Angewandte Chemie International Edition最新文献_第7页

Fast-Charging Hard Carbons: A Fully Organic SEI Enables Low-Coordination Interfacial Environments and Fast Na+ Desolvation. 快速充电硬碳：全有机SEI实现低配位界面环境和快速Na+脱溶。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202516068

Yi Zhang,Da Tie,Zhiyong Xiong,Xiaodong Lin,Shuo Liu,Qihang Tan,Alexandru Vlad,Maowen Xu,Yong-Sheng Hu,Yuruo Qi

{"title":"Fast-Charging Hard Carbons: A Fully Organic SEI Enables Low-Coordination Interfacial Environments and Fast Na+ Desolvation.","authors":"Yi Zhang,Da Tie,Zhiyong Xiong,Xiaodong Lin,Shuo Liu,Qihang Tan,Alexandru Vlad,Maowen Xu,Yong-Sheng Hu,Yuruo Qi","doi":"10.1002/anie.202516068","DOIUrl":"https://doi.org/10.1002/anie.202516068","url":null,"abstract":"Fast-charging capability becomes a critical bottleneck for the practical deployment of sodium-ion batteries (SIBs), particularly due to sluggish Na+ desolvation and interfacial transport at hard carbon (HC) anodes. Herein, we present a comprehensive study on Na+ desolvation and transport kinetics across solid electrolyte interphases (SEIs) with diverse chemical natures. Although inorganic-rich SEIs are generally regarded as favorable for Na+ transport, our results reveal that certain organic-rich SEIs can deliver comparable or even superior kinetic performance. Guided by these insights, we construct a Poly(MMA)-based artificial SEI on commercial HC (Type-1), which reorganizes the Na+-DME solvation shell at the inner Helmholtz plane into a Na+-DME/Poly(MMA) coordination environment. This interfacial reconstruction markedly enhances Na+ desolvation and interphase transport, enabling exceptional rate performance (236 mA h g-1 at 5 C) and long-term cycling stability (99% capacity retention over 1000 cycles) for the commercial Type-1 HC. The effectiveness of the Poly(MMA)-derived interphase is further validated in both coin-type and pouch-type full sodium-ion chemistries, as well as in lithium-ion batteries. This work unveils the pivotal role of interfacial solvation structure, beyond the organic/inorganic ratios of SEI, in governing Na+ kinetics, offering a new design paradigm for next-generation fast-charging SIBs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"129 1","pages":"e202516068"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331892","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Two-Stage Catalytic Conversion of Carbon Dioxide Into Aromatics Via Methane. 甲烷催化二氧化碳两段转化为芳烃的研究。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202517563

Josepha J G Kromwijk,Angela E M Melcherts,Luke de Jong,Jules F van Leusden,Joris C L Janssens,Ramon Oord,Ward van der Stam,Matteo Monai,Bert M Weckhuysen

{"title":"Two-Stage Catalytic Conversion of Carbon Dioxide Into Aromatics Via Methane.","authors":"Josepha J G Kromwijk,Angela E M Melcherts,Luke de Jong,Jules F van Leusden,Joris C L Janssens,Ramon Oord,Ward van der Stam,Matteo Monai,Bert M Weckhuysen","doi":"10.1002/anie.202517563","DOIUrl":"https://doi.org/10.1002/anie.202517563","url":null,"abstract":"In the refinery of the future, the input shifts from crude oil to biomass, plastic, and CO2. Therefore, we need to find alternative routes to produce chemical building blocks, such as aromatics, which are used in products like, for example, fuels. In this study, we investigated a two-stage route to produce benzene from CO2. In two sequential reactions, CO2 is first converted into methane over a Ni/TiO2 catalyst, and methane is further reacted to yield benzene using a Mo/ZSM-5 catalyst via the methane dehydroaromatization (MDA) reaction. Through a combination of thermodynamic calculations and experiments, we found the goldilocks conditions for performing this two-stage process. The unreacted CO2 and H2 from the first reaction extended the benzene production in the second reaction. Using a reaction mixture of CO2, H2, and CH4 resulted in benzene production of at least 72 h, by suppressing carbon growth on the catalyst surface. However, the concentration range in which CO2 and H2 can be added to the feed without losing benzene production is narrow, as we show with H2 fluctuation experiments. We demonstrate that the combination of CO2 methanation and MDA allows us to catalytically convert CO2 into benzene with an overall yield of 5%.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"34 1","pages":"e202517563"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331748","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Gas-Proton Microenvironment Modulation for Enhanced CO2-to-Formate Electroreduction. 气体-质子微环境调制增强co2 -to-甲酸电还原。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202516163

