Pub Date : 2026-10-13DOI: 10.1016/j.ensm.2026.105597
Zehao Xu, Minghao Huang, Kai Zhang, Xuan Ye, Ming Li, Huguo Zhou, Weilong Kong, Rulong Zhou, Xianfu Sun, Qian Hou, Hongfa Xiang
High-voltage Li metal batteries offer appealing high energy density but suffer from simultaneous interfacial instability at both cathode and anode, where cathode particle degradation, uncontrolled interphase growth, and uneven Li deposition remain major impediments to long-term cycling and calendar life. Here, we introduce a novel concept of counter-directed migratory ionic additives, whose anions and cations move towards the cathode and anode respectively to reconfigure the Helmholtz layer under the intrinsic electric field of the battery. We employ theoretical simulations and in-situ Raman spectra for verification of the field responsiveness and migration behavior of anions/cations. The NO3- anions enriched at the high-voltage cathode, are found to promote inorganic-rich cathode‑electrolyte interphase (CEI) and inhibit electrolyte decomposition. The Pyr13+ cations enriched at the Li anode exert electrostatic shielding effects and electrostatically attract TFSI⁻ anions to facilitate more LiF, while NO3- decomposes into N-containing inorganics, thereby improving the solid electrolyte interphase (SEI) and homogenizing Li deposition. Together, these synergistic dual-interphase improvements translate into enhanced coulombic efficiency, superior rate capability, and significantly improved long-term cycling stability of 4.6 V Li||NCM811 cells. Counter-directed migratory ionic additives provide a versatile and broadly applicable platform to tackle the challenge of synergistic dual-interphase regulation in energy-dense Li metal batteries.
高压锂金属电池具有吸引人的高能量密度，但阴极和阳极同时存在界面不稳定，阴极颗粒降解，界面生长不受控制，锂沉积不均匀仍然是长期循环和日历寿命的主要障碍。在此，我们引入了一种新的反定向迁移离子添加剂的概念，其阴离子和阳离子分别向阴极和阳极移动，以在电池的本征电场下重新配置亥姆霍兹层。我们采用理论模拟和原位拉曼光谱来验证阴离子/阳离子的场响应性和迁移行为。在高压阴极富集NO3-阴离子，促进富无机阴极-电解质界面（CEI），抑制电解质分解。在锂阳极富集的Pyr13+阳离子发挥静电屏蔽作用，静电吸引TFSI毒血症，促进更多的LiF，而NO3-分解为含n无机物，从而改善固体电解质界面（SEI），使锂沉积均质化。总之，这些协同双间期改进转化为提高库仑效率，优越的速率能力，并显着提高4.6 V Li||NCM811电池的长期循环稳定性。反定向迁移离子添加剂为解决高能量锂金属电池中协同双界面调节的挑战提供了一个通用的、广泛适用的平台。
{"title":"Cation-Anion Counter-Directed Migration Enabled Synergistic Dual-Interphase Engineering for High-Voltage Li Metal Batteries","authors":"Zehao Xu, Minghao Huang, Kai Zhang, Xuan Ye, Ming Li, Huguo Zhou, Weilong Kong, Rulong Zhou, Xianfu Sun, Qian Hou, Hongfa Xiang","doi":"10.1016/j.ensm.2026.105597","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105597","url":null,"abstract":"High-voltage Li metal batteries offer appealing high energy density but suffer from simultaneous interfacial instability at both cathode and anode, where cathode particle degradation, uncontrolled interphase growth, and uneven Li deposition remain major impediments to long-term cycling and calendar life. Here, we introduce a novel concept of counter-directed migratory ionic additives, whose anions and cations move towards the cathode and anode respectively to reconfigure the Helmholtz layer under the intrinsic electric field of the battery. We employ theoretical simulations and in-situ Raman spectra for verification of the field responsiveness and migration behavior of anions/cations. The NO<ce:inf loc=\"post\">3</ce:inf><ce:sup loc=\"post\">-</ce:sup> anions enriched at the high-voltage cathode, are found to promote inorganic-rich cathode‑electrolyte interphase (CEI) and inhibit electrolyte decomposition. The Pyr<ce:inf loc=\"post\">13</ce:inf><ce:sup loc=\"post\">+</ce:sup> cations enriched at the Li anode exert electrostatic shielding