Angewandte Chemie International Edition最新文献_第9页

Activating Interfacial Ion Exchange in Composite Electrolyte to Realize High‐Rate and Long‐Cycling Solid‐State Lithium Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202425221

Qiannan Zhu, Ke Yang, Likun Chen, Xufei An, Shaoke Guo, Yuhang Li, Yuetao Ma, Yidan Cao, Ming Liu, Yan-Bing He

{"title":"Activating Interfacial Ion Exchange in Composite Electrolyte to Realize High‐Rate and Long‐Cycling Solid‐State Lithium Batteries","authors":"Qiannan Zhu, Ke Yang, Likun Chen, Xufei An, Shaoke Guo, Yuhang Li, Yuetao Ma, Yidan Cao, Ming Liu, Yan-Bing He","doi":"10.1002/anie.202425221","DOIUrl":"https://doi.org/10.1002/anie.202425221","url":null,"abstract":"Composite solid electrolytes (CSEs) are promising candidates for solid‐state lithium metal batteries. However, the poor cross‐phase Li+ transport restricts the rate performance and cycle life of the batteries. Herein, we revealed the Li+ percolation behavior in poly(vinylidene fluoride) (PVDF)‐based CSEs with Li6.4La3Zr1.4Ta0.6O12 filler. The de‐coordination barrier from Li+ clusters determines interfacial Li+ transport capability. We then employed a designed N‐methyl‐2,2,2‐trifluoroacetamide (NMTFA) ligand to lower the de‐coordination energy and activate interfacial Li+ exchange, The ionic conductivity is therefore increased from 3.32×10‐4 to 7.30×10‐4 S cm‐1. By tracking the 6Li and 7Li substitution process, it was identified that the proportion of interfacial Li+ transport increases from 11% to 26%. The NMTFA also contributes to the formation of inorganic‐rich interphases with electrodes. As a result, the Li||LiNi0.8Co0.1Mn0.1O2 solid‐state batteries exhibit ultra‐long lifespan of 2400, 3000 and 10000 times at 2, 5 and 10C, respectively, as well as achieve 1000 cycles at 50 °C and 300 cycles at ‐30 °C. This work highlights the critical role of interfacial Li+ transport for the CSEs with “polymer‐Li+ clusters‐filler” configuration to realize high‐rate and long‐cycling solid‐state lithium batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"57 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723371","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

Competitive Coordination Induced Crystallization Regulation for Efficient and Stable Sn-Pb Perovskite Solar Cells

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202501188

Zhongmin Zhou, Cheng Li, Mingzhe Zhu, Shuming Zhang, Jiahui Cheng, Huijie Cao, Peng Cheng, Wenjian Yan, Chao Wang, Fang Yue

{"title":"Competitive Coordination Induced Crystallization Regulation for Efficient and Stable Sn-Pb Perovskite Solar Cells","authors":"Zhongmin Zhou, Cheng Li, Mingzhe Zhu, Shuming Zhang, Jiahui Cheng, Huijie Cao, Peng Cheng, Wenjian Yan, Chao Wang, Fang Yue","doi":"10.1002/anie.202501188","DOIUrl":"https://doi.org/10.1002/anie.202501188","url":null,"abstract":"The faster crystallization rate of Sn perovskite compared with Pb perovskite leads to the spatial component inhomogeneity and inferior quality of the Sn-Pb perovskite films, which increases the quasi-Fermi level splitting (QFLS) deficit and accelerates the oxidative degradation of the films, thus undercutting the efficiency and stability of Sn-Pb perovskite solar cells. Herein, we propose a thermodynamic selective strategy to mediate the crystallization rate between the Sn- and Pb-based perovskite by introducing methyl 5-aminolevulinate hydrochloride (5-AH) in perovskite precursor solution. The SnI2 competes with PbI2 in coordinating with 5-AH to form the thermodynamically favored SnI2-5-AH adducts with stronger SnI2-Cl− according to molecular orbital interactions, thereby delaying the crystallization of Sn-based perovskite. Such crystallization regulation improves the composition uniformity and the crystallization quality, which effectively suppresses non-radiative recombination and reduces the QFLS deficit. Additionally, the strong interaction between Sn2+ and 5-AH as well as reductive grain boundaries inhibits the oxidation of Sn2+. Therefore, the optimal devices with 5-AH exhibit an improved PCE of 23.76% with a high voltage of 0.885 V and long-term stability, maintaining 89% of initial efficiency under continuous irradiation for 1100 h at the maximum power point under AM 1.5G.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"30 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723884","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

