Angewandte Chemie International Edition最新文献

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Operando Magnetic Resonance Imaging for Visualizing Electrochemical Triple-Phase Boundary. 电化学三相边界可视化的操作磁共振成像。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202506183
Shuo-Hui Cao,Wen-Long Jiang,Chun-Yu Qiu,Hui-Jun Sun,Li-Na Wang,Jun-Bo Sheng,Li-Fei Ji,Shuo Liu,Zu-Rong Ni,Shu-Hu Yin,Xiao-Ping Zhang,Yan-Xia Jiang,Yu-Cheng Wang,Zhi-You Zhou,Zhong Chen,Shi-Gang Sun
{"title":"Operando Magnetic Resonance Imaging for Visualizing Electrochemical Triple-Phase Boundary.","authors":"Shuo-Hui Cao,Wen-Long Jiang,Chun-Yu Qiu,Hui-Jun Sun,Li-Na Wang,Jun-Bo Sheng,Li-Fei Ji,Shuo Liu,Zu-Rong Ni,Shu-Hu Yin,Xiao-Ping Zhang,Yan-Xia Jiang,Yu-Cheng Wang,Zhi-You Zhou,Zhong Chen,Shi-Gang Sun","doi":"10.1002/anie.202506183","DOIUrl":"https://doi.org/10.1002/anie.202506183","url":null,"abstract":"The triple-phase boundary (TPB) is a complex interface where gas, liquid, and solid phases converge, crucially regulating the efficiency and performance of many electrochemical devices such as fuel cells and batteries. However, conventional characterization techniques struggle to capture the dynamic processes and flooding at TPB. To address this, we develop operando electrochemical magnetic resonance imaging (EC-MRI), an inherently non-invasive technique sensitive to 1H, which probes both bulk and boundary regions, enabling real-time visualization of TPB evolution and a deeper understanding of its function at the device level under operational conditions. In a study of proton exchange membrane fuel cell (PEMFC), with a focus on the kinetically sluggish O2 reduction reaction in cathode, operando EC-MRI quantitatively illustrates the interplay between power output, water content, and TPB evolution. It reveals that the TPB maps undergo significant spatial and dynamic variations, with TPB deterioration, rather than apparent water accumulation, directly triggering flooding, as proved using catalysts with different water generation and adsorption capabilities. Our finding opens new perspectives on water management and TPB design, with potential applications in other critical electrochemical processes such as H2 oxidation, CO2 reduction, and N2 reduction, underscoring the value of operando EC-MRI for real-time diagnostics of electrochemical devices.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"47 1","pages":"e202506183"},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136799","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
Layered‐Spinel Heterogeneous Structure and Oxygen Vacancies Enable Superior Electrochemical Performance for Li‐Rich Cathodes 层状尖晶石非均相结构和氧空位使富锂阴极具有优越的电化学性能
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202501539
Pengkun Yang, Long Shang, Huimin Wang, Zhenhua Yan, Kai Zhang, Yixin Li, Jun Chen
{"title":"Layered‐Spinel Heterogeneous Structure and Oxygen Vacancies Enable Superior Electrochemical Performance for Li‐Rich Cathodes","authors":"Pengkun Yang, Long Shang, Huimin Wang, Zhenhua Yan, Kai Zhang, Yixin Li, Jun Chen","doi":"10.1002/anie.202501539","DOIUrl":"https://doi.org/10.1002/anie.202501539","url":null,"abstract":"Lithium‐rich manganese‐based oxides (LRMOs) materials are considered to be the next‐generation cathode for high‐energy Li‐ion/metal batteries owing to their superior specific capacity, high operation voltage and low cost. However, the commercial application of LRMOs is constrained by the surface structure degradation and lattice oxygen release, resulting in low initial coulombic efficiency (ICE) and rapid voltage and capacity decay. Herein, we propose a facile sorbic acid‐assisted surface treatment strategy to construct homogeneous multifunctional interface layers composed of layered‐spinel heterogeneous structure and oxygen vacancies on the surface of LRMOs, which