Pub Date : 2024-06-11DOI: 10.1149/1945-7111/ad570a
Suyash Oka, Ratul Mitra Thakur, Chen Wang, Vishaal Vidyaprakash, Coby Scrudder, D. Lagoudas, James Boyd, Micah J. Green, J. Lutkenhaus
Structural batteries require electrodes with integrated energy storage and load-bearing properties. Adoption of structural batteries can lead to mass and volume savings in electrified transportation and aerospace applications by storing energy within the object’s structural elements. However, to date, active materials investigated in structural batteries exhibit poor rate capabilities at higher C-rates and even worse performance at lower temperatures due to diffusion limitations. Organic radical polymers are promising alternatives because they possess fast-charging properties and good cycling stability. In this work, we integrate an organic radical polymer with carbon fiber (CF) fabric, in which the polymer acts as the active cathode material and the CF fabric possesses excellent tensile strength, modulus and electronic conductivity. At 20°C, the structural cathodes exhibited a reversible capacity of 67 mAh g-1 at 1C-rate and an 88% capacity retention at 25C-rate. Further, these structural electrodes retained more than 50% of their performance at -10°C (versus 20°C). These electrodes were further examined in a full cell containing a graphite-based anode, demonstrating a pathway for utilizing redox-active polymer-based active materials in structural and fast-charging organic batteries.
结构电池需要具有综合储能和承重特性的电极。在电气化交通和航空航天应用中，采用结构电池可以通过在物体的结构元件中储存能量来节省质量和体积。然而，迄今为止，在结构电池中研究的活性材料在较高的 C 速率下表现出较低的速率能力，而在较低温度下，由于扩散限制，其性能甚至更差。有机自由基聚合物具有快速充电特性和良好的循环稳定性，因此是很有前途的替代品。在这项工作中，我们将有机自由基聚合物与碳纤维（CF）织物结合在一起，其中聚合物作为活性阴极材料，而碳纤维织物则具有出色的拉伸强度、模量和电子导电性。在 20°C 时，结构阴极在 1C 速率下的可逆容量为 67 mAh g-1，在 25C 速率下的容量保持率为 88%。此外，这些结构电极在 -10°C 时（相对于 20°C）的性能保持率超过 50%。在含有石墨阳极的完整电池中对这些电极进行了进一步检验，证明了在结构性快速充电有机电池中利用氧化还原活性聚合物基活性材料的途径。
{"title":"Fast-Charging Carbon Fiber Structural Battery Electrodes Using an Organic Polymer Active Material","authors":"Suyash Oka, Ratul Mitra Thakur, Chen Wang, Vishaal Vidyaprakash, Coby Scrudder, D. Lagoudas, James Boyd, Micah J. Green, J. Lutkenhaus","doi":"10.1149/1945-7111/ad570a","DOIUrl":"https://doi.org/10.1149/1945-7111/ad570a","url":null,"abstract":"\u0000 Structural batteries require electrodes with integrated energy storage and load-bearing properties. Adoption of structural batteries can lead to mass and volume savings in electrified transportation and aerospace applications by storing energy within the object’s structural elements. However, to date, active materials investigated in structural batteries exhibit poor rate capabilities at higher C-rates and even worse performance at lower temperatures due to diffusion limitations. Organic radical polymers are promising alternatives because they possess fast-charging properties and good cycling stability. In this work, we integrate an organic radical polymer with carbon fiber (CF) fabric, in which the polymer acts as the active cathode material and the CF fabric possesses excellent tensile strength, modulus and electronic conductivity. At 20°C, the structural cathodes exhibited a reversible capacity of 67 mAh g-1 at 1C-rate and an 88% capacity retention at 25C-rate. Further, these structural electrodes retained more than 50% of their performance at -10°C (versus 20°C). These electrodes were further examined in a full cell containing a graphite-based anode, demonstrating a pathway for utilizing redox-active polymer-based active materials in structural and fast-charging organic batteries.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141358747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-11DOI: 10.1149/1945-7111/ad570b
Vamsi Krishna Garapati, N. N. Dingari, Mahesh Mynam, Beena Rai
Lithium-ion batteries (LIBs) powering electric vehicles and large-scale energy storage depend significantly on the composition of liquid electrolyte for optimal performance. We propose a framework coupling Bayesian optimization and physics based battery models to identify electrolytes optimal for specific set of requirements such as less capacity fade and internal heating etc. Our approach is validated through multiple case studies, demonstrating the framework’s efficacy in optimizing electrolyte properties. Additionally, we introduce a deviation index to quantify the proximity of the optimal electrolyte to those in a predefined database. With adaptability to various LIB metrics and battery chemistries, it provides a systematic and efficient approach for screening electrolytes based on system-level performance using physics-based models, contributing to advancements in battery technology for sustainable energy storage systems.
