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Studies on the Biomimetic Synthesis of Marine Ladder Polyethers via Endo‐Selective Epoxide‐to‐Epoxonium Ring‐Opening Cascades Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Jia-Xi Xiao, Feng-Xing Li, Shu-Jian Ren, Jin Qu
Marine ladder polyethers have attracted the attention of chemists and biologists because of their potent biological activities. Synthetic chemists have attempted to construct their polyether frameworks by epoxide ring‐opening cascades, as Nakanishi hypothesis describes. However, Baldwin’s rules of ring closure state that exo‐selective intramolecular cyclization of epoxy alcohols is preferred over endo‐selective
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Concomitant Near‐Infrared Photothermy and Photoluminescence of Rod‐Shaped Au52(PET)32 and Au66(PET)38 Synthesized Concurrently Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Wanmiao Gu, Yue Zhou, Wenying Wang, Qing You, Wentao Fan, Yan Zhao, Guoqing Bian, Runguo Wang, Liang Fang, Nan Yan, Nan Xia, Lingwen Liao, Zhikun Wu
Gold nanoclusters exhibiting concomitant photothermy (PT) and photoluminescence (PL) under near‐infrared (NIR) light irradiation are rarely reported, and some fundamental issues remain unresolved for such materials. Herein, we concurrently synthesized two novel rod‐shaped Au nanoclusters, Au52(PET)32 and Au66(PET)38 (PET = 2‐phenylethanethiol), and precisely revealed that their kernels were 4 × 4 ×
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Spirobifluorene Trimers : High Triplet Pure Hydrocarbon Hosts for Highly Efficient Blue Phosphorescent Organic Light‐Emitting Diodes. Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 denis Ari, Yue-Jian yang, cassandre Quinton, zuoquan Jiang, Dong-Ying Zhou, Cyril Poriel
Pure aromatic hydrocarbon materials (PHC) represent a new generation of host materials for phosphorescent OLEDs (PhOLEDs), free of heteroatoms. They reduce the molecular complexity, can be easily synthesized and are an important direction towards robust devices. As heteroatoms can be involved in bonds dissociations in operating OLEDs through exciton induced degradation process, developing novel PHCs
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Redox Approaches to Carbene Generation in Catalytic Cyclopropanation Reactions Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Mingxin Liu, Christopher Uyeda
Transition metal‐catalyzed carbene transfer reactions have a century‐old history in organic chemistry and are a primary method for the synthesis of cyclopropanes. Much of the work in this field has focused on the use of diazo compounds and related precursors, which can transfer a carbene fragment to a catalyst with concomitant loss of a stable byproduct. Despite the utility of this approach, there
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Stereodivergent Construction of 1,5/1,7‐Nonadjacent Tetrasubstituted Stereocenters Enabled by Pd/Cu‐Cocatalyzed Asymmetric Heck Cascade Reaction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Panpan Li, Zijiao Liu, Xiaohong Huo, Wanbin Zhang
The construction of chiral motifs containing nonadjacent stereocenters in an enantio‐ and diastereoselective manner has long been a challenging task in synthetic chemistry, especially with respect to their stereodivergent synthesis. Herein, we describe a protocol that enables the enantio‐ and diastereoselective construction of 1,5/1,7‐nonadjacent tetrasubstituted stereocenters through a Pd/Cu‐cocatalyzed
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Bioorthogonal Delivery of Carbon Disulfide in Living Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Ruohan Zhao, Yinghan Chen, Yong Liang
Carbon disulfide (CS2) is an environmental pollutant, which is deadly hazardous to the workers under chronic or acute exposure. However, the toxicity mechanisms of CS2 are still unclear due to the scarcity of biocompatible donors, which can release CS2 in cells. Here we developed the first bioorthogonal CS2 delivery system based on the “click‐and‐release” reactions between mesoionic 1,3‐thiazolium‐5‐thiolates
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Enantio‐ and Z‐Selective δ‐Hydroarylation of Aryl‐Substituted 1,3‐Dienes via Rh‐Catalyzed Conjugate Addition Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Hima Kozhummal, Sandip Kumar Das, Christopher Cooze, Rylan J. Lundgren
Metal‐catalyzed enantioselective conjugate arylations of electron‐poor alkenes are highly selective processes for C(sp2)–C(sp3) bond formation. δ‐Selective hydroarylations of electron‐poor 1,3‐dienes are less well developed and reactions that deliver high enantioselectivity while giving single alkene isomer products are elusive. Here we report the Rh‐catalyzed δ‐arylation of aryl‐substituted 1,3‐dienes
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Engineering Low Volume Resuscitants for the Prehospital Care of Severe Hemorrhagic Shock Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Trey J. Pichon, Xu Wang, Ethan E. Mickelson, Wen-Chia Huang, Shayna L. Hilburg, Sarah Stucky, Melissa Ling, Alexander E. St. John, Kristyn M. Ringgold, Jessica M. Snyder, Lilo D. Pozzo, Maggie Lu, Nathan J. White, Suzie Pun
