Pub Date : 2025-10-30DOI: 10.1007/s11581-025-06804-1
Shuaijing Ji, Xiuye Wang, Fengqian Wang, Wuxin Sha, Danpeng Cheng, Zhenxing Wang, Zhongwen Ouyang, Shun Tang, Yuancheng Cao
With the rapid increase in retired lithium iron phosphate (LiFePO4, LFP) batteries and the rising demand for carbon neutrality, efficient and sustainable recycling of spent LFP cathodes has become a pressing research priority. This review systematically compares three representative recycling approaches—pyrometallurgical, hydrometallurgical, and direct regeneration—highlighting their respective mechanisms, advantages, and limitations. Pyrometallurgy, while industrially mature, suffers from high energy consumption and elemental loss. Hydrometallurgy enables high recovery yields but generates significant chemical waste. In contrast, direct regeneration preserves the cathode structure and offers notable advantages in energy efficiency, environmental impact, and cost-effectiveness. Life cycle assessment results based on the EverBatt model show that direct regeneration significantly reduces greenhouse gas emissions and process costs compared to other methods. Finally, the review outlines current challenges and research directions toward scalable, green, and economically viable LFP recycling technologies.
{"title":"Recycling methods for spent lithium iron phosphate cathode materials","authors":"Shuaijing Ji, Xiuye Wang, Fengqian Wang, Wuxin Sha, Danpeng Cheng, Zhenxing Wang, Zhongwen Ouyang, Shun Tang, Yuancheng Cao","doi":"10.1007/s11581-025-06804-1","DOIUrl":"10.1007/s11581-025-06804-1","url":null,"abstract":"<div><p>With the rapid increase in retired lithium iron phosphate (LiFePO<sub>4</sub>, LFP) batteries and the rising demand for carbon neutrality, efficient and sustainable recycling of spent LFP cathodes has become a pressing research priority. This review systematically compares three representative recycling approaches—pyrometallurgical, hydrometallurgical, and direct regeneration—highlighting their respective mechanisms, advantages, and limitations. Pyrometallurgy, while industrially mature, suffers from high energy consumption and elemental loss. Hydrometallurgy enables high recovery yields but generates significant chemical waste. In contrast, direct regeneration preserves the cathode structure and offers notable advantages in energy efficiency, environmental impact, and cost-effectiveness. Life cycle assessment results based on the EverBatt model show that direct regeneration significantly reduces greenhouse gas emissions and process costs compared to other methods. Finally, the review outlines current challenges and research directions toward scalable, green, and economically viable LFP recycling technologies.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 12","pages":"12511 - 12521"},"PeriodicalIF":2.6,"publicationDate":"2025-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145802513","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zinc-ion batteries offer environmentally friendly and reliable energy storage alternatives. They may also lower the cost of producing next-generation battery technologies. Transition metal oxide-based materials have large theoretical capacities, are abundant in nature, are inexpensive, and have effective redox reactions, making them promising cathode materials for zinc-ion batteries. V₂O₅ and V₂O₅-based materials are being studied for cathode materials in zinc ion batteries due to their high theoretical capacitance and efficient electrochemical properties. Researchers are exploring doping, composite synthesis, and electrolyte optimization for improving the electrochemical potential of zinc-ion batteries. The functioning of zinc-ion batteries, the possibilities of V₂O₅-based materials as cathodes, certain V₂O₅-based hybrid materials, substantial and continuing studies, and future challenges have been adequately covered in this article.
