Pub Date : 2024-07-15DOI: 10.1149/1945-7111/ad6379
Daniel R. Baker, Mark W. Verbrugge, Brian J Koch
We developed a parameter regression scheme that can be used with battery models of interest to the battery-analysis community. We show that the recent reduced order model (ROM1, 2022 J. Electrochem. 169 070520, DOI: 10.1149/1945-7111/ac7c93), which is based on a perturbation solution, can be used in place of the full system of nonlinear partial differential equations with minimal loss of accuracy for the conditions of this work, which are relevant for electric vehicle applications. The use of the computationally efficient ROM1, cast in the Python programming language, along with a routine native to Python for the nonlinear regression of model parameters through the minimization of the squared differences between experimental results and model calculations, provides a fast method for the overall endeavor. We applied the procedure to examine Ni0.89Co0.05Mn0.05Al0.01O2, a high-capacity material that is of increasing interest with respect to electric vehicles and other products that rely on batteries of high energy density. Difficulties encountered in this work include the large number of parameters governing the battery model, parameter sensitivity in the regression analyses, and the potential for multiple solutions. We close this publication with a discussion of these challenges and open questions with respect to parameter identification.
我们开发了一种参数回归方案，可用于电池分析界感兴趣的电池模型。我们展示了基于扰动解法的最新降阶模型（ROM1，2022 J. Electrochem.使用 Python 编程语言编写的计算效率高的 ROM1 以及 Python 原生例程，通过最小化实验结果与模型计算结果之间的平方差对模型参数进行非线性回归，为整个工作提供了一种快速方法。我们应用该程序研究了 Ni0.89Co0.05Mn0.05Al0.01O2，这是一种高容量材料，在电动汽车和其他依赖高能量密度电池的产品中越来越受到关注。这项工作中遇到的困难包括电池模型的参数数量庞大、回归分析中的参数敏感性以及可能出现的多重解决方案。最后，我们讨论了这些挑战以及参数识别方面的开放性问题。
{"title":"Parameter Regression for Porous Electrodes Employed in Lithium-Ion Batteries and Application to Ni0.89Co0.05Mn0.05Al0.01O2","authors":"Daniel R. Baker, Mark W. Verbrugge, Brian J Koch","doi":"10.1149/1945-7111/ad6379","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6379","url":null,"abstract":"\u0000 We developed a parameter regression scheme that can be used with battery models of interest to the battery-analysis community. We show that the recent reduced order model (ROM1, 2022 J. Electrochem. 169 070520, DOI: 10.1149/1945-7111/ac7c93), which is based on a perturbation solution, can be used in place of the full system of nonlinear partial differential equations with minimal loss of accuracy for the conditions of this work, which are relevant for electric vehicle applications. The use of the computationally efficient ROM1, cast in the Python programming language, along with a routine native to Python for the nonlinear regression of model parameters through the minimization of the squared differences between experimental results and model calculations, provides a fast method for the overall endeavor. We applied the procedure to examine Ni0.89Co0.05Mn0.05Al0.01O2, a high-capacity material that is of increasing interest with respect to electric vehicles and other products that rely on batteries of high energy density. Difficulties encountered in this work include the large number of parameters governing the battery model, parameter sensitivity in the regression analyses, and the potential for multiple solutions. We close this publication with a discussion of these challenges and open questions with respect to parameter identification.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141647470","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 : 2024-07-15DOI: 10.1149/1945-7111/ad637a
Bennet Timke, Martin Winter, P. Niehoff
Safety tests are usually conducted on fresh cells. However, occurring lithium plating for example due to harsh aging conditions or electrode inhomogeneities can negatively affect the thermal properties of cells over their lifespan. Recent literature studies showed serious deterioration of the thermal cell properties due to lithium plating while other studies showed no impact at all. These differences are at least partly explained by different amounts of metallic lithium. Here, the impact of the amount of lithium plating on the thermal cell properties was investigated. 1 Ah LiNi0.8Co0.1Mn0.1O2 (NMC811) || artificial graphite pouch cells were aged at 0 °C between zero and ten cycles. The amount of lithium plating was found to influence the self-heating-rates reached during the initial phase of a thermal safety experiment, but did not have a major impact on the safety at higher temperatures. Despite the presence of lithium plating of up to 15% of the initial capacity, none of the cells showed exothermic self-heating for more than three consecutive measuring points below 85 °C. An impact on the onset temperature of first permanent exothermic reactions could only be reliably detected if a cell had already suffered from 10 % capacity loss due to lithium plating.
