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Refractive Index Measurement of Lithium Ion Battery Electrolyte with Etched Surface Cladding Waveguide Bragg Gratings and Cell Electrode State Monitoring by Optical Strain Sensors
摘要： In this scientific publication, a new sensor approach for status monitoring, such as state of charge and state of health, of lithium ion batteries by using special Bragg gratings inscribed into standard optical glass fibers is presented. In addition to well-known core gratings, embedded into the anode of 5 Ah lithium ion pouch cells as a strain monitoring unit, the manufacturing of a surface cladding waveguide Bragg grating sensor incorporated into the cell’s separator, that is sensitive to changes of the refractive index of the surrounding medium, is demonstrated. On the basis of the experiments carried out, characteristics of the cell behavior during standard cyclization and recognizable marks in subsequent post-mortem analyses of the cell components are shown. No negative influence on the cell performance due to the integrated sensors have been observed; however, the results show a clear correlation between fading cell capacity and changes of the interior optical signals. Additionally, with the novel photonic sensor, variations in the electrolyte characteristics are determinable as the refractive index of the solution changes at different molar compositions. Furthermore, with the manufactured battery cells, abuse tests by overcharging were conducted, and it was thereby demonstrated how internal battery sensors can derive additional information beyond conventional battery management systems to feasibly prevent catastrophic cell failures. The result of the research work is an early stage photonic sensor that combines chemical, mechanical and thermal information from inside the cell for an enhanced battery status analysis.
关键词： lithium ion,battery aging,cladding waveguide,battery electrolyte,optical sensors,battery safety,fiber Bragg grating,electrode active material,status monitoring
更新于2025-11-28 14:23:57
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Efficiency and Quality Issues in the Production of Black Phosphorus by Mechanochemical Synthesis: A Multi-Technique Approach
摘要： Black phosphorus (BP) is a two-dimensional material potentially of great interest for applications in the fields of energy, sensing, and microelectronics. One of the most interesting methods to obtain BP is the conversion from red phosphorus (RP) by means of high-energy mechanochemical synthesis. To date, however, this synthesis process was not well characterized. In this work, starting from the mathematical model of energy transfer during the ball milling process, we investigate the effects on RP → BP conversion of three experimental parameters, the rotation speed, the milling time, and the weight ratio between the spheres and the milled material (BtPw ratio). The efficiency of the conversion process was verified by solid-state NMR, Raman spectroscopy, and X-ray diffraction. Whereas the first two parameters have a minor importance, the BtPw ratio plays a primary role in the RP → BP conversion. Yields approaching 100% can be obtained also with short milling times (15 min) and adequate rotation speed (e.g., 500 r.p.m.), provided that the BtPw ratio >40:1 is used. These results confirm the energy sustainability of the mechanochemical synthesis approach.
关键词： diffraction,solid-state NMR,anode,post-lithium ion batteries,Raman,mechanochemical synthesis
更新于2025-11-21 11:18:25
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Optimization of a parallel-plate RF probe for high resolution thin film imaging
摘要： Choosing an MR probe with the correct dimensions and high sensitivity is critical for magnetic resonance imaging, especially high resolution thin film imaging. In this work, a parallel‐plate resonator has been optimized for strength and uniformity of the B1 magnetic field. The parallel‐plate resonator is designed for high resolution imaging in the direction perpendicular to the plates. The optimization process was undertaken through simulation with CST Micro Wave Studio, followed by experiment. A 400 μm capillary tube, filled with doped water, was used for testing the optimized probe in a 2.4 T magnet. It is shown that increasing the width of the copper leads connected to the plates increases the homogeneity of the B1 magnetic field by almost 90%. The best approach to increase the sensitivity and the homogeneity of the probe was to maintain the dimensions of the plates and copper leads but to add additional capacitors at the corners to distribute the current. This approach produces a 40% stronger B1 magnetic field and increases the homogeneity by almost 85%. The experimental B1 magnetic field of the parallel‐plate prototype agrees within 20% of the value found through simulation, for specified power. The experimental MRI results show that it is possible to achieve a nominal resolution of 10 μm between the plates for suitable samples using the optimized probe. The optimized parallel‐plate resonator, combined with a phase encode SE SPI method, may be used for high resolution studies of lithium‐ion transport in the electrolyte solution of lithium‐ion batteries.
