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Single Crystal and Pentatwinned Gold Nanorods Result in Chiral Nanocrystals with Reverse Handedness Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Kyle Van Gordon, Bing Ni, Robin Girod, Mikhail Mychinko, Francisco Bevilacqua, Sara Bals, Luis M Liz-Marzán
Handedness is an essential attribute of chiral nanocrystals, having a major influence on their properties. During chemical growth, the handedness of nanocrystals is usually tuned by selecting the corresponding enantiomer of chiral molecules involved in asymmetric growth, often known as chiral inducers. We report that, even using the same chiral inducer enantiomer, the handedness of chiral gold nanocrystals
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Oxygen Vacancies Boosted Hydronium Intercalation: A Paradigm Shift in Aluminum-based Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Chengxiang Huang, Zhou Jiang, Fuxi Liu, Wenwen Li, Qing Liang, Zhenzhen Zhao, Xin Ge, Kexin Song, Lirong Zheng, Xin Zhou, Sifan Qiao, Wei Zhang, Weitao Zheng
In aqueous aluminum-ion batteries(AAIBs), the insertion/extraction chemistry of Al3+ often leads to poor kinetics, whereas the rapid diffusion kinetics of hydrated hydrogen ions (H3O+) may offer the solution. However, the presence of considerable Al3+ in the electrolyte hinders the insertion reaction of H3O+. Herein, we report how oxygen-deficient α-MoO3 nanosheets unlock selective H3O+ insertion in
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Dehydration-Induced Cluster Consolidation in a Metal–Organic Framework for Sieving Hexane Isomers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Zhi-Jie Jiang, Ying Wang, Dong Luo, Rong-Jia Wei, Weigang Lu, Dan Li
Metal–organic frameworks (MOFs) that exhibit dynamic phase-transition behavior under external stimuli could have great potential in adsorptive separations. Here we report on a zinc-based microporous MOF (JNU-80) and its reversible transformation between two crystalline phases: large pore (JNU-80-LP) and narrow pore (JNU-80-NP). Specifically, JNU-80-LP can undergo a dehydration-induced cluster consolidation
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Type I [4σ + 4π] vs [4σ + 4π - 1] Cycloadditions Accessing Medium-Sized Carbocycles and Discovery of a Liver X Receptor β-Selective Ligand Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-22 Cheng Jiang, Lingfei Hu, Shuna Shen, Jianyu Zhang, Xi Wang, Dongxu Ma, Gang Lu, Tao Xu
The transition-metal-catalyzed [4 + 4] cycloaddition leading to cyclooctanoids has been centralizing on dimerization between 1,3-diene type substrates. Here, we extend a [4σ + 4π - 1] and [4σ + 4π] cycloaddition strategy to access the 7/8-membered fused carbocycles through Rh-catalyzed coupling between the 4σ-donor (benzocyclobutenones) and pendant diene (4π) motifs. The two pathways can be controlled
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Linker Mediated Electronic-State Manipulation of Conjugated Organic Polymers Enabling Highly Efficient Oxygen Reduction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Rui Ma, Chenglong Tang, Yonglin Wang, Xiaoxue Xu, Mingjie Wu, Xun Cui, Yingkui Yang
Conjugated polymers with tailorable composition and microarchitecture are propitious for modulating catalytic properties and deciphering inherent structure-performance relationships. Herein, we report a facile linker engineering strategy to manipulate the electronic states of metallophthalocyanine conjugated polymers and uncover the vital role of organic linkers in facilitating electrocatalytic oxygen
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A Naphthalenetetracarboxdiimide-Containing Covalent Organic Polymer: Preparation, Single Crystal Structure and Battery Application Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Qiang Dong, Tuoya Naren, Lei Zhang, Weixuan Jiang, Miaomiao xue, Xiang Wang, Libao Chen, Chun-Sing Lee, Qichun Zhang
Inspired by dative boron-nitrogen (B←N) bonds proven to be the promising dynamic linkage for the construction of crystalline covalent organic polymers/frameworks (COPs/COFs), we employed 1,4-bis(benzodioxaborole) benzene (BACT) and N,N'-Di(4-pyridyl)-1,4,5,8-naphthalenetetracarboxdiimide (DPNTCDI) as the corresponding building blocks to construct a functional COP (named as CityU-25), which had been
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Meta-Selective Copper-Catalyzed C–H Arylation of Pyridines and Isoquinolines through Dearomatized Intermediates Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Shu-Min Guo, Pengwei Xu, Armido Studer
C(sp2)–H functionalization offers an efficient strategy for the synthesis of various elaborated N-containing heteroarenes. Along these lines, oxazino pyridines that can be readily prepared from pyridines, have been introduced as powerful substrates in radical- and ionic-mediated meta-C–H functionalization. However, the regioselective meta-C–H arylation of pyridines remains a great challenge. Herein
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NIR-II Fluorescence Sensor Based on Steric Hindrance Regulated Molecular Packing for In Vivo Epilepsy Visualization Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Mengyao Zhao, Weiping Lai, Benhao Li, Tianwen Bai, Chunyan Liu, Yanfei Lin, Shixuan An, Longhua Guo, Lei Li, Jianbo Wang, Fan Zhang