{"title":"An updated review on the potential of V₂O₅-based materials for zinc-ion batteries","authors":"Naveen Chandra Joshi, Hemant Kumar Joshi, Prateek Gururani","doi":"10.1007/s11581-025-06792-2","DOIUrl":"10.1007/s11581-025-06792-2","url":null,"abstract":"<div><p>Zinc-ion batteries offer environmentally friendly and reliable energy storage alternatives. They may also lower the cost of producing next-generation battery technologies. Transition metal oxide-based materials have large theoretical capacities, are abundant in nature, are inexpensive, and have effective redox reactions, making them promising cathode materials for zinc-ion batteries. V₂O₅ and V₂O₅-based materials are being studied for cathode materials in zinc ion batteries due to their high theoretical capacitance and efficient electrochemical properties. Researchers are exploring doping, composite synthesis, and electrolyte optimization for improving the electrochemical potential of zinc-ion batteries. The functioning of zinc-ion batteries, the possibilities of V₂O₅-based materials as cathodes, certain V₂O₅-based hybrid materials, substantial and continuing studies, and future challenges have been adequately covered in this article.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 12","pages":"12575 - 12586"},"PeriodicalIF":2.6,"publicationDate":"2025-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145802516","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-10-28DOI: 10.1007/s11581-025-06800-5
Chenxu Fang, Yiwen Dai, Chengming Hao, Handong Li
Recycling spent lithium iron phosphate (LiFePO4) batteries, ubiquitous in electric vehicles and energy storage, is crucial for sustainability. However, the prevalent carbon coating, essential for battery performance, presents significant challenges during recycling processes. The melt growth of LiFePO4 crystals from a carbon-decorated LiFePO4 amorphous powder precursor via the Bridgman method was studied. The electrochemical performance of the regenerated LiFePO4 materials is significantly degraded which should be attributed to the presence of Fe-related defects. The results suggest decarbonization as a necessary step for achieving phase-pure crystalline LiFePO4 from wasted LiFePO4 batteries.
{"title":"Melt growth of LiFePO4 crystals from Carbon-decorated LiFePO4 powder for recycling purpose","authors":"Chenxu Fang, Yiwen Dai, Chengming Hao, Handong Li","doi":"10.1007/s11581-025-06800-5","DOIUrl":"10.1007/s11581-025-06800-5","url":null,"abstract":"<div><p>Recycling spent lithium iron phosphate (LiFePO<sub>4</sub>) batteries, ubiquitous in electric vehicles and energy storage, is crucial for sustainability. However, the prevalent carbon coating, essential for battery performance, presents significant challenges during recycling processes. The melt growth of LiFePO<sub>4</sub> crystals from a carbon-decorated LiFePO<sub>4</sub> amorphous powder precursor via the Bridgman method was studied. The electrochemical performance of the regenerated LiFePO<sub>4</sub> materials is significantly degraded which should be attributed to the presence of Fe-related defects. The results suggest decarbonization as a necessary step for achieving phase-pure crystalline LiFePO<sub>4</sub> from wasted LiFePO<sub>4</sub> batteries.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 12","pages":"12611 - 12618"},"PeriodicalIF":2.6,"publicationDate":"2025-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145802579","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
MnPO4∙H2O is an ideal precursor for the preparation of LiMnPO4. However, the instability of Mn3+ in an aqueous solution necessitates the implementation of the existing preparation methods, which are carried out in ethanol and produce toxic gases such as NO and NO2. In this work, a radical-oxidation coupled phosphate stabilization strategy is proposed for synthesizing MnPO4∙H2O in an aqueous solution. The strategy involves the initial oxidation of Mn2+ to Mn3+ by sulfate radicals, which are produced through the thermal activation of Na2S2O8. Subsequently, Mn3+ is stabilized by H3PO4, leading to the formation of MnPO4∙H2O. By implementing this strategy, the mesoporous MnPO4∙H2O precursor can be readily obtained through a reaction at 90 °C for 5 h. Subsequently, the prepared LiMnPO4/C inherits the mesoporous structure of the MnPO4∙H2O precursor, exhibiting excellent electrochemical performance. Specifically, the mesoporous LiMnPO4/C delivers an initial capacity of 115.8 mAh g−1 with a capacity retention of 83.1% after 100 cycles at 10 C. The enhanced performance is mainly attributed to the mesoporous structure, which facilitates electrolyte penetration, reduces interfacial charge transfer impedance, and accelerates Li+ diffusion. The environmentally benign and scalable strategy presented here opens a new approach to the synthesis of high-performance LiMnPO4/C.