安全测试通常在新鲜电池上进行。然而，由于苛刻的老化条件或电极不均匀等原因造成的镀锂现象会对电池的热性能产生负面影响。最近的文献研究表明，镀锂会导致电池热性能严重下降，而其他研究则表明完全没有影响。这些差异至少部分是由不同的金属锂含量造成的。在此，我们研究了镀锂量对热电池性能的影响。1 Ah LiNi0.8Co0.1Mn0.1O2 (NMC811) || 人工石墨袋电池在 0 °C 下进行了零至十次循环老化。研究发现，镀锂量会影响热安全实验初始阶段达到的自加热速率，但对较高温度下的安全性影响不大。尽管锂镀层高达初始容量的 15%，但没有一个电池在 85 °C 以下连续三个以上的测量点出现放热自热现象。只有在锂镀层导致电池容量损失 10% 的情况下，才能可靠地检测到首次永久性放热反应的起始温度。
{"title":"Impact of Different Amounts of Lithium Plating on the Thermal Safety of Lithium Ion Cells","authors":"Bennet Timke, Martin Winter, P. Niehoff","doi":"10.1149/1945-7111/ad637a","DOIUrl":"https://doi.org/10.1149/1945-7111/ad637a","url":null,"abstract":"\u0000 Safety tests are usually conducted on fresh cells. However, occurring lithium plating for example due to harsh aging conditions or electrode inhomogeneities can negatively affect the thermal properties of cells over their lifespan. Recent literature studies showed serious deterioration of the thermal cell properties due to lithium plating while other studies showed no impact at all. These differences are at least partly explained by different amounts of metallic lithium. Here, the impact of the amount of lithium plating on the thermal cell properties was investigated. 1 Ah LiNi0.8Co0.1Mn0.1O2 (NMC811) || artificial graphite pouch cells were aged at 0 °C between zero and ten cycles. The amount of lithium plating was found to influence the self-heating-rates reached during the initial phase of a thermal safety experiment, but did not have a major impact on the safety at higher temperatures. Despite the presence of lithium plating of up to 15% of the initial capacity, none of the cells showed exothermic self-heating for more than three consecutive measuring points below 85 °C. An impact on the onset temperature of first permanent exothermic reactions could only be reliably detected if a cell had already suffered from 10 % capacity loss due to lithium plating.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141648837","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 : 2024-07-15DOI: 10.1149/1945-7111/ad6378
Kumar Raju, Laura Wheatcroft, May Ching Lai, Amoghavarsha Mahadevegowda, Louis F. J. Piper, Caterina Ducati, Beverley Inkson, M. Volder
Calendering of battery electrodes is a commonly used manufacturing process that enhances electrode packing density and therefore improves the volumetric energy density. While calendering is standard industrial practice, it is known to crack cathode particles, thereby increasing the electrode surface area. The latter is particularly problematic for new Ni-rich layered transition metal oxide cathodes, such as NMC811, which are known to have substantial surface-driven degradation processes. To establish appropriate calendering practices for these new cathode materials, we conducted a comparative analysis of uncalendered electrodes with electrodes that have a 35% porosity and 25% for single crystal and polycrystalline NMC811. PC cathodes show clear signs of cracking and decrease in rate capability when calendered to 25% porosity, whereas SC cathodes, achieve better cycling stability and no penalty in rate performance at these high packing densities. These findings suggest that SC cathodes should be calendered more densely, we provide a comprehensive overview of both electrochemical and material characterisation methods that corroborate why PC and SC electrodes show such different degradation behaviour. Overall, this work is important because it shows how new single-crystal cathode materials can offer additional advantages in terms of rate performance and cycling stability by calendaring them more densely
{"title":"Influence of Cathode Calendering Density on the Cycling Stability of Li-Ion Batteries Using NMC811 Single or Poly Crystalline Particles","authors":"Kumar Raju, Laura Wheatcroft, May Ching Lai, Amoghavarsha Mahadevegowda, Louis F. J. Piper, Caterina Ducati, Beverley Inkson, M. Volder","doi":"10.1149/1945-7111/ad6378","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6378","url":null,"abstract":"\u0000 Calendering of battery electrodes is a commonly used manufacturing process that enhances electrode packing density and therefore improves the volumetric energy density. While calendering is standard industrial practice, it is known to crack cathode particles, thereby increasing the electrode surface area. The latter is particularly problematic for new Ni-rich layered transition metal oxide cathodes, such as NMC811, which are known to have substantial surface-driven degradation processes. To establish appropriate calendering practices for