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Cover Picture: Visible‐Light Activation of Diorganyl Bis(pyridylimino) Isoindolide Aluminum(III) Complexes and Their Organometallic Radical Reactivity (Angew. Chem. Int. Ed. 19/2024) Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Jonas O. Wenzel, Johannes Werner, Alexander Allgaier, Joris van Slageren, Israel Fernández, Andreas‐Neil Unterreiner, Frank Breher
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A Universal Self‐Propagating Synthesis of Aluminum‐Based Oxyhalide Solid‐State Electrolytes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Simeng Zhang, Yang Xu, Han Wu, Tianlu Pang, Nian Zhang, Changtai Zhao, Junyi Yue, Jiamin Fu, Shengjie Xia, Xiangzhen Zhu, Guanzhi Wang, Hui Duan, Biwei Xiao, Tao Mei, Jianwen Liang, Xueliang Sun, Xiaona Li
Inorganic solid‐state electrolytes (SSEs) play a vital role in high‐energy all‐solid‐state batteries (ASSBs). However, the current method of SSE preparation usually involves high‐energy mechanical ball milling and/or a high‐temperature annealing process, which is not suitable for practical application. Here, a facile strategy is developed to realize the scalable synthesis of cost‐effective aluminum‐based
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Water and Air Stable Copper(I) Complexes of Tetracationic Catenane Ligands for Oxidative C–C Cross‐Coupling Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Man Pang Tang, Lihui Zhu, Yulin Deng, Yixiang Shi, Samuel Kin-Man Lai, Xiaoyong Mo, Xin-Yu Pang, Chunyu Liu, Wei Jiang, Edmund Chun Ming Tse, Ho Yu Au-Yeung
Aqueous soluble and stable Cu(I) molecular catalysts featuring a catenane ligand composed of two dicationic, mutually repelling but mechanically interlocked macrocycles are reported. The ligand interlocking not only fine‐tunes the coordination sphere and kinetically stabilizes the Cu(I) against air oxidation and disproportionation, but also buries the hydrophobic portions of the ligands and prevents
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Kinetic Control of Complexity in Multiple Dynamic Libraries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 David S. Rivero, Yaiza Pérez-Pérez, Marcelle D. Perretti, Tanausú Santos, Jimena Scoccia, David Tejedor, Romen Carrillo
Multiple dynamic libraries of compounds are generated when more than one reversible reaction comes into play. Commonly, two or more orthogonal reversible reactions are used, leading to non‐communicating dynamic libraries which share no building blocks. Only a few examples of communicating libraries have been reported, and in all those cases, building blocks are reversibly exchanged from one library
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Bifunctional Ligand Enables Gold‐Catalyzed Propargyl C‐H Functionalization via Reactive Gold Allenylidene Intermediate Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Yongliang Wei, Jingxing Jiang, Yaru Jing, Zhuofeng Ke, Liming Zhang
Gold allenylidene species have been seldom exploited as reactive intermediates in synthetically versatile catalytic reactions. By employing alkynylbenziodoxoles as the substrates and bifunctional WangPhos as the metal ligand, this work demonstrated ready catalytic access to these intermediates of general substitution patterns and their electrophilic reactivities at the γ‐carbon center with a diverse
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Acyclic Cucurbit[n]uril Receptors Function as Solid State Sequestrants for Organic Micropollutants Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Suvenika Perera, Alok Shaurya, Michael Baptiste, Peter Y Zavalij, Lyle Isaacs
The accumulation of organic micropollutants (OMP) in aquatic systems is a major societal problem that can be addressed by approaches including nanofiltration, flocculation, reverse osmosis and adsorptive methods using insoluble materials (e.g. activated carbon, MOFs, nanocomposites). More recently, polymeric versions of supramolecular hosts (e.g. cyclodextrins, calixarenes, pillararenes) have been
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An Unprecedented [BO2]‐Based Deep‐Ultraviolet Transparent Nonlinear Optical Crystal by Superhalogen Substitution Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Shuai Liu, Xingxing Jiang, Lu Qi, Yilei Hu, Kaining Duanmu, Chao Wu, Zheshuai Lin, Zhipeng Huang, Mark G. Humphrey, Chi Zhang
Solid‐state structures with the superhalogen [BO2]− have thus far only been observed with a few compounds whose syntheses require high reaction temperatures and complicated procedures, while their optical properties remain almost completely unexplored. Herein, we report a facile, energy‐efficient synthesis of the first [BO2]‐based deep‐ultraviolet (deep‐UV) transparent oxide K9[B4O5(OH)4]3(CO3)(BO2)·7H2O
