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Anion Concentration–Regulated Interface Stabilization Enabling High-Performance Lithium Metal Batteries 阴离子浓度调节界面稳定实现高性能锂金属电池
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-01-15 DOI: 10.1002/eem2.70266
Seung-Yeon Jung, Min-Jeong Yi, So Hee Kim, June Huh, Jiung Cho, Jong-Seong Bae, Seung-Ho Yu
{"title":"Anion Concentration–Regulated Interface Stabilization Enabling High-Performance Lithium Metal Batteries","authors":"Seung-Yeon Jung,&nbsp;Min-Jeong Yi,&nbsp;So Hee Kim,&nbsp;June Huh,&nbsp;Jiung Cho,&nbsp;Jong-Seong Bae,&nbsp;Seung-Ho Yu","doi":"10.1002/eem2.70266","DOIUrl":"https://doi.org/10.1002/eem2.70266","url":null,"abstract":"<p>Rechargeable Li metal batteries offer high energy density due to the high capacity and low reduction potential of Li metal anodes, but their practical application is hindered by dendritic growth that induces significant volume expansion, low Coulombic efficiency (CE), and safety risks. To address these challenges, we rationally designed an electrolyte based on a systematic investigation of the effect of anion-rich environments on interfacial stability. To specifically probe the role of anions, we employed a concentrated electrolyte system. Lithium bis(fluoromethanesulfonyl)imide (LiFSI) was selected as the lithium salt in combination with diethyl ether (DEE), a monodentate ether that reduces steric hindrance and promotes simplified solvation behavior. The optimized 6 <span>m</span> LiFSI-DEE electrolyte enabled Li symmetric and Li/Cu cells to cycle stably for over 1200 h at 0.5 mA c m<sup>−2</sup> and 1 mAh cm<sup>−2</sup>, demonstrating superior interfacial stability, a benefit that extended to Li/LFP full cells and Cu/LFP anode-less cells, both of which showed significantly improved cycling performance. The 6 <span>m</span> electrolyte promotes anion decomposition, forming a LiF-rich solid electrolyte interphase (SEI) that stabilizes the interface. In addition, the interfacial morphological evolution was directly visualized by <i>operando</i> optical microscopy and SEM, confirming a more uniform and compact Li deposition. These results highlight that anion concentration effectively modulates the Li<sup>+</sup> solvation environment and SEI chemistry, providing a robust design strategy for next-generation Li metal battery electrolytes.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70266","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Multifunctional Phosphorus Doping: Integrating Enhanced Ionic/Electronic Transport and Interface Optimization for Silicon Oxycarbide Anodes 多功能磷掺杂:集成增强离子/电子输运和界面优化碳化硅阳极
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-02-11 DOI: 10.1002/eem2.70301
Yingying Shen, Yun Zheng, Jiangmin Jiang, Yike Huang, Yinan Liu, Rong Chen, Pingshan Jia, Lifen Long, Congcong Zhang, Huaiyu Shao
{"title":"Multifunctional Phosphorus Doping: Integrating Enhanced Ionic/Electronic Transport and Interface Optimization for Silicon Oxycarbide Anodes","authors":"Yingying Shen,&nbsp;Yun Zheng,&nbsp;Jiangmin Jiang,&nbsp;Yike Huang,&nbsp;Yinan Liu,&nbsp;Rong Chen,&nbsp;Pingshan Jia,&nbsp;Lifen Long,&nbsp;Congcong Zhang,&nbsp;Huaiyu Shao","doi":"10.1002/eem2.70301","DOIUrl":"https://doi.org/10.1002/eem2.70301","url":null,"abstract":"<p>Polymer-derived silicon oxycarbide (SiOC) is a promising anode material for lithium-ion batteries due to its high specific capacity, low operating potential, structural stability, and tunable components. However, its practical application is hindered by poor intrinsic electronic/ionic conductivity and unstable solid-electrolyte interphase (SEI). Herein, in this work, a phosphorus (P)-doped SiOC material was successfully