{"title":"Nickel-Anchored N-Enriched CNTs Nucleated via CoNi Alloy for Sustainable Zinc–Air Batteries","authors":"Ashwini Anshu, Shubham Kumar Parate, Sanjit Kumar Parida, Pavan Nukala, Balaram Sahoo","doi":"10.1021/acsaem.6c02672","DOIUrl":"https://doi.org/10.1021/acsaem.6c02672","url":null,"abstract":"<p>Rationally designed, multifunctional, highly efficient, robust, and cost-effective non-precious-metal-based bifunctional oxygen electrocatalysts have attracted substantial interest in the field of clean energy over the last few decades. A catalyst designed with surface charge-storage-like properties is of great significance for sustainable Zn–air batteries. However, preparing such an interface requires complex synthesis and purification. Here, we used binary CoNi alloy nanoparticles as nuclei in a single-step pyrolytic synthesis to create a novel hybrid of nickel-anchored nitrogen-doped carbon nanotubes (CNTs). The improved sample showcases a bifunctional interface capable of both oxygen evolution and reduction, along with efficient EDLC-type surface charge storage. As a result, the hybrid structure exhibits capacitive characteristics, making it a potential candidate for supercapacitor-assisted zinc–air battery configurations. This superstructure (CoNi/CNTs) enabled ZAB to reach an open-circuit voltage of 1.447 V and a power density of 141.29 mW/cm<sup>2</sup>. This promising performance is attributed to the active surfaces of the N-doped compartmentalized CNTs. Furthermore, the synergistic interactions between the catalytically active carbon centers, anchoring ultrasmall Ni clusters, and CoNi alloy nanoparticles further improve the catalytic activity. Our findings emphasize the potential for clean-energy applications by demonstrating the practical benefits of integrating charge-storage-like properties in the catalyst architecture for sustainable Zn–air batteries.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"14474–14490"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368649","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shuqing Cao, Jiaming Xu, Zhiyuan Ma, Shangjing Yang, Boyu Mu, Hong Liu, Rui He, Yu Xia
{"title":"Ultrathin-Gap MXene/Carbon Nanotube Microsupercapacitors for High-Performance Alternating Current-Line Filtering","authors":"Shuqing Cao, Jiaming Xu, Zhiyuan Ma, Shangjing Yang, Boyu Mu, Hong Liu, Rui He, Yu Xia","doi":"10.1021/acsaem.6c02122","DOIUrl":"https://doi.org/10.1021/acsaem.6c02122","url":null,"abstract":"<p>The continued miniaturization of modern electronic devices has created an urgent demand for next-generation AC-line filtering capacitors capable of replacing conventional aluminum electrolytic capacitors. Here, we report a high-performance AC-line filter based on MXene/CNT liquid crystal, fabricated into cross-finger electrodes via spin coating followed by supercritical drying. Precise control over the interelectrode gap width was achieved using femtosecond laser direct writing, enabling gap sizes as small as 5 µm. Systematic electrochemical characterization reveals that the electrode with a 5 µm gap width exhibits an ultralow equivalent series resistance of 0.15 Ω cm<sup>2</sup> and a highly negative phase angle of –84° at 120 Hz. Owing to rapid ion transport within MXene/CNT architecture and the ultranarrow electrode spacing, the device delivers superior high-frequency response with a 0.1 ms relaxation time constant, and efficient AC-line filtering performance. These results demonstrate the strong potential of MXene-based microsupercapacitors as compact, high-performance alternatives to traditional electrolytic capacitors for powering next-generation electronic systems.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"13972–13981"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mouli Das Dawn, Ankita Mondal, Bhanu Bhusan Khatua, Kumar Biradha
