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Intrarenal pH‐Responsive Self‐Assembly of Luminescent Gold Nanoparticles for Diagnosis of Early Kidney Injury Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Zhipeng Zhao, Kui He, Ben Liu, Wenyan Nie, Xiaoxi Luo, Jinbin Liu
Metabolic acidosis‐induced kidney injury (MAKI) is asymptomatic and lack of clinical biomarkers in early stage, but rapidly progresses to severe renal fibrosis and ultimately results in end‐stage kidney failure. Therefore, developing rapid and noninvasive strategies direct responsive to renal tubular acidic microenvironment rather than delayed biomarkers are essential for timely renoprotective interventions
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Converting Carbon Dioxide into Carbon Nanotubes by Reacting with Ethane Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Yong Yuan, Erwei Huang, Sooyeon Hwang, Ping Liu, Jingguang G. Chen
The urgency to mitigate environmental impacts from anthropogenic CO2 emissions has propelled extensive research efforts on CO2 reduction. The current work reports a novel approach involving transforming CO2 and ethane into carbon nanotubes (CNTs) using earth‐abundant metals (Fe, Co, Ni) at 750 °C. This route facilitates long‐term carbon storage via generating high‐value CNTs and produces valuable syngas
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Ultrastrong Graphene Sheets Assembled with Nanoconfined Water Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Zhiyong Tang
Highly ordered assembly of two‐dimensional (2D) nanoplatelets plays a key role in enhancing the mechanical properties of layered nanocomposites. Layer‐by‐layer (LbL) assembly, vacuum‐assisted filtration, and blade coating have been used to fabricate layered nanocomposites. However, the intrinsic wrinkles of 2D nanoplatelets and defects derived from assembling approaches make it difficult to align 2D
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Phase Engineering of High‐Entropy Alloy for Enhanced Electrocatalytic Nitrate Reduction to Ammonia Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Rong Zhang, Yaqin Zhang, Bo Xiao, Shaoce Zhang, Yanbo Wang, Huilin Cui, Chuan Li, Yue Hou, Ying Guo, Tao Yang, Jun Fan, Chunyi Zhi
Directly electrochemical conversion of nitrate (NO3−) is an efficient and environmentally friendly technology for ammonia (NH3) production but is challenged by highly selective electrocatalysts. High‐entropy alloys (HEAs) with unique properties are attractive materials in catalysis, particularly for multi‐step reactions. Herein, we first reported the application of HEA (FeCoNiAlTi) for electrocatalytic
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In‐situ Ultrafast Construction of Zinc Tungstate Interface Layer for Highly Reversible Zinc Anodes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Jin Cao, Haiyang Wu, Dongdong Zhang, Ding Luo, Lulu Zhang, Xuelin Yang, Jiaqian Qin, Guanjie He
Constructing artificial solid electrolyte interface on the Zn anode surface is recognized as an appealing method to inhibit zinc dendrites and side reactions, whereas the current techniques are complex and time‐consuming. Here, a robust and zincophilic zinc tungstate (ZnWO4) layer has been in situ constructed on the Zn anode surface (denoted as ZWO@Zn) by an ultrafast chemical solution reaction. Comprehensive
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Gas‐Phase Formation of Sulfurous Acid (H2SO3) in the Atmosphere Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Torsten Berndt, Erik H. Hoffmann, Andreas Tilgner, Hartmut Herrmann
Sulfurous acid (H2SO3) is known to be thermodynamically instable decomposing into SO2 and H2O. All attempts to detect this elusive acid in solution failed up to now. Reported H2SO3 formation from an experiment carried out in a mass spectrometer as well as results from theoretical calculations, however, indicated a possible kinetic stability in the gas phase. Here, it is shown experimentally that H2SO3
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Reaction, Recognition, Relay: Anhydride Hydrolysis Reported by Conformationally Responsive Fluorinated Foldamers in Micelles Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Benedicte Doerner, Flavio della Sala, Siyuan Wang, Simon John Webb
Natural membrane receptors are proteins that can report on changes in the concentration of external chemical messengers. Messenger binding to a receptor produces conformational changes that are relayed through the membrane into the cell; this information allows cells to adapt to changes in their environment. Artificial membrane receptors (R)‐1 and (S)‐1 are helical α‐aminoisobutyric acid (Aib) foldamers
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An in‐situ‐tag‐generation proximity labeling technology for recording cellular interactions Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Yunyan Yao, Ru Jia, Chuanming Liu, Haiqi Wang, Ting Li, Xiaocui Zheng, Tong Zhong, Nan Feng, Jiahui Sun, Ke Li, Ran Xie, Lijun Ding, Chao Yan, Lin Ding, Huangxian Ju
Obtaining information about cellular interactions is fundamental to the elucidation of physiological and pathological processes. Proximity labeling technologies have been widely used to report cellular interactions in situ; however, the reliance on addition of tag molecules typically restricts their application to regions where tags can readily diffuse, while the application in, for example, solid