synthesized, and the P is incorporated into the SiOC network via P–O–Si bonding. This P-doping strategy introduced additional free electrons and enhanced the ordering of free-carbon phase. Also, it induced the formation of LiF and Li<sub>3</sub>PO<sub>4</sub>-rich SEI. These modifications collaboratively led to good rate performance and cycling stability. The optimized SiOC-P electrode delivered a high reversible capacity of 860.1 mAh g<sup>−1</sup>, an excellent capacity retention of 81.1% after 700 cycles at 1.0 A g<sup>−1</sup>, and a good rate capacity of 383.4 mAh g<sup>−1</sup> even at 5.0 A g<sup>−1</sup>. Density functional theory calculations also reveal that Si–O–P promotes the ionic/electronic transport among the SiOC-P bulk. This work offers valuable insights into heteroatom doping strategies for tailoring SiOC-based materials and facilitates their practical application in high-energy-density batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70301","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696294","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enabling High-Loading Aqueous Zinc–Sulfur Batteries Via a Ni Single-Atom Catalytic Host with Hierarchical Sulfur Reservoirs 通过具有分层硫储层的镍单原子催化载体实现高负载锌硫水溶液电池
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-02-16 DOI: 10.1002/eem2.70300
Zuoshu Wang, Xueyan Yang, Guochao Zhao, Dewei Wang, Yuhong Chen
{"title":"Enabling High-Loading Aqueous Zinc–Sulfur Batteries Via a Ni Single-Atom Catalytic Host with Hierarchical Sulfur Reservoirs","authors":"Zuoshu Wang,&nbsp;Xueyan Yang,&nbsp;Guochao Zhao,&nbsp;Dewei Wang,&nbsp;Yuhong Chen","doi":"10.1002/eem2.70300","DOIUrl":"https://doi.org/10.1002/eem2.70300","url":null,"abstract":"<p>Aqueous zinc–sulfur batteries have drawn considerable interest owing to their high theoretical capacity, intrinsic safety, and cost-effectiveness. Nevertheless, the sulfur cathode typically exhibits sluggish two-electron solid-state conversion reactions, resulting in a lower discharge voltage and inefficient sulfur utilization. Herein, we design a nickel single-atom-anchored on N-doped carbon hollow structure featuring an internal three-dimensional network-like skeleton as the sulfur host to address these issues. The nickel single-atom-anchored on N-doped carbon hollow structure synergistically combines atomic Ni-N<sub>4</sub> catalytic sites as well as a hollow structure possessing a high specific surface area and hierarchical nanopores. Consequently, the resulting S@Ni-SAs/NCHS achieves a high sulfur loading of ~74 wt% and a specific capacity of 1664.6 mAh g<sup>−1</sup> at 0.1 A g<sup>−1</sup> with a low polarization of 0.35 V. Besides, it maintains a capacity of 1154.4 mAh g<sup>−1</sup> at 5 A g<sup>−1</sup> and shows a retained capacity of 1038.6 mAh g<sup>−1</sup> after 1000 cycles at 2 A g<sup>−1</sup>, which corresponds to a decay rate of 0.03% per cycle. Density functional theory calculations reveal that the Ni-N<sub>4</sub> site serves as an efficient electron donor, facilitating charge transfer and reducing the energy barrier of the rate-determining step from 1.845 eV to 1.458 eV. Furthermore, a pouch cell with a high areal sulfur loading demonstrates specific capacities of 1200–1400 mAh g<sup>−1</sup> under various bending states with discharge plateaus about 0.8 V, retaining 83.4% capacity after 200 cycles. This work underscores the critical role of integrating Ni atomic catalysis with well-developed porosity within the carbon hollow structure for developing high-performance aqueous zinc–sulfur batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70300","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696545","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Activating and Stabilizing Lattice Oxygen in Spinel NiCo2O4 through F, Mn Dual Doping for Rechargeable Zinc–Air Batteries 可充电锌-空气电池用F、Mn双掺杂活化和稳定尖晶石NiCo2O4中晶格氧