{"title":"Hybrid Supercapacitor Based on Functionalized Ni-MOF Composite: Achieving Superior Power Density in Asymmetric Energy Storage Device","authors":"Mouli Das Dawn, Ankita Mondal, Bhanu Bhusan Khatua, Kumar Biradha","doi":"10.1021/acsaem.6c02601","DOIUrl":"https://doi.org/10.1021/acsaem.6c02601","url":null,"abstract":"<p>Hybrid energy storage systems have gained significant attention for addressing rising global energy demands by combining the complementary strengths of batteries and supercapacitors. Their practical implementation, however, requires simultaneous achievement of high energy and power densities, long-term cycling stability, and robust capacitance retention, criteria often limited by the inadequate functionality and structural instability of conventional electrode materials. In this work, a bromine-functionalized nickel-based MOF (<strong>Ni-HBTM</strong>) containing free carboxylic acid groups was synthesized to overcome these limitations. The <strong>Ni-HBTM</strong> metal–organic framework (MOF) delivered a specific capacitance of 620.22 F/g at 1 A/g in an alkaline electrolyte. When integrated with reduced graphene oxide (<strong>Ni-HBTM@rGO_20</strong>), the composite achieved an impressive specific capacitance of 1237.3 F/g at 1 A/g. An asymmetric supercapacitor (ASC) assembled using <strong>Ni-HBTM@rGO_20</strong> as the positive electrode exhibited a specific capacitance of 174.04 F/g, energy density of 54.39 Wh/kg at 1 A/g, and a power density of 11,250 W/kg at 15 A/g current densities with 94% capacitance retention after 10,000 cycles, which is a significantly high specific capacitance and power density for Ni-MOF-based composites in comparable conditions. The ASC successfully powered light-emitting diodes (LEDs), demonstrating the potential of functionalized MOF-based materials to bridge the performance gap between batteries and supercapacitors and offering an approach toward next-generation all-solid-state energy storage devices.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"14409–14421"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368567","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Maryem EL Hayany, Majid EL Kassaoui, Abdelilah Benyoussef, Jean-Michel Nunzi, Omar Mounkachi
{"title":"Three-Dimensional Porous Silicon-Carbon Polymorph: Li/Na Functionalization toward High-Efficiency Hydrogen Storage","authors":"Maryem EL Hayany, Majid EL Kassaoui, Abdelilah Benyoussef, Jean-Michel Nunzi, Omar Mounkachi","doi":"10.1021/acsaem.6c02543","DOIUrl":"https://doi.org/10.1021/acsaem.6c02543","url":null,"abstract":"<p>Porous materials decorated with alkali metals have emerged as attractive candidates for reversible hydrogen storage because they can simultaneously provide high adsorption capacity, suitable adsorption strength, and rapid hydrogen transport. Motivated by this strategy, the present work explores the hydrogen-storage behavior of three-dimensional porous silicon-carbon polymorph 3D-t(SiC)<sub>12</sub> after Li and Na functionalization using density functional theory (DFT) calculations together with ab initio molecular dynamics (AIMD) simulations. Both alkali metals interact strongly with the host framework, exhibiting binding energies of –2.58 eV for Li and –2.10 eV for Na, which indicates thermodynamically stable decoration and minimizes the tendency toward metal clustering. A clear distinction is observed between the two decorating species, with Li producing significantly stronger interactions with hydrogen molecules than Na. As a result, the Li-functionalized framework stores as many as 34 H<sub>2</sub> molecules, corresponding to a gravimetric capacity of 6.39 wt %, while maintaining an average adsorption energy of –0.167 eV per H<sub>2</sub>, a value favorable for reversible adsorption and desorption. Under identical conditions, Na decoration yields a lower storage capacity of 5.86 wt %. Thermodynamic calculations predict hydrogen release within an average temperature window of 267–368 K and equilibrium pressures between 8 and 20 bar, highlighting practical operating conditions. Dynamic stability is confirmed by AIMD simulations, which show that the hydrogenated structures remain intact throughout the simulations while preserving reversible adsorption characteristics. In addition, hydrogen diffusion on the Li-decorated surface proceeds through remarkably small activation barriers of only 0.010–0.178 eV, suggesting highly efficient molecular transport across the porous network. Collectively, these findings demonstrate that Li-functionalized 3D-<em>t</em>(SiC)<sub>12</sub> is a highly promising solid-state hydrogen-storage material and provide valuable design principles for next-generation porous hydrogen-storage materials.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"14349–14364"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368568","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lonneke van Eijk, Jayson Foster, Lei Ding, Weitian Wang, Genevieve Stelmacovich, Feng-Yuan Zhang, Adam Paxson, Svitlana Pylypenko
