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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Degradation in Ni-Rich LiNi 1– x – y Mn x Co y O 2 /Graphite Batteries: Impact of Charge Voltage and Ni Content

Ni-rich LiNi 1– x–y Mn x CoyO 2 (NMC) materials are attractive as cathodes for Li-ion batteries due to their high energy density and low Co content. However, these materials may display poor electrochemical reversibility relating to structural and interfacial instabilities. The influence of Ni content and level of delithiation during charge on degradation mechanisms and relevance to electrochemical cycling behavior are probed for LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) and LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode materials in a full cell configuration under two upper voltage limits (4.1 and 4.3 V). The combined use of dQ/dV analysis of electrochemical voltage profiles, operando XRD, and postcycling scanning electron microscopy (SEM) measurements indicates that a major contributor to capacity fade is the large anisotropic volume change from an H2 $\leftrightarrows$ H3 phase transition and associated mechanical degradation particularly for NMC811. Notably, transition metal dissolution and deposition on the negative electrode are found to correlate with the structural changes occurring in the cathode under high voltage charge. X-ray photoelectron spectroscopy (XPS) analyses of the cycled cathodes reveal a more organic-rich cathode–electrolyte interphase (CEI) when cycling to 4.3 V with lower relative amounts of LiF. Surface reconstruction is not a significant factor under these cycling conditions as determined by soft X-ray absorption spectroscopy (sXAS) analysis. The results emphasize the opportunity to match the electrochemical test parameters with the specific NMC active material to mitigate degradation and extend cycle life.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Understanding the Mechanism of Secondary Cation Release from the (001) Surface of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 : Insights from First-Principles

The transformations of complex metal oxides in aqueous settings must be studied to form a chemical understanding of how technologically relevant nanomaterials impact the environment upon disposal. Owing to the inherent heterogeneity and structural complexity of the ternary intercalation material Li(Ni x Mn y Co 1-x-y )O 2 (NMC), the mechanisms of chemical processes at the solid–water interfac e are challenging to model. Here, density functional theory (DFT) + solvent ion methodology is used to study the energetics of stepwise release of two surface metals following unique pathways. Further, the study spans different combinations of metal removal and also considers unique patterns of defects formed by modeling the NMC surface in supercells. The approach here also considers the equilibration of the surface with the surroundings between successive metal removals. A key finding is that a second metal removal prefers to proceed at a metal lattice site adjacent to the initial defect, and this is attributed in part to how the resulting slab with two metal vacancies maintains the most antiferromagnetic couplings between the remaining Ni/Mn.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Surface Structure, Morphology, and Stability of Li(Ni 1/3 Mn 1/3 Co1/3)O 2 Cathode Material

Layered Li(Ni 1-x-y Mn x Co y )O 2 (NMC) oxides are promising cathode materials capable of addressing some of the challenges associated with next-generation energy storage devices. In particular, improved energy densities, longer cycle-life, and improved safety characteristics with respect to current technologies are needed. However, sufficient knowledge on the atomic-scale processes governing these metrics in working cells is still lacking. Herein, Density Functional Theory (DFT) is employed to predict the stability of several low-index surfaces of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 (NMC111) as a function of Li and O chemical potentials. Predicted particle shapes are compared with those of single crystal NMCs synthesized under different conditions. The most stable surfaces for stoichiometric NMC111 are predicted to be the non-polar (104), the polar (012) and (001), and the reconstructed, polar (110) surfaces. Results indicate that intermediate spin Co 3+ ions lower the (104) surface energy. Furthermore, it was found that removing oxygen from the (012) surface was easier than from the (104) surface, suggesting a facet dependence on surface-oxygen vacancy formation. In conclusion, these results give important insights into design criteria for the rational control of synthesis parameters as well as establish a foundation on which future, mechanistic studies of NMC surface instabilities can be developed.

