Energy Storage Materials最新文献

{"title":"Trace Copper-Mediated Crystal Structure Modulation Enables Superior Stable Sodium Storage in NASICON Cathodes","authors":"Zheng Hu, Yuxin Ran, Junpeng Xie, Xusheng Wang, Jianqiu Zhu, Yao Liu, Liang Ma, Wenjie Mai, Jinliang Li","doi":"10.1016/j.ensm.2026.105445","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105445","url":null,"abstract":"As a representative NASICON-type cathode, Na<ce:inf loc=\"post\">3</ce:inf>V<ce:inf loc=\"post\">2</ce:inf>(PO<ce:inf loc=\"post\">4</ce:inf>)<ce:inf loc=\"post\">3</ce:inf> (NVP) is hindered by intrinsically sluggish electron transport within the V-O framework, which induces severe polarization and rapid capacity decay under high-rate operation. In this work, we propose crystal structure modulation enabled by the introduction of trace amounts of Cu to overcome the electronic and structural limitations of NVP. Replacing V3+ with trace amounts of Cu<ce:sup loc=\"post\">2+</ce:sup> alters the local energy landscape, thereby improving local structural symmetry and stability over extended cycling. Furthermore, extending along the c‑axis directly enlarges the Na‑ion migration pathways, resulting in a 2.7-fold increase in ionic conductance. This behavior simplifies the two-phase reaction mechanism and leads to improved cycling performance over a wide temperature range. Benefiting from this modification, the optimized NVP delivers 112.3 mAh g<ce:sup loc=\"post\">-1</ce:sup> at 0.2 C and retains an 86% capacity retention after 10,000 cycles at 50 C. Remarkably, high stability is maintained from -20°C (97.3 mAh g<ce:sup loc=\"post\">-1</ce:sup> at 0.2 C) to 60°C (92.3 mAh g<ce:sup loc=\"post\">-1</ce:sup> at 20 C), outperforming all previously reported works. We believe that our trace copper-mediated crystal structure of NASICON-type cathodes offers a guiding pathway for developing next-generation, highly stable cathode materials.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"159 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148717432","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":"Bionic topology reconstruction drives confined competitive ligand-exchange hopping dynamics in hydrogel electrolytes to achieve high-performance structural Zn-Ion batteries","authors":"Junhang Xu, Zhongyuan Shi, Yifei Liu, Qigang Han, Shuqing Kou","doi":"10.1016/j.ensm.2026.105446","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105446","url":null,"abstract":"Developing hydrogel electrolytes with both high ionic conductivity and mechanical robustness remains a core challenge for structural batteries. Inspired by scorpion slit sensilla, we propose a stretch-induced topological reconfiguration strategy to achieve a highly uniaxial synergistic orientation of silver nanowires and Ti<ce:inf loc=\"post\">3</ce:inf>C<ce:inf loc=\"post\">2</ce:inf>T<ce:inf loc=\"post\">x</ce:inf> MXene within a polyacrylamide hydrogel (S-OAMP), building ordered 1D confined nanochannels. Within this confined framework, a confined competitive ligand-exchange hopping (C<ce:glyph name=\"sbnd\"></ce:glyph>CLEH) mechanism is revealed. This mechanism thermodynamically disrupts the conventional hydration steady state by generating a binding energy of ΔG=-5.8 kJ mol<ce:sup loc=\"post\">-1</ce:sup>, driving a transition of Zn<ce:sup loc=\"post\">2+</ce:sup> from 3D random diffusion to 1D directional transport featuring a low energy barrier of Ea=29.8 kJ mol<ce:sup loc=\"post\">-1</ce:sup>. The S-OAMP electrolyte delivers a superior ionic conductivity of 52.9 mS cm<ce:sup loc=\"post\">-1</ce:sup> and a high Zn<ce:sup loc=\"post\">2+</ce:sup> transference number of 0.89. Compounded with carbon fibers, under varying tensile loads, the transverse contraction of S-OAMP driven by the anisotropic Poisson effect radially compresses the 1D channels, achieving a remarkable discharge capacity recovery of nearly two-thirds and further validating the applicability of the C<ce:glyph name=\"sbnd\"></ce:glyph>CLEH mechanism. Structural batteries retain 81.9% capacity over 1400 cycles, and Zn||Zn symmetric cells endure prolonged cycling exceeding 2600 h. The C<ce:glyph name=\"sbnd\"></ce:glyph>CLEH mechanism provides a new paradigm for designing high-load-bearing, long-lifespan solid-state energy materials.