these new cathode materials, we conducted a comparative analysis of uncalendered electrodes with electrodes that have a 35% porosity and 25% for single crystal and polycrystalline NMC811. PC cathodes show clear signs of cracking and decrease in rate capability when calendered to 25% porosity, whereas SC cathodes, achieve better cycling stability and no penalty in rate performance at these high packing densities. These findings suggest that SC cathodes should be calendered more densely, we provide a comprehensive overview of both electrochemical and material characterisation methods that corroborate why PC and SC electrodes show such different degradation behaviour. Overall, this work is important because it shows how new single-crystal cathode materials can offer additional advantages in terms of rate performance and cycling stability by calendaring them more densely","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141644661","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 : 2024-07-12DOI: 10.1149/1945-7111/ad6291
Hao Wang, Bingqian Sun, Cheng Peng
All-solid-state iron-air batteries (ASSIABs) offer a promising high-temperature battery technology for sustainable large-scale energy storage. However, current ASSIAB performance is insufficient to meet the application requirements, primarily due to the sluggish nature of solid-state electrochemical redox reactions. Here, we briefly describe the development of high-temperature iron-air batteries and conduct an in-depth analysis of ASSIABs, including key materials and the battery reaction mechanisms. We also discuss the current challenges of ASSIABs, suggesting possible strategies to enhance their performance. We hope that this perspective can offer valuable insights into the development of high-performance ASSIABs for large-scale energy storage applications.
{"title":"All-Solid-State Iron-Air Batteries: A Promising High-Temperature Battery Technology for Large-Scale Energy Storage","authors":"Hao Wang, Bingqian Sun, Cheng Peng","doi":"10.1149/1945-7111/ad6291","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6291","url":null,"abstract":"\u0000 All-solid-state iron-air batteries (ASSIABs) offer a promising high-temperature battery technology for sustainable large-scale energy storage. However, current ASSIAB performance is insufficient to meet the application requirements, primarily due to the sluggish nature of solid-state electrochemical redox reactions. Here, we briefly describe the development of high-temperature iron-air batteries and conduct an in-depth analysis of ASSIABs, including key materials and the battery reaction mechanisms. We also discuss the current challenges of ASSIABs, suggesting possible strategies to enhance their performance. We hope that this perspective can offer valuable insights into the development of high-performance ASSIABs for large-scale energy storage applications.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141654964","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 : 2024-07-12DOI: 10.1149/1945-7111/ad6292
Thomas A. Yersak, Yubin Zhang, Hasnain Hafiz, N. Pieczonka, Hernando J. Gonzalez Malabet, Hayden Cunningham, Mei Cai
The performance of all solid-state batteries is limited by poor interfacial contact between active material and solid-state electrolyte (SSE) particles. Semi-solid batteries utilize a secondary electrolyte phase to wet the SSE/AM interface to improve cell performance. Solvate ionic liquids (SILs) are one class of liquid electrolytes under consideration for use in semi-solid batteries. This paper focuses on the Li(G3)TFSI SIL consisting of the bis(trifluoromethanesulfonyl)imide (TFSI-) anion coupled to a [Li(G3)]+ solvate cation. Sulfide SSEs are normally subject to nucleophilic attack by trigylme (G3), however, strong coordination of Li+ to G3 in the [Li(G3)]+ solvate cation prevents this reaction from taking place. Consequently, the stability of sulfide SSE depends on the ideal 1:1 molar ratio of G3 to TFSI, which may be difficult to maintain. We studied the chemical stability of 70Li2S·(30-x)P2S5·xP2O5 (x = 0, 2, 5, 10) (oxy)sulfide solid-state electrolyte in Li(G3)TFSI SIL. By physical measurement, UV-Vis spectroscopy, electrochemical evaluation, X-ray photoelectron spectroscopy, and first principles calculation it is shown that increased oxygen content improves the stability of SSE in various Li(G3)xTFSI (x = 1, 2, 3, 4) liquid electrolytes. The results suggest that an oxysulfide SSE + SIL semi-solid electrolyte is a good choice for future semi-solid battery designs.