25 ENERGY STORAGE↗
DOE OSTI2019

Distinction between Intrinsic and X-ray-Induced Oxidized Oxygen States in Li-Rich 3d Layered Oxides and LiAlO 2

Resonant inelastic X-ray scattering (RIXS) at the O K-edge is considered a prime technique to identify bulk oxidized oxygen formation, but its fundamental interpretation is not straightforward. In this study, we intentionally induce RIXS signatures of oxidized oxygen upon beam exposure in LiAlO 2 polymorphs that are easily distinguished because of their wide band gaps. After careful consideration of beam exposure effects on Li[Li 0.144 Ni 0.136 Mn 0.544 Co 0.136 ]O 2 (LR-NMC), we conclude that oxidized oxygen features are inherent at high states of charge and are lost upon aggressive beam exposure. The extracted oxidized oxygen line shapes from our X-ray irradiation studies for both LiAlO 2 (induced) and LR-NMC (inherent) are found to have an additional oxidized oxygen RIXS feature not observed in O 2 gas studies. This study highlights the unique insight of O K-edge RIXS into determining the nature and stability of oxidized oxygen states.

36 MATERIALS SCIENCE↗
DOE OSTI2020

How Bulk Sensitive is Hard X-ray Photoelectron Spectroscopy: Accounting for the Cathode–Electrolyte Interface when Addressing Oxygen Redox

Sensitivity to the `bulk' oxygen core orbital makes hard X-ray photoelectron spectroscopy (HAXPES) an appealing technique for studying oxygen redox candidates. Various studies have reported an additional O 1s peak (530-531 eV) at high voltages, which has been considered a direct signature of the bulk oxygen redox process. Here, we find the emergence of a 530.4 eV O 1s HAXPES peak for three model cathodes, Li 2 MnO 3 , Li-rich NMC, and NMC 442, that shows no clear link to oxygen redox. Instead, the 530.4 eV peak for these three systems is attributed to transition metal reduction and electrolyte decomposition in the near-surface region. Claims of oxygen redox relying on photoelectron spectroscopy must explicitly account for the surface sensitivity of this technique and the extent of the cathode degradation layer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Calibration-Free Quantitative Analysis of Lithium-Ion Battery (LiB) Electrode Materials Using Laser-Induced Breakdown Spectroscopy (LIBS)

Recent years have seen a surge in the demand for high-performance battery electrode materials for automotive and various electronic device applications. Improving battery performance requires precise knowledge of the structure–composition properties of active electrode materials. To this effect, quantitative and precise estimation of the composition of advanced electrode materials, containing trace amounts of dopants, provide immense value toward developing next-generation high-capacity battery materials. Herein, we demonstrate the application of calibration-free laser-induced breakdown spectroscopy (LIBS) as a powerful analytical tool for rapid and reliable quantitative spectrochemical characterizations of layered Li metal oxide cathodes containing Mo and Cr dopants (<5 atom %). Specifically, we employ the LIBS using an internal calibration methodology to establish the quantitative elemental ratios of major (Ni, Mn, Co) and trace dopant (Cr, Mo) transition metals to bulk Li contents in diverse cathode material samples such as LiNi 0.5 Mn 0.5 O 2 (NM-50/50), LiNi 0.33 Mn 0.33 Co 0.33 O 2 (NMC), LiNi 0.317 Mn 0.317 Co 0.317 Cr 0.05 O 2 (Cr-doped NMC), and LiNi 0.5– x /2 Mn 0.5– x /2 Mo x O 2 ( x = 0.03, 0.04, 0.05) (Mo-doped NM-50/50) that were synthesized via sol–gel routes. The LIBS-estimated elemental compositions are in good agreement with the nominal stoichiometric values. Furthermore, ex situ LIBS characterizations presented here pave the path for future high-efficacy application of calibration-free quantitative LIBS for rapid in situ analyses of elemental composition changes in battery electrode materials under operation that need not resort to off-site analytical techniques requiring cumbersome sample preparations and/or external standards.

25 ENERGY STORAGE↗
DOE OSTI2019

Unveiling the Role of Al 2 O 3 in Preventing Surface Reconstruction During High-Voltage Cycling of Lithium-Ion Batteries