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Domain Swapping in Abiotic Foldamers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Shuhe Wang, Barbara Wicher, Céline Douat, Victor Maurizot, Ivan Huc
Foldamer sequences that adopt tertiary helix‐turn‐helix folds mediated by helix‐helix hydrogen bonding in organic solvents have been previously reported. In an attempt to create genuine abiotic quaternary structures, i.e. assemblies of tertiary structures, new sequences were prepared that possess additional hydrogen bond donors at positions that may promote an association between the tertiary folds
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Design of Solid Polycationic Electrolyte to Enable Durable Chloride‐Ion Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Xu Yang, Zhiqiang Fu, Ran Han, Yaojie Lei, Shijian Wang, Xin Zhao, Yuefeng Meng, Hao Liu, Dong Zhou, Doron Aurbach, Guoxiu Wang
The high energy density and cost‐effectiveness of chloride‐ion batteries (CIBs) make them promising alternatives to lithium‐ion batteries. However, the development of CIBs is greatly restricted by the lack of compatible electrolytes to support cost‐effective anodes. Herein, we present a rationally designed solid polycationic electrolyte (SPE) to enable room‐temperature chloride‐ion batteries utilizing
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In‐Situ Cyclized Polyacrylonitrile as an Electron Selective Layer for n‐i‐p Perovskite Solar Cell with Enhanced Efficiency and Stability Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Wei-Min Gu, Ke-Jian Jiang, Xinning Jiao, Cai-Yan Gao, Xin-Heng Fan, Yanlin Song, Lian-Ming Yang
In‐situ cyclized polyacrylonitrile (CPAN) is developed to replace n‐type metal oxide semiconductors (TiO2 or SnO2) as an electron selective layer (ESL) for highly efficient and stable n‐i‐p perovskite solar cells (PSCs). The CPAN layer is fabricated via facile in‐situ cyclization reaction of polyacrylonitrile (PAN) coated on a conducting glass substrate. The CPAN layer is robust and insoluble in common
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Graphical Abstract: Angew. Chem. Int. Ed. 19/2024 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25
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A Thermosalient and Mechanically Compliant Organic Crystalline Optical Waveguide Switcher Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Qi Di, Marieh B. Al-Handawi, Liang Li, Panče naumov, Hongyu Zhang
The dense and ordered molecular arrangements endow dynamic molecular crystals with fast response, rapid energy conversion, low energy dissipation, and strong coupling between heat/light and mechanical energy. Most of the known dynamic crystals can only respond to a single stimulus, and materials that can respond to multiple stimuli are rare. Here, we report an organic crystalline material that can
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Discovery of a Plant 14‐3‐3 Inhibitor Possessing Isoform Selectivity and In Planta Activity Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Kotaro Nishiyama, Yusuke Aihara, Takehiro Suzuki, Koji Takahashi, Toshinori Kinoshita, Naoshi Dohmae, Ayato Sato, Shinya Hagihara
Synthetic modulators for plant 14‐3‐3s are promising chemical tools both for understanding the 14‐3‐3‐related signaling pathways and controlling plant physiology. Here, we describe a novel small‐molecule inhibitor for 14‐3‐3 proteins ofArabidopsis thaliana. The inhibitor was identified from unexpected products in DMSO stock solution of an in‐house chemical library. Mass spectroscopy, mutant‐based analyses
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Macrocycle‐Based Charge Transfer Cocrystals with Dynamically Reversible Chiral Self‐Sorting Display Chain Length‐Selective Vapochromism to Alkyl Ketones Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Meng-Jie Gu, Wei-Chen Guo, Xiao-Ni Han, Ying Han, Chuan-Feng Chen
Chirality‐driven self‐sorting plays an essential role in controlling the biofunction of biosystems, such as the chiral double‐helix structure of DNA from self‐recognition by hydrogen bonding. However, achieving precise control over the chiral self‐sorted structures and their functional properties for the bioinspired supramolecular systems still remains a challenge, not to mention realizing dynamically
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Grain‐Boundary‐Rich RuO2 Porous Nanosheet for Efficient and Stable Acidic Water Oxidation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Weidong He, Xiaohong Tan, Yingying Guo, Yuhang Xiao, Hao Cui, Chengxin Wang
RuO2 has been considered as the most likely acidic oxygen evolution reaction (OER) catalyst to replace IrO2, but its performance, especially long‐term stability under harsh acidic conditions, is still unacceptable. Here, we propose a grain boundary (GB) engineering strategy by fabricating the ultrathin porous RuO2 nanosheet with abundant of grain boundaries (GB‐RuO2) as an efficient acid OER catalyst
