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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 : 2024-05-14 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 : 2024-05-14 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 : 2024-05-14 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 : 2024-05-14 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 : 2024-05-14 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 : 2024-05-14 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 : 2024-05-14 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
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Leveraging DNA‐encoded Cell‐mimics for Environment‐adaptive Transmembrane Channel Release‐induced Cell Death Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Chunying Li, Dan Wang, Haiyan Gao, Ting Fu, Lei He, Da Han, Weihong Tan
The advancement of cell‐mimic materials, which can forge sophisticated physicochemical dialogues with living cells, has unlocked a realm of intriguing prospects within the fields of synthetic biology and biomedical engineering. Inspired by the evolutionarily acquired ability of T lymphocytes to release perforin and generate transmembrane channels on targeted cells for killing, herein we present a pioneering
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Ruthenium Nanoclusters and Single Atoms on α‐MoC/N‐Doped Carbon Achieves Low‐input/Input‐free Hydrogen Evolution via Decoupled/Coupled Hydrazine Oxidation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Yapeng Li, Shuwen Niu, Peigen Liu, Rongrong Pan, Huaikun Zhang, Nazir Ahmad, Yi Shi, Xiao Liang, Mingyu Cheng, Shenghua Chen, Junyi Du, Maolin Hu, Dingsheng Wang, Wei Chen, Yadong Li
The hydrazine oxidation‐assisted H2 evolution method promises low‐input and input‐free hydrogen production. However, developing high‐performance catalysts for hydrazine oxidation (HzOR) and hydrogen evolution (HER) is challenging. Here, we introduce a bifunctional electrocatalyst α‐MoC/N‐C/RuNSA, merging ruthenium (Ru) nanoclusters (NCs) and single atoms (SA) into cubic α‐MoC nanoparticles‐decorated
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Efficient Enzymatic Synthesis of Carbamates in Water Using Promiscuous Esterases/Acyltransferases Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Hannes Meinert, Florian Oehlschläger, Clemens Cziegler, Jan Rockstroh, Irene Marzuoli, Serena Bisagni, Michael Lalk, Thomas Bayer, Hans Iding, Uwe Bornscheuer
Biocatalysis provides an attractive approach to facilitate synthetic reactions in aqueous media. Motivated by the discovery of promiscuous aminolysis activity of esterases, we exploited the esterase from Pyrobaculum calidifontis VA1 (PestE) for the synthesis of carbamates from different aliphatic, aromatic, and arylaliphatic amines and a set of carbonates such as dimethyl‐, dibenzyl‐, or diallyl carbonate
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Fluorophilic Sigma(σ)‐Lock Self‐Healable Copolymers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Samriddhi Gaikwad, Marek W Urban
Although F‐containing molecules and macromolecules are often used in molecular biology to increase the binding with Lewis acidic groups by introducing favorable C‐F dipoles, there is virtually no experimental evidence and limited understanding of the nature of these interactions, especially their role in synthetic polymeric materials. These studies elucidate the molecular origin of inter‐ and intra‐chain
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An Asymmetric Coumarin‐Anthracene Conjugate as Efficient Fullerene‐Free Acceptor for Organic Solar Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Nirmala Niharika Bhuyan, Shyam Shankar S., Subhra Jyoti Panda, Chandra Shekhar Purohit, Rahul Singhal, Ganesh D. Sharma, Amaresh Mishra
Asymmetric wide‐bandgap fullerene‐free acceptors (FFAs) play a crucial role in organic solar cells (OSCs). Here, we designed and synthesized a simple asymmetric coumarin‐anthracene conjugate named CA‐CN with optical bandgap of 2.1 eV in a single‐step condensation reaction. Single crystal X‐ray structure analysis confirms various multiple intermolecular non‐covalent interactions. The molecular orbital
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A Fluorine‐Effect‐Enabled Photocatalytic 4‐Exo‐Trig Cyclization Cascade to Access Fluoroalkylated Cyclobutanes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Yulu Zhou, Zhenzhen Wu, Jinming Xu, Zuxiao Zhang, Hanliang Zheng, Gangguo Zhu
Cyclobutanes are popular structural units in bioactive compounds and versatile intermediates in synthetic chemistry, but their synthesis is challenging owing to high ring strain. In this study, a novel method for highly regio‐ and diastereoselective synthesis of fluoroalkylcyclobutanes bearing vicinal quaternary and tertiary stereocenters is realized by a photocatalytic 4‐exo‐trig cyclization cascade