Steric Coordinated Electrolytes for Fast-charging and Low-temperature Energy-dense Lithium-ion Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202502978

Xu Liu, Jingwei Zhang, Jia Li, Lianqiang Peng, Zihang Xi, Xuanyu Yun, Kun Li, Huaqing Yu, Yawen Li, Weiwei Xie, Jun Chen, Qing Zhao

{"title":"Steric Coordinated Electrolytes for Fast-charging and Low-temperature Energy-dense Lithium-ion Batteries","authors":"Xu Liu, Jingwei Zhang, Jia Li, Lianqiang Peng, Zihang Xi, Xuanyu Yun, Kun Li, Huaqing Yu, Yawen Li, Weiwei Xie, Jun Chen, Qing Zhao","doi":"10.1002/anie.202502978","DOIUrl":"https://doi.org/10.1002/anie.202502978","url":null,"abstract":"Electrolytes are known as the dominant factors for fast-charging affordability and low-temperature capability of lithium-ion batteries (LIBs). Unfortunately, the current electrolytes can hardly simultaneously satisfy all the required characteristics, including sufficient ion transport, high oxidation/reduction interfacial stability, and fast de-solvation process over a wide-temperature range. Here, we report a solution by designing electrolyte solvents that coordinate with Li+ in steric configuration. The steric coordinated electrolytes (SCEs) can overcome the dilemma of quasi-planer coordinated ether electrolytes that has to be weakly coordinated with Li+ to avoid solvent co-intercalation towards graphite (Gr) anode, therefore enabling the merits including sufficiently dissociation of Li-salt with high ionic conductivity, low de-solvation energy, and forming electrode-electrolyte interphase with low energy barrier. As results, the SCEs with only single-salt and single-solvent (trimethoxymethane) achieve fast kinetics towards Gr anode and high oxidation stability. The LiNi0.8Co0.1Mn0.1O2 (NCM811)||Gr LIBs can reach 80% state of the charge in 6 min, and the Ah-level energy-dense pouch cells (4.5-volt) retain 82.96% (500 cycles) and 85.94% (200 cycles) of initial capacities at room temperature and -20°C, respectively. Our work deepens the fundamental understanding of Li-ion solvation structures and affords an effective approach to design sustainable fluro-free electrolytes for battery systems.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"34 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723887","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

Unusual MurC Ligase and Peptidoglycan Discovered in Lachnospiraceae Using a Fluorescent L-Amino Acid Based Selective Labeling Probe

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202503049

Yahui Du, Yixia Wang, Ming Yang, Liyuan Lin, Jie Zhang, Zhi Huang, Chang Liu, Shuangjiang Liu, Jinbiao Ma, Chaoyong Yang, Wei Wang

{"title":"Unusual MurC Ligase and Peptidoglycan Discovered in Lachnospiraceae Using a Fluorescent L-Amino Acid Based Selective Labeling Probe","authors":"Yahui Du, Yixia Wang, Ming Yang, Liyuan Lin, Jie Zhang, Zhi Huang, Chang Liu, Shuangjiang Liu, Jinbiao Ma, Chaoyong Yang, Wei Wang","doi":"10.1002/anie.202503049","DOIUrl":"https://doi.org/10.1002/anie.202503049","url":null,"abstract":"Developing selective labeling probes for specific bacterial taxa can not only facilitate the study of target bacteria but also deepen our understanding of the microbial diversity at structural and molecular levels. The availability of such probes, however, remains very limited. In this study, by exploiting the variation of amino acids in peptidoglycan stem peptide, we designed a fluorescent L-amino acid probe and found that it could selectively target the family Lachnospiraceae (a major Gram-positive family in murine gut microbiome) in vivo. The following in vitro test using two Roseburia species validated the probe's labeling. We then discovered that the labeling site was the first amino acid (L-alanine in most bacteria), which links the stem peptide with N-acetylmuramic acid, a process catalyzed by a highly conserved enzyme MurC. Enzyme assay of Roseburia MurC demonstrated its ability to conjugate a fluorescent L-amino acid and other non-L-Ala amino acids to UPD-N-acetylmuramic acid. Subsequent X-ray crystallography analysis uncovered a substantially enlarged inner space in this enzyme, which can partially explain its tolerance to these atypical substrates. The resulting unusual peptidoglycan structures lead to significantly reduced activation of the NOD immune receptors, suggesting a new mechanism for the host to accommodate these highly abundant commensals.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"183 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723888","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

