ACS Nano
·
2025
·
IF 16
Shengxi Li,Yanxin Shang,Xuening Ren,Anqi Zhao,Nan Chen,Li Li,Feng Wu,Renjie Chen
Aqueous lithium-ion batteries (ALIBs) have attracted increasing attention for their inherent safety and environmental benefits. However, the narrow electrochemical stability window of water (1.23 V) imposed by hydrogen evolution reaction (HER) and high melting point (0 °C) critically limits the energy density and low-temperature operation. In this work, we report an electrolyte design principle that water activity can be suppressed by strengthening the O–H bonds between water molecules and regulating the pH. A strong polar solvent N,N-dimethylformamide (DMF) interacts with H2O through intermolecular hydrogen bonds, thereby reinforcing the covalent O–H bonds of water. Meanwhile, KOH renders the electrolyte alkaline, inhibiting water dissociation kinetics and consequently raising the HER overpotential. The designed LD1.7W0.6–KOH electrolyte exhibits a freezing point below −82 °C and expanded electrochemical stability window of 4.3 V. The 2.5 V aqueous LiMn2O4/Li4Ti5O12 full cell delivers 2000 cycles at a rate of 6 C with a Coulombic efficiency of 99% at 30 °C and over 1950 cycles at 0 °C. This work offers atomic-level insights into alkaline HER while providing guidance for advancing low-temperature aqueous batteries by tuning the electrolyte structures.
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高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Chenglin Wei,Mengdi Sun,Baoguo Zhang,Zhangyong Yan,Zihao Dang,Yongkang Xu,Lin Wu,Ya Hu
Benefiting from the low cost and natural abundance of sulfur, as well as its excellent theoretical performance metrics - including a capacity of 1675 mAh g −1 and an energy density of 2600 Wh kg −1 - lithium-sulfur (Li-S) batteries have attracted considerable attention for next-generation energy storage. However, their practical deployment is severely hindered by the intrinsic shuttle effect of lithium polysulfides (LiPSs), which leads to the loss of active materials and poor cycling stability. In this work, we report a facile hydrothermal-calcination strategy to synthesize porous nanosheet-structured Fe-doped nickel oxide (Fe-NiO) as a functional separator modifier for Li-S batteries. The polar nature of NiO enables strong chemical interactions with LiPSs, effectively anchoring polysulfides on the cathode side and suppressing the shuttle effect. Furthermore, Fe doping significantly increases the density of surface active sites, thereby enhancing the adsorption and catalytic conversion of LiPSs into insoluble Li 2 S 2 /Li 2 S species, which promotes redox kinetics and mitigates capacity fading. When applied to Li-S cells, the Fe-NiO-modified separator markedly improves the electrochemical performance, delivering a high reversible capacity of 1150 mAh g −1 at 0.2C, an excellent rate capability of 505 mAh g −1 at 5C, and outstanding long-term stability with a minimal capacity decay of 0.091 % per cycle over 500 cycles at 1C. This study presents a simple and scalable strategy for separator engineering, providing a promising pathway toward high-performance Li-S batteries.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Yang Tingting,Yang Maolin,Huang Zhongyuan,Wang Rui,Ji Wenhai,Lu Peng-Han,Zeng Tao,Li Zenan,Wang Jun,Dunin-Borkowski Rafal E.,Jin Lei,Xiao Yinguo
Layered Li-rich Mn-based (LRM) oxides are promising cathode materials for next-generation high-energy batteries. However, their commercialization is hindered by intrinsic structural issues and subsequent degradation processes. In order to address the degradation mechanisms, we use operando neutron diffraction and scanning transmission electron microscopy to follow the microstructural degeneration of the LRM oxides in a prepared full cell with a graphite anode. The methods enable both real-time phase analysis and structural evolution mapping across a wide field of view. The LRM oxide is observed to initially have a partially ordered Li 2 MnO 3 -like structure with multiple planar defects. It transitions from an ordered monoclinic phase to a disordered rhombohedral phase as a result of irreversible Li + migration and transition metal rearrangement during cycling. Especially after the first full charge, the interlayer (001) twining-like structures and local intralayer frustrations formed. Over cycling, the intralayer frustrations further develop into pore-like microstructures along the {012} twinning boundary in the bulk of the particles, which contributes significantly to performance reduction. The results clarify the link between microstructure degradation and performance loss and provide valuable insights into the optimization of high-performance cathodes.
