JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yunsong Ran,Tong Liu,Shangyan Zhou,Chunliang Yang,Xiaodan Wang,Dong Zou,Jiling Song,Hao Wen,Yuandong Zheng,Fei Liu
The growing demand for advanced energy storage technologies has accelerated significant advances in solid-state lithium metal batteries (SSLMBs). Among which, Li 1+X Al X Ti 2-X (PO 4 ) 3 (LATP) solid-state electrolyte has attracted much attention due to its competitive room-temperature (RT, 25 °C) Li + conductivity, air stability and economics. In this study, a composite electrolyte consisting of uniformly eLATP nanosheets embedded in a PVDF/LiTFSI matrix has address the limitations of ionic conductivity and interfacial stability in quasi-solid-state lithium metal batteries (QSSLMBs). Significantly, the eLATP nanosheets are uniformly distributed in the PVDF/eLATP composite, which greatly improves the ionic transport capacity and mechanical strength. Simultaneously, such uniform distribution ensures uniform current density and stress distribution, which effectively inhibits the growth of lithium dendrites. As expected, the Li/PVDF/eLATP/Li symmetric cells achieve an outstanding long-term lifespan of 6500 h at 0.1 mA cm −2 , with 1000 h of efficient operation even at 0.5 mA cm −2 at RT. In addition, full cells paired with the LFP cathodes achieve 91.08 % capacity retention after 1000 cycles at 1C, with an ultralow average decay rate of 0.00036 % per cycle at 5C(RT). Furthermore, the Li||NCM cells demonstrate exceptional cycling stability under 2C conditions at 25 °C. Overall, a novel composite solid-state electrolyte with excellent electrochemical properties has been engineered.
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高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Xiaomi Tang,Kaiwei Yang,Zihao Zhang,Hong Chen,Xueqing Li,Guandan Lu,Yuelong Xu,Xiangjing Zhang,Xiaoyang Xu
Covalent organic frameworks (COFs), with customizable/functionalized skeleton and tunable/ordered channel structure, demonstrate high capability for rapid Li + intercalation/deintercalation to address the challenge of dynamic charge storage imbalance between battery-type anodes and capacitor-type cathodes in lithium-ion capacitors (LICs). Herein, we firstly synthesized hydrophenazine (HP)-linked COF HA-DQ powders with a pore size of 2.2 nm, featuring a fully conjugated crystalline D-A skeleton with enhanced local polarization. Further, the –Cl group with strong electronegativity was introduced into form COF HA-Cl to employ its synergistic interaction with active N sites for further inducing pronounced local polarization, which facilitates rapid Li + intercalation/deintercalation for ensuring accelerated anodic kinetics (simulated Li + diffusion energy barrier value of 0.018 eV in COF HA-Cl ). Then, following the COF HA-Cl anode prelithiated to 800 mAh g −1 , the constructed AC//COF HA-Cl LICs deliver the optimal capacity performance, such as a high energy density of 24.4 Wh kg −1 at a power density of 100 W kg −1 , and exhibited strong good cycling stability, maintaining 82.6 % of its initial capacity after 2000 cycles. This work addressed kinetic and capacity imbalance in LIC electrodes through molecular and pore structure design of COF materials, paving the way for future miniaturized and wearable electronics.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Miao Wang,Chen Mou,Kai Wang,Wenjun Wang,Zhenyue Zhang,Ruan Chi
The rapid development of electrical vehicle urgently requires high-performance Li-ion battery that can operate over a wide temperature range. Herein, disodium hydrogen phosphate dodecahydrate encapsulated with silica were embedded to polyvinylidene fluoride as DHPD@SiO 2 /PVDF (DSP) membrane. The DSP based cell exhibited superior average discharge capacity (132 mAhg −1 ) and coulombic efficiency (96%) under room temperature as the silica shell in nanocapsules could enhance electrolyte affinity, separator porosity and mechanical strength to reduce interfacial resistance and increase Li-ion conductivity. Furthermore, the DSP membrane is leakage-proof with a comparable latent heat due to the synergistic effect between porous silica and hydrophobic PVDF. When battery discharged in cold environment, heat release from hydrate salt solidification could mitigate the damage to alleviate discharge capacity degradation by 57.7%. The present design of separator that integrating electrochemical properties promotion and low-temperature thermal management provides a novel and efficient strategy to enhance wide-temperature-range performance of battery.
