Wenze Cao , Kai Zhang , Jing Wang , Yiwei Li , Yu Chen , Ningning Yang , Zenan Zhao , Yong Zhao , Lian Wang , Pan Chen , Feng Wu , Guoqiang Tan
{"title":"Self-assembled silica-cellulose-ether ternary nanocomposite electrolytes for robust quasi-solid-state lithium metal batteries","authors":"Wenze Cao , Kai Zhang , Jing Wang , Yiwei Li , Yu Chen , Ningning Yang , Zenan Zhao , Yong Zhao , Lian Wang , Pan Chen , Feng Wu , Guoqiang Tan","doi":"10.1016/j.ensm.2025.104067","DOIUrl":"10.1016/j.ensm.2025.104067","url":null,"abstract":"<div><div>Solid electrolytes are a key enabling technology for the safe operation of Li-metal batteries, as they can suppress side reactions and Li dendrites. However, their microstructural heterogeneity and metastability largely restrict their mechanical and electrochemical properties. Herein we report a one-pot sol-gel self-assembly for in-situ constructing silica-cellulose-ether nanocomposite as solid-state electrolytes in Li-metal batteries. The obtained composite features mesoporous silica nanoparticles grafted to functional cellulose nanofibers to form cross-linked frameworks, in which liquid ether electrolytes are in-situ immobilized. By regulating chemical interactions between three nanocomponents for optimizing electrolyte's distribution and ionic conduction, such composite design enables excellent electrochemical properties, showing rapid Li<sup>+</sup> ionic conductivity (6.9 × 10<sup>−4</sup> S cm<sup>−1</sup>) and high electrochemical oxidation tolerance (4.87 V vs Li/Li<sup>+</sup>). Notably, the quasi-solid-state Li-metal batteries using composite membranes exhibit outstanding battery performance: Li//LiFePO<sub>4</sub> cell delivers an ultra-high capacity retention of 97.5 % after 200 cycles, and Li//RuO<sub>2</sub>-O<sub>2</sub> cell exhibits an extended cycle-life over 300 cycles.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104067"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143071682","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}
A. Avila Cardenas , M. Beaudhuin , L.H.B. Nguyen , N. Herlin-Boime , C. Haon , L. Monconduit
{"title":"An optimized electrically conductive Si-Fe matrix to boost the performance of Si electrodes in Li-ion batteries","authors":"A. Avila Cardenas , M. Beaudhuin , L.H.B. Nguyen , N. Herlin-Boime , C. Haon , L. Monconduit","doi":"10.1016/j.ensm.2025.104086","DOIUrl":"10.1016/j.ensm.2025.104086","url":null,"abstract":"<div><div>The development of Si-based anodes has opened the venue to increase the energy density in lithium-ion batteries (LIBs). Nonetheless, the use of Si-based electrodes usually leads to a gradual loss in the cell's electrochemical performance due to the significant volume expansion of silicon in electrode reactions. Combining silicon, a poor electronic conductor, with an electronically conductive Li-inactive phase, is a promising strategy to alleviate the volume expansion of silicon during lithiation and delithiation while providing a robust electronic network. Si-Fe alloys are prospective candidates which could be used to maintain the electronic network in the silicon electrodes. In this study, different Si-Fe alloys are synthesized using ball-milling (BM) and arc melting (AM) techniques, leading to highly different chemical compositions and powder morphologies to better understand the role of iron silicide inactive phases in electrochemical reactions and optimize their performance. The use of AM results in the formation of Si and α-Fe<sub>2</sub>Si<sub>5</sub> conducting matrix in a desired ratio, as expected from the Si-Fe binary phase diagram, while BM generates a mixture of phases, including undesirable products. Thanks to the presence of the inactive iron silicide phase (α-Fe<sub>2</sub>Si<sub>5</sub>), the electrical conductivity of the Si/α-Fe<sub>2</sub>Si<sub>5</sub> composite can be increased up to 10<sup>3</sup> S m<sup>-1</sup>, five orders of magnitude compared to pristine Si. The electrochemical testing results show that the performance of such a composite is strongly influenced by the balance between Si and inactive iron silicide phase, as well as their interparticle contact. Dilatometry tests in full cell configuration also demonstrate the advantage of using α-Fe<sub>2</sub>Si<sub>5</sub> as a matrix to buffer Si volume change, prevent the loss of active material, and maintain a reversible swelling of 24 % throughout cycling up to the 45th cycle. After optimization of electrode and electrolyte formulations, such composites could significantly outperform current Si/C electrodes in terms of volumetric capacity, rate capability and long-term cycling.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104086"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077405","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}