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Tunable Interfacial Electric Field‐Mediated Cobalt‐Doped FeSe/Fe3Se4 Heterostructure for High‐Efficiency Potassium Storage Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Lili Song, Shilin Zhang, Liping Duan, Renke Li, Yifan Xu, Jiaying Liao, Liang Sun, Xiaosi Zhou, Zaiping Guo
The interfacial electric field (IEF) in the heterostructure can accelerate electron transport and ion migration, thereby enhancing the electrochemical performance of potassium‐ion batteries (PIBs). Nevertheless, the quantification and modulation of the IEF for high‐efficiency PIB anodes currently remains a blank slate. Herein, we achieve for the first time the quantification and tuning of IEF via amorphous
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Planar Tetranuclear Uranium Hydride Cluster Supported by ansa‐Bis(cyclopentadienyl) Ligands Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Kai Li, Iker del Rosal, Yue Zhao, Laurent Maron, Congqing Zhu
Polynuclear metal hydride clusters play important roles in various catalytic processes, with most of the reported polynuclear metal hydride clusters adopting a polyhedral three‐dimensional structure. Herein, we report the first example of a planar tetranuclear uranium hydride cluster [(CpCMe2CMe2Cp)U]4(μ2‐H)4(μ3‐H)4 (U4H8). It was synthesized by reacting an ansa‐bis(cyclopentadienyl) ligand‐supported
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Rapid Defect Engineering in FeCoNi/FeAl2O4 Hybrid for Enhanced Oxygen Evolution Catalysis: A Pathway to High‐Performance Electrocatalysts Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Yuhao Chen, Jiang Xu, Yujie Chen, Luqi Wang, Shuyun Jiang, Zong-Han Xie, Tianran Zhang, Paul Munroe, Shengjie Peng
Rational modulation of surface reconstruction in the oxygen evolution reaction (OER) utilizing defect engineering to form efficient catalytic activity centers is a topical interest in the field of catalysis. The introduction of point defects has been demonstrated to be an effective strategy to regulate the electronic configuration of electrocatalysts, but the influence of more complex planar defects
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Insights into E. coli cyclopropane fatty acid synthase (CFAS) towards enantioselective carbene free biocatalytic cyclopropanation. Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Iman Omar, Michele Crotti, Chuhan Li, Krisztina Pisak, Blazej Czemerys, Salvatore Ferla, Aster van Noord, Caroline Paul, Kersti Karu, Cagakan Ozbalci, Ulrike Eggert, Richard Lloyd, Sarah Barry, Daniele Castagnolo
Cyclopropane fatty acid synthases (CFAS) are a class of S‐adenosylmethionine (SAM) dependent methyltransferase enzymes able to catalyse the cyclopropanation of unsaturated phospholipids. Since CFAS enzymes employ SAM as a methylene source to cyclopropanate alkene substrates, they have the potential to be mild and more sustainable biocatalysts for cyclopropanation transformations than current carbene
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Template‐guided Silicon Micromotor Assembly for Enhanced Cell Manipulation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Yuxin Gao, Leyan Ou, Kunfeng Liu, Yuan Guo, Wanyuan Li, Ze Xiong, Changjin Wu, Jizhuang Wang, Jinyao Tang, Dan Li
Light‐driven micro/nanorobots (LMNRs) are tiny, untethered machines with great potential in fields like precision medicine, nano manufacturing, and various other domains. However, their practicality hinges on developing light‐manipulation strategies that combine versatile functionalities, flexible design options, and precise controllability. Our study introduces an innovative approach to construct
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Rechargeable Zn‐H2O hydrolysis battery for hydrogen storage and production Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Muya Cai, Hao Shi, Yu Zhang, Jiakang Qu, Hongya Wang, Yanyang Guo, Kaifa Du, Wei Li, Bowen Deng, Dihua Wang, Huayi Yin
Reactive metals hydrolysis offers significant advantages for hydrogen storage and production. However, the regeneration of common reactive metals (e.g., Mg, Al, etc.) is energy‐intensive and produces unwanted byproducts such as CO2 and Cl2. Herein, we employ Zn as a reactive mediator that can be easily regenerated by electrolysis of ZnO in an alkaline solution with a Faradaic efficiency of > 99.9%
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New Alkalescent Electrolyte Chemistry for Zinc‐Ferricyanide Flow Battery Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Liping Zhi, Chenyi Liao, Pengcheng Xu, Fusai Sun, Fengtao Fan, Guohui Li, Zhizhang Yuan, Xianfeng Li