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-01-18 DOI: 10.1002/eem2.70259
Jitong Li, Lifei Qu, Dongxu Yang, Haosheng Zhu, Hongwei Li, Yongcheng Li, Riming Hu, Peng Zhang, Benhua Xu
{"title":"Activating and Stabilizing Lattice Oxygen in Spinel NiCo2O4 through F, Mn Dual Doping for Rechargeable Zinc–Air Batteries","authors":"Jitong Li,&nbsp;Lifei Qu,&nbsp;Dongxu Yang,&nbsp;Haosheng Zhu,&nbsp;Hongwei Li,&nbsp;Yongcheng Li,&nbsp;Riming Hu,&nbsp;Peng Zhang,&nbsp;Benhua Xu","doi":"10.1002/eem2.70259","DOIUrl":"https://doi.org/10.1002/eem2.70259","url":null,"abstract":"<p>The oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are critical to the charge/discharge performance of zinc–air batteries (ZABs). The slow reaction kinetics of OER significantly limit the performance improvement of ZABs. Herein, an ingenious dual-doping strategy was devised, wherein Mn atoms substituted some of the metal ions in NiCo<sub>2</sub>O<sub>4</sub> to induce lattice distortion and generate oxygen vacancies. F atoms were then substituted into these vacancies to synthesize NiMn<sub>0.075</sub>Co<sub>2</sub>O<sub>4-X</sub>F<sub>X</sub>. By activating and stabilizing lattice oxygen, stable synergistic effects between adsorbate evolution mechanism (AEM) and lattice oxygen mechanism (LOM) are achieved. Without generating any active impurity phases, the intrinsic activity of the catalyst was enhanced. Electrochemical tests exhibit that NiMn<sub>0.075</sub>Co<sub>2</sub>O<sub>4-X</sub>F<sub>X</sub> presents a small Tafel slope of 62.80 mV·dec<sup>−1</sup>, low overpotential of 321 mV at 10 mA·cm<sup>−2</sup> for the OER, which is superior to that of the commercial RuO<sub>2</sub> catalyst. Furthermore, the ZABs assembled by the optimal catalyst (NiMn<sub>0.075</sub>Co<sub>2</sub>O<sub>4-X</sub>F<sub>X</sub>) deliver a peak power density of 257.6 mW·cm<sup>−2</sup>, which exceeds that of the conventional Pt/C + RuO<sub>2</sub> catalyst. In situ test results indicate that the dual-doping strategy effectively activates lattice oxygen, reducing the voltage required to generate the surface active phase during the OER. Theoretical calculations demonstrate that this dual-element doping strategy shifts the O-2p band center toward the Fermi level and enhances hybridization of the metal 3d orbitals, promoting the evolution of AEM toward LOM. This work provides a strategic research for precisely regulating catalysts to enhance the intrinsic activity.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70259","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696582","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Design of High-Performance MnCo1.5Cu0.5O4 Spinel Contact Material with Optimized Electrical Conductivity and Thermal Stability for Solid Oxide Electrolysis Cells by Cu Doping Cu掺杂固体氧化物电解电池中高性能MnCo 1.5 Cu 0.5 O 4尖晶石触点材料的优化电导率和热稳定性
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-01-05 DOI: 10.1002/eem2.70220
Haozhen Li, Shuai Yuan, Xingtong Mao, Hao Shi, Hengyong Tu, Chao Ma, Lei Zhu, Zhen Huang