Globally, traumatic injury is a leading cause of suffering and death. The ability to curtail damage and ensure survival after major injury requires a time‐sensitive response balancing organ perfusion, blood loss, and portability, underscoring the need for novel therapies for the prehospital environment. Currently, there are few options available for damage control resuscitation (DCR) of trauma victims
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Biocatalytic Strategy for the Highly Stereoselective Synthesis of Fluorinated Cyclopropanes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Juan D Villada, Jadab Majhi, Valentin Lehuédé, Michelle E Hendricks, Katharina Neufeld, Veronica Tona, Rudi Fasan
Fluorinated cyclopropanes are highly desired pharmacophores in drug discovery owing to the rigidity nature of the cyclopropane ring and the beneficial effects of C–F bonds on the pharmacokinetic properties, cell permeability, and metabolic stability of drug molecules. Herein a biocatalytic strategy for the stereoselective synthesis of mono‐fluorinated and gem‐difluoro cyclopropanes is reported though
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Electrochemical generation of aryl radicals from organoboron reagents enabled by pulsed electrosynthesis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Maxime Boudjelel, Jessica Zhong, Lorenzo Ballerini, Ian Vanswearingen, Rossul Al-Dhufari, Christian Malapit
Aryl radicals play a pivotal role as reactive intermediates in chemical synthesis, commonly arising from aryl halides and aryl diazo compounds. Expanding the repertoire of sources for aryl radical generation to include abundant and stable organoboron reagents would significantly advance radical chemistry and broaden their reactivity profile. While traditional approaches utilize stoichiometric oxidants
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Selective Macrocyclization of Unprotected Peptides with an Ex Situ Gaseous Linchpin Reagent Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Yuxuan Ding, Simon S. Pedersen, Haofan Wang, Baorui Xiang, Yixian Wang, Zhi Yang, Yuxiang Gao, Emilia Morosan, Matthew R. Jones, Han Xiao, Zachary T. Ball
Peptide cyclization has dramatic effects on a variety of important properties, enhancing metabolic stability, limiting conformational flexibility, and altering cellular entry and intracellular localization. The hydrophilic, polyfunctional nature of peptides creates chemoselectivity challenges in macrocyclization, especially for natural sequences without biorthogonal handles. Herein, we describe a gaseous
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An Amphiphilic Cell‐Penetrating Macrocycle for Efficient Cytosolic Delivery of Proteins, DNA and CRISPR Cas9 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Somayah Qutub, Imtiyaz Bhat, Batoul Maatouk, Basem Moosa, Kashif Nawaz, Escarlet Diaz Galicia, Aliyah Fakim, Weibin Lin, Raik Grünberg, Stefan Arold, Niveen M. Khashab
The discovery of safe platforms that can circumvent the endocytic pathway is of great significance for biological therapeutics that are usually degraded during endocytosis. Here we show that self‐assembled and dynamic macrocycles can passively diffuse through the cell membrane and deliver a broad range of biologics including proteins, CRISPR Cas9 and ssDNA directly to the cytosol while retaining their
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Engineering Ultrathin CuxS Layer on Planar Sb2S3 Photocathode to Enhance Photoelectrochemical Transformation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Shuai Zhou, Li-Jun Zhang, Jian Li, Chen-Ho Tung, Li-Zhu Wu
Sb2S3 has been extensively used as light absorber for photoelectrochemical cell. However, its p‐type nature may result in the formation of Schottky junction with substrates, thus hindering the collection of photogenerated holes. Herein, an ultrathin CuxS layer is successfully engineered as the bottom junction for Sb2S3 for the first time. Capitalizing on its impressive electrical properties and superior
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Symmetry‐breaking of Dibenzo[b,d]thiophene Sulfone Enhancing Polaron Generation for Boosted Photocatalytic Hydrogen Evolution Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Wei-Cheng Lin, Yi-Hsiang Wu, Yu-En Sun, Mohamed M. Elsenety, Wan-Chi Lin, Jui-Chen Yen, Hung-Kai Hsu, Bo-Han Chen, Hung-Yi Huang, Chia-An Chang, Tse-Fu Huang, Ying-Rang Zhuang, Yuan-Ting Tseng, Kun-Han Lin, Shang-Da Yang, Chi-Hua Yu, Ho-Hsiu Chou
The current bottleneck in the development of efficient photocatalysts for hydrogen evolution is the limited availability of high‐performance acceptor units. Over the past nine years, dibenzo[b,d]thiophene sulfone (DBS) has been the preferred choice for the acceptor unit. Despite extensive exploration of alternative structures as potential replacements for DBS, a superior substitute remains elusive