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Reconstructing Solvation Structure by Steric Hindrance‐Coordination Push‐Pull of Dipolymer‐H2O‐Zn2+ toward Long‐life Aqueous Zinc‐Metal Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Die Luo, Xinyu Ma, Pan Du, Zuo Chen, Qiurui Lin, Yuhan Liu, Ben Niu, Xianru He, Xin Wang
Aqueous zinc‐metal batteries are prospective energy storge devices due to their intrinsically high safety and cost effectiveness. Yet, uneven deposition of zinc ions in electrochemical reduction and side reactions at the anode interface significantly hinder their development and application. Here, we propose a solvation‐interface attenuation strategy enabled by a frustrated tertiary amine amphiphilic
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Bottom‐up Growth of Convex Sphere with Adjustable Cu(0)/Cu(I) Interfaces for Effective C2 Production from CO2 Electroreduction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Huan Liu, Chenghan Yang, Tong Bian, Huijun Yu, Yuming Zhou, Yiwei Zhang
One challenge confronting the Cu2O catalysts in the electrocatalysis of carbon dioxide reduction reaction (CO2RR) is the reduction of active Cu(I) species, resulting in low selectivity and quick deactivation. In this study, we for the first time introduce a bottom‐up growth of convex sphere with adjustable Cu(0)/Cu(I) interfaces (Cux@Cu2O convex spheres). Interestingly, the interfaces are dynamically
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Photon Upconversion Cooperates with Downshifting in Chiral Systems: Modulation, Amplification, and Applications of Circularly Polarized Luminescence Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Tonghan Zhao, Pengfei Duan
Circularly polarized luminescence (CPL)‐active materials are increasingly recognized for their potential applications such as 3D imaging, data storage, and optoelectronic devices. Typically, CPL materials have required high‐energy (HE) photons for excitation to emit low‐energy (LE) circularly polarized light, a process known as downshifting CPL (DSCPL). However, the emergence of upconverted CPL (UCCPL)
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Interlayer Structure Manipulation of FeOCl/MXene with Soft/Hard Interface Design for Safe Water Production Using Dechlorination Battery Deionization Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-04 Jingjing Lei, Xiaochen Zhang, Junce Wang, Fei Yu, Mingxing Liang, Xinru Wang, Zhuanfang Bi, Guangyi Shang, Haijiao Xie, Jie Ma
Suffering from the susceptibility to decomposition, the potential electrochemical application of FeOCl has greatly been hindered. The rational design of the soft‐hard material interface can effectively address the challenge of stress concentration and thus decomposition that may occur in the electrodes during charging and discharging. Herein, interlayer structure manipulation of FeOCl/MXene using soft‐hard
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Formation of a Porous Crystalline Mg1‒ x Al2O y Overlayer on Metal Catalysts via Controlled Solid‐State Reactions for High‐temperature Stable Catalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Lihua Cai, Shanlei Han, Wenlong Xu, Si Chen, Xianxian Shi, Junling Lu
Catalyst deactivation by sintering and coking is a long‐standing issue in metal‐catalyzed harsh high‐temperature hydrocarbon reactions. Ultrathin oxide coatings of metal nanocatalysts have recently appeared attractive to address this issue, while the porosity of the overlayer is difficult to control to preserve the accessibility of embedded metal nanoparticles, thus often leading to a large decrease
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Eosinophil‐activating Semiconducting Polymer Nanoparticles for Cancer Photo‐immunotherapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Chi Zhang, Jingsheng Huang, Mengke Xu, Jie Yu, Wei Xin, Shasha He, Kanyi Pu
Eosinophils are important immune effector cells that affect T cell‐mediated antitumor immunity. However, the low frequency and restrained activity of eosinophils restricted the development of cancer immunotherapies. We herein report an eosinophil‐activating semiconducting polymer nanoparticle (SPNe) to improve photodynamic tumor immunogenicity, modulate eosinophil chemotaxis, and reinvigorate T‐cell
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A Stretchable and Tough Graphene Film Enabled by Mechanical Bond Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Chunyu Wang, Boyue Gao, Fuyi Fang, Wenhao Qi, Ge Yan, Jun Zhao, Wenbin Wang, Ruixue Bai, Zhaoming Zhang, Zhitao Zhang, Wenming Zhang, Xuzhou Yan
The pursuit of fabricating high‐performance graphene films has aroused considerable attention due to their potential for practical applications. However, developing both stretchable and tough graphene films remains a formidable challenge. To address this issue, we herein introduce mechanical bond to comprehensively improve the mechanical properties of graphene films, utilizing [2]rotaxane as the bridging
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ß‐Phenethylamine Synthesis via Latent Dual Electrophilicity of N‐Pyridinium Aziridines Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Samya Samanta, Promita Biswas, Braeden O'Bannon, David C Powers