Alkaline zinc‐ferricyanide flow batteries are efficiency and economical as energy storage solutions. However, they suffer from low energy density and short calendar life. The strongly alkaline conditions (3 mol L‐1 OH‐) reduce the solubility of ferri/ferro‐cyanide (normally only 0.4 mol L‐1 at 25 oC) and induce the formation of zinc dendrites at the anode. Here, we report a new zinc‐ferricyanide flow
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Back Cover: Cavity‐Directed Synthesis of Labile Polyoxometalates for Catalysis in Confined Spaces (Angew. Chem. Int. Ed. 19/2024) Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Cui‐Lian Liu, Mhamad Aly Moussawi, Givi Kalandia, David E. Salazar Marcano, William E. Shepard, Tatjana N. Parac‐Vogt
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Revealing Na+‐coordination Induced Failure Mechanism of Metal Sulfide Anode for Sodium Ion Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Yuchen Fu, Jun Sun, Yunsheng Zhang, Wei Qu, Weichao Wang, Meng Yao, Yun Zhang, Qian Wang, Yongfu Tang
Metal sulfide (MS) is regarded as a promising candidate of the anode materials for sodium‐ion battery (SIB) with ideal capacity and low cost, yet still suffers from the inferior cycling stability and voltage degradation. Herein, the coordination relationship between the discharge product Na2S with the Na+ (NaPF6) in the electrolyte, is revealed as the root cause for the cycling failure of MS. Na+‐coordination
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Inside Cover: Anion‐Involved Solvation Structure of Lithium Polysulfides in Lithium–Sulfur Batteries (Angew. Chem. Int. Ed. 19/2024) Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-25 Yun‐Wei Song, Liang Shen, Nan Yao, Shuai Feng, Qian Cheng, Jin Ma, Xiang Chen, Bo‐Quan Li, Qiang Zhang
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Catalytic Asymmetric Cascade Dearomatization of Indoles via a Photoinduced Pd-Catalyzed 1,2-Bisfunctionalization of Butadienes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-20 Xiaohang Zhan, Zhiwen Nie, Na Li, Ao Zhou, Haotian Lv, Mingrong Liang, Keqin Wu, Guijuan Cheng, Qin Yin
Photoinduced Pd-catalyzed bisfunctionalization of butadienes with a readily available organic halide and a nucleophile represents an emerging and attractive method to assemble versatile alkenes bearing various functional groups at the allylic position. However, enantiocontrol and/or diastereocontrol in the C-C or C-X bond-formation step have not been solved due to the open-shell process. Herein, we
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Ratiometric Afterglow Luminescent Imaging of Matrix Metalloproteinase-2 Activity via an Energy Diversion Process Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Weijing Huang, Wenhui Zeng, Zheng Huang, Daqing Fang, Hong Liu, Min Feng, Liang Mao, Deju Ye
Ratiometric afterglow luminescent (AGL) probes are attractive for in vivo imaging due to their high sensitivity and signal self-calibration function. However, there are currently few ratiometric AGL probes available for imaging enzymatic activity in living organisms. Here, we present an energy diversion (ED) strategy that enables the design of an enzyme-activated ratiometric AGL probe (RAG-RGD) for
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Temporal-Focusing Multiphoton Excitation Single-Molecule Localization Microscopy Using Spontaneously Blinking Fluorophores Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Jian-Zong Lai, Chun-Yu Lin, Shean-Jen Chen, Yu-Min Cheng, Manabu Abe, Tzu-Chau Lin, Fan-Ching Chien
Single-molecule localization microscopy (SMLM) based on temporal-focusing multiphoton excitation (TFMPE) and single-wavelength excitation is used to visualize the three-dimensional (3D) distribution of spontaneously blinking fluorophore-labeled subcellular structures in a thick specimen with a nanoscale-level spatial resolution. To eliminate the photobleaching effect of unlocalized molecules in out-of-focus
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The 18F-Difluoromethyl Group: Challenges, Impact and Outlook Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Joseph Ford, Sebastiano Ortalli, Veronique Gouverneur
The difluoromethyl functionality has proven useful in drug discovery, as it can modulate the properties of bioactive molecules. For PET imaging, this structural motif has been largely underexploited in (pre)clinical radiotracers due to a lack of user-friendly radiosynthetic routes. This Minireview provides an overview of the challenges facing radiochemists and summarises the efforts made to date to
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Reaction Environment Regulation for Electrocatalytic CO2 Reduction in Acids Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 min Zeng, Wensheng Fang, Yiren Chen, Xinyi Zhang, Yongming Hu, Bao Yu Xia