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Elevated Water Oxidation by Cation Leaching Enabled Tunable Surface Reconstruction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Songzhu Luo, Chencheng Dai, Yike Ye, Qian Wu, Jiarui Wang, Xiaoning Li, Shibo Xi, Zhichuan J. Xu
Water electrolysis is one promising and eco‐friendly technique for energy storage, yet its overall efficiency is hindered by the sluggish kinetics of oxygen evolution reaction (OER). In response, developing strategies to boost OER catalyst performance is crucial. With the advances in characterization techniques, an extensive phenomenon of surface structure evolution into an active amorphous layer was
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Creating High‐entropy Single Atoms on Transition Disulfides through Substrate‐induced Redox Dynamics for Efficient Electrocatalytic Hydrogen Evolution Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 zhaoyan luo, Yirun Guo, Changjie He, Yi Guan, Lei Zhang, Yongliang Li, Qianling Zhang, Chuanxin He, Xueliang Sun, Xiangzhong Ren
The controllable anchoring of multiple metal single‐atoms (SAs) into a single support exhibits scientific and technological opportunities,while marrying the concentration‐complex multimetallic SAs and high‐entropy SAs (HESAs) into one SAC system remains a substantial challenge.Here, we present a substrate‐mediated SAs formation strategy to successfully fabricate a library of multimetallic SAs and HESAs
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Influence of Donor Skeleton on Intramolecular Electron Transfer Amount for Efficient Perovskite Solar Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-16 Shengwei Geng, Jialong Duan, Naimin Liu, Hui Li, Xixi Zhu, Xingxing Duan, Qiyao Guo, Jie Dou, Benlin He, Yuanyuan Zhao, Qunwei Tang
The passivation of the defects derived from rapid‐crystallization with electron‐donating molecules is always a prerequisite to obtain desirable perovskite films for efficient and stable solar cells, thus, the in‐depth understanding on the correlations between molecular structure and passivation capacity is of great importance for screening passivators. Here, we introduce the double‐ended amide molecule
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Corrigendum: Electrochemical Nickel‐Catalyzed Hydrogenation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15
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Corrigendum: Electrochemical Nickel‐Catalyzed Hydrogenation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15
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Chemoenzymatic Synthesis of 2‐Aryl Thiazolines from 4‐Hydroxybenzaldehydes Using Vanillyl Alcohol Oxidases Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Haowen Zhang, Shuhan Xie, Jun Yang, Ning Ye, Feng Gao, Fabrice Gallou, Lei Gao, Xiaoguang Lei
Nitrogen heterocycles are commonly found in bioactive natural products and drugs. However, the biocatalytic tools for nitrogen heterocycle synthesis are limited. Herein, we report the discovery of vanillyl alcohol oxidases (VAOs) as efficient biocatalysts for the one‐pot synthesis of 2‐aryl thiazolines from various 4‐hydroxybenzaldehydes and aminothiols. The wild‐type biocatalyst features a broad scope
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Strong Swelling and Symmetrization in Siliceous Zeolites due to Hydrogen Insertion at High Pressure Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Mario Santoro, Jérôme Rouquette, Marco Fabbiani, Francesco di Renzo, Benoît Coasne, Weiwei Dong, Konstantin Glazyrin, Julien Haines
Hydrogen and helium saturate the 1D pore systems of the high‐silica (Si/Al>30) zeolites Theta‐One (TON), and Mobile‐Twelve (MTW) at high pressure based on x‐ray diffraction, Raman spectroscopy and Monte Carlo simulations. In TON, a strong 22% volume increase occurs above 5 GPa with a transition from the collapsed P21 to a symmetrical, swelled Cmc21 form linked to an increase in H2 content from 12 H2/unit
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Enantioselective Synthesis of Sulfinamidines via Asymmetric Nitrogen Transfer from N‐H Oxaziridines to Sulfenamides Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Marc Fimm, Fumito Saito
Sulfinamidines are promising aza‐SIV chiral building blocks in asymmetric synthesis and drug discovery. However, no report has documented their enantioselective synthesis. Here we present an enantioselective synthesis of sulfinamidines via electrophilic amination of sulfenamides using an enantiopure N‐H oxaziridine. The resulting enantiomerically enriched primary sulfinamidines are configurationally
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On Tautomerism and Amphoterism: An In‐Depth Structural and Physicochemical Characterization of Ammeline and Some of Its Salts Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Thaddäus Koller, Simon M.J. Endraß, Markus Rösch, Kristian Witthaut, Thomas M. Klapötke, Wolfgang Schnick
