Pub Date : 2026-01-03DOI: 10.1016/j.jpowsour.2025.239246
Jihyeon Bae , Youngjun Shin , Seoa Kim, Jangho Park, Sanghyuk Park, Kyungjung Kwon
Aluminum is both a popular dopant for LiNixCoyMn1-x-yO2 cathode active materials to improve Li-ion battery (LIB) performance and a major impurity in LIB recycling. In this study, Li[Ni1/3Co1/3Mn1/3]1-xAlxO2 (NCMA, x = 0.05 and 2 mol%) is synthesized via coprecipitation and solid-state methods to investigate the influence of Al incorporation on its physiochemical and electrochemical properties. The sphericity of the secondary particles in NCMA samples doped with Al by coprecipitation decreases with increasing Al content, which adversely affects the electrochemical performance. In contrast, the Al doping expands lithium interslab layer and suppresses cation mixing, irrespective of the doping method. A secondary LiAlO2 phase is detected in NCMA with the high Al content by the solid-state method, contributing to enhanced rate performance. Overall, it can be concluded that an appropriate amount of Al doping helps to enhance cycling stability, and the samples doped via the solid-state method exhibit superior electrochemical performance. These findings highlight that controlled Al incorporation not only stabilizes the layered structure but also provides a design strategy for optimizing both recycled and newly synthesized NCM cathode active materials.
铝是提高锂离子电池（LIB）性能的常用正极活性材料掺杂剂，也是锂离子电池（LIB）回收的主要杂质。本研究采用共沉淀法和固相法合成Li[Ni1/3Co1/3Mn1/3]1-xAlxO2 (NCMA, x = 0.05, 2 mol%)，研究Al掺入对其理化和电化学性能的影响。在共沉淀法掺杂Al的NCMA样品中，二次粒子的球形度随着Al含量的增加而降低，对电化学性能产生不利影响。相反，无论掺杂方式如何，Al掺杂都会使锂板间层膨胀并抑制阳离子混合。在高Al含量的NCMA中，通过固态法检测到二级LiAlO2相，有助于提高速率性能。综上所述，适量的Al掺杂有助于提高循环稳定性，通过固态法掺杂的样品表现出优异的电化学性能。这些发现强调，控制铝的掺入不仅稳定了层状结构，而且为优化回收和新合成的NCM阴极活性材料提供了一种设计策略。
{"title":"Maximizing the doping effect of Al in LiNixCoyMn1-x-yO2 cathode active materials for Li-ion batteries","authors":"Jihyeon Bae , Youngjun Shin , Seoa Kim, Jangho Park, Sanghyuk Park, Kyungjung Kwon","doi":"10.1016/j.jpowsour.2025.239246","DOIUrl":"10.1016/j.jpowsour.2025.239246","url":null,"abstract":"<div><div>Aluminum is both a popular dopant for LiNi<sub>x</sub>Co<sub>y</sub>Mn<sub>1-x-y</sub>O<sub>2</sub> cathode active materials to improve Li-ion battery (LIB) performance and a major impurity in LIB recycling. In this study, Li[Ni<sub>1/3</sub>Co<sub>1/3</sub>Mn<sub>1/3</sub>]<sub>1-x</sub>Al<sub>x</sub>O<sub>2</sub> (NCMA, x = 0.05 and 2 mol%) is synthesized via coprecipitation and solid-state methods to investigate the influence of Al incorporation on its physiochemical and electrochemical properties. The sphericity of the secondary particles in NCMA samples doped with Al by coprecipitation decreases with increasing Al content, which adversely affects the electrochemical performance. In contrast, the Al doping expands lithium interslab layer and suppresses cation mixing, irrespective of the doping method. A secondary LiAlO<sub>2</sub> phase is detected in NCMA with the high Al content by the solid-state method, contributing to enhanced rate performance. Overall, it can be concluded that an appropriate amount of Al doping helps to enhance cycling stability, and the samples doped via the solid-state method exhibit superior electrochemical performance. These findings highlight that controlled Al incorporation not only stabilizes the layered structure but also provides a design strategy for optimizing both recycled and newly synthesized NCM cathode active materials.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239246"},"PeriodicalIF":7.9,"publicationDate":"2026-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882703","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239174
Chikwesiri Imediegwu , Milo S.P. Shaffer , Mary P. Ryan , Ajit Panesar
Effective battery design is complex, requiring the resolution of multiple conflicting demands. Even where optimal electrode thickness, porosity, and architecture have been determined for isolated electrodes, designing optimal electrode parameters in full-cell configurations remains challenging. The performances of the positive and negative electrodes are linked due to the need to balance their capacities and complicated by differing rate-limiting mechanisms and ion transport asymmetries, under charge and discharge. This work develops a rational strategy for full-cell electrode design. First, validated, physics-based continuum models are used to determine Pareto fronts identifying best target negative and positive electrode thickness and porosity, under charge and discharge. The calculated ion concentrations provide a mechanistic understanding of the charge/discharge asymmetry. These Pareto fronts are then plotted in the areal capacity-volumetric energy density plane to identify the most effective electrode combinations. The approach is illustrated for a lithium-ion cell configuration using a graphite negative electrode and a LiNi0.6Mn0.2Co0.2O2 positive electrode (Gr/NMC622) but can be generalised to other electrode pairs and battery chemistries.
