surface lattice oxygen of LiCoO2 at 4.6 V, through the preferential coordination between derived products of the tris(pentafluorophenyl)borane electrolyte additive and LiCoO2. Combining a series of in situ and ex situ characterization methods with temporal and spatial resolution, it was revealed that the emergence of peroxy-like species (O22–) at high potentials is one of the origins of the instability of LiCoO2, which can be well inhibited thanks to interfacial B–O complexing. Thus, oxygen loss and interfacial side reactions can be drastically retarded, which consequently provides a more stable chemical environment for Co element, avoiding the dissolution and valence reduction of Co. Owing to the well-anchored Co and O elements, undesirable phase transition and local coordination structure change are suppressed, hence improving the capacity retention and rate performance of LiCoO2 at 4.6 V. This study provides an interfacial complexing strategy to stabilize the high-voltage LiCoO2 cathode.
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PubMed
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Dong Chen,Jinhui Li,Lihan Zhang,Kuan Wang,Manling Sui,Pengfei Yan
Biphasic composite materials have been demonstrated to be effective in enhancing the structural stability and electrochemical performance of layered cathodes for sodium-ion batteries. Herein, based on the cationic potential methodology and co-doping strategy, we design a biphasic O3/P2 composite layered cathode (85NFMLCC, Na 0.85 Ca 0.02 Ni 0.2 Li 0.1 Fe 0.15 Co 0.05 Mn 0.5 O 2 ) and further integrate surface modification to achieve superior cycling performance, which is prepared by a simple one-pot solid state sintering method. Comprehensive structural characterizations reveal that the surface modification is realized by an inner Co-enriched layer and an outmost Ca-coating layer, which enables much improved rate capability and cycling stability simultaneously. In situ XRD confirms that biphasic design effectively suppresses the harmful phase transition during high voltage cycling, and the bilayer surface modification further enhances the cathode interfacial kinetics and robustness. The electrochemical tests demonstrated that 85NFMLCC exhibits a high specific capacity (136.7 mAhg −1 at 0.1C), superior cycling stability and rate capability at 2.0–4.3 V, 97.8 % capacity retention after 100 cycles at 0.1C and 84.5 % capacity retention after 800 cycles at 1C 2.0–4.0 V. This work demonstrates that biphasic composite with proper surface modification is a very promising design route toward high performance high voltage cathode material for sodium-ion batteries.
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高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Siyu Sun,Huipeng Zeng,Baichuan Cui,Mingjia Zhi,Jing Zheng,Zhanglian Hong,Jijian Xu
Lithium metal batteries (LMBs) face severe interfacial degradation due to uncontrolled lithium dendrite growth and electrolyte decomposition. Conventional electrolytes fail to concurrently stabilize lithium metal anodes and high-voltage cathodes owing to competing parasitic reactions. Here, we report a softly solvating electrolyte composed of 1,3-dioxane (1,3-DX) and dual salts─lithium bis(fluorosulfonyl)imide/lithium hexafluorophosphate (LiFSI/LiPF6)─that leverages anion-complementary coordination to decouple interfacial requirements. The solvent’s steric hindrance softens Li+–solvent interactions, enabling FSI– and PF6– to spatially separate their interfacial functions: FSI– drives LiF-rich solid-electrolyte interphase (SEI) formation on Li metal, while PF6– constructs a thin (<10 nm) cathode–electrolyte interphase (CEI) on LiNi0.5Co0.2Mn0.3O2 (NCM523) cathodes. Raman and 17O NMR spectra confirm suppressed solvent coordination and anion-aggregate dominance. Li||NCM523 cells utilizing this electrolyte achieve over 80% capacity retention after 100 cycles at 4.3 V, with a high average Coulombic efficiency (CE) above 99.0%. Cross-sectional scanning electron microscopy/transmission electron microscopy (SEM/TEM) reveals crack-free cathodes and robust, homogeneous SEI and CEI layers. Remarkably, the Li||NCM523 cells maintain 36.9% capacity retention of their room-temperature performance (54.7 vs 148.3 mAh g–1) at 0.2 C and −30 °C, highlighting the electrolyte’s low-temperature compatibility. This work establishes an anion-synergistic design strategy to reconcile bulk ion transport with dual electrodes.