Jifeng Wu,Yu Li,Miao Hu,Tingsong Li,Moyu Yi,Xiangyun Xiao,Honglin Li,Yongfeng Guo,Yoji Kobayashi,Magnus Rueping,Wan-Lu Li,Huabin Zhang,Kuo-Wei Huang

{"title":"Gas-Proton Microenvironment Modulation for Enhanced CO2-to-Formate Electroreduction.","authors":"Jifeng Wu,Yu Li,Miao Hu,Tingsong Li,Moyu Yi,Xiangyun Xiao,Honglin Li,Yongfeng Guo,Yoji Kobayashi,Magnus Rueping,Wan-Lu Li,Huabin Zhang,Kuo-Wei Huang","doi":"10.1002/anie.202516163","DOIUrl":"https://doi.org/10.1002/anie.202516163","url":null,"abstract":"Precise control of interfacial water structure is essential for suppressing side reactions and enabling selective CO2 electroreduction at industrial current densities. Here, we synthesize a series of bismuth-based catalysts with spatially encoded superhydrophilic-superhydrophobic nanodomains by partially embedding polyvinylidene fluoride (PVDF) into Bi nanoparticles. This strategy creates interfacial polarity patterns that stabilize *OCHO intermediates while suppressing hydrogen and CO evolution. Compared to the PVDF-free control, the optimized Bi-PVDF catalyst exhibits significantly enhanced formate partial current density, Faradaic efficiency (FE), and long-term stability. It achieves > 90% FE at -200 mA cm-2 for 50 h and maintains high selectivity up to -700 mA cm-2. Operando spectroscopy and multiscale simulations reveal that the dual-wettability interface modulates local hydration and charge distribution, promoting selective intermediate formation while kinetically suppressing side pathways. By addressing the longstanding challenge of coupled gas-proton transport, this work offers a mechanism-driven and scalable strategy to construct interfacial microenvironments for high-rate, selective CO2 electroreduction.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"101 1","pages":"e202516163"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145338574","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Post-Selenium-Leaching Induced Fast Micro-Bubble Detachment on Nickel-Iron-Based OER Catalyst for Efficient AEM-WE. 硒浸出后诱导镍-铁基OER催化剂上的快速微泡剥离

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202517132

Shiwen Ding,Zhiheng Li,Gaoxin Lin,Yunxuan Ding,Linqin Wang,Licheng Sun

{"title":"Post-Selenium-Leaching Induced Fast Micro-Bubble Detachment on Nickel-Iron-Based OER Catalyst for Efficient AEM-WE.","authors":"Shiwen Ding,Zhiheng Li,Gaoxin Lin,Yunxuan Ding,Linqin Wang,Licheng Sun","doi":"10.1002/anie.202517132","DOIUrl":"https://doi.org/10.1002/anie.202517132","url":null,"abstract":"Developing efficient and durable oxygen evolution reaction (OER) catalysts is critical for advancing anion exchange membrane water electrolysers (AEM-WE) for green hydrogen production driven by solar or wind power. This study explored the impact of the selenium (Se) modification on the OER performance of nickel-iron layered double hydroxide-based catalysts (i.e., NiFeSe), focusing on micro-bubble formation/detachment and its role in optimizing mass transport. The introduction of Se influenced the surface and interface properties of the NiFeSe, including enhanced surface roughness, facilitated rapid nucleation and detachment of smaller oxygen bubbles, and reduced bubble-induced diffusion limitations. As a result, the NiFeSe catalyst achieved a low overpotential of 190 mV at 1000 mA cm-2 and demonstrated a high durability beyond 2000 h in 1 M KOH. In the practical AEM-WE device, it reached 8800 mA cm-2 at 2.0 V and worked continuously for over 3000 h at 1000 mA cm-2. These findings highlight the crucial role of selenium-induced micro-bubble formation/detachment in improving mass transport and catalytic efficiency, providing new insights for next-generation OER catalysts in industrial water electrolysis.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"27 1","pages":"e202517132"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145338553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Metastable Crystalline Cobalt Iron Oxide Nano-Flakes with Antiferromagnetic/Ferrimagnetic Composition Mosaicity. 具有反铁磁/铁磁成分嵌合性的亚稳晶体氧化钴铁纳米片。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202504171

