Shuo Li , Jing Liu , Shengchang Li , Teng Fu , Yi Zong , Han Ding , Yecheng Zou , Yongming Zhang , Xuejing Cui , Xin Zhou , Luhua Jiang
{"title":"Volcano-type relationship between interfacial Pt–S bonds and oxygen reduction activity in sulfur-doped carbon-supported Pt3Co catalysts","authors":"Shuo Li , Jing Liu , Shengchang Li , Teng Fu , Yi Zong , Han Ding , Yecheng Zou , Yongming Zhang , Xuejing Cui , Xin Zhou , Luhua Jiang","doi":"10.1016/j.jechem.2025.08.014","DOIUrl":"10.1016/j.jechem.2025.08.014","url":null,"abstract":"<div><div>Pt-based nanoalloys, as the state-of-the-art oxygen reduction reaction (ORR) catalysts, still face significant challenges in terms of activity and long-term stability in proton-exchange membrane fuel cells (PEMFCs). Here, we report a dual-sulfur regulation strategy to achieve gradient regulation of the interfacial platinum–sulfur (Pt–S) bonds in sulfur-doped carbon-supported Pt<sub>3</sub>Co catalysts, revealing a volcano-type relationship between the ORR activity and the amount of interfacial Pt–S covalent bonds. The optimized Pt<sub>3</sub>Co-SH/S-C catalyst exhibits superior ORR performance with a half-wave potential (<em>E</em><sub>1/2</sub>) of 0.923 V, which is 23 mV higher than that of the commercial Pt/C, and remarkable stability, with only a 3 mV decrease in <em>E</em><sub>1/2</sub> after 80,000 cycles of accelerated durability testing (ADT). Furthermore, the Pt<sub>3</sub>Co-SH/S-C cathode-based membrane electrode assembly (MEA) could deliver a peak power density of 1.15 W cm<sup>−2</sup> in H<sub>2</sub>-O<sub>2</sub> mode at 90 °C with exceptional durability. Theoretical calculations reveal that interfacial Pt–S covalent bonds cause a downward shift of the Pt <em>d</em>-band center, as compared to that in Pt<sub>3</sub>Co, alleviating the excessive adsorption of *OH and thus enhancing ORR kinetics. This work establishes a new paradigm for tailoring metal-support interactions via interfacial bonding engineering, providing a rational strategy for designing durable high-performance ORR catalysts for PEMFCs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 728-736"},"PeriodicalIF":14.9,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144988736","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chaoyang Shi , Guangtao Luo , Danyang Wei, Haodong Jin, Linxiang Zhou, Haoqi Li, Mingli Xu
{"title":"Synergistic charge-regulation of Fe-N4O1 sites coupled with MnO2 clusters via dual-ligand effect for enhanced oxygen reduction reaction","authors":"Chaoyang Shi , Guangtao Luo , Danyang Wei, Haodong Jin, Linxiang Zhou, Haoqi Li, Mingli Xu","doi":"10.1016/j.jechem.2025.07.086","DOIUrl":"10.1016/j.jechem.2025.07.086","url":null,"abstract":"<div><div>It is challenging to rationally construct synergistic charge-regulation of active sites and a lower energy barrier of the determining step for efficient oxygen reduction reaction (ORR). In this work, a novel catalyst (MnO<sub>2</sub>)<sub>cluster</sub>/Fe,Mn-N-C with Fe-N<sub>4</sub>O<sub>1</sub> site coupled by MnO<sub>2</sub> sub-nanometer clusters was successfully synthesized, which is attributed to the dicyanodiamine-glycine (DCD-Gly) dual-ligand effect. Specifically, the higher electrophilic index and the preferential coordination with Fe of N in DCD, and the chelating coordination of Gly with Mn. Experimental and theoretical calculation results indicate that preferential coordination of Fe with N atoms in DCD generates Fe-N<sub>4</sub>O<sub>1</sub> sites with axial oxygen coordination, while the coordination of Mn with Gly generates a large number of MnO<sub>2</sub> sub-nanometer clusters. DFT calculations showed that axial oxygen altered the reaction-determining step of ORR at the FeN<sub>4</sub>O<sub>1</sub> site. Meanwhile, the MnO<sub>2</sub> sub-nanoclusters further lowered the adsorption energy barriers of the reaction intermediates. This synergistic charge-regulation improved the ORR performance of (MnO<sub>2</sub>)<sub>cluster</sub>/Fe,Mn-N-C (<em>E</em><sub>1/2</sub> = 0.90 V). Meanwhile, (MnO<sub>2</sub>)<sub>cluster</sub>/Fe,Mn-N-C catalyst also exhibits a discharge power density of 201 mW cm<sup>−2</sup> in Zn-air batteries, which was much higher than the commercial Pt/C+RuO<sub>2</sub>. The strategy of ligand effect-driven construction provided a new idea for the electronic structure modulation of a monatomic catalyst.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 701-710"},"PeriodicalIF":14.9,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144932850","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhenkang Lin, Jing Yang, Chunyu Li, Shilong Wang, Wenzhong Cong, Teng Li, Lin Qi, Kening Sun, Cheng Fan