Murong Xi , Zhenjie Liu , Zihan Qi , Yudai Huang , Wei Wang , Juan Ding , Zhouliang Tan , Hongtao Liu
{"title":"Electrolyte for Zn metal battery under extreme temperature operations design by Lewis acid-base chemically mediated polymerization of cyclic ether","authors":"Murong Xi , Zhenjie Liu , Zihan Qi , Yudai Huang , Wei Wang , Juan Ding , Zhouliang Tan , Hongtao Liu","doi":"10.1016/j.ensm.2025.104091","DOIUrl":"10.1016/j.ensm.2025.104091","url":null,"abstract":"<div><div>The high interfacial stability, low metal corrosion, excellent dendrite inhibition, and good ionic conductivity are crucial for the electrolyte employed in extreme temperature operations of zinc ion batteries. However, these properties are seldom achieved simultaneously, particularly at low temperatures. In this study, we report a novel weakly solvated electrolyte that is controllably synthesized through Lewis acid-base chemical mediation of the polymerized 1,3-dioxolane (pDOL) chain length. This results in a wide electrochemical window (2.87 V vs<em>.</em> Zn/Zn<sup>2+</sup>), a rapid Zn<sup>2+</sup> de-solvation process and appropriate ionic conductivity in a wide temperature range (–70 ∼ +25 °C) at low salt concentration. The long-chain pDOL solvent endows the electrolyte with excellent dendrite inhibition (5400 h at 25 °C, 1086 h at –20 °C, and 1024 h at –40 °C), and also addresses the issue of undesired self-corrosion. The differential behavior of the Zn plating/stripping process and interfacial chemistry in this novel electrolyte at various temperatures was analyzed using multiple characterization techniques. Notably, the Zn//PANI full cells exhibit enhanced electrochemical properties, including a high capacity retention ratio and excellent cycling stability under extreme temperature operations from –70 to +25 °C. This work demonstrates a promising approach for the design of electrolytes tailored for extreme operating conditions.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104091"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077406","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}
Lei Wang , Fu-Da Yu , Lan-Fang Que , Xiang-Gong Zhang , Ke-Yu Xie
{"title":"Degradation behavior of Ah-level Li-ion pouch cell during repeated fast charging within a wide temperature region","authors":"Lei Wang , Fu-Da Yu , Lan-Fang Que , Xiang-Gong Zhang , Ke-Yu Xie","doi":"10.1016/j.ensm.2025.104096","DOIUrl":"10.1016/j.ensm.2025.104096","url":null,"abstract":"<div><div>Quantifying the impact of temperature on the degradation behavior of the pouch cell during repeated fast charging is crucial for improving its fast-charging performance, especially in extreme conditions. Here, critical factors including electrochemical behavior, dynamic limitation, interfacial chemistry, structure evolution, and gas production affecting the battery degradation mechanisms have been explored and quantified based on the Ah-level LiNi<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>O<sub>2</sub>||graphite pouch cells. The battery delivers high specific capacity and acceptable reversibility in the early cycles at 50 °C, and capacity decay occurs with the increased cycles; at 0 °C, the battery shows high polarization, low specific capacity, and poor cycle stability. As revealed by electrochemical analysis, the battery performance at 0 °C is mainly limited by the sluggish interfacial kinetics and the uneven SEI layer with a low proportion of LiF and a high content of Li<sub>x</sub>O<sub>y</sub>. In contrast, high temperature accelerates the side reaction between electrolyte and cathode, inducing electrolyte decomposition, gas generation, and mechanical pulverization. Moreover, theoretical simulation reveals that the average cell temperature at 273 K is the highest. Both NCM523 cathode and graphite anode at 273 K have the greatest stress and deformation after one cycle at 8C, and the most cracks found on the cycled NCM523 particles at 323 K are mainly due to its severe side reaction. Based on these results, strategies for achieving fast-charging LIBs at extreme conditions can be proposed.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104096"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192704","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}