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Energy Technology
·
2025
·
IF 3.6
Ming Yan,Haoyu Chen,Yu Zhu,Yuxiao Deng,Zhuanlong Yan,Ziyi Lu,Yanlin Chen
In this study, NH 2 –SiO 2 @Ti 3 C 2 T x core–shell microspheres with different Ti 3 C 2 T x contents are prepared by coating Ti 3 C 2 T x nanosheets on the surfaces of SiO 2 microspheres using an electrostatic self-assembly method. The structures, elemental compositions, and microscopic morphologies of NH 2 –SiO 2 @Ti 3 C 2 T x microspheres are investigated by X-Ray diffraction, Fourier-transform infrared spectroscopy, field-emission scanning electron microscopy, and X-Ray photoelectron spectroscopy. The results show that Ti 3 C 2 T x nanosheets are uniformly coated on the surfaces of the SiO 2 microspheres, and the surfaces of the SiO 2 microspheres are modified by NH 2 . The maximum specific surface area of NH 2 –SiO 2 @Ti 3 C 2 T x composite doped with 15 wt% Ti 3 C 2 T x is 29.937 m 2 g −1 , with an average pore size of 0.11848 cm 3 g −1 . The electrochemical performance test results show that after 100 cycles at a C rate of 0.2C, the specific capacity of the NH 2 –SiO 2 @Ti 3 C 2 T x anode material increases by 270.1% compared to that of SiO 2 , reaching 142.5 mAh g −1 . Compared with SiO 2 , the NH 2 –SiO 2 @Ti 3 C 2 T x materials have higher electrical conductivities and Li ion diffusion rates, thereby improving their rate performances, and the discharge specific capacities and cycling stability are superior to those of the SiO 2 anode material.
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ACS Applied Polymer Materials
·
2022
·
IF 4.855
Jiuqing Liu,Lishun Bai,Junying He,Cheng Wang,Qihou Li,Feifei Song,Zikun Hong,Ya Chen,Fanli Zeng,Chen Cheng,Zehao Chen
Lithium–oxygen (Li–O2) batteries, having an ultrahigh theoretical energy density (3500 Wh kg–1), have gained a lot of attention. However, its application is seriously obstructed by pivotal issues like instability of lithium metal anode, low energy efficiency, and electrolyte decomposition. Herein, a separator modification method based on interfacial polymerization (IP) was proposed by us to solve these issues. The obtained interfacial polymerization layer shows good ion-selective permeability on the surface of the polyetherimide (PEI) separator, and the ion transport of the larger EMIM+, TFSI–, and BF4– between the electrodes is greatly inhibited. Consequently, the representative P2-PEI separator presents the best cycle performance and the Li–O2 battery assembled with it can stably operate over 135 cycles, even under a current density of 0.05 mA cm–2 and a limited specific capacity of 1000 mAh g–1.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 14
·9354-9363
·
IF 12.732
Zheng Si,Baozhao Shi,Jin Huang,Ye Yu,You Han,Jinli Zhang,Wei Li
Nickel-rich layered oxides (LiNixCoyMn1−x−yO2) (x ≥ 0.8, NCM) are intensively developed cathode materials for lithium-ion batteries owing to their high energy and low price, however, their application is impeded by poor cycle stability. Herein we explored a Ti and F co-doped Li(Ni0.8Co0.1Mn0.1)O2 cathode through a solid phase reaction using the precursors of TiO2 and NH4F. Combining the characterization results of XRD, Ar sputtering assisted XPS, HRTEM, in situ XRD, etc, it is illustrated that Ti4+ and F− co-modification can synergistically modulate the lattice parameter and the Ni2+/Li+ mixing degree for the Li(Ni0.8Co0.1Mn0.1)O2 cathode material. Particularly, density functional theory (DFT) calculations demonstrate that Ti and F co-doping is beneficial to form stable crystal structures with a layered phase and rock-salt phase. Ti4+ and F− co-dopants induce the formation of an ultra-thin rock-salt phase on the cathode surface, which provides a protective layer on the nickel-rich cathode surface, so as to enhance the electrochemical performance. The optimal Ti4+ and F− co-doped sample 0.5Ti@0.5F-NCM shows a superior discharge capacity of 202.2 mA h g−1 at 1C and 45 °C, and a capacity retention of 88.1% after 200 cycles, much higher than the retention of 45.2% for NCM. For 0.5Ti@0.5F-NCM, the lithium-ion diffusion coefficients after the 1st and 100th cycles are 2.67 × 10−11 cm2 s−1 and 7.14 × 10−12 cm2 s−1 respectively, larger than those of the pristine NCM (1.37 × 10−11 cm2 s−1 and 4.52 × 10−12 cm2 s−1). The Ti4+ and F− co-doping can suppress the H2–H3 phase change of the cathode during the charge and discharge process and reduce the charge transfer resistance. The results provide a simple and feasible design strategy via cation@anion dopants to boost the electrochemical performance of nickel-rich cathodes for lithium-ion batteries.