{"title":"Investigation of IrRuOx-Based Porous Transport Electrodes as a Function of Post-Treatments","authors":"Lonneke van Eijk, Jayson Foster, Lei Ding, Weitian Wang, Genevieve Stelmacovich, Feng-Yuan Zhang, Adam Paxson, Svitlana Pylypenko","doi":"10.1021/acsaem.6c02191","DOIUrl":"https://doi.org/10.1021/acsaem.6c02191","url":null,"abstract":"<p>This study examines the effects of post-treatment annealing (argon, vacuum, air; 200–500 °C) on electrodeposited IrRuO<sub>x</sub> porous transport electrodes (PTEs) using X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDS). The aim is to investigate how these treatments influence the material's composition, structure, and their respective impact on electrochemical properties. Electrochemical testing reveals atmosphere-dependent pathways: argon annealing improves stability up to 400 °C but produces Ir enrichment and heterogeneity at 500 °C that degrades performance; air annealing stabilizes oxidized species at 200 °C but yields larger activity and stability losses by 300 °C; and vacuum annealing at 200 °C preserves activity while improving stability. XPS characterization focuses on the analysis of Ir 4f, Ru 3d, and O 1s regions. For Ir 4f and Ru 3d spectra, simple metrics that didn’t involve fitting are explored, whereas for O 1s, deconvolution strategies are evaluated and a six-component model is adopted. In many cases, simple XPS metrics, binding energy (BE) and full width at half maximum (FWHM), capture trends that correlate with catalytic activity and stability, while detailed fitting is necessary to resolve complex oxygen speciation in other cases. Additionally, XPS-derived metrics are correlated with electrochemical performance using principal component analysis (PCA), highlighting patterns within a complex dataset. These results advance our understanding of XPS analysis of Ir-based catalysts, emphasize the importance of thorough and careful analysis, and highlight opportunities for combining simple metrics with multivariate analysis for the development of more efficient materials.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"13982–13995"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368548","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Umair Nisar, Nico Huijssen, Diana Chaykina, Fieke van den Bruele, Clementine Warres, Tarek Lutz, Margret Wohlfahrt-Mehrens, Markus Hölzle, Auke Kronemeijer, Peter Axmann, Marilena Mancini
{"title":"Elucidating the Role of sALD-Deposited ZrOx Coatings on the Electrochemical Performance of LiNi0.5Mn1.5O4 Cathodes","authors":"Umair Nisar, Nico Huijssen, Diana Chaykina, Fieke van den Bruele, Clementine Warres, Tarek Lutz, Margret Wohlfahrt-Mehrens, Markus Hölzle, Auke Kronemeijer, Peter Axmann, Marilena Mancini","doi":"10.1021/acsaem.6c02561","DOIUrl":"https://doi.org/10.1021/acsaem.6c02561","url":null,"abstract":"<p>LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> (LNMO) is a promising high-voltage, cobalt-free cathode material but suffers from severe interfacial degradation that limits the cycling stability of LNMO/graphite cells. Here, spatial atomic layer deposition (sALD) was employed to deposit conformal nano-ZrO<sub><em>x</em></sub> coatings directly onto LNMO composite electrodes, providing a scalable approach for electrode-level interface engineering. The influence of coating thickness and substrate translation speed on electrochemical performance was systematically investigated. Increasing the ZrO<sub><em>x</em></sub> thickness improved the long-term stability of LNMO/graphite cells but increased interfacial resistance, highlighting the trade-off between interfacial protection and charge-transfer kinetics. A ZrO<sub><em>x</em></sub> thickness of 3.0 nm provided the optimum balance, extending cell end-of-life by 71% compared with pristine LNMO while maintaining good rate capability. Post-mortem X-ray fluorescence analysis revealed reduced Mn and Ni deposition on graphite anodes, consistent with suppressed cathode–anode cross-talk. Furthermore, reducing the substrate translation speed from 10 to 5 mm s<sup>–1</sup> further increased the end-of-life of the LNMO/graphite cells by 51%. These results demonstrate that both coating thickness and sALD processing parameters are critical for developing durable, high-voltage LNMO/graphite cells.