{"title":"Computational Method for Optimal Electrolyte Screening Using Bayesian Optimization and Physics Based Battery Model","authors":"Vamsi Krishna Garapati, N. N. Dingari, Mahesh Mynam, Beena Rai","doi":"10.1149/1945-7111/ad570b","DOIUrl":"https://doi.org/10.1149/1945-7111/ad570b","url":null,"abstract":"\u0000 Lithium-ion batteries (LIBs) powering electric vehicles and large-scale energy storage depend significantly on the composition of liquid electrolyte for optimal performance. We propose a framework coupling Bayesian optimization and physics based battery models to identify electrolytes optimal for specific set of requirements such as less capacity fade and internal heating etc. Our approach is validated through multiple case studies, demonstrating the framework’s efficacy in optimizing electrolyte properties. Additionally, we introduce a deviation index to quantify the proximity of the optimal electrolyte to those in a predefined database. With adaptability to various LIB metrics and battery chemistries, it provides a systematic and efficient approach for screening electrolytes based on system-level performance using physics-based models, contributing to advancements in battery technology for sustainable energy storage systems.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141357023","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-11DOI: 10.1149/1945-7111/ad5707
Xinhua Zhu, Marta Cazorla Soult, Benny Wouters, M. H. Mamme
Anomalous diffusion impedance due to the solid-state Li+ diffusion in Li-ion batteries is often troublesome for the analysis. In this work, we propose a novel analytical Parallel-diffusion Warburg (PDW) model and couple it with the conventional equivalent electrical circuit model (EECM) analysis to tackle this long-standing challenge. The analytical expression of the PDW is derived from the classical Fickian diffusion framework, introducing non-unified diffusion coefficients that originate from the diverse crystalline conditions of Li+ diffusion paths, as theoretically demonstrated in the atomistic modeling results. The proposed approach (EECM + PDW) is successfully employed to study the diffusion impedance of thin-film LiNi0.5Mn1.5O2 (LNMO) electrodes and porous LiNi0.80Co0.15Al0.05O2 (NCA) electrodes, demonstrating the applicability and robustness of this method.
{"title":"Study of Solid-State Diffusion Impedance in Li-Ion Batteries Using Parallel-Diffusion Warburg Model","authors":"Xinhua Zhu, Marta Cazorla Soult, Benny Wouters, M. H. Mamme","doi":"10.1149/1945-7111/ad5707","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5707","url":null,"abstract":"\u0000 Anomalous diffusion impedance due to the solid-state Li+ diffusion in Li-ion batteries is often troublesome for the analysis. In this work, we propose a novel analytical Parallel-diffusion Warburg (PDW) model and couple it with the conventional equivalent electrical circuit model (EECM) analysis to tackle this long-standing challenge. The analytical expression of the PDW is derived from the classical Fickian diffusion framework, introducing non-unified diffusion coefficients that originate from the diverse crystalline conditions of Li+ diffusion paths, as theoretically demonstrated in the atomistic modeling results. The proposed approach (EECM + PDW) is successfully employed to study the diffusion impedance of thin-film LiNi0.5Mn1.5O2 (LNMO) electrodes and porous LiNi0.80Co0.15Al0.05O2 (NCA) electrodes, demonstrating the applicability and robustness of this method.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141358780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-11DOI: 10.1149/1945-7111/ad5709
Patricia Bassil, Coumba Fall, Karim Boutamine, Frédéric Favier, S. Le Vot
Graphite felt is widely utilized as a porous carbon electrode in aqueous redox flow batteries (RFBs). However, its inherent hydrophobic nature and limited electrochemical activity present challenges. While the correlation between RFB performance and electrode properties has been extensively studied for vanadium chemistry and other inorganic redox active materials, it remains scarce in literature for organic systems. In this study, we employ air plasma treatment, known for its controllability, solvent-free nature, and short treatment duration, to modify commercially available graphite felt for RFB applications. A comprehensive analysis is conducted to establish correlations between plasma treatment, physical properties, electrochemical characteristics, and overall cell performance in aqueous RFBs. Comparative evaluation reveals a significant enhancement, with treated graphite felt exhibiting an 85% increase in capacity at 140 mA cm-2 compared to its pristine counterpart. By intentionally utilizing authentic RFB electrodes and employing state-of-the-art ferrocyanide posolyte, this study underscores the crucial role of the interface, even for rapid (reversible) redox-active materials utilized in AORFBs.