ß‐Phenethylamines are widely represented in biologically and pharmacologically active organic small molecules. Here, we introduce N‐pyridinium aziridines as latent dual electrophiles for the synthesis of ß‐phenethylamines. Bromide‐promoted ring opening generates ß‐halopyridinium amines. Selective Ni‐catalyzed C–C cross‐coupling between organozinc nucleophiles and the benzylic C–Br electrophile affords
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Spin‐State Control in Dysprosium(III) Metallacrown Magnets via Thioacetal Modification Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Wei Deng, Si-Guo Wu, Ze-Yu Ruan, Ya-Ping Gong, Shan-Nan Du, Hai-Ling Wang, Yan-Cong Chen, Wei-Xiong Zhang, Jun-Liang Liu, Ming-Liang Tong
Integrating controllable spin states into single‐molecule magnets (SMMs) enables precise manipulation of magnetic interactions at a molecular level, but remains a synthetic challenge. Herein, we developed a 3d‐4f metallacrown (MC) magnet [DyNi5(quinha)5(Clsal)2(py)8](ClO4)∙4H2O (H2quinha = quinaldichydroxamic acid, HClsal = 5‐chlorosalicylaldehyde) wherein a square planar NiII is stabilized by chemical
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Active Oxygenated Structure‐Intensified CO2 Capture Enables Efficient Electrochemical Ethylene Production Over Carbon Nanofibers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Tingting Zhang, Jun Wang, Huishan Shang, Bing Zhang, Yanqiang Huang, Jing He, Xu Xiang
The pursuit of high efficacy C–C coupling during the electrochemical CO2 reduction reaction remains a tremendous challenge owing to the high energy barrier of CO2 activation and insufficient coverage of the desired intermediates on catalytic sites. Inspired by the concept of capture‐coupled CO2 activation, we fabricated quinone‐grafted carbon nanofibers via an in situ oxidative carbonylation strategy
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Metal Ions Trigger the Gelation of Cysteine‐Containing Peptide‐Appended Coordination Cages Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Meng Li, Huangtianzhi Zhu, Simone Adorinni, Weichao Xue, Andrew Heard, Ana M. Garcia, Slavko Kralj, Jonathan Russell Nitschke, Silvia Marchesan
We report a series of coordination cages that incorporate peptide chains at their vertices, prepared through subcomponent self‐assembly. Three distinct heterochiral tripeptide subcomponents were incorporated, each exhibiting an L–D–L stereoconfiguration. Through this approach, we prepared and characterized three tetrahedral metal‐peptide cages that incorporate thiol and methylthio groups. The gelation
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Probing Particle‐Carbon/Binder Degradation Behavior in Fatigued Layered Cathode Materials through Machine Learning Aided Diffraction Tomography Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Weibo Hua, Jinniu Chen, Dario Ferreira Sanchez, Björn Schwarz, Yang Yang, Anatoliy Senyshyn, Zhenguo Wu, Chong-Heng Shen, Michael Knapp, Helmut Ehrenberg, Sylvio Indris, Xiaodong Guo, Xiaoping Ouyang
Understanding how reaction heterogeneity impacts cathode materials during Li‐ion battery (LIB) electrochemical cycling is pivotal for unraveling their electrochemical performance. Yet, experimentally verifying these reactions has proven to be a challenge. To address this, we employed scanning μ‐XRD computed tomography to scrutinize Ni‐rich layered LiNi0.6Co0.2Mn0.2O2 (NCM622) and Li‐rich layered Li[Li0
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Fluorinated Surface Engineering towards High‐rate and Durable Potassium‐ion Battery Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Xixue Zhang, Feng Wu, Difan Fang, Renjie Chen, Li Li
Solid electrolyte interphase (SEI) crucially affects the rate performance and cycling lifespan, yet to date more extensive research is still needed in potassium‐ion batteries. We report an ultra‐thin and KF‐enriched SEI triggered by tuned fluorinated surface design in electrode. Our results reveal that fluorination engineering alters the interfacial chemical environment to facilitate inherited electronic
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A Gold(I)–Acetylene Complex Synthesised using Single‐Crystal Reactivity Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Chloe L Johnson, Daniel J Storm, Muhammad Arif Sajjad, Matthew R Gyton, Simon B Duckett, Stuart A Macgregor, Andrew S Weller, Miquel Navarro, Jesus Campos
Using single‐crystal to single‐crystal solid/gas reactivity the gold(I) acetylene complex [Au(L1)(η2‐HC≡CH)][BArF4] is cleanly synthesized by addition of acetylene gas to single crystals of [Au(L1)(CO)][BArF4] [L1 = tris‐2‐(4,4’‐di‐tert‐butylbiphenyl)phosphine, ArF = 3,5‐(CF3)2C6H3]. This simplest gold‐alkyne complex has been characterized by single crystal X‐ray diffraction, solution and solid‐state
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Aggregation Enhanced Thermally Activated Delayed Fluorescence through Spin‐Orbit Coupling Regulation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Wei Zhang, Shuai Li, Yujie Gong, Jiachen Zhang, Yujie Zhou, Jie Kong, Hongbing Fu, Meng Zhou
