Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 24
·14565-14574
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IF 10.733
Yadong Ruan,Yang Lu,Xiao Huang,Jianmeng Su,Changzhi Sun,Jun Jin,Zhaoyin Wen
Solid-state lithium batteries (SSBs) promise high energy and power densities, as well as enhanced safety, owing to the use of Li metal and nonflammable solid-state electrolytes. In particular, cubic garnet-type Ta-substituted Li7La3Zr2O12 (LLZTO) is known for its high ionic conductivity and stability against Li metal. However, poor interfacial contact of the Li/LLZO interface is an obstacle that has come to light in the face of more demanding applications. Herein, to tackle this problem, a novel and facile strategy is demonstrated using H3PO4 to react with the Li2CO3/LiOH passivation layer of the LLZTO surface to form a uniform Li3PO4 modification layer. The Li3PO4 layer not only promotes interfacial wettability by reducing the significant difference of the surface energy, but also produces a robust solid electrolyte interphase (SEI) to inhibit lithium dendrite penetration. The symmetric cell exhibits a dramatically reduced interfacial resistance of 7.0 Ohm cm2 and ultrastable galvanostatic cycling, over 1600 hours at 0.1 mA cm−2 and over 450 hours at 0.5 mA cm−2. Besides this, hybrid solid-state full cells matched with different cathodes also displayed excellent electrochemical performances. LiFePO4 exhibited stable cycling (∼150 mA h g−1) and a good rate performance. In particular, for a S cathode, the coulombic efficiencies remained higher than 99% over 200 cycles. The use of a ternary NCM523 cathode also confirmed the anodic interfacial stability up to high voltage (4.5 V). Therefore, this facile strategy provides a stepping stone for future applications of solid-state Li-ion and Li–S batteries.
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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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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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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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiaohui Song,Rui Huang,Xin Liang,Yang Wang,Qian Hou,Binghui Ge,Qiaobao Zhang,Febri Baskoro,Afriyanti Sumboja,Rong Xiang,Hongfa Xiang,Zhimei Huang
The commercialization of Li-S batteries is constrained by the unstable interface, severe shuttle of polysulfides, and sluggish kinetic conversion reactions. Electrolyte regulation is a straightforward and efficient way to tackle those mentioned issues. Herein, a multifunctional electrolyte additive of 2,5-Dimercapto-1,3,4-thiadiazole (DMTD) is introduced in the ether-based electrolyte, which can be lithiated into Li 2 -DMTD when contacted with the Li or Li 2 S during the discharge process. The generated Li 2 -DMTD can operate as a highly ionic-conducting protective coating on the Li surface, inhibiting the formation of Li dendrites, and increasing interface stability. Then, it is reversibly oligomerized with Li 2 S, forming two organosulfur oligomers during the ensuing electrochemical process. Such a modified reaction routine can reduce the shuttle effect and speed up the reaction kinetics of Li 2 S at the cathode, preventing cathode passivation and boosting active material utilization. As a result, The Li||Li symmetric cells with DMTD exhibit about 5-fold cycle life than the reference cell under 5 mA cm −2 current density. Meanwhile, the initial charge voltage of Li||Li 2 S battery is greatly decreased from 3.7 V to 3.0 V with DMTD, and the assembled Li-S cell shows an improved capacity retention from 45.7 % to 81.2 % after 320 cycles. Therefore, this work successfully tackled the critical issues by designing functional organosulfur electrolyte additives in LSBs, which provides theoretical guidance for the electrolyte design in LSBs.