{"title":"Air Plasma Modification of Graphite-Based Electrode for Improved Performance of Aqueous Redox Flow Batteries","authors":"Patricia Bassil, Coumba Fall, Karim Boutamine, Frédéric Favier, S. Le Vot","doi":"10.1149/1945-7111/ad5709","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5709","url":null,"abstract":"\u0000 Graphite felt is widely utilized as a porous carbon electrode in aqueous redox flow batteries (RFBs). However, its inherent hydrophobic nature and limited electrochemical activity present challenges. While the correlation between RFB performance and electrode properties has been extensively studied for vanadium chemistry and other inorganic redox active materials, it remains scarce in literature for organic systems. In this study, we employ air plasma treatment, known for its controllability, solvent-free nature, and short treatment duration, to modify commercially available graphite felt for RFB applications. A comprehensive analysis is conducted to establish correlations between plasma treatment, physical properties, electrochemical characteristics, and overall cell performance in aqueous RFBs. Comparative evaluation reveals a significant enhancement, with treated graphite felt exhibiting an 85% increase in capacity at 140 mA cm-2 compared to its pristine counterpart. By intentionally utilizing authentic RFB electrodes and employing state-of-the-art ferrocyanide posolyte, this study underscores the crucial role of the interface, even for rapid (reversible) redox-active materials utilized in AORFBs.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141359099","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-11DOI: 10.1149/1945-7111/ad5706
Zeyu Li, Fuzhen Wang, Zebo Huang
The high safety factor of all-vanadium redox flow batteries (VRFBs) has positioned them as a leading choice for large-scale stationary energy storage. However, their further development is limited by their low energy density and high cost. Flow field performance emerges as a critical factor significantly influencing battery performance. In this paper, we propose a novel spiral flow field (NSFF), which deviates from the commonly serpentine and parallel flow fields. Our research findings demonstrate that, at a flow rate of 180 mL min-1 and a current density of 90 mA cm-2, the NSFF achieves, respectively, 3.65% and 9.8% higher energy efficiency compared to the serpentine and parallel flow fields. Moreover, the state of health of the NSFF after multiple cycles reaches an impressive level of 72.18%, surpassing that of the serpentine and parallel flow fields by 9.97% and 32.12%, respectively.
全钒氧化还原液流电池（VRFB）的高安全系数使其成为大规模固定储能的主要选择。然而，由于能量密度低、成本高，它们的进一步发展受到了限制。流场性能成为影响电池性能的关键因素。在本文中，我们提出了一种新型螺旋流场（NSFF），它不同于常见的蛇形流场和平行流场。我们的研究结果表明，在流速为 180 mL min-1 和电流密度为 90 mA cm-2 的条件下，NSFF 比蛇形流场和平行流场的能量效率分别高出 3.65% 和 9.8%。此外，经过多次循环后，NSFF 的健康状况达到了令人印象深刻的 72.18%，分别比蛇形流场和平行流场高出 9.97% 和 32.12%。
{"title":"Numerical Analysis and Research on Mass Transfer Performance of Vanadium Redox Flow Battery Based on Novel Spiral Flow Field","authors":"Zeyu Li, Fuzhen Wang, Zebo Huang","doi":"10.1149/1945-7111/ad5706","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5706","url":null,"abstract":"\u0000 The high safety factor of all-vanadium redox flow batteries (VRFBs) has positioned them as a leading choice for large-scale stationary energy storage. However, their further development is limited by their low energy density and high cost. Flow field performance emerges as a critical factor significantly influencing battery performance. In this paper, we propose a novel spiral flow field (NSFF), which deviates from the commonly serpentine and parallel flow fields. Our research findings demonstrate that, at a flow rate of 180 mL min-1 and a current density of 90 mA cm-2, the NSFF achieves, respectively, 3.65% and 9.8% higher energy efficiency compared to the serpentine and parallel flow fields. Moreover, the state of health of the NSFF after multiple cycles reaches an impressive level of 72.18%, surpassing that of the serpentine and parallel flow fields by 9.97% and 32.12%, respectively.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141360012","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-10DOI: 10.1149/1945-7111/ad5623
Danfeng Ying, Xufeng Zhou, Tengsheng Chi, Meichen Liu, Yimei Li, Wei Wang, Z. Liu
