Pouch Battery Research Articles

Expansion force signal based rapid detection of early thermal runaway for pouch batteries

With the extensive application of lithium-ion batteries in electric vehicles and energy storage stations, thermal safety issues have increasingly become the focus of public attention. To alleviate the safety concerns, a qualified battery management system (BMS) must be able to detect and warn of thermal abuse before it develops into a thermal runaway (TR). For the first time, the expansion force characteristics of the pouch battery module during the early heating stage of TR under typical working conditions are analyzed, which proves that the expansion force signal can reflect the internal abnormal heating earlier than the terminal voltage and the surface temperature, and has better noise resistance. Furthermore, the electromechanical coupling model (EmCM) is improved for more accurate open-loop expansion force estimation. On this basis, an expansion force based early TR rapid detection framework is proposed with less 3 min expend in tests, in which the Kalman filter ensures the stability and convergence/divergence of the observer estimation error, and the reliability of fault judgment is ensured by the adaptive threshold designed by the model structure.

A polysulfides adsorption strategy through cation-anion interactions for achieving high-safety lithium-sulfur batteries in multiple scenarios

The widespread application of lithium-sulfur batteries (LSBs) is hindered by challenges such as the shuttle effect of polysulfides (LiPSs), slow reaction kinetics, and fire safety concerns. In this study, surface-functionalized boron nitride nanosheets (ChBN) are prepared and employed as functional separator coatings, enabling multiple application scenarios of LSBs. Specifically, a creative strategy of cation-anion interactions is constructed through the strong chemisorption of N+ on the ChBN surface to Sn- in LiPSs. In addition, the boron nitride and N+ showed synergistic effects on adsorption-catalysis, further facilitating the rapid and sufficient deposition of Li2S. The prepared LSBs with ChBN + SP/PP separators exhibit excellent cycle stability (an ultralow capacity degradation of 0.034 % per cycle over 500 cycles at 2C). These LSBs are available over a wide temperature range of −20 to 60 °C, offering a capacity of 1208 mA h/g at 60 °C and 919 mA h/g at −20 °C. Furthermore, the presence of ChBN effectively improves the fire-safety of pouch batteries through the condensed-phase flame retardant mechanism. This simple fabrication process of ChBN is effective and favorable for large-scale manufacturing, which provides a feasible method for the development of high-safety LSBs.

Electrolyte Reconfiguration by Cation/Anion Cross‐coordination for Highly Reversible and Facile Sodium Storage

Hard carbon (HC) materials are promising anodes for sodium‐ion batteries (SIBs) owing to low cost, high specific capacity and low working potential. However, the poor compatibility of the electrolyte with HC leads to low initial coulombic efficiency (ICE) and sluggish Na+ transport kinetics. Here, we propose an electrolyte reconfiguration strategy based on the hard and soft acid and base (HSAB) theory by introducing methyltriphenylphosphonium bromide (MTPPB). MTPPB can realize a spontaneous cross‐coordination solvation structure with NaPF6 by selective affinity, synchronously optimizing the interfacial chemistry and sodium storage process. The advantages of the chemical π‐π bridging of MTPP+‐HC and interaction of MTPP+‐PF6− contribute to preferential and oriented reduction of PF6−, forming a low‐resistance supramolecular SEI. Additionally, Na+‐Br− coordination weakens the Na+‐solvent interactions, facilitating Na+ de‐solvation kinetics. Consequently, the HC||Na cell achieves a superior ICE of 96.6%, desirable rate capability under 25 °C and invisible capacity decay after 500 cycles at 1 C under −20 °C. The Na4Fe3(PO4)2P2O7||HC pouch battery displays a high ICE of 90.3% and a 15% increment of energy density under 25 °C. This work provides a guidance through electrolyte reconfiguration engineering for designing practical HC‐based SIBs with high energy/power density and long‐life span in the extended operating‐temperature range.

Electrolyte Reconfiguration by Cation/Anion Cross-coordination for Highly Reversible and Facile Sodium Storage.