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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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ACS Nano
·
2025
·
IF 16
Hualong Wu,Jiahao Dong,Jiantao Li,Guiyang Gao,Liang Lin,Ailin Liu,Hongfei Zheng,Guanyi Wang,Junxiang Liu,Laisen Wang,Jie Lin,Khalil Amine,Dong-Liang Peng,Qingshui Xie,Jun Lu
Low initial Coulombic efficiency and severe capacity/voltage fading during cycling caused by serious irreversible oxygen release, especially in the initial cycle, and resultantly induced unstable electrode/electrolyte interfacial chemistry, largely prohibit the commercial application of high-capacity Li-rich layered oxide cathodes (LLOs). In this work, a dual reductive gas interface cotreatment strategy is applied to regulate the lattice oxygen redox activity and reversibility with a multiple defective structure design including Li/O/TM (TM = transition metal) vacancies and the intrinsic TM doping as well as a full-surface protective layer, which can suppress the irreversible TM migration and then undesirable phase transformation, resisting the corrosion of electrolyte during cycling effectively. Importantly, the introduced reversible SO32–/SO42– redox couple that provides extra capacity compensation could alleviate the distortion of oxygen-central octahedral structure and structural collapse caused by immoderate oxygen oxidation. Thus, the lattice oxygen redox chemistry is optimized, with negligible oxygen loss during the initial cycle. And the designed AS-LLO cathode with greatly enhanced structure stability shows high-capacity retentions of 99.2% at 0.3C after 100 cycles and 82.4% even after 1000 cycles at 5C. This work provides a guideline for manipulating the oxygen redox chemistry to achieve long-lifespan Li-rich layered oxide cathodes for high-energy-density lithium batteries.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Cheng Zhu,Liu Hang,Zhang Menghang,Pan Hui,Sheng Chuanchao,Li Wei,Wagemaker Marnix,He Ping,Zhou Haoshen
Rechargeable Li||I 2 batteries based on liquid organic electrolytes suffer from pronounced polyiodides shuttling and safety concerns, which can be potentially tackled by the use of solid-state electrolytes. However, current all-solid-state Li||I 2 batteries only demonstrate limited capacity based on a two-electron I − /I 2 polyiodides chemistry at elevated temperatures, preventing them from rivaling state-of-the-art lithium-ion batteries. Herein, we report a fast, stable and high-capacity four-electron solid-conversion I − /I 2 /I + chemistry in all-solid-state Li||I 2 batteries at room temperature. Through the strategic use of a highly conductive, chlorine-rich solid electrolyte Li 4.2 InCl 7.2 as the catholyte, we effectively activate the I 2 /I + redox couple. This activation is achieved through a robust I-Cl interhalogen interaction between I 2 and the catholyte, facilitated by an interface-mediated heterogeneous oxidation mechanism. Moreover, apart from serving as Li-ion conduction pathway, the Li 4.2 InCl 7.2 catholyte is demonstrated to show a reversible redox behavior and contribute to the electrode capacity without compromising its conductivity. Based on the I − /I 2 /I + four-electron chemistry, the as-designed all-solid-state Li||I 2 batteries deliver a high specific capacity of 449 mAh g -1 at 44 mA g -1 based on I 2 mass and an impressive cycling stability over 600 cycles with a capacity retention of 91% at 440 mA g -1 and at 25 °C.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jiaqi Wu,Bin Liu,Jian Qian,Yuan Tao,Chenxiao Lin,Ruicheng Wang,Jie Gao,Yonggao Xia
The rapid growth of the electric vehicle industry is generating large quantities of spent lithium-ion batteries. However, these batteries have complex compositions, making current recycling processes inefficient at recovering valuable metals. Herein, lithium and aluminum from spent lithium-ion batteries were directly extracted and used to prepare aluminum-based lithium-ion adsorbents through a facile co-precipitation approach for the first time. This approach eliminates aluminum interference with nickel, cobalt, and manganese, simplifying the recovery of cathode materials. The developed aluminum-based lithium adsorbent displayed excellent ion selectivity and stability, with an adsorption capacity of 7.44 mg/g from a 500 mg/L lithium solution at 30℃, maintaining 96.18 % capacity after seven adsorption cycles. Additionally, this adsorption process follows pseudo-second-order kinetics and the Sips model. Cation competition experiments showed the ionic selectivity follow the sequence Li + > Mg 2+ > Na + > K + > Ca 2+ . This approach enables a one-step regeneration and utilization of lithium-aluminum resources from spent lithium-ion batteries, potentially lowering recycling costs and holds promise for large-scale applications.
