Chunrong Ma , Hui Li , Zhaoying Li , Guangshuai Han , Xiao Tang , Ji Qian , Renjie Chen
{"title":"Atomic Co-driven catalysis in MoS₂ for accelerated charge transfer and stable interfacial chemistry in sodium-ion batteries","authors":"Chunrong Ma , Hui Li , Zhaoying Li , Guangshuai Han , Xiao Tang , Ji Qian , Renjie Chen","doi":"10.1016/j.ensm.2025.104611","DOIUrl":"10.1016/j.ensm.2025.104611","url":null,"abstract":"<div><div>Maximizing initial Coulombic efficiency (ICE) is crucial for the practical deployment of sodium-ion batteries (SIBs), yet remains challenging due to uncontrolled interfacial side reactions and sluggish charge transport. Here, we present an in situ electrochemical catalysis strategy enabling atomic-level Co doping in MoS₂, which simultaneously regulates its electronic configuration and interfacial chemistry. The engineered Co–S–C catalytic sites accelerate the cleavage of P–F and C–O bonds from NaPF₆ and diglyme, respectively, inducing rapid formation of an ultrathin, highly conductive inorganic-rich SEI layer. This suppresses irreversible parasitic reactions and drastically enhances ICE to an unprecedented 96 %. Additionally, Co incorporation drives a 2H-to-1T phase transition via Mo 4d orbital reorganization, weakening Mo–S bonds and boosting Na⁺/electron transport. The resulting Co–MoS₂/SC anode delivers exceptional electrochemical performance, with 288 mAh g⁻¹ at 20 A g⁻¹ and 96 % capacity retention over 2000 cycles at 10 A g⁻¹. This work offers a powerful strategy for interfacial catalysis-driven phase engineering, unlocking new opportunities for high-efficiency, high-rate sodium storage.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104611"},"PeriodicalIF":20.2,"publicationDate":"2025-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145056862","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}
Yinghui Zhao , Zhiwei Ni , Zhengran Wang , Hui Shao , Yihao Li , Yifan Li , Fangbing Dong , Shenglin Xiong , Jinkui Feng
{"title":"From liquid to solid: Advanced electrolyte design strategies for next-generation high-performance anode-free lithium/sodium/potassium batteries","authors":"Yinghui Zhao , Zhiwei Ni , Zhengran Wang , Hui Shao , Yihao Li , Yifan Li , Fangbing Dong , Shenglin Xiong , Jinkui Feng","doi":"10.1016/j.ensm.2025.104608","DOIUrl":"10.1016/j.ensm.2025.104608","url":null,"abstract":"<div><div>Anode-free lithium/sodium/potassium batteries have emerged as promising candidates for next-generation energy storage due to their simplified structure, high energy density, low cost, and enhanced safety. However, their practical application is still hindered by finite metal sources and the high reactivity of metals. Recent progress in electrolyte design has demonstrated great potential to overcome these limitations. In liquid electrolytes, tailored electrolyte formulations have significantly improved the cycling performance of anode-free batteries (AFBs). Furthermore, advancements in solid-state electrolytes have further enhanced the stability of AFBs by suppressing side reactions at the solid-solid interface. This review summarizes advanced electrolyte design strategies for high-performance anode-free lithium/sodium/potassium batteries, spanning from liquid to solid-state systems. The underlying mechanisms are thoroughly analyzed, with an emphasis on electrolyte formulation and interface engineering strategies. A systematic comparison between liquid and solid electrolytes is also presented. Future directions are outlined to guide the practical application of AFBs. This review may further inspire the development of other anode-free systems, such as Al-, Mg-, and Zn-based batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104608"},"PeriodicalIF":20.2,"publicationDate":"2025-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145056866","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}
Hao Tong , Jianwei Li , Mingyan Chuai , Yilun Sun , Zimin Yang , Yifan Su , Xinbin Nie , Siting Deng , Mingqiang Wu , Guoliang Chai
