Electrode degradation processes at various Li-ion batteries ’ state-of-health (SoH 100 %, 80 %, 50 %, and 30 %) and cycling temperatures (5 ◦ C, 23 ◦ C, and 45 ◦ C) were investigated. For this purpose, the standard format of Li-ion cylindrical 18,650 batteries with Si-Graphite negative and LiNi 0 ⋅ 8 Co 0 ⋅ 1 Mn 0 ⋅ 1 O 2 (NMC811) positive electrodes were cycled with registering battery parameters and the electrochemical impedance spectrum were recorded after every 200 cycles. Once reaching their end-of-life, electrodes from cycled batteries were subjected to post-mortem analysis. NMC811 positive electrode was observed to crack during the charge and discharge processes, suffered by irreversible phase transition, transition metal dissolution, cathode electrolyte interphase growth, and cation mixing. The Si-Graphite negative electrode material was also affected by crack formation, layer exfoliation, solid electrolyte interphase (SEI) recompositing, Li dendrite growth, transition metal contamination, and Si dissolution. Degradation of components leads to an increase of the contact resistance, Li + diffusion limitations, reduction of active materials participating in Li-ion storage and, as a result, capacity fade that finally rendered the battery utilization unfeasible. Degradation processes can be detected by capacity fade and impedance growth of the full battery. High temperature accelerates electrode degradation processes when low temperature leads to SEI and Li dendrite growth.

Aging mechanisms of NMC811/Si-Graphite Li-ion batteries

Current lithium-ion battery (LIB) management technique relying solely on the limited time-domain measurements appears to reach its limit, and incorporating new sensing information, particularly the impedance of LIB, offers a promising path for improvement. Using the non-stationary random driving profile of electric vehicle (EV), a method to extract online passive electrochemical impedance spectroscopy (OPEIS) is proposed and validated, with relevant factors influencing its efficacy also investigated. The particularity of actual driving profile is revealed both theoretically and experimentally, and beyond expectation, the highly differentiated driving profiles yield a similar spectral pattern, which facilitates the acquisition of OPEIS. Continuous OPEIS characterized by the distribution of relaxation time (DRT) ranging from 0.2 Hz to 3 kHz are analyzed in detail under different battery conditions. Compared with offline reference EIS, most of the measurement errors are <3%. Based on the acquired spectral information and OPEIS, a safety-relevant detector and an internal temperature estimator for LIB are presented, and they can both realize a near instant electrochemical sensing up to 1 Hz. As the underlying opportunities of OPEIS are outlined, challenges in its reliable acquisition and engineering implementation are evaluated as well. By comprehensively discussing the realization of OPEIS, research in this paper is expected to provide valuable references for a more effective battery management. 

Research on online passive electrochemical impedance spectroscopy and its outlook in battery management

This review presents a thorough investigation of factors affecting fast charging, battery modeling, key state estimation and fast charging control strategies and provides a forward-looking perspective on AI enabled fast charging technology of LIBs. 

AI enabled fast charging of lithium-ion batteries of electric vehicles during their life cycle: review, challenges and perspectives

Bleomycins (BLMs) are widely used in clinics as antitumor agents. However, BLM-based chemotherapies often accompany severe pulmonary fibrosis (PF). Human bleomycin hydrolase is a cysteine protease that can convert BLMs into inactive deamido-BLMs. In this study, mannose-modified hierarchically porous UiO-66 (MHP-UiO-66) nanoparticles (NPs) were used to encapsulate the recombinant human bleomycin hydrolase (rhBLMH). When rhBLMH@MHP-UiO-66 was intratracheally instilled into the lungs, the NPs were transported into the epithelial cells, and rhBLMH prevented the lungs from PF during BLM-based chemotherapies. Encapsulation of rhBLMH in the MHP-UiO-66 NPs protects the enzyme from proteolysis in physiological conditions and enhances cellular uptake. In addition, the MHP-UiO-66 NPs significantly enhance the pulmonary accumulation of intratracheally instilled rhBLMH, thus providing more efficient protection of the lungs against BLMs during the chemotherapies.

Pulmonary Delivery of Recombinant Human Bleomycin Hydrolase Using Mannose-Modified Hierarchically Porous UiO-66 for Preventing Bleomycin-Induced Pulmonary Fibrosis.