Hard carbon (HC) materials are promising anodes for sodium-ion batteries (SIBs) owing to low cost, high specific capacity and low working potential. However, the poor compatibility of the electrolyte with HC leads to low initial coulombic efficiency (ICE) and sluggish Na+ transport kinetics. Here, we propose an electrolyte reconfiguration strategy based on the hard and soft acid and base (HSAB) theory by introducing methyltriphenylphosphonium bromide (MTPPB). MTPPB can realize a spontaneous cross-coordination solvation structure with NaPF6 by selective affinity, synchronously optimizing the interfacial chemistry and sodium storage process. The advantages of the chemical π-π bridging of MTPP+-HC and interaction of MTPP+-PF6- contribute to preferential and oriented reduction of PF6-, forming a low-resistance supramolecular SEI. Additionally, Na+-Br- coordination weakens the Na+-solvent interactions, facilitating Na+ de-solvation kinetics. Consequently, the HC||Na cell achieves a superior ICE of 96.6%, desirable rate capability under 25 °C and invisible capacity decay after 500 cycles at 1 C under -20 °C. The Na4Fe3(PO4)2P2O7||HC pouch battery displays a high ICE of 90.3% and a 15% increment of energy density under 25 °C. This work provides a guidance through electrolyte reconfiguration engineering for designing practical HC-based SIBs with high energy/power density and long-life span in the extended operating-temperature range.

High-entropy strategy to suppress volumetric strain and enhance diffusion rate of Na3V2(PO4)2F3 cathode for durable and high-areal-capacity zinc-ion battery pouch cells

Aqueous zinc-ion batteries are pivotal contributors to the global energy transformation. Cathode materials with NASICON-type structures are promising candidates for zinc-ion batteries but are hindered by their low electrical conductivity, sluggish ionic diffusion, and structural instability. This work introduces a high-entropy, carbon-coated NASICON-type Na3V2(PO4)2F3 (HE-NVPF@C) cathode by incorporating five metal elements (Al, Zn, Mn, Cr, and Nb) mainly into the V sites of the VO4F2 octahedral structure. Systematic experimental and simulation studies of the Zn2+ storage mechanism in high-entropy NASICON-type cathode are presented for the first time. The high-entropy doping strategy contributes to significantly enhanced cycling stability by suppressing Jahn-Teller distortion, reducing lattice change during Zn2+ extraction and insertion, and decreasing the Zn2+ migration energy barrier. As a result, the HE-NVPF@C cathode demonstrates exceptional cycling stability over 6000 cycles at 20 C with a capacity loss of a mere 0.0031 % per cycle and a high areal capacity retention of 2.17 mAh cm−2. In addition, the pouch cell provides a long cycling lifespan with 90.8 % capacity retention at 5 C after 200 cycles. This feasible high-entropy approach broadens the perspective for developing practical zinc-ion batteries with a long cycle lifespan and high areal capacity.

A Novel Super-Toughness and Self-Healing Solid Polymer Electrolyte for Solid Sodium Metal Batteries.

Solid sodium metal batteries (SSMBs) offer an alternative promising power source for electrochemical energy storage due to their high energy density and high safety. However, the inherent sodium dendrite growth and poor mechanical properties of electrolytes seriously limit their application. Herein, a network structure composed of polyethylene oxide-based composite polymer electrolyte (CPE) is designed with liquid metal nanoparticles (LM) for SSMBs, in which LM can move in the solid electrolyte with the electric field driven. This effect can facilitate the inactivated sodium return to the metal sodium anode, and alloy with dendrites at the same time, which is beneficial for inhibiting the growth of dendrites. The symmetric cell with the CPE containing LM achieves good cyclic stability of more than 1800 and 800h at 0.1 and 0.2mAcm-2, respectively. The energy density of the pouch battery can reach 230Whkg-1. In sum, LM presents great potential to be employed as a performance reinforcement filler for CPEs, which paves the way for achieving high-performance SSMBs.

Magnetic Supraparticles as Identifiers in Single-Layer Lithium-Ion Battery Pouch Cells.

