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Electrochemical Testing and Benchmarking of Compositionally Complex Lithium Argyrodite Electrolytes for All-Solid-State Battery Application 用于全固态电池应用的成分复杂的 Argyrodite 锂电解质的电化学测试和基准测试
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-23 DOI: 10.1002/batt.202400112
Jianxuan Du, Jing Lin, Ruizhuo Zhang, Prof. Shuo Wang, Dr. Sylvio Indris, Prof. Helmut Ehrenberg, Dr. Aleksandr Kondrakov, Dr. Torsten Brezesinski, Dr. Florian Strauss

Ceramic ion conductors play a pivotal role as electrolytes in solid-state batteries (SSBs). Aside from the ionic conductivity, their (electro)chemical stability has a profound effect on the performance. Lithium thiophosphates represent a widely used class of superionic materials, yet they suffer from limited stability and are known to undergo interfacial degradation upon battery cycling. Knowledge of composition-dependent properties is essential to improving upon the stability of thiophosphate solid electrolytes (SEs). In recent years, compositionally complex (multicomponent) and high-entropy lithium argyrodite SEs have been reported, having room-temperature ionic conductivities of σion>10 mS cm−1. In this work, various multi-cationic and -anionic substituted argyrodite SEs are electrochemically tested via cyclic voltammetry and impedance spectroscopy, as well as under operating conditions in SSB cells with layered Ni-rich oxide cathode and indium-lithium anode. Cation substitution is found to negatively affect the electrochemical stability, while anion substitution (introducing Cl/Br and increasing halide content) has a beneficial effect on the cyclability, especially at high current rates.

陶瓷离子导体作为电解质在固态电池(SSB)中发挥着举足轻重的作用。除了离子导电性之外,其(电)化学稳定性对性能也有深远影响。硫代磷酸锂是一类广泛使用的超离子材料,但它们的稳定性有限,而且已知在电池循环时会发生界面降解。要提高硫代磷酸盐固态电解质(SE)的稳定性,了解其成分相关特性至关重要。近年来,成分复杂(多组分)、高熵的箭石锂固态电解质已有报道,其室温离子电导率 σion > 10 mS cm-1。在这项工作中,通过循环伏安法和阻抗光谱法对各种多阳离子和阴离子取代的箭石 SE 进行了电化学测试,并在 SSB 电池(带层状富氧化镍阴极和铟锂阳极)的工作条件下进行了测试。结果发现,阳离子取代会对电化学稳定性产生负面影响,而阴离子取代(引入 Cl-/Br- 和增加卤化物含量)则会对循环性产生有利影响,尤其是在高电流速率下。
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引用次数: 0
Anion-Derived Solid Electrolyte Interphase Enabled by Diluent Modulated Dimethyl Carbonate-Based Localized High Concentration Electrolytes for Lithium Metal Batteries 通过稀释剂调制碳酸二甲酯局部高浓度电解质实现阴离子衍生固体电解质相间,用于锂金属电池
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-22 DOI: 10.1002/batt.202400238
Hanlu Zheng, Yu Zhong, Changdong Gu, Xiuli Wang, Prof. Jiangping Tu

Carbonate-based electrolytes generally suffer from low Coulombic efficiency and poor cycling stability in lithium metal batteries. In this work, localized high concentration electrolytes (LHCEs) based on dimethyl carbonate (DMC) with varying diluent additions are designed. LHCEs demonstrate higher Li+ transference numbers and a greater proportion of contact ion pairs (CIPs) and ion pair aggregates (AGGs) in the solvation structures, facilitating the formation of anion-derived solid electrolyte interphase (SEI). Furthermore, LHCEs enhance the Coulombic efficiency of Li||Cu cells and improve the anodic stability against lithium. One of these LHCEs, prepared with appropriate diluent addition, exhibits excellent capacity retention in Li||NCM622 cells at 0.5 C after 150 cycles, thus presenting promising possibilities for the development of high energy density lithium metal batteries.