Though over-lithiation of graphite can increase the initial specific capacity of the anodes, the cycling stability is unsatisfactory as metallic lithium depositing on the surface of graphite has poor reversibility. In this work, we utilize electrochemical co-intercalation of Li+ and diethylene glycol dimethyl ether (DEGDME) to prepare [Li-DEGDME]+-graphite co-intercalation compounds ([Li-DEGDME]-Gr) from pristine graphite. The expanded d-spacing and abundant cross-layer voids in the intralayer structure of [Li-DEGDME]-Gr owing to the co-intercalation of [Li-DEGDME]+ complex ions and parasitic chemical reactions between solvent molecules and graphene layers promotes the migration of bare Li+ and provides sufficient interior space for extra lithium-storage. As a result, a much higher lithium-storage capacity of 810 mAh g-1 can be successfully achieved. The extra lithium-storage is proved to originate from the deposition of lithium metal inside the enclosed nanoscale space of the as modified graphite, which inhibits the formation of lithium dendrites, isolates lithium metal from electrolytes and avoids volumetric expansion, enabling the [Li-DEGDME]-Gr electrodes to exhibit better cycling stability with high specific capacity. This work proposes a new strategy to enhance the reversibility of lithium metal plating/stripping by accommodating lithium deposition inside modified carbon materials, thus effectively increases the reversible capacity of graphite-based anode materials.
虽然石墨的过度锂化可以提高负极的初始比容量，但由于金属锂沉积在石墨表面的可逆性较差，因此循环稳定性并不理想。在这项工作中，我们利用 Li+ 和二乙二醇二甲醚（DEGDME）的电化学共掺杂，从原始石墨中制备出[Li-DEGDME]+-石墨共掺杂化合物（[Li-DEGDME]-Gr）。由于[Li-DEGDME]+复合离子的共掺杂以及溶剂分子与石墨烯层之间的寄生化学反应，[Li-DEGDME]-Gr的层内结构中d间距扩大，跨层空隙丰富，促进了裸Li+的迁移，并为额外的锂存储提供了充足的内部空间。因此，可以成功实现 810 mAh g-1 的更高储锂容量。事实证明，额外的锂存储源自金属锂在改性石墨封闭的纳米级空间内的沉积，这抑制了锂枝晶的形成，将金属锂与电解质隔离开来，避免了体积膨胀，从而使[Li-DEGDME]-Gr电极表现出更好的循环稳定性和更高的比容量。这项工作提出了一种新策略，通过在改性碳材料内部容纳锂沉积来增强金属锂镀层/剥离的可逆性，从而有效提高石墨基负极材料的可逆容量。
{"title":"Dendrite/Volume Expansion-Free Lithium Deposition Inside the Enclosed Nanoscale Space of Electrochemically Modified Graphite","authors":"Danfeng Ying, Xufeng Zhou, Tengsheng Chi, Meichen Liu, Yimei Li, Wei Wang, Z. Liu","doi":"10.1149/1945-7111/ad5623","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5623","url":null,"abstract":"\u0000 Though over-lithiation of graphite can increase the initial specific capacity of the anodes, the cycling stability is unsatisfactory as metallic lithium depositing on the surface of graphite has poor reversibility. In this work, we utilize electrochemical co-intercalation of Li+ and diethylene glycol dimethyl ether (DEGDME) to prepare [Li-DEGDME]+-graphite co-intercalation compounds ([Li-DEGDME]-Gr) from pristine graphite. The expanded d-spacing and abundant cross-layer voids in the intralayer structure of [Li-DEGDME]-Gr owing to the co-intercalation of [Li-DEGDME]+ complex ions and parasitic chemical reactions between solvent molecules and graphene layers promotes the migration of bare Li+ and provides sufficient interior space for extra lithium-storage. As a result, a much higher lithium-storage capacity of 810 mAh g-1 can be successfully achieved. The extra lithium-storage is proved to originate from the deposition of lithium metal inside the enclosed nanoscale space of the as modified graphite, which inhibits the formation of lithium dendrites, isolates lithium metal from electrolytes and avoids volumetric expansion, enabling the [Li-DEGDME]-Gr electrodes to exhibit better cycling stability with high specific capacity. This work proposes a new strategy to enhance the reversibility of lithium metal plating/stripping by accommodating lithium deposition inside modified carbon materials, thus effectively increases the reversible capacity of graphite-based anode materials.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141364528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-10DOI: 10.1149/1945-7111/ad561f
Vamsee Krishna Teki, Jahnavi Kasi, Saiprakash Chidurala, Subhashree Priyadarshini, S. Joga, M. K. Maharana, C. Panigrahi