{"title":"Maximising lithium battery performance by capacity balancing: Determining the Pareto fronts for electrode thickness and porosity","authors":"Chikwesiri Imediegwu , Milo S.P. Shaffer , Mary P. Ryan , Ajit Panesar","doi":"10.1016/j.jpowsour.2025.239174","DOIUrl":"10.1016/j.jpowsour.2025.239174","url":null,"abstract":"<div><div>Effective battery design is complex, requiring the resolution of multiple conflicting demands. Even where optimal electrode thickness, porosity, and architecture have been determined for isolated electrodes, designing optimal electrode parameters in full-cell configurations remains challenging. The performances of the positive and negative electrodes are linked due to the need to balance their capacities and complicated by differing rate-limiting mechanisms and ion transport asymmetries, under charge and discharge. This work develops a rational strategy for full-cell electrode design. First, validated, physics-based continuum models are used to determine Pareto fronts identifying best target negative and positive electrode thickness and porosity, under charge and discharge. The calculated ion concentrations provide a mechanistic understanding of the charge/discharge asymmetry. These Pareto fronts are then plotted in the areal capacity-volumetric energy density plane to identify the most effective electrode combinations. The approach is illustrated for a lithium-ion cell configuration using a graphite negative electrode and a LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub> positive electrode (Gr/NMC622) but can be generalised to other electrode pairs and battery chemistries.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239174"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239218
Xiangjie Fu , Xingkao Zhang , Xingliang He , Zhijie He , Li Ma , Haowen Wang , Ju Rong , Hanqing Li , Xiaohua Yu
With the growing demand for high energy storage performance across various industries, two-dimensional (2D) materials garner significant attention due to their immense potential as secondary battery electrodes. Among these, molybdenum diselenide (MoSe2) stands out as a highly promising anode material owing to its exceptional mechanical properties, electrical conductivity, and thermal stability. This study employs first-principles density functional theory (DFT) calculations to systematically evaluate the application potential of monolayer MoSe2 as an anode material for Li+, Na+, and K+ batteries. Results demonstrate that MoSe2 exhibits high theoretical specific capacities of 422 mAh·g−1 for both lithium-ion batteries (LIB) and sodium-ion batteries (SIB), and 246 mAh·g−1 for potassium-ion batteries (PIB). Ab initio molecular dynamics (AIMD) simulations reveal that MoSe2 maintains structural integrity at elevated temperatures up to 1000 K, and demonstrates excellent thermodynamic stability. Furthermore, during ion adsorption, MoSe2 exhibits metallic behavior, which indicates its superior electronic conductivity. Simultaneously, MoSe2 exhibits moderate average open-circuit voltage (OCV) and extremely low ion diffusion barriers (Li: 0.036 eV, Na: 0.016 eV, K: 0.012 eV), which suggests outstanding rate performance and charge transport capability. Consequently, this work demonstrates the significant potential of MoSe2 as a high-performance secondary battery anode material.
{"title":"First-principles design of high-performance monolayer MoSe2 anode for multiple ions batteries","authors":"Xiangjie Fu , Xingkao Zhang , Xingliang He , Zhijie He , Li Ma , Haowen Wang , Ju Rong , Hanqing Li , Xiaohua Yu","doi":"10.1016/j.jpowsour.2025.239218","DOIUrl":"10.1016/j.jpowsour.2025.239218","url":null,"abstract":"<div><div>With the growing demand for high energy storage performance across various industries, two-dimensional (2D) materials garner significant attention due to their immense potential as secondary battery electrodes. Among these, molybdenum diselenide (MoSe<sub>2</sub>) stands out as a highly promising anode material owing to its exceptional mechanical properties, electrical conductivity, and thermal stability. This study employs first-principles density functional theory (DFT) calculations to systematically evaluate the application potential of monolayer MoSe<sub>2</sub> as an anode material for Li<sup>+</sup>, Na<sup>+</sup>, and K<sup>+</sup> batteries. Results demonstrate that MoSe<sub>2</sub> exhibits high theoretical specific capacities of 422 mAh·g<sup>−1</sup> for both lithium-ion batteries (LIB) and sodium-ion batteries (SIB), and 246 mAh·g<sup>−1</sup> for potassium-ion batteries (PIB). Ab initio molecular dynamics (AIMD) simulations reveal that MoSe<sub>2</sub> maintains structural integrity at elevated temperatures up to 1000 K, and demonstrates excellent thermodynamic stability. Furthermore, during ion adsorption, MoSe<sub>2</sub> exhibits metallic behavior, which indicates its superior electronic conductivity. Simultaneously, MoSe<sub>2</sub> exhibits moderate average open-circuit voltage (OCV) and extremely low ion diffusion barriers (Li: 0.036 eV, Na: 0.016 eV, K: 0.012 eV), which suggests outstanding rate performance and charge transport capability. Consequently, this work demonstrates the significant potential of MoSe<sub>2</sub> as a high-performance secondary battery anode material.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239218"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882805","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239172