碳酸盐基电解质在锂金属电池中普遍存在库仑效率低和循环稳定性差的问题。在这项工作中,设计了基于碳酸二甲酯(DMC)的局部高浓度电解质(LHCEs),并添加了不同的稀释剂。LHCEs 在溶解结构中表现出更高的 Li+ 转移数量和更大比例的接触离子对(CIPs)和离子对聚集体(AGGs),从而促进了阴离子衍生固态电解质间相(SEI)的形成。此外,LHCEs 还能提高锂||铜电池的库仑效率,并改善对锂的阳极稳定性。其中一种 LHCEs 经适当添加稀释剂制备后,在 0.5 C 温度下循环 150 次后,在锂|NCM622 电池中表现出优异的容量保持能力,从而为高能量密度锂金属电池的开发提供了广阔的前景。
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引用次数: 0
Enhancing Ion Adsorption Capability through the Strong Interaction in Co9S8-Carbon Hybrids Achieves Superior Sodium Ion Storage 通过 Co9S8 碳杂化物中的强相互作用增强离子吸附能力,实现卓越的钠离子储存效果
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-21 DOI: 10.1002/batt.202400170
Xinyi Ma, Xiaoyue He, Lai Yu, Nazir Ahmad, Zongzhi Tao, Zi Xuan Jiang, Jia Cheng Liang, Prof. Suyuan Zeng, Prof. Liang Shi, Prof. Genqiang Zhang

Metal sulfides materials are promising anode candidates for Na+ storage due to their low cost and high theoretical capacity, while the complex phase transition and inevitable volume expansion during cycling restrain their practical applications. Herein, a simple one-pot manipulation strategy was designed to construct Co9S8 nanoparticles strongly encapsulated in carbon nanotubes (Co9S8@C/NTs) composite structure with enhanced structural stability and reaction kinetics, resulting in greatly improved Na+ storage performance. Specifically, the obtained Co9S8@C/NTs could exhibit a remarkable capacity of 500 mAh g−1 at 0.5 A g−1 after 100 cycles and exceptional cycling stability over 600 cycles with 88 % capacity retention at 1 A g−1. Furthermore, the theoretical calculations combined with systematic characterizations confirm that the strong interaction between Co9S8 and the carbon matrix could greatly enhance the Na+ adsorption ability and facilitate the electron transfer dynamics for superior Na+ storage capability. More importantly, the full cell device can deliver an outstanding energy density of 144.32 Wh kg−1 and a decent cycling life with 82 % capacity retention of almost 100 cycles at 0.1 A g−1. This work could provide more valuable insights for designing advanced metal sulfide nanocomposites and demonstrate fascinating prospects for commercial application.

金属硫化物材料因其低成本和高理论容量而成为具有潜力的 Na+ 储存阳极候选材料,但其复杂的相变和循环过程中不可避免的体积膨胀限制了其实际应用。本文设计了一种简单的一锅操作策略,构建了Co9S8纳米颗粒强包覆碳纳米管(Co9S8@C/NTs)复合结构,增强了结构稳定性和反应动力学,从而大大提高了Na+存储性能。具体而言,所获得的 Co9S8@C/NTs 在 0.5 A g-1 条件下循环 100 次后,容量可达 500 mAh g-1;在 1 A g-1 条件下循环 600 次后,容量保持率为 88%,具有优异的循环稳定性。此外,理论计算结合系统表征证实,Co9S8 与碳基质之间的强相互作用可大大提高 Na+ 的吸附能力,并促进电子传递动力学,从而实现卓越的 Na+ 储存能力。更重要的是,这种全电池器件的能量密度高达 144.32 Wh kg-1,循环寿命长,在 0.1 A g-1 的条件下可循环 100 次,容量保持率高达 82%。这项工作可为设计先进的金属硫化物纳米复合材料提供更多灵感,并展示出令人着迷的商业应用前景。
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引用次数: 0
Operando Temperature Dynamic Investigation of Electric Double-Layer Capacitors Containing Organic Electrolytes 含有机电解质的双电层电容器的操作温度动态研究
IF 5.7 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-19 DOI: 10.1002/batt.202400242
Fabian Alexander Kreth, Lukas Köps, Scott W. Donne, Andrea Balducci

Invited for this month's cover picture is the Balducci's group who works on the development of innovative electrolytes and materials for safer, high-performance supercapacitors and batteries, and on advanced real-time characterization techniques to improve the understanding of aging and charge storage processes in electrochemical devices. The front cover illustrates a supercapacitor evaluated with the screening technique presented in this report. It highlights different electrolyte compositions, indicated by chemical compounds above the setup. This approach provides insights into how capacitance, energy, power, entropy, and enthalpy respond to changes in temperature and voltage. Read the full text of the Research Article at 10.1002/batt.202300581.