Recent achievements in high-energy batteries have been made by using Ni-rich NMC cathodes (LiNi x Mn y Co 1–x–y O 2 with x > 0.5) in conjunction with higher cell voltages. However, these gains have come at a cost of fast capacity fade and poor rate performace. In our previous study, we showed that Al 2 O 3 ALD coatings on LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) and LiNi 0.8 Co 0.15 Al 0.05 O 2 (NCA) cathodes prevented surface phase transitions, reduced impedance, and extended cycle life in high voltage cells. In this work, neutron diffraction (ND), X-ray photoelectron spectroscopy (XPS), and electron energy loss spectroscopy (EELS) are used to fully investigate the mechanism by which ALD surface coatings mitigate NMC811 cathode degredation. Refinement of ND patterns indicated no changes in the bulk crystal structure of cycled cathodes with or without the Al 2 O 3 coating. Rather, the improved performance of ALD-coated cathodes is clearly due to surface stabilization. EELS established that all three transition metal oxidation states were reduced at the surface of the uncoated cathode after cycling, whereas the coated cathode showed no changes in surface oxidation states relative to the bulk. The surface coatings also prevented transition metal dissolution and crossover. XPS analysis of the anode harvested from cycled cells with uncoated cathodes showed significant amounts of Mn deposited within the SEI. In contrast, no Mn could be detected on the anodes cycled with coated cathodes. These results affirm that ALD coatings can effectively reduce the reactivity of the NMC surface and prevent detrimental side reactions that shorten battery cycle life.

25 ENERGY STORAGE↗
DOE OSTI2022

Stability Enhancement and Microstructural Modification of Ni-Rich Cathodes via Halide Doping

In this study, elemental doping is an effective strategy to modify surface and bulk chemistry in NMC cathode materials. By adding small amounts of lithium halide salts during the calcination process, the Ni-rich NMC811 cathode is doped with Br, Cl, or F halogens. The dopant type has a significant impact on the lithiation process and heavily influences the final cathode porosity and surface morphology. Utilizing a variety of electrochemical, surface, and bulk characterization techniques, it is demonstrated that an initial content of 5 mol % LiBr or LiCl in the lithium source is effective in improving capacity retention while also providing excellent rate performance. The improvements are attributed to a substantial increase in specific surface area, the formation of a stable cathode electrolyte interface (CEI) layer, and suppressed surface reconstruction. In addition, the particle microstructure is better equipped to handle cyclic volume changes with increased values of critical crack lengths. Overall, it is demonstrated that anion doping via the addition of lithium halide salts is a facile approach toward Ni-rich NMC modification for enhanced cathode performance.

25 ENERGY STORAGE↗
DOE OSTI2018

Accelerated Evolution of Surface Chemistry Determined by Temperature and Cycling History in Nickel-Rich Layered Cathode Materials

Nickel-rich layered cathode materials have the potential to enable cheaper and higher energy lithium ion batteries. However, these materials face major challenges (e.g., surface reconstruction, microcracking, potential oxygen evolution) that can hinder the safety and cycle life of lithium ion batteries. Many studies of nickel-rich materials have focused on ways to improve performance. Understanding the effects of temperature and cycling on the chemical and structural transformations is essential to assess the performance and suitability of these materials for practical battery applications. This study is focused on the spectroscopic analysis of surface changes within a strong performing LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode material. We found that surface chemical and structural transformations (e.g., gradient metal reduction, oxygen loss, reconstruction, dissolution) occurred quicker and deeper than expected at higher temperatures. Even at lower temperatures, the degradation occurred rapidly and eventually matched the degradation at high temperatures. Despite these transformations, our performance results showed that a better performing nickel-rich NMC is possible. Establishing relationships between the atomic, structural, chemical, and physical properties of cathode materials and their behavior during cycling, as we have done here for NMC811, opens the possibility of developing lithium ion batteries with higher performance and longer life. Finally, our study also suggests that a separate, systematic, and elaborate study of surface chemistry is necessary for each NMC composition and electrolyte environment.

25 ENERGY STORAGE↗
DOE OSTI2021

Degradation by Kinking in Layered Cathode Materials

Layered cathode materials are commonly used in lithium and sodium ion batteries, but they are prone to degradation under electrochemical cycling during battery operation. Here we report a new type of degradation mechanism through the electrochemically induced mechanical buckling and delamination cracking of intercalation layers in a P2 Na 0.7 -Ni 0.3 Mn 0.6 Co 0.1 O 2 (Na-NMC) cathode material. Kinks form in the delaminated layers due to severe local bending, and each kink consists of a vertical array of dislocations, resulting from an easy slip between transition metal oxide layers. In situ mechanical compression experiments directly reveal the kink formation due to strong mechanical anisotropy parallel and perpendicular to the intercalation layers in single-crystal Na-NMC. In situ electrochemical experiments indicate that kinks form during the desodiation process. Our results unveil a new mechanism of electrochemically induced mechanical degradation stemming from weak interlayer bonding in layered cathode materials. In conclusion, this work has broad implications for the mitigation of degradation associated with irreversible interlayer slip in layered cathode materials.