The electrocatalytic CO2 reduction reaction (CO2RR) is a sustainable route for converting CO2 into value-added fuels and feedstocks, advancing a carbon-neutral economy. The electrolyte critically influences CO2 utilization, reaction rate and product selectivity. While typically conducted in neutral/alkaline aqueous electrolytes, the CO2RR faces challenges due to (bi)carbonate formation and its crossover
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Chemical Control of Fluorescence Lifetime towards Multiplexing Imaging Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Junbao Ma, Feng Luo, Chia-Heng Hsiung, Jianan Dai, Zizhu Tan, Songtao Ye, Lina Ding, Baoxing Shen, Xin Zhang
Fluorescence lifetime imaging has been a powerful tool for biomedical research. Recently, fluorescence lifetime-based multiplexing imaging has expanded imaging channels by using probes that harbor the same spectral channels and distinct excited state lifetime. While it is desirable to control the excited state lifetime of any given fluorescent probes, the rational control of fluorescence lifetimes
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Delocalizing Excitation for Highly-Active Organic Photovoltaic Catalysts Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Zhenzhen Zhang, Chaoying Xu, Qianlu Sun, Yufan Zhu, Wenlong Yan, Guilong Cai, Yawen Li, Wenqin Si, Xinhui Lu, Weigao Xu, Ye Yang, Yuze Lin
Localized excitation in traditional organic photocatalysts typically prevents the generation and extraction of photo-induced free charge carriers, limiting their activity enhancement under illumination. Here, we enhance delocalized photoexcitation of small molecular photovoltaic catalysts by weakening their electron-phonon coupling via rational fluoro-substitution. The optimized 2FBP-4F catalyst we
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Machine Learning Molecular Dynamics Shows Anomalous Entropic Effect on Catalysis via Surface Pre-melting of Nanoclusters Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Fu-Qiang Gong, Yun-Pei Liu, Ye Wang, Weinan E, Zhong-Qun Tian, Jun Cheng
Due to the superior catalytic activity and efficient utilization of noble metals, nanocatalysts are extensively used in the modern industrial production of chemicals. The surface structures of these materials are significantly influenced by reactive adsorbates, leading to dynamic behavior under experimental conditions. The dynamic nature poses significant challenges in studying the structure-activity
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Cyclometallated Imides as Templates for the H-Bond Directed Iridium-Catalyzed Asymmetric Hydrogenation of N-Methyl, N-Alkyl and N-Aryl Imines Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Yisong Wen, Marc Fernández-Sabaté, Agustí Lledós, Giuseppe Sciortino, James Eills, Irene Marco-Rius, Antoni Riera, Xavier Verdaguer
A combined computational and experimental approach allowed us to develop the most selective catalysts for the direct hydrogenation of N-methyl and N-alkyl imines described to date. Iridium catalysts with a cyclometallated cyclic imide group provide selectivity of up to 99% enantiomeric excess. Computational studies show that the selectivity results from the combined effect of H-bonding of the imide
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Repurposing Visible‐Light‐Excited Ene‐Reductases for Diastereo‐ and Enantioselective Lactones Synthesis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Jinhai Yu, Qiaoyu Zhang, Beibei Zhao, Tianhang Wang, Yu Zheng, Binju Wang, Yan Zhang, Xiaoqiang Huang
Repurposing enzymes to catalyze non‐natural asymmetric transformations that are difficult to achieve using traditional chemical methods is of significant importance. Although radical C‐O bond formation has emerged as a powerful approach for constructing oxygen‐containing compounds, controlling the stereochemistry poses a great challenge. Here we present the development of a dual bio‐/photo‐catalytic
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Paper Spray Mass Spectrometry with On‐Paper Electrokinetic Manipulations: Part‐ Per‐Trillion Detection of Per/Polyfluoroalkyl Substances in Water and Opioids in Urine Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Magnus Rydberg, Merlin Bruening, Nicholas Manicke
We developed a simple, paper‐based device that enables sensitive detection by mass spectrometry (MS) without solid phase extraction or other sample preparation. Using glass fiber filter papers within a 3D printed holder, the device employs electrokinetic manipulations to stack, separate, and desalt charged molecules on paper prior to spray into the MS. Due to counter‐balanced electroosmotic flow and
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An Integrative Chemical Recycling Approach for Catalytic Oxidation of Epoxy Resin and in‐situ Separation of Degraded Products Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Lulu Liu, Xuehui Liu, Xiaohui Li, Shimei Xu, Yu-Zhong Wang