{"title":"Improved Stability of Oxysulfide Solid-State Electrolytes in Li(G3)TFSI Solvate Ionic Liquid Electrolyte","authors":"Thomas A. Yersak, Yubin Zhang, Hasnain Hafiz, N. Pieczonka, Hernando J. Gonzalez Malabet, Hayden Cunningham, Mei Cai","doi":"10.1149/1945-7111/ad6292","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6292","url":null,"abstract":"\u0000 The performance of all solid-state batteries is limited by poor interfacial contact between active material and solid-state electrolyte (SSE) particles. Semi-solid batteries utilize a secondary electrolyte phase to wet the SSE/AM interface to improve cell performance. Solvate ionic liquids (SILs) are one class of liquid electrolytes under consideration for use in semi-solid batteries. This paper focuses on the Li(G3)TFSI SIL consisting of the bis(trifluoromethanesulfonyl)imide (TFSI-) anion coupled to a [Li(G3)]+ solvate cation. Sulfide SSEs are normally subject to nucleophilic attack by trigylme (G3), however, strong coordination of Li+ to G3 in the [Li(G3)]+ solvate cation prevents this reaction from taking place. Consequently, the stability of sulfide SSE depends on the ideal 1:1 molar ratio of G3 to TFSI, which may be difficult to maintain. We studied the chemical stability of 70Li2S·(30-x)P2S5·xP2O5 (x = 0, 2, 5, 10) (oxy)sulfide solid-state electrolyte in Li(G3)TFSI SIL. By physical measurement, UV-Vis spectroscopy, electrochemical evaluation, X-ray photoelectron spectroscopy, and first principles calculation it is shown that increased oxygen content improves the stability of SSE in various Li(G3)xTFSI (x = 1, 2, 3, 4) liquid electrolytes. The results suggest that an oxysulfide SSE + SIL semi-solid electrolyte is a good choice for future semi-solid battery designs.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141652162","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 : 2024-07-12DOI: 10.1149/1945-7111/ad6296
Xue Qi, Ziyin Wang, Honglin Yuan, Hongmin Gao, Xinshui Ren, Hua Chen, Hehua Zhang, D. Chang, Hongzhi Pan
Acetaminophen (ACP), a common analgesic and antipyretic medication, can harm the liver when overdosed and its metabolites can contaminate the environment, so it is necessary to monitor the concentration precisely and reliably. In this work, we successfully synthesized cerium oxide/nitrogen-doped reduced graphene oxide (CeO2/N-rGO) composite nanomaterials using a one-step hydrothermal method. Using composite nanomaterials, we created an electrochemical sensing detection platform for ACP detection. The synthesized materials were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. The constructed electrochemical sensor exhibits good ACP detection ability under the synergistic effect of CeO2 and N-rGO. Under optimal experimental conditions, the sensor displayed a linear range for the detection of ACP of 1~200 μM and the lowest detection limit of 0.79 μM, exhibiting outstanding selectivity, stability, and repeatability. Furthermore, the sensor was effectively applied to detect ACP in tap water samples, which offers a wide range of possible applications in actual sample testing.
{"title":"A Novel Electrochemical Sensing Based on Cerium Oxide/Nitrogen-Doped Reduced Graphene Oxide for Sensitive Detection of Acetaminophen","authors":"Xue Qi, Ziyin Wang, Honglin Yuan, Hongmin Gao, Xinshui Ren, Hua Chen, Hehua Zhang, D. Chang, Hongzhi Pan","doi":"10.1149/1945-7111/ad6296","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6296","url":null,"abstract":"\u0000 Acetaminophen (ACP), a common analgesic and antipyretic medication, can harm the liver when overdosed and its metabolites can contaminate the environment, so it is necessary to monitor the concentration precisely and reliably. In this work, we successfully synthesized cerium oxide/nitrogen-doped reduced graphene oxide (CeO2/N-rGO) composite nanomaterials using a one-step hydrothermal method. Using composite nanomaterials, we created an electrochemical sensing detection platform for ACP detection. The synthesized materials were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. The constructed electrochemical sensor exhibits good ACP detection ability under the synergistic effect of CeO2 and N-rGO. Under optimal experimental conditions, the sensor displayed a linear range for the detection of ACP of 1~200 μM and the lowest detection limit of 0.79 μM, exhibiting outstanding selectivity, stability, and repeatability. Furthermore, the sensor was effectively applied to detect ACP in tap water samples, which offers a wide range of possible applications in actual sample testing.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141652972","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}
As the demand for portable electronic and electric vehicles increase, it is necessary to pursue batteries with longer cycle life, higher energy density, and overall better performance. Because lithium sources are limited and lithium metal is expensive, it is necessary to find alternatives. Rechargeable sodium (Na) batteries have attracted great research interest because of their high natural abundance, low cost of sodium resources, and electrochemical similarity with lithium batteries. However, despite the potential to become the next generation of energy storage, the application of sodium metal batteries is mainly hindered by sodium dendrites and "dead" sodium, which reduce battery coulombic efficiency, shorten battery life, and even cause safety problems. The formation of Na dendrites is mainly due to the uncontrolled Na deposition behavior of sodium ions in the absence of nucleation site regulation. Therefore, the sodium deposition is crucial to the final status of Na anodes. Here, we first analyze the growth mechanism of sodium dendrites, then review the research progress of nucleation sites on inhibiting the formation of sodium dendrites, and finally discuss the practical application of sodium batteries and the future challenges of metallic sodium anodes, hoping to stimulate more research interests of researchers.