关键词： lithium-ion battery,optimization,MRI,parallel-plate resonator
更新于2025-09-23 15:23:52
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Nanoparticle Emissions from Metal-Assisted Chemical Etching of Silicon Nanowires for Lithium Ion Batteries
摘要： As one of the most promising anode materials for high-capacity lithium ion batteries (LIBs), silicon nanowires (SiNWs) have been studied extensively. The metal-assisted chemical etching (MACE) is a low-cost and scalable method for SiNWs synthesis. Nanoparticle emissions from the MACE process, however, are of grave concerns due to their hazardous effects on both occupational and public health. In this study, both airborne and aqueous nanoparticle emissions from the MACE process for SiNWs with three sizes of 90 nm, 120 nm, and 140 nm are experimentally investigated. The prepared SiNWs are used as anodes of LIB coin cells, and the experimental results reveal that the initial discharge and charge capacities of LIB electrodes are 3636 and 2721 mAh g-1 with 90 nm SiNWs, 3779 and 2712 mAh g-1 with 120 nm SiNWs, and 3611 and 2539 mAh g-1 with 140 nm SiNWs. It is found that, for 1 kW h of LIB electrodes, the MACE process for 140 nm SiNWs produces a high concentration of airborne nanoparticle emissions of 2.48 × 109 particles/cm3; the process for 120 nm SiNWs produces a high mass concentration of aqueous particle emissions, with a value of 9.95 × 105 mg/L. The findings in this study can provide experimental data of nanoparticle emissions from the MACE process for SiNWs for LIB applications, and can help the environmental impact assessment and life cycle assessment of the technology in the future.
关键词： Lithium ion batteries (LIBs),Metal-assisted chemical etching (MACE),Nanoparticle emissions,Silicon nanowires (SiNWs)
更新于2025-09-23 15:23:52
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In Situ Measurement of Phase Boundary Kinetics during Initial Lithiation of Crystalline Silicon through Picosecond Ultrasonics
摘要： Studying the kinetics of phase transformation and phase boundary propagation during initial lithiation of silicon electrodes in lithium ion batteries is relevant to understanding their performance. Such studies are usually challenging due to the difficulties in measuring the phase boundary velocity in the interior of the sample. Here we introduce a non-invasive, in situ method to measure the progression of the phase boundary in a planar specimen geometry while maintaining well-controlled lithium flux and potential. We developed an apparatus integrating an electrochemical cell with picosecond ultrasonics to probe the propagating phase boundary in real time. Phase propagation during initial lithiation of crystalline silicon, which is an example of a high capacity anode, is investigated. The primary objective of this manuscript is to report on the experimental technique development and some preliminary results. For lithiation normal to the (100) plane, we observe the phase boundary velocity to be approximately 12 pm/s and x to be 3.73 in LixSi under galvanostatic lithiation with a current density of 40 μA/cm2. The growth rate of the lithiated phase and the reaction rate coefficient are examined using a Deal-Grove type model.
关键词： Lithium ion battery,In situ,Phase boundary propagation,Crystalline silicon,Picosecond ultrasonics
更新于2025-09-23 15:23:52
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Easy preparation of nanoporous Ge/Cu3Ge composite and its high performances towards lithium storage
摘要： Nanoporous Ge/Cu3Ge composite is fabricated simply through selective dealloying of GeCuAl precursor alloy in dilute alkaline solution. The as-made Ge/Cu3Ge is characterized by three dimensional (3D) bicontinuous network nanostructure which comprises of substantial nanoscale pore voids and ligaments. Owing to the 3D porous architecture and the introduction of well-conductive Cu3Ge, the lithium storage performances of Ge are dramatically enhanced in terms of higher cycling stability and superior rate performance. Nanoporous Ge/Cu3Ge anode delivers steady capacities above 1000 mA h g-1 upon cycling for 70 loops at 400 mA g-1. In particular, after 300 cycles at the high rate of 3200 mA g-1 the capacity retention for Ge/Cu3Ge is able to reach a maximum of 99.3%. On the contrary, the pure nanoporous Ge encounters severe capacity decay. In view of the outstanding energy storage performances and easy preparation, nanoporous Ge/Cu3Ge exhibits great application potential as an advanced anode in lithium storage related technologies.
关键词： dealloying,anode,lithium ion batteries,nanoporous,germanium
更新于2025-09-23 15:23:52
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GeO <sub/>2</sub> Encapsulated Ge Nanostructure with Enhanced Lithium-Storage Properties
摘要： Germanium (Ge)-based nanostructures, especially those with germanium dioxide (GeO2), have drawn great interest for applications in lithium (Li)-ion batteries due to their ultrahigh theoretical Li+ storage capability (8.4 Li/Ge). However, GeO2 in conventional Ge(s)/GeO2(c) (where (c) means the core and (s) means the shell) composite anodes with Ge shell outside GeO2 undergoes an irreversible conversion reaction, which restricts the maximum capacity of such batteries to 1126 mAhg?1 (the equivalent of storing 4.4 Li+). In this work, a porous GeO2(s)/Ge(c) nanostructure with GeO2 shell outside Ge cores are successfully fabricated utilizing the Kirkendall effect and used as a lithium-ion battery anode, giving a substantially improved capacity of 1333.5 mAhg?1 at a current density of 0.1 Ag?1 after 30 cycles and a stable long-time cycle performance after 100 cycles at a current density of 0.5 A g?1. The enhanced battery performance is attributed to the improved reversibility of GeO2 lithiation/delithiation processes catalyzed by Ge in the properly structured porous GeO2(s)/Ge(c) nanostructure.