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Small
·
2024
·
IF 13
Li Luo,Kui Liang,Zeba Khanam,Xincheng Yao,Muhammad Mushtaq,Ting Ouyang,M.-Sadeeq Balogun,Yexiang Tong
Flexible lithium-ion batteries (FLIBs) are intensively studied using free-standing transition metal oxides (TMOs)-based anode materials. However, achieving high areal capacity TMO-based anode materials is yet to be effectively elucidated owing to the poor adhesion of the active materials to the flexible substrate resulting in low active mass loading, and hence low areal capacity is realized. Herein, a novel monolithic rutile TiO 2 microparticles on carbon cloth (ATO/CC) that facilitate the flower-like arrangement of TiO 2 nanowires (denoted ATO/CC/OTO) is demonstrated as high areal capacity anode for FLIBs. The optimized ATO/CC/OTO anode exhibits high areal capacity (5.02 mAh cm −2 @0.4 mA cm −2 ) excellent rate capability (1.17 mAh cm −2 @5.0 mA cm −2 ) and remarkable cyclic stability (over 500 cycles). A series of morphological, kinetic, electrochemical, in situ Raman, and theoretical analyses reveal that the rational phase boundaries between the microparticles and nanowires contribute to promoting the Li storage activity. Furthermore, a 16.0 cm 2 all-FLIB pouch cell assembled based on the ATO/CC/OTO anode and LiNiCoMnO 2 cathode coated on ATO/CC (ATO/CC/LNCM) exhibits impressive flexibility under different folding conditions, creating opportunity for the development of high areal capacity anodes in future flexible energy storage devices.
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高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Shuangshuang Zhu,Zhenxi Li,Shilun Gao,Tianhui Cheng,Ruijie Guo,Dandan Yang,Wei Niu,Junli Yu,Huabin Yang,Peng-Fei Cao
Quasi-solid polymer electrolytes (QSPEs) have been attracted significant attentions due to their benefits for simultaneously improved safety and energy density of batteries. Developing electrolytes capable of forming a stable solid electrolyte interphase (SEI) layer is a great challenge for QSPE-based lithium (Li) metal batteries (LMBs). Herein, unlike previously reports that the reconstruction of Li + solvation structures in QSPE requires time-consuming bottom-up polymer synthesis, in current study, a facile approach has been developed to reconstruct the Li + solvation structures in QSPE by adjustment of the salt concentrations. The high proportion of Li + -anion complexes can effectively accelerate interfacial Li + diffusion, mitigate the decompositions of organic solvents and induces the formation of a LiF-rich SEI layer, contributing to suppressed Li-dendrite growth. As a result, the Li/QSPE-3/LiFePO 4 (LFP) cell performs an ultralong lifespan with capacity retention of 77.4% over 3000 cycles at 1 C. With a high-voltage LiCoO 2 cathode, the cell can stably cycle over 200 cycles at 25 °C (capacity retention of ∼83.8%). With accelerated ion transport dynamics due to the reconstructed Li + solvation structure, the QSPE-3 (the salt concentration is 3 M) is applicable in a wide temperature range. The Li/QSPE-3/LFP full cell exhibits 58.1% and 102.6% of discharge capacity at −15 and 90 °C, respectively, compared to those operated at 25 °C. This study demonstrates a facile yet effective approach on enhancing electrode/electrolyte interfacial stability, enabling the LMBs with simultaneously enhanced safety and high energy density.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Li Peiying,Hao Jinjin,He Shuang,Chang Zenghua,Li Xiaolei,Wang Rennian,Ma Wen,Wang Jiantao,Lu Yuhao,Li Hong,Zhang Liqun,Zhou Weidong
Polymer-based quasi-solid-state electrolytes (QSSE) are believed to be the most feasible candidates for solid-state batteries, but they are hindered by relatively lower ionic conductivity and narrower electrochemical window. Here, we synthesize a series of ether-free acrylates containing Li + -ligands for high-voltage-stable QSSEs. Our findings demonstrate that the polymer-involved solvation structure is critical in determining the ionic conductivity, and low-temperature crystallization of the polymer can be used for non-destructive life extension of batteries. The prepared polymers do not contain ether unit and exhibit a polymerization degree of 99% in cells without residual double-bonded monomer, endowing them with high antioxidation capability and compatibility with high-voltage positive electrodes including LiNi 0.85 Co 0.075 Mn 0.075 O 2 , 4.6 V LiCoO 2 and 4.8 V Li 1.13 Ni 0.3 Mn 0.57 O 2 . The confinement of liquid in QSSEs effectively suppresses the interfacial reactions, but the residual interface reactions still gradually consume liquid electrolytes and cause capacity fading, due to the limited diffusion of the confined solvent to wet the interface. Through crystallizing the polymer matrices at −50 °C, the confined liquid in QSSEs is released and re-wets the Li-metal/polymer interface, thereby recovering the capacity and extending the life of solid-state batteries in a non-destructive manner.