{"title":"Bifunctional electrolyte additive sustains high efficient zinc-iodine batteries via respirable-interphase formation and polyiodide ion suppression","authors":"Hao Tong , Jianwei Li , Mingyan Chuai , Yilun Sun , Zimin Yang , Yifan Su , Xinbin Nie , Siting Deng , Mingqiang Wu , Guoliang Chai","doi":"10.1016/j.ensm.2025.104609","DOIUrl":"10.1016/j.ensm.2025.104609","url":null,"abstract":"<div><div>Aqueous zinc–iodine batteries hold immense potential for grid-scale storage owing to their inherent safety, cost-effectiveness, and eco-friendliness. However, their commercialization is hindered by limited cycle life caused by irreversible Zn plating/stripping and I<sub>2</sub>/I<sup>−</sup> redox reaction. Herein, we propose 1-(2-hydroxyethyl)-1-methylguanidine dihydrogen phosphate (HMDP) as an effective bifunctional additive that not only stabilizes Zn anode by forming a respirable-interphase but also suppresses the generation of polyiodide ion at the cathode by separating I<sub>2</sub> and I<sup>−</sup>. The Zn//Cu cells with HMDP achieve a Coulombic efficiency of 99.63 % over 650 cycles (2 mA cm<sup>−2</sup>, 1 mAh cm<sup>−2</sup>) and retain 85.83 % initial efficiency after 7-day calendar aging. Surprisingly, the Zn//Zn symmetric cells with HMDP deliver an ultra-long cycle-life of 5150 h (0.5 mA cm<sup>−2</sup>, 0.5 mAh cm<sup>−2</sup>) thanks to the formation of respirable-interphase. Meanwhile, the Zn//I<sub>2</sub> full cells retain 81.04 % capacity at 2 A <em>g</em><sup>−1</sup> after >3000 cycles due to the suppression of polyiodide ion. This work establishes strategies of I<sub>2</sub>–I<sup>−</sup> separator and respirable-interphase to design advanced zinc-iodine batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104609"},"PeriodicalIF":20.2,"publicationDate":"2025-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043677","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}
{"title":"Fluorinated electrolytes for lithium–sulfur and beyond-lithium metal–sulfur batteries","authors":"Avinash Raulo , Saheed Lateef , Hunter McRay , Kaushek Rahul Ilancheran , Fabio Albano , Golareh Jalilvand","doi":"10.1016/j.ensm.2025.104600","DOIUrl":"10.1016/j.ensm.2025.104600","url":null,"abstract":"<div><div>Metal–sulfur batteries, particularly lithium–sulfur (Li–S) systems, have attracted significant attention due to their high theoretical energy densities, low cost, and sustainability benefits arising from sulfur’s abundance and non-toxicity. Despite extensive research, their practical deployment remains limited by persistent challenges such as polysulfide shuttling and metal anode degradation, which collectively lead to poor coulombic efficiency and limited cycle life. These issues are further intensified in emerging systems employing sodium, potassium, magnesium, calcium, and siliconbased anodes. Fluorinated electrolytes have emerged as a promising approach to address these limitations. Fluorination enhances oxidative stability, suppresses polysulfide dissolution, promotes stable solid–electrolyte interphase (SEI) formation, and improves safety. Although widely studied in lithium-ion and lithium-metal batteries, fluorinated electrolytes remain underexplored in metal–sulfur systems, despite growing evidence of their potential to mitigate key degradation pathways. This review provides a mechanism-focused analysis of fluorinated electrolytes for metal–sulfur batteries, with a particular emphasis on Li–S systems. It begins by assessing the limitations of conventional electrolytes and examines how fluorinated solvents, salts, and additives influence polysulfide solubility, electrode interfacial stability, and overall electrochemical performance. The discussion then extends to emerging non-lithium metal–sulfur systems, where fluorinated electrolytes can improve stability. Environmental and economic considerations are addressed, followed by an outlook on key parameters and target goals for realizing practical metal–sulfur batteries by leveraging fluorinated electrolytes. By connecting electrolyte design to specific failure mechanisms, this review establishes a framework for targeted materials development and outlines future directions for advancing high-performance, practical metal–sulfur batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104600"},"PeriodicalIF":20.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043674","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}
Mengyao Shi, Tianjiang Sun, Weijia Zhang, Min Cheng, Qiong Sun, Zhanliang Tao