The development of effective recycling technologies is essential for the recovery and reuse of the raw materials required for lithium-ion batteries (LIBs). Future recycling processes depend on accessible information, necessitating the implementation of a digital battery passport. The European battery regulation mandates the use of a machine-readable identifier physically attached to the batteries for accessing digital information. Since externally applied optical labels are vulnerable to mechanical damage, technologies for identification without these restrictions could be beneficial. This study demonstrates that magnetic supraparticles (SPs) can be used for contactless identification of lithium nickel manganese cobalt oxide (NMC) battery pouch cells via magnetic particle spectroscopy (MPS) and that multiple pouch cells can be discriminated based on their specific magnetic code. A comparison of three independent model scenarios revealed that the detection of SPs and the impact on cell performance are dependent on the integration location. The results validate the concept of magnetic identification in metallic environments with MPS as an alternative to optical labeling methods. This study provides a foundation for the development of a new selective labeling and identification technology for batteries, with the potential to facilitate recycling and contribute to a more sustainable future.

Searching for thermal shutdown separators in lithium-ion batteries: Paradigm and practice

This paper focuses on the thermal shutdown separators for thermal runaway control in lithium-ion batteries (LIB). In electrical cars (EV), thermal runaway is the most catastrophic and life-threatening failure mode. Here we reexamined 17 reported phase-change-based thermal shutdown separators and suggested a new design paradigm for thermal shutdown separators of EV level batteries. Through accelerating rate calorimeter (ARC), we have obtained the thermal response curves of three typical EV level batteries: LFP 18,650 battery, NCM 18,650 battery and NCM pouch battery and summarized their critical temperatures. Taking NCM pouch battery as an example, we formed a searching zone for the 17 phase-change-based thermal shutdown separators and found that only 7 of them falling into the promising zone. After analysis on these 7 composite materials, we designed a new trial composite material PBS/PI, which turned out successful in all the following thermal and electrochemical tests. Moreover, we are aware from the beginning that all the reported materials are only tested in button batteries and may not as well apply to EV level batteries. Our own practice has also shown this discrepancy. Thereby we employed thermal simulation to help mapping the discrepancy between the button battery and pouch battery. The results shows that the thermal shutdown happens much earlier in the button battery when elevating the temperature, which tricks researchers into misjudging the material feasibility. This work offers avenues for the searching of thermal shutdown separators in EV level batteries.

A Clay-Based Quasi-Solid-State electrolyte with high cation selective channels for High-Performance aqueous Zinc-Ion batteries

A clay-based quasi-solid-state electrolyte was prepared using dimethyl sulfoxide (DMSO) intercalated kaolinite as the raw material to suppress the adverse effects of free water molecules on aqueous zinc-ion batteries (AZIBs). Based on the inherent water absorption and retention properties of clay kaolinite, as well as the interlayer modification, this clay-based quasi-solid-state electrolyte not only achieved a low water content but also exhibited a strong water binding effect, which restricted the HER and side reactions involving water participation. Furthermore, the intercalation of DMSO increased the number of negative charges on the surface of kaolinite, resulting in the formation of a continuous spatial electrostatic field area around the kaolinite particles, which played a role in cation selectivity. The ionic transference number of the quasi-solid-state electrolyte reached 0.91. Additionally, the intercalation of DMSO broadened the interlayer ionic transport channels of kaolinite, further enhancing the transport efficiency of Zn2+ in the quasi-solid-state electrolyte, achieving uniform deposition of Zn2+ on the surface of the Zn anode, and suppressing dendrite growth to maintain a stable quasi-solid-state electrolyte/Zn anode interface. Zn||MnO2 battery assembled with this electrolyte demonstrated a discharge specific capacity of 301 mAh/g at a current density of 60 mA g−1. The Zn||MnO2 battery could be stably cycled for 1000 cycles at a current density of 150 mA g−1, and after 1000 cycles, the battery still maintained a discharge specific capacity of 248.2 mAh/g with a capacity retention rate of 84.8 %, showing excellent capacity performance and cycle stability. The Zn||MnO2 pouch battery could still provide stable power under heavy pressure, bending, and continuous tapping and had the potential for use in flexible batteries.

Bidirectional pH Buffer Effect Facilitates High-Reversible Aqueous Zinc Ion Batteries.