Fluorescence sensing is crucial to study biological processes and diagnose diseases, especially in the second near-infrared (NIR-II) window with reduces background signals. However, it's still a great challenge to construct "off-on" sensors when the sensing wavelength extends into the second near-infrared (NIR-II) region to obtain higher imaging contrast, mainly due to the difficult synthesis of spectral
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Conjugation and Topology Engineering of 2D π-d Conjugated Metal-Organic Frameworks for Robust Potassium Organic Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Linqi Cheng, Meiling Qi, Jie Yu, Xupeng Zhang, Heng-Guo Wang, Fengchao Cui, Yinghui Wang
The evolution of two-dimensional conjugated metal-organic frameworks (2D c-MOFs) provides a significant prospect for researching the next generation of green and advanced energy storage systems (ESSs). Especially, conjugation and topology engineering serve as an irreplaceable character in adjusting the electrochemical properties of ESSs. Herein, we proposed a novel strategy using conjugation and topology
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Blue Long Afterglow and Ultra Broadband Vis-NIR Emission from All-Inorganic Copper-Doped Silver Halide Single Crystals Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Sijia Wang, Runze Liu, Juntao Li, Caixia Meng, Jianyong Liu, Junsheng Chen, Pengfei Cheng, Kaifeng Wu
All-inorganic metal halides with afterglow emission have attracted increasing attention due to their significantly longer afterglow duration and higher stability compared to their organic-inorganic hybrid counterparts. However, their afterglow colors have not yet reached the blue spectral region. Here, we report all-inorganic copper-doped Rb2AgBr3 single crystals with ultralong blue afterglow (>300
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A Dicopper(II)-Based Carbonic Anhydrase Model - Quantum-Chemical Evaluation of the Mechanistic Pathway Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Peter Comba, Gunasekaran Velmurugan, Philipp Baur
The cyanobacterium Prochloron didemni, an obligate symbiont of different species of colonial ascidians, occurring in the Pacific and Indian Oceans, produces a variety of cyclic peptides. These patellamide-type macrocycles lead to relatively stable dicopper(II) complexes that are extremely efficient carbonic anhydrase mimics, the most active model systems known so far. Importantly, it recently was shown
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Perfluorooxosulfate Salts as SOF4-Gas-Free Precursors to Multidimensional SuFEx Electrophiles Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Armir Zogu, Karim Ullah, Stefanos Spanopoulos, Ermal Ismalaj, Wim M. De Borggraeve, Joachim Demaerel
Sulfur(VI) Fluoride Exchange (SuFEx) chemistry stands as a well-established method for swiftly constructing complex molecules in a modular fashion. An especially promising segment of this toolbox is reserved for multidimensional SuFEx hubs: three or more substituents pluggable into a singular SVI centre to make ‘beyondlinear’ clicked constructions. Sulfurimidoyl difluorides (RNSOF2) stand out as the
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Catalytic Asymmetric Cascade Dearomatization of Indoles via a Photoinduced Pd‐Catalyzed 1,2‐Bisfunctionalization of Butadienes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-20 Xiaohang Zhan, Zhiwen Nie, Na Li, Ao Zhou, Haotian Lv, Mingrong Liang, Keqin Wu, Guijuan Cheng, Qin Yin
Photoinduced Pd‐catalyzed bisfunctionalization of butadienes with a readily available organic halide and a nucleophile represents an emerging and attractive method to assemble versatile alkenes bearing various functional groups at the allylic position. However, enantiocontrol and/or diastereocontrol in the C‐C or C‐X bond‐formation step have not been solved due to the open‐shell process. Herein, we
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Temporal‐Focusing Multiphoton Excitation Single‐Molecule Localization Microscopy Using Spontaneously Blinking Fluorophores Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-20 Jian-Zong Lai, Chun-Yu Lin, Shean-Jen Chen, Yu-Min Cheng, Manabu Abe, Tzu-Chau Lin, Fan-Ching Chien
Single‐molecule localization microscopy (SMLM) based on temporal‐focusing multiphoton excitation (TFMPE) and single‐wavelength excitation is used to visualize the three‐dimensional (3D) distribution of spontaneously blinking fluorophore‐labeled subcellular structures in a thick specimen with a nanoscale‐level spatial resolution. To eliminate the photobleaching effect of unlocalized molecules in out‐of‐focus
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Chemical Control of Fluorescence Lifetime towards Multiplexing Imaging Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-20 Junbao Ma, Feng Luo, Chia-Heng Hsiung, Jianan Dai, Zizhu Tan, Songtao Ye, Lina Ding, Baoxing Shen, Xin Zhang
Fluorescence lifetime imaging has been a powerful tool for biomedical research. Recently, fluorescence lifetime‐based multiplexing imaging has expanded imaging channels by using probes that harbor the same spectral channels and distinct excited state lifetime. While it is desirable to control the excited state lifetime of any given fluorescent probes, the rational control of fluorescence lifetimes
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Controlled Biocatalytic Synthesis of a Metal Nanoparticle‐Enzyme Hybrid: Demonstration for Catalytic H2‐driven NADH Recycling Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-20 Lucy B. F. Browne, Tim Sudmeier, Maya A. Landis, Christopher S. Allen, Kylie Alison Vincent