Chenxing Yang , Yuefeng Su , Wen Su , Siyuan Ma , Xinyu Zhu , Shaobo Wu , Yongjian Li , Lai Chen , Duanyun Cao , Meng Wang , Qing Huang , Yibiao Guan , Feng Wu , Ning Li
{"title":"Synergistically tailoring Kongming-lock morphology and Li+/Ni2+ intermixing to achieve ultrahigh-volumetric-energy-density layered Li-rich oxide cathodes","authors":"Chenxing Yang , Yuefeng Su , Wen Su , Siyuan Ma , Xinyu Zhu , Shaobo Wu , Yongjian Li , Lai Chen , Duanyun Cao , Meng Wang , Qing Huang , Yibiao Guan , Feng Wu , Ning Li","doi":"10.1016/j.ensm.2025.104019","DOIUrl":"10.1016/j.ensm.2025.104019","url":null,"abstract":"<div><div>The rapid growth of energy storage systems demands higher-performance lithium-ion batteries (LIBs). However, state-of-the-art polycrystalline (PC) LIB cathodes struggle with low compaction density, limiting their use in volume-constrained applications. While single-crystal (SC) materials such as LiCoO<sub>2</sub> suffer from low gravimetric energy density. Inspired by the traditional Chinese puzzle, we propose a lithium-rich manganese-based (LMR) cathode with a Kongming lock (KML)-like morphology that optimally regulates Li⁺/Ni<sup>2+</sup> intermixing. Cross-sectional scanning electron microscopy (SEM) confirms enhanced compaction density contributed by the micron-sized primary particles. High-resolution transmission electron microscopy (HRTEM) then shows Li⁺ diffusion-favorable {010} planes on the secondary particle surfaces, improving Li⁺ transport. As a result, electrochemical testing demonstrates an initial discharge capacity of 253 mAh g<sup>-1</sup>, with 96.3 % capacity retention after 100 cycles at 0.1C, and an ultra-high volumetric energy density of approximately 3050 Wh L<sup>-1</sup>, surpassing that of SC-LiCoO<sub>2</sub>. Synchrotron-based characterizations, combined with wide-angle X-ray scattering (WAXS), density functional theory (DFT), and finite element analysis, confirm the local structural, crystalline, and morphological stability of KML. This study underscores the importance of morphology design in cathode materials and advances the development of high gravimetric and volumetric energy density LMR cathodes for next-generation LIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104019"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935375","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":"Vertical & lateral ion-flux modulated ion-conductive SEI for high-performance Li-metal batteries","authors":"Yiping Liu , Yuxin Huang , Qiang Zhang , Rouyan Guo , Guangqi Zhang , Jie Dong , Liancheng Zhao , Liming Gao","doi":"10.1016/j.ensm.2025.104020","DOIUrl":"10.1016/j.ensm.2025.104020","url":null,"abstract":"<div><div>Ideal solid electrolyte interphase (SEI) is required for non-dendrite lithium (Li) deposition of lithium metal batteries (LMBs). However, the spontaneously-formed SEI is non-homogenous in the composition and structure and thus cause oriented distribution of Li<sup>+</sup> flux, which leads to the detrimental formation of lithium dendrites and poor cyclability of batteries. Here we propose a vertical & lateral ion-flux modulated ion-conductive SEI for high-voltage Li-metal batteries. A fluorinated MCM-41 (FMCM-41) modified LiPF<sub>6</sub> electrolyte is designed to construct the SEI film, which consists of homogenously distributed LiF and Li<sub>x</sub>SiO<sub>y</sub>, to regulate Li<sup>+</sup> transport paths in the lateral and the vertical direction, respectively, achieving uniform lithium plating. With the FMCM-41 modified electrolyte, the prepared Li||Li cell presents a long-term stability over 1000 h, and the Li||NCM622 full cell exhibits outstanding cycling performance with a high specific capacity of 169.9 mAh g<sup>-1</sup> and a high-capacity retention of 93.3 % over 100 cycles at 0.5 C. This lateral-vertical concept provides a promising strategy for designing a desired SEI with uniform Li<sup>+</sup> transport paths to achieve ultra-long and high-rates lithium metal batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104020"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935376","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}