研究领域:
电化学
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材料科学
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能源存储
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界面化学
·
锂离子电池
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PubMed
高影响因子
Journal of Energy Chemistry
·
2022
·
IF 13.599
Qi Ye,Haoyue Liang,Shuhao Wang,Can Cui,Cheng Zeng,Tianyou Zhai,Huiqiao Li
Poly (ethylene oxide) (PEO)-based solid polymer electrolyte is always the most promising candidate for preparing thinner, lighter and safer lithium-ion batteries. However, the lithium dendrites growth of lithium anode and the high-voltage oxidation of cathode are easy to cause the PEO-based battery failure. The way to deal with the different challenges on both sides of the anode and cathode is pursued all the time. In this study, we reported a new strategy to construct the PVDF/PEO/PVDF three-layer structure for solid polymer electrolyte (marked as PVDF@PEO) using PVDF as the functional “skin”. The PVDF@PEO electrolyte can effectively prevent from the lithium dendrites, and shows a stable cycling life over 1000 h in the Li/PVDF@PEO/Li cell. In addition, the PVDF@PEO electrolyte exhibits higher oxidation resistance and can be matched with high-voltage LiCoO 2 cathode. The Li/PVDF@PEO/ LiCoO 2 cell delivered a specific capacity of about 150 mAh g −1 over 150 cycles and maintained good cycling stability. Our research provides insights that the polymer electrolytes constructed with PVDF functional “skin” can simultaneously meet the challenges of both anode and cathode in solid-state lithium-ion batteries (SSLIBs).
研究领域:
材料科学
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电化学
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能源存储
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高分子化学
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固态电池
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界面工程
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DOI
高影响因子
Advanced Composites and Hybrid Materials
·
2025
·Vol. 8
·期 4
·286
·
IF 21.8
Mao Gaoqiang,Lu Jingfan,Cai Haiyan,Yu Wanjing,Tong Hui,Guo Xueyi,Zeng Leiying,Jiang Long
Increasing the operating voltage can significantly increase the energy density of LiCoO 2 , but it is accompanied by severe structural damage and interface degradation. Especially at a high voltage above 4.5 V, LiCoO 2 faces severe challenges, such as irreversible phase transition, lattice oxygen loss, and electrode–electrolyte interface evolution. Herein, a high-voltage LiCoO 2 cathode material with bulk doping and surface coating synergistic modification was designed and prepared. The doped Mg 2+ ions entered the lithium layers as pillars, stabilizing the layered framework. Meanwhile, Li 1.3 La 0.3 Ti 1.7 (PO 4 ) 3 was uniformly coated on the surface of LiCoO 2 , which is beneficial for suppressing Co 3+/2+ ion leaching and interface side reactions during cycling. Furthermore, Li 1.3 La 0.3 Ti 1.7 (PO 4 ) 3 is a fast ion conductor, which facilitates the rapid transport of lithium ions on the surface of the cathode material. Owing to the synergistic effect of Mg 2+ ion doping and Li 1.3 La 0.3 Ti 1.7 (PO 4 ) 3 coating, the orbitals of Co 3d and O 2p in LiCoO 2 crystal are changed, and the irreversible phase transition and oxygen loss are inhibited. The modified material exhibited an excellent electrochemical performance. A discharge capacity of 175.5 mAh·g −1 at 10 C rate, as well as a capacity retention of 90.14% after 200 cycles at 1 C rate, was achieved in the modified material. This work supplies a new method for developing high-voltage oxide cathodes through bulk and interfacial modification.