enhance the structure stability and improve the activity and reversibility of the anionic oxygen redox reactions. The multifunctional interfacial layers effectively suppress irreversible oxygen release and alleviate unfavorable layered‐spinel phase transformation. As a consequence, the treated LRMOs cathode displays improved ICE of 88.3%, high capacity retention rate (87.9% at 1 C after 150 cycles) and low voltage decay ratio (1.26 mV per cycle). These findings provide a valuable new idea to improve the comprehensive electrochemical performance of LRMOs through multi‐strategy synergistic interface engineering techniques.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"22 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136734","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
Systematic Evaluation of Polarizing Agents for Dynamic Nuclear Polarization Enhanced NMR 动态核极化增强核磁共振极化剂的系统评价
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202505944
Ran Wei, Gilles Casano, Yuxuan Zhang, Ivanska M. Gierbolini-Colón, Yu Rao, Shubha S. Gunaga, Faith J. Scott, Jiaxin Zhou, Satyaki Chatterjee, Sanyog Kumari, Hakim Karoui, Mang Huang, Snorri Th. Sigurdsson, Gaël De Paëpe, Yangping Liu, Frédéric Mentink-Vigier, Amrit Venkatesh, Olivier Ouari, Lyndon Emsley
{"title":"Systematic Evaluation of Polarizing Agents for Dynamic Nuclear Polarization Enhanced NMR","authors":"Ran Wei, Gilles Casano, Yuxuan Zhang, Ivanska M. Gierbolini-Colón, Yu Rao, Shubha S. Gunaga, Faith J. Scott, Jiaxin Zhou, Satyaki Chatterjee, Sanyog Kumari, Hakim Karoui, Mang Huang, Snorri Th. Sigurdsson, Gaël De Paëpe, Yangping Liu, Frédéric Mentink-Vigier, Amrit Venkatesh, Olivier Ouari, Lyndon Emsley","doi":"10.1002/anie.202505944","DOIUrl":"https://doi.org/10.1002/anie.202505944","url":null,"abstract":"Dynamic nuclear polarization (DNP) can significantly enhance the sensitivity of NMR spectroscopy, via the transfer of polarization from unpaired electrons to nuclei. As a result, there is considerable interest in improving DNP efficiency, particularly through the development of new polarizing agents (PAs). Here, a series of 32 PAs, including 26 dinitroxide and 6 hetero biradicals, of which 11 are introduced for the first time, were evaluated in DNP NMR experiments at magnetic field strengths of 9.4 T, 14.1 T, and 21.1 T. The PAs soluble in aqueous media were compared for different proton concentrations. A detailed comparison of the enhancement factors, polarization build-up times, contribution factors, and the resulting overall sensitivity factors is provided. We find that the class of narrow-line-broad-line biradicals not only yield the best performance at high field (21.1 T and 14.1 T), but also remain among the best at intermediate fields (9.4 T). Specifically, we find that SNAPol-1 and HyTEK2 are consistently among the best performing radicals at any field. Among the dinitroxide biradicals, notably at 9.4 T, the AsymPol-POK and M-TinyPol families stand out in proton-dense aqueous matrices, and a newly-developed dinitroxide, NaphPolCbo, is found to provide the best overall sensitivity factor in organic solvent.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"33 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136963","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
Fully Conjugated Sp2 Carbon-Linked Covalent Organic Frameworks Enables Accelerated Exciton Process for Superior Singlet Oxygen Photosynthesis for Water Remediation. 全共轭Sp2碳链共价有机框架加速激子过程用于水修复的单线态氧光合作用。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202509141
Siyuan Guo,Kun Zhao,Luwen Liang,Zifan Li,Bin Han,Xinwen Ou,Shan Yao,Zhiqing Lin,Zhimin Dong,Yunhai Liu,Liqun Ye,Bo Weng,Yanpeng Cai,Zhifeng Yang