关键词： porous,Kirkendall effect,nanostructures,lithium ion batteries,GeO2(s)/Ge(c)
更新于2025-09-23 15:22:29
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Probing Electrolyte Solvents at Solid/Liquid Interface Using Gap-Mode Surface-Enhanced Raman Spectroscopy
摘要： Understanding the aprotic solution structures at the immediate vicinity of solid/liquid interface (SLI) is critically important for next generation lithium ion battery development. Yet, it is still challenging to investigate the carbonate chemical profiles close to the diffuse layer (about 10 nm) of the electrical double layer at SLI due to the lack of a ultrahigh surface sensitive tool. In this work, we demonstrate the structures of commonly used carbonate solvents (ethylene carbonate (EC) and diethyl carbonate (DEC)) and a carbonate additive (fluoroethylene carbonate (FEC)) in a commercial Li-ion battery electrolyte can be determined at ～17 nm above the electrode surface. This is only enabled by a nanogap surface-enhanced Raman spectroscopy (SERS) technique based on a monolayer gold nanoparticle (Au NP) ensemble. The SERS enhancement factor (EF) of those carbonates was found to depend on the molecular polarizability, with the maximum EF at ～105 found for EC and FEC. Despite their alike chemical structures, this monolayer Au NP SERS substrate is fully capable of discrimiating the different Raman finger prints of EC and FEC. Compared to EC, several vibration modes in FEC, such as C-C skeletal deformation, ring breathing band and C=O stretching band, shift to higher frequencies because of the displacement of a hydrogen atom by a much heavier fluorine atom in a methylene bridge. This counterintuitive observation against the commonly used “ball and spring” model in vibrational spectroscopy is mostly due to the increased bond strength in the FEC ring versus that of EC. A second order empirical polynomial best describes the correlation between the SERS band integration of EC or DEC molar concentration. Our findings open up new opportunities for in-depth understanding of the electrolyte molecular vibrational behaviors at direct solid/liquid interface and developing advanced electrolytes for next generation lithium-ion batteries.
关键词： carbonate solvents,electrolyte,solid/liquid interface,lithium-ion battery,surface-enhanced Raman spectroscopy
更新于2025-09-23 15:22:29
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Metaheuristic <i>Ab Initio</i> Optimum Search for Doping Effects in Nanocarbons
摘要： We have developed a combined approach of metaheuristic optimization algorithms (MOA), such as the genetic algorithm, with an ab-initio materials simulation engine. Concurrent run of the ab-initio calculations with each different parameter set selected by the MOA searches the optimum condition within a given input-parameter space. Using this methodology, the optimum dopant and its position/structure at a graphene edge are found to be a multiple N-atoms doping at graphitic sites, which predicts to lead to better charging/discharging performance when it is used as an anode material of Li-ion battery.
关键词： genetic algorithm,lithium-ion battery,nano-carbon,ab-initio simulation,doping effect
更新于2025-09-23 15:22:29
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Electrochemical and Structural Investigation on Ultrathin ALD ZnO and TiO <sub/>2</sub> Coated Lithium-Rich Layered Oxide Cathodes
摘要： Ultrathin coatings (1.5 ± 0.3 nm) of titanium dioxide and zinc oxide were deposited on lithium-rich layered oxide cathodes (Li1.2Mn0.6Ni0.2O2, LLO) by atomic layer deposition (ALD). The structures, electrochemical performances, and thermal stabilities of these coatings were investigated. An ultrathin uniform coating was obtained for TiO2 but not for ZnO because of di?erences in the layer growth mechanism. Regarding the initial charge?discharge curves under a current density of 0.04 C rate, the TiO2 coated samples exhibited a higher discharge capacity, 242 mAhg?1, compared with the ZnO coated samples, 220 mAhg?1, or the pristine samples, 228 mAhg?1. Both coated samples exhibited more stable cycling performance and thermal stability than the pristine samples. After 80 cycles under 0.5 C rate, the TiO2 and ZnO coated samples were found to have higher capacity retention (～94% and 78%, respectively) than the pristine samples (68%). The reaction temperature of the exothermic peak of the TiO2 and ZnO coated samples at 4.8 V shifted to 280 °C with heat release of 88.7 J/g for TiO2 and 270 °C with heat release of 154.6 J/g for ZnO. This is compared with an exothermic peak at 258 °C with heat release of 253.5 J/g for the pristine sample. In particular, an enhanced rate capability was only observed for the TiO2 coated samples. When the current densities were higher than 2 C rate, the TiO2 coated samples exhibited superior capacities than the pristine and ZnO coated samples. At a current density of 5 and 10 C rate, the capacities were found to be 120 and 95 mAhg?1. The improved electrochemical performances were mainly attributed to lower resistance ?lm. This feature lead to more preactivation of the charge transfer, which resulted from the layer morphology of the TiO2 LLO, smoother electron transport, and suppression of more side reactions, when compared with the island structure of the ZnO ?lm.
关键词： ZnO,Cathode,Atomic layer deposition,Lithium-rich layered oxides,TiO2,Lithium ion battery
更新于2025-09-23 15:21:21