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"67 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148717434","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":"Engineering high-spin cobalt centers via cation-anion co-doping to boost polysulfide conversion in lithium-sulfur batteries","authors":"Fen Li, Guo Liu, Qi Zeng, Xiaoxiang Sun, Jiayou Tao, Chang Li, Zhenxing Zhang, Jijun Zhao","doi":"10.1016/j.ensm.2026.105447","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105447","url":null,"abstract":"Catalytic strategies currently provide an effective way to tackle the shuttle effect and sluggish reaction kinetics in lithium-sulfur batteries. While elemental doping has been employed to tailor the electronic structure of catalysts, the concerted manipulation of spin states at active centers via cation-anion co-doping remains incompletely explored. Here, we devise an Fe and P co-doping strategy to forge a spin-polarized CoSe<ce:inf loc=\"post\">2</ce:inf> catalyst through a hydrothermal route followed by gas-phase phosphorization. Density functional theory calculations, substantiated by experimental evidence, reveal that P doping first induces adjacent Co atoms to adopt a high-spin configuration. On this basis, the implanted Fe centers further trigger 3d electron spin flipping on additional vicinal Co atoms across asymmetric Fe-Se-Co bridges, elevating them from a low-spin (t<ce:inf loc=\"post\">2g</ce:inf><ce:sup loc=\"post\">6</ce:sup>e<ce:inf loc=\"post\">g</ce:inf><ce:sup loc=\"post\">1</ce:sup>) to a high-spin (t<ce:inf loc=\"post\">2g</ce:inf><ce:sup loc=\"post\">5</ce:sup>e<ce:inf loc=\"post\">g</ce:inf><ce:sup loc=\"post\">2</ce:sup>) state. This sequential synergy significantly amplifies the overall spin polarization, refines orbital hybridization between metal sites and polysulfides, diminishes antibonding electron occupation, and enhances adsorption bond orders, thereby substantially boosting sulfur conversion kinetics. Li-S batteries incorporating this catalyst attain a stellar reversible capacity of 622.7 mAh g⁻<ce:sup loc=\"post\">1</ce:sup> at 4 C and stable 2000-cycle longevity at 4 C, with a capacity decay rate of merely 0.033% per cycle. This work charts a new avenue for elevating lithium-sulfur battery efficacy through spin-state engineering powered by cation-anion co-doping.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"15 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148717433","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":"Analysis of stress evolution in lithium metal anodes during plating and stripping cycles","authors":"Kurt R. Hebert","doi":"10.1016/j.ensm.2026.105428","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105428","url":null,"abstract":"Liquid cell batteries with lithium metal anodes may exhibit degraded Coulombic efficiency due to plating of porous, filamentary deposits. Experiments suggest that filament growth is controlled by lithium diffusion-induced compressive stress. In situ wafer curvature measurements can reveal the dynamic stress response of lithium deposits during cycling, but the interpretation of these experiments is complicated by the unknown and changing deposit morphology. Here, a new modeling approach is introduced that avoids this difficulty by focusing on the curvature response in open-circuit intervals during cycling. We demonstrate fitting of experimental curvature transients to characterize evolution of deposit morphology, metal-phase diffusion and mechanical deformation in cycling experiments. The model is based on metal-phase diffusion accommodated by elastic deformation and power-law creep, and is validated by comparison of the fit creep parameters with independent nanoindentation experiments. The results provide evidence for the presence of diffusion-induced compressive stress in plating periods. Lithium stripping is shown to generate tensile stress in lithium in a micron-thick surface-adjacent layer, consistent with experimental observations of submicron near-surface voids.