本期封面图片邀请的是 Balducci 小组,该小组致力于为更安全、高性能的超级电容器和电池开发创新的电解质和材料,以及先进的实时表征技术,以提高对电化学设备老化和电荷存储过程的了解。封面展示了利用本报告中介绍的筛选技术评估的超级电容器。它突出显示了不同的电解质成分,由设置上方的化合物表示。这种方法有助于深入了解电容、能量、功率、熵和焓如何对温度和电压的变化做出反应。阅读研究文章全文,请访问 10.1002/batt.202300581。
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引用次数: 0
Cover Feature: Unveiling the Potential of Silicon-Air Batteries for Low-Power Transient Electronics: Electrochemical Insights and Practical Application (Batteries & Supercaps 5/2024) 揭示硅-空气电池在低功耗瞬态电子设备中的潜力:电化学见解与实际应用
IF 5.7 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-19 DOI: 10.1002/batt.202400244
Saul Said Montiel Guerrero, Yasin Emre Durmus, Hermann Tempel, Christian Roth, Hans Kungl, Stefan van Waasen, Yair Ein-Eli, Rüdiger-A. Eichel

The Cover Feature illustrates the silicon-air batteries, powered by silicon, as a groundbreaking solution for energizing transient electronics. By incorporating partial self-destruction mechanisms, they enhance data security and impose a controlled device lifespan. After being used as the energetic fuel, silicon can turn into silica sand, completing its life cycle. This innovative application seamlessly integrates energy storage and electronics, offering practical advancements in technology and data security. More information can be found in the Research Article by Y. E. Durmus and co-workers.

封面专题介绍了以硅为动力的硅-空气电池,它是为瞬态电子设备供电的开创性解决方案。通过采用部分自毁机制,它们提高了数据安全性,并对设备寿命进行了控制。在用作能量燃料后,硅可以变成硅砂,完成其生命周期。这一创新应用将能量存储和电子器件完美地结合在一起,为技术和数据安全带来了切实的进步。更多信息,请参阅 Y. E. Durmus 及其合作者的研究文章。Durmus 及其合作者的研究文章中。
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引用次数: 0
Cover Picture: Operando Temperature Dynamic Investigation of Electric Double-Layer Capacitors Containing Organic Electrolytes (Batteries & Supercaps 5/2024) 含有机电解质的双电层电容器的操作温度动态研究
IF 5.7 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-19 DOI: 10.1002/batt.202400243
Fabian Alexander Kreth, Lukas Köps, Scott W. Donne, Andrea Balducci

The Front Cover illustrates a supercapacitor evaluated with the screening technique. It highlights different electrolyte compositions, indicated by chemical compounds above the setup. This approach provides insights into how capacitance, energy, power, entropy, and enthalpy respond to changes in temperature and voltage. More information can be found in the Research Article by F. A. Kreth and co-workers.

封面展示了利用筛选技术评估的超级电容器。它突出显示了不同的电解质成分,由设置上方的化合物表示。这种方法有助于深入了解电容、能量、功率、熵和焓如何对温度和电压的变化做出反应。更多信息,请参阅 F. A. Kreth 及其合作者的研究文章。Kreth 及其合作者的研究文章中。
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引用次数: 0
Regulating Diffusion Coefficient of Li+ by High Binding Energy Anion towards Ultra-Low Temperature Lithium-Ion Batteries 利用高结合能阴离子调节 Li+ 的扩散系数,实现超低温锂离子电池
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-18 DOI: 10.1002/batt.202400246
Qiu Chen, Pan Luo, Li Liao, Yin Shen, Xiaoshuang Luo, Xinpeng Li, Xuanzhong Wen, Jialin Song, Dr. Bo Yu, Dr. Junchen Chen, Dr. Bingshu Guo, Prof. Mingshan Wang, Prof. Yun Huang, Fuliang Liu, Dr. Jiangtao Liu, Zhedong Li, Jingrun Ma, Shuiyong Wang, Prof. Xing Li

Electrolyte design is the optimal strategy to achieve extremely low temperature operation of lithium-ion batteries. Here, the diffusion coefficient of Li+ is proposed to improve the ion transport kinetics at low temperatures. The diffusion coefficient of Li+ is improved by constructing a Li+ solvation sheath with weak steric effects. Specifically, high binding energy BF4 anions are added to a 1 M LiPF6 in propyl acetate (PA) electrolyte. Since the binding energy of Li+ with BF4 is greater than that of PA. Therefore, the small-sized BF4 replaces the large-sized PA molecule to form a Li+ solvation sheath with a weak steric effect, which increases the diffusion coefficient of Li+. Using the high diffusion coefficient electrolyte, the 800 mAh pouch cell retain 91 % and 75 % of its room temperature capacity at −40 °C(0.5 C rate) and −60 °C (0.2 C rate), respectively. And it also shows stable cycling at −40 °C. This work provides a new strategy for designing low-temperature electrolytes of lithium-ion batteries.