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ACS Nano
·
2024
·
IF 15.8
Yuansheng Shi,Fushan Geng,Yang Sun,Pengfeng Jiang,Wang Hay Kan,Wei Tong,Xueyi Lu,Guoyu Qian,Nan Zhang,Bin Wei,Bingwen Hu,Dapeng Cao,Xia Lu
The irrational utilization of an anionic electron often accompanies structural degradation with an irreversible cation migration process upon cycling in sodium-layered oxide cathodes. Moreover, the insufficient understanding of the anionic redox involved cation migration makes the design strategies of high energy density electrodes even less effective. Herein, a P3-Na0.67Li0.2Fe0.2Mn0.6O2 (P3-NLFM) cathode is proposed with the in-plane disordered Li distribution after an in-depth remolding of the Li ribbon-ordered P3-Na0.6Li0.2Mn0.8O2 (P3-NLM) layered oxide. The disordered Li sublattice in the transition metal slab of P3-NLFM leads to the dispersed |O2p orbitals, the lowered charge transfer gap, and the suppressed phase transition at high voltages. Then the enhanced Mn–O interaction and electronic stability are disclosed by the crystal orbital Hamilton population (COHP) analysis at high voltage in P3-NLFM. Furthermore, ab initio molecular dynamics (AIMD) simulation suggests the order/disorder of the transition metal layer is highly correlated with the stability of the Li sublattice. The cross-layer migration and loss of Li in P3-NLM are suppressed in P3-NLFM to enable the high reversibility upon cycling. As a result, the P3-NLFM delivers a high capacity of 163 mAh g–1 without oxygen release and an enhanced capacity retention of 81.9% (vs 42.9% in P3-NLM) after 200 cycles, which constitutes a promising approach for sustainable oxygen redox in rechargeable batteries.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wentao Lin,Jiapeng Liu,Lichun Xue,Yueqing Li,Haoze Yu,Yongqiang Xiong,Dengjie Chen,Francesco Ciucci,Jing Yu
Liquid organic electrolytes commonly employed in commercial Li-ion batteries suffer from safety issues such as flammability and explosions. Replacing liquid electrolytes with nonflammable electrolytes has become increasingly attractive in the development of safe, high-energy Li-metal batteries (LMBs). In this work, nonflammable, robust, and flexible composite polymer–polymer electrolytes (PPEs) were successfully fabricated by flame-retardant solution casting with polyimide (PI) and polyvinylidene fluoride (PVDF). The optimized nonflammable PPEs (e.g., PPE-50) demonstrate not only good mechanical properties (i.e., a high tensile strength of 29.6 MPa with an elongation at break of 87.2%), but also high Li salts dissolubility, the former of which ensures the suppression of Li dendrites, while the latter further improves the ionic conductivity (∼1.86 × 10 −4 S cm −1 at 30 °C). The resulting symmetric cells (Li|PPE-50|Li) offer excellent Li stripping and plating stability for 1000 h at 0.5 mA cm −2 /0.25 mAh cm −2 and 600 h at 2.0 mA cm −2 /1.0 mAh cm −2 . In addition, the LiFePO 4 |PPE-50|Li half cells show high cycling performance (e.g., a reversible discharge capacity of 135.9 mAh g −1 after 300 cycles at 1C) and rate capability (e.g., 117.2 mAh g −1 at 4C). The PPE-50 is also compatible with a high-voltage cathode (e.g., LiNi 0.5 Mn 0.3 Co 0.2 O 2 ), and the resulting batteries demonstrate long-term cycling stability with a high cut-off voltage of 4.5 V vs. Li/Li + . Because of the incorporation of a mechanically robust and thermally stable PI, a polar PVDF, and flame-retardant trimethyl phosphate (TMP) within PPEs, as well as the coordination between Li salts and TMP, and the interaction between Li salts and polymers (especially between Li bis(oxalato)borate) and PI, as well as the bis(oxalato)borate anion and PI), PPEs show great potential for practical and high-energy LMBs without safety concerns.