Stimuli-Responsive Equilibrium in N-Heterocyclic Carbene-Supported Transition Metal Complexes: Selective Isolation of Multinuclear Species

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202505558

Shashi Kumar, Arnab Rit

{"title":"Stimuli-Responsive Equilibrium in N-Heterocyclic Carbene-Supported Transition Metal Complexes: Selective Isolation of Multinuclear Species","authors":"Shashi Kumar, Arnab Rit","doi":"10.1002/anie.202505558","DOIUrl":"https://doi.org/10.1002/anie.202505558","url":null,"abstract":"The AgI-N-heterocyclic carbene (NHC) complexes (3a,b) derived from a bis(NHC) ligand 1, which exhibit a temperature- and concentration-dependent equilibrium between the trinuclear and tetranuclear forms has been successfully isolated, that is slow on NMR time scale. Intriguingly, by freezing this slow equilibrium, facilitated by strong and stable H-bonding, we could achieve selective isolation of the tetranuclear species (3a,b-II). On the other hand, encapsulation of an anionic guest, ClO4, led to exclusive formation of the guest encapsulated trinuclear AgI-NHC complex, 3a-I. This is unprecedented and marks the first instance where selective isolation of both the species involved in an equilibrium using a C-donor ligand could be attained. In contrast, distinct behavior was observed with the AuI-ion, possessing the same linear geometry however with stronger M-CNHC bonds. In this context, a stable non-exchangeable ≈ 1:1 mixture (4a,b) of the tri- and tetranuclear AuI-NHC complexes were obtained via transmetalation of both the equilibrating (3a,b) and the H-bonded tetranuclear AgI-NHC complexes (3a,b-II). Moreover, by aptly adjusting the reaction parameters of transmetalation process, the trinuclear AuI-NHC complex (4a,b-I) could indeed be obtained selectively. Overall, this study highlights a pioneering approach for the control of an equilibrium between different nuclearity metallo-supramolecular species engaging C-donor ligands.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"96 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723893","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

Prebiotic Interconversion of Pyruvate and Lactate over Zeolite-Supported Ni Catalyst

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202503747

Youngdong Song, Eko Budiyanto, Ashwani Kumar, Gautier Landrot, Harun Tüysüz

{"title":"Prebiotic Interconversion of Pyruvate and Lactate over Zeolite-Supported Ni Catalyst","authors":"Youngdong Song, Eko Budiyanto, Ashwani Kumar, Gautier Landrot, Harun Tüysüz","doi":"10.1002/anie.202503747","DOIUrl":"https://doi.org/10.1002/anie.202503747","url":null,"abstract":"Submarine hydrothermal vents harbor diverse microbial communities and have long intrigued researchers studying the origin of life. Transition metals in these environments can be reduced by serpentinization, potentially forming zeolite-supported transition metal nanoparticles capable of driving prebiotic chemistry. This inorganic structure could catalyze biochemical reactions including converting metabolically crucial pyruvate before the emergence of biological processes. This study explores the catalytic interconversion of pyruvate and lactate, mediated by lactate dehydrogenase in biochemical systems, using inorganic zeolite Y-supported Ni nanoparticles (Ni/Y) under mild hydrothermal vent conditions. Our results demonstrate that Ni/Y effectively catalyzes the hydrogenation of pyruvate in an inert environment, facilitated by the in situ generation of H₂ through an autocatalytic reaction between Ni/Y and H₂O. Post-reaction analysis by X-ray absorption spectroscopy revealed structural transformations in the catalyst, including the formation of unique nickel oxide and hydroxide species, along with extra-framework aluminum from zeolite dealumination, resulting in a thin amorphous nickel oxide/hydroxide layer. Notably, Ni/Y also enables the oxidative reconversion of lactate to pyruvate under atmospheric conditions—an essential reaction catalyzed by lactate dehydrogenase in biological systems. These findings underscore the potential prebiotic role of Ni/Y, suggesting they may have catalyzed the synthesis of key metabolic intermediates.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"87 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723883","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

Iridium-Catalyzed Asymmetric Allenylic Substitution via Kinetic Resolution Enabled by New Monodentate Ligands