Anna Rabe,Franz-Philipp Schmidt,Shohreh Rafiezadeh,Soma Salamon,Joachim Landers,Mirco Eckhardt,Christoph Pratsch,Benedikt Beckmann,Felix Thomas Haase,David Kordus,Mauricio Lopez Luna,Clara Rettenmaier,Thomas Götsch,Axel Knop-Gericke,Arno Bergmann,Janis Timoshenko,Beatriz Roldan Cuenya,Oliver Gutfleisch,Mirijam Zobel,Rossitza Pentcheva,Heiko Wende,Thomas Lunkenbein,Malte Behrens

{"title":"Metastable Crystalline Cobalt Iron Oxide Nano-Flakes with Antiferromagnetic/Ferrimagnetic Composition Mosaicity.","authors":"Anna Rabe,Franz-Philipp Schmidt,Shohreh Rafiezadeh,Soma Salamon,Joachim Landers,Mirco Eckhardt,Christoph Pratsch,Benedikt Beckmann,Felix Thomas Haase,David Kordus,Mauricio Lopez Luna,Clara Rettenmaier,Thomas Götsch,Axel Knop-Gericke,Arno Bergmann,Janis Timoshenko,Beatriz Roldan Cuenya,Oliver Gutfleisch,Mirijam Zobel,Rossitza Pentcheva,Heiko Wende,Thomas Lunkenbein,Malte Behrens","doi":"10.1002/anie.202504171","DOIUrl":"https://doi.org/10.1002/anie.202504171","url":null,"abstract":"By thermal decomposition of a crystalline hydroxycarbonate precursor with a Co:Fe ratio of 2:1, crystals with alternating ferrimagnetic and antiferromagnetic nano-domains were synthesized using a facile synthetic approach that combined bottom-up co-precipitation of the precursor with a self-assembled top-down nano-structuring during spinel formation. Due to the miscibility gap of the spinel phase diagram at this composition, a topotactic segregation into CoFe2O4-like and Co3O4-like domains takes place at 400 °C, giving rise to porous crystalline nano-flakes with spatial compositional fluctuations on a scale of approximately 5 nm. Experimental methods and density functional theory showed that the metastable nature of this interface-rich material is manifested in the unexpectedly low lattice parameter of the iron-rich domains, which can be explained by the compressive strain executed on this phase due to mosaicity. Investigations of the magnetic properties revealed an exchange bias effect, due to this unique microstructure, which is typically known for thin films or core/shell nanoparticles. Treatment at temperatures higher than 450 °C causes this microstructure to break down, the lattice strain to relax, and finally leads to properties expected for the thermodynamically stable phases according to the phase diagram.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"27 1","pages":"e202504171"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331844","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Catalytic Nano-Reactor Engineering of Metal Single-Atom Site and Metal-Free Chemical Group for Accelerating Sulfur Redox Electrocatalysis. 加速硫氧化还原电催化的金属单原子位和无金属化学基团催化纳米反应器工程。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202517190