25 ENERGY STORAGE↗
DOE OSTI2013

Correlating cation ordering and voltage fade in a lithium–manganese-rich lithium-ion battery cathode oxide: a joint magnetic susceptibility and TEM study

Structure–electrochemical property correlation is presented for lithium–manganese-rich layered–layered nickel manganese cobalt oxide (LMR–NMC) having composition Li1.2Co0.1Mn0.55Ni0.15O2 (TODA HE5050) in order to examine the possible reasons for voltage fade during short-to-mid-term electrochemical cycling. The Li1.2Co0.1Mn0.55Ni0.15O2 based cathodes were cycled at two different upper cutoff voltages (UCV), 4.2 V and 4.8 V, for 1, 10, and 125 cycles; voltage fade was observed after 10 and 125 cycles only when the UCV was 4.8 V. Magnetic susceptibility and selected-area electron diffraction data showed the presence of cation ordering in the pristine material, which remained after 125 cycles when the UCV was 4.2 V. When cycled at 4.8 V, the magnetic susceptibility results showed the suppression of cation ordering after one cycle; the cation ordering diminished upon further cycling and was not observed after 125 cycles. Selected-area electron diffraction data from oxides oriented towards the [0001] zone axis revealed a decrease in the intensity of cation-ordering reflections after one cycle and an introduction of spinel-type reflections after 10 cycles at 4.8 V; after 125 cycles, only the spinel-type reflections and the fundamental O3 layered oxide reflections were observed. A significant decrease in the effective magnetic moment of the compound after one cycle at 4.8 V indicated the presence of lithium and/or oxygen vacancies; analysis showed a reduction of Mn4+ (high spin/low spin) in the pristine oxide to Mn3+ (low spin) after one cycle. The effective magnetic moment was higher after 10 and 125 cycles at 4.8 V, suggesting the presence of Mn3+ in a high spin state, which is believed to originate from distorted spinel (Li2Mn2O4) and/or spinel (LiMn2O4) compounds. The increase in effective magnetic moments was not observed when the oxide was cycled at 4.2 V, indicating the stability of the structure under these conditions. This study shows that structural rearrangements in the LMR–NMC oxide happen only at higher potentials (4.8 V, for example) and provides evidence of a direct correlation between cation ordering and voltage fade.

Mohanty, Debasish↗
DOE OSTI2019

Single-crystal based studies for correlating the properties and high-voltage performance of Li[Ni x Mn y Co 1₋x₋y ]O 2 cathodes

Safe and stable cycling of lithium-ion battery cathodes at high voltages is essential for meeting next-generation energy storage demands, yet the lack of fundamental understanding of the correlation of a material's properties and reactivities largely hinders current progress. Here, we demonstrate how single-crystal samples with well-controlled physical characteristics can be used to unambiguously establish the relationships among specific properties, surface chemistry and electrochemical performance, enabling rational design of better performing cathode materials. Layered Li[Ni x Mn y Co 1₋x₋y ]O 2 (NMC) crystals, with four different particle shapes of an octahedron (Oct), truncated octahedron (T-Oct), polyhedron (Poly) and platelet (Plate), were prepared to vary the presence of (104), (001) and (012) family facets on the surface. This represents the first experimental verification of NMC morphologies that were theoretically calculated in the past. Systematic studies on the impact of isolated physical properties reveal the important roles of the Ni content, particle size and facet on surface stability and electrochemical performance. We show that compared to (012) surface dominated samples, high-voltage cycling stability was much improved on the (001) dominated Plate sample, suggesting that replacing the (012) surface with lower energy (001) and/or (104) surfaces can be effective in stabilizing NMCs during high energy applications. Our study moreover provides insights into how tailoring a material's surface properties can be used as an important route in balancing cathode capacity and stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

A functional SrF 2 coated separator enabling a robust and dendrite-free solid electrolyte interphase on a lithium metal anode