effects and electrostatically attract TFSI⁻ anions to facilitate more LiF, while NO<ce:inf loc=\"post\">3</ce:inf><ce:sup loc=\"post\">-</ce:sup> decomposes into N-containing inorganics, thereby improving the solid electrolyte interphase (SEI) and homogenizing Li deposition. Together, these synergistic dual-interphase improvements translate into enhanced coulombic efficiency, superior rate capability, and significantly improved long-term cycling stability of 4.6 V Li||NCM811 cells. Counter-directed migratory ionic additives provide a versatile and broadly applicable platform to tackle the challenge of synergistic dual-interphase regulation in energy-dense Li metal batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"13 1","pages":"105597"},"PeriodicalIF":20.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221591","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-13DOI: 10.1016/j.ensm.2026.105594
Jiapeng Zhao, Jiyao Zhou, Wenjin Zhang, Xinyue Deng, Chenghui Sun, Weixiao Ji, He Huang, Siping Pang
Mission-critical one-time-use systems may require sustained electrochemical power supply during normal operation and an on-demand energetic response at the terminal stage. Integrating these temporally separated energy-release modes at the active-material level could improve mass/volume utilization and mission adaptability. Here we report 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) as a supramolecularly stabilized polynitro cathode with dual-mode energy-release potential for high-specific-energy primary lithium batteries. Alternating nitro−amino substitution organizes TATB into a hydrogen-bonded, π−π-stacked network, affording ultralow solubility (0.02 mg mL−1), high thermal stability (Td = 372°C), and mechanical insensitivity (IS > 40 J; FS > 360 N). An FEC-containing electrolyte promotes proton-coupled deep nitro-to-amino conversion while regulating cathode and Li-metal interfaces. Consequently, TATB||Li primary cells deliver 1826 mAh g−1TATB and a TATB-mass-based specific energy of 4382 Wh kg−1TATB, retaining 99% capacity after 3 months. Under lean-Li conditions, a 4.90 mg cm−2 TATB cathode paired with a 50-μm-thick Li anode delivers 8.31 mAh cm−2 and 91% TATB utilization. Separately, the TATB active material resists routine thermal/mechanical stimuli but exhibits energetic response under deliberate booster-assisted initiation. Together, these results establish TATB as an active-material-level proof-of-concept cathode chemistry that couples high-specific-energy battery discharge with triggerable energetic potential.
关键任务的一次性使用系统在正常运行期间可能需要持续的电化学电源，在终端阶段需要按需的能量响应。在活性物质层面整合这些暂时分离的能量释放模式可以提高质量/体积利用率和任务适应性。在这里，我们报道了1,3,5-三氨基-2,4,6-三硝基苯（TATB）作为一种具有双模式能量释放电位的超分子稳定多硝基阴极，用于高比能一次锂电池。交替硝基-氨基取代将TATB组织成一个氢键，π- π堆叠网络，具有超低溶解度（0.02 mg mL - 1），高热稳定性（Td = 372°C）和机械不敏感性（IS > 40 J; FS > 360 N）。含fec的电解质在调节阴极和锂金属界面的同时促进质子耦合的深度氮-氨基转化。因此，TATB||Li原代电池提供1826 mAh g - 1TATB和4382 Wh kg - 1TATB的基于TATB质量的比能，在3个月后保持99%的容量。在贫锂条件下，4.90 mg cm−2的TATB阴极与50 μm厚的锂阳极搭配，可提供8.31 mAh cm−2和91%的TATB利用率。另外，TATB活性材料抵抗常规的热/机械刺激，但在有意的助推器辅助启动下表现出能量反应。总之，这些结果确立了TATB作为一种活性材料级的概念验证阴极化学，将高比能电池放电与可触发的能量势耦合在一起。