{"title":"Fuzzy physics-informed thermal diagnostics via non-invasive frequency-domain signature distillation in high-energy-density batteries","authors":"Zhenkang Lin, Jing Yang, Chunyu Li, Shilong Wang, Wenzhong Cong, Teng Li, Lin Qi, Kening Sun, Cheng Fan","doi":"10.1016/j.jechem.2025.08.018","DOIUrl":"10.1016/j.jechem.2025.08.018","url":null,"abstract":"<div><div>Accurate real-time monitoring of internal temperature in lithium-ion batteries remains critical for preventing thermal runaway, as conventional approaches sacrifice either computational efficiency or cross-scenario robustness. We present a generalized fuzzy physics-informed framework that distills thermally sensitive electrochemical processes while circumventing redundant physical constraints, thereby establishing an explicit mechanism-constrained mapping between frequency-domain signals and internal temperature. This framework facilitates online thermal estimation, with dynamic validations in LiFePO<sub>4</sub>/graphite 18650-type cells confirming real-time capability with near-instantaneous acquisition (∼6 s per measurement), exceptional accuracy (±0.5 °C) within the operational temperature range (30–50 °C), and operational resilience across 20 %–80 % state-of-charge. The framework maintains predictive fidelity (±1.0 °C at 30 °C and ±4.0 °C at 60 °C, 95 % prediction intervals) across 80 %–100 % state-of-health while demonstrating adaptability to cathode materials and structural architectures. This strategy resolves the competing imperatives of physical interpretability, computational efficiency, and cross-scenario generalizability, offering a universal paradigm for embedded thermal management in safety-critical applications.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 856-866"},"PeriodicalIF":14.9,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144996154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shaomin Kang , Jingjing Liu , Xu Wu , Ming Gao , MengMeng Lou , Chen Wang , Mingxing Shi , Guolin Tong
{"title":"CNTs-enabled enhanced capacitive deionization desalination: From material innovation to electrode optimization and device integration","authors":"Shaomin Kang , Jingjing Liu , Xu Wu , Ming Gao , MengMeng Lou , Chen Wang , Mingxing Shi , Guolin Tong","doi":"10.1016/j.jechem.2025.08.017","DOIUrl":"10.1016/j.jechem.2025.08.017","url":null,"abstract":"<div><div>Capacitive deionization (CDI), as an emerging desalination technique, has been intensively explored because of its energy-saving, cost-effectiveness and sustainability. Despite the promise, CDI systems still encounter various challenges involving active sites, mass transfer and stability that severely limit their further application. So far, there is still much-limited review across material, electrodes and devices to cope with the above challenges. Notably, carbon nanotubes (CNTs), have garnered significant attention owing to their exceptional conductivity, high specific surface area (<em>S</em><sub>BET</sub>), unique skeleton role and superior mechanical strength. More importantly, CNTs serve multifunctional roles in CDI systems, including active materials, conductive agents, binders, and even current collectors, while also making for the thick electrode framework construction. Specifically, this review first discusses current challenges in CDI system design. Subsequently, it systemic highlights how CNTs address these issues through material innovation, electrode optimization and device integration. Eventually, a conceptual model for CNT composite self-supporting CDI systems is further proposed, aiming to exploit advanced CDI desalination systems. Overall, this review underscores the pivotal role of CNTs in overcoming technical bottlenecks and driving the practical application of CDI for sustainable water treatment.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 617-639"},"PeriodicalIF":14.9,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144917588","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jingwei Mao , Yi Wei , Ying Ding , Yufeng Liu , Junhui Wang , Kaifeng Wu , Zijian Deng , Ze Yu , Yefu Liu , Huolin Huang