{"title":"Modulating Zn2+ bulk-interfacial kinetics via ionic eutectic network for high reversible Zn anode operated at 100 °C","authors":"Mengyao Shi, Tianjiang Sun, Weijia Zhang, Min Cheng, Qiong Sun, Zhanliang Tao","doi":"10.1016/j.ensm.2025.104606","DOIUrl":"10.1016/j.ensm.2025.104606","url":null,"abstract":"<div><div>Deep eutectic electrolytes (DEEs) typically suffer from high viscosity and low ionic conductivity (<10 mS cm<sup>-1</sup>), leading to severe battery polarization and limited cycle life, which significantly hinders their practical application in aqueous zinc-ion batteries (AZIBs). To overcome this bottleneck, this study developed an innovative \"water-in-salt\" ionic eutectic electrolyte (IEE). This design increases free ion concentration and reduces system viscosity (10.9 mPa s), significantly enhancing bulk ion transport and achieving an ionic conductivity (41.7 mS cm<sup>-1</sup>) unattainable by conventional DEEs. Simultaneously, the low water activity of the IEE synergizes with its unique anion-cluster solvation structure to strongly suppress side reactions, enabling a Zn||PANI cell to achieve 100 % Coulombic efficiency even at 100 °C. Furthermore, replacing the conventional solid electrolyte interphase protection mechanism with electric double layer regulation and reducing the Zn<sup>2+</sup> de-solvation energy barrier not only enabled dendrite-free Zn deposition but also substantially optimized interfacial kinetics. This resulted in stable cycling for 1000 h in a Zn||Zn half-cell under ultra-low polarization. Leveraging these combined advantages, the IEE-based full cell demonstrates exceptional rate capability and long-term cycling stability. This work provides a novel approach to overcoming the design limitations of DEEs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104606"},"PeriodicalIF":20.2,"publicationDate":"2025-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043725","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}
Arul Saravanan Raaju Sundhar , Dohyun Im , Miyoung Kim , Sang-Jae Kim
{"title":"A heuristic strategy for converting Ni-rich hydroxide precursors into sustainable fast-charging cathodes for next-generation lithium-ion batteries","authors":"Arul Saravanan Raaju Sundhar , Dohyun Im , Miyoung Kim , Sang-Jae Kim","doi":"10.1016/j.ensm.2025.104605","DOIUrl":"10.1016/j.ensm.2025.104605","url":null,"abstract":"<div><div>Ni-rich R-3m polycrystalline layered oxides (LiNi<sub>1-x</sub>M<sub>x</sub>O<sub>2;</sub> M = Mn, Co, Ti; 0 ≤ x ≤ 0.2) are among the most promising Li-ion battery cathodes, combining high energy density with cost-effective production. However, their fast-charging capability is hampered at high voltages due to sluggish Li<sup>+</sup> transport and structural degradation. Herein, we report a heuristic, solid-state co-doping strategy employing boron (B<sup>3+</sup>) and titanium (Ti<sup>4+</sup>) to simultaneously engineer the bulk structure and surface chemistry of Ni-rich cathodes. The co-doped materials demonstrate exceptional stability in lithium-graphite full cells, retaining >86% capacity after 500 cycles at a 4C charge rate, even across elevated cutoff voltages (4.3-4.5 V) and high Ni contents (80–100 mol%). Multiscale characterization reveals three critical morphological features: (i) radially arranged nanosheet-like grains that alleviate anisotropic lattice strain; (ii) an in-situ formed Li-B-O surface layer that mitigates electrolyte decomposition at high voltage; and (iii) a defect-mediated cation-mixed interphase that pillars the layered structure under extreme delithiation. Extension of this strategy to ultra-high Ni systems, including LiNi<sub>0.9</sub>Co<sub>0.1</sub>O<sub>2</sub> and LiNiO<sub>2</sub>, yielded comparable enhancements. Mechanistic insights further enabled the rational selection of earth-abundant pillaring elements, enhancing the scalability and sustainability of the proposed doping system. This work underscores the potential of defect phase engineering and microstructural control without reliance on group V/VI dopants for the development of robust, fast-charging Ni-rich cathodes.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104605"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043676","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}