Ammeline is a simple, readily available, molecular compound, which has been known for nearly 200 years. Despite that, no proper structural characterization of ammeline has been conducted so far. For this reason, the prevalent tautomeric form of ammeline in the solid remained unknown to this date. In the course of this study, its crystal structure was finally established by single‐crystal X‐ray diffraction
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An Enzymatic Prodrug‐like Route to Thio and Selenoamides Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Keishi Ishida, Agnieszka Litomska, Kyle L. Dunbar, Christian Hertweck
6‐Thioguanine (6TG) is a clinically used antitumor agent that was rationally designed as a DNA‐targeting antimetabolite, but it also occurs naturally. 6TG is a critical virulence factor produced by Erwinia amylovorans, a notorious plant pathogen that causes fire blight of pome fruit trees. The biosynthesis of the rare thioamide metabolite involves an adenylating enzyme (YcfA) and a sulfur‐mobilizing
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All‐Inorganic sp‐Chain Ligands: Isoelectronic B/N Analogues of E. O. Fischer's Alkynylcarbynes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Luis Walter, Krzysztof Radacki, Rian Dewhurst, Rüdiger Bertermann, Maik Finze, Holger Braunschweig
Borylation of a tungsten‐bound N2 ligand and halide abstraction provides access to a cationic complex with an unprecedented linear NNBR ligand. This complex undergoes [3+2] cycloaddition with azides, and an unexpected chain‐extension reaction with an iminoborane, leading to a complex with a five‐atom B/N chain. These two [NNBR]‐containing complexes, inorganic analogues of E. O. Fischer's alkynylcarbynes
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Hidden Impurities Generate False Positives in Single Atom Catalyst Imaging Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Nicolò Allasia, Sean Michael Collins, Quentin Mathieu Ramasse, Gianvito Vilé
Single‐atom catalysts (SACs) are an emerging class of materials, leveraging maximum atom utilization and distinctive structural and electronic properties to bridge heterogeneous and homogeneous catalysis. Direct imaging methods, such as aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy, are commonly applied to confirm the atomic dispersion of active sites
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Enantioselective Synthesis of Heteroatom‐Linked Non‐Biaryl Atropisomers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Abdelati Naghim, Jean RODRIGUEZ, Olivier Chuzel, Gaëlle Chouraqui, Damien Bonne
Atropisomers hold significant fascination, not only for their prevalence in natural compounds but also for their biological importance and wide‐ranging applications as chiral materials, ligands, and organocatalysts. While biaryl and heterobiaryl atropisomers are commonly studied, the enantioselective synthesis of less abundant heteroatom‐linked non‐biaryl atropisomers presents a formidable challenge
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Lone‐Pair‐p Bond Strength Unveiled by a Combined Experimental and Computational Study Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Cristian L. Gutiérez-Peña, Ana Gutiérrez-Blanco, Dmitry G. Gusev, Macarena Poyatos, Eduardo Victor Peris
A series of naphthalene‐diimide (NDI) and perylene‐diimide (PDI) connected bis‐N‐heterocyclic carbene complexes of iridium (III) have been prepared and fully characterized. The analysis of their NMR spectroscopic features, together their molecular structures show that these species display lone pair‐p interactions between the chloride ligands of the Ir(III) complex and the heterocycles of the NDI/PDI
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Constructing High‐performance Cobalt‐based Environmental Catalysts from Spent Lithium‐Ion Batteries: Unveiling Overlooked Roles of Copper and Aluminum from Current Collectors Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Jianxing Liang, Kan Li, Feng Shi, Jingdong Li, Jia-nan Gu, Yixin Xue, Chenyu Bao, Mingming Guo, Jinping Jia, Maohong Fan, Tonghua Sun
Converting spent lithium‐ion batteries (LIBs) cathode materials into environmental catalysts has drawn more and more attention. Herein, we fabricated a Co3O4‐based catalyst from spent LiCoO2 LIBs (Co3O4‐LIBs) and found that the role of Al and Cu from current collectors on its performance is nonnegligible. The density functional theory calculations confirmed that the doping of Al and/or Cu upshifts
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[22]Pentaphyrins(2.0.1.1.0) Displaying N‐Fusion, Pyrrole‐Rearrangement, and Dimerization Reactions Upon Oxidation and Metalation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Jinchao Chen, Le Liu, Yutao Rao, Ling Xu, Mingbo Zhou, Bangshao Yin, Soji Shimizu, Daiki Shimizu, Atsuhiro Osuka, Jianxin Song