Electrochemical impedance spectroscopy (EIS) is a very effective methodology employed in the evaluation of performance and degradation mechanisms associated with lithium-ion batteries. In order to comprehend the complex electrochemical processes taking place within these energy storage devices, reliable and effective diagnostic tools are required due to the constant improvements in battery technology. EIS methodology has gained prominence as a very effective non-destructive method for examining the electrochemical characteristics of batteries. This technique offers significant contributions by providing useful insights into the internal operations of batteries. The main objective of this study is to create an electrical equivalent circuit model of a lithium-ion battery based on physics, and then use EIS to comprehend the electrical behavior and impedance of the battery to evaluate its performance under various operating scenarios. We seek to identify the critical elements influencing the battery's capacity, performance, and lifespan by capturing the intricate interaction of EIS. The results of this research are going to enhance the understanding of battery behavior and supporting the design as a more reliable and efficient energy storage systems for a wide range of applications, from portable electronic devices to electric vehicles and renewable energy integration.
电化学阻抗光谱（EIS）是评估锂离子电池性能和降解机制的一种非常有效的方法。由于电池技术的不断改进，为了理解这些储能设备中发生的复杂电化学过程，需要可靠有效的诊断工具。EIS 方法作为检查电池电化学特性的一种非常有效的非破坏性方法，已经得到了广泛应用。这项技术为深入了解电池的内部运作做出了重要贡献。本研究的主要目的是根据物理学原理创建锂离子电池的电气等效电路模型，然后使用 EIS 理解电池的电气行为和阻抗，以评估其在各种操作情况下的性能。我们试图通过捕捉 EIS 错综复杂的相互作用，找出影响电池容量、性能和寿命的关键因素。这项研究的成果将加深人们对电池行为的理解，并支持设计出更可靠、更高效的储能系统，广泛应用于便携式电子设备、电动汽车和可再生能源集成等领域。
{"title":"Analysis of Lithium-ion Batteries through Electrochemical Impedance Spectroscopy Modeling","authors":"Vamsee Krishna Teki, Jahnavi Kasi, Saiprakash Chidurala, Subhashree Priyadarshini, S. Joga, M. K. Maharana, C. Panigrahi","doi":"10.1149/1945-7111/ad561f","DOIUrl":"https://doi.org/10.1149/1945-7111/ad561f","url":null,"abstract":"\u0000 Electrochemical impedance spectroscopy (EIS) is a very effective methodology employed in the evaluation of performance and degradation mechanisms associated with lithium-ion batteries. In order to comprehend the complex electrochemical processes taking place within these energy storage devices, reliable and effective diagnostic tools are required due to the constant improvements in battery technology. EIS methodology has gained prominence as a very effective non-destructive method for examining the electrochemical characteristics of batteries. This technique offers significant contributions by providing useful insights into the internal operations of batteries. The main objective of this study is to create an electrical equivalent circuit model of a lithium-ion battery based on physics, and then use EIS to comprehend the electrical behavior and impedance of the battery to evaluate its performance under various operating scenarios. We seek to identify the critical elements influencing the battery's capacity, performance, and lifespan by capturing the intricate interaction of EIS. The results of this research are going to enhance the understanding of battery behavior and supporting the design as a more reliable and efficient energy storage systems for a wide range of applications, from portable electronic devices to electric vehicles and renewable energy integration.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141361201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-10DOI: 10.1149/1945-7111/ad5622
Vinit Nagda, Henrik Ekström, Artem Kulachenko
Lithium-ion batteries (LIBs) are widely chosen for energy storage owing to their high coulombic efficiency and energy density. Within the positive electrode materials of LIBs, the structural integrity of secondary particles, composed of randomly oriented single-crystal primary particles, is crucial for sustained performance. These particles can fracture as a result of both mechanical stress and chemical interactions within the solid. Modelling LIBs is a complex task involving electro-chemo-mechanical phenomena and their interactions on different length scales. This study proposes a numerical modeling framework to investigate the active particle degradation and its impact on electrochemical performance. The model integrates mechanical and electrochemical processes, tracking crack evolution and mechanical failure through phase field damage. The coupled time-dependent non-linear partial differential equations are solved in a finite element framework using COMSOL Multiphysics. The model offers numerical insights into intergranular and transgranular fracture within secondary particles. The electrolyte infiltration into cracks reduces the electrochemical overpotential due to the increase in electrochemically active surface area, positively affecting performance. However, prolonged cycling with particle cracking poses severe threat to the battery performance and capacity. This comprehensive numerical modeling approach provides valuable insights into the intricate interplay of mechanical and electrochemical factors governing LIB performance and degradation.