电解质设计是实现锂离子电池超低温运行的最佳策略。这里提出了利用 Li+ 的扩散系数来改善低温下离子传输动力学的方法。通过构建具有弱立体效应的 Li+ 溶解鞘,可以提高 Li+ 的扩散系数。具体来说,在醋酸丙酯(PA)电解液中的 1M LiPF6 中加入高结合能的 BF4- 阴离子。由于 Li+ 与 BF4- 的结合能大于 PA 的结合能。因此,小尺寸的 BF4- 取代了大尺寸的 PA 分子,形成了一个具有弱立体效应的 Li+ 溶解鞘,从而提高了 Li+ 的扩散系数。使用高扩散系数电解质的 800 mAh 袋装电池在-40℃(0.5C 速率)和-60℃(0.2C 速率)条件下分别保持了室温容量的 91% 和 75%。它还能在-40℃下稳定循环。这项工作为锂离子电池低温电解质的设计提供了一种新策略。
{"title":"Regulating Diffusion Coefficient of Li+ by High Binding Energy Anion towards Ultra-Low Temperature Lithium-Ion Batteries","authors":"Qiu Chen,&nbsp;Pan Luo,&nbsp;Li Liao,&nbsp;Yin Shen,&nbsp;Xiaoshuang Luo,&nbsp;Xinpeng Li,&nbsp;Xuanzhong Wen,&nbsp;Jialin Song,&nbsp;Dr. Bo Yu,&nbsp;Dr. Junchen Chen,&nbsp;Dr. Bingshu Guo,&nbsp;Prof. Mingshan Wang,&nbsp;Prof. Yun Huang,&nbsp;Fuliang Liu,&nbsp;Dr. Jiangtao Liu,&nbsp;Zhedong Li,&nbsp;Jingrun Ma,&nbsp;Shuiyong Wang,&nbsp;Prof. Xing Li","doi":"10.1002/batt.202400246","DOIUrl":"10.1002/batt.202400246","url":null,"abstract":"<p>Electrolyte design is the optimal strategy to achieve extremely low temperature operation of lithium-ion batteries. Here, the diffusion coefficient of Li<sup>+</sup> is proposed to improve the ion transport kinetics at low temperatures. The diffusion coefficient of Li<sup>+</sup> is improved by constructing a Li<sup>+</sup> solvation sheath with weak steric effects. Specifically, high binding energy BF<sub>4</sub><sup>−</sup> anions are added to a 1 M LiPF<sub>6</sub> in propyl acetate (<b>PA</b>) electrolyte. Since the binding energy of Li<sup>+</sup> with BF<sub>4</sub><sup>−</sup> is greater than that of PA. Therefore, the small-sized BF<sub>4</sub><sup>−</sup> replaces the large-sized PA molecule to form a Li<sup>+</sup> solvation sheath with a weak steric effect, which increases the diffusion coefficient of Li<sup>+</sup>. Using the high diffusion coefficient electrolyte, the 800 mAh pouch cell retain 91 % and 75 % of its room temperature capacity at −40 °C(0.5 C rate) and −60 °C (0.2 C rate), respectively. And it also shows stable cycling at −40 °C. This work provides a new strategy for designing low-temperature electrolytes of lithium-ion batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"7 11","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140626922","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Novel Li-Ion Battery Diagnostics; Detection of Redox Peaks Utilising Plasmonic Fibre Optic Sensors and Evaluation of Interference on Cell Function 锂离子袋细胞中的基于等离子体的光纤传感器,检测氧化还原峰值和不干扰细胞功能
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-18 DOI: 10.1002/batt.202400079
Christopher Gardner, Elin Langhammer, Vlad Marsic, Joe Fleming, Alexander J. Roberts, Tazdin Amietszajew

In this study we demonstrate detection of redox peaks in Li-ion pouch cells during cyclic voltammetry (CV), via the optical signal of plasmonic based fibre optic sensors placed inside Li-ion pouch cells. The sensors are placed inside the pouch cells during manufacture, allowing diagnostic data to be obtained from directly inside the cells in real time. We further present data showing the battery cell remains agnostic to the presence of fibre optic sensors over repeated cycling through analysis of the formation cycles, electrochemical impedance spectroscopy (EIS) analysis, coulombic efficiency data, capacity data and post-mortem materials analysis. This study provides evidence of the utility of fibre optic based diagnostic sensors, and in particular the novel use of plasmonic based fibre optic sensors, as an in situ battery diagnostic technique and potential research tool to investigate battery cell phenomena.