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INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Wenfeng Zhou,Qing Zhang,Wen-Dong Yao,Huaiguo Xue,Sheng-Ping Guo
One of the key scientific issues for exploration of novel infrared nonlinear optical (NLO) crystals is to obtain ones with good hybrid NLO behaviors. Herein, we report four diamond-like Ag-based sulfides via stepwise Li substitution of Ag in Ag2ZnSnS4, including Ag2ZnSnS4 (1), (Li1.22Ag0.78)ZnSnS4 (2), (Li1.58Ag0.42)ZnSnS4 (3), and Li2ZnSnS4 (4). With the increase of Li content, the sulfide’s noncentrosymmetric crystal structure changes from tetragonal I42m for 1, to orthorhombic Pmn21 for 2 and 3, and to monoclinic Pn for 4. Accordingly, their NLO responses are improved along with the increase of Li content, viz. from non-NLO-active for 1, to non-phase-matchable for 2 and 3, and to phase-matchable for 4. Their optical band gaps also increase regularly. The relationship between their chemical compositions, crystal structures, and NLO activities is investigated by means of chemical structural analysis and theoretical calculation. This work offers a new systematic case for designing promising NLO-active compounds via rarely adopted cation’s stepwise partial substitution and understanding the chemical composition–structure–NLO property relationship.
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JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Licheng Zhang,Jinfeng Li,Ruirui Liu,Yongquan Zhou,Yuze Zhang,Lianmin Ji,Lijuan Li
Efficient separation of lithium from salt lake brine with high Na/Li ratio is of great importance for the development of new energy industry. Liquid-liquid extraction using β-diketone system was proved to be an effective approach to separate lithium from alkaline metal ions, while the separation effect of lithium to alkali earth ions needs further investigation. In this work we proposed an extraction process using HBTA/TRPO system to recovery lithium from salt lake brine with high Na/Li ratio. The conditions of saponification, extraction, eluting, stripping and regeneration process was optimized by equilibrium experiments. Through the process, lithium, calcium and magnesium were extracted to the organic phase and then stripped step by step to obtain lithium-rich solution, then the stability of the process and organic was tested by cycle experiments, the results indicated the proposed method was effective and stable. Theoretical study based on density functional theory was conducted to expound the extraction selectivity to different metal ions, and the energy change, electrostatic potential and Mulliken charge of the complexes was obtained, the calculated results suggested the stability of the complexes followed the sequence: Mg 2+ > Ca 2+ > Li + > Na + > K + , which is consistent with the experimental results. The present work may provide a novel way to efficiently recover lithium from salt lake brine with high Na/Li ratio.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Yangyang Wang,Xue Wang,Bingcheng Ge,Jianxin Guo,Carlos Fernandez,Qiuming Peng
The Li–CO2 battery is a potential energy storage device that not only possesses a theoretical energy density as high as 1876 W h kg–1 but also alleviates the consumption of fossil resources by converting the greenhouse gas CO2 into electric energy. However, some technique bottlenecks, such as high overpotential, low recyclability, and low energy density, severely prohibit its application rhythm. Here, we prepare a binder-free MXene–MnO2 composite film using vacuum-assisted filtration and in situ reduction, which can be used as a freestanding cathode for Li–CO2 batteries. This MXene–MnO2 film electrode bestows good cycle stability (∼220 cycles), high specific capacity, and lower overpotential (∼0.89 V) in Li–CO2 batteries. Both experimental tests and first-principles calculations reveal that the enhanced electrochemical properties are associated with three aspects. First, the MXene–MnO2 film offers a high electrical conductivity and porous structure, which provide fast transport channels for electrons and ions. Then, the replacement of Mn by Ti increases the adsorption of Li ions, which facilitates the rapid decomposition of Li2CO3. Finally, the synergistic effect of MXene and MnO2 exposes a large number of active sites, which increases the capacity of Li–CO2 batteries. Therefore, this self-supporting strategy on the MXene composite paves a way to develop high-performance Li–CO2 batteries.
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