Jiameng Yu , Tianyi Gao , Ruixin Hao , Yuanyuan Cui , Luyao Wang , Yihang Yang , Yuyao Zhang , Wenbo Zhai , Fenwei Cui , Ziran Xu , Xiangchen Hu , Ning Xue , Yi Yu , Fei Song , Hui Zhang , Zhi Liu , Wei Liu
{"title":"Evaluating the feasibility and air stability of high-entropy doping in garnet electrolytes","authors":"Jiameng Yu , Tianyi Gao , Ruixin Hao , Yuanyuan Cui , Luyao Wang , Yihang Yang , Yuyao Zhang , Wenbo Zhai , Fenwei Cui , Ziran Xu , Xiangchen Hu , Ning Xue , Yi Yu , Fei Song , Hui Zhang , Zhi Liu , Wei Liu","doi":"10.1016/j.ensm.2025.104603","DOIUrl":"10.1016/j.ensm.2025.104603","url":null,"abstract":"<div><div>High-entropy electrolytes have attracted extensive attention for their potential to overcome the limits of traditional materials. However, confirming the accurate synthesis of a single-phase high-entropy electrolyte remains a challenge. Herein, we develop a quinary garnet electrolyte of cubic phase with high resistance to air corrosion. By employing a straightforward method that analyzes the variations of diffraction peak intensity, we can evaluate the feasibility of high-entropy doping, the degree of cubic phase, and the extent of H<sup>+</sup>/Li<sup>+</sup> exchange. Meanwhile, ambient pressure X-ray photoelectron spectroscopy is utilized to investigate the degradation of garnet electrolyte by H<sub>2</sub>O, with the failure mechanism further elucidated by nuclear magnetic resonance analysis. On this basis, the high-entropy garnet electrolyte demonstrated increased cubic phase content and better air stability, compared with traditional counterpart. Consequently, a higher current critical density is achieved, facilitating the integration of commercial cathodes with high area capacities into the quasi-solid-state batteries. Our findings provide an effective method for synthesizing and evaluating high entropy electrolytes.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104603"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026043","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}
Wenli Xin , Yaheng Geng , Hui Zhang , Lei Zhang , Yu Han , Zichao Yan , Fangyi Cheng , Zhiqiang Zhu
{"title":"Stabilizing electrolytic Zn||MnO2 batteries under lean electrolyte conditions via synergistic anode and electrolyte engineering","authors":"Wenli Xin , Yaheng Geng , Hui Zhang , Lei Zhang , Yu Han , Zichao Yan , Fangyi Cheng , Zhiqiang Zhu","doi":"10.1016/j.ensm.2025.104601","DOIUrl":"10.1016/j.ensm.2025.104601","url":null,"abstract":"<div><div>Electrolytic Zn||MnO<sub>2</sub> batteries utilizing acidic electrolytes are promising for large-scale energy storage owing to their high energy/power densities. However, they encounter challenges such as hydrogen evolution corrosion on Zn anodes and excessive electrolyte-to-cathode capacity ratios (E/C ratio > 0.05 mL mAh<sup>−1</sup>). Here, we introduce a synergistic approach combining a zeolitic imidazolate frameworks (ZIFs)-coated Zn anode and acetic acid (HOAc)-modified electrolyte to stabilize electrolytic Zn||MnO<sub>2</sub> batteries under lean electrolyte conditions. Specifically, HOAc substitutes partial imidazole ligands within the ZIFs coating, forming a dense, acid-resistant amorphous ZIFs (aZIFs) layer that effectively mitigates Zn anode corrosion. Simultaneously, the HOAc-modified electrolyte acts as a proton reservoir for the MnO<sub>2</sub> cathode, enabling reversible MnO<sub>2</sub>/Mn<sup>2+</sup> redox chemistry. This dual modification allows the ZIFs@Zn||MnO<sub>2</sub> coin cell to retain 80.4 % capacity after 1000 cycles at 5.0 A g<sup>–1</sup> and the pouch cell to achieve an output voltage exceeding 1.5 V at 0.5 A g<sup>−1</sup> with a E/C ratio of 0.018 mL mAh<sup>−1</sup>. Our work provides a feasible approach to develop practical electrolytic Zn||MnO<sub>2</sub> batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104601"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145025765","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}
Shusheng Tao , Xiquan Ke , Dongxiao Li , Zheng Luo , Huimin Lian , Shengrui Gao , Shaozhen Huang , Wentao Deng , Hongshuai Hou , Guipeng Yu , Guoqiang Zou , Xiaobo Ji