研究领域:
材料科学
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电化学
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储能技术
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锂离子电池
·
正极材料
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DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Xiaodong Bai,Chaoliang Zheng,Heng Zhang,Jian Liu,Panpan Wang,Baojia Xia,Jianling Li
PEO-based all-solid-state electrolytes are extensively utilized and researched owing to their exceptional safety, low-mass-density, and cost-effectiveness. However, the low oxidation potential of PEO makes the interface problem with the high-voltage cathode extremely severe. In this work, the impedance of PEO-based all-solid-state batteries with high-voltage cathode (NCM811) was studied at different potentials. The Nyquist plots displayed a gyrate arc at low-frequencies for NCM811/PEO interface. Based on the kinetic modeling, it was deduced that there is a decomposition reaction of PEO-matrix in addition to de-embedded reaction of NCM811, and the PEO intermediate product (dehydra-PEO) adsorbed on the electrode surface leading to low-frequency inductive arcs. Furthermore, the distribution of relaxation time shows the dehydra-PEO results in the kinetic tardiness of the charge transfer process in the temporal dimension. Hence, an artificial interface layer (CEI x ) was modified on the surface of NCM811 to regulate the potential of cathode/electrolyte interface to prevent the high-voltage deterioration of PEO. NCM/CEI x /PEO batteries exhibit capacity retentions of 96.0%, 84.6%, and 76.8% after undergoing 100 cycles at cut-off voltages of 4.1, 4.2, and 4.3 V, respectively. Therefore, here the failure mechanism of high-voltage PEO electrolyte is investigated by EIS and a proposed solving strategy is presented.
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Song Zhenyou,Wang Tengrui,Yang Hua,Kan Wang Hay,Chen Yuwei,Yu Qian,Wang Likuo,Zhang Yini,Dai Yiming,Chen Huaican,Yin Wen,Honda Takashi,Avdeev Maxim,Xu Henghui,Ma Jiwei,Huang Yunhui,Luo Wei
Stable solid electrolytes are essential to high-safety and high-energy-density lithium batteries, especially for applications with high-voltage cathodes. In such conditions, solid electrolytes may experience severe oxidation, decomposition, and deactivation during charging at high voltages, leading to inadequate cycling performance and even cell failure. Here, we address the high-voltage limitation of halide solid electrolytes by introducing local lattice distortion to confine the distribution of Cl − , which effectively curbs kinetics of their oxidation. The confinement is realized by substituting In with multiple elements in Li 3 InCl 6 to give a high-entropy Li 2.75 Y 0.16 Er 0.16 Yb 0.16 In 0.25 Zr 0.25 Cl 6 . Meanwhile, the lattice distortion promotes longer Li-Cl bonds, facilitating favorable activation of Li + . Our results show that this high-entropy halide electrolyte boosts the cycle stability of all-solid-state battery by 250% improvement over 500 cycles. In particular, the cell provides a higher discharge capacity of 185 mAh g −1 by increasing the charge cut-off voltage to 4.6 V at a small current rate of 0.2 C, which is more challenging to electrolytes|cathode stability. These findings deepen our understanding of high-entropy materials, advancing their use in energy-related applications.
研究领域:
材料科学
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电化学
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能源存储
·
电池技术
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DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Qiaoyi Yan,Zhengzheng Liu,Feng Wu,Renjie Chen,Li Li
Sustainable recycling of degraded LiCoO 2 (LCO) cathode is critical for minimizing the environmental footprint of lithium-ion batteries. Herein, we propose an upcycling method that converts degraded LCO into high-voltage cathodes by constructing a compositional and structural dual-gradient structure, guided by the effective ionic potential (EIP, Φ* ), a descriptor for foreign dopant diffusivity in degraded LCO lattices. Specifically, low- Φ* dopants tend to exhibit high bulk diffusivity, whereas high- Φ* dopants are retained near the surface, which promotes the formation of the compositional gradient and leads to a structural transition in LCO from a fully disordered, dense surface to an ordered layered structure in the bulk. This structure endows the upcycled cathode with a stabilized surface and low-strain bulk structure, enabling its superior electrochemical performance over the commercial counterpart at cut-off potentials of 4.6 and 4.65 V. Comprehensive kinetic and thermodynamic analyses reveal the critical role of vacancies in spent LCO for this structural engineering: Bulk vacancies facilitate the formation of deeper dopant concentration gradients within particles, while vacancies near the surface promote the development of a continuous and dense surface disordered structure. Multiscale characterizations and theoretical calculations elucidate the relationship between the engineered structure and the electrochemical stability of the upcycled cathode.