Integrating aggregation‐induced emission (AIE) into thermally activated delayed fluorescence (TADF) emitters holds great promise for the advancement of highly efficient organic light emitting diodes (OLEDs). Despite recent advancements, a thorough comprehension of the underlying mechanisms remains imperative for the practical application of such materials. In this work, we introduce a novel approach
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Organocatalytic Enantioselective 1,12‐Addition of Alkynyl Biphenyl Quinone Methides Formed In Situ Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Xing Wang, Boming Shen, Meiwen Liu, Ziyang Wang, Chang Liu, Pengfei Li, Peiyuan Yu, Wenjun Li
The chemistry of quinone methides formed in situ has been flourishing in recent years. In sharp contrast, the development and utilization of biphenyl quinone methides are rare. Herein, we achieved a remote stereocontrolled 1,12‐conjugate addition of biphenyl quinone methides formed in situ for the first time. In the presence of a suitable chiral phosphoric acid, alkynyl biphenyl quinone methides were
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Switchable Dual Circularly Polarized Luminescence in Through‐Space Conjugated Chiral Foldamers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Pingchuan Shen, Shaoshao Jiao, Zeyan Zhuang, Xiaobing Dong, Shaoxin Song, Jinshi Li, Ben Zhong Tang, Zujin Zhao
Organic materials with switchable dual circularly polarized luminescence (CPL) are highly desired because they can not only directly radiate tunable circularly polarized light themselves but also induce CPL for guests by providing chiral environment in self‐assembled structures or serving as the hosts for energy transfer systems. However, most organic molecules only exhibit single CPL and it remains
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Dimensional Regulation in Metal‐Free Perovskites by Compositional Engineering to Achieve Record Low X‐ray Detection Limits Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Pengxiang Dong, Chensheng Lin, Ning Ye, Min Luo
Utilizing the manipulation of perovskite dimensions has been proven as an effective approach in regulating perovskite properties. Nevertheless, achieving precise control over the dimensions of perovskites within the same system poses a significant challenge. In this study, we introduce a sophisticated method to attain precise dimensional control in metal‐free perovskites (MFPs), specifically through
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Controlling On‐Surface Photoactivity: The Impact of π‐Conjugation in Anhydride‐Functionalized Molecules on a Semiconductor Surface Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-03 Federico Frezza, Ana Sánchez-Grande, Sofia Canola, Anna Lamancová, Pingo Mutombo, Qifan Chen, Christian Wäckerlin, Karl-Heinz Ernst, Matthias Muntwiler, Nicola Zema, Marco Di Giovannantonio, Dana Nachtigallová, Pavel Jelínek
On‐surface synthesis has become a prominent method for growing low‐dimensional carbon‐based nanomaterials on metal surfaces. However, the necessity of decoupling organic nanostructures from metal substrates to exploit their properties requires either transfer methods or new strategies to perform reactions directly on inert surfaces. The use of on‐surface light‐induced reactions directly on semiconductor/insulating
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Gold‐Catalysed Heck Reaction: Fact or Fiction? Correspondence on “Unlocking the Chain Walking Process in Gold Catalysis” Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Peter H. M. Budzelaar, Manfred Bochmann, Martina Landrini, Luca Rocchigiani
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Zeolitic Imidazolate Frameworks as Solid‐State Nanomachines Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Joohan Nam, Seokjin Kim, Eunji Jin, Soochan Lee, Hye Jin Cho, Seung Kyu Min, Wonyoung Choe
Machines have continually developed with the needs of daily life and industrial applications. While the careful design of molecular‐scale devices often displays enhanced properties along with mechanical movements, controlling mechanics within solid‐state molecular structures remains a significant challenge. Here, we explore the distinct mechanical properties of zeolitic imidazolate frameworks (ZIFs)
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Back Cover: Crystal Engineering of MOF‐Derived Bimetallic Oxide Solid Solution Anchored with Au Nanoparticles for Photocatalytic CO2 Reduction to Syngas and C2 Hydrocarbons Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Ning‐Yu Huang, Bai Li, Duojie Wu, Zhen‐Yu Chen, Bing Shao, Di Chen, Yu‐Tao Zheng, Wenjuan Wang, Chunzhen Yang, Meng Gu, Lei Li, Qiang Xu
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Correspondence on “Organo‐Mediator Enabled Electrochemical Deuteration of Styrenes” Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Simon Kolb, Daniel B. Werz
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Ligand Isomerization Driven Electrocatalytic Switching Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Alagar Raja Kottaichamy, Mohammed Azeezulla Nazrulla, Muskan Parmar, Ravikumar Thimmappa, Mruthyunjayachari Chattanahalli Devendrachari, Chathakudath Prabhakaran Vinod, Michael Volokh, Harish Makri Nimbegondi Kotresh, Menny Shalom, Musthafa Ottakam Thotiyl