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202506350

Youshao Tu, Xiangfeng Lin, Jie Lin, Chaoshen Zhang, Jianwei Sun

{"title":"Iridium-Catalyzed Asymmetric Allenylic Substitution via Kinetic Resolution Enabled by New Monodentate Ligands","authors":"Youshao Tu, Xiangfeng Lin, Jie Lin, Chaoshen Zhang, Jianwei Sun","doi":"10.1002/anie.202506350","DOIUrl":"https://doi.org/10.1002/anie.202506350","url":null,"abstract":"Iridium-catalyzed asymmetric allenylic substitution represents a useful method for the construction of allenes bearing an allenylic central chirality, but current success has uniformly relied on only one specific chiral bidentate ligand. Herein we address the limitation by the design of a new type of monodentate ligands leading to not only excellent enantiocontrol in allenylic substitution, but also efficient kinetic resolution of α-allenylic alcohols, a new phenomenon never observed before in iridium-catalyzed allenylic substitution. This is also a rare demonstration of non-enzymatic kinetic resolution of α-allenylic alcohols. A range of highly enantioenriched allenylic diarylmethanes and α-allenylic alcohols could be accessed under mild conditions. Control experiments and DFT studies indicated that this process proceeds by an SN1 pathway featuring a rate-determining ionization step followed by ligand-controlled enantiodetermining nucleophilic addition. The newly designed rigid and bulky ligands modified from SPHENOL was believed to assemble the key iridium-bound allenylic carbocation intermediate in a different complexation mode, thus serving as the origin of enantiocontrol and the unprecedented kinetic resolution.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"37 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723885","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

Temperature and Solvent Dual Switch Photochromic Chiral Ionic Hydrogen Bonded Organic Framework for Circularly Polarized Luminescence and Advanced Encryption

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202504645

Bin Zhou, Li-Hui Cao, Ming-Feng Huang, Yi Yang, Simeng Qi, Xiao-Jie Cao, Xu-Yong Chen

{"title":"Temperature and Solvent Dual Switch Photochromic Chiral Ionic Hydrogen Bonded Organic Framework for Circularly Polarized Luminescence and Advanced Encryption","authors":"Bin Zhou, Li-Hui Cao, Ming-Feng Huang, Yi Yang, Simeng Qi, Xiao-Jie Cao, Xu-Yong Chen","doi":"10.1002/anie.202504645","DOIUrl":"https://doi.org/10.1002/anie.202504645","url":null,"abstract":"Multi-response encryption materials with temperature control and time resolution have attracted widespread attention due to their unique response characteristics and higher application security. The design and development of photochromic crystalline materials with multiple stimulus responses remain challenging. In this study, we report a pair of responsive photochromic chiral ionic hydrogen bonded organic framework (iHOF) R/S-iHOF-19 controlled by both temperature and solvent through charge-assisted synthesis. The chromophore tetrakis(4-sulfophenyl)ethylene (H4TPE) acts as an electron donor and (1R/S,2R/S)-1,2-diphenylethylenediamine (R/S-DPEN) as an electron acceptor and chiral source. Water and methanol molecules connect the donor and acceptor and interact to build a 3D supramolecular framework. Notably, water and methanol molecules form independent hydrogen-bonding channels within the iHOF structural framework providing a transfer path for the photoinduced electrons. Surprisingly, the formation of a continuous chiral supramolecular framework by R/S-DPEN while generating photo-induced radicals under ultraviolet (UV) irradiation at -20 °C imparts excellent circularly polarised luminescence (CPL) properties to R/S-iHOF-19. The glum values reach -1.8 × 10-3 and +3.75 × 10-3, respectively, and show an enhancement of the circular polarisation of light with decreasing temperature. This CPL with unique low-temperature stimulus-responsive photochromism provides new guidance and perspectives for the development of information security and multiple encryption materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"59 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723886","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

Inside Front Cover: Chemical Process Development in the Pharmaceutical Industry in Europe: Insights and Perspectives from Industry Scientists

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202505858

Joachim Krueger, André P. Dieskau, Jorma Hassfeld, Joerg Gries, Oliver Block, Hilmar Weinmann, Daniel Kaufmann, Stefan Hildbrand, Volker Kraft, Robert Moeckel, Juan R. Dehli, Ulrich Scholz, Carl Friedrich Nising

引用次数: 0

Outside Front Cover: Roadmap to Catalytic Abatement of Gas Phase Per‐ and Polyfluoroalkyl Substances (PFAS)

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI: 10.1002/anie.202506110

Patrick Lott, Florian Maurer, Arik Beck

引用次数: 0