研究领域:
材料科学
·
电化学
·
可持续能源
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电池回收
·
固态化学
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PubMed
高影响因子
ADVANCED MATERIALS
·
2020
·Vol. 33
·期 1
·2002325
·
IF 27.398
Shaojie Chen,Jingxuan Zhang,Lu Nie,Xiangchen Hu,Yuanqi Huang,Yi Yu,Wei Liu
Metallic lithium (Li), considered as the ultimate anode, is expected to promise high-energy rechargeable batteries. However, owing to the continuous Li consumption during the repeated Li plating/stripping cycling, excess amount of the Li metal anode is commonly utilized in lithium-metal batteries (LMBs), leading to reduced energy density and increased cost. Here, an all-solid-state lithium-metal battery (ASSLMB) based on a garnet-oxide solid electrolyte with an ultralow negative/positive electrode capacity ratio (N/P ratio) is reported. Compared with the counterpart using a liquid electrolyte at the same low N/P ratios, ASSLMBs show longer cycling life, which is attributed to the higher Coulombic efficiency maintained during cycling. The effect of the species of the interface layer on the cycling performance of ASSLMBs with low N/P ratio is also studied. Importantly, it is demonstrated that the ASSLMB using a limited Li metal anode paired with a LiFePO 4 cathode (5.9 N/P ratio) delivers a stable long-term cycling performance at room temperature. Furthermore, it is revealed that enhanced specific energies for ASSLMBs with low N/P ratios can be further achieved by the use of a high-voltage or high mass-loading cathode. This study sheds light on the practical high-energy all-solid-state batteries under the constrained condition of a limited Li metal anode.
研究领域:
材料科学
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电化学
·
能量存储
·
电池技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Pingping Chen,Qinghui Zeng,Qingyuan Li,Ruihua Zhao,Zhenfeng Li,Xin Wen,Wen Wen,Yu Liu,Anqi Chen,Zengxi Li,Xiangfeng Liu,Liaoyun Zhang
Solid-state polymer electrolytes (SPEs) have gained considerable attention in the application of all-solid-state lithium batteries (ASSLBs), but the low ionic conductivity at room temperature and inferior interfacial compatibility largely drag the practical development of SPEs. Herein, a ketone-containing poly(allyl acetoacetate) (PAAA) based polymer electrolyte is designed and prepared for the first time. The structure of ester and ketone groups provides PAAA polymers with not only strong dissociation of lithium salts but also weak coordination interactions with Li + ions. Thus the prepared PAAA polymer electrolytes show excellent ion conductive behavior with ionic conductivity as high as 1.1 × 10 -4 S cm −1 at 30 °C. Moreover, the PAAA polymer electrolytes still maintain superior viscoelasticity without compromising mechanical integrity. When assembling cells, the reduction-tolerant poly(ethylene oxide) (PEO) polymer electrolytes are employed as interlayers between the PAAA SPEs and lithium electrodes in order to improve interfacial stability. As a result, the hierarchical polymer electrolytes possess wide electrochemical window above 4.8 V, thus matching well with LiFePO 4 or Li 1.2 Ni 0.2 Mn 0.6 O 2 high-voltage cathode. The hierarchical structure does not affect interfacial contact, and the Li/PEO-PAAA-PEO/Li cells show low interfacial resistance and stable striping/plating behavior for at least 500 h at 0.2 mA cm −2 and 60 °C. This study enriches carbonyl-based polymer electrolytes by allying ketone with ester groups, and provides guidance for designing novel high-performance polymer electrolytes for practical application.
研究领域:
材料科学
·
电化学
·
电池技术
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高影响因子
危险品化学品经营许可证（带存储）