Exploration of expanded porphyrins with unprecedented reactivities has remained important. Here [22]pentaphyrins(2.0.1.1.0) were synthesized as a constitutional isomer of sapphyrin by acid‐catalyzed cyclization of 1,14‐dibromo‐5,10‐diaryltripyrrin with 1,2‐di(pyrro‐2‐ly)ethenes. These pentaphyrins display roughly planar structures and varying aromaticities depending upon the vinylene structures. The
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Highly Stable MOF‐Type Lead Halide Luminescent Ferroelectrics Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Chen Sun, Yukong Li, Jinlin Yin, Dongyang Li, Chao Wu, Chi Zhang, Honghan Fei
Lead halide molecular ferroelectrics represent an important class of luminescent ferroelectrics, distinguished by their high chemical and structural tunability, excellent processability and distinctive luminescent characteristics. However, their inherent instability, prone to decomposition upon exposure to moisture and light, hinders their broader ferroelectric applications. Herein, for the first time
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A Processible and Ultrahigh‐temperature Organic Photothermal Material through Spontaneous and Quantitative [2+2] Cycloaddition–Cycloreversion Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Pengbo Han, He Xu, Guiquan Zhang, Anjun Qin, Ben Zhong Tang
Energy conversion, particularly light to heat conversion, has garnered significant attention owing to its prospect in renewable energy exploitation and utilization. Most previous efforts have focused on developing organic photothermal materials for low‐temperature applications, whereas the importance of simplifying the preparation methods of photothermal materials and enhancing their maximum photothermal
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π‐Conjugated Nanohoops: A new generation of curved materials for organic electronics Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Rupam ROy, clement Brouillac, emmanuel jacques, cassandre Quinton, Cyril Poriel
Nanohoops, cyclic association of π‐conjugated systems to form a hoop‐shaped molecule, have been widely developed in the last 15 years. Beyond the synthetic challenge, the strong interest towards these molecules arise from their radially‐oriented π‐orbitals, which provide singular properties to these fascinating structures. Thanks to their particular cylindrical arrangement, this new generation of curved
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Strong and Tough MXene Bridging‐induced Conductive Nacre Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Jia Yan, Tianzhu Zhou, Xinyu Yang, Zejun Zhang, Lei Li, Zhaoyong Zou, Zhengyi Fu, Qunfeng Cheng
Nacre is a classic model, providing an inspiration for fabricating high‐performance bulk nanocomposites with the two‐dimensional platelets. However, the “brick” of nacre, aragonite platelet, is an ideal building block for making high‐performance bulk nanocomposites. Herein, we demonstrated a strong and tough conductive nacre through reassembling aragonite platelets with bridged by MXene nanosheets
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Controlling Tin Halide Perovskite Oxidation Dynamics in Solution for Perovskite Optoelectronic Devices Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Mohammad Kahaj Khaja Nazeeruddin, Shun Tian, Guixiang Li, Roland C. Turnell-Ritson, Zhaofu Fei, Aurélien Bornet, Paul J. Dyson
As a leading contender to replace lead halide perovskites, tin‐based perovskites have demonstrated ever increasing performance in solar cells and light‐emitting diodes (LEDs). They tend to be processed with dimethyl sulfoxide (DMSO) solvent, which has been identified as a major contributor to the Sn(II) oxidation during film fabrication, posing a challenge to the further improvement of Sn‐based perovskites
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Alumina ‐ Stabilized SEI and CEI in Potassium Metal Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Pengcheng Liu, Hongchang Hao, Aditya Singla, Bairav S. Vishnugopi, John Watt, Partha P. Mukherjee, David Mitlin
Aluminum oxide (Al2O3) nanopowder is spin‐coated onto both sides of commercial polypropene separator to create artificial solid‐electrolyte interphase (SEI) and artificial cathode electrolyte interface (CEI) in potassium metal batteries (KMBs). This significantly enhances the stability, including of KMBs with Prussian Blue (PB) cathodes. For example, symmetric cells are stable after 1,000 cycles at
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Ionic Hydrogen Bond‐Assisted Catalytic Construction of Nitrogen Stereogenic Center via Formal Desymmetrization of Remote Diols Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-15 Zhongfu Luo, Minghong Liao, Wei Li, Sha Zhao, Kun Tang, Pengcheng Zheng, Yonggui Robin Chi, Xinglong Zhang, Xingxing Wu
The control of noncarbon stereogenic centers is of profound importance owing to their enormous interest in bioactive compounds and chiral catalyst or ligand design for enantioselective synthesis. Despite various elegant approaches have been achieved for construction of S‐, P‐, Si‐ and B‐stereocenters over the past decades, the catalyst‐controlled strategies to govern the formation of N‐stereogenic