随着便携式电子产品和电动汽车需求的增加，有必要追求循环寿命更长、能量密度更高、整体性能更好的电池。由于锂资源有限且锂金属价格昂贵，因此有必要寻找替代品。可充电钠（Na）电池因其天然含量高、钠资源成本低以及与锂电池电化学性质相似而引起了人们极大的研究兴趣。然而，尽管钠金属电池有望成为下一代储能电池，但其应用主要受到钠枝晶和 "死 "钠的阻碍，它们降低了电池的库仑效率，缩短了电池寿命，甚至引发安全问题。钠枝晶的形成主要是由于钠离子在缺乏成核位点调节的情况下不受控制的钠沉积行为。因此，钠沉积对 Na 阳极的最终状态至关重要。在此，我们首先分析了钠枝晶的生长机理，然后回顾了成核位点抑制钠枝晶形成的研究进展，最后探讨了钠电池的实际应用和金属钠阳极未来面临的挑战，希望能激发更多研究人员的研究兴趣。
{"title":"Recent Progress of Regulation Factors on the Deposition of Sodium Anodes","authors":"Conggu Tang, Chuyi Cai, Jindan Zhang, Feng Gao, Tao Hu, Zhu Pu, Jingzeng Weng, Mengqi Zhu","doi":"10.1149/1945-7111/ad6290","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6290","url":null,"abstract":"\u0000 As the demand for portable electronic and electric vehicles increase, it is necessary to pursue batteries with longer cycle life, higher energy density, and overall better performance. Because lithium sources are limited and lithium metal is expensive, it is necessary to find alternatives. Rechargeable sodium (Na) batteries have attracted great research interest because of their high natural abundance, low cost of sodium resources, and electrochemical similarity with lithium batteries. However, despite the potential to become the next generation of energy storage, the application of sodium metal batteries is mainly hindered by sodium dendrites and \"dead\" sodium, which reduce battery coulombic efficiency, shorten battery life, and even cause safety problems. The formation of Na dendrites is mainly due to the uncontrolled Na deposition behavior of sodium ions in the absence of nucleation site regulation. Therefore, the sodium deposition is crucial to the final status of Na anodes. Here, we first analyze the growth mechanism of sodium dendrites, then review the research progress of nucleation sites on inhibiting the formation of sodium dendrites, and finally discuss the practical application of sodium batteries and the future challenges of metallic sodium anodes, hoping to stimulate more research interests of researchers.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141653392","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 : 2024-07-12DOI: 10.1149/1945-7111/ad6293
Eliran Evenstein, Sarah Taragin, A. Saha, M. Noked, Rosy Rosy
Most next-generation electrode materials are prone to interfacial degradation, which eventually spreads to the bulk and impairs electrochemical performance. One promising method for reducing interfacial degradation is to surface engineer the electrode materials to form an artificial cathode electrolyte interphase as a protective layer. Nevertheless, the majority of coating techniques entail wet processes, high temperatures, or exposure to ambient conditions. These experimental conditions are only sometimes conducive and can adversely affect the material structure or composition. Therefore, we investigate the efficacy of a low-temperature, facile atomic surface reduction (ASR) using trimethylaluminum vapors as a surface modification strategy for Li and Mn-rich NCM (LMR-NCM). The results presented herein manifest that the extent of TMA-assisted ASR is temperature-dependent. All tested temperatures demonstrated improved electrochemical performance. However, ASR carried out at temperatures > 100°C was more effective in preserving the structural integrity and improving the electrochemical performance. Electrochemical testing revealed improved rate capabilities, cycling stability, and capacity retention of ASR-treated LMR-NCM. Additionally, post-cycling high-resolution scanning electron microscopy analysis verified that after extended cycling, ASR carried out at T > 100°C showed no cracks or cleavage, demonstrating the efficiency of this method in preventing surface degradation.