{"title":"A supramolecularly stabilized polynitro cathode with dual-mode energy-release potential for high-specific-energy primary lithium batteries","authors":"Jiapeng Zhao, Jiyao Zhou, Wenjin Zhang, Xinyue Deng, Chenghui Sun, Weixiao Ji, He Huang, Siping Pang","doi":"10.1016/j.ensm.2026.105594","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105594","url":null,"abstract":"Mission-critical one-time-use systems may require sustained electrochemical power supply during normal operation and an on-demand energetic response at the terminal stage. Integrating these temporally separated energy-release modes at the active-material level could improve mass/volume utilization and mission adaptability. Here we report 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) as a supramolecularly stabilized polynitro cathode with dual-mode energy-release potential for high-specific-energy primary lithium batteries. Alternating nitro−amino substitution organizes TATB into a hydrogen-bonded, π−π-stacked network, affording ultralow solubility (0.02 mg mL<ce:sup loc=\"post\">−1</ce:sup>), high thermal stability (T<ce:inf loc=\"post\">d</ce:inf> = 372°C), and mechanical insensitivity (IS > 40 J; FS > 360 N). An FEC-containing electrolyte promotes proton-coupled deep nitro-to-amino conversion while regulating cathode and Li-metal interfaces. Consequently, TATB||Li primary cells deliver 1826 mAh g<ce:sup loc=\"post\">−1</ce:sup><ce:inf loc=\"post\">TATB</ce:inf> and a TATB-mass-based specific energy of 4382 Wh kg<ce:sup loc=\"post\">−1</ce:sup><ce:inf loc=\"post\">TATB</ce:inf>, retaining 99% capacity after 3 months. Under lean-Li conditions, a 4.90 mg cm<ce:sup loc=\"post\">−2</ce:sup> TATB cathode paired with a 50-μm-thick Li anode delivers 8.31 mAh cm<ce:sup loc=\"post\">−2</ce:sup> and 91% TATB utilization. Separately, the TATB active material resists routine thermal/mechanical stimuli but exhibits energetic response under deliberate booster-assisted initiation. Together, these results establish TATB as an active-material-level proof-of-concept cathode chemistry that couples high-specific-energy battery discharge with triggerable energetic potential.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"26 1","pages":"105594"},"PeriodicalIF":20.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-12DOI: 10.1016/j.ensm.2026.105596
Saehyun Kim, Yubeen Lee, Sungbin Shin, Seongwon Lee, Dong Gyu Lee, Taehun Chung, Dong-Yeob Han, Sangyeop Lee, Tae Kyung Lee, Soojin Park, Youn Soo Kim
Aqueous zinc metal batteries (AZMBs) require electrolytes that reconcile the opposing roles of water at the cathode and zinc (Zn) metal anode. While sufficient water promotes cathodic reaction kinetics and capacity, excessive water activity triggers parasitic reactions and electrochemically inactive byproducts at the Zn anode. However, conventional homogeneous hydrogel polymer electrolytes (GPEs) fail to satisfy these conflicting interfacial requirements. Here, we report a gradient-structured Janus GPE, achieved by dissolving acrylonitrile, a hydrophobic monomer with very low water miscibility, into an aqueous electrolyte using the Hofmeister effect. Using two substrates with contrasting polar mismatches, this strategy yields a Janus GPE with different hydrophilicities on its two surfaces and a gradient porous structure. When implemented in AZMB pouch cells, the Janus GPE delivers 97.7% capacity retention after 250 cycles in the pristine state and 92.6% retention relative to the pristine initial capacity over 400 cycles under folding. This performance stems from its asymmetric architecture: The more hydrophilic surface facing the cathode provides a water-rich pathway for Zn2+ transport and cathodic kinetics, while the less hydrophilic surface facing the Zn anode lowers water activity, suppresses parasitic reactions, and preserves interfacial integrity during bending. Overall, the Janus GPE establishes a bend-resilient interfacial design for flexible AZMBs, simultaneously advancing cathode utilization and Zn anode stability.