{"title":"Design of High-Performance MnCo1.5Cu0.5O4 Spinel Contact Material with Optimized Electrical Conductivity and Thermal Stability for Solid Oxide Electrolysis Cells by Cu Doping","authors":"Haozhen Li,&nbsp;Shuai Yuan,&nbsp;Xingtong Mao,&nbsp;Hao Shi,&nbsp;Hengyong Tu,&nbsp;Chao Ma,&nbsp;Lei Zhu,&nbsp;Zhen Huang","doi":"10.1002/eem2.70220","DOIUrl":"10.1002/eem2.70220","url":null,"abstract":"<p>As promising contact material candidates in solid oxide cells, spinel-type MnCo<sub>2-x</sub>Cu<sub>x</sub>O<sub>4</sub> (0 ≤ x ≤ 0.5) and Cu<sub>1.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> powders were synthesized via sol–gel and co–precipitation methods to investigate the effects of Cu doping on electrical and structural properties. Cu substitution introduced additional variable-valent cations and elevated Mn oxidation state via charge compensation. This valence modulation promoted electron hopping between abundant Mn<sup>4+</sup>/Mn<sup>3+</sup> and Cu<sup>2+</sup>/Cu<sup>+</sup> redox pairs, leading to higher electrical conductivity. Cu doping also reduced lattice rigidity, as evidenced by increased thermal expansion coefficients. After 1000-h aging at 850 °C in air, a multi-layer assembly with MnCo<sub>1.5</sub>Cu<sub>0.5</sub>O<sub>4</sub> as contact layer exhibited a stable area-specific resistance (ASR) value of ~10 mΩ cm<sup>2</sup> and good compatibility with MnCo<sub>2</sub>-coated SUS441 interconnects. Post-mortem analysis revealed that the resistance was mainly attributed to a well-defined Cr oxide interlayer. Though Cu<sub>1.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> contact layer led to a thinner oxide scale, continuous Cr outward diffusion may deteriorate the cell performance. Finally, MnCo<sub>1.5</sub>Cu<sub>0.5</sub>O<sub>4</sub> was applied to a single-cell stack under H<sub>2</sub>O/CO<sub>2</sub> co-electrolysis operation for 600 h and achieved an electrolysis voltage of ~1.3 V at a current density of 0.4 A cm<sup>−2</sup>. Overall, Cu-doped Mn-Co spinels demonstrate great potential as highly conductive contact materials with tunable thermal properties for solid oxide electrolysis cell applications.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70220","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147913432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Crystal Orientation Regulation and Dynamic Protection via Dual Interface Engineering for Dendrite-Free Zinc Deposition 基于双界面工程的无枝晶锌沉积晶体取向调节与动态保护
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-02-15 DOI: 10.1002/eem2.70306
Xin Wu, Ruiqian Li, Yujie Cao, Zixian Zhu, Zhengye Yang, Menghao Xia, Hongwei Kang, Huizhu Yu, Rencheng Jin
{"title":"Crystal Orientation Regulation and Dynamic Protection via Dual Interface Engineering for Dendrite-Free Zinc Deposition","authors":"Xin Wu,&nbsp;Ruiqian Li,&nbsp;Yujie Cao,&nbsp;Zixian Zhu,&nbsp;Zhengye Yang,&nbsp;Menghao Xia,&nbsp;Hongwei Kang,&nbsp;Huizhu Yu,&nbsp;Rencheng Jin","doi":"10.1002/eem2.70306","DOIUrl":"https://doi.org/10.1002/eem2.70306","url":null,"abstract":"<p>The rampant dendrite and parasitic reactions in aqueous zinc-ion batteries seriously hinder its practical application. Herein, a novel organic/inorganic dual interface layer is developed by in-situ constructing of zinc hydroxide sulfate hydrate (ZHS) under the induction of a di-pentaerythritol (DPE) pre-coating. This design achieves dendrite-free Zn deposition through the synergistic integration of crystallographic orientation regulation and dynamic self-adaptive protection. The crystallographic orientation includes two dimensions: 1) Hydrogen-bond-guided horizontal growth of zinc hydroxide sulfate hydrate (ZHS) along the (001) crystal plane, and 2) ZHS-induced epitaxial alignment of Zn deposition on the (002) plane. This dual crystallographic modulation achieves uniform interfacial ion flux distribution and suppresses the formation of dendrites. Simultaneously, the dynamic evolution of the DPE/ZHS interphase adaptively alleviates mechanical stress during plating/stripping cycles, ensuring conformal interfacial contact and effectively mitigating water-induced side reactions. As a result, the engineered Zn anode exhibits exceptional cycling stability, surpassing 4500 h at 1 mA cm<sup>−2</sup> with a coulombic efficiency of 99.79%, while full cells paired with V<sub>2</sub>O<sub>5</sub> cathodes retain nearly 100% capacity after 3000 cycles at 5 A g<sup>−1</sup>. This work provided a novel perspective on regulating interfacial byproducts to stabilize Zn anodes.