Yuvaraj Subramanian , Jung-Jae Park , Sung Kang , Kwang-Sun Ryu
Oxyhalide solid electrolytes have been extensively investigated for lithium solid-state batteries due to their exceptional Li-ion conductivity, which surpasses that of well-known systems such as halide and sulfide solid electrolytes. In this perspective, we select the oxyhalide LiTaOCl4 system, however, it exhibits a low ionic conductivity in the range of 2–3 mS cm−1. Consequently, this work aims to enhance the ionic conductivity of the oxyhalide electrolyte through fine-tuning of the oxygen content. We prepare a series of oxyhalide systems, LiTaO1+xCl6-2x (0 ≤ x ≤ 0.5), through a ball milling process. Remarkably, the LiTaO1.35Cl3.3 electrolyte exhibits a 3-fold increase in ionic conductivity (7.34 mS cm−1) compared to the base electrolyte. The LiTaO1.35Cl3.3 electrolyte also presents an electrochemical stability window of 2.35–3.75 V, which is broader than that of sulfide solid electrolytes. The solid-state battery employing the LiTaO1.35Cl3.3 electrolyte exhibits a higher discharge capacity of 182 mAh g−1 at a 0.1 C rate compared to LiTaOCl4, which achieves 155.6 mAh g−1. We conclude that the highly ionic conducting nature of the excess oxygen-incorporated oxyhalide solid electrolyte significantly enhances electrochemical performance. Thus, it is deemed a promising candidate for future lithium solid-state batteries.
由于氧卤化物固体电解质具有优异的锂离子导电性，因此已被广泛研究用于锂固态电池，其导电性优于卤化物和硫化物固体电解质等众所周知的系统。从这个角度来看，我们选择了氧化卤化物LiTaOCl4体系，然而，它在2-3 mS cm−1的范围内表现出较低的离子电导率。因此，本工作旨在通过微调氧含量来提高氧化卤化物电解质的离子电导率。通过球磨工艺制备了LiTaO1+xCl6-2x（0≤x≤0.5）系列氧化卤化物体系。值得注意的是，与碱电解质相比，LiTaO1.35Cl3.3电解质的离子电导率提高了3倍（7.34 mS cm−1）。LiTaO1.35Cl3.3电解质也呈现出2.35 ~ 3.75 V的电化学稳定窗口，比硫化物固体电解质更宽。采用LiTaO1.35Cl3.3电解质的固态电池在0.1 C倍率下的放电容量为182 mAh g−1，而LiTaOCl4的放电容量为155.6 mAh g−1。结果表明，过量含氧氧化卤化物固体电解质的高离子导电性显著提高了电化学性能。因此，它被认为是未来锂固态电池的有前途的候选者。
{"title":"Fine-tuning of oxygen content enables fast Li-ion transport in oxy-chloride solid electrolyte for high voltage all-solid-state batteries","authors":"Yuvaraj Subramanian , Jung-Jae Park , Sung Kang , Kwang-Sun Ryu","doi":"10.1016/j.jpowsour.2025.239172","DOIUrl":"10.1016/j.jpowsour.2025.239172","url":null,"abstract":"<div><div>Oxyhalide solid electrolytes have been extensively investigated for lithium solid-state batteries due to their exceptional Li-ion conductivity, which surpasses that of well-known systems such as halide and sulfide solid electrolytes. In this perspective, we select the oxyhalide LiTaOCl<sub>4</sub> system, however, it exhibits a low ionic conductivity in the range of 2–3 mS cm<sup>−1</sup>. Consequently, this work aims to enhance the ionic conductivity of the oxyhalide electrolyte through fine-tuning of the oxygen content. We prepare a series of oxyhalide systems, LiTaO<sub>1+x</sub>Cl<sub>6-2x</sub> (0 ≤ x ≤ 0.5), through a ball milling process. Remarkably, the LiTaO<sub>1.35</sub>Cl<sub>3.3</sub> electrolyte exhibits a 3-fold increase in ionic conductivity (7.34 mS cm<sup>−1</sup>) compared to the base electrolyte. The LiTaO<sub>1.35</sub>Cl<sub>3.3</sub> electrolyte also presents an electrochemical stability window of 2.35–3.75 V, which is broader than that of sulfide solid electrolytes. The solid-state battery employing the LiTaO<sub>1.35</sub>Cl<sub>3.3</sub> electrolyte exhibits a higher discharge capacity of 182 mAh g<sup>−1</sup> at a 0.1 C rate compared to LiTaOCl<sub>4</sub>, which achieves 155.6 mAh g<sup>−1</sup>. We conclude that the highly ionic conducting nature of the excess oxygen-incorporated oxyhalide solid electrolyte significantly enhances electrochemical performance. Thus, it is deemed a promising candidate for future lithium solid-state batteries.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239172"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882701","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239239
Kun Yang , Yichi Zhang , Zhuoyu Feng , Yanrong Zhu , Zhengxiang Song , Jinhao Meng
Accurate estimation of battery states is critical for monitoring safety. Impedance has emerged as a powerful parameter for precisely estimating key states of batteries. However, fast battery impedance measurements always require high generation frequency hardware, which limit their practical applications. The objective of this paper is to decrease the generation frequency while keeping short measurement time. In this paper, the discrete interval binary sequence (DIBS) is used with enhanced low-frequency component. Meanwhile, impedance of low-frequency region is calculated by discrete Fourier transform (DFT), and impedance of high-frequency region is calculated by S transform (ST) through averaging eight edges. The experimental results confirm effectiveness of this method. With only 3 Hz generation frequency, precise impedance measurements within the range of 0.1 Hz–1000 Hz are achieved in just 10.33 s. Verification is conducted with different battery states. The normalized root mean square errors (NRMSEs) and mean absolute percentage errors (MAPEs) of the measurements are below 2.32 % and 2.03 %, respectively.