Although many approaches have been proposed to recycling waste epoxy resin (EP), the separation of mixed degraded products remains a challenge due to their similar structures. To address this, we present a catalytic oxidation strategy that enables mild degradation of EP and in‐situ separation of degraded products through supramolecular interactions. The oxidative degradation relies on FeIV=O radicals
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The Role of the Molecular Encapsulation Effect in Stabilizing Hydrogen‐Bond‐Rich Gel‐State Lithium Metal Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Hantao Xu, Wei Deng, Lei Shi, Juncai Long, Yongcai Zhang, Lin Xu, Liqiang Mai
Gel‐state polymer electrolytes with superior mechanical properties, self‐healing abilities and high Li+ transference numbers can be obtained by in situ polymerization of monomers with hydrogen‐bonding moieties. However, it is overlooked that the active hydrogen atoms in hydrogen‐bond donors experience displacement reactions with lithium metal in lithium metal batteries (LMBs), leading to corrosion
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Crystalline Porous Organic Frameworks Based on Multiple Dynamic Linkages Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Bo Liu, Panyue Guo, Xinyu Guan, Xuexue Tian, Fei Du, Weiqing Xie, Hai-Long Jiang
A novel class of crystalline porous materials has been developed utilizing multilevel dynamic linkages, including covalent B‐O, dative B←N and hydrogen bonds. Typically, boronic acids undergo in situ condensation to afford B3O3‐based units, which further extend to molecular complexes or chains via B←N bonds. The obtained superstructures are subsequently interconnected via hydrogen bonds and π‐π interactions
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Hyperbranched Vitrimer for Ultrahigh Energy Dissipation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Lin Cheng, Jun Zhao, Zhongqiang Xiong, Sijun Liu, Xuzhou Yan, Wei Yu
Polymers are ideally utilized as damping materials due to the high internal friction of molecular chains, enabling effective suppression of vibrations and noises in various fields. Current strategies rely on broadening the glass transition region or introducing additional relaxation components to enhance the energy dissipation capacity of polymeric damping materials. However, it remains a significant
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Synthesis of 18F‐labeled Aryl Trifluoromethyl Sulfones, ‐Sulfoxides, and ‐Sulfides for Positron Emission Tomography Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Lukas Veth, Albert D. Windhorst, Danielle J. Vugts
Positron emission tomography (PET) is becoming increasingly important in nuclear medicine and drug discovery. To date, the development of many potential PET tracers is hampered by the lack of suitable synthetic pathways for their preparation. This is particularly true for the highly desired radiolabeling of compounds bearing [18F]CF3‐groups. For instance, S(O)nCF3‐groups (n = 0, 1, 2) serve as structural
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On the Dendrite‐Suppressing Effect of Laser‐Processed Polylactic Acid‐Derived Carbon Coated Zinc Anode in Aqueous Zinc Ion Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Maryam Abouali, Sadaf Adhami, Somayeh Asadi Haris, Recep Yuksel
A major bottleneck limiting the commercialization of aqueous zinc ion batteries (AZIBs) is dendrite formation on the zinc anode during the plating/stripping process, which leads to rapid performance and device failure. In this regard, researchers are trying to design more stable anodes toward suppressing dendrite formation. One possible solution to tackle this problem and to extend the cycling life
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A Photodynamic and Photochemotherapeutic Platinum‐Iridium Charge‐Transfer Conjugate for Anticancer Therapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Huayun Shi, Oliver W. L. Carter, Fortuna Ponte, Cinzia Imberti, Miguel A. Gomez‐Gonzalez, Fernando Cacho‐Nerin, Paul D. Quinn, Julia E. Parker, Emilia Sicilia, Huaiyi Huang, Peter J. Sadler
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Bioorthogonal Cu Single‐atom Nanozyme for Synergistic Nanocatalytic Therapy, Photothermal Therapy, Cuproptosis, and Immunotherapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Luyan Wu, Huihui Lin, Xiang Cao, Qiang Tong, Fangqi Yang, Yinxing Miao, Deju Ye, Quli Fan
Single‐atom nanozymes (SAzymes) with atomically dispersed active sites are potential substitutes for natural enzymes. A systematic study of its multiple functions can in‐depth understand SAzymes’s nature, which remains elusive. Here, we develop a novel ultrafast synthesis of sputtered SAzymes by in situ bombarding‐embedding technique. Using this method, sputtered copper (Cu) SAzymes (CuSA) is developed