An unstable solid electrolyte interphase (SEI) and accompanying Li metal dendrites are the key impediments to commercialization of high-energy lithium metal batteries (LMBs). We employ a strontium fluoride (SrF 2 ) microsphere coated polypropylene (PP) separator to stabilize the SEI and to prevent dendrites from growing. This approach is tested with Li∥Cu half-cells, Li∥Li symmetrical cells, and Li∥NMC full LMBs, there being a major improvement in each case. The Li∥Cu cell with SrF 2 maintains a stable coulombic efficiency (CE) of 80% after 100 cycles, when tested at 0.25 mA cm -2 to a capacity of 0.5 mA h cm -2 . By comparison, the uncoated PP reference has a CE of 10% in cycle 60. The Li∥Li cell with SrF 2 exhibits a markedly smaller voltage polarization and is able to stably cycle for approximately 340 h vs. the reference which begins to display severe voltage instability at 200 h. The Li∥NMC full LMB with SrF 2 shows an initial discharge capacity of 173 mA h g -1 , with 167 mA h g -1 (96.5%) being retained after 200 cycles at 200 mA g -1 (1C rate). The SrF 2 containing LMB also has a substantially improved rate capability over the reference, the difference being drastic even at the highest testing rate of 20C. First-principles calculations based on DFT indicate that lithium ions prefer to adsorb onto the SrF 2 surface, which should create a more uniform ion flux and reduce the propensity for dendrite nucleation. Finally in parallel, the SrF 2 spheres bind with the SEI layer, creating a tough in situ formed composite membrane that mechanically stabilizes a planar metal interface.

25 ENERGY STORAGE↗
DOE OSTI2011

Recent results on nuclear structure functions for light nuclei

We discuss the nuclear EMC effect with particular emphasis on recent data for light nuclei including {sup 2}H, {sup 3}He, {sup 4}He, {sup 9}Be, {sup 12}C and {sup 14}N. In order to verify the consistency of available data, we calculate the {chi}{sup 2} deviation between different data sets. We find a good agreement between the results from the NMC, SLAC E139, and HERMES experiments. However, our analysis indicates an overall normalization offset of about 2% in the data from the recent JLab E03-103 experiment with respect to previous data for nuclei heavier than {sup 3}He. We also discuss the extraction of the neutron/proton structure function ratio F{sub 2}{sup n}/F{sub 2}{sup p} from the nuclear ratios {sup 3}He/{sup 2}H and {sup 2}H/{sup 1}H. Our analysis shows that the E03-103 data on {sup 3}He/{sup 2}H require a renormalization of about 3% in order to be consistent with the F{sub 2}{sup n}/F{sub 2}{sup p} ratio obtained from the NMC experiment. After such a renormalization, the {sup 3}He data from the E03-103 data and HERMES experiments are in a good agreement. We also present a detailed comparison between data and model calculations, which include a description of the nuclear binding, Fermi motion and off-shell corrections to the structure functions of bound proton and neutron, as well as the nuclear pion and shadowing corrections.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Extending the limits of powder diffraction analysis: diffraction parameter space, occupancy defects, and atomic form factors

Although the determination of site occupancies is often a major goal in Rietveld refinement studies, the accurate refinement of site occupancies is exceptionally challenging due to the many correlations and systematic errors that have a hidden impact on the final refined occupancy parameters. Through the comparison of results independently obtained from neutron and synchrotron powder diffraction, improved approaches capable of detecting occupancy defects with an exceptional sensitivity of 0.1% (absolute) in the class of layered NMC Li-ion battery cathode materials have been developed. A new method of visualizing the diffraction parameter space associated with crystallographic site scattering power through the use of f* diagrams is described and this method is broadly applicable to ternary compounds. The f* diagrams allow the global minimum fit to be easily identified and also permit a robust determination of the number and type of occupancy defects within a structure. Through a comparison of neutron and X-ray diffraction results, a systematic error in the synchrotron results was identified using f* diagrams for a series of NMC compounds. Using neutron diffraction data as a reference, this error was shown to specifically result from problems associated with the neutral oxygen X-ray atomic form factor and could be eliminated by using the ionic O 2- form factor for this anion while retaining the neutral form factors for cationic species. The f* diagram method offers a new opportunity to experimentally assess the quality of atomic form factors through powder diffraction studies on chemically related multi-component compounds.