{"title":"Impact of Mechanical Degradation in Polycrystalline NMC Particle on the Electrochemical Performance of Lithium-Ion Batteries","authors":"Vinit Nagda, Henrik Ekström, Artem Kulachenko","doi":"10.1149/1945-7111/ad5622","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5622","url":null,"abstract":"\u0000 Lithium-ion batteries (LIBs) are widely chosen for energy storage owing to their high coulombic efficiency and energy density. Within the positive electrode materials of LIBs, the structural integrity of secondary particles, composed of randomly oriented single-crystal primary particles, is crucial for sustained performance. These particles can fracture as a result of both mechanical stress and chemical interactions within the solid. Modelling LIBs is a complex task involving electro-chemo-mechanical phenomena and their interactions on different length scales. This study proposes a numerical modeling framework to investigate the active particle degradation and its impact on electrochemical performance. The model integrates mechanical and electrochemical processes, tracking crack evolution and mechanical failure through phase field damage. The coupled time-dependent non-linear partial differential equations are solved in a finite element framework using COMSOL Multiphysics. The model offers numerical insights into intergranular and transgranular fracture within secondary particles. The electrolyte infiltration into cracks reduces the electrochemical overpotential due to the increase in electrochemically active surface area, positively affecting performance. However, prolonged cycling with particle cracking poses severe threat to the battery performance and capacity. This comprehensive numerical modeling approach provides valuable insights into the intricate interplay of mechanical and electrochemical factors governing LIB performance and degradation.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141365410","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-10DOI: 10.1149/1945-7111/ad5624
Timon Lazaridis, R. K. F. Della Bella, H. Gasteiger
Tailored design of carbon supports and their pore morphologies is crucial to achieve the ambitious durability and performance targets for future proton exchange membrane fuel cells (PEMFCs). We compared platinum catalysts supported on solid Vulcan carbon, porous Ketjenblack carbon, and accessible porous modified Ketjenblack carbon in a voltage cycling-based accelerated stress test (AST) with frequent intermittent characterizations. We derived how catalyst morphologies affect cell performance and electrochemical properties (electrode roughness factor, ORR activity, oxygen transport resistances) at beginning-of-life (BoL) and in various states of degradation up to 200,000 voltage cycles. We confirmed the enhanced Pt surface area retention of porous carbon-supported catalysts, ascribed to well-shielded Pt particles in internal pores, but find that this comes at the expense of lower initial high current density performance already at BoL. Accessible porous carbon-supported catalysts with wider pores mostly retain those durability benefits while, simultaneously, maximizing H2/air performance at all current densities due to improved oxygen transport. We also tracked changes in catalyst accessibility throughout voltage cycling by analyzing local oxygen transport resistances and relative humidity-dependent platinum utilization. We propose that catalysts with porous carbon supports undergo oxidative pore opening, followed by continuous migration of internal Pt particles to the external carbon surface.