Here we demonstrate the preparation of enzyme‐metal biohybrids of NAD+ reductase with biocatalytically‐synthesised small gold nanoparticles (NPs, <10 nm) and core‐shell gold‐platinum NPs for tandem catalysis. Despite the variety of methods available for NP synthesis, there remains a need for more sustainable strategies which also give precise control over the shape and size of the metal NPs for applications
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Cyclometallated Imides as Templates for the H‐Bond Directed Iridium‐Catalyzed Asymmetric Hydrogenation of N‐Methyl, N‐Alkyl and N‐Aryl Imines Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Yisong Wen, Marc Fernández-Sabaté, Agustí Lledós, Giuseppe Sciortino, James Eills, Irene Marco-Rius, Antoni Riera, Xavier Verdaguer
A combined computational and experimental approach allowed us to develop the most selective catalysts for the direct hydrogenation of N‐methyl and N‐alkyl imines described to date. Iridium catalysts with a cyclometallated cyclic imide group provide selectivity of up to 99% enantiomeric excess. Computational studies show that the selectivity results from the combined effect of H‐bonding of the imide
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Reaction Environment Regulation for Electrocatalytic CO2 Reduction in Acids Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 min Zeng, Wensheng Fang, Yiren Chen, Xinyi Zhang, Yongming Hu, Bao Yu Xia
The electrocatalytic CO2 reduction reaction (CO2RR) is a sustainable route for converting CO2 into value‐added fuels and feedstocks, advancing a carbon‐neutral economy. The electrolyte critically influences CO2 utilization, reaction rate and product selectivity. While typically conducted in neutral/alkaline aqueous electrolytes, the CO2RR faces challenges due to (bi)carbonate formation and its crossover
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Delocalizing Excitation for Highly‐Active Organic Photovoltaic Catalysts Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Zhenzhen Zhang, Chaoying Xu, Qianlu Sun, Yufan Zhu, Wenlong Yan, Guilong Cai, Yawen Li, Wenqin Si, Xinhui Lu, Weigao Xu, Ye Yang, Yuze Lin
Localized excitation in traditional organic photocatalysts typically prevents the generation and extraction of photo‐induced free charge carriers, limiting their activity enhancement under illumination. Here, we enhance delocalized photoexcitation of small molecular photovoltaic catalysts by weakening their electron‐phonon coupling via rational fluoro‐substitution. The optimized 2FBP‐4F catalyst we
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Reversal of the Regioselectivity of Iron‐Promoted Hydrogenation and Hydrohalogenation of gem‐Difluoroalkenes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Yu-Yang Zhang, Yuchen Zhang, Xiao-Song Xue, Feng-Ling Qing
The reaction regioselectivity of gem‐difluoroalkenes is dependent on the intrinsic polarity. Thus, the reversal of the regiose‐lectivity of the addition reaction of gem‐difluoroalkenes remains a formidable challenge. Herein, we described an unprecedented reversal of regioselectivity of hydrogen atom transfer (HAT) to gem‐difluoroalkenes triggered by Fe–H species for the formation of difluoroalkyl radicals
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Cyclodextrin ‘Chaperones’ Enable Quasi‐Ideal Supramolecular Network Formation and Enhanced Photodimerization of Hydrophobic, Red‐shifted Photoswitches in Water Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Daniel Hoenders, Simon Ludwanowski, Christopher Barner-Kowollik, Andreas Walther
Precision‐engineered light‐triggered hydrogels are important for a diversity of applications. However, fields such as biomaterials require wavelength outside the harsh UV regime to prevent photodamage, typically requiring chromophores with extended p‐conjugation that suffer from poor water solubility. Herein, we demonstrate how cyclodextrins can be used as auxiliary agents to not only solubilize such
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One‐Component Cationic Lipids for Systemic mRNA Delivery to Splenic T Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Xinyue Zhang, Kexin Su, Shiqi Wu, Lixin Lin, Shun He, Xinxin Yan, Lu Shi, Shuai Liu
Unlocking the full potential of mRNA immunotherapy necessitates targeted delivery to specific cell subsets in the spleen. Four‐component lipid nanoparticles (LNPs) utilized in numerous clinical trials are primarily limited in hepatocyte and muscular targeting, highlighting the imperative demand for targeted and simplified non‐liver mRNA delivery systems. Herein, we report the rational design of one‐component
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M‐N3 Configuration on Boron Nitride Boosts Singlet Oxygen Generation via Peroxymonosulfate Activation for Selective Oxidation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Jianzheng Zhen, Jiahao Sun, Xiangwei Xu, Zenglong Wu, Wenkai Song, Yunzhan Ying, Shikun Liang, Lingshan Miao, Jiazhen Cao, Weiyang Lv, Changsheng Song, Yuyuan Yao, Mingyang Xing
Singlet oxygen (1O2) is an essential reactive species responsible for selective oxidation of organic matter, especially in Fenton‐like processes. However, due to the great limitations in synthesizing catalysts with well‐defined active sites, the