{"title":"Quantum well engineering in quasi-2D perovskites unlocks efficiency-stability synergy for photovoltaics","authors":"Jingwei Mao , Yi Wei , Ying Ding , Yufeng Liu , Junhui Wang , Kaifeng Wu , Zijian Deng , Ze Yu , Yefu Liu , Huolin Huang","doi":"10.1016/j.jechem.2025.07.085","DOIUrl":"10.1016/j.jechem.2025.07.085","url":null,"abstract":"<div><div>Quasi-2D perovskites offer enhanced stability for photovoltaic applications but suffer from compromised charge transport due to uncontrolled phase separation and nonideal quantum well (QW) distribution. Contrary to the prevailing belief that maximizing 3D-like phases optimizes performance, we demonstrate that strategic narrowing QW distribution into high<em>-n</em> phases while avoiding undesirable graded configurations (common in quasi-2D systems) unlocks unprecedented efficiency-stability synergy. Using 1,4-cyclohexanedimethanamine (CDMA) as a crystallization-directing spacer, we realize three advances. (a) High<em>-n</em> phases with minimized <em>n</em>-value dispersion establish a uniform energy landscape, significantly reducing interphase charge transfer barriers and suppressing voltage losses. (b) Lattice matching between adjacent high<em>-n</em> phases substantially alleviates microstrain accumulation, thereby mitigating defect generation and non-radiative recombination. (c) Strategic predominance of robust high<em>-n</em> phases achieves dual optimization: it excludes hygroscopic 3D-like phases and eliminates mobility-limiting low<em>-n</em> phases, thereby ensuring efficient charge dynamics while fortifying the perovskite’s intrinsic phase stability. The synergy of these advances enables the CDMA PSCs to achieve a champion efficiency of 19.02 %, making them among the highest-efficiency quasi-2D DJ PSCs. The unencapsulated device demonstrated remarkable stability, maintaining 92 % of its initial PCE after 5000 h in air. This work redefines phase engineering priorities, demonstrating that manipulating QW distribution in quasi-2D perovskites has the potential to address the efficiency-stability trade-off.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 1042-1051"},"PeriodicalIF":14.9,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145117921","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Minghui Zhang , Derong Wang , Sibo Wang , Shiyue Gao , Ye Chen , Qi Yang , Xiaoqi Sun , Yanfeng Dong , Jieshan Qiu
{"title":"Hydrated eutectic electrolyte enabling stable low-temperature zinc metal batteries with a tuned inner Helmholtz plane and a solid electrolyte interface","authors":"Minghui Zhang , Derong Wang , Sibo Wang , Shiyue Gao , Ye Chen , Qi Yang , Xiaoqi Sun , Yanfeng Dong , Jieshan Qiu","doi":"10.1016/j.jechem.2025.08.015","DOIUrl":"10.1016/j.jechem.2025.08.015","url":null,"abstract":"<div><div>Aqueous zinc metal batteries (ZMBs) are promising for grid-scale energy storage, but their practical application is hindered by limited cycling life and inferior low-temperature performance, primarily due to Zn dendrite growth and parasitic reactions at the electrolyte-electrode interface. To address these challenges, we develop a new and cheap hydrated eutectic electrolyte (HEE) composed of ZnCl<sub>2</sub>, choline chloride (ChCl), and H<sub>2</sub>O, which can fundamentally tune desirable interface chemistries for dendrite-free and low-temperature ZMBs. The optimized HEE with a solvation structure of ZnCl<sub>3</sub>(ChCl)(H<sub>2</sub>O)<sub>2</sub> shows a high conductivity of 15.98 mS cm<sup>−1</sup> and excellent freeze resistance below −40 °C. It has been found that hydrogen bonding between ChCl and H<sub>2</sub>O effectively reduces water activity, while preferential adsorption of ChCl molecules at the inner Helmholtz plane promotes the formation of a protective solid electrolyte interphase (SEI) on Zn metal anodes, which greatly suppresses the dendrites and side reactions. Therefore, the HEE endows the as-fabricated Zn//Zn symmetric cells and Zn//polyaniline full batteries with superior electrochemical performance at −40 °C, such as a long cycling life of 870 h at 1 mA cm<sup>−2</sup> and 1 mAh cm<sup>−2</sup> and a high capacity of 75 mAh g<sup>−1</sup> at 0.3 A g<sup>−1</sup>. The HEE reported here may pave a new way to construct high-performance ZMBs for specific low-temperature application scenarios.