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70306","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696078","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Contaminant-to-Protection: In Situ Built Tri-Component Barrier Enables Ultralong-Cycling NASICON-Based Sodium Metal Batteries 污染物到保护:原位构建的三组分屏障使nasicon基钠金属电池能够超长循环
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-01-19 DOI: 10.1002/eem2.70273
Wenhao Tang, Ao Li, Zhengyang Wu, Shiyue Li, Ruiping Liu
{"title":"Contaminant-to-Protection: In Situ Built Tri-Component Barrier Enables Ultralong-Cycling NASICON-Based Sodium Metal Batteries","authors":"Wenhao Tang,&nbsp;Ao Li,&nbsp;Zhengyang Wu,&nbsp;Shiyue Li,&nbsp;Ruiping Liu","doi":"10.1002/eem2.70273","DOIUrl":"https://doi.org/10.1002/eem2.70273","url":null,"abstract":"<p>NASICON-type Na<sub>3</sub>Zr<sub>2</sub>Si<sub>2</sub>PO<sub>12</sub> (NZSP) is a promising electrolyte for solid-state sodium battery due to its high ionic conductivity and wide electrochemical window. Unfortunately, the sodiophobicity of NZSP leads to extremely poor interfacial contact, which represents a substantial hindrance to its practical application. Herein, a “one stone two birds” strategy is proposed to decompose the contamination layer of NZSP and form a super-sodiophilic and electron-blocking hybrid interlayer consisting of Na<sub>3</sub>Sb alloy, NaCl and Na<sub>2</sub>O. The hybrid interlayer can not only improve the wettability of NZSP to Na and promote the rapid migration of Na<sup>+</sup> ions, but also effectively prevent the electron from intruding into the electrolyte at the interface and inhibit the growth of dendrites. Consequently, a dendrite-free sodium plating/stripping can be achieved even at critical current densities as high as 1.4 mA cm<sup>−2</sup> and the sodium symmetric cell can be stably cycled for more than 3600 h at 0.5 mA cm<sup>−2</sup>/0.5 mAh cm<sup>−2</sup>. In addition, the solid-state full cell coupled with the Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode delivers capacities of 103.3 mAh g<sup>−1</sup> under 0.5 C for 300 cycles at room temperature. This work offers an effective and innovative strategy to address the interfacial issues of solid-state sodium metal batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70273","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696422","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Toward Safer and Sustainable Lithium Metal Batteries: Fluorine-Free Solid Polymer Electrolytes 迈向更安全和可持续的锂金属电池:无氟固体聚合物电解质
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-01-30 DOI: 10.1002/eem2.70271
David Fraile-Insagurbe, Leire Meabe, Brigette Althea Fortuin, Itsaso Segura-Laparra, Elene Sasieta-Barrutia, Rosalía Cid, Javier Carrasco, Władysław Wieczorek, Maria Forsyth, Michel Armand, María Martínez-Ibañez