Shengjie Wei,Xingxin Hu,Rongyan Yang,Baixiong Liu,Qi Kang,Xijun Wang,Yuxiang Hu

{"title":"Catalytic Nano-Reactor Engineering of Metal Single-Atom Site and Metal-Free Chemical Group for Accelerating Sulfur Redox Electrocatalysis.","authors":"Shengjie Wei,Xingxin Hu,Rongyan Yang,Baixiong Liu,Qi Kang,Xijun Wang,Yuxiang Hu","doi":"10.1002/anie.202517190","DOIUrl":"https://doi.org/10.1002/anie.202517190","url":null,"abstract":"Precisely constructing atomic engineering of catalytic site and thus accelerating sulfur redox kinetics are meaningful but challenging for energy storage and conversion. Herein, the catalytic nano-reactor engineering containing Fe-N4 catalytic site and the adjacent PO chemical group as synergistic catalytic site (Fe-N4/CNPO) was first designed for Li-S batteries with remarkably improved performance. The adjacent PO chemical group of Fe-N4 site in catalytic nano-reactor simultaneously strengthened the adsorption of lithium polysulfides and facilitated the fracture of Li─S bonds by Li─O interaction, thus lowering the free energy change of potential-determining step and accelerating sulfur redox kinetics, which was further verified via density functional theory calculation. The optimized Fe-N4/CNPO modified separator exhibited much higher battery capacity of 1322.1 mAh g-1 at 0.2 C and enhanced long-term stability (low capacity decay of 0.08% per cycle over 500 cycles at 1.0 C). This work demonstrated the enormous potentiality of catalytic nano-reactor engineering containing metal single-atom catalytic site and chemical group as synergistic catalytic site for accelerating sulfur redox in metal-sulfur batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"56 1","pages":"e202517190"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331902","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Light-Induced Chemiluminescence Microscopy for Imaging Heterogeneous Photo-Fenton-Type Activity on Individual Hematite Photocatalysts. 光致化学发光显微镜研究单个赤铁矿光催化剂的非均相光芬顿型活性。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202509277

Taeyoon Kim,Joohoon Kim

引用次数: 0

A General Strategy to Develop Intramolecular Spirocyclic Boron Dipyrromethene Fluorophores for Self-Blinking Super-Resolution Imaging. 分子内螺旋体环硼二硝基甲基荧光团自闪烁超分辨率成像的一般策略。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202518973

Huiquan Zuo,Yiran Liu,Long Wang,Ruotong Li,Xing Guo,Luying Guo,Heng Li,Maoguo Li,Xinfu Zhang,Lijuan Jiao,Yi Xiao,Erhong Hao

{"title":"A General Strategy to Develop Intramolecular Spirocyclic Boron Dipyrromethene Fluorophores for Self-Blinking Super-Resolution Imaging.","authors":"Huiquan Zuo,Yiran Liu,Long Wang,Ruotong Li,Xing Guo,Luying Guo,Heng Li,Maoguo Li,Xinfu Zhang,Lijuan Jiao,Yi Xiao,Erhong Hao","doi":"10.1002/anie.202518973","DOIUrl":"https://doi.org/10.1002/anie.202518973","url":null,"abstract":"Intramolecular spirocyclic fluorophores, with their controllable on-off switching, have enabled diverse stimuli-responsive probes and serve as cornerstones of self-blinking super-resolution imaging. However, their design has been largely restricted to Rhodamine frameworks, while boron dipyrromethene (BODIPY) dyes, renowned for their superior photostability, brightness, and near-infrared tunability, remain underutilized due to the inherent rigidity of the indacene core. To overcome this limitation, we developed a general molecular engineering strategy to confer BODIPY with spirocyclic functionality: Introducing 2-(hydroxymethyl)phenyl or 2-carboxyphenyl groups at the meso-position as intramolecular nucleophiles, coupled with electron-withdrawing groups at α/β-positions to modulate core electron density and enhance meso-carbon's electrophilicity. We present the first single-crystal X-ray structure of a spirocyclized BODIPY, unambiguously confirming the closed form and its blinking mechanism. By tuning this system, we established a clear pKa-structure-activity relationship, enabling precise prediction and customization of the open-closed equilibrium. The resulting spirocyclization-capable BODIPYs exhibited exceptional brightness up to ∼87,122 M-1 cm-1, and enable self-blinking super-resolution imaging of mitochondria and lysosomes in living cells under low-power laser density (≥32 W cm-2) without requiring imaging-enhancing buffers. This work pioneers the extension of intramolecular spirocyclization to the BODIPY scaffold, establishing a general design strategy for a new class of high-performance, stimuli-responsive probes.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"12 1","pages":"e202518973"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145338555","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Built-in Axial Electric Field-Driven Electron-Rich Monomolecular Co Sites for Promoting CO2 Electroreduction to CO Over Ultrawide Potential Window. 内置轴向电场驱动的富电子单分子Co位在超宽电位窗口上促进CO2电还原为Co。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202511671

Xiaoran Su,Botao Hu,Yingzheng Zhang,Chuhao Liu,Caiyue Wang,Lirong Zheng,Di Zhao,Jiatao Zhang,Chen Chen