{"title":"Fully Conjugated Sp2 Carbon-Linked Covalent Organic Frameworks Enables Accelerated Exciton Process for Superior Singlet Oxygen Photosynthesis for Water Remediation.","authors":"Siyuan Guo,Kun Zhao,Luwen Liang,Zifan Li,Bin Han,Xinwen Ou,Shan Yao,Zhiqing Lin,Zhimin Dong,Yunhai Liu,Liqun Ye,Bo Weng,Yanpeng Cai,Zhifeng Yang","doi":"10.1002/anie.202509141","DOIUrl":"https://doi.org/10.1002/anie.202509141","url":null,"abstract":"Photocatalytic oxygen (O2) activation via energy transfer offers a sustainable approach for singlet oxygen (1O2) synthesis, while its performance suffers from the ultrafast exciton dissociation and sluggish intersystem crossing (ISC) process. Up to date, exciton regulation is still in its infancy. Here, via linkage engineering of covalent organic frameworks (COFs), we propose a fully conjugated sp2 carbon-linked COFs (sp2c-Py-Bpy COFs) with strong exciton interaction and fast ISC for boosted 1O2 photosynthesis. The sp2c-Py-Bpy COFs delivers a record-high 1O2 yield (624 μM min-1) with 100% selectivity, which is ca. 8 times that of the traditional imine-bridged COFs (Im-Py-Bpy COFs, ca. 95.8% selectivity), outperforming documented systems. Transient absorption spectroscopy and theoretical investigations demonstrate that the fully conjugated sp2 carbon linkage of sp2c-Py-Bpy COFs can enhance Coulomb interaction, promote ISC and push forward the transfer of triplet exciton to the O2 adsorption sites throughout the COFs matrix, jointly facilitating the energy transfer process for efficient 1O2 photosynthesis and bypassing the traditional electron transfer process. Hence, sp2c-Py-Bpy COFs can selectively degrade acetaminophen within minutes under visible light irradiation and enables stable degradation of emerging pollutants in a continuous flow membrane reactor (20 × 30 × 2 cm) utilizing natural sunlight and dissolved O2.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"172 1","pages":"e202509141"},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136711","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
Complementary Hydrogen-bonded Functionalized Mixed Conducting Terpolymers for High Performance n-type Organic Electrochemical Transistors and Healable Inverters 用于高性能n型有机电化学晶体管和可修复逆变器的互补氢键功能化混合导电三元聚合物
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202505011
Junxin Chen, Jiayao Duan, Runxia Wang, Juntao Tan, Zhengke Li, Iain McCulloch, Wan Yue
{"title":"Complementary Hydrogen-bonded Functionalized Mixed Conducting Terpolymers for High Performance n-type Organic Electrochemical Transistors and Healable Inverters","authors":"Junxin Chen, Jiayao Duan, Runxia Wang, Juntao Tan, Zhengke Li, Iain McCulloch, Wan Yue","doi":"10.1002/anie.202505011","DOIUrl":"https://doi.org/10.1002/anie.202505011","url":null,"abstract":"High-performing n-type organic electrochemical transistors (OECTs),crucial for integrated circuits in wearable bioelectronics,demand organic mixed ion-electron conductors (OMIECs) that exhibit efficient mixed conduction and biological functionality for practical applications.However,the development of self-healing OMIECs has not yet been achieved due to the lack of suitable synthetic strategies.Here,we present a design concept through incorporating dynamic cross-linked hydrogen-bonded in the polymer backbone for the first demonstration of self-healing polymeric mixed conductors, enabling high-performing OECTs and high gain, self-healing inverters. These devices exhibit a mixed conducting figure of merit µC* of 118 F cm−1 V−1 s−1, three times higher than the copolymer without hydrogen bond, along with simultaneously improved volumetric capacitance and electron mobility. These improvements are attributed to the unique microstructure created by hydrogen bond, which results in a closer π-π stacking distance within smaller crystalline domain sizes. Additionally, a cost-effective post-processing side chain removal method is proposed, which retains high performance