MnPO4∙H2O是制备LiMnPO4的理想前驱体。然而,由于Mn3+在水溶液中的不稳定性,需要采用现有的制备方法,这些方法是在乙醇中进行的,并且会产生NO和NO2等有毒气体。在这项工作中,提出了一种在水溶液中合成MnPO4∙H2O的自由基氧化耦合磷酸盐稳定策略。该策略涉及通过Na2S2O8热活化产生的硫酸盐自由基将Mn2+初始氧化为Mn3+。随后,Mn3+被H3PO4稳定,形成MnPO4∙H2O。采用该策略,在90℃条件下反应5 h即可得到介孔MnPO4∙H2O前驱体,制备的LiMnPO4/C继承了MnPO4∙H2O前驱体的介孔结构,表现出优异的电化学性能。具体来说,在10℃下循环100次后,LiMnPO4/C的初始容量为115.8 mAh g−1,容量保持率为83.1%。性能的增强主要归功于介孔结构,有利于电解质的渗透,降低了界面电荷转移阻抗,加速了Li+的扩散。本文提出的环境友好且可扩展的策略为合成高性能LiMnPO4/C开辟了一条新途径。
{"title":"Radical-oxidation coupled phosphate stabilization strategy: an aqueous and scalable route to mesoporous MnPO4∙H2O precursor for high-performance LiMnPO4 cathodes","authors":"Kanghui Cai, Binsheng Hong, Xueling Hu, Zhenkun Li, Jing Su, Xiaoyan Lv, Yanxuan Wen","doi":"10.1007/s11581-025-06803-2","DOIUrl":"10.1007/s11581-025-06803-2","url":null,"abstract":"<div><p>MnPO<sub>4</sub>∙H<sub>2</sub>O is an ideal precursor for the preparation of LiMnPO<sub>4</sub>. However, the instability of Mn<sup>3+</sup> in an aqueous solution necessitates the implementation of the existing preparation methods, which are carried out in ethanol and produce toxic gases such as NO and NO<sub>2</sub>. In this work, a radical-oxidation coupled phosphate stabilization strategy is proposed for synthesizing MnPO<sub>4</sub>∙H<sub>2</sub>O in an aqueous solution. The strategy involves the initial oxidation of Mn<sup>2+</sup> to Mn<sup>3+</sup> by sulfate radicals, which are produced through the thermal activation of Na<sub>2</sub>S<sub>2</sub>O<sub>8</sub>. Subsequently, Mn<sup>3+</sup> is stabilized by H<sub>3</sub>PO<sub>4</sub>, leading to the formation of MnPO<sub>4</sub>∙H<sub>2</sub>O. By implementing this strategy, the mesoporous MnPO<sub>4</sub>∙H<sub>2</sub>O precursor can be readily obtained through a reaction at 90 °C for 5 h. Subsequently, the prepared LiMnPO<sub>4</sub>/C inherits the mesoporous structure of the MnPO<sub>4</sub>∙H<sub>2</sub>O precursor, exhibiting excellent electrochemical performance. Specifically, the mesoporous LiMnPO<sub>4</sub>/C delivers an initial capacity of 115.8 mAh g<sup>−1</sup> with a capacity retention of 83.1% after 100 cycles at 10 C. The enhanced performance is mainly attributed to the mesoporous structure, which facilitates electrolyte penetration, reduces interfacial charge transfer impedance, and accelerates Li<sup>+</sup> diffusion. The environmentally benign and scalable strategy presented here opens a new approach to the synthesis of high-performance LiMnPO<sub>4</sub>/C.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 12","pages":"12653 - 12667"},"PeriodicalIF":2.6,"publicationDate":"2025-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145802409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-10-28DOI: 10.1007/s11581-025-06790-4
Manish Kumar Singla, Mohammad Aljaidi, Jyoti Gupta, Pradeep Jangir, Arpita, Ramesh Kumar, Reena Jangid, EI-Sayed M. EI-Kenawy, Amal H. Alharbi
Proper modeling, control and optimization of Proton Exchange Membrane Fuel Cells (PEMFCs) depends on the correct extraction of parameters. This is a nonlinear identification problem that is complex and involves the estimation of seven interdependent parameters using empirical voltage-current data. The paper suggests a new metaheuristic approach, the Starfish Optimization Algorithm (SFOA) based on the regenerative and coordinated feeding behaviors of starfish. The algorithm is strictly tested by reducing the sum-square error (SSE) of the model predictions and experimental data of twelve different PEMFC stacks, whose power was 12 W to 6 kW. The effectiveness of SFOA is proved by the comparative analysis with nine state-of-the-art algorithms (GJO, COA, RSA, PO, SO, YDSE, AOA, RIME, DE). The results consistently indicate that SFOA has the most accuracy with the smallest mean error of 0.0255 being the lowest, the smallest SSE as well as being very robust with a small standard deviation of 1.69E-05. Moreover, SFOA is computationally highly efficient and can reach the optimal solution in 0.38 s, much faster than any of the benchmarked algorithms. The reliability and accuracy of SFOA are validated statistically through convergence curves, box plot analysis and Friedman ranking tests. This study has made SFOA a powerful new instrument in improving the accuracy of fuel cell models, which is essential to create real-time control schemes, system design optimization, and critical monitoring processes.