Le Zhang, Min Lin, Zihong Yu, Youxia Huang, Qiangchao Sun, Xionggang Lu, Hongwei Cheng
{"title":"Tyrosine additives with rich-polar functional groups provide multi-protections for ultra-stable zinc metal anodes","authors":"Le Zhang, Min Lin, Zihong Yu, Youxia Huang, Qiangchao Sun, Xionggang Lu, Hongwei Cheng","doi":"10.1016/j.ensm.2025.104022","DOIUrl":"10.1016/j.ensm.2025.104022","url":null,"abstract":"<div><div>The widespread commercialization of aqueous Zinc-Ion batteries (AZIBs) is severely limited by dendrite growth and rampant parasitic reactions. While various additives have been introduced to improve the stability of zinc anodes, a single polar functional group additive cannot provide comprehensive protection for zinc anodes. Here, a low-cost, high-functionality Tyrosine (Tyr) organic small molecule is utilized as an electrolyte additive to achieve ultra-stable zinc metal anodes. The findings indicated that the electronegative carboxyl group tended to participate in the solvation sheath of Zn<sup>2+</sup>. The zinc-philic amino group and hydrophobic benzene ring synergistically construct a hydrophobic electric double layer on the surface of the zinc anode. The hydrophilic nature of the hydroxyl group enables it to capture free water molecules and reconstruct the hydrogen bonding network of the electrolyte. More importantly, the strong adsorption of Tyr molecule is beneficial to induce the formation of an <em>in-situ</em> organic-inorganic hybrid solid electrolyte interface layer, thereby further enhancing protection for the zinc anode. Profiting from the synergistic effect of the polyfunctional group in the Tyr additive, the Zn||Zn cell exhibits ultra-long cycle stability over 3800 h (∼ 20 times vs. ZnSO<sub>4</sub>) at 1.0 mA cm<sup>‒2</sup>, 1 mAh cm<sup>‒2</sup> and an ultra-high cumulative plated capacity of 8.75 Ah cm<sup>‒2</sup> at 5.0 mA cm<sup>−2</sup>. Furthermore, the Zn||Cu cell delivers a significantly improved reversibility with an average Coulomb efficiency of 99.88 % after 3000 cycles. This finely regulated electrolyte, leveraging the synergistic effects of multiple functional groups, heralds a promising trajectory for the advancement of enduring Zn metal batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104022"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142939517","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}
Lea C. Meyer , Abilash Kanish Thiagarajan , Alexey Koposov , Andrea Balducci
{"title":"Unravelling the mechanism of potassium-ion storage into graphite through electrolyte engineering","authors":"Lea C. Meyer , Abilash Kanish Thiagarajan , Alexey Koposov , Andrea Balducci","doi":"10.1016/j.ensm.2025.104021","DOIUrl":"10.1016/j.ensm.2025.104021","url":null,"abstract":"<div><div>Graphite is one of the most widely used anode materials in potassium-ion batteries (PIBs). However, the exact mechanism of K<sup>+</sup>ions intercalation into graphite has not yet been fully understood. In addition, the intercalation process strongly depends on the selection of the electrolyte system. In this work, we evaluated the use of an electrolyte containing 1.5 M potassium bis(fluorosulfonyl)imide (KFSI) dissolved in a mixture of propylene carbonate (PC)/ 1,1,2,2-tetraethoxyethane (TEG)/ vinyl ethylene carbonate (VEC) (62:36:2 vol.%). Using such an electrolyte system it was possible to obtain experimental evidence for the formation of KC<sub>16</sub> during the potassium intercalation and deintercalation using <em>in situ</em> Raman spectroscopy and operando X-ray diffraction (XRD). The results are supported by the visual observation of a color change of the graphite electrode surface during the intercalation of K<sup>+</sup> ions into the graphite lattice. In addition, it has been demonstrated that the selected electrolyte system eliminates the co-intercalation of the solvent into the graphite structure.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104021"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142961960","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}
Su Hwan Jeong , In-Kyung Kim , Suyoon Eom , Hwiryeong Hwang , Young Hwa Jung , Joo-Hyung Kim