The prevailing view about molecular catalysts is that the central metal ion is responsible for the reaction mechanism and selectivity, whereas the ligands mainly affect the reaction kinetics. Here, we question this paradigm and show that ligands have a dramatic influence on the selectivity of the product. We show how even a seemingly small change in ligand isomerization sharply alters the selectivity
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Kinase Inhibition via Small Molecule‐Induced Intramolecular Protein Cross‐Linking Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Xuan Wang, Jie Sun, Huisi Huang, Guanghui Tang, Peng Chen, Menghua Xiang, Lin Li, Zhi-Min Zhang, Liqian Gao, Shao Q. Yao
Remarkable progress has been made in the development of cysteine‐targeted covalent inhibitors. In kinase drug discovery, covalent inhibitors capable of targeting other nucleophilic residues (i.e. lysine, or K) has emerged in recent years. Besides a highly conserved catalytic lysine, almost all human protein kinases possess an equally conserved glutamate/aspartate (e.g. E/D) that forms a K‐E/D salt
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Total Synthesis of Lissodendoric Acid A Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Francesca M. Ippoliti, Laura G. Wonilowicz, Nathan J. Adamson, Evan R. Darzi, Joyann S. Donaldson, Daniel J. Nasrallah, Milauni M. Mehta, Andrew V. Kelleghan, K. N. Houk, Neil K. Garg
We describe a full account of our synthetic strategy leading to the first total synthesis of the manzamine alkaloid lissodendoric acid A . These efforts demonstrate that strained cyclic allenes are valuable synthetic building blocks and can be employed efficiently in total synthesis.
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Alkene 1,3‐Difluorination via Transient Oxonium Intermediates Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Alice C. Dean, E. Harvey Randle, Andrew J. D. Lacey, Guiherme A. Marczak Giorio, Sayad Doobary, Benjamin D. Cons, Alastair Lennox
The 1,3‐difunctionalization of unactivated alkenes is an under‐explored transformation that leads to moieties that are otherwise challenging to prepare. Herein, we report a hypervalent iodine‐mediated 1,3‐difluorination of homoallylic (aryl) ethers to give unreported 1,3‐difluoro‐4‐oxy groups with moderate to excellent diastereoselectivity. The transformation proceeds through a different mode of reactivity
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Solvation Properties of Neutral Gold Species in Supercritical Water Studied By THz Spectroscopy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Jan Noetzel, Philipp Schienbein, Harald Forbert, Dominik Marx
Supercritical water provides distinctly different solvation properties compared to what is known from liquid water. Despite its prevalence deep in the Earth’s crust and its role in chemosynthetic ecosystems in the vicinity of hydrothermal vents, molecular insights into its solvation mechanisms are still very scarce compared to what is known for liquid water. Recently, neutral metal particles have been
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[2+1] Cycloadditions Modulate the Hydrophobicity of Ni‐N4 Single‐Atom Catalysts for Efficient CO2 Electroreduction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Siyan Shu, Tao Song, Cheng Wang, Hao Dai, Lele Duan
Microenvironment regulation of M‐N4 single‐atom catalysts (SACs) is a promising way to tune their catalytic properties toward the electrochemical CO2 reduction reaction. However, strategies that can effectively introduce functional groups around the M‐N4 sites through strong covalent bonding and under mild reaction conditions are highly desired. Taking the hydrophilic Ni‐N4 SAC as a representative
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Pyridinium‐Yne Click Polymerization: A Facile Strategy toward Functional Poly(Vinylpyridinium Salt)s with Multidrug‐Resistant Bacteria Killing Ability Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Benzhao He, Ying Li, Meng Li, Miaomiao Kang, Xinyue Liu, Jiachang Huang, Dong Wang, Jacky W. Y. Lam, Ben Zhong Tang
Polymeric materials with antibacterial properties hold great promise for combating multidrug‐resistant bacteria, which pose a significant threat to public health. However, the synthesis of most antibacterial polymers typically involves complicated and time‐consuming procedures. In this study, we demonstrate a simple and efficient strategy for synthesizing functional poly(vinylpyridinium salt)s via
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A Stable Chichibabin Diradicaloid with Near‐Infrared Emission Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Xingmao Chang, Mona E. Arnold, Rémi Blinder, Julia Zolg, Jonathan Wischnat, Joris van Slageren, Fedor Jelezko, Alexander J. C. Kuehne, Max von Delius
Conjugated molecules with multiple radical centers such as the iconic Chichibabin diradicaloid hold promise as building blocks in materials for quantum sensing and quantum information processing. However, it is a considerable challenge to design simple analogues of the Chichibabin hydrocarbon that are chemically inert, exhibit high diradical character and emit light at a distinct wavelength that may
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Electrocatalytic Formal C(sp2)–H Alkylations via Nickel‐Catalyzed Cross‐Electrophile Coupling with Versatile Arylsulfonium Salts Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Takuya Michiyuki, Simon L. Homölle, Neeraj Kumar Pandit, Lutz Ackermann