in n-type OECTs. Remarkably, inverters based on the hydrogen-bonded terpolymer demonstrate high gain and self-healing capabilities through solvent vapor exposure and annealing treatment. Insights from these terpolymers emphasize the use of dynamic hydrogen bonds in the conjugated backbone to enhance performance and enable self-healing high-gain inverters, advancing wearable bioelectronics for practical applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"152 1","pages":"e202505011"},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144146307","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
Photoswitchable Antimicrobial Metallohelices 光开关抗菌金属螺旋
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202508959
Changhao Liu, Mi Li, Xinyu Wang, Guoqing Li, Xue Zhao, Xuebin Wang, Siying Qin, Xuejian Zhang, Nicola J. Rogers, Xin Zhang, Qianshuo Dong, Guy J. Clarkson, Yuji Wang, Xinyi Yang, Peter Scott, Rubing Wang, Hualong Song
{"title":"Photoswitchable Antimicrobial Metallohelices","authors":"Changhao Liu, Mi Li, Xinyu Wang, Guoqing Li, Xue Zhao, Xuebin Wang, Siying Qin, Xuejian Zhang, Nicola J. Rogers, Xin Zhang, Qianshuo Dong, Guy J. Clarkson, Yuji Wang, Xinyi Yang, Peter Scott, Rubing Wang, Hualong Song","doi":"10.1002/anie.202508959","DOIUrl":"https://doi.org/10.1002/anie.202508959","url":null,"abstract":"Chiral subcomponent self-assembly is used to access optically pure, metallo-helical species based on Zn and Fe(II) and incorporating three trans-azobenzene units. UV-visible, circular dichroism and NMR spectroscopies, alongside X-ray crystallographic and DFT computational studies are used to unambiguously characterize a highly reversible stepwise photochemical transformation to an all-cis state in which structural integrity and optical purity have been retained. While the all-trans state of the water-soluble enantiomers exhibited low or moderate activity against Gram-positive strains, irradiation at 365 nm led to up to eight-fold reduction in MIC. Electron microscopy and a cell permeability assay indicate a membrane disruption mechanism; the higher activity of the photochemically-generated all-cis state is consistent with its more compact supramolecular fold.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"34 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136964","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
Dual Enzyme-Responsive Polymer-Drug Conjugates Induce Diverse Cells Mutual Transcytosis to Achieve Deep Pancreatic Tumor Penetration. 双酶反应聚合物-药物偶联物诱导多种细胞相互胞吞,实现胰腺深部肿瘤穿透。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202506038
Rui Sun,Yifan Zhang,Ying Piao,Jiajia Xiang,Shiqun Shao,Quan Zhou,Jianbin Tang,Chengyuan Dong,Zhuxian Zhou,Youqing Shen
{"title":"Dual Enzyme-Responsive Polymer-Drug Conjugates Induce Diverse Cells Mutual Transcytosis to Achieve Deep Pancreatic Tumor Penetration.","authors":"Rui Sun,Yifan Zhang,Ying Piao,Jiajia Xiang,Shiqun Shao,Quan Zhou,Jianbin Tang,Chengyuan Dong,Zhuxian Zhou,Youqing Shen","doi":"10.1002/anie.202506038","DOIUrl":"https://doi.org/10.1002/anie.202506038","url":null,"abstract":"Enzyme-responsive active transporting nanomedicines have shown promise in overcoming the tumor-dense extracellular matrix barrier by inducing cancer cells' intercellular transcytosis to deliver drugs deep into solid tumors. However, nanomedicine only responsive to the cancer cell-related enzyme is not very effective in pancreatic tumors because successive transcytosis cannot be established among the cancer cells, which are scattered in a large number of cancer-associated fibroblasts (CAFs). Here are reported dual-enzyme responsive 7-ethyl-10-hydroxycamptothecin (SN38)-polymer conjugates capable of inducing transcytosis among cancer cells and CAFs to infiltrate pancreatic tumors efficiently. The conjugates are zwitterionic for