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Register a new userThermal conductivity of intercalation, conversion, and alloying lithium-ion battery electrode materials as function of their state of charge
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Upon insertion and extraction of lithium, materials important for electrochemical energy storage can undergo changes in thermal conductivity (${Lambda}$) and elastic modulus ($it M$). These changes are attributed to evolution of the intrinsic thermal carrier lifetime and interatomic bonding strength associated with structural transitions of electrode materials with varying degrees of reversibility. Using in situ time-domain thermoreflectance (TDTR) and picosecond acoustics, we systemically study $Lambda$ and $it M$ of conversion, intercalation and alloying electrode materials during cycling. The intercalation V$_{2}$O$_{5}$ and TiO$_{2}$ exhibit non-monotonic reversible ${Lambda}$ and $it M$ switching up to a factor of 1.8 (${Lambda}$) and 1.5 ($it M$) as a function of lithium content. The conversion Fe$_{2}$O$_{3}$ and NiO undergo irreversible decays in ${Lambda}$ and $it M$ upon the first lithiation. The alloying Sb shows the largest and partially reversible order of the magnitude switching in ${Lambda}$ between the delithiated (18 W m$^{-1}$ K$^{-1}$) and lithiated states (<1 W m$^{-1}$ K$^{-1}$). The irreversible ${Lambda}$ is attributed to structural degradation and pulverization resulting from substantial volume changes during cycling. These findings provide new understandings of the thermal and mechanical property evolution of electrode materials during cycling of importance for battery design, and also point to pathways for forming materials with thermally switchable properties.
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Solid state battery technology has recently garnered considerable interest from companies including Toyota, BMW, Dyson, and others. The primary driver behind the commercialization of solid state batteries (SSBs) is to enable the use of lithium metal as the anode, as opposed to the currently used carbon anode, which would result in ~20% energy density improvement. However, no reported solid state battery to date meets all of the performance metrics of state of the art liquid electrolyte lithium ion batteries (LIBs) and indeed several solid state electrolyte (SSE) technologies may never reach parity with current LIBs. We begin with a review of state of the art LIBs, including their current performance characteristics, commercial trends in cost, and future possibilities. We then discuss current SSB research by focusing on three classes of solid state electrolytes: Sulfides, Polymers, and Oxides. We discuss recent and ongoing commercialization attempts in the SSB field. Finally, we conclude with our perspective and timeline for the future of commercial batteries.
Lithium-intercalated layered transition-metal oxides, LixTMO2, brought about a paradigm change in rechargeable batteries in recent decades and show promise for use in memristors, a type of device for future neural computing and on-chip storage. Thermal transport properties, although being a crucial element in limiting the charging/discharging rate, package density, energy efficiency, and safety of batteries as well as the controllability and energy consumption of memristors, are poorly managed or even understood yet. Here, for the first time, we employ quantum calculations including high-order lattice anharmonicity and find that the thermal conductivity k of LixTMO2 materials is significantly lower than hitherto believed. More specifically, the theoretical upper limit of k of LiCoO2 is 6 W/m-K, 2-6 times lower than the prior theoretical predictions. Delithiation further reduces k by 40-70% for LiCoO2 and LiNbO2. Grain boundaries, strains, and porosity are yet additional causes of thermal-conductivity reduction, while Li-ion diffusion and electrical transport are found to have only a minor effect on phonon thermal transport. The results elucidate several long-standing issues regarding the thermal transport in lithium-intercalated materials and provide guidance toward designing high-energy-density batteries and controllable memristors.
This study explores the potentialities of Scanning Thermal Microscopy (SThM) technique as a tool for measuring thermal transporting properties of carbon-derived materials issued from thermal conversion of organic polymers, such as the most commonly known polyimide (PI), Kapton. For quantitative measurements, the Null Point SThM (NP-SThM) technique is used in order to avoid unwanted effects as the parasitic heat flows through the air and the probe cantilever. Kapton HN films were pyrolysed in an inert atmosphere at temperatures up to 1200{deg}C to produce carbon-based residues with varying degree of conversion to free sp2 disordered carbon. The thermal conductivity of carbon materials ranges from 0.2 to 2 Wm-1K-1 depending on the temperature of the carbonization process (varied between 500{deg}C and 1200{deg}C). In order to validate the applicability of NP-SThM approach to these materials, the results were compared to those obtained with the three more traditional techniques, namely photo-thermal radiometry, flash laser analysis and micro-Raman thermometry. It was found that NP SThM data are in excellent agreement with previous work using more traditional techniques. We used the NP-SThM technique to differentiate structural heterogeneities or imperfections at the surface of the pyrolysed Kapton on the basis of measured local thermal conductivity.
The hot disk transient plane source (TPS) method is a widely used standard technique (ISO 22007-2) for the characterization of thermal properties of materials, especially the thermal conductivity, k. Despite its well-established reliability for a wide variety of common materials, the hot disk TPS method is also known to suffer from a substantial systematic errors when applied to low-k thermal insulation materials. Here, we present a combined numerical and experimental study on the influence of the geometry of hot disk sensor on measured value of low-k materials. We demonstrate that the error is strongly affected by the finite thickness and thermal mass of the sensors insulation layer was well as the corresponding increase of the effective heater size beyond the radius of the embedded metal heater itself. We also numerically investigate the dependence of the error on the sample thermal properties, confirming that the errors are worse in low-k samples. A simple correction function is also provided, which converts the apparent (erroneous) result from a standard hot disk TPS measurement to a more accurate value. A standard polyimide sensor was also optimized using both wet and dry etching to provide more accurate measurement directly. Experimentally corrected value of k for Airloy x56 aerogel and a commercial silica aerogel using the numerical correction factor derived based on the standard TPS sensor is in excellent agreement with the directly measured value from the TPS sensor using the optimized polyimide sensor. Both of these methods can reduce the errors to less than 4% as compared to around 40% error of overestimation from raw values measured with the pristine sensor. Such results show that both the numerical correction to a pristine senor or an optimized sensor are capable of providing highly accurate value of thermal conductivity for such materials.
Various bandstructure engineering methods have been studied to improve the performance of graphitic transparent conductors; however none demonstrated an increase of optical transmittance in the visible range. Here we measure in situ optical transmittance spectra and electrical transport properties of ultrathin-graphite (3-60 graphene layers) simultaneously via electrochemical lithiation/delithiation. Upon intercalation we observe an increase of both optical transmittance (up to twofold) and electrical conductivity (up to two orders of magnitude), strikingly different from other materials. Transmission as high as 91.7% with a sheet resistance of 3.0 {Omega} per square is achieved for 19-layer LiC6, which corresponds to a figure of merit {sigma}_dc/{sigma}_opt = 1400, significantly higher than any other continuous transparent electrodes. The unconventional modification of ultrathin-graphite optoelectronic properties is explained by the suppression of interband optical transitions and a small intraband Drude conductivity near the interband edge. Our techniques enable the investigation of other aspects of intercalation in nanostructures.
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