Aqueous zinc ion batteries (AZIBs) stand out from the crowd of energy storage equipment for their superior energy density, enhanced safety features, and affordability. However, the notorious side reaction in the zinc anode and the dissolution of the cathode materials led to poor cycling stability has hindered their further development. Herein, ammonium salicylate (AS) is a bidirectional electrolyte additive to promote prolonged stable cycles in AZIBs. NH4 + and C6H4OHCOO- collaboratively stabilize the pH at the interface of the electrolyte/electrode and guide the homogeneous deposition of Zn2+ at the zinc anode. The higher adsorption energy of NH4 + compared to H2O on the Zn (002) crystal plane mitigates the side reactions on the anode surface. Moreover, NH4 + is similarly adsorbed on the cathode surface, maintaining the stability of the electrode. C6H4OHCOO- and Zn2+ are co-intercalation/deintercalation during the cycling process, contributing to the higher electrochemical performance of the full cell. As a result, with the presence of AS additive, the Zn//Zn symmetric cells achieved 700h of highly reversible cycling at 5mA cm-2. In addition, the assembled NH4V4O10(NVO)//Zn coin and pouch batteries achieved higher capacity and higher cycle lifetime, demonstrating the practicality of the AS electrolyte additive.

Modeling state-of-charge dependent mechanical response of lithium-ion batteries with volume expansion

The behavior of lithium-ion batteries under mechanical abuse conditions has been studied extensively in recent years. Typically, characterization is performed by conducting experiments on discharged batteries to minimize the chances of thermal runaway and fire. However, studies have shown that material models calibrated at discharged state may not be as accurate at higher states of charge. In this study, a combined experimental-numerical method is proposed to simulate the stiffening of mechanical response in electrode stacks/jellyrolls of lithium-ion batteries at various states of charge and levels of confinement. Our study indicates that the mechanical properties of the jellyroll do not inherently change as a function of the state of charge, rather, the primary cause of the higher stiffness in charged batteries is the volume expansion of the jellyroll during charging. Therefore, mechanical characterization tests are conducted at the discharged state and the expansion of the jellyroll is induced in the finite element models to match the equivalent volume at the desired state of charge. In the second phase of the simulation, mechanical abuse loading is applied to validate the accuracy of simulations using the test data. This method was applied and validated for both pouch and cylindrical batteries with high accuracy.

Interfacial local activation strategy tailoring selective zinc deposition pattern for stable zinc anodes

"Tip effect" triggered by uneven zinc deposition accelerates the growth of Zn dendrites. The unfavorable interfacial activity gradient aggravates zinc deposition at the tips, which is the root cause of zinc dendrites. This study reports an interfacial local activation strategy to reconfigure the interfacial activity gradient of zinc anode to promote more stable operation of zinc batteries. A locally activated zinc anode (Zn-ILA) is proposed as the proof-of-concept zinc anode by constructing high-active microchannels to induce preferential zinc deposition, while the remaining low-active region is accompanied by zinc epitaxial growth, thus achieving bottom-up zinc deposition at the anode interface. A fabrication method based on nanosecond pulsed laser is used to modify the zinc anode by creating high-active microchannels through thermal impingement. Additionally, low-active regions covered by dense ZnO nanoparticles are also formed due to the plasma effect. The laser-induced cross-scale oxide layers help improve the corrosion resistance at the full zinc anode interface. The proposed interfacial local activation strategy enables ordered selective deposition at the Zn-ILA interface owing to the activity gradient, as well as stabilizes the long-term operation of symmetric and full cells. The effectiveness of Zn-ILA is also validated in large-area pouch batteries, showing great potential for large-scale energy storage systems.

The numerical and experimental investigation of the transient behaviours of a lithium-ion pouch battery cell under dynamic conditions

In this paper, the transient model of a high energy density Lithium-ion pouch battery cell is developed under dynamic conditions. The battery cell has a capacity of 73 Ah and volumetric energy density of 642 Wh L−1. This is one of the few studies included the electro-thermal behaviour of high energy density battery under transient conditions by using second ordered model. The transient model indicated that the state of charge (SOC) decreased by 7 % at the end of the WLTP driving cycle and this value is good agreement with the experimental data. Moreover, the developed model provides an accurate prediction of the terminal voltage with a R2 value of 0.99 and a maximum relative error of 2.0 %. Furthermore, the proposed model predicts the electro-thermal characteristics more precisely and the heat generation rate and the entropic term can also be determined without using measurement device. The calculated total heat emitted from battery is about 6W at 1 C-rate for constant current and the heat generation rate is a peak value of ±1.75 105 Wm−3 under dynamic conditions. By using the estimated heat generation rate, more effective cold plates will be designed for thermal management of high energy density battery cells.