{"title":"Toward Safer and Sustainable Lithium Metal Batteries: Fluorine-Free Solid Polymer Electrolytes","authors":"David Fraile-Insagurbe,&nbsp;Leire Meabe,&nbsp;Brigette Althea Fortuin,&nbsp;Itsaso Segura-Laparra,&nbsp;Elene Sasieta-Barrutia,&nbsp;Rosalía Cid,&nbsp;Javier Carrasco,&nbsp;Władysław Wieczorek,&nbsp;Maria Forsyth,&nbsp;Michel Armand,&nbsp;María Martínez-Ibañez","doi":"10.1002/eem2.70271","DOIUrl":"https://doi.org/10.1002/eem2.70271","url":null,"abstract":"<p>Fluorinated compounds have long played a key role in solid-state lithium metal polymer batteries (SSLMPBs). Yet, growing environmental and safety concerns associated with fluorine have intensified the search for safer and more sustainable alternatives. Cyano-substituted imidazoles have recently emerged as promising candidates to replace conventional sulfonyl imide-based anions, offering efficient charge delocalization and the potential to form fluorine-free anions. In this work, we introduce lithium 2,4,5-tricyanoimidazolide (LiTIM), a fluorine-free lithium salt, as a component of a solid polymer electrolyte (SPE) based on poly(ethylene oxide) (PEO) and as a catholyte in LiFePO<sub>4</sub> (LFP)-based cathodes. To assess the impact of fluorine, LiTIM is compared to its fluorinated analogues: lithium 4,5-dicyano-2-(trifluoromethyl)imidazole (LiTDI) and lithium 4,5-dicyano-2-(pentafluoroethyl)imidazole (LiPDI). In-depth physicochemical and electrochemical characterization reveals that LiTIM exhibits competitive lithium diffusion coefficient (<i>D</i><sub>Li+</sub>, at 40 °C, <i>D</i><sub>Li+</sub> (LiTIM) = 5.2 × 10<sup>−9</sup> cm<sup>2</sup> s<sup>−1</sup> &gt; <i>D</i><sub>Li+</sub> (LiPDI/PEO) = 1.7 × 10<sup>−9</sup> cm<sup>2</sup> s<sup>−1</sup> &gt; <i>D</i><sub>Li</sub><sup>+</sup> (LiTDI/PEO) = 1.4 × 10<sup>−9</sup> cm<sup>2</sup> s<sup>−1</sup>) and full cell performance (capacity retention at C/5, after 200 cycles (LiTIM/PEO = 92% &gt; LiTDI/PEO = 88% &gt; LiPDI/PEO = 82%)) comparable to that of its fluorinated counterparts. This is primarily attributed to its restricted anion mobility (<i>D</i><sub>anion</sub> (LiTIM/PEO) = 1.1 × 10<sup>−8</sup> cm<sup>2</sup> s<sup>−1</sup> &lt; <i>D</i><sub>anion</sub> (LiPDI/PEO) = 1.6 × 10<sup>−8</sup> cm<sup>2</sup> s<sup>−1</sup> ≈ <i>D</i><sub>anion</sub> (LiTDI/PEO) = 1.7 × 10<sup>−8</sup> cm<sup>2</sup> s<sup>−1</sup>) and competitive LiCN-based solid electrolyte interphase (SEI) layer formation. These findings highlight the viability of LiTIM as a nonfluorinated salt for SSLMPBs, offering a pathway toward more sustainable, environmentally friendly, and safer battery technologies.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70271","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696515","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Entropy-Driven Innovations: Entropy Stabilized Oxides for High-Performance Next-Generation Lithium–Sulfur Batteries 熵驱动创新:用于高性能下一代锂硫电池的熵稳定氧化物
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2026-03-03 DOI: 10.1002/eem2.70297
Hassan Raza, Jialiang Wei, Zhicai Wang, Zhaoyang Lv, Junye Cheng, Jia Xu, Liang An, Yuliang Liu, Sergey Ryazantsev, Shukui Li, Guangping Zheng
{"title":"Entropy-Driven Innovations: Entropy Stabilized Oxides for High-Performance Next-Generation Lithium–Sulfur Batteries","authors":"Hassan Raza,&nbsp;Jialiang Wei,&nbsp;Zhicai Wang,&nbsp;Zhaoyang Lv,&nbsp;Junye Cheng,&nbsp;Jia Xu,&nbsp;Liang An,&nbsp;Yuliang Liu,&nbsp;Sergey Ryazantsev,&nbsp;Shukui Li,&nbsp;Guangping Zheng","doi":"10.1002/eem2.70297","DOIUrl":"https://doi.org/10.1002/eem2.70297","url":null,"abstract":"<p>Lithium–sulfur batteries are known as promising next-generation energy storage devices owing to their elevated theoretical energy density (∼2600 W h kg<sup>−1</sup>), cost-effectiveness, and environmental sustainability. Nonetheless, the issues of lithium polysulfide shuttle effect, considerable volume expansion, inadequate electrical conductivity, and slow redox kinetics have hindered their practical application. The use of high-entropy-stabilized oxides consisting of numerous different chemical elements that provide phase stabilization by a high configurational entropy presents an innovative