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"14422–14437"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368603","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Capacity–Retention Balance Determines Single-Crystal Payoff in Ni-Rich Cathodes","authors":"Zenghua Tian, Huazhang Zhou, Mingle Chu, Sainan Yao, Xudong Li, Yongming Zhu","doi":"10.1021/acsaem.6c03137","DOIUrl":"https://doi.org/10.1021/acsaem.6c03137","url":null,"abstract":"<p>Single crystallization is widely pursued to mitigate structural degradation in Ni-rich layered cathodes, yet its practical value remains difficult to define because improved durability can be accompanied by kinetic limitations and an initial-capacity penalty. Here, we establish a literature-derived quantitative framework that converts this long-standing trade-off into a measurable payoff criterion. Directly comparable polycrystalline–single-crystal cathode pairs from 12 datasets and 42 test contexts were evaluated through logarithmic response ratios describing initial-capacity, retention, and end-of-test capacity effects. Single-crystal cathodes showed higher retention in 67% of comparisons but higher initial capacity in only 19%, while 64% ultimately achieved a higher end-of-test capacity. These results identify compensation between early capacity sacrifice and durability gain as the central determinant of single-crystal benefit. Cross-dataset analysis further shows that this payoff is condition-dependent. The resulting break-even framework shifts single crystallization from a qualitative stability preference to a quantitative materials selection principle and offers a broader strategy for evaluating energy-storage materials in which long-term durability is gained at the expense of initial performance.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"14732–14739"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368619","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Oxygen Functionalization Enables Magnesium Storage in a TiC3 Monolayer: A First-Principles Study of Mg Adsorption and Migration","authors":"Jongee Park","doi":"10.1021/acsaem.6c02951","DOIUrl":"https://doi.org/10.1021/acsaem.6c02951","url":null,"abstract":"<p>Magnesium-ion batteries motivate the search for lightweight hosts with favorable storage energetics and accessible migration paths. We used density-functional theory to study Mg adsorption and migration on pristine and oxygen-functionalized TiC<sub>3</sub>. Adsorption on the pristine sheet is unfavorable relative to bulk Mg (+0.67 eV), whereas an isolated Mg atom binds at the B2 surface site of the partially oxidized sheet at –0.39 eV. For the sampled configurations, the PBE loading hull follows <em>n</em> = 0 → 1 → 4 → 12, where n is the number of Mg atoms in the Ti<sub>1</sub><sub>6</sub>C<sub>4</sub><sub>8</sub>O<sub>4</sub> cell. The <em>n</em> = 12 endpoint gives a theoretical host-mass capacity of 457 mAh g<sup>–1</sup>, with voltage plateaus of 0.358, 0.249, and 0.014 V. Dispersion-inclusive relaxation retains a positive <em>n</em> = 4 → 12 insertion voltage, although its value depends on the treatment. Seven-image CI-NEB calculations give dilute B2–B3 surface barriers of 0.699 eV for the O-adjacent P1 path and 1.074 eV for the surface-void P6 path. These results show how oxygen functionalization changes Mg adsorption and the local migration environment. The low anode voltage and moderate dilute migration barrier should be considered together when assessing this model host.