{"title":"Built-in Axial Electric Field-Driven Electron-Rich Monomolecular Co Sites for Promoting CO2 Electroreduction to CO Over Ultrawide Potential Window.","authors":"Xiaoran Su,Botao Hu,Yingzheng Zhang,Chuhao Liu,Caiyue Wang,Lirong Zheng,Di Zhao,Jiatao Zhang,Chen Chen","doi":"10.1002/anie.202511671","DOIUrl":"https://doi.org/10.1002/anie.202511671","url":null,"abstract":"Using renewable electricity to convert CO2 into CO offers a sustainable route to producing a versatile intermediate to synthesize various chemicals and fuels. However, the conversion at scale is largely constrained owing to the lack of potential-universal feasibility. Here, we developed an electrocatalyst featuring CoPc anchored ZnO with rich oxygen vacancies (CoPc@ZnOv), thus improving the activity and selectivity of CO2-to-CO conversion. Notably, the FEco of CoPc@ZnOv remains above 90% over an ultrawide potential window of 1.3 V (-0.7 to -2.0 V versus RHE) in H-type cell, 1.40 V (-0.4 to -1.8 V versus RHE) in flow cell and 1.0 V (low cell voltages of 2.0-3.0 V) in the MEA device, surpassing those of previously reported molecular CoPc-based electrocatalysts and even most single metal site materials. Density functional theory calculations combined with in-situ spectroscopies reveal that the built-in axial electric field arising from the p-n junction rectification effect could drive electron-rich single Co-N4 sites with asymmetric charge distribution and geometric curvature, which promotes *COOH formation (i.e., strong CO2 adsorption, rapid H2O dissociation and proton supply), *CO desorption and as well suppresses the hydrogen evolution reaction, thus favoring the production of CO via CO2RR over ultrawide potential windows. This work presents a novel catalyst design strategy of asymmetrical monomolecular Co-N4 sites based on the built-in axial electric field theory, as well as a new way to tune the out-of-plane polarization for improved catalytic performance.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"101 1","pages":"e202511671"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331797","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ether-Anchored MOFs Enable Stable Pseudosuspension Electrolytes for High-Energy Lithium Metal Batteries. 醚锚定mof为高能锂金属电池提供稳定的假悬浮电解质。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-21 DOI: 10.1002/anie.202518384

Yu Han,Yong Chen,Tonghui Zhang,Zhiye Hao,Lianlian He,Weiting Ma,Taolue Wen,Shunshun Zhao,Qimin Peng,Zhenzhen Shen,Robin Wang,Guoxiu Wang,Shimou Chen

{"title":"Ether-Anchored MOFs Enable Stable Pseudosuspension Electrolytes for High-Energy Lithium Metal Batteries.","authors":"Yu Han,Yong Chen,Tonghui Zhang,Zhiye Hao,Lianlian He,Weiting Ma,Taolue Wen,Shunshun Zhao,Qimin Peng,Zhenzhen Shen,Robin Wang,Guoxiu Wang,Shimou Chen","doi":"10.1002/anie.202518384","DOIUrl":"https://doi.org/10.1002/anie.202518384","url":null,"abstract":"Rational electrolyte design, capable of simultaneously accelerating bulk ion transport and stabilizing interfacial chemistry, is indispensable for achieving high-energy-density lithium metal batteries (LMBs). Here, we demonstrate that short-chain ether-functionalized metal-organic frameworks (S@MOFs) meet these requirements by efficiently tailoring Li⁺ coordination and reconstructing the electrode/electrolyte interphase, achieving durable interfacial ion transport kinetics. Synergistic experimental and theoretical investigations demonstrate that the S@MOF-based electrolyte features distinctive pseudosuspension characteristics, harnessing ether chemistry that affords Li-metal compatibility and Li-salt coordination in concert with MOF's abundant binding sites and ordered rigid frameworks. The resultant S@MOF-based electrolyte delivers robust thermodynamic stability across -10 to 60 °C, even in LiNi0.8Co0.1Mn0.1O2 (NCM811)||Li full-cell configurations. Under lean-electrolyte and 50 µm-thick Li-metal configurations, it achieves 92.40% capacity retention for LiCoO2||Li after 1000 cycles. Remarkably, 90.70% for quasi-solid-state NCM811||Li (500 cycles), and 93.21% for Na3V2(PO4)3||Na (3000 cycles) were obtained, confirming its broad applicability across alkali-metal battery chemistries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"59 1","pages":"e202518384"},"PeriodicalIF":16.6,"publicationDate":"2025-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145338581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0