A lightweight carbon-incorporated polymer current collector for improving the performance and safety of lithium-ion batteries

The current collector plays a crucial role in transporting electrons and mechanical support of electrodes for lithium-ion batteries (LIBs). Commercial Cu and Al foil with high density deliver no capacity, so decreasing the weight of the metallic current collector is an effective method for enhancing the energy density of batteries. In this study, we prepared a carbon-incorporated polyimide (CIPI) current collector with a lightweight areal density of 1.41 mg cm−2 and voltage window of 0–5 V. CIPI can suppress the current collector corrosion and improve the long-term cycling performance of high-voltage cathode. Besides, CIPI decreases polarization resistance and relieves the volume expansion of SiOx particles, demonstrating a high capacity retention after 200 cycles. In nail penetration tests, the maximum temperature of the pouch battery with CIPI is only 46.73 % of the battery using Cu and Al foil. In addition, the mechanical flexibility makes CIPI suitable for flexible batteries, delivering ultra-stable voltage even when repeatedly folded in half. The CIPI opens a new pathway to develop high energy density and high safety LIBs and promotes the development of flexible and wearable storage devices.

Stress and Strain Characterization for Evaluating Mechanical Safety of Lithium-Ion Pouch Batteries under Static and Dynamic Loadings

The crashworthiness of electric vehicles depends on the response of lithium-ion cells to significant deformation and high strain rates. This study thoroughly explores the mechanical behavior due to damage of lithium-ion battery (LIB) cells, focusing on Lithium Nickel Manganese Cobalt Oxide (NMC) and Lithium Iron Phosphate (LFP) types during both quasi-static indentation and dynamic high-velocity penetration tests. Employing a novel approach, a hemispherical indenter addresses gaps in stress–strain data for pouch cells, considering crucial factors like strain rate/load rate and battery cell type. In the finite element method (FEM) analysis, the mechanical response is investigated in two stages. First, a viscoplastic model is developed in Abaqus/Standard to predict the indentation test. Subsequently, a thermomechanical model is formulated to predict the high-speed-impact penetration test. Considering the high plastic strain rate of the LIB cell, adiabatic heating effects are incorporated into this model, eliminating heat conduction between elements. Addressing a notable discrepancy from prior research, this work explores the substantial reduction in force observed when transitioning from a single cell to a stack of two cells. The study aims to unveil the underlying reasons and provide insights into the mechanical behavior of stacked cells.

Distribution strategy of flexible phase change materials for pouch battery thermal management considering temperature non-uniformity

Flexible composite phase change materials (CPCMs) have been extensively studied in the thermal management of cylindrical lithium-ion batteries and proven to have a good cooling effect. However, passive cooling of pouch lithium-ion batteries with severe uneven temperature distribution has not received the attention it deserves. The thermal management of pouch battery based on passive cooling of flexible PCMs considering the heat-generating structure of pouch batteries needs to be further studied. Herein, CPCMs with different thermal conductivity were prepared, and four different distribution modes of CPCMs, including partial coverage and complete coverage, were applied to thermal management of pouch battery. Results indicated that the maximum temperature (Tmax) and maximum temperature difference (ΔTmax) can be kept separately within 35 °C and 5 °C in the passive thermal management of a single battery except upper coverage at discharge rate of 5C, and the middle coverage (case B) showed excellent temperature control in partial coverage cases. Equally noteworthy was that the increase in thermal conductivity increased the ΔTmax in partial coverage cases, while showing the opposite trend for full coverage (case ABC). Furthermore, only passive cooling of pouch battery pack did not meet the safety requirements under the discharge rate cycle of 5C. Under the active–passive combination mode, case B can control the Tmax (32.22 °C) and ΔTmax (4.69 °C) within a safe range, which was superior to case ABC (Tmax = 35.53 °C, ΔTmax = 5.04 °C). This conclusion provides technical support for the pouch battery to seek economic, stable and efficient thermal management.