大多数下一代电极材料都容易发生界面降解，这种降解最终会扩散到体层，损害电化学性能。减少界面降解的一种可行方法是对电极材料进行表面工程处理，形成人工阴极电解质间相作为保护层。然而，大多数涂层技术都需要湿法工艺、高温或暴露在环境条件下。这些实验条件有时会对材料结构或成分产生不利影响。因此，我们研究了利用三甲基铝蒸汽进行低温、简易原子表面还原 (ASR) 作为富锂和富锰 NCM（LMR-NCM）表面改性策略的功效。本文介绍的结果表明，三甲基铝辅助原子表面还原的程度与温度有关。所有测试温度下的电化学性能都有所改善。不过，在温度大于 100°C 时进行的 ASR 更能有效地保持结构完整性和改善电化学性能。电化学测试表明，经过 ASR 处理的 LMR-NCM 的速率能力、循环稳定性和容量保持率均有所提高。此外，循环后的高分辨率扫描电子显微镜分析证实，在温度大于 100°C 的条件下进行的 ASR 经过长时间循环后，没有出现裂纹或断裂，证明这种方法能有效防止表面降解。
{"title":"Investigating the Temperature Dependency of Trimethyl Aluminum Assisted Atomic Surface Reduction of Li and Mn Rich NCM","authors":"Eliran Evenstein, Sarah Taragin, A. Saha, M. Noked, Rosy Rosy","doi":"10.1149/1945-7111/ad6293","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6293","url":null,"abstract":"\u0000 Most next-generation electrode materials are prone to interfacial degradation, which eventually spreads to the bulk and impairs electrochemical performance. One promising method for reducing interfacial degradation is to surface engineer the electrode materials to form an artificial cathode electrolyte interphase as a protective layer. Nevertheless, the majority of coating techniques entail wet processes, high temperatures, or exposure to ambient conditions. These experimental conditions are only sometimes conducive and can adversely affect the material structure or composition. Therefore, we investigate the efficacy of a low-temperature, facile atomic surface reduction (ASR) using trimethylaluminum vapors as a surface modification strategy for Li and Mn-rich NCM (LMR-NCM). The results presented herein manifest that the extent of TMA-assisted ASR is temperature-dependent. All tested temperatures demonstrated improved electrochemical performance. However, ASR carried out at temperatures > 100°C was more effective in preserving the structural integrity and improving the electrochemical performance. Electrochemical testing revealed improved rate capabilities, cycling stability, and capacity retention of ASR-treated LMR-NCM. Additionally, post-cycling high-resolution scanning electron microscopy analysis verified that after extended cycling, ASR carried out at T > 100°C showed no cracks or cleavage, demonstrating the efficiency of this method in preventing surface degradation.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141655651","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 : 2024-07-12DOI: 10.1149/1945-7111/ad6297
Xinsheng Wu, Jay Whitacre
Previous attempts to enhance the stability and performance of MnO2-based cathodes for use in aqueous alkaline electrolytes, primarily KOH-based, have relied on a range of additives. This work demonstrates that the fast capacity decay of the MnO2-based cathode materials in alkaline electrolytes is mainly due to spontaneous manganese dissolution when cycling through the second-electron reaction voltage range. Reducing relative electrolyte content and using carbon materials that have a high specific surface area suppresses manganese dissolution and thus extends the cycle life of the electrode material while reducing overall battery costs. Moreover, reducing the size of the MnO2 particles and decreasing the cycling rate are found to increase manganese dissolution and negatively impact the performance of the electrode material, indicating a sensitivity to material surface area. Lastly, Fe-MnO2-based low-cost battery chemistry was also demonstrated based on the second electron reaction of the MnO2 in an electrolyte lean environment, which could be promising for grid-level energy storage.