{"title":"Covalent organic framework-engineered separators enabling selective sodium ion transport for sodium metal anode storage","authors":"Shusheng Tao , Xiquan Ke , Dongxiao Li , Zheng Luo , Huimin Lian , Shengrui Gao , Shaozhen Huang , Wentao Deng , Hongshuai Hou , Guipeng Yu , Guoqiang Zou , Xiaobo Ji","doi":"10.1016/j.ensm.2025.104599","DOIUrl":"10.1016/j.ensm.2025.104599","url":null,"abstract":"<div><div>Sodium metal energy storage devices with high power/energy densities offer scalability without requiring complex presodiation. However, the sluggish migration of Na<sup>+</sup> and the uncontrollable growth of sodium dendrites have hindered their commercial adoption. Herein, we construct functionalized separators using quinoline carboxylic acid covalent organic frameworks (QL-COFs) to achieve selective Na<sup>+</sup> transport and uniform deposition. Molecular dynamics simulations and theoretical calculations confirm that QL-COFs with uniform pore structures restrict PF<sub>6</sub><sup>-</sup> ion migration while providing highly selective transport channels for Na<sup>+</sup>, doubling the Na<sup>+</sup> transference number to 0.89 (<em>vs.</em> 0.43 for polyethylene separators), surpassing values reported for state-of-the-art functionalized separators and solid-state electrolytes. <em>In-situ</em> XRD directly visualizes the reversible Na<sup>+</sup> deposition/stripping behavior on Cu foil, corroborated by the stable Coulombic efficiency of Na-Cu cells over 800 h, jointly demonstrating that the uniform pore architecture of QL-COFs guides homogeneous Na<sup>+</sup> electrodeposition. The modified separator enables symmetric cells to achieve 1300-h cycling stability and empowers a sodium metal capacitor to deliver 203.33 Wh kg<sup>-1</sup> at an ultrahigh power density of 24,000 W kg<sup>-1</sup>, surpassing the performance metrics of previously reported devices. This work first elucidates the mechanism of QL-COF-modified separators in accelerating Na<sup>+</sup> migration, expands the application boundaries of COF materials, and proposes a new paradigm for constructing scalable sodium metal capacitors.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104599"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026045","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}
Huiting Xu , Shiyuan Fan , Huibin Liu , Peng Guo , Nanxing Ji , Chunli Li , Honghai Wang , Wenchao Peng , Xiaobin Fan , Jiapeng Liu
{"title":"The modulation of adsorption balance effect for promoting selenium cathode redox reaction kinetics in aqueous zinc-selenium battery","authors":"Huiting Xu , Shiyuan Fan , Huibin Liu , Peng Guo , Nanxing Ji , Chunli Li , Honghai Wang , Wenchao Peng , Xiaobin Fan , Jiapeng Liu","doi":"10.1016/j.ensm.2025.104604","DOIUrl":"10.1016/j.ensm.2025.104604","url":null,"abstract":"<div><div>Aqueous zinc-selenium (Zn-Se) battery shows promising applications because of its inherent safety and high theoretical capacity. However, the slow redox reaction kinetics of Se cathode limit its development. The strategy of designing functional catalytic host materials with suitable adsorption ability is essential to promote Se redox reaction kinetics. We construct a catalytic host material consisting of axially oxygen-coordinated Cu single atoms and neighboring Cu atomic clusters (Cu-N<sub>4</sub>O/Cu<sub>ACs</sub>) to probe its modulation mechanism of suitable adsorption ability on Se redox reaction. The Cu-N<sub>4</sub>O/Cu<sub>ACs</sub> enable the aqueous Zn-Se battery to exhibit a specific capacity of 643 mAh g<sup>–1</sup> at 0.2 A g<sup>–1</sup> and fast Se redox reaction kinetics. Experimental characterization and density functional theory confirm the “adsorption balance effect” of Cu-N<sub>4</sub>O/Cu<sub>ACs</sub>. The neighboring Cu<sub>ACs</sub> can enhance the adsorption ability for Se species. The axially coordinated O atoms can promote electron delocalization and downshift d-band center, weakening the excess adsorption ability brought by Cu<sub>ACs</sub> and lowering the energy barrier of redox reaction. The adsorption balance effect between clusters of Cu<sub>ACs</sub> and axial O atom causes Cu-N<sub>4</sub>O/Cu<sub>ACs</sub> to exhibit excellent catalytic effect. This work gives new insights for the optimization of the catalytic behavior between the adsorption ability of SACs and redox reaction kinetics in aqueous Zn-Se battery.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104604"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043675","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}