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Nanoscale
·
2021
·Vol. 13
·期 30
·13065-13071
·
IF 7.79
Kun Wang,Yongyuan Hu,Jian Pei,Fengyang Jing,Zhongzheng Qin,Huabin Kong,Jinli Wang,Yumin Zhou,Gang Chen
High-capacity Co2VO4 has become a potential anode material for lithium-ion batteries (LIBs), benefiting from its lower output voltage during cycling than other cobalt vanadates. However, the application of this new conversion-type electrode is still hampered by its inherent large volume variation and poor kinetics. Here, a 2D–2D heterostructure building strategy has been developed to enhance the electrode performance of Co2VO4 through construction of Co/Co2VO4 nanocomposites converted from the in situ phase separation of Co2V2O7·3.3H2O nanosheets. Co/Co2VO4 based on face-to-face contact exhibits the optimized stacking configuration, where Co nanocrystals give gaps of several nanometers between stacked Co2VO4 nanosheets, enabling full contact with the electrolyte, a shorter transport path of lithium ions and more reactive sites. With this design, Co/Co2VO4 anodes deliver outstanding reversible capacity (750 mA h g−1 at 1 A g−1) with ultrahigh capacity retention rate, and excellent cycle stability at high rate (520 mA h g−1 at 5 A g−1 retained after 400 cycles). An “active center's charge transfer—capacity compensation” model was proposed based on capacity analysis, XPS depth analysis and HRTEM observation to uncover the fundamental reason of the excellent cycle performance. This in situ 2D–2D heterostructure constructing strategy may open up the possibility for designing high-performance LIBs.
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CARBON
·
2015
·
IF 6.196
Feng Wu,Lili Shi,Daobin Mu,Hongliang Xu,Borong Wu
A novel hierarchical structure carbon/sulfur composite is presented based on carbon fiber matrices, which are synthesized by electrospinning. The fibers are constituted with hollow graphitized carbon spheres formed using catalytic Ni nano-particles as hard templates. Sulfur is loaded to the carbon substrates via thermal vaporization. The structure and composition of the hierarchical carbon fiber/S composite are characterized with X-ray diffraction, scanning electron microscopy, transmission electron microscopy , Raman spectroscopy , and nitrogen adsorption isotherms . The electrochemical performance is evaluated by cyclic voltammetry and galvanostatic charge–discharge. The results exhibit an initial discharge capacity of 845 mA h g −1 at 0.25 C (420 mA g −1 ), with a retention of 77% after 100 cycles. A discharge capacity of 533 mA h g −1 is still attainable when the rate is up to 1.0 C. The good cycling performance and rate capability are contributed to the uniform dispersion of sulfur, the conductive network of carbon fibers and hollow graphitized carbon spheres.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Shuting Li,Manting Li,Limin Chen,Jianying Yang,Zhao Wang,Fan Yang,Linhong He,Xinchun Li
Artificial nanochannels have seen great progress in energy storage, molecular filters, nanofluidic diodes, and biosensors. Precisely recognizing and transporting molecules or ions underpin the basis of artificial nanochannels. Here, we report highly efficient Li + responsive nanochannels by design of functionalized porous anodic aluminum oxide (AAO) membranes. The 12-crown-4 unit was tethered to the synthesized spiropyran molecule, creating a smart Li + responsive element, photochromic crowned spiropyran (CE-SP). The crown unit can specifically bind with Li + while exempting the harassment of other metallic cations; and importantly, the spiropyran moiety possesses reversible photochemistry response, adding the flexibility to regulate ion transport behaviors. Upon the ultraviolet light stimulus, hydrophobic CE-SP molecules transform to positively charged crowned merocyanine (CE-MC), which can further convert to oxygen-negative ions in weak alkaline environment, thereby forming O - -Li + interaction. Such structural evolutions enable to deftly tune the surface charge and wettability of the nanochannels, and thus ingeniously manipulate Li + recognition profiled by ionic current signal. Moreover, electrically-driven release of the captured Li + can be realized in an amiable condition, showing controllable capture-to-release ability. Finite element simulation unveils the fundamental mechanisms of ion transport pertaining to Li + recognition events in the nanoconfinement. This work thus paves a way to construct high-performance Li + -selective nanodevice, and holds promise for Li + -related electrochemistry energy research.