Producing sp3‐hybridized carbon‐enriched molecules is of particular interest due to their high success rate in clinical trials. The installation of aliphatic chains onto aromatic scaffolds was accomplished by nickel‐catalyzed C(sp2)–C(sp3) cross‐electrophile coupling with arylsulfonium salts. Thus, simple non‐prefunctionalized arenes could be alkylated through the formation of aryldibenzothiophenium
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Intermolecular Enantioselective Amination Reactions Mediated by Visible Light and a Chiral Iron Porphyrin Complex Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Hussayn Ahmed, Biki Ghosh, Stefan Breitenlechner, Malte Feßner, Christian Merten, Thorsten Bach
In the presence of 1 mol% of a chiral iron porphyrin catalyst, various 3‐arylmethyl‐substituted 2‐quinolones and 2‐pyridones underwent an enantioselective amination reaction (20 examples; 93‐99% ee). The substrates were used as the limiting reagents, and fluorinated aryl azides (1.5 equiv.) served as nitrene precursors. The reaction is triggered by visible light which allows a facile dediazotation
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Anion‐Reinforced Solvation Structure Enables Stable Operation of Ether‐Based Electrolyte in High‐Voltage Potassium Metal Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Mengjia Gu, Xunzhu Zhou, Qian Yang, Shenxu Chu, Lin Li, Jiaxin Li, Yuqing Zhao, Xing Hu, Shuo Shi, Zhuo Chen, Yu Zhang, Shulei Chou, Kaixiang Lei
Electrolytes with anion‐dominated solvation are promising candidates to achieve dendrite‐free and high‐voltage potassium metal batteries. However, it's challenging to form anion‐reinforced solvates at low salt concentrations. Herein, we construct an anion‐reinforced solvation structure at a moderate concentration of 1.5 M with weakly coordinated cosolvent ethylene glycol dibutyl ether. The unique solvation
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Stabilizing Few‐Atom Platinum Clusters by Zinc Single‐Atom‐Glue for Efficient Anti‐Markovnikov Alkene Hydrosilylation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Ruilong Li, Ge Yu, Ze Lin, Xingen Lin, Junyi Du, Xiaoping Gao, Chenliang Su, Yuen Wu
Few‐atom metal clusters (FAMCs) exhibit superior performance in catalyzing complex molecular transformations due to their special spatial environments and electronic states, compared to single‐atom catalysts (SACs). However, achieving the efficient and accurate synthesis of FAMCs while avoiding the formation of other species, such as nanoparticles and SACs, still remains challenges. Herein, we report
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NETosis‐Inspired Cell Surface‐Constrained Framework Nucleic Acids Traps (FNATs) for Cascaded Extracellular Recognition and Cellular Behavior Modulation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Hangsheng Gong, Yihan Zhang, Yuan Xue, Bowen Fang, Yuting Li, Xudong Zhu, Yi Du, Pai Peng
Upon pathogenic stimulation, activated neutrophils release nuclear DNA into the extracellular environment, forming web‐like DNA structures known as neutrophil extracellular traps (NETs), which capture and kill bacteria, fungi, and cancer cells. This phenomenon is commonly referred to as NETosis. Inspired by this, we introduce a cell surface‐constrained web‐like framework nucleic acids traps (FNATs)
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Cobalt‐Mediated Photochemical C−H Arylation of Pyrroles Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Julia Märsch, Sebastian Reiter, Thomas Rittner, Rafael E. Rodriguez-Lugo, Maximilian Whitfield, Daniel J. Scott, Roger Jan Kutta, Patrick Nuernberger, Regina de Vivie-Riedle, Robert Wolf
Precious metal complexes remain ubiquitous in photoredox catalysis (PRC) despite concerted efforts to find more earth‐abundant catalysts and replacements based on 3d metals in particular. Most otherwise plausible 3d metal complexes are assumed to be unsuitable due to short‐lived excited states, which has led researchers to prioritize the pursuit of longer excited‐state lifetimes through careful molecular
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Patterned Photonic Actuators with Dynamic Shape‐Morphing and Color‐Changing Capabilities Fabricated by Athermal Embossing Technology Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-02 Nina Qian, Jun Hu, Shuai Huang, Zhiyang Liu, Meng Wang, Patrick Keller, Hong Yang
Stimuli‐responsive patterned photonic actuators, characterized by their patterned nano/microscale structures and capacity to demonstrate synergistic color changes and shape morphing in response to external stimuli, have attracted intense scientific attention. However, traditional patterned photonic actuator systems still face limitations such as cumbersome and time‐consuming preparation processes and
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Innovative Approach to Chiral Polyurethanes: Asymmetric Copolymerization with Isocyanates Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-01 Yong-Qiang Teng, Bai-Hao Ren, Ye Liu, Jie Gao, Wei-Min Ren, Xiao-Bing Lu