{"title":"Fast battery impedance measurement based on discrete Fourier transform and S transform with discrete interval binary sequence","authors":"Kun Yang , Yichi Zhang , Zhuoyu Feng , Yanrong Zhu , Zhengxiang Song , Jinhao Meng","doi":"10.1016/j.jpowsour.2025.239239","DOIUrl":"10.1016/j.jpowsour.2025.239239","url":null,"abstract":"<div><div>Accurate estimation of battery states is critical for monitoring safety. Impedance has emerged as a powerful parameter for precisely estimating key states of batteries. However, fast battery impedance measurements always require high generation frequency hardware, which limit their practical applications. The objective of this paper is to decrease the generation frequency while keeping short measurement time. In this paper, the discrete interval binary sequence (DIBS) is used with enhanced low-frequency component. Meanwhile, impedance of low-frequency region is calculated by discrete Fourier transform (DFT), and impedance of high-frequency region is calculated by S transform (ST) through averaging eight edges. The experimental results confirm effectiveness of this method. With only 3 Hz generation frequency, precise impedance measurements within the range of 0.1 Hz–1000 Hz are achieved in just 10.33 s. Verification is conducted with different battery states. The normalized root mean square errors (NRMSEs) and mean absolute percentage errors (MAPEs) of the measurements are below 2.32 % and 2.03 %, respectively.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239239"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239216
Iqra Shaheen , Wei-Hao Chiu , Yu-Xian Lee , Shih-Hsuan Chen , Jen-Fu Hsu , Kun-Mu Lee
Graphite felt (GF) is a porous carbonized polymer used as multifunctional electrodes in energy and environmental electrochemical devices. Despite its high surface area, limited surface-active sites reduce catalytic activity. Furthermore, its intrinsic hydrophobicity requires hydrophilic pretreatment for effective electrochemical performance. Graphitic Carbon Nitride (g-C3N4) enables structural regulation by creating conjugated systems through its electronic structure, thereby expanding its multifunctionality and applications in electrode materials. An optimal g-C3N4 concentration on the GF ensures better conductivity, resulting in higher electrochemical activity. This study used thermal polymerization to decorate GF with g-C3N4 (GCN/GF), and nano GCN/GF electrode showed excellent hydrophilicity, lowest charge-transfer resistance (Rct), and high electrochemical activity. An optimally decorated g-C3N4 showed minimal agglomeration, better distribution on GF surfaces, and superior active sites for VO2+/VO2+ redox reaction. Its uniform decoration of g-C3N4 facilitated charge transport, enhanced hydrophilicity, and improved electrolyte access, reducing electrochemical polarization during active species transfer, and energy efficiency improved to 84.13 % at 80 mA cm−2. The long-term cycling performance confirmed the durability of the vanadium redox flow battery (VRFB) with the nano GCN/GF electrode, exhibiting negligible degradation for 1000 cycles. These findings highlight the potential of g-C3N4 as a cost-effective alternative to noble metals for high-performance VRFB electrodes.