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Small
·
2023
·Vol. 19
·期 23
·2300106
·
IF 13.3
Ziqin Liu,Xin Dong,Jing Wen,Pu Hu,Chaoqun Shang
The high reactivity of Li metal and the inhomogeneous Li deposition leads to the formation of Li dendrites and “dead” Li, which impedes the performance of Li metal batteries (LMBs) with high energy density. The regulating and guiding the Li dendrite nucleation is a desirable tactic to realize concentrated distribution of Li dendrites instead of completely inhibiting dendrite formation. Here, a Fe-Co-based Prussian blue analog with hollow and open framework (H-PBA) is employed to modify the commercial polypropylene separator (PP@H-PBA). This functional PP@H-PBA can guide the lithium dendrite growth to form uniform lithium deposition and activate the inactive Li. In details, the H-PBA with macroporous structure and open framework can induce the growth of lithium dendrites via space confinement, while the positive Fe/Co-sites lowered by polar cyanide (−CN) of PBA can reactivate the inactive Li. Thus, the Li|PP@H-PBA|Li symmetric cells exhibit long-term stability at 1 mA cm −2 for 1 mAh cm −2 over 500 h. And the Li-S batteries with PP@H-PBA deliver favorable cycling performance at 500 mA g −1 for 200 cycles.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 62
·15479-15483
·
IF 5.236
Jingfang F. Zhou,Rukang K. Li
Graphical LiNaTiTa 2 P 2 O 13 displays an open framework comprised of staggered [Ti 1/3 Ta 2/3 O 3 ] ∞ layers and PO 4 tetrahedra with a herringbone-like stacking pattern, similar to monophosphate niobium bronzes. The existence of pentagonal tunnels, hosting the Li + and Na + ions, endow LiNaTiTa 2 P 2 O 13 a moderate ion transport capability (4.67×10 −4 S/cm at 823 K). In addition, the layers constituted by corner-sharing TiO6 and TaO6 octahedra endow a possibility as being photo-catalyst. The successful substitution of Nb for Ta results in the optical absorption red-shifted towards visible range with a narrowing band gap comparable to that of TiO 2 (3.2 eV). Herein, we report a detailed structural, electric, thermal and optical analysis of a titanium and tantalum phosphate LiNaTiTa 2 P 2 O 13 . The title compound is comprised of typical ReO 3 -type layers constituted by corner-sharing TiO 6 and TaO 6 octahedra, bridged by PO 4 tetrahedra, and the structure is closely related to monophosphate niobium bronzes. The existence of pentagonal tunnels, hosting the Li + and Na + ions, endows LiNaTiTa 2 P 2 O 13 a moderate ion transportation behavior (4.67×10 −4 S/cm at 823 K). In addition, the successful substitution of Nb for Ta in LiNaTiTa 2 P 2 O 13 results in the optical absorption red-shift towards visible range with a narrowing band gap, which may provide a route of isomorphic replacement to band engineering for photo-catalysis.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2017
·Vol. 164
·期 7
·A1695
·
IF 3.259
Yanhua Zhang,Fei Chen,Dunjie Yang,Wenping Zha,Junyang Li,Qiang Shen,Xulong Zhang,Lianmeng Zhang
All-solid-state lithium batteries (ASLBs) have been dramatically attracted recently for its ability of solving the safety issues in traditional lithium ion batteries using liquid electrolyte. However the poor Li+ transportation between the active material particles in the cathode greatly deteriorate the specific capacity of ASLBs. Herein, we design a composite cathode composed of polyethylene oxide (PEO) and LiCoO2 (LCO) in which a three-dimensional (3D) continuous Li+ conductive network forms. With the decrease of the LCO: PEO ratio, the 3D Li+ conductive network gradually becomes continuous, and the corresponding discharge capacity increase from 50 to 136 mAh g−1. At LCO: PEO = 6:1 and 4:1, the corresponding ASLBs has a very high discharge capacity of 136 and 124 mAh g−1, respectively, representing approximately 98% and 90% of the theoretical discharge capacity. The capacity retention after 5 cycles is 97%∼98% of the 2nd cycle, which confirms stable cycle performance of the battery. The FTIR results show that, in the composite cathode, the LCO particles transport Li+ cations by coordinating CO functional group in PEO chains. Compared with other optimized ASLBs based on LLZO solid elctrolyte, our battery has higher specific capacity while being tested under the highest current rate.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Liping Wu,Chuyue Cai,Xi Yu,Zihe Chen,Yuxin Hu,Fang Yu,Shengjun Zhai,Tao Mei,Li Yu,Xianbao Wang
Lithium sulfur batteries (LSBs) are regarded as one of the most promising energy storage devices due to the high theoretical capacity and energy density. However, the shuttling lithium polysulfides (LiPSs) from the cathode and the growing lithium dendrites on the anode limit the practical application of LSBs. To overcome these challenges, a novel three-dimensional (3D) honeycombed architecture consisting of a local interconnected Co3O4 successfully assembled into a scalable modified layer through mutual support, which is coated on commercial separators for high-performance LSBs. On the basis of the 3D honeycombed architecture, the modified separators not only suppress effectively the “shuttle effects” but also allow for fast lithium-ions transportation. Moreover, the theoretical calculations results exhibit that the collaboration of the exposed (111) and (220) crystal planes of Co3O4 is able to effectively anchor LiPSs. As expected, LSBs with 3D honeycombed Co3O4 modified separators present a reversible specific capacity with 1007 mAh g–1 over 100 cycles at 0.1 C. More importantly, a high reversible capacity of 808 mAh g–1 over 300 cycles even at 1 C is also acquired with the modified separators. Therefore, this proposed strategy of 3D honeycombed architecture Co3O4 modified separators will give a new route to rationally devise durable and efficient LSBs.
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