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Living Self‐Assembly of Monodisperse Micron‐Sized Polymer Vesicles Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Hui Pan, Changxu Zhang, Wenfeng Jiang, Yongfeng Zhou
Artificial vesicles are recognized as powerful platforms for a large body of research across the disciplines of chemistry, physics and biology. Despite the great progress, control of the size distribution to make uniform vesicles remains fundamentally difficult due to the highly uncontrollable growth kinetics, especially for micron‐sized vesicles. Here we report a template‐free living self‐assembly
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Hierarchical Self‐assembly of Multidimensional Functional Materials from Sequence‐defined Peptoids Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Li Shao, Dehong Hu, Shao-Liang Zheng, Thi Kim Hoang Trinh, Wenhao Zhou, Haoyu Wang, Yanxu Zong, Changning Li, Chun-Long Chen
Hierarchical self‐assembly represents a powerful strategy for the fabrication of functional materials across various length scales. However, achieving precise formation of functional hierarchical assemblies remains a significant challenge and requires a profound understanding of molecular assembly interactions. In this study, we present a molecular‐level understanding of the hierarchical assembly of
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Building Co16‐N3‐based UiO‐MOF to Expand Design Parameters for MOF Photosensitization Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Guang-Chen Guo, Jiong-Peng Zhao, Song Guo, Wen-Xiong Shi, Fu-Chen Liu, Tong-Bu Lu, Zhi-Ming Zhang
The construction of secondary building units (SBUs) in versatile metal–organic frameworks (MOFs) represents a promising method for developing multi‐functional materials, especially for improving their sensitizing ability. Herein, we developed a dual small molecules auxiliary strategy to construct a high‐nuclear transition‐metal‐based UiO‐architecture Co16‐MOF‐BDC with visible‐light‐absorbing capacity
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Record High Iodate Anion Capture by a Redox‐Active Cationic Polymer Network Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Qi Guo, Jie Li, Yuting Zhao, Lingyi Li, Linwei He, Fuqiang Zhao, Fuwan Zhai, Mingxing Zhang, Long Chen, Zhifang Chai, Shuao Wang
As a critical radioactive anionic contaminant, traditional adsorbents primarily remove iodate (IO3‐) through ion exchange or hard acid‐hard base interactions, but suffer from limited affinity and capacity. Herein, employing the synergistic effect of ion exchange and redox, we successfully synthesized a redox‐active cationic polymer network (SCU‐CPN‐6, [C9H10O2N5•Cl]n) by merging guanidino groups with
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Crystalline Olefin‐Linked Chiral Covalent Organic Frameworks as a Platform for Asymmetric Catalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Ting He, Ivan Keng Wee On, Shuai Bi, Ziyue Huang, Jingjing Guo, Zhifang Wang, Yanli Zhao
The construction of olefin‐linked chiral covalent organic frameworks (COFs) with high crystallinity is highly desirable while remains great challenge due to the poor reversibility of the formation reaction for the olefin linkages during the in situ structural self‐healing process. Herein, we successfully synthesized two sets of enantiomeric olefin‐linked COFs. The chiral catalytic groups are uniformly
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Crown Ether Electrolyte Induced Li2O2 Amorphization for Low Polarization and Long Lifespan Li‐O2 batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Meng Li, Jiaxin Wu, Zichang You, Zhongqin Dai, Yuanfan Gu, Lei Shi, Meifen Wu, Zhaoyin Wen
Lithium‐oxygen batteries possess an extremely high theoretical energy density, rendering them a prime candidate for next‐generation secondary batteries. However, they still face multiple problems such as huge charge polarization and poor cycle life, which lay a significant gap between laboratory research and commercial applications. In this work, we adapt 15‐crown‐5 ether (C15) as solvent to regulate
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Silylenes with a small chalcogenide substituent: Tuning frontier orbital energies from O to Te Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Maximilian P. Müller, Alexander Hinz
The general synthesis of heteroleptic acyclic silylenes with a bulky carbazolyl substituent (dtbpCbz) is detailed and a series of compounds with a chalcogenide substituent of the type [(dtbpCbz)SiE16R] (E16R = OtBu, SEt, SePh, TePh) is reported. With the bulky carbazolyl substituent present, the chalcogenide moiety can be very small, as is shown by incorporating groups as small as ethyl, phenyl or