The introduction of nitrogen‐containing functional groups to chiral polymer backbones enables the tailoring of physical properties and offers opportunities for further post‐polymerization modification. However, the substrate scope of such polymers is extremely limited because monomers having nitrogen‐containing groups can change coordination state with respect to the metal centers, thus decreasing
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Vibration‐Dependent Dual‐Phosphorescent Cu4 Nanocluster with Remarkable Piezochromic Behavior Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-01 Xiao-Jing Zhang, Meng-En Sun, Fang Sun, Yan Jin, Xi-Yan Dong, Si Li, Hai-Yang Li, Gaosong Chen, Yongping Fu, Yonggang Wang, Qing Tang, Yuchen Wu, Lei Jiang, Shuang-Quan Zang
The dual emission (DE) characteristics of atomically precise copper nanoclusters (Cu NCs) are of significant theoretical and practical interest. Despite this, the underlying mechanism driving DE in Cu NCs remains elusive, primarily due to the complexities of excited state processes. Herein, a novel [Cu4(PPh3)4(C≡C‐p‐NH2C6H4)3]PF6 (Cu4) NC, shielded by alkynyl and exhibiting DE, was synthesized. Hydrostatic
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tert‐Butyl as a Functional Group: Non‐Directed Catalytic Hydroxylation of Sterically Congested Primary C−H Bonds Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-01 Siu-Chung Chan, Andrea Palone, Massimo Bietti, Miquel Costas
The tert‐butyl group is a common aliphatic motif extensively employed to implement steric congestion and conformational rigidity in organic and organometallic molecules. Because of the combination of a high bond dissociation energy (~ 100 kcal mol‐1) and limited accessibility, in the absence of directing groups, neither radical nor organometallic approaches are effective for the chemical modification
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Synthesis of Unsymmetrical Trisulfides from S‐Substituted Sulphenylthiosulphates Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-01 Shuaishuai Liang, Liye Ma, Zihao Guo, Fanmin Liu, Zijian Lin, Wen-bin Yi
Trisulfide unit is widely found in natural products and has garnered attention due to the unique pharmacological and physiochemical properties. However, despite limited progress, widely applicable approaches for constructing unsymmetrical trisulfides have so far remain scarce. In this work, an easy‐to‐prepare, solid‐state and scalable reagent, S‐substituted sulphenylthiosulphate, has been developed
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Thermal and photoinduced radical cascade annulation using aryl isonitriles: An approach to quinoline‐derived benzophosphole oxides Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Shyam Kumar Banjare, Lena Lezius, Elena Sophia Horst, Dirk Leifert, Constantin Gabriel Daniliuc, Fatmah Alasmary, Armido Studer
Herein, we present a radical cascade addition cyclization sequence to access quinoline‐based benzophosphole oxides from ortho‐alkynylated aromatic phosphine oxides using various aryl isonitriles as radical acceptors and inexpensive tert‐butyl‐hydroperoxide (TBHP) as a terminal oxidant in the presence of a catalytic amount of silver acetate. Alternatively, the same cascade can be realized through a
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Autophagy‐Inducing MoO3‐x Nanowires Boost Photothermal‐Triggered Cancer Immunotherapy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Lizhen He, Qi Chen, Qichen Lu, Meijin Yang, Bin Xie, Tianfeng Chen, Xun Wang
Autophagy could play suppressing role in cancer therapy by facilitating release of tumor antigens from dying cells and inducing immunogenic cell death (ICD). Therefore, discovery and rational design of more effective inducers of cytotoxic autophagy is expected to develop new strategies for finding innovative drugs for precise and successful cancer treatment. Herein, we develop MoO3‐x nanowires (MoO3‐x
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Purely Organic Room‐Temperature Phosphorescence Molecule for High‐Performance Non‐Doped Organic Light‐Emitting Diodes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Xiaoluo Peng, Peng Zou, Jiajie Zeng, Xing Wu, Dian Xie, Yan Fu, Dezhi Yang, Dongge Ma, Ben Zhong Tang, Zujin Zhao
Purely organic molecules with room‐temperature phosphorescence (RTP) are potential luminescent materials with high exciton utilization for organic light‐emitting diodes (OLEDs), but those exhibiting superb electroluminescence (EL) performances are rarely explored, mainly due to their long phosphorescence lifetimes. Herein, a robust purely organic RTP molecule, 3,6‐bis(5‐phenylindolo[3,2‐a]carbazol
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Mechanical‐Force‐Induced Non‐spontaneous Dehalogenative Deuteration of Aromatic Iodides Enabled by Using Piezoelectric Materials as a Redox Catalyst Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Ruiling Qu, Shan Wan, Xuemei Zhang, Xiaohong Wang, Li Xue, Qingqing Wang, Gui-Juan Cheng, Lunzhi Dai, Zhong Lian
The development of green and efficient deuteration methods is of great significance for various fields such as organic synthesis, analytical chemistry, and medicinal chemistry. Herein, we have developed a dehalogenative deuteration strategy using piezoelectric materials as catalysts in a solid‐phase system under ball‐milling conditions. This non‐spontaneous reaction is induced by mechanical force.