and efficient approach to resolve these issues of lithium–sulfur batteries. Meanwhile, understanding of the unique properties and versatile applications of entropy-driven phases remain incomplete. This review not only offers a comprehensive examination on the entropy-driven phase structures of high-entropy-stabilized oxides but also highlights their application in improving the efficacy of sulfur composite cathodes in lithium–sulfur batteries batteries. The structural and electrochemical benefits of different types of high-entropy-stabilized oxides for use in lithium–sulfur batteries batteries are analyzed, elucidating their roles in enhancing sulfur usage, mitigating shuttle effects, and facilitating stable cycling. The analysis delineates prospective avenues in the synthesis, characterization, and system integration of lithium–sulfur batteries batteries, expediting the commercialization of high-entropy-stabilized oxide-based lithium–sulfur batteries battery technology.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70297","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696090","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
ZnO-Coated Silicon Oxide Nano-Anode: Synergistic Enhancement of Cycling and Thermal Stability of Lithium-Ion Batteries zno包覆氧化硅纳米阳极:协同增强锂离子电池的循环和热稳定性
IF 13.8 2区 材料科学
Energy & Environmental Materials Pub Date : 2026-08-06 Epub Date: 2025-08-28 DOI: 10.1002/eem2.70126
Keren Shi, Wende Yi, Weikang Su, Qiaowei Xiao, Ziyan Wang, Xiaoyu Li, Jingyang Mu, Wufei Tang, Zhihan Peng, Huiqin Yao
{"title":"ZnO-Coated Silicon Oxide Nano-Anode: Synergistic Enhancement of Cycling and Thermal Stability of Lithium-Ion Batteries","authors":"Keren Shi,&nbsp;Wende Yi,&nbsp;Weikang Su,&nbsp;Qiaowei Xiao,&nbsp;Ziyan Wang,&nbsp;Xiaoyu Li,&nbsp;Jingyang Mu,&nbsp;Wufei Tang,&nbsp;Zhihan Peng,&nbsp;Huiqin Yao","doi":"10.1002/eem2.70126","DOIUrl":"https://doi.org/10.1002/eem2.70126","url":null,"abstract":"<p>Silicon oxide (SiO) has great potential as a high-capacity anode for lithium-ion batteries, but its practical use is limited by excessive volume expansion (&gt;200%) and rapid capacity fade, especially at high temperatures. Traditional strategies, like carbon coating and nanostructuring, only partially address these issues. This study introduces a novel approach by synthesizing porous SiO microspheres encapsulated within a conformal ZnO shell (MS-ZnO). The internal porosity absorbs volumetric strain, while the ZnO shell provides mechanical stability, preventing electrode disintegration. MS-ZnO (M-Z: Zinc oxide coating on SiO) shows significantly reduced swelling (32.4% vs 94.8% for ZnO unmodified SiO (P-M)) and a high reversible capacity of 978.65 mAh g<sup>−1</sup> after 500 cycles, double that of unmodified SiO. At 90 °C, MS-ZnO maintains a stable Coulombic efficiency of ~75%, compared with ~32% for unmodified SiO, indicating excellent thermal stability. In full-cell tests with LiFePO<sub>4</sub>, MS-ZnO delivers 151 mAh g<sup>−1</sup> at 0.2C with 83.5% capacity retention after 100 cycles. GITT and DFT analysis reveal that the ZnO shell enhances Li<sup>+</sup> diffusion and mechanical strength. This work presents ZnO encapsulation as a transformative strategy to overcome volume change and thermal instability, unlocking the potential of SiO anodes for high-performance, high-safety lithium-ion batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"9 5","pages":""},"PeriodicalIF":13.8,"publicationDate":"2026-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70126","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148696474","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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