石墨毡（GF）是一种多孔碳化聚合物，在能源和环境电化学装置中用作多功能电极。尽管它的表面积很大，但有限的表面活性位点降低了催化活性。此外，其固有的疏水性需要亲水性预处理才能获得有效的电化学性能。石墨氮化碳（g-C3N4）通过其电子结构创建共轭系统，从而扩展其在电极材料中的多功能性和应用，从而实现结构调节。GF上最佳的g-C3N4浓度确保了更好的导电性，从而提高了电化学活性。本研究采用热聚合的方法，用g-C3N4 （GCN/GF）修饰GF，纳米GCN/GF电极具有优异的亲水性、最低的电荷转移电阻（Rct）和较高的电化学活性。经过优化修饰的g-C3N4具有最小的团聚、更好的GF表面分布和更好的VO2+/VO2+氧化还原反应活性位点。g-C3N4的均匀修饰促进了电荷传输，增强了亲水性，改善了电解质的获取，减少了活性物质转移过程中的电化学极化，在80 mA cm−2下，能量效率提高到84.13%。长期循环性能证实了纳米GCN/GF电极的钒氧化还原液流电池（VRFB）的耐久性，在1000次循环中表现出可以忽略的退化。这些发现突出了g-C3N4作为高性能VRFB电极的一种具有成本效益的贵金属替代品的潜力。
{"title":"Heterogeneous graphite felt electrodes decorated with nanostructured graphitic carbon nitride for enhanced redox kinetics in vanadium redox flow batteries","authors":"Iqra Shaheen , Wei-Hao Chiu , Yu-Xian Lee , Shih-Hsuan Chen , Jen-Fu Hsu , Kun-Mu Lee","doi":"10.1016/j.jpowsour.2025.239216","DOIUrl":"10.1016/j.jpowsour.2025.239216","url":null,"abstract":"<div><div>Graphite felt (GF) is a porous carbonized polymer used as multifunctional electrodes in energy and environmental electrochemical devices. Despite its high surface area, limited surface-active sites reduce catalytic activity. Furthermore, its intrinsic hydrophobicity requires hydrophilic pretreatment for effective electrochemical performance. Graphitic Carbon Nitride (g-C<sub>3</sub>N<sub>4</sub>) enables structural regulation by creating conjugated systems through its electronic structure, thereby expanding its multifunctionality and applications in electrode materials. An optimal g-C<sub>3</sub>N<sub>4</sub> concentration on the GF ensures better conductivity, resulting in higher electrochemical activity. This study used thermal polymerization to decorate GF with g-C<sub>3</sub>N<sub>4</sub> (GCN/GF), and nano GCN/GF electrode showed excellent hydrophilicity, lowest charge-transfer resistance (R<sub>ct</sub>), and high electrochemical activity. An optimally decorated g-C<sub>3</sub>N<sub>4</sub> showed minimal agglomeration, better distribution on GF surfaces, and superior active sites for VO<sup>2+</sup>/VO<sub>2</sub><sup>+</sup> redox reaction. Its uniform decoration of g-C<sub>3</sub>N<sub>4</sub> facilitated charge transport, enhanced hydrophilicity, and improved electrolyte access, reducing electrochemical polarization during active species transfer, and energy efficiency improved to 84.13 % at 80 mA cm<sup>−2</sup>. The long-term cycling performance confirmed the durability of the vanadium redox flow battery (VRFB) with the nano GCN/GF electrode, exhibiting negligible degradation for 1000 cycles. These findings highlight the potential of g-C<sub>3</sub>N<sub>4</sub> as a cost-effective alternative to noble metals for high-performance VRFB electrodes.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239216"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239229
Shuang-shuang Zhang , Yong-qi Tian , Bo-yao Zhang , Yu-wen Pan , Yi-bo Wang , Jun Xiang , De-peng Zhao , Rong-da Zhao , Fu-fa Wu , Li-hua Miao
Given the pressing global energy crisis, developing high-performance, stable electrocatalysts for hydrogen production through water electrolysis is of paramount significance. In this work, a nickel-cobalt (Ni-Co) precursor is first synthesized on a nickel foam (NF) substrate via a hydrothermal approach, the layered structure of the precursor enables the atomic-scale dispersion of Co2+ and Ni2+ ions, ensuring that the two metal elements are uniformly distributed in the selenide at a 1:1 ratio after subsequent selenization. Additionally, it can act as a template to guide the selenization and composite reactions, allowing the final product to retain a certain layered derived structure. followed by the in-situ growth of a Co0.5Ni0.5Se2@NiFe-LDH(Nickel-Iron Layered Double Hydroxide) heterostructured catalyst on its surface. Electrochemical tests in a 1 M KOH electrolyte reveal that the as-prepared catalyst exhibits exceptional hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activities: at a current density of 50 mA cm−2, the required overpotentials are merely 219 mV and 247 mV, respectively. More notably, when tested in an alkaline seawater electrolysis system-an environment closer to practical application scenarios-the catalyst retains its high catalytic efficiency, with the HER and OER overpotentials increasing only slightly to 223 mV and 249 mV (at 50 mA cm−2). These results underscore the catalyst's promising potential for real-world applications and provide a novel strategy for the design of high-efficiency bifunctional electrocatalysts for water electrolysis.