long blood circulation. Once in the tumor, the γ-glutamyl transpeptidase (GGT) overexpressed on the tumor endothelial and cancer cells, or the fibroblast-activated protease (FAP) on CAFs, can cleave the γ-glutamylamide or the prolylglycine dipeptide amides, producing primary amines. The cationized conjugate then induces transcytosis among cancer cells and CAFs, establishing successive intercellular transport to infiltrate the tumor. The conjugates' enzyme reactivity and overall hydrophobicity determine their cationization and transcytosis behaviors. The conjugates with high hydrophobicity and fast cationization show potent antitumor activity in pancreatic cancer patient-derived xenograft and orthotopic tumor models. This study provides an active transportation strategy to overcome the delivery barrier of tumors with rich stroma cells.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"3 1","pages":"e202506038"},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136680","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
Interfacial Engineering and Structural Modulation of RuO2-Based Catalysts for Highly Active and Durable Oxygen Evolution Reaction in Acidic Environment. 酸性环境下高活性持久析氧反应的钌基催化剂的界面工程与结构调控
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202509768
Ming Zhao,Weiwei Yang,Zhijun Wang,Jie Zhang,Liangyong Jia,Jiahui Li,Xinyu Chen,Xinyang Liu,Huayang Zhang,Jingkai Lin,Qingjun Chen
{"title":"Interfacial Engineering and Structural Modulation of RuO2-Based Catalysts for Highly Active and Durable Oxygen Evolution Reaction in Acidic Environment.","authors":"Ming Zhao,Weiwei Yang,Zhijun Wang,Jie Zhang,Liangyong Jia,Jiahui Li,Xinyu Chen,Xinyang Liu,Huayang Zhang,Jingkai Lin,Qingjun Chen","doi":"10.1002/anie.202509768","DOIUrl":"https://doi.org/10.1002/anie.202509768","url":null,"abstract":"Developing highly active and durable catalysts for the oxygen evolution reaction (OER) under acidic conditions is key to commercializing green hydrogen production via water splitting. Here, we fabricated a cobalt oxide (Co3O4)-synergised nickel-doped ruthenium oxide (Ni-RuO2) heterojunction on reduced graphene oxide (Co3O4/Ni-RuO2/rGO) as an efficient and durable OER electrocatalyst in acidic electrolytes. The interface of Co3O4/Ni-RuO2 heterojunction and doping of Ni into RuO2, as well as their effect on electronic structure, were examined by advanced characterizations. With only 1.36 wt% RuO2, the Co3O4/Ni-RuO2/rGO heterojunction revealed an ultra-low overpotential of 195 and 305 mV at 10 and 100 mA cm-2, respectively. Moreover, the catalyst's performance was well maintained after operating for 100 h at 500 mA cm-2, suggesting great promise for practical applications. Density functional theory calculations and in-situ Raman analysis indicate that both the heterojunction structure and Ni doping play crucial roles in enhancing the OER activity and durability. This study provides a promising avenue for developing cost-effective electrocatalysts with superior activity and stability for advanced energy conversion.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"56 1","pages":"e202509768"},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136798","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
Topologically Entangled Network Polymer Electrolyte with Ionophilic-Protonation Dual Side Chains for High-Voltage Lithium-Metal Batteries. 高压锂金属电池的亲离子质子化双侧链拓扑纠缠网络聚合物电解质。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202507222
Longjie He,Yiting Shao,Shibin Li,Yihang Nie,Ying Chu,Guo Feng,Xuancheng Liu,Qingying Li,Dan Luo,Xin Wang,Zhongwei Chen