在这项研究中,我们展示了在循环伏安法(CV)过程中,通过放置在锂离子小袋电池内部的基于等离子体的光纤传感器的光学信号来检测锂离子小袋电池中的氧化还原峰。这些传感器在制造过程中就被放置在袋式电池内部,从而可以直接从电池内部实时获取诊断数据。我们进一步提供的数据显示,通过对形成周期、电化学阻抗光谱(EIS)分析、库仑效率数据、容量数据和死后材料分析进行分析,电池在反复循环过程中与光纤传感器的存在无关。这项研究证明了基于光纤的诊断传感器的实用性,特别是基于等离子体的光纤传感器的新用途,可作为一种现场电池诊断技术和潜在的研究工具,用于研究电池单元现象。
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引用次数: 0
Agar-Based Interface for Suppressing Parasitic Reactions toward High-Performance Aqueous Zn-Ion Batteries 抑制寄生反应的琼脂基界面,实现高性能水性锌离子电池
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-16 DOI: 10.1002/batt.202400159
Dr. Yi-Fan Qu, Dr. Xin Liu, Dr. Jia-Wei Qian, Prof. Jingwei Chen, Prof. Li-Feng Chen

With advantages including high capacity, intrinsic safety and low cost, aqueous zinc-ion batteries (AZIBs) are ideal electrochemical energy storage devices for large-scale and portable energy storage. However, the development of AZIBs suffers from tricky challenges, such as the notorious Zn dendrite growth and severe parasitic reactions. Herein, as a low-cost and nontoxic biomass, agar is adopted to construct an interface layer on Zn foil to mitigate side reactions and induce uniform Zn deposition on Zn anodes. The interaction between Zn2+ and polar functional groups of agar can regulate Zn2+ distribution and promote Zn2+ desolvation, thus simultaneously achieving homogenous Zn deposition and suppressed hydrogen evolution reaction. Meanwhile, SO42− anions are blocked from contacting Zn surface due to electrostatic repulsion, greatly restraining corrosion and passivation. Consequently, Zn||A-Cu asymmetric cell operates normally for 590 cycles with an average coulombic efficiency of 99.5 %, suggesting good reversibility of Zn plating/stripping. Notably, A-Zn symmetric cell exhibits a long lifespan of 1100 h at 2 mA cm−2. Furthermore, the A-Zn||NVO full cell displays a superb capacity retention of 94.8 % after 3600 cycles at 5 A g−1. This work offers a novel interface modification method for constructing stable and dendrite-free anodes of AZIBs.