在全球能源危机日益严重的背景下，开发高性能、稳定的电解制氢电催化剂具有重要意义。本研究首先通过水热法在泡沫镍（NF）衬底上合成了镍钴（Ni-Co）前驱体，前驱体的层状结构使Co2+和Ni2+离子在原子尺度上分散，确保两种金属元素在随后的硒化后以1:1的比例均匀分布在硒化物中。此外，它还可以作为模板来指导硒化和复合反应，使最终产物保持一定的层状衍生结构。然后在其表面原位生长Co0.5Ni0.5Se2@NiFe-LDH（镍铁层状双氢氧化物）异质结构催化剂。在1 M KOH电解液中进行的电化学测试表明，所制备的催化剂具有优异的析氢反应（HER）和析氧反应（OER）活性：在电流密度为50 mA cm - 2时，所需过电位分别仅为219 mV和247 mV。更值得注意的是，当在碱性海水电解系统（更接近实际应用场景的环境）中进行测试时，催化剂保持了高催化效率，HER和OER过电位仅略微增加到223 mV和249 mV （50 mA cm - 2）。这些结果强调了催化剂在实际应用中的良好潜力，并为设计高效的双功能水电解电催化剂提供了一种新的策略。
{"title":"In-situ grown Co0.5Ni0.5Se2@Nickel-Iron layered double hydroxide heterostructure on nickel foam for high-performance bifunctional electrocatalysis in alkaline and seawater electrolysis","authors":"Shuang-shuang Zhang , Yong-qi Tian , Bo-yao Zhang , Yu-wen Pan , Yi-bo Wang , Jun Xiang , De-peng Zhao , Rong-da Zhao , Fu-fa Wu , Li-hua Miao","doi":"10.1016/j.jpowsour.2025.239229","DOIUrl":"10.1016/j.jpowsour.2025.239229","url":null,"abstract":"<div><div>Given the pressing global energy crisis, developing high-performance, stable electrocatalysts for hydrogen production through water electrolysis is of paramount significance. In this work, a nickel-cobalt (Ni-Co) precursor is first synthesized on a nickel foam (NF) substrate via a hydrothermal approach, the layered structure of the precursor enables the atomic-scale dispersion of Co<sup>2+</sup> and Ni<sup>2+</sup> ions, ensuring that the two metal elements are uniformly distributed in the selenide at a 1:1 ratio after subsequent selenization. Additionally, it can act as a template to guide the selenization and composite reactions, allowing the final product to retain a certain layered derived structure. followed by the in-situ growth of a Co<sub>0.5</sub>Ni<sub>0.5</sub>Se<sub>2</sub>@NiFe-LDH(Nickel-Iron Layered Double Hydroxide) heterostructured catalyst on its surface. Electrochemical tests in a 1 M KOH electrolyte reveal that the as-prepared catalyst exhibits exceptional hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activities: at a current density of 50 mA cm<sup>−2</sup>, the required overpotentials are merely 219 mV and 247 mV, respectively. More notably, when tested in an alkaline seawater electrolysis system-an environment closer to practical application scenarios-the catalyst retains its high catalytic efficiency, with the HER and OER overpotentials increasing only slightly to 223 mV and 249 mV (at 50 mA cm<sup>−2</sup>). These results underscore the catalyst's promising potential for real-world applications and provide a novel strategy for the design of high-efficiency bifunctional electrocatalysts for water electrolysis.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239229"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882804","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239029
Sourabh S. Chougule , Rakesh Kulkarni , Ernesto Chicardi , Arun Thirumurugan , Abdullah K. Alanazi , N. Clament Sagaya Selvam , A. Anto Jeffery , Krishnakumar Balu , Namgee Jung
Developing multicomponent hybrid catalysts with optimized structures and tailored electrochemical properties is vital for efficient water splitting. Herein, iron/iron sulphide/N-doped carbon/molytungsten oxysulphide (Fe/FeSx/NC/MoWOxSy) multicomponent hybrid catalysts are fabricated by disproportionation reaction between amorphous molytungsten oxysulphide (MoWOxSy) and iron pthalocyanine (Fe(H2Pc)). The study elucidates the role of how multiple heterointerfaces play vital role in enhancing hydrogen and oxygen evolution reaction (HER/OER) kinetics. Structural and microscopic analyses reveal Fe/FeSx nanoparticles embedded in N-doped carbon, which envelops on 2D MoWOxSy sheets. Strong interfacial coupling between Fe/FeSx/NC and MoWOxSy modulates the electronic structure, increases conductivity, and enriches surface active sites, yielding synergistic catalytic effects. The hybrid exhibits outstanding bifunctional activity in alkaline KOH, with η10 values of 22 mVRHE (HER) and 110 mVRHE (OER). As a bifunctional catalyst pair (Fe/FeSx/NC/MoWOxSy‖Fe/FeSx/NC/MoWOxSy), it drives overall water splitting at 1.42 V and 10 mA cm−2, maintaining stability over 100 h. Post-catalysis analysis identifies the reconstructed FeOOH@Fe/FeSx/NC/MoWOxSy as the probable active phase, where electronic interactions and efficient charge transfer underpin surface reaction kinetics leading to exceptional performance. This multicomponent design offers a promising strategy for high-efficiency water splitting and broader electrochemical energy applications.