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Assembly of Glycopeptides in Living Cells Resembling Viral Infection for Cargo Delivery Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Feng Tian, Ruo-Chen Guo, Chunxia Wu, Xin Liu, Zeyu Zhang, Yamei Wang, Hao Wang, Gongyu Li, Zhilin Yu
Self‐assembly in living cells represents one versatile strategy for drug delivery; however, it suffers from the limited precision and efficiency. Inspired by viral traits, we here report a cascade targeting‐hydrolysis‐transformation (THT) assembly of glycosylated peptides in living cells holistically resembling viral infection for efficient cargo delivery and combined tumor therapy. We design a glycosylated
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Including the Ensemble of Unstructured Conformations in the Analysis of Protein's Native State by High‐Pressure NMR Spectroscopy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Frederic Berner, Michael Kovermann
The analysis of pressure induced changes in the chemical shift of proteins allows statements on structural fluctuations proteins exhibit at ambient pressure. The inherent issue of separating general pressure effects from structural related effects on the pressure dependence of chemical shifts has so far been addressed by considering the characteristics of random coil peptides on increasing pressure
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Bithiophene‐Functionalized Infrared Two‐Photon Absorption Metal Complexes as Single‐Molecule Platforms for Synergistic Photodynamic, Photothermal, and Chemotherapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Xue-Lian li, Meng-Fan wang, Li-Zhen Zeng, Guo-Kui Li, Run-Yu Zhao, Fu-Dan Liu, Yun Li, Yu-Fei Yan, Qishuai Liu, Zhao Li, Hongbin Zhang, Xiaoxia Ren, Feng Gao
A planar conjugated ligand functionalized with bithiophene and its Ru(II), Os(II), and Ir(III) complexes have been constructed as single‐molecule platform for synergistic photodynamic, photothermal, and chemotherapy. The complexes have significant two‐photon absorption at 808 nm and remarkable singlet oxygen and superoxide anion production in aqueous solution and cells when exposed to 808 nm infrared
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Enantiopure [6]‐Azairidahelicene by Dynamic Kinetic Resolution of a Configurationally Labile [4]‐Helicene Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Ariadna Pazos, Carlos M Cruz, Juan M. Cuerva, Ivan Rivilla, Fernando P. Cossío, Zoraida Freixa
A pair of enantiopure [6]‐azairidahelicenes incorporating chirality at the metal center and on the helicenic ligand were synthesized by dynamic kinetic resolution (dkr) of a configurationally labile [4]‐helicenic ligand (4‐(2‐pyridyl)‐benzo[g]phenanthrene, L1H) using bis‐cyclometalated chiral‐at‐metal only iridium(III) precursors as chiral inductors. The origin of the observed dkr is attributed to
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C(sp3)–H (N‐Phenyltetrazole)thiolation as an Enabling Tool for Molecular Diversification Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Ashley Zachmann, Justine Drappeau, Shubin Liu, Erik John Alexanian
Methods enabling the broad diversification of C(sp3)–H bonds from a common intermediate are especially valuable in chemical synthesis. Herein, we report a site‐selective (N‐phenyltetrazole)thiolation of aliphatic and (hetero)benzylic C(sp3)–H bonds using a commercially available disulfide to access N‐phenyltetrazole thioethers. The thioether products are readily elaborated in diverse fragment couplings
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The Role of Hydrogen Bonds in Thermally Responsive Crystallization‐Driven Template Autocatalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-24 Huimin Wu, Qing-Xuan Chen, Yang Su, Zhen Chen
Autocatalysis has been well recognized to implicate in the emergence of life and is intrinsic to the biomolecular replication. Recently, an efficient template autocatalysis driven by solvent‐free crystallization has been reported. Herein, we unveil the role of intermolecular hydrogen (H) bonds formed by amides in crystallization‐driven template autocatalysis (CDTA), which involves the autocatalytic
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Discovery of (±)-Penindolenes Reveals an Unusual Indole Ring Cleavage Pathway Catalyzed by P450 Monooxygenase Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Ling-Hong Meng, Takayoshi Awakawa, Xiao-Ming Li, Zhiyang Quan, Sui-Qun Yang, Bin-Gui Wang, Ikuro Abe
(±)-Penindolenes A–D (1–4), the first representatives of indole terpenoids featuring a γ-lactam skeleton, were isolated from the mangrove-derived endophytic fungus Penicillium brocae MA-231. Our bioactivity tests revealed their potent antimicrobial and acetylcholinesterase inhibitory activities. The biosynthetic reactions by the five enzymes PbaABCDE leading to γ-lactam ring formation were identified