{"title":"Engineering the local chemistry through fe substitution in layered P2-Na0.7Ni0.2Co0.2Mn0.6O2 for high-performance Sodium-Ion batteries","authors":"Su Hwan Jeong , In-Kyung Kim , Suyoon Eom , Hwiryeong Hwang , Young Hwa Jung , Joo-Hyung Kim","doi":"10.1016/j.ensm.2025.104041","DOIUrl":"10.1016/j.ensm.2025.104041","url":null,"abstract":"<div><div>Sodium-ion batteries (SIBs) are considered promising alternatives to lithium-ion batteries (LIBs) for large-scale applications. Layered transition metal oxides are mainly used as cathode materials to enhance energy density and electrochemical performances. In this study, we compare Mn-based P2-type Na<sub>0.7</sub>Ni<sub>0.2</sub>Co<sub>0.2</sub>Mn<sub>0.6</sub>O<sub>2</sub> (NCM) with partially Fe-substituted Na<sub>0.7</sub>Ni<sub>0.2</sub>Co<sub>0.2</sub>Mn<sub>0.5</sub>Fe<sub>0.1</sub>O<sub>2</sub> (NCMF) via facile solid-state synthesis. Interestingly, Fe-substitution improves not only structural stability but also Na<sup>+</sup> diffusion kinetics. It is found that the P2-O2 phase transition at high voltage region is mitigated with smaller volume change and enhanced oxygen redox reaction as demonstrated by in-situ X-ray diffraction and ex-situ X-ray photoelectron spectroscopy. In addition, density functional theory calculations exhibit that NCMF expedites Na<sup>+</sup> diffusion and reduces the site energy difference between Na<sub>f</sub> and Na<sub>e</sub> by decreasing Na occupancy in the Na<sub>f</sub> site, which is located right below the transition metal ions. As a result, the NCMF electrode delivers a high initial energy density of 601.5 Wh kg<sup>-1</sup> with an average discharge voltage of 3.05 V (V vs. Na<sup>+</sup>/Na). It also shows a high discharge capacity of 168.15 mAh g<sup>-1</sup> at 0.5 C with excellent capacity retention of 68.7 % after 100 cycles within a wide voltage range of 1.5–4.5 V. These findings provide a significant impact of Na site occupancy difference for improving electrochemical performance and structural stability as a rational method for the commercialization of SIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104041"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987482","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}
Ridong Hu , Chong Mao , Hao Zhuo , Xiaobing Dai , Lewen Yang , Xugang Shu , Yang Li , Zhanqiang Li , Wenhong Ruan , Fujie Yang , Xudong Chen
{"title":"Molecular space linkage of dipentacyclic anhydride additives for long-lifespan Li-metal batteries with Ni-rich cathode","authors":"Ridong Hu , Chong Mao , Hao Zhuo , Xiaobing Dai , Lewen Yang , Xugang Shu , Yang Li , Zhanqiang Li , Wenhong Ruan , Fujie Yang , Xudong Chen","doi":"10.1016/j.ensm.2025.104033","DOIUrl":"10.1016/j.ensm.2025.104033","url":null,"abstract":"<div><div>The precarious interfacial chemistry between the electrode and electrolyte is the determining step that restricts the long cycle life of Ni-rich-based Li-metal batteries. Here we show that the robust cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) layers can be engineered by tuning the spatial linking structure of dipentacyclic anhydride (DPA) additives. Specifically, an inorganic-rich CEI/SEI layer induced by CBDA (a DPA featuring a quaternary ring spatial linking structure) exhibits superior Li<sup>+</sup> interfacial kinetics and an ultra-stable cycle performance, outperforming the other systems. As a result, the NCM811ǁLi cells containing CBDA show excellent long-term performances, even under high voltage, high load, and high charge-discharge current density, respectively. The coin-cell using a low-loading cathode exhibits 129 mAh g-<sup>1</sup> discharged capacity for over 200 cycles at a 6 C rate. Moreover, The high-loading cathode retains 80 % capacity after 312 cycles at 1.0 C. Furthermore, the NCM811ǁLi pouch cell demonstrated a capacity retention rate of 99.8 % after 50 cycles. Prolonged stable cycling for 900 cycles (93 % capacity retention) in an NCM811ǁGraphite pouch cell is enabled by CBDA. The DPA-based additives in this work offer a highly promising and feasible route to achieving a long-term and high-capacity lithium battery featuring a Ni-rich cathode.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 ","pages":"Article 104033"},"PeriodicalIF":18.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142989633","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}