{"title":"Gradient-Structured Janus Hydrogel Electrolyte via One-Pot Aqueous Copolymerization for Flexible Aqueous Zinc Metal Batteries","authors":"Saehyun Kim, Yubeen Lee, Sungbin Shin, Seongwon Lee, Dong Gyu Lee, Taehun Chung, Dong-Yeob Han, Sangyeop Lee, Tae Kyung Lee, Soojin Park, Youn Soo Kim","doi":"10.1016/j.ensm.2026.105596","DOIUrl":"10.1016/j.ensm.2026.105596","url":null,"abstract":"<div><div>Aqueous zinc metal batteries (AZMBs) require electrolytes that reconcile the opposing roles of water at the cathode and zinc (Zn) metal anode. While sufficient water promotes cathodic reaction kinetics and capacity, excessive water activity triggers parasitic reactions and electrochemically inactive byproducts at the Zn anode. However, conventional homogeneous hydrogel polymer electrolytes (GPEs) fail to satisfy these conflicting interfacial requirements. Here, we report a gradient-structured Janus GPE, achieved by dissolving acrylonitrile, a hydrophobic monomer with very low water miscibility, into an aqueous electrolyte using the Hofmeister effect. Using two substrates with contrasting polar mismatches, this strategy yields a Janus GPE with different hydrophilicities on its two surfaces and a gradient porous structure. When implemented in AZMB pouch cells, the Janus GPE delivers 97.7% capacity retention after 250 cycles in the pristine state and 92.6% retention relative to the pristine initial capacity over 400 cycles under folding. This performance stems from its asymmetric architecture: The more hydrophilic surface facing the cathode provides a water-rich pathway for Zn<sup>2+</sup> transport and cathodic kinetics, while the less hydrophilic surface facing the Zn anode lowers water activity, suppresses parasitic reactions, and preserves interfacial integrity during bending. Overall, the Janus GPE establishes a bend-resilient interfacial design for flexible AZMBs, simultaneously advancing cathode utilization and Zn anode stability.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"92 ","pages":"Article 105596"},"PeriodicalIF":19.3,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149214308","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-01Epub Date: 2026-09-23DOI: 10.1016/j.ensm.2026.105553
Feng Guo, Luis D. Couto, Hamid Hamed, Khiem Trad, Dong Zhang, Ru Hong, Guangdi Hu, Mohammadhosein Safari
The flat voltage plateau of lithium iron phosphate (LFP)/graphite cells makes electrochemical-state errors and voltage-measurement abnormalities produce similar innovations, complicating state-of-charge (SOC) estimation. This work proposes an electrochemically constrained residual-bias compensation dual extended Kalman filter (RBC-DEKF) with uncertain-initialization commissioning. A thermal control-oriented parameter-grouped single-particle model (CPG-SPMT) provides paired-electrode dynamics and terminal-voltage prediction, while a separately configurable voltage-discrepancy state accommodates systematic residuals. When the initial SOC is uncertain, residual adaptation is suspended over a verified-healthy startup window. Buffered data support electrochemically constrained trajectory matching, followed by calibrated state replay and residual-channel reactivation. Frozen cross-cycle healthy-residual calibration supports commissioning and remains in the voltage prediction after handover. Evaluation covers 216 additive-bias and 168 multiplicative-gain profiles over 24 A123 temperature–drive-cycle trajectories. Relative to Single-EKF, the original RBC-DEKF reduces mean SOC RMSE from 7.646 to 0.170 percentage points for additive bias and from 22.646 to 0.356 percentage points for gain faults. Separately, 18 nonzero-initial-error profiles on three representative 50%-SOC-anchored segments give a full-record mean SOC RMSE of 1.747 percentage points, including startup, for the commissioned realization, versus 11.192 and 11.400 for the always-on RBC-DEKF and conventional joint EKF. Representative delayed bias, 10-s ramp, and gain tests show that the corrected SOC trajectory remains stable after fault introduction. The central contribution is electrochemically constrained temporal coordination of uncertain-state recovery and subsequent voltage-discrepancy accommodation.