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 711-718"},"PeriodicalIF":14.9,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144932852","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qiang Xu , Hao Liu , Shuliang Lv , Yilong Han , Xue Ji , Chang Ma , Jian Li , Zhijia Zhang , Yanmei Jin , Qinxin Xie , Haihui Liu
{"title":"Dynamic anchoring and catalysis via Co-Nb dual sites in lithium-sulfur batteries","authors":"Qiang Xu , Hao Liu , Shuliang Lv , Yilong Han , Xue Ji , Chang Ma , Jian Li , Zhijia Zhang , Yanmei Jin , Qinxin Xie , Haihui Liu","doi":"10.1016/j.jechem.2025.08.016","DOIUrl":"10.1016/j.jechem.2025.08.016","url":null,"abstract":"<div><div>Single-atom catalysts are promising for lithium-sulfur (Li-S) batteries due to their high degree of atomic utilization and strong interactions with lithium polysulfides (LiPSs). However, the limited number of active sites and their rapid saturation hinder the continuous adsorption and efficient conversion of LiPSs. Herein, we report a bimetallic catalyst comprising single cobalt atoms (Co<sub>SA</sub>) and niobium atomic clusters (Nb<sub>AC</sub>) anchored on graphene-like nanosheets (Co<sub>SA</sub>Nb<sub>AC</sub>/NC), which are synthesized via a cohesive energy-driven selective metal aggregation strategy. This dual-site configuration forms an electronically asymmetric interface, where Nb<sub>AC</sub> anchors LiPSs via Coulombic and Lewis acid-base interactions, while Co<sub>SA</sub> enables S–S bond polarization and cleavage through d-p orbital coupling. The interfacial charge redistribution and orbital coupling between Co and Nb facilitate electron transfer between catalytic sites. Therefore, the S/Co<sub>SA</sub>Nb<sub>AC</sub>/NC cathode maintains a high areal capacity of 6.12 mAh cm<sup>−2</sup> after 60 cycles under a high sulfur loading of 6.2 mg cm<sup>−2</sup>. This work demonstrates a rational design strategy for high-performance Li-S cathodes via synergistic bimetallic catalysis.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 719-727"},"PeriodicalIF":14.9,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144925558","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dan Li , Xing Zhi , Lei Zhang , Fangxi Xie , Mingmei Wu
{"title":"Direct regeneration of spent lithium-ion batteries: Advancing from powder to cell","authors":"Dan Li , Xing Zhi , Lei Zhang , Fangxi Xie , Mingmei Wu","doi":"10.1016/j.jechem.2025.08.013","DOIUrl":"10.1016/j.jechem.2025.08.013","url":null,"abstract":"<div><div>The rapid advancement of electric vehicles (EVs) has led to a substantial increase in spent lithium-ion batteries (LIBs), necessitating effective recycling pathways to recover the reusable battery components. Traditional recycling methods, such as pyrometallurgy and hydrometallurgy, represent battery-component destructive pathways with high energy consumption and substantial waste emissions, leading to considerable environmental issues. In contrast, direct regeneration technologies preserve the integrity of battery components on certain levels, offering a more sustainable and energy-efficient approach. However, these technologies are hindered by complex pre-treatment procedures, underscoring the need for a simplified route to effectively restore battery performance. This Review categorizes recent advancements in direct regeneration strategies at three levels—powder, electrode, and cell—focusing on their fundamental mechanisms, technological pathways, and socioeconomic sustainability. Among these, cell-level direct regeneration technologies exhibit the highest economic benefits and the lowest waste emissions, positioning them as a promising solution for large-scale battery recovery. By highlighting the potential of cell-level direct regeneration, this review aims to drive further research and development toward scalable and simplified strategies for the efficient reuse of spent LIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 767-789"},"PeriodicalIF":14.9,"publicationDate":"2025-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987944","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lingfeng Huang , Xueying Wang , Sheng Huang , Shuanjin Wang , Dongmei Han , Hui Guo , Min Xiao , Yuezhong Meng