{"title":"Topologically Entangled Network Polymer Electrolyte with Ionophilic-Protonation Dual Side Chains for High-Voltage Lithium-Metal Batteries.","authors":"Longjie He,Yiting Shao,Shibin Li,Yihang Nie,Ying Chu,Guo Feng,Xuancheng Liu,Qingying Li,Dan Luo,Xin Wang,Zhongwei Chen","doi":"10.1002/anie.202507222","DOIUrl":"https://doi.org/10.1002/anie.202507222","url":null,"abstract":"The development of high-voltage solid-state lithium-metal batteries (HVSSLMBs) is severely limited by unstable ion transport, insufficient oxidative stability, and poor electrode-electrolyte interface (EEI) compatibility of conventional solid electrolytes. Herein, we report a topologically entangled polymer electrolyte featuring ionophilic-protonation dual side chains. The ionophilic functional groups on these side chains provide abundant coordination sites, significantly enhancing Li+ transport, while exposed carboxyl (-COOH) groups induce protonation on the cathode surface, effectively suppressing transition metal (TM) ion migration. The topologically entangled polymer network ensures uniform electric-field distribution, mitigates lattice-oxygen release, and maintains continuous Li+ conduction. As a result, this electrolyte achieves a high room-temperature ionic conductivity of 0.81 mS cm-1 and an oxidation stability up to 4.9 V. Moreover, the in situ formed inorganic species (LiF, Li2O, and Li2CO3), stabilized the EEI, enabling stable cycling of the symmetric cell for 2000 hours. Batteries assembled with a high-voltage Li1.2Ni0.13Mn0.54Co0.13O2 (LRMO) cathode retain a specific capacity of 217.37 mAh g-1 after 250 cycles, and Ah-level pouch cell utilizing an LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode exhibits stable cycling performance over 150 cycles. These findings demonstrate the great promise of this strategy for the development of high-energy-density lithium-metal batteries with outstanding cycling performance and long-term stability.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"58 1","pages":"e202507222"},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136800","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
Identification of Ti(salen)-Complexes for Efficient Catalysis in Single Electron Steps by Cyclic Voltammetry (CV). 循环伏安法(CV)鉴定单电子步骤高效催化Ti(salen)配合物。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-05-26 DOI: 10.1002/anie.202507673
Andreas Gansäuer,Niklas Schmickler,Sergei Gerber,Lennart Hanz,Stefan Grimme,Zheng-Wang Qu,Inke Siewert
{"title":"Identification of Ti(salen)-Complexes for Efficient Catalysis in Single Electron Steps by Cyclic Voltammetry (CV).","authors":"Andreas Gansäuer,Niklas Schmickler,Sergei Gerber,Lennart Hanz,Stefan Grimme,Zheng-Wang Qu,Inke Siewert","doi":"10.1002/anie.202507673","DOIUrl":"https://doi.org/10.1002/anie.202507673","url":null,"abstract":"We describe the identification of an active Ti(salen)-catalyst for the radical arylation of epoxides by a CV study of mechanism-based predictors, such as the redox potentials of the complexes and their EqCr-equilibria, for the success of catalysis. Surprisingly, the by far most active catalyst features an uncommon tetrasubstituted ligand backbone that renders chloride binding to the active Ti(III) species less favorable and thereby increases catalyst activity due to improved substrate binding. Catalysis is most efficient in the 'green' solvent ethyl acetate and can be initiated using base metals as well as electrochemical methods for the reduction of the Ti(salen)-precatalyst. Compared to the commonly employed titanocene catalysis, the use of the newly developed Ti(salen)-catalyst allows for the use of milder and more sustainable reactions conditions, a broader substrate scope as well as facile modification of the catalyst's electronic and steric properties.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"142 1","pages":"e202507673"},"PeriodicalIF":16.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144136679","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
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