25 ENERGY STORAGE↗
DOE OSTI2017

Neutron Multiplicity Counting Moments for Fissile Mass Estimation in Scatter-Based Neutron Detection Systems

Neutron multiplicity counting (NMC) techniques are widely used for nuclear materials accountability and international safeguards applications to quantitatively evaluate characteristic properties pertaining to fissile material. Mathematical models for NMC moments have been previously derived for systems that use capture-based detectors; however, these models are not applicable when scatter-based detectors are used because of “neutron cross talk.” Neutron cross talk occurs when a single neutron scatters and deposits energy above threshold into multiple detectors causing spurious increase in multiplicity counts; this, in turn, has caused fissile mass to be overestimated when not treated. In this paper, we propose new mathematical models derived from point kinetics to correct for neutron cross-talk effects up to any arbitrary order N, where N denotes the maximum number of counts a single neutron can cause. The new models were used to estimate the fissile mass of plutonium metal and oxide samples with effective 240 Pu mass ranging from 2.5 to 250 g. The adequacy of the models was confirmed using simulations of a conceptual scatter-based neutron multiplicity counter (e.g., organic scintillators) using MCNPX v2.7e with the PoliMi fission event generating extension. The fissile mass estimates with no correction for neutron cross-talk events yielded an average relative deviation from the true 240 Pu eff mass of 55.94% and 84.56% for metal and oxide samples, respectively. When neutron cross-talk events of order N = 2 are included in the model, the fissile mass estimates yielded an average relative deviation of 11.89% for metal and 13.21% for oxide samples. Accounting for neutron cross-talk events of order N = 3 resulted in fissile mass estimates with an average relative deviation of 9.58% and 10.51% for metal and oxide samples, respectively. These mass estimates were compared to a reference case (i.e., no neutron crosstalk effects) that yielded an average relative deviation of 6.81% and 4.77% for metal and oxide samples, respectively. In conclusion, the discrepancy between the estimates from the proposed model and the reference case is attributed to the assumed value of N, which sets a finite upper bound on the order of cross-talk events the model treats (i.e., the model for N = 3 assumes that a neutron will never cause more than three counts).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Manufacturing Cathodes via Dry-Processing for Lithium-Ion Batteries

Conventional lithium-ion battery (LIB) electrodes are prepared through a wet slurry process with n-methyl pyrrolidone solvent, especially for cathodes. The wet slurry process encounters several disadvantages such as binder migration, electrode cracking in thick electrodes, energy intense heat-dry NMP solvent removal, and costly NMP recovery. The cost and energy consumption of coating and drying of electrode are about 11.5 % and > 46 % in LIB manufacturing, respectively. Thereby, it is essential to develop a facile roll-to-roll solvent-free LIB electrode processing for reducing the cost and energy consumption. Recently, the Maxwell-type dry processing (DP) shines new lights on LIB manufacturing, which mainly bases on dry mixing (DM) of electrode component powder followed by calendering into electrode films and laminating onto current collectors, realizing the rapid manufacturing of LIB electrodes in a powder-to-film manner for industries. This report shares some recent progress on the DP from our group. We aim to further advance the manufacturing science of DP by correlating the processing conditions with electrode properties and performance. Particularly, we investigate the effect of DM, and compression on the polytetrafluoroethylene (PTFE) binder fiberization, porosity, mechanical properties, electrical conductivity and electrochemical behaviors of electrodes. The DM study suggests that PTFE fiberization heavily relies on the degree of DM. Insufficient DM results in poor PTFE fiberization while outrageous DM damages the formed PTFE fibers. Both negatively affect the mechanical behaviors of the electrodes and their rate capability. However, moderate DM is highly beneficial. In addition, our study of the porosity impact reveals that LiNi0.8Mn0.1Co0.1O2 (NMC) secondary particles can be broken into primary particles due to compression, especially at low porosity. Those fractured NMC secondary particles exhibit lower modulus. We propose that a moderate porosity of around 32% favors the electronic conductivity, charge transfer impedance and rate capability. The study of the cathodic electrolyte interphase layer of PTFE-based DPed electrode confirms that side reactions of PTFE binder due to the formation of LiF in LiClO4-based electrolyte.

Tao, Runming↗