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Sequential Selective Dissolution of Coinage Metals in Recyclable Ionic Media Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Anže Zupanc, Joseph Install, Timo Weckman, Marko M. Melander, Mikko J. Heikkilä, Marianna Kemell, Karoliina Honkala, Timo Juhani Repo
Coinage metals Cu, Ag and Au are essential for modern electronics and their recycling from waste materials is becoming increasingly important to guarantee the security of their supply. Designing new sustainable and selective procedures that would substitute currently used processes is crucial. Here, we describe an unprecedented approach for the sequential dissolution of single metals from Cu, Ag and
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NbC Nanoparticles Decorated Carbon Nanofibers as Highly Active and Robust Heterostructural Electrocatalysts for Ammonia Synthesis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Zhihao Zhang, Aihui Niu, Yaxin Lv, Haoran Guo, Jun Song Chen, Qian Liu, Kai Dong, Xuping Sun, Tingshuai Li
Transition‐metal carbides with metallic properties have been extensively used as electrocatalysts due to their excellent conductivity and unique electronic structures. Herein, NbC nanoparticles decorated carbon nanofibers (NbC@CNFs) are proposed as an efficient and robust catalyst for electrochemical synthesis of ammonia from nitrate/nitrite reduction, which achieves a high Faradaic efficiency (FE)
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Industrial‐scale Hard Carbon Designed to Regulate Electrochemical Polarization for Fast Sodium Storage Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Chun Wu, Yunrui Yang, Yinghao Zhang, Hui Xu, Wenjie Huang, XiangXi He, Qinghang Chen, Huanhuan Dong, Lin Li, Xingqiao Wu, Shulei Chou
Given the merits of abundant resource, low cost and high electrochemical activity, hard carbons have been regarded as one of the most commercializable anode material for sodium‐ion batteries (SIBs). However, poor rate capability is one of the main obstacles that severely hinder its further development. In addition, the relationships between preparation method, material structure and electrochemical
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Surface Coordination Modulated Morphological Anisotropic Engineering of Iron‐Benzoquinone Frameworks for Lithium‐Ion Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Jiarun Geng, Yaohui Huang, Yihe Guo, Haixia Li, Fujun Li
Morphological anisotropic engineering is powerful to synthesize metal‐organic frameworks (MOF) with versatile physicochemical properties for diverse applications ranging from gas storage/separation to electrocatalysis and batteries, etc. Herein, we developed a carbon substrate guided strategy for facet‐anisotropic growth of Fe‐THBQ (tetrahydroxy‐1,4‐benzoquinone) frameworks, which is built with cubic
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Upgrading Electrolyte Antioxidant Chemistry by Constructing Potential Scaling Relationship Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Ruhong Li, Zunchun Wu, Shuoqing Zhang, Jia Liu, Liwu Fan, Tao Deng, Lixin Chen, Xiulin Fan
Rational design of advanced electrolytes to improve the high‐voltage capability has been attracting wide attention as one critical solution to enable next‐generation high‐energy‐density batteries. However, the limited understanding of electrolyte antioxidant chemistry as well as the lack of valid quantization approaches have resulted in knowledge gap, which hinders the formulation of new electrolytes
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Size Control of Chiral Nanospheres Obtained via Nanoprecipitation of Helical Poly(phenylacetylene)s in the Absence of Surfactants Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Manuel Núñez-Martínez, Manuel Fernández-Míguez, Emilio Quiñoá, Felix Freire
Nanostructuration of dynamic helical polymers such as poly(phenylacetylene)s (PPAs) depends on the secondary structure adopted by the polymer and the functional group used to connect the chiral pendant to the PPA backbone. Thus, while PPAs with dynamic and flexible scaffolds (para‐ and meta‐substituted, ω1< 165º) generate by nanoprecipitation low polydisperse nanospheres with controllable size at different
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Hydrazone‐Linked Covalent Organic Frameworks Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Huifen Zhuang, Can Guo, Jianlin Huang, Liwen Wang, Zixi Zheng, Hai-Ning Wang, Yifa Chen, Ya-Qian Lan
Hydrazone‐linked covalent organic frameworks (COFs) with structural flexibility, heteroatomic sites, post‐modification ability and high hydrolytic stability have attracted great attention from scientific community. Hydrazone‐linked COFs, as a subclass of Schiff‐base COFs, was firstly reported in 2011 by Yaghi’s group and later witnessed prosperous development in various aspects. Their adjustable structures