{"title":"Reducing Manganese Dissolution in Electrolytic Manganese Dioxide Electrodes in NaOH Electrolyte","authors":"Xinsheng Wu, Jay Whitacre","doi":"10.1149/1945-7111/ad6297","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6297","url":null,"abstract":"\u0000 Previous attempts to enhance the stability and performance of MnO2-based cathodes for use in aqueous alkaline electrolytes, primarily KOH-based, have relied on a range of additives. This work demonstrates that the fast capacity decay of the MnO2-based cathode materials in alkaline electrolytes is mainly due to spontaneous manganese dissolution when cycling through the second-electron reaction voltage range. Reducing relative electrolyte content and using carbon materials that have a high specific surface area suppresses manganese dissolution and thus extends the cycle life of the electrode material while reducing overall battery costs. Moreover, reducing the size of the MnO2 particles and decreasing the cycling rate are found to increase manganese dissolution and negatively impact the performance of the electrode material, indicating a sensitivity to material surface area. Lastly, Fe-MnO2-based low-cost battery chemistry was also demonstrated based on the second electron reaction of the MnO2 in an electrolyte lean environment, which could be promising for grid-level energy storage.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141652949","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 : 2024-07-12DOI: 10.1149/1945-7111/ad6294
Jingpeng Zhang, Xiwen Ke, Yong Wang, Juanjuan Xue
The presence of oxygen vacancy defects significantly impacts the crystal structure and electrochemical attributes of phosphate cathodes. In this investigation, LiMn0.65Fe0.35PO4 materials with varying levels of oxygen vacancy defects were synthesized via hydrogen plasma-induced reduction. It was observed that the content of oxygen vacancy defects on the crystal surface increased proportionately with the rise in hydrogen (H2) flow rate. Notably, the LMFP-3 sample, prepared with an H2 flow rate of 10 mL min-1, demonstrated superior electrochemical performance, characterized by a 159.7 mAh g-1 discharge capacity at 0.1C and a remarkable 99.8% capacity retention at 5C after 200 cycles. This enhancement in electrochemical performance is attributed to the improved intrinsic conductivity of the LiMn0.65Fe0.35PO4 material due to the presence of oxygen vacancy defects. However, it is important to note that an excessively high H2 flow rate can lead to the formation of Fe2P impurities, which hinder lithium ion (Li+) diffusion. Furthermore, theoretical calculations conducted using density functional theory provide a rational explanation for the observed improvement in electronic conductivity. The introduction of oxygen vacancy defects results in a significant reduction in the Band gap, which is highly beneficial for enhancing the intrinsic conductivity of the LiMn0.65Fe0.35PO4 materials.
{"title":"The Effect of Oxygen Vacancy Defects on the Structure and Electrochemical Behaviors of LiMn0.65Fe0.35PO4 Cathode","authors":"Jingpeng Zhang, Xiwen Ke, Yong Wang, Juanjuan Xue","doi":"10.1149/1945-7111/ad6294","DOIUrl":"https://doi.org/10.1149/1945-7111/ad6294","url":null,"abstract":"\u0000 The presence of oxygen vacancy defects significantly impacts the crystal structure and electrochemical attributes of phosphate cathodes. In this investigation, LiMn0.65Fe0.35PO4 materials with varying levels of oxygen vacancy defects were synthesized via hydrogen plasma-induced reduction. It was observed that the content of oxygen vacancy defects on the crystal surface increased proportionately with the rise in hydrogen (H2) flow rate. Notably, the LMFP-3 sample, prepared with an H2 flow rate of 10 mL min-1, demonstrated superior electrochemical performance, characterized by a 159.7 mAh g-1 discharge capacity at 0.1C and a remarkable 99.8% capacity retention at 5C after 200 cycles. This enhancement in electrochemical performance is attributed to the improved intrinsic conductivity of the LiMn0.65Fe0.35PO4 material due to the presence of oxygen vacancy defects. However, it is important to note that an excessively high H2 flow rate can lead to the formation of Fe2P impurities, which hinder lithium ion (Li+) diffusion. Furthermore, theoretical calculations conducted using density functional theory provide a rational explanation for the observed improvement in electronic conductivity. The introduction of oxygen vacancy defects results in a significant reduction in the Band gap, which is highly beneficial for enhancing the intrinsic conductivity of the LiMn0.65Fe0.35PO4 materials.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141654103","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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