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"61 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148717544","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":"Single-walled carbon nanotube film based self-adhesive air electrode featuring interaction-enhanced dual sites for high-performance Zn-Air batteries","authors":"Yu Meng, Zhong-Qiang Ni, Rui-Hong Xie, Mengke Zou, Hao Yang, Yi-Long Chen, Pengfei Xie, Jin-Cheng Li, Peng-Xiang Hou, Chang Liu","doi":"10.1016/j.ensm.2026.105441","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105441","url":null,"abstract":"The realization of Zn-air batteries (ZABs) for electric vehicles and portable devices critically depends on high-performance air electrodes capable of fast mass transport, efficient catalysis for the oxygen reduction/evolution reactions (ORR/OER) and desirable oxidation resistance, but the actual assembly is still a great challenge. In this work, a single-walled carbon nanotube (SWCNT) multifunctional film is proposed directly as binder-free air electrode to overcome the dilemma. Specifically, FeNi₃ nanoparticles are anchored on SWCNTs during the film synthesis, whereas the Fe-N<ce:inf loc=\"post\">4</ce:inf> moieties are introduced via a post-treatment process involving sublimation of iron phthalocyanine. Thereinto, high-quality SWCNT units ensure excellent stability of the resulting electrode due to the intrinsic property of high oxidation resistance and three-dimensional interwoven SWCNT bundles without any binder are qualified for fast O<ce:inf loc=\"post\">2</ce:inf> diffusion to active sites. Furthermore, combined experimental results and theoretical calculations reveal that FeNi nanoparticles and Fe-N<ce:inf loc=\"post\">4</ce:inf> moieties anchored on the curved nanotube walls interact synergistically to boost catalytic activities. As a result, the film electrode exhibits a low overall overpotential of 0.63 V (E<ce:inf loc=\"post\">OER/10</ce:inf>-E<ce:inf loc=\"post\">ORR/half</ce:inf>), better than the precious metal-based catalysts (Pt/C-Ir/C: 0.72V). When directly assembled into binder-free air electrodes for ZABs, ultrahigh output performance (peak power density: 251 mW cm<ce:sup loc=\"post\">-2</ce:sup>) and ultralong-life charge-discharge cycling stability (1600 h) are realized.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"26 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148692350","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":"Synergistic Interphase and Electrolyte Stabilization through Integrating Complementary Functional Groups into a Single Molecular Framework for High-Voltage NCM811 Cathodes with High-Temperature Adaptability","authors":"Mingjun Ma, Haolei Chen, Haonan Huang, Yijie Lin, Yuling Fu, Shuai Chen, Huahua Chen, Xinqi Chen, Jiarong He, Lidan Xing, Weishan Li","doi":"10.1016/j.ensm.2026.105439","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105439","url":null,"abstract":"Ni-rich LiNi<ce:inf loc=\"post\">0.8</ce:inf>Co<ce:inf loc=\"post\">0.1</ce:inf>Mn<ce:inf loc=\"post\">0.1</ce:inf>O<ce:inf loc=\"post\">2</ce:inf> (NCM811) is a promising high-voltage cathode material for high-energy-density lithium-ion batteries (LIBs). However, its practical application is hindered by the instability of the cathode–electrolyte interface under high-voltage and elevated-temperature operating conditions. Herein, 6-fluoro-3-cyanopyridine (FCP) is introduced as a multifunctional film-forming electrolyte additive to stabilize the NCM811 cathode, enabling synergistic improvements in high-voltage stability (4.5 V) and thermal stability under elevated-temperature conditions (55°C). Density functional theory calculations and electrochemical characterizations reveal that FCP preferentially undergoes oxidative decomposition, forming a LiF/-C=N-C-enriched cathode-electrolyte interphase (CEI) on the NCM811 surface. The resulting CEI effectively enhances the structural stability of the NCM811 cathode, suppressing irreversible surface phase reconstruction and transition-metal dissolution during high-voltage cycling while facilitating Li<ce:sup loc=\"post\">+</ce:sup> transport kinetics. Consequently, NCM811/Li half-cells with 2.0 wt.% FCP exhibit much higher capacity retentions of 63.9% after 600 cycles at 25°C and 74.2% after 200 cycles at 55°C within 3.0∼4.5 V, significantly outperforming those with the Base electrolyte (32.1% and 59.9%, respectively). The practicality of the FCP additive is further demonstrated in NCM811/graphite full-cells, which deliver superior capacity retentions of 80.0% after 500 cycles at 25°C and 70.6% after 200 cycles at 55°C, compared with 57.8% and 32.8%, respectively, for the Base electrolyte. This work provides valuable insights into the design of multifunctional electrolyte additives by integrating complementary functional groups into a single molecular framework, offering an effective strategy for stabilizing high-voltage NCM811 cathodes and advancing high-energy-density LIBs with enhanced high-temperature durability.