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Coupling CO2 Reduction and Acetyl‐CoA Formation: The Role of a CO Capturing Tunnel in Enzymatic Catalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Jakob Ruickoldt, Jae-Hun Jeoung, Maik Alexander Rudolph, Frank Lennartz, Julian Kreibich, Reinhard Schomäcker, Holger Dobbek
The bifunctional CO‐dehydrogenase/acetyl‐CoA synthase (CODH/ACS) complex couples the reduction of CO2 to the condensation of CO with a methyl‐moiety and CoA to acetyl‐CoA. Catalysis occurs at two sites connected by a tunnel transporting the CO. Here, we investigated how the bifunctional complex and its tunnel support catalysis using the CODH/ACS from Carboxydothermus hydrogenoformans as a model. Although
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Tuning Adsorbate‐Mediated Strong Metal‐Support Interaction by Oxygen Vacancy: A Case Study in Ru/TiO2 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Juan Li, Lin Zhang, Xingda An, Kai Feng, Xuchun Wang, Jiari He, Yang Huang, Jingjing Liu, Liang Zhang, Binhang Yan, Chaoran Li, Le He
The adsorbate‐mediated strong metal‐support interaction (A‐SMSI) offers a reversible means of altering the selectivity of supported metal catalysts, thereby providing a powerful tool for facile modulation of catalytic performance. However, the fundamental understanding of A‐SMSI remains inadequate and methods for tuning A‐SMSI are still in their nascent stages, impeding its stabilization under reaction
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Electrochemiluminescence Microscopy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Neso Sojic, Sara Knežević, Dongni Han, Baohong Liu, Dechen Jiang
Electrochemiluminescence (ECL) is rapidly evolving from an analytical method into an optical microscopy. The orthogonality of the electrochemical trigger and the optical readout distinguishes it from classic microscopy and electrochemical techniques, owing to its near‐zero background, remarkable sensitivity, and absence of photobleaching and phototoxicity. In this review, we summarize the recent advances
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3D‐Printed Carbon Nanoneedle Electrodes for Dopamine Detection in Drosophila Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Zijun Shao, He Zhao, Kelly E. Dunham, Qun Cao, Nickolay V. Lavrik, B. Jill Venton
In vivo electrochemistry in small brain regions or synapses requires nanoelectrodes with long straight tips for submicron scale measurements. Nanoelectrodes can be fabricated using a Nanoscribe two‐photon printer, but annealed tips curl if they are long and thin. We propose a new pulling‐force strategy to fabricate a straight carbon nanoneedle structure. A micron‐width bridge is printed between two
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One‐Pot Synthesis of 1,3‐Cyclohexadienes by Birch Reduction in the Presence of Carbonyl Compounds Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Torsten Linker, Tobias Krüger-Braunert
Birch reductions are well‐known transformations of arenes, applied for large scale synthesis of 1,4‐cyclohexadienes. Herein, we describe first reactions of benzoic acids in the presence of carbonyl compounds, affording aldol products in moderate to high yields. Alkyl aldehydes give the expected nonconjugated dienes by reaction at the α‐position. Interestingly, the intermediately formed enolate attacks
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Bioinspired Tetranuclear Manganese Cubane Complex as an Efficient Molecular Electrocatalyst for Two‐electron Water Oxidation Towards Hydrogen Peroxide Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Tongshuai Wang, Wenxiu Li, Gang Wu
Stable homogenous two‐electron water oxidation electrocatalysts are highly demanded to understand the precise mechanism and reaction intermediates of electrochemical H2O2 production.Here we report a tetranuclear manganese complex with a cubane structure which can electrocatalyze water oxidation to hydrogen peroxide under alkaline and neutral conditions. Such a complex demonstrates an optimal Faradaic
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Acyl Phosphates as Chemically Fueled Building Blocks for Self‐Sustaining Protocells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-14 Oleksii Zozulia, Christine M. E. Kriebisch, Brigitte A. K. Kriebisch, Héctor Soria-Carrera, Kingu Rici Ryadi, Juliana Steck, Job Boekhoven
Lipids spontaneously assemble into vesicle‐forming membranes. Such vesicles serve as compartments for even the simplest living systems. Vesicles have been extensively studied for constructing synthetic cells or as models for protocells—the cells hypothesized to have existed before life. These compartments exist almost always close to equilibrium. Life, however, exists out of equilibrium. In this work
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Graphical Abstract: Angew. Chem. Int. Ed. 21/2024 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13