质子交换膜燃料电池(pemfc)的正确建模、控制和优化取决于参数的正确提取。这是一个复杂的非线性辨识问题,涉及使用经验电压-电流数据估计七个相互依赖的参数。本文提出了一种基于海星再生和协调摄食行为的元启发式算法——海星优化算法。通过降低12个功率为12 W ~ 6 kW的PEMFC堆的模型预测和实验数据的和平方误差(SSE),对该算法进行了严格的测试。通过与GJO、COA、RSA、PO、SO、YDSE、AOA、RIME、DE等9种最先进算法的对比分析,证明了SFOA算法的有效性。结果一致表明,SFOA的准确率最高,平均误差最小,为0.0255;SSE最小,标准差较小,为1.69E-05,具有很强的鲁棒性。此外,SFOA具有很高的计算效率,可以在0.38 s内达到最优解,比任何基准算法都快得多。通过收敛曲线、箱形图分析和Friedman排序检验,对SFOA的可靠性和准确性进行了统计验证。该研究使SFOA成为提高燃料电池模型准确性的强大新工具,这对于创建实时控制方案,系统设计优化和关键监控过程至关重要。
{"title":"Enhanced mathematical modeling of PEM fuel cells using the starfish optimization algorithm","authors":"Manish Kumar Singla, Mohammad Aljaidi, Jyoti Gupta, Pradeep Jangir, Arpita, Ramesh Kumar, Reena Jangid, EI-Sayed M. EI-Kenawy, Amal H. Alharbi","doi":"10.1007/s11581-025-06790-4","DOIUrl":"10.1007/s11581-025-06790-4","url":null,"abstract":"<div><p>Proper modeling, control and optimization of Proton Exchange Membrane Fuel Cells (PEMFCs) depends on the correct extraction of parameters. This is a nonlinear identification problem that is complex and involves the estimation of seven interdependent parameters using empirical voltage-current data. The paper suggests a new metaheuristic approach, the Starfish Optimization Algorithm (SFOA) based on the regenerative and coordinated feeding behaviors of starfish. The algorithm is strictly tested by reducing the sum-square error (SSE) of the model predictions and experimental data of twelve different PEMFC stacks, whose power was 12 W to 6 kW. The effectiveness of SFOA is proved by the comparative analysis with nine state-of-the-art algorithms (GJO, COA, RSA, PO, SO, YDSE, AOA, RIME, DE). The results consistently indicate that SFOA has the most accuracy with the smallest mean error of 0.0255 being the lowest, the smallest SSE as well as being very robust with a small standard deviation of 1.69E-05. Moreover, SFOA is computationally highly efficient and can reach the optimal solution in 0.38 s, much faster than any of the benchmarked algorithms. The reliability and accuracy of SFOA are validated statistically through convergence curves, box plot analysis and Friedman ranking tests. This study has made SFOA a powerful new instrument in improving the accuracy of fuel cell models, which is essential to create real-time control schemes, system design optimization, and critical monitoring processes.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 12","pages":"13229 - 13268"},"PeriodicalIF":2.6,"publicationDate":"2025-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145802435","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}