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"14699–14709"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368644","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Hydrogen Evolution Performance of a Co-Doped MoNi4 Electrode Prepared by Laser Direct Writing Technology","authors":"Jiawei Dong, Wence Xu, Yanqin Liang, Zhonghui Gao, Hui Jiang, Zhaoyang Li, Ling Li, Dan Luo, Zhenduo Cui, Wei Li, Zhongwei Chen, Shengli Zhu","doi":"10.1021/acsaem.6c02673","DOIUrl":"https://doi.org/10.1021/acsaem.6c02673","url":null,"abstract":"<p>The alkaline hydrogen evolution reaction (HER) is a promising pathway for the large-scale production of green hydrogen. Due to the high water dissociation energy barrier in alkaline media, high energy consumption is required. In this work, a Co-doped MoNi<sub>4</sub> self-supported electrode (Co-MoNi<sub>4</sub>/NM) prepared by laser direct writing (LDW) is reported as an efficient electrocatalyst for HER. The introduction of Co hinders the long-range ordered growth of the MoNi<sub>4</sub> single phase, creating a MoNi<sub>4</sub>/Mo/Ni multiphase heterostructure with rich geometric defects. The electron-rich catalyst weakens the O–H bonds of water molecules, increasing the proportion of free water to provide reactants for subsequent water dissociation. As a result, Co-MoNi<sub>4</sub>/NM exhibits high HER catalytic performance with an overpotential of 131.2 mV at a current density of 100 mA cm<sup>–2</sup>. Under simulated industrial conditions (6 M KOH, 60 °C), the electrode demonstrates exceptional HER kinetics with a low overpotential of 227.8 mV at 1 A cm<sup>–2</sup> and robust chronopotentiometric durability for 100 h. Furthermore, the assembled two-electrode electrolyzer (Co-MoNi<sub>4</sub>/NM || Co-MoNi<sub>4</sub>/NM) delivers a high current density of 1 A cm<sup>–2</sup> at a low cell voltage of 1.74 V with long-term operational stability. This study elucidates the mechanism of interfacial water reconstruction driven by electronic modulation, offering a technological paradigm for developing highly efficient industrial-grade electrodes for hydrogen production.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"14491–14500"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368652","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Multiscale Design of Poly(ethylene oxide)-Based Composite Electrolyte: Enabling High Ionic Conductivity and Interfacial Stability for Lithium Metal Batteries","authors":"Biao Huang, Yongcheng Chen, Xinyi Zhou, Lixin Song, Chengcai Li, Guojin Liu, Hailin Zhu, Yuhai Guo","doi":"10.1021/acsaem.6c02536","DOIUrl":"https://doi.org/10.1021/acsaem.6c02536","url":null,"abstract":"<p>PEO-based solid-state electrolytes (PSEs) suffer from insufficient mechanical strength, low ionic conductivity, and poor interfacial stability, which severely undermines their feasibility for practical applications. The conventional approach of adding plasticizers to enhance ionic conductivity is often accompanied by a loss of mechanical strength and carries the risk of side reactions at the lithium metal interface. To address this contradiction, a multiscale engineering strategy is developed by incorporating coumarin into the PEO/LiTFSI/SN system and subsequently embedding the mixtures within a PTFE fibrous membrane to afford a structurally integrated electrolyte. At the macroscale, the PTFE rigid scaffold interpenetrates the electrolyte and reinforces it mechanically. At the microscale, the co-plasticization of PEO by SN and coumarin significantly reduces its crystallinity, thereby creating fast ion transport channels. At the nanoscale, coumarin acts as a sacrificial agent that induces the formation of a thin and uniform solid electrolyte interphase (SEI) on the lithium metal anode, thereby enhancing the interfacial stability. The resulting polymer electrolyte exhibits a maximum tensile strength of 9.7 MPa and a puncture resistance of 5.9 N, and delivers an optimized ionic conductivity of 0.79 × 10<sup>–3</sup> S cm<sup>–1</sup> at 60 °C. The Li∥Li symmetric cells based on this electrolyte demonstrate stable cycling for over 3200 cycles at current densities of 0.1 mA cm<sup>–2</sup>. Furthermore, the corresponding LiFePO<sub>4</sub>∥Li full cells achieve a high-capacity retention of 84.1% after 700 cycles at 0.5C. This study provides insights into multicomponent SSEs and an avenue to address the bottlenecks of solid-state Li-metal batteries.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 21","pages":"14338–14348"},"PeriodicalIF":5.5,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368653","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}