开发具有优化结构和定制电化学性能的多组分杂化催化剂是实现高效水分解的关键。通过非晶态氧化钨钼（MoWOxSy）与酞菁铁（Fe(H2Pc)）的歧化反应，制备了铁/硫化铁/ n掺杂碳/氧化钨钼（Fe/FeSx/NC/MoWOxSy）多组分杂化催化剂。该研究阐明了多异质界面在增强析氢/析氧反应（HER/OER）动力学中的重要作用。结构和微观分析表明，Fe/FeSx纳米颗粒嵌入在n掺杂碳中，包裹在二维MoWOxSy薄片上。Fe/FeSx/NC与MoWOxSy之间的强界面耦合调节了电子结构，提高了电导率，丰富了表面活性位点，产生了协同催化效应。杂交种在碱性KOH中表现出良好的双功能活性，η值为22 mVRHE （HER）和110 mVRHE （OER）。作为双功能催化剂对（Fe/FeSx/NC/MoWOxSy‖Fe/FeSx/NC/MoWOxSy），它驱动整体水在1.42 V和10 mA cm - 2下分裂，在100小时内保持稳定性。催化后分析确定重建FeOOH@Fe/FeSx/NC/MoWOxSy为可能的活性相，其中电子相互作用和有效的电荷转移支撑表面反应动力学，导致卓越的性能。这种多组分设计为高效水分解和更广泛的电化学能量应用提供了一种有前途的策略。
{"title":"Multiple-interface engineering in Fe/FeSx/NC/MoWOxSy hybrid electrocatalyst via disproportionation reaction for efficient water splitting","authors":"Sourabh S. Chougule , Rakesh Kulkarni , Ernesto Chicardi , Arun Thirumurugan , Abdullah K. Alanazi , N. Clament Sagaya Selvam , A. Anto Jeffery , Krishnakumar Balu , Namgee Jung","doi":"10.1016/j.jpowsour.2025.239029","DOIUrl":"10.1016/j.jpowsour.2025.239029","url":null,"abstract":"<div><div>Developing multicomponent hybrid catalysts with optimized structures and tailored electrochemical properties is vital for efficient water splitting. Herein, iron/iron sulphide/N-doped carbon/molytungsten oxysulphide (Fe/FeS<sub>x</sub>/NC/MoWO<sub>x</sub>S<sub>y</sub>) multicomponent hybrid catalysts are fabricated by disproportionation reaction between amorphous molytungsten oxysulphide (MoWO<sub>x</sub>S<sub>y</sub>) and iron pthalocyanine (Fe(H<sub>2</sub>Pc)). The study elucidates the role of how multiple heterointerfaces play vital role in enhancing hydrogen and oxygen evolution reaction (HER/OER) kinetics. Structural and microscopic analyses reveal Fe/FeS<sub>x</sub> nanoparticles embedded in N-doped carbon, which envelops on 2D MoWO<sub>x</sub>S<sub>y</sub> sheets. Strong interfacial coupling between Fe/FeS<sub>x</sub>/NC and MoWO<sub>x</sub>S<sub>y</sub> modulates the electronic structure, increases conductivity, and enriches surface active sites, yielding synergistic catalytic effects. The hybrid exhibits outstanding bifunctional activity in alkaline KOH, with η<sub>10</sub> values of 22 mV<sub>RHE</sub> (HER) and 110 mV<sub>RHE</sub> (OER). As a bifunctional catalyst pair (Fe/FeS<sub>x</sub>/NC/MoWO<sub>x</sub>S<sub>y</sub>‖Fe/FeS<sub>x</sub>/NC/MoWO<sub>x</sub>S<sub>y</sub>), it drives overall water splitting at 1.42 V and 10 mA cm<sup>−2</sup>, maintaining stability over 100 h. Post-catalysis analysis identifies the reconstructed FeOOH@Fe/FeS<sub>x</sub>/NC/MoWO<sub>x</sub>S<sub>y</sub> as the probable active phase, where electronic interactions and efficient charge transfer underpin surface reaction kinetics leading to exceptional performance. This multicomponent design offers a promising strategy for high-efficiency water splitting and broader electrochemical energy applications.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"665 ","pages":"Article 239029"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145938656","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239165
Rasoul Salehi, Shengbing Jiang, Xinyu Du, Brian Koch, Jing Gao, Raneen Taha
Loss of active material (LAM) is an important failure mechanism in lithium-ion batteries that accelerates performance degradation and initiates unsafe side reactions. A detailed experimental analysis is presented in this paper on the impact of different types of anode LAM on cell and electrode performance followed by two detection algorithms. The anode LAM is emulated by introducing loss of active materials during the cell manufacturing and before the cell assembly. Three major groups of results are provided including a) cell level performance metrics measured by the cell capacity b) teardown analysis after cycling cells that visualizes how electrode surfaces degrade due to the injected LAM types c) electrode level potentials measured by a reference electrode. The electrode potentials demonstrate how anode and cathode behaviors change and evolve due to anode LAM. Finally, detection algorithms are presented with experimental validation results to detect LAM at the electrode level (when it is observable) and predict nonuniformity of lithium distribution in electrodes due to the active material deficiency.