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Ligand Meta‐Anchoring Strategy in Metal‐Organic Frameworks for Remarkable Promotion of Quantum Yields Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Qicheng Yu, Herman H. Y. Sung, Feng Gao, Ian D. Williams, Jacky W. Y. Lam, Jianwei Sun, Ben Zhong Tang
Aggregation is a conventional method to enhance the quantum yields (QYs) of pure organic luminophores due to the restriction of intramolecular motions (RIM). However, how to realize RIM in metal‐organic frameworks (MOFs) is still unclear and challenging. In this work, the ligand meta‐anchoring strategy is first proposed and proved to be an effective and systematic approach to restrict the intramolecular
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Metal Poly(heptazine imides) as Multifunctional Photocatalysts for Solar Fuel Production Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Christian Mark Pelicano, Markus Antonietti
Solar‐driven photocatalysis employing particulate semiconductors represents a promising approach for sustainable production of valuable chemical feedstock. Metal poly(heptazine imide) (MPHI), a novel 2D ionic carbon nitride, has been recognized as an emerging photocatalyst with distinctive properties. In this minireview, we first delineate the forefront innovations of MPHI photocatalysts, spanning
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Built‐in Electric Fields in Heterostructured Lamellar Membranes Enable Highly Efficient Rejection of Charged Mass Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Chongchong Chen, Xiaoli Wu, Jingjing Chen, Siyu Liu, Yongzheng Wang, Wenjia Wu, Jie Zhang, Jingtao Wang, Zhongyi Jiang
Separation membranes with homogeneous charge channels are the mainstream to reject charged mass by forming electrical double layer (EDL). However, the EDL often compresses effective solvent transport space and weakens channel‐ion interaction. Here, built‐in electric fields (BIEFs) are constructed in lamellar membranes by assembling the heterostructured nanosheets, which contain alternate positively‐charged
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Sucrose‐Powered Liposome Nanosensors for Urinary Glucometer‐Based Monitoring of Cancer Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Dongtao Zhou, Zhibin Zhang, Liqing Pan, Yanyi Wang, Jingjing Yang, Yanfeng Gao, Yujun Song
Timely detection of early‐stage cancer holds immense potential in enhancing prognostic outcomes. There is an increasing desire for versatile tools to enable simple, sensitive, and cost‐effective cancer detection. By exploiting the extraintestinal metabolic inertness and efficiency renal clearance of sucrose, we designed a liposome nanosensor using sucrose as a messenger to convert tumor‐specific esterase
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A Versatile Microfluidic Platform for Extravasation Studies Based on DNA Origami – Cell Interactions Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Miguel García-Chamé, Parvesh Wadhwani, Juliana Pfeifer, Ute Schepers, Christof Niemeyer, Carmen M. Domínguez
The adhesion of circulating tumor cells (CTCs) to the endothelial lumen and their extravasation to surrounding tissues are crucial in the seeding of metastases and remain the most complex events of the metastatic cascade to study. Integrins expressed on CTCs are major regulators of the extravasation process. This knowledge is primarily derived from animal models and biomimetic systems based on artificial
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Glycol Monomethyl Ether‐Substituted Carbazolyl Hole‐Transporting Material for Stable Inverted Perovskite Solar Cells with Efficiency of 25.52% Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-30 Hui Zhou, Weiling Wang, Yuwei Duan, Rui Sun, Yong Li, Zhuang Xie, Dongfang Xu, Meizi Wu, Youliang Wang, Hongxiang Li, Qunping Fan, Yang Peng, Yao Yao, Chentong Liao, Qiang Peng, Shengzhong Liu, Zhike Liu
Organic self‐assembled molecules (OSAMs) based hole transporting materials play a pivotal role in achieving highly efficient and stable inverted perovskite solar cells (IPSCs). However, the reported carbazol‐based OSAMs have serious drawbacks, such as poor solubility in alcohol solution, worse matched energy arrangement with perovskite, and limited molecular species, which greatly limit the device