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Scalable Precise Nanofilm Coating and Gradient Al Doping Enable Stable Battery Cycling of LiCoO2 at 4.7 V Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Jia Yao, Yuyu Li, Tiantian Xiong, Yameng Fan, Lingfei Zhao, Xiangxin Cheng, Yunan Tian, Lele Li, Yan Li, Wen Zhang, Peng Yu, Pingmei Guo, Zehui Yang, Jian Peng, Lixing Xue, Jiazhao Wang, Zhaohuai Li, Ming Xie, Huakun Liu, Shixue Dou
The quest for smart electronics with higher energy densities has intensified the development of high‐voltage LiCoO2 (LCO). Despite their potential, LCO materials operating at 4.7 V faces critical challenges, including interface degradation and structural collapse. Herein, we propose a collective surface architecture through precise nanofilm coating and doping that combines an ultra‐thin LiAlO2 coating
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Protonation of an Imine‐linked Covalent Organic Framework for Efficient H2O2 Photosynthesis under Visible Light up to 700 nm Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Qiong Zhu, Li Shi, Zhuo Li, Guisheng Li, Xiaoxiang Xu
Covalent organic frameworks (COFs) are promising photocatalysts for H2O2 production from water via oxygen reduction reactions (ORR). The design of COFs for efficient H2O2 production indubitably hinges on an in‐depth understanding of their ORR mechanisms. In this work, taking an imine‐linked COF as an example, we demonstrate that protonation of the functional units such as imine, amine, and triazine
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Quantification of native lignin structural features with gel‐phase 2D‐HSQC0 reveals lignin structural changes during extraction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Claire L. Bourmaud, Stefania Bertella, Anna Bosch Rico, Steven D. Karlen, John Ralph, Jeremy Luterbacher
Our ability to study and valorize the lignin fraction of biomass is hampered by the fundamental and still unmet challenge of precisely quantifying native lignin’s structural features. Here, we developed a rapid elevated‐temperature 1H–13C Heteronuclear Single‐Quantum Coherence Zero (HSQC0) NMR method that enables this precise quantification of native lignin structural characteristics even with whole
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A General Strategy for Sustainable 3D Printing Based on A Multifunctional Photoinitiator Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Dajun Xiong, Pengfei Ruan, Zongan Li, Wenbin Yi, Jieping Wang
A multifunctional photoinitiator is presented, offering precise control over light‐induced polymerization initiation at 450 nm and material degradation at 365 nm. This is accomplished by covalently linking photoactive bis(acyl)phosphane oxide and photocleavable o‐nitrobenzyl ether moieties onto the surface of γ‐cyclodextrin. Upon degradation, the resulting linear polymers can be easily re‐dissolved
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Highly Efficient Self‐Assembly of Heterometallic [2]Catenanes and Cyclic Bis[2]catenanes via Orthogonal Metal‐Coordination Interactions Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Qian Feng, Rui Ding, Yali Hou, Zeyuan Zhang, Yafei Zhang, Haifei Liu, Chenxing Guo, Gang He, Bo Zheng, Yanmin Zhang, Mingming Zhang
Although catenated cages have been widely constructed due to their unique and elegant topological structures, cyclic catenanes formed by the connection of multiple catenane units have been rarely reported. Herein, based on the orthogonal metal‐coordination‐driven self‐assembly, we prepare a series of heterometallic [2]catenanes and cyclic bis[2]catenanes, whose structures are clearly evidenced by single‐crystal
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Stepwise Protonation of Three‐Dimensional Covalent Organic Frameworks for Enhancing Hydrogen Peroxide Photosynthesis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Pengfei Dong, Xinyu Xu, Taikang Wu, Rengan Luo, Weisu Kong, Zhiyuan Xu, Shuai Yuan, Jun Zhou, Jianping Lei
Three‐dimensional covalent organic frameworks (3D COFs), recognized for their tailorable structures and accessible active sites, offer a promising platform for developing advanced photocatalysts. However, the difficulty in the synthesis and functionalization of 3D COFs hinders their further development. In this study, we present a series of 3D‐bcu‐COFs with 8 connected porphyrin units linked by linear
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An Alkyne‐bridged Covalent Organic Framework Featuring Interactive Pockets for Bromine Capture Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Ankita De, Sattwick Haldar, Johannes Schmidt, Saeed Amirjalayer, Fanny Reichmayr, Nikolaj Lopatik, Leonid Shupletsov, Eike Brunner, Inez Weidinger, Andreas Schneemann
The high degree of corrosivity and reactivity of bromine, which is released from various sources poses a serious threat to the environment. Moreover, its coexistence with iodine forming an equilibrium compound, iodine monobromide (IBr) necessitates the selective capture of bromine from halogen mixtures. The electrophilicity of halogens to π‐electron rich structures enabled us to strategically design