锌离子水电池(AZIBs)具有容量大、内在安全和成本低等优点,是大规模和便携式储能的理想电化学储能设备。然而,AZIBs 的开发面临着棘手的挑战,例如臭名昭著的锌枝晶生长和严重的寄生反应。在本文中,琼脂作为一种低成本、无毒的生物质,被用来在锌箔上构建界面层,以减轻副反应并诱导锌在锌阳极上均匀沉积。Zn2+ 与琼脂极性官能团之间的相互作用可以调节 Zn2+ 的分布,促进 Zn2+ 的脱溶,从而同时实现均匀的 Zn 沉积和抑制氢演化反应。同时,由于静电排斥作用,SO42- 阴离子被阻止与 Zn 表面接触,从而大大抑制了腐蚀和钝化。因此,Zn||A-Cu 不对称电池可正常运行 590 个周期,平均库仑效率为 99.5%,表明 Zn 镀层/剥离具有良好的可逆性。值得注意的是,在 2 mA cm-2 电流条件下,A-Zn 对称电池的寿命长达 1100 小时。此外,A-Zn||NVO 全电池在 5 A g-1 的条件下循环 3600 次后,容量保持率高达 94.8%。这项研究为构建稳定、无树枝状突起的 AZIBs 阳极提供了一种新颖的界面改性方法。
{"title":"Agar-Based Interface for Suppressing Parasitic Reactions toward High-Performance Aqueous Zn-Ion Batteries","authors":"Dr. Yi-Fan Qu,&nbsp;Dr. Xin Liu,&nbsp;Dr. Jia-Wei Qian,&nbsp;Prof. Jingwei Chen,&nbsp;Prof. Li-Feng Chen","doi":"10.1002/batt.202400159","DOIUrl":"10.1002/batt.202400159","url":null,"abstract":"<p>With advantages including high capacity, intrinsic safety and low cost, aqueous zinc-ion batteries (AZIBs) are ideal electrochemical energy storage devices for large-scale and portable energy storage. However, the development of AZIBs suffers from tricky challenges, such as the notorious Zn dendrite growth and severe parasitic reactions. Herein, as a low-cost and nontoxic biomass, agar is adopted to construct an interface layer on Zn foil to mitigate side reactions and induce uniform Zn deposition on Zn anodes. The interaction between Zn<sup>2+</sup> and polar functional groups of agar can regulate Zn<sup>2+</sup> distribution and promote Zn<sup>2+</sup> desolvation, thus simultaneously achieving homogenous Zn deposition and suppressed hydrogen evolution reaction. Meanwhile, SO<sub>4</sub><sup>2−</sup> anions are blocked from contacting Zn surface due to electrostatic repulsion, greatly restraining corrosion and passivation. Consequently, Zn||A-Cu asymmetric cell operates normally for 590 cycles with an average coulombic efficiency of 99.5 %, suggesting good reversibility of Zn plating/stripping. Notably, A-Zn symmetric cell exhibits a long lifespan of 1100 h at 2 mA cm<sup>−2</sup>. Furthermore, the A-Zn||NVO full cell displays a superb capacity retention of 94.8 % after 3600 cycles at 5 A g<sup>−1</sup>. This work offers a novel interface modification method for constructing stable and dendrite-free anodes of AZIBs.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"7 9","pages":""},"PeriodicalIF":5.1,"publicationDate":"2024-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140570759","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Data-Driven Design of NASICON-Type Electrodes Using Graph-Based Neural Networks 利用基于图形的神经网络,以数据为导向设计 NASICON 型电极
IF 5.1 4区 材料科学 Q2 ELECTROCHEMISTRY Pub Date : 2024-04-16 DOI: 10.1002/batt.202400186
Dr. Yoonsu Shim, Dr. Incheol Jeong, Junpyo Hur, Prof. Dr. Hyoungjeen Jeen, Prof. Dr. Seung-Taek Myung, Prof. Dr. Kang Taek Lee, Prof. Dr. Seungbum Hong, Prof. Dr. Jong Min Yuk, Dr. Chan-Woo Lee

Sodium superionic conductor (NASICON)-type cathode materials are considered promising candidates for high-performance sodium-ion batteries (SIBs) because of the abundance and low cost of raw materials. However, NASICON-type cathodes suffer from low capacities. This limitation can be addressed through the activation of sodium-excess phases, which can enhance capacities up to theoretical values. Thus, this paper proposes the use of transition metal (TM)-substituted Na3V2(PO4)2F3 (NVPF) to induce sodium-excess phases. To identify suitable doping elements, an inverse design approach is developed, combining machine learning prediction and density functional theory (DFT) calculations. Graph-based neural networks are used to predict two crucial properties, i. e., the structural stability and voltage level. Results indicate that the use of TM-substituted NVPF materials leads to about 150 % capacity enhancement with reduced time and resource requirements compared with the direct design approach. Furthermore, DFT calculations confirm improvements in cyclability, electronic conductivity, and chemical stability. The proposed approach is expected to accelerate the discovery of superior materials for battery electrodes.

钠超离子导体(NASICON)型阴极材料由于原材料丰富且成本低廉,被认为是高性能钠离子电池(SIB)的理想候选材料。然而,NASICON 型阴极的容量较低。这一限制可以通过活化钠过剩相来解决,活化钠过剩相可以将容量提高到理论值。因此,本文提出使用过渡金属 (TM) 取代的 Na3V2(PO4)2F3 (NVPF) 来诱导钠过剩相。为确定合适的掺杂元素,结合机器学习预测和密度泛函理论(DFT)计算,开发了一种反向设计方法。基于图形的神经网络被用来预测两个关键特性,即结构稳定性和电压水平。结果表明,与直接设计方法相比,使用 TM 取代的 NVPF 材料可将容量提高约 150%,同时减少了时间和资源需求。此外,DFT 计算还证实了可循环性、电子导电性和化学稳定性的改善。所提出的方法有望加速发现电池电极的优质材料。
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引用次数: 0
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