Analysis of the performance evolution and failure mechanisms of commercial Li-ion batteries is crucial for improving testing methods, accurately modeling battery performance, and ensuring safe battery operation. Here, we present the results of a 2-year aging study conducted on commercial large-format LiNiMnCoO2-graphite pouch cells. Loss of lithium inventory (LLI) and loss of positive electrode active material (LAMPE) are shown to dominate capacity fade, as quantified by differential voltage-capacity analysis; only a small amount of LAMPE was measured in extracted electrode material, indicating that LAMPE in full cells was due to electrode dry-out. Resistance evolution, observed by direct current pulses and electrochemical impedance spectroscopy analyzed using the distribution of relaxation times, shows complex trends. Particle cracking and electrode expansion is theorized to cause most changes to resistance. Post-mortem measurements reveal a 10% increase in electrode stack thickness and substantial gas generation, with lithium plating observed in extreme cycling conditions, causing large resistance increases. Circumstantial evidence for self-discharge via redox shuttle, which decomposes the electrolyte, is shown. Overall, electrolyte stability was determined to be the limiting factor for cell lifetime. The impacts of many degradation mechanisms on diagnostic signals substantially overlap, making it challenging to monitor cell health and safety. 

Lithium loss, resistance growth, electrode expansion, gas evolution, and Li plating: Analyzing performance and failure of commercial large-format NMC-Gr lithium-ion pouch cells

Self-Cleaving Protein Linkers with Modulated Ph-Responsiveness: A New Platform for Selective Control of Protein Drug Function


 This article presents the development, parameterization, and experimental validation of a pseudo-three-dimensional multiphysics aging model of a 500 mAh high-energy lithium-ion cell with graphite anode and NMC cathode. This model includes electrochemical reactions for SEI formation at the graphite anode, lithium plating, and SEI formation on plated lithium. The thermodynamics of the aging reactions are modeled depending on temperature and ion concentration and the kinetics are described with an Arrhenius-type rate law. Good agreement of model predictions with galvanostatic charge/discharge measurements and electrochemical impedance spectroscopy is observed over a wide range of operating conditions. The model allows quantification of capacity loss due to cycling near beginning-of-life and visualization of aging colormaps as a function of operating conditions. The model predictions are also qualitatively verified through voltage relaxation, cell expansion, and cell cycling measurements. Based on this full model, six different aging indicators for determination of the limits of fast charging are derived from post-processing simulations of a reduced pseudo-two-dimensional isothermal model without aging mechanisms. The most successful indicator is based on combined plating and SEI kinetics calculated from battery states available in the reduced model. This methodology is applicable to standard pseudo-two-dimensional models available both commercially and as open source.

https://iopscience.iop.org/article/10.1149/1945-7111/acb8e1/pdf

Determining the Limits of Fast Charging of a High-Energy Lithium-Ion NMC/Graphite Pouch Cell Through Combined Modeling and Experiments

Various impedance-based and nonlinear frequency response-based methods for determining the state-of-health (SOH) of commercial lithium-ion cells are evaluated. Frequency response-based measurements provide a spectral representation of dynamics of underlying physicochemical processes in the cell, giving evidence about its internal physical state. The investigated methods can be carried out more rapidly than controlled full discharge and thus constitute prospectively more efficient measurement procedures to determine the SOH of aged lithium- ion cells. We systematically investigate direct use of electrochemical impedance spectroscopy (EIS) data, equivalent circuit fits to EIS, distribution of relaxation times analysis on EIS, and nonlinear frequency response analysis. SOH prediction models are developed by correlating key parameters of each method with conventional capacity measurement (i.e., current integration). The practical feasibility, reliability and uncertainty of each of the established SOH models are considered: all models show average RMS error in the range 0.75% – 1.5% SOH units, attributable principally to cell-to-cell variation. Methods based on processed data (equivalent circuit, distribution of relaxation times) are more experimentally and numerically demanding but show lower average uncertainties and may offer more flexibility for future application.

/pdf/comparison-of-methodologies-to-estimate-state-of-health-of-35n40waz.pdf

Comparison of Methodologies to Estimate State-of-Health of Commercial Li-Ion Cells from Electrochemical Frequency Response Data

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Self-Cleaving Protein Linkers with Modulated Ph-Responsiveness: A New Platform for Selective Control of Protein Drug Function

Determining the Limits of Fast Charging of a High-Energy Lithium-Ion NMC/Graphite Pouch Cell Through Combined Modeling and Experiments

Comparison of Methodologies to Estimate State-of-Health of Commercial Li-Ion Cells from Electrochemical Frequency Response Data