{"title":"Flame-retardant polycarbonate-based single-ion conducting polymer electrolyte for high-safety lithium batteries","authors":"Lingfeng Huang , Xueying Wang , Sheng Huang , Shuanjin Wang , Dongmei Han , Hui Guo , Min Xiao , Yuezhong Meng","doi":"10.1016/j.jechem.2025.07.083","DOIUrl":"10.1016/j.jechem.2025.07.083","url":null,"abstract":"<div><div>The low lithium transference number of conventional dual-ion polymer electrolytes will lead to concentration polarization and lithium dendrite growth, thereby affecting the safety and cycling performance of lithium batteries. Herein, we report a flame-retardant polycarbonate-based single-ion conducting polymer electrolyte (PAGEC-B/PFN). Due to the immobilization of anions within the polycarbonate cross-linking network, PAGEC-B/PFN exhibits a high lithium transference number (0.86), which is beneficial for alleviating concentration polarization and suppressing the growth of lithium dendrite. With the assistance of the TEP flame retardant and FEC, as well as LiNO<sub>3</sub> additives, PAGEC-B/PFN exhibits excellent flame retardancy, high ionic conductivity, and outstanding interfacial compatibility with the lithium metal anode. As expected, PAGEC-B/PFN achieves a high critical current density of up to 2.0 mA cm<sup>−2</sup> and stable cycling of Li||Li cell for over 2200 h. Meanwhile, LFP||PAGEC-B/PFN||Li cell delivers a specific capacity of 147.8 mA h g<sup>−1</sup> at 0.5 C and exhibits excellent cycling performance over 600 cycles. This work provides a strategy for designing solid-state lithium batteries with high safety and high performance.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 659-669"},"PeriodicalIF":14.9,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144925557","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xuwei Chen , Chenxin Ye , Zeqi Huang , Hong Gao , Hao Yang , Weihua Cai , Ying Ma , Jianshan Ye
{"title":"Low-valent multielement synergy stabilizing bimetallic Prussian blue cathode for ultra-fast and highly stable sodium-ion batteries","authors":"Xuwei Chen , Chenxin Ye , Zeqi Huang , Hong Gao , Hao Yang , Weihua Cai , Ying Ma , Jianshan Ye","doi":"10.1016/j.jechem.2025.08.010","DOIUrl":"10.1016/j.jechem.2025.08.010","url":null,"abstract":"<div><div>The rational design of Prussian blue analogue (PBA) cathodes with bimetallic reaction centers represents a cornerstone strategy for high-energy sodium-ion batteries (SIBs), yet their electrochemical performance is inherently limited by structural instability and sluggish kinetics. Herein, we propose a multielement co-doping strategy to achieve a holistic optimization of bimetallic Na<sub>2</sub>Mn<sub>0.5</sub>Fe<sub>0.5</sub>[Fe(CN)<sub>6</sub>] (MFHCF) by substituting N-coordinated sites with Mg<sup>II</sup>, Co<sup>II</sup>, and Ni<sup>II</sup>. Specifically, the MgCoNi-MFHCF delivers a superior rate capability (145.9 and 85.3 mAh g<sup>−1</sup> under 0.1 and 30 C, respectively), outstanding cycling stability (83.1% capacity retention over 1000 cycles), and high energy density (304.5 Wh kg<sup>−1</sup> for the full cell). In situ/ex situ techniques and theoretical calculations reveal that the MgCoNi-MFHCF experiences a reversible tri-phase transition with mitigated volume contraction/expansion, which originates from the alleviation of the Jahn-Teller distortion. It is considered that the cation doping enhances redox reaction reversibility through stabilized transition-metal coordination environments while reducing bandgaps and lowering ionic diffusion energy barrier, leading to accelerated electrochemical kinetics. This study establishes a generalizable multielement engineering strategy for high-performance cathode materials with bimetallic reaction centers for SIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 640-649"},"PeriodicalIF":14.9,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144932308","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}