{"title":"When voltage sensors fail: Electrochemically constrained fault-tolerant state estimation for flat-plateau LFP batteries","authors":"Feng Guo, Luis D. Couto, Hamid Hamed, Khiem Trad, Dong Zhang, Ru Hong, Guangdi Hu, Mohammadhosein Safari","doi":"10.1016/j.ensm.2026.105553","DOIUrl":"10.1016/j.ensm.2026.105553","url":null,"abstract":"<div><div>The flat voltage plateau of lithium iron phosphate (LFP)/graphite cells makes electrochemical-state errors and voltage-measurement abnormalities produce similar innovations, complicating state-of-charge (SOC) estimation. This work proposes an electrochemically constrained residual-bias compensation dual extended Kalman filter (RBC-DEKF) with uncertain-initialization commissioning. A thermal control-oriented parameter-grouped single-particle model (CPG-SPMT) provides paired-electrode dynamics and terminal-voltage prediction, while a separately configurable voltage-discrepancy state accommodates systematic residuals. When the initial SOC is uncertain, residual adaptation is suspended over a verified-healthy startup window. Buffered data support electrochemically constrained trajectory matching, followed by calibrated state replay and residual-channel reactivation. Frozen cross-cycle healthy-residual calibration supports commissioning and remains in the voltage prediction after handover. Evaluation covers 216 additive-bias and 168 multiplicative-gain profiles over 24 A123 temperature–drive-cycle trajectories. Relative to Single-EKF, the original RBC-DEKF reduces mean SOC RMSE from 7.646 to 0.170 percentage points for additive bias and from 22.646 to 0.356 percentage points for gain faults. Separately, 18 nonzero-initial-error profiles on three representative 50%-SOC-anchored segments give a full-record mean SOC RMSE of 1.747 percentage points, including startup, for the commissioned realization, versus 11.192 and 11.400 for the always-on RBC-DEKF and conventional joint EKF. Representative delayed bias, 10-s ramp, and gain tests show that the corrected SOC trajectory remains stable after fault introduction. The central contribution is electrochemically constrained temporal coordination of uncertain-state recovery and subsequent voltage-discrepancy accommodation.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105553"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149084626","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
All-solid-state lithium batteries (ASSLBs) are poised to revolutionize energy storage technologies, but the development of solid-state electrolytes (SSEs) that simultaneously offer high ionic conductivity, mechanical deformability, and high-voltage stability remains a formidable challenge. Here, we report a novel heterogeneous oxyhalide SSE, LiAl0.5Ga0.5Cl2.5O0.75(LAGCO), featuring LiCl nanocrystals embedded within an amorphous Li–M–Cl–O (M = Al, Ga) matrix. This unique architecture, synthesized via a facile mechanochemical route, integrates mechanical resilience with continuous, isotropic Li+ transport pathways. LAGCO exhibits a high ionic conductivity of 0.822 mS cm−1 at 25 °C and an intermediate Young's modulus of 2.612 GPa. Its mechanical compliance enables intimate interfacial contact and effectively buffers volumetric strain during cycling. When paired with the high-nickel LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode with a high active-materials loading of 8.91 mg cm−2, the LAGCO-based ASSLBs deliver a discharge capacity of 167.67 mAh g−1. Moreover, the cell exhibits outstanding long-term stability, retaining 86.02% of its capacity after 1000 cycles at 0.5 C (NCM811 loading: 5.35 mg cm−2). Furthermore, the estimated raw material cost (40.80 USD kg−1) of LAGCO is significantly lower than that of many advanced halide electrolytes containing costly elements. This work provides a potentially scalable and cost-effective strategy for designing heterogeneous SSEs with optimized mechanical and electrochemical properties for next-generation energy storage.