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In Situ Self‐Assembled Active and Stable Ir@MnOx/La0.7Sr0.3Cr0.9Ir0.1O3‐δ Interfaces for CO2 Electrolysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Yuxiang Shen, Shuo Wang, Rongtan Li, Houfu Lv, Mingrun Li, Na Ta, Xiaomin Zhang, Yuefeng Song, Qiang Fu, Guoxiong Wang, Xinhe Bao
Solid oxide electrolysis cells are prospective approaches for CO2 utilization but face significant challenges due to the sluggish reaction kinetics and poor stability of the fuel electrodes. Herein, we strategically addressed the long‐standing trade‐off phenomenon between enhanced exsolution and improved structural stability via topotactic ion exchange. The surface dynamic reconstruction of the MnOx/La0
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Influence of Ti‐incorporated Zeolite Topology and Pore Condensation on Vapor Phase Propylene Epoxidation Kinetics with Gaseous H2O2 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Ohsung Kwon, E. Zeynep Ayla, David S. Potts, David Flaherty
Vapor‐phase propylene (C3H6) epoxidation kinetics with hydrogen peroxide (H2O2) strongly reflects the physical properties of Ti‐incorporated zeolite catalysts and the presence of spectating molecules (“solvent”) near active sites even without a bulk liquid phase. Steady‐state turnover rates of C3H6 epoxidation and product selectivities vary by orders of magnitudes, depending on the zeolite silanol
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Interfacial Super‐Assembly of Vacancy Engineered Ultrathin‐Nanosheets toward Nanochannels for Smart Ion Transport and Salinity Gradient Power Conversion Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Abuduheiremu Awati, Ran Yang, Ting Shi, Shan Zhou, Xin Zhang, Hui Zeng, Yaokang Lv, Kang Liang, Lei Xie, Dazhang Zhu, Mingxian Liu, Biao Kong
Ion‐selective nanochannel membranes assembled from two‐dimensional (2D) nanosheets hold immense promise for power conversion using salinity gradient. However, they face challenges stemming from insufficient surface charge density, which impairs both permselectivity and durability. Herein, we present a novel vacancy‐engineered, oxygen‐deficient NiCo layered double hydroxide (NiCoLDH)/cellulose nanofibers‐wrapped
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Designing Dual‐Site Catalysts for Selectively Converting CO2 into Methanol Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Wenjie Cui, Fei Wang, Xiao Wang, Yuou Li, Xiaomei Wang, Yi Shi, Shuyan Song, Hongjie Zhang
The variability of CO2 hydrogenation reaction demands new potential strategies to regulate the fine structure of the catalysts for optimizing the reaction pathways. Herein, we report a dual‐site strategy to boost the catalytic efficiency of CO2‐to‐methanol (MA) conversion. A new descriptor, τ, was initially established for screening the promising candidates with low‐temperature activation capability
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Dynamic Near‐Infrared Circularly Polarized Luminescence Encoded by Transient Supramolecular Chiral Assemblies Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Qian Wang, Hanren Xu, Zhen Qi, Ju Mei, He Tian, Da-Hui Qu
Circularly polarized luminescence (CPL) is promising for applications in many fields. However, most systems involving CPL are within the visible range; near‒infrared (NIR) CPL‒active materials, especially those that exhibit high glum values and can be controlled spatially and temporally, are rare. Herein, dynamic NIR‒CPL with a glum value of 2.5[[EQUATION]]10‒2 was achieved through supramolecular coassembly
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Unveiling Dynamic Structure and Bond Evolutions in BiOIO3 Photocatalysts during CO2 Reduction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Yujie Lan, Yajun Zhang, Xiaojuan Huang, Yingpu Bi
We have established a correlation between photocatalytic activity and dynamic structure/bond evolutions of BiOIO3‐based photocatalysts during CO2 reduction by combining operando X‐ray diffraction with photoelectron spectroscopy. More specifically, the selective photo‐deposition of PtOx species on BiOIO3 (010) facets could effectively promote the electron enrichment on Bi active sites of (100) facets
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Unraveling Stoichiometry Effect in Nickel‐Tungsten Alloys for Efficient Hydrogen Oxidation Catalysis in Alkaline Electrolytes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Ye-Hua Wang, Yu Yang, Fei-Yue Gao, Xiao-Long Zhang, Lei Zhu, Hui-Kun Yan, Peng-Peng Yang, Min-Rui Gao