Suppressing Surface Oxidation of Pyrite FeS2 by Cobalt Doping in Lithium Sulfur Batteries.

Lithium-sulfur batteries have emerged as a promising energy storage device due to ultra-high theoretical capacity, but the slow kinetics of sulfur and polysulfide shuttle hinder the batteries' further development. Here, the 10% cobalt-doped pyrite iron disulfide electrocatalyst deposited on acetylene black as a separator coating in lithium-sulfur batteries is reported. The adsorption rate to the intermediate Li2S6 is significantly improved while surface oxidation of FeS2 is inhibited: iron oxide and sulfate, thus avoiding FeS2 electrocatalyst deactivation. The electrocatalytic activity has been evaluated in terms of electronic resistivity, lithium-ion diffusion, liquid-liquid, and liquid-solid conversion kinetics. The coin batteries exhibit ultra-long cycle life at 1C with an initial capacity of 854.7 mAh g-1 and maintained at 440.8 mAh g-1 after 920 cycles. Furthermore, the separator is applied to a laminated pouch battery with a sulfur mass of 326 mg (3.7 mg cm-2) and retained the capacity of 590 mAh g-1 at 0.1 C after 50 cycles. This work demonstrates that FeS2 electrocatalytic activity can be improved when Co-doped FeS2 suppresses surface oxidation and provides a reference for low-cost separator coating design in pouch batteries.

Improving reaction uniformity of high‐loading lithium‐sulfur pouch batteries

Improving reaction uniformity of high‐loading lithium‐sulfur pouch batteries

Observation and modeling of dynamic fracture behaviors of battery cell under impact loading using enhanced representative volume element concept

The burgeoning electric automobile industry has increased interest in battery safety. Battery cells experience significant mechanical stress during operation, including the impact of accidents and vibrations from driving. The potential for thermal runaway reactions in battery cells raises safety concerns. Although numerous researchers have defined the dynamic behavior of battery cells and proposed numerical models to describe it, few studies have focused on the high-strain rate mechanical impact phase correlated with the onset of fracture. In this study, we describe the dynamic behavior of pouch battery cells and propose a modeling method to study their mechanical failure under impact situations. Impact tests are conducted at various velocities and heights. To overcome numerical issues commonly encountered under rapid deformation scenarios, a new finite element model is developed based on the representative volume element model. The proposed approach efficiently simulates continuous crack propagation and brittleness behavior during impact by permitting the individual behavior of the cell components. Therefore, engineers can reliably design safer electric vehicle battery cells by measuring the properties of the cell components.

Converting a low-cost industrial polymer into organic cathodes for high mass-loading aqueous zinc-ion batteries

Aqueous zinc-ion batteries (AZIBs) using organic cathodes have emerged as a sustainable energy storage technology benefitting from high safety, low cost, and abundant feedstocks. However, most organic cathodes are n-type polyaromatic compounds and conjugated polymers, which require sophisticated synthesis, provide a low operational voltage and slow Zn2+ diffusion kinetics. Herein, we report access to p-type radical polymer cathodes from a commercially available poly(methyl vinyl ether-alt-maleic anhydride) (poly(MVE-alt-MA)) polymer. The modification of poly(MVE-alt-MA) with 4-amino-TEMPO produces radical polymers (PTEMPO) that are easily scalable to tens of grams. The corresponding polymer AZIBs deliver a capacity of 92 mAh g-1 at 10 C with 95 % capacity retention over 1000 cycles. Importantly, the electrode composites and battery assembly procedure are optimised so that no fluoro-containing electrolytes and binders are needed, and cheap carbon additives can be used. We assemble the Swagelok batteries, small pouch, and large pouch batteries with a high mass-loading of 7.8 to 50 mg cm-2, demonstrating nearly 100 % Coulombic efficiency. The pouch battery with 0.8–0.9 g of active polymer displayed a 60-mAh capacity with 1.5 V operational voltage. This work paves the way for simple and practical implementation of polymer AZIBs for real-world applications.