{"title":"Trading Off Initial PEM Fuel Cell Performance versus Voltage Cycling Durability for Different Carbon Support Morphologies","authors":"Timon Lazaridis, R. K. F. Della Bella, H. Gasteiger","doi":"10.1149/1945-7111/ad5624","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5624","url":null,"abstract":"\u0000 Tailored design of carbon supports and their pore morphologies is crucial to achieve the ambitious durability and performance targets for future proton exchange membrane fuel cells (PEMFCs). We compared platinum catalysts supported on solid Vulcan carbon, porous Ketjenblack carbon, and accessible porous modified Ketjenblack carbon in a voltage cycling-based accelerated stress test (AST) with frequent intermittent characterizations. We derived how catalyst morphologies affect cell performance and electrochemical properties (electrode roughness factor, ORR activity, oxygen transport resistances) at beginning-of-life (BoL) and in various states of degradation up to 200,000 voltage cycles. We confirmed the enhanced Pt surface area retention of porous carbon-supported catalysts, ascribed to well-shielded Pt particles in internal pores, but find that this comes at the expense of lower initial high current density performance already at BoL. Accessible porous carbon-supported catalysts with wider pores mostly retain those durability benefits while, simultaneously, maximizing H2/air performance at all current densities due to improved oxygen transport. We also tracked changes in catalyst accessibility throughout voltage cycling by analyzing local oxygen transport resistances and relative humidity-dependent platinum utilization. We propose that catalysts with porous carbon supports undergo oxidative pore opening, followed by continuous migration of internal Pt particles to the external carbon surface.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141363138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-10DOI: 10.1149/1945-7111/ad5625
T. Taskovic, Alison Clarke, J. Harlow, Sasha Martin-Maher, Kenneth Tuul, Ethan Eastwood, Michel Johnson, Jeff R. Dahn
Li[Ni0.6Mn0.4Co0.0]O2/graphite (NMC640, balanced for 4.1 V cut-off) and Li[Ni0.83Mn0.06Co0.11]O2/graphite (Ni83, balanced for 4.06 V cut-off) pouch cells were tested using lab-simulated autoclave conditions. After every cycle, the cells at either 3.4, 3.7, or 3.9 V were placed in a 120°C oven for 40 min to undergo an “autoclave” run, then continued for another cycle. Electrolyte blends using lithium bis(fluorosulfonyl)imide (LiFSI) salt were used to improve the cycle-life of autoclaved cells. The lab autoclave protocol was also performed on LiFePO4/graphite (LFP) and NMC commercial cylindrical cells, which were advertised for use in or found in autoclaved medical devices. LFP cells performed poorly in the simulated autoclave tests, while commercial high-temperature-tolerant NMC cylindrical cells and the pouch cells performed similarly. In continuous testing at 85°C, the pouch cells had better capacity retention than both cylindrical cell types. However, the pouch cells suffered from electrolyte permeation through the polymer seals. The pouch cell chemistries incorporated in cylindrical cell format would probably give superior performance to the commercial cells in the autoclave tests. Cell lifetimes were improved when cells were placed into the 120°C oven at a lower voltage suggesting that hospitals should charge Li-ion cells after the autoclaving process instead of standard practice of before
{"title":"An Investigation of Li-Ion Cell Degradation Caused by Simulated Autoclave Cycles","authors":"T. Taskovic, Alison Clarke, J. Harlow, Sasha Martin-Maher, Kenneth Tuul, Ethan Eastwood, Michel Johnson, Jeff R. Dahn","doi":"10.1149/1945-7111/ad5625","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5625","url":null,"abstract":"\u0000 Li[Ni0.6Mn0.4Co0.0]O2/graphite (NMC640, balanced for 4.1 V cut-off) and Li[Ni0.83Mn0.06Co0.11]O2/graphite (Ni83, balanced for 4.06 V cut-off) pouch cells were tested using lab-simulated autoclave conditions. After every cycle, the cells at either 3.4, 3.7, or 3.9 V were placed in a 120°C oven for 40 min to undergo an “autoclave” run, then continued for another cycle. Electrolyte blends using lithium bis(fluorosulfonyl)imide (LiFSI) salt were used to improve the cycle-life of autoclaved cells. The lab autoclave protocol was also performed on LiFePO4/graphite (LFP) and NMC commercial cylindrical cells, which were advertised for use in or found in autoclaved medical devices. LFP cells performed poorly in the simulated autoclave tests, while commercial high-temperature-tolerant NMC cylindrical cells and the pouch cells performed similarly. In continuous testing at 85°C, the pouch cells had better capacity retention than both cylindrical cell types. However, the pouch cells suffered from electrolyte permeation through the polymer seals. The pouch cell chemistries incorporated in cylindrical cell format would probably give superior performance to the commercial cells in the autoclave tests. Cell lifetimes were improved when cells were placed into the 120°C oven at a lower voltage suggesting that hospitals should charge Li-ion cells after the autoclaving process instead of standard practice of before","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141363398","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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