{"title":"Insights into anode loss of active material mechanisms and detection algorithms","authors":"Rasoul Salehi, Shengbing Jiang, Xinyu Du, Brian Koch, Jing Gao, Raneen Taha","doi":"10.1016/j.jpowsour.2025.239165","DOIUrl":"10.1016/j.jpowsour.2025.239165","url":null,"abstract":"<div><div>Loss of active material (LAM) is an important failure mechanism in lithium-ion batteries that accelerates performance degradation and initiates unsafe side reactions. A detailed experimental analysis is presented in this paper on the impact of different types of anode LAM on cell and electrode performance followed by two detection algorithms. The anode LAM is emulated by introducing loss of active materials during the cell manufacturing and before the cell assembly. Three major groups of results are provided including a) cell level performance metrics measured by the cell capacity b) teardown analysis after cycling cells that visualizes how electrode surfaces degrade due to the injected LAM types c) electrode level potentials measured by a reference electrode. The electrode potentials demonstrate how anode and cathode behaviors change and evolve due to anode LAM. Finally, detection algorithms are presented with experimental validation results to detect LAM at the electrode level (when it is observable) and predict nonuniformity of lithium distribution in electrodes due to the active material deficiency.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239165"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-02DOI: 10.1016/j.jpowsour.2025.239241
Ashok Kushwaha , Sayantika Bhakta , Mukhtiar Ahmed , Andrei Filippov , Rong An , Patrik Johansson , Faiz Ullah Shah
Flame-resistant and fluorine-free electrolytes based on (combining) the salts lithium saccharinate (LiSac) and lithium bis(oxalato)borate (LiBOB) in a single solvent triethyl phosphate (TEP) solvent and vinylene carbonate (VC) additive are presented and evaluated for lithium metal battery application. The dual salt electrolyte, 1.5 M LiSac + 0.2 M LiBOB in TEP w. 2 % VC, clearly outperforms the single salt ones in terms of electrochemical performance, especially vs. LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes, properties that originate in a Li+ cation first solvation shell mainly composed of Sac and BOB anions, promoting formation of a mechanically stable, inorganic-rich cathode electrolyte interphase layer, which by X-ray photoelectron spectroscopy was revealed to comprise Li3N, BxOy and SO32− species. Overall, this also results in stable cycling, and a capacity retention of 86 % in both Li||LiFePO4 and Li||NMC811 cells after 500 cycles at 1C rate – hence offering an intrinsically safer electrolyte that also enables the use of both lithium metal anodes and medium-to-high-voltage cathodes.
提出了一种以糖酸锂（LiSac）和硼酸锂（LiBOB）为单溶剂（磷酸三乙酯（TEP）溶剂和碳酸乙烯酯（VC）添加剂）为单溶剂（组合）的阻燃无氟电解质，并对其在锂金属电池中的应用进行了评价。在TEP w. 2% VC中，1.5 M LiSac + 0.2 M LiBOB双盐电解质的电化学性能明显优于单盐电解质，特别是与LiNi0.8Mn0.1Co0.1O2 （NMC811）阴极相比，其性能源于主要由Sac和BOB阴离子组成的Li+阳离子第一溶剂化壳，促进形成机械稳定，富含无机的阴极电解质间相层，x射线光电子能谱显示该层由Li3N组成。BxOy和SO32−种。总的来说，这也导致了稳定的循环，在1C倍率下500次循环后，Li||LiFePO4和Li||NMC811电池的容量保持率为86%，因此提供了一种本质上更安全的电解质，也可以使用锂金属阳极和中高压阴极。
{"title":"Dual fluorine-free salt electrolytes for medium-to-high voltage lithium metal batteries","authors":"Ashok Kushwaha , Sayantika Bhakta , Mukhtiar Ahmed , Andrei Filippov , Rong An , Patrik Johansson , Faiz Ullah Shah","doi":"10.1016/j.jpowsour.2025.239241","DOIUrl":"10.1016/j.jpowsour.2025.239241","url":null,"abstract":"<div><div>Flame-resistant and fluorine-free electrolytes based on (combining) the salts lithium saccharinate (LiSac) and lithium bis(oxalato)borate (LiBOB) in a single solvent triethyl phosphate (TEP) solvent and vinylene carbonate (VC) additive are presented and evaluated for lithium metal battery application. The dual salt electrolyte, 1.5 M LiSac + 0.2 M LiBOB in TEP w. 2 % VC, clearly outperforms the single salt ones in terms of electrochemical performance, especially <em>vs.</em> LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) cathodes, properties that originate in a Li<sup>+</sup> cation first solvation shell mainly composed of Sac and BOB anions, promoting formation of a mechanically stable, inorganic-rich cathode electrolyte interphase layer, which by X-ray photoelectron spectroscopy was revealed to comprise Li<sub>3</sub>N, B<sub>x</sub>O<sub>y</sub> and SO<sub>3</sub><sup>2−</sup> species. Overall, this also results in stable cycling, and a capacity retention of 86 % in both Li||LiFePO<sub>4</sub> and Li||NMC811 cells after 500 cycles at 1C rate – hence offering an intrinsically safer electrolyte that also enables the use of both lithium metal anodes and medium-to-high-voltage cathodes.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"667 ","pages":"Article 239241"},"PeriodicalIF":7.9,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145882702","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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