全固态锂电池（ASSLBs）有望彻底改变储能技术，但同时提供高离子电导率、机械变形性和高压稳定性的固态电解质（sse）的开发仍然是一个艰巨的挑战。在这里，我们报道了一种新的非均相氧化卤化物SSE， LiAl0.5Ga0.5Cl2.5O0.75(LAGCO)，其特征是LiCl纳米晶体嵌入无定形Li-M-Cl-O （M = Al, Ga）矩阵中。这种独特的结构，通过简单的机械化学路线合成，将机械弹性与连续的、各向同性的Li+运输途径结合起来。LAGCO在25℃时离子电导率为0.822 mS cm−1，中间杨氏模量为2.612 GPa。它的机械顺应性使紧密的界面接触，并有效地缓冲循环过程中的体积应变。当与高镍LiNi0.8Co0.1Mn0.1O2 （NCM811）阴极配对时，具有8.91 mg cm−2的高活性材料负载，lagco基ASSLBs的放电容量为167.67 mAh g−1。此外，该电池表现出出色的长期稳定性，在0.5 C （NCM811负载：5.35 mg cm−2）下循环1000次后，其容量仍保持86.02%。此外，LAGCO的估计原材料成本（40.80美元kg−1）明显低于许多含有昂贵元素的高级卤化物电解质。这项工作为设计具有优化机械和电化学性能的异构sse提供了一种具有潜在可扩展性和成本效益的策略，用于下一代储能。
{"title":"A crystalline-amorphous heterostructured oxyhalide electrolyte for high-performance all-solid-state lithium batteries","authors":"Jinfeng Zeng, Tenglong Lu, Weicai Zhang, Haoliang Huang, Wei Wang, Fei Lin, Jingcheng Lu, Kepan Yan, Chao Ma, Miao Liu, Lifeng Liu","doi":"10.1016/j.ensm.2026.105543","DOIUrl":"10.1016/j.ensm.2026.105543","url":null,"abstract":"<div><div>All-solid-state lithium batteries (ASSLBs) are poised to revolutionize energy storage technologies, but the development of solid-state electrolytes (SSEs) that simultaneously offer high ionic conductivity, mechanical deformability, and high-voltage stability remains a formidable challenge. Here, we report a novel heterogeneous oxyhalide SSE, LiAl<sub>0.5</sub>Ga<sub>0.5</sub>Cl<sub>2.5</sub>O<sub>0.75</sub>(LAGCO), featuring LiCl nanocrystals embedded within an amorphous Li–M–Cl–O (M = Al, Ga) matrix. This unique architecture, synthesized via a facile mechanochemical route, integrates mechanical resilience with continuous, isotropic Li<sup>+</sup> transport pathways. LAGCO exhibits a high ionic conductivity of 0.822 mS cm<sup>−1</sup> at 25 °C and an intermediate Young's modulus of 2.612 GPa. Its mechanical compliance enables intimate interfacial contact and effectively buffers volumetric strain during cycling. When paired with the high-nickel LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cathode with a high active-materials loading of 8.91 mg cm<sup>−2</sup>, the LAGCO-based ASSLBs deliver a discharge capacity of 167.67 mAh g<sup>−1</sup>. Moreover, the cell exhibits outstanding long-term stability, retaining 86.02% of its capacity after 1000 cycles at 0.5 C (NCM811 loading: 5.35 mg cm<sup>−2</sup>). Furthermore, the estimated raw material cost (40.80 USD kg<sup>−1</sup>) of LAGCO is significantly lower than that of many advanced halide electrolytes containing costly elements. This work provides a potentially scalable and cost-effective strategy for designing heterogeneous SSEs with optimized mechanical and electrochemical properties for next-generation energy storage.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105543"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149084583","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Simultaneously enhancing intrinsic catalytic activity and oxygen diffusion is essential for developing high-performance oxygen reduction reaction electrocatalysts, yet achieving both remains challenging. Herein, a cross-scale consolidation strategy is developed to integrate atomically dispersed Co−N4 sites and metallic atomic clusters (Co ACs) within a hollow carbon nanoflower framework (Co-SAAC@HCMF). The Co−N4/Co AC microregions boost intrinsic activity through atomic-scale electronic modulation, while the hollow nanoflower architecture ameliorates oxygen diffusion at the architectural scale. As a result, the optimized Co-SAAC@HCMF catalyst delivers a high half-wave potential of 0.887 V vs. RHE and excellent durability with 97.4% current retention after 50 000 s. When applied in zinc-air batteries, Co-SAAC@HCMF exhibits a high peak power density of 241 mW cm−2 and a specific capacity of 813 mAh gZn−1. Moreover, the Co-SAAC@HCMF + RuO2 air cathode enables stable charge-discharge cycling for over 1000 h. Theoretical calculations and in situ infrared spectroscopy reveal that neighboring Co ACs upshift the Co D-band center of adjacent Co−N4 sites and lower the free-energy barrier for *OOH formation, thereby accelerating ORR kinetics. Complementary transport analyses and finite-element simulations further demonstrate that the hollow nanoflower framework facilitates O2 diffusion and alleviates mass-transfer limitations. This work establishes a cross-scale design principle that integrates single-atom/atomic-cluster electronic interactions with oxygen diffusion-oriented nanostructure engineering for efficient energy-relative electrocatalysis.