Anion‐exchange membrane fuel cells provide the possibility to use platinum group metal‐free catalysts, but the anodic hydrogen oxidation reaction (HOR) suffers from sluggish kinetics and its source is still debated. Here, over nickel‐tungsten (Ni‐W) alloy catalysts, we show that the Ni:W ratio greatly governs the HOR performance in alkaline electrolyte. Experimental and theoretical studies unravel
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A General Iron‐Catalyzed Decarboxylative Oxygenation of Aliphatic Carboxylic Acids Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Luca Mareen Denkler, Meghana Aladahalli Shekar, Tak Shing Jason Ngan, Luke Wylie, Dinar Abdullin, Tobias Hett, Frank Hendrik Pilz, Barbara Kirchner, Olav Schiemann, Patrycja Kielb, Ala Bunescu, Marianne Engeser, Gregor Schnakenburg
We report an iron‐catalyzed decarboxylative C(sp3)–O bond‐forming reaction under mild, base‐free conditions with visible light irradiation. The transformation uses readily available and structurally diverse carboxylic acids, iron photocatalyst, and 2,2,6,6‐tetramethylpiperidine 1‐oxyl (TEMPO) derivatives as oxygenation reagents. The process exhibits a broad scope in acids possessing a wide range of
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Reverse Separation of Carbon Dioxide and Acetylene in Two Isostructural Copper Pyridine‐Carboxylate Frameworks Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Jing-Hong Li, You-Wei Gan, Jun-Xian Chen, Rui-Biao Lin, Yisi Yang, Hui Wu, Wei Zhou, Banglin Chen, Xiao-Ming Chen
Separating acetylene from carbon dioxide is important but highly challenging due to their similar molecular shapes and physical properties. Adsorptive separation of carbon dioxide from acetylene can directly produce pure acetylene but is hardly realized because of relatively polarizable acetylene binds more strongly. Here, we reverse the CO2 and C2H2 separation by adjusting the pore structures in two
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Highly Efficient Acidic Electrosynthesis of Hydrogen Peroxide at Industrial‐Level Current Densities Promoted by Alkali Metal Cations Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-13 Peike Cao, Xueyang Zhao, Yanming Liu, Haiguang Zhang, Kun Zhao, Shuo Chen, Hongtao Yu, Fan Dong, Nathaniel N. Nichols, Jingguang G. Chen, Xie Quan
Acidic H2O2 synthesis through electrocatalytic 2e– oxygen reduction presents a sustainable alternative to the energy‐intensive anthraquinone oxidation technology. Nevertheless, acidic H2O2 electrosynthesis suffers from low H2O2 Faradaic efficiencies primarily due to the competing reactions of 4e– oxygen reduction to H2O and hydrogen evolution in environments with high H+ concentrations. Here, we demonstrate
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Designed Additive to Regulated Crystallization for High Performance Perovskite Solar Cell Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-11 Yang Cao, Nan Yan, Mingzi Wang, Danyang Qi, Jiafan Zhang, Xin Chen, Ru Qin, Fengwei Xiao, Guangtao Zhao, Yucheng Liu, Xuediao Cai, Kui Zhao, Shengzhong (Frank) Liu, Jiangshan Feng
It is a crucial role for enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs) to prepare high‐quality perovskite films, which can be achieved by delaying the crystallization of perovskite film. Hence, we designed difluoroacetic anhydride (DFA) as an additive to regulating crystallization process thus reducing defect formation during perovskite film formation. It was found
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Switching between the [2π+2σ] and Hetero‐[4π+2σ] Cycloaddition Reactivity of Bicyclobutanes with Lewis Acid Catalysts Enables the Synthesis of Spirocycles and Bridged Heterocycles Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-11 Ji-Jie Wang, Lei Tang, Yuanjiu Xiao, Wen-Biao Wu, Guoqiang Wang, Jian-Jun Feng
The exploration of the complex chemical diversity of bicyclo[n.1.1]alkanes and their use as benzene bioisosteres has garnered significant attention over the past two decades. Regiodivergent syntheses of thiabicyclo[4.1.1]octanes (S‐BCOs) and highly substituted bicyclo[2.1.1]hexanes (BCHs) using a Lewis acid‐catalyzed formal cycloaddition of bicyclobutanes (BCBs) and 3‐benzylideneindoline‐2‐thione derivatives
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Dumbbell‐Shaped, Block‐Graft Copolymer with Aligned Domains for High‐performance Hydrocarbon Polymer Electrolyte Membranes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-05-11 So Youn Lee, Du Ru Kang, Jong-Gil Oh, Il Seok Chae, Jong Hak Kim
Given the environmental concerns surrounding fluoromaterials, the use of high‐cost perfluorinated sulfonic acids (PFSAs) in fuel cells and water electrolysis contradicts the pursuit of clean energy systems. Herein, we present a fluorine‐free dumbbell‐shaped block‐graft copolymer, derived from the cost‐effective triblock copolymer poly(styrene‐b‐ethylene‐co‐butylene‐b‐styrene) (SEBS), for polymer electrolyte