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高影响因子
Journal of Energy Chemistry
·
2019
·
IF 5.162
Xi Zheng,Ying Liao,Zhongru Zhang,Jianping Zhu,Fucheng Ren,Huajin He,Yuxuan Xiang,Yezhen Zheng,Y. Yang
Ethyl-(2,2,2-trifluoroethyl) carbonate (ETFEC) is investigated as a solvent component in high-voltage electrolytes for LiNi 0.5 Mn 1.5 O 4 (LNMO). Our results show that the self-discharge behavior and the high temperature cycle performance can be significantly improved by the addition of 10% ETFEC into the normal carbonate electrolytes, e.g., the capacity retention improved from 65.3% to 77.1% after 200 cycles at 60 °C. The main reason can be ascribed to the high stability of ETFEC which prevents large oxidation of the electrolyte on the cathode surface . In addition, we also explore the feasibility of electrolytes using single fluoriated-solvents with and without additives. Our results show that the cycle performance of LNMO material can be greatly improved in 1 M LiPF 6 + pure ETFEC-solvent system with 2 wt% ethylene carbonate (EC) or ethylene sulfate (DTD). The capacity retention of the LNMO materials is 93% after 300 cycles, even better than that of carbonate-based electrolytes. It is shown that the additives are oxidized on the surface of LNMO particles and contribute to the formation of cathode/electrolyte interphase (CEI) films. This composite CEI film plays a crucial role in suppressing the serious decomposition of the electrolyte at high voltage.
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ZEITSCHRIFT FUR NATURFORSCHUNG SECTION A-A JOURNAL OF PHYSICAL SCIENCES
·
2022
·Vol. 77
·期 7
·715-722
·
IF 1.712
Jinghao Zhuang,Wenlin Feng,Bo Zhou,Qili Zhang,Chong Liu,Yao Gong
A series of CaSr(WO 4 ) 2 : Eu 3+ and CaSr(WO 4 ) 2 : Eu 3+ , Li + phosphors with different Eu 3+ or Eu 3+ /Li + molar contents were successfully synthesized by high-temperature solid-state reaction. Through a series of characterization methods, the composition, structure and luminescence characteristics of the sample are obtained. Upon excitation at 393 nm, the strong red light corresponding to the 5 D 0 → 7 F 2 transition of Eu 3+ can be observed. The effect of Li + charge compensation on the photoluminescence of the sample is studied. The strongest red emission is obtained through 1% Eu 3+ and 1% Li + doping. All of the results indicate that Li + charge compensation can effectively enhance the red emissions intensity of Eu 3+ -doped CaSr(WO 4 ) 2 phosphors.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Xue Ye,Jing Wu,Jianneng Liang,Yipeng Sun,Xiangzhong Ren,Xiaoping Ouyang,Dazhuan Wu,Yongliang Li,Lei Zhang,Jiangtao Hu,Qianling Zhang,Jianhong Liu
Low cycling Coulombic efficiency (CE) and messy Li dendrite growth problems have greatly hindered the development of anode-free Li-metal batteries (AFLBs). Thus, functional electrolytes for uniform lithium deposition and lithium/electrolyte side reaction suppression are desired. Here, we report a locally fluorinated electrolyte (LFE) medium layer surrounding Cu foils to tailor the chemical compositions of the solid-electrolyte interphase (SEI) in AFLBs for inhibiting the immoderate Li dendrite growth and to suppress the interfacial reaction. This LFE consists of highly concentrated LiTFSI dissolved in a fluoroethylene carbonate and/or succinonitrile plastic mixture. The CE of Cu||LiNi0.8Co0.1Mn0.1O2 (NCM811) AFLB increased to a high level of 99% as envisaged, and the cycling ability was also highly improved. These improvements are facilitated by the formation of a uniform, dense, and LiF-rich SEI. LiF possesses high interfacial energy at the LiF/Li interface, resulting in a more uniform Li deposition process as proved by density functional theory (DFT) calculation results. This work provides a simple yet utility tech for the enhancement of future high-energy-density AFLBs.
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高影响因子
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