{"title":"Cross-scale consolidation of cobalt single atoms toward enhanced oxygen reduction reaction in zinc-air batteries","authors":"Yong Zheng, Jingyu Guan, Weiyi He, Ruifeng Chen, Pengcheng Zhao, Junpeng Ma, Minzhi Ma, Liu Yang, Zhongwei Chen","doi":"10.1016/j.ensm.2026.105546","DOIUrl":"10.1016/j.ensm.2026.105546","url":null,"abstract":"<div><div>Simultaneously enhancing intrinsic catalytic activity and oxygen diffusion is essential for developing high-performance oxygen reduction reaction electrocatalysts, yet achieving both remains challenging. Herein, a cross-scale consolidation strategy is developed to integrate atomically dispersed Co−N<sub>4</sub> sites and metallic atomic clusters (Co ACs) within a hollow carbon nanoflower framework (Co-SAAC@HCMF). The Co−N<sub>4</sub>/Co AC microregions boost intrinsic activity through atomic-scale electronic modulation, while the hollow nanoflower architecture ameliorates oxygen diffusion at the architectural scale. As a result, the optimized Co-SAAC@HCMF catalyst delivers a high half-wave potential of 0.887 V vs. RHE and excellent durability with 97.4% current retention after 50 000 s. When applied in zinc-air batteries, Co-SAAC@HCMF exhibits a high peak power density of 241 mW cm<sup>−2</sup> and a specific capacity of 813 mAh g<sub>Zn</sub><sup>−1</sup>. Moreover, the Co-SAAC@HCMF + RuO<sub>2</sub> air cathode enables stable charge-discharge cycling for over 1000 h. Theoretical calculations and in situ infrared spectroscopy reveal that neighboring Co ACs upshift the Co D-band center of adjacent Co−N<sub>4</sub> sites and lower the free-energy barrier for *OOH formation, thereby accelerating ORR kinetics. Complementary transport analyses and finite-element simulations further demonstrate that the hollow nanoflower framework facilitates O<sub>2</sub> diffusion and alleviates mass-transfer limitations. This work establishes a cross-scale design principle that integrates single-atom/atomic-cluster electronic interactions with oxygen diffusion-oriented nanostructure engineering for efficient energy-relative electrocatalysis.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105546"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149085230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-01Epub Date: 2026-09-11DOI: 10.1016/j.ensm.2026.105525
Taoxiang Qian, Guobin Xu, Shaoyu Hou, Yi Feng, Yaping Wang, Qian Cheng, Guobin Zhang, Shuzhang Niu, Dongju Fu
The rapid growth of electric vehicles has produced huge numbers of spent lithium-ion batteries. As the primary anode material, spent graphite requires urgent recycling to alleviate resource shortage and mitigate environmental risks. This review systematically summarizes recent progress in recycling and high-value utilization of spent graphite anode. We first describe how graphite fails during long time battery operation, typical include particle cracking, solid electrolyte interface damage, lithium dendrites growth, or copper foil corrosion. Next, primary pretreatment processes (safe disassembly, advanced crushing, foam flotation, and chemical leaching) are outlined as essential preliminary engineering steps. Focusing on structural restoration, we critically review direct regeneration technologies, encompassing optimized high-temperature graphitization, chemical remediation, and emerging low-carbon routes such as flash Joule heating, deep eutectic solvent leaching, pre-lithiation, and ultrafast physical heating (microwave). Beyond direct reuse, spent graphite can be upgraded into functional carbon materials for supercapacitors, water cleaning, and catalysts. Finally, we assessed the industrial feasibility of these methods in terms of both production costs and carbon footprint. This work provides comprehensive theoretical guidance for establishing a closed-loop, sustainable graphite recycling system.
{"title":"Spent graphite as a novel resource: Advanced regeneration technologies and life closed-loop sustainability","authors":"Taoxiang Qian, Guobin Xu, Shaoyu Hou, Yi Feng, Yaping Wang, Qian Cheng, Guobin Zhang, Shuzhang Niu, Dongju Fu","doi":"10.1016/j.ensm.2026.105525","DOIUrl":"10.1016/j.ensm.2026.105525","url":null,"abstract":"<div><div>The rapid growth of electric vehicles has produced huge numbers of spent lithium-ion batteries. As the primary anode material, spent graphite requires urgent recycling to alleviate resource shortage and mitigate environmental risks. This review systematically summarizes recent progress in recycling and high-value utilization of spent graphite anode. We first describe how graphite fails during long time battery operation, typical include particle cracking, solid electrolyte interface damage, lithium dendrites growth, or copper foil corrosion. Next, primary pretreatment processes (safe disassembly, advanced crushing, foam flotation, and chemical leaching) are outlined as essential preliminary engineering steps. Focusing on structural restoration, we critically review direct regeneration technologies, encompassing optimized high-temperature graphitization, chemical remediation, and emerging low-carbon routes such as flash Joule heating, deep eutectic solvent leaching, pre-lithiation, and ultrafast physical heating (microwave). Beyond direct reuse, spent graphite can be upgraded into functional carbon materials for supercapacitors, water cleaning, and catalysts. Finally, we assessed the industrial feasibility of these methods in terms of both production costs and carbon footprint. This work provides comprehensive theoretical guidance for establishing a closed-loop, sustainable graphite recycling system.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105525"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148980541","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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