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"14 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148692126","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":"Constructing 3D Ion-Conductive Binder Networks for Boosted Prelithiation Kinetics and Interfacial Stability of High-Loading Si/C Anodes","authors":"Wenjie He, Zhigang Li, Zhuo Li, Zimu Su, Xu Chen, Kangsheng Huang, Yue Xiao, Jia Yang, Gai Wu, Xiangjun Chen, Jiangmin Jiang","doi":"10.1016/j.ensm.2026.105433","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105433","url":null,"abstract":"The practical application of high-loading silicon-carbon (Si/C) anodes is hindered by sluggish and non-uniform prelithiation, stemming from inadequate lithium-ion (Li<ce:sup loc=\"post\">+</ce:sup>) transport and large volume changes. To address this, we have designed a three-dimensional (3D) networked ion-conductive binder, which leverages abundant sulfonate (-SO<ce:inf loc=\"post\">3</ce:inf><ce:sup loc=\"post\">−</ce:sup>) groups as Li<ce:sup loc=\"post\">+</ce:sup> hopping sites, thus synergizing with dynamic hydrogen bonds to construct a continuous 3D Li<ce:sup loc=\"post\">+</ce:sup> transport network. This network not only accommodates volume changes but also enables rapid and homogeneous Li<ce:sup loc=\"post\">+</ce:sup> migration. By combining ex/in-situ characterization with theoretical simulations, we reveal that the -SO<ce:inf loc=\"post\">3</ce:inf><ce:sup loc=\"post\">−</ce:sup> groups facilitate Li<ce:sup loc=\"post\">+</ce:sup> desolvation and promote the formation of a robust, LiF-rich solid electrolyte interphase (SEI). As a result, the modified Si/C electrode achieves an exceptional initial Coulombic efficiency (ICE) of 102.7% and a high areal capacity of 4.63 mAh cm<ce:sup loc=\"post\">−2</ce:sup> after ∼3 minutes of prelithiation at 5 mg cm<ce:sup loc=\"post\">−2</ce:sup>. When paired with an NCM85 cathode, the full-cell delivers an ICE of 89.36% and retains an energy density of 484 Wh kg<ce:sup loc=\"post\">−1</ce:sup> after 50 cycles. This work elucidates the pivotal roles between prelithiation kinetics and interfacial stability, which establishes a functional-binder design strategy for overcoming the critical bottlenecks in high-capacity Si-based lithium-ion batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"24 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148692046","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":"Pyridinic Dipole–Engineered Interfacial Design for Developing Fast-Charging and Ultra-Stable Silicon Anodes","authors":"Song Kyu Kang, Hyeonju Kim, Sung-Dae Kim, Sang Ho Lee, Won Bae Kim","doi":"10.1016/j.ensm.2026.105431","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105431","url":null,"abstract":"To establish a generic design strategy for fast-charging and high-capacity-retention Si anode structures, synergistic control over the interactions between interfacial layers and electrolyte chemistry is considered essential. Here, we developed electronically polarized pyridinic interfacial layers on a Si-decorated carbon nanofiber architecture, with the ultimate goal to facilitate the formation of a stable LiF-rich solid–electrolyte interphase. Furthermore, the Lewis basicity of pyridinic nitrogen effectively modulated local Li<ce:sup loc=\"post\">+</ce:sup> coordination at the interface, thereby inducing effective lithiation kinetics even on the intrinsically sluggish Si (111) facet. As a result, the engineered Si anode architecture delivered a high discharge capacity of ∼ 1850 mAh g<ce:sup loc=\"post\">−1</ce:sup> at an ultrahigh current density of 10 A g<ce:sup loc=\"post\">−1</ce:sup> and sustained a reversible capacity of ∼ 1700 mAh g<ce:sup loc=\"post\">−1</ce:sup> over 300 cycles (∼ 90 % retention). Notably, full-cell configurations paired with LiNi<ce:inf loc=\"post\">0.8</ce:inf>Co<ce:inf loc=\"post\">0.1</ce:inf>Mn<ce:inf loc=\"post\">0.1</ce:inf>O<ce:inf loc=\"post\">2</ce:inf>-based cathodes retained outstanding cycling performance, with ∼ 90 % of the initial capacity at 0.5 C over 160 cycles, highlighting that bespoke interfacial dipole engineering offers a powerful strategy for regulating SEI chemistry and enabling high-performance Si anodes for next-generation lithium-ion storage systems.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"36 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148692347","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":"Revisit Solvation Chemistry in High-Concentration Ether-based Electrolytes to Stabilize Alloy-Type Anodes of Sodium Ion Batteries","authors":"Qian Yao, Cheng Zheng, Zhenjie Cheng, Gulian Wang, Jizhen Ma, Zhongchao Bai, Shixue Dou, Nana Wang, Guoxiu Wang, Jian Yang","doi":"10.1016/j.ensm.2026.105436","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105436","url":null,"abstract":"Alloy-based anodes are promising for sodium-ion batteries but suffer from large volume variation during cycling. Although ether-based electrolytes benefit many alloy-based anodes, they fail for Sb. Here, mechanical property and volume variation are proposed to explain the greater challenge with Sb (versus Bi and Sn). Then, a high-concentration electrolyte is developed for commercial Sb powders (μ-Sb) by using THF as the solvent for its good solubility to sodium salts, low molecular polarity and small molecule size. Theoretical simulations indicate that the increasing salt concentration makes the anions in the solvation sheath shift from monodentate to polydentate. This change results in weakened P-F bonds, reduced LUMO energy levels and increased Na-ion number within one cluster, promoting the formation of a NaF-rich solid electrolyte interphase on the surface. Such an interphase greatly enhances ion conductivity and mechanical resilience, improving the electrochemical performance of μ-Sb. This electrolyte is also compatible to Sn and Bi. These results advance our understandings of solvation structures and interface chemistry critical for high-performance sodium-ion batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"101 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148692346","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":"Enhanced Particle Interlocking and Interface Design in Dry-Processed Polymer-in-Ceramic Composite Electrolytes with Multifunctional Silane","authors":"Tamene Beshaw Tirfie, Desalegn Yilma Kibret, Tadesu Hailu Mengesha, Behrouz Bazri, Liang-Yin Kuo, Yi-Shiuan Wu, Jeng-Kuei Chang, Rajan Jose, Chun-Chen Yang","doi":"10.1016/j.ensm.2026.105434","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105434","url":null,"abstract":"Polymer-in-ceramic composite solid-state electrolytes (PICSEs) are a promising strategy for realizing next-generation solid-state batteries (SSBs). However, poor intrinsic interfacial compatibility between the ceramic and polymer matrix and inadequate contact at the electrode-electrolyte interfaces remain serious challenges. Herein, a multifunctional 3-(trimethoxysilyl) propylmethacrylate (TMSPM) molecule is grafted on the Li<ce:inf loc=\"post\">6.25</ce:inf>Al<ce:inf loc=\"post\">0.25</ce:inf>La<ce:inf loc=\"post\">3</ce:inf>Zr<ce:inf loc=\"post\">2</ce:inf>O<ce:inf loc=\"post\">12</ce:inf> (LALZO) particle’s surface. Consequently, we prepared a PICSE with 60 wt.% TMSPM-functionalized LALZO active filler and polymer matrix (hereafter denoted as PICSE60) via thermal extrusion blending. To further improve both the PICSE60/electrode interface and the ceramic/polymer matrix interface, PEGDMA crosslinking was sequentially engineered as an integrated interfacial interlayer (denoted as C-PICSE60). This molecular-level interface engineering helped bridge the ceramic/polymer matrix interphase and enhanced Li<ce:sup loc=\"post\">+</ce:sup> flux throughout the bulk PICSEs via multiple Li<ce:sup loc=\"post\">+</ce:sup> coordination with TMSPM (Li⋅⋅⋅- O=C) and PEO (Li⋅⋅⋅- O‒C). Experimental and computational modeling elucidated the role of TMSPM in molecular bridging between the composite components. Consequently, C-PICSE60, containing a small amount of LiDFOB/LiDFP-based liquid electrolyte, exhibited a high Li⁺ transference number (<ce:italic>ca.</ce:italic> 0.65), ionic conductivity (0.66 mS cm⁻¹, RT), a wide electrochemical window (5.21 V vs. Li/Li⁺), and stable symmetric-cell cycling for over 2900 h. The Li||LiFePO₄ full cells exhibited long cycling stability, retaining 90.83% capacity after 1150 cycles at 0.5 C/1 C. The full cell with a high-voltage polyacrylonitrile-coated single-crystal LiNi<ce:inf loc=\"post\">0.86</ce:inf>Co<ce:inf loc=\"post\">0.05</ce:inf>Mn<ce:inf loc=\"post\">0.05</ce:inf>Al<ce:inf loc=\"post\">0.04</ce:inf>O<ce:inf loc=\"post\">2</ce:inf> (PAN@SC-NCMA86) cathode exhibited 80.82% capacity retention after 550 cycles at 0.5 C (2.8–4.3 V). This work provides new insights into an integrated engineering strategy for achieving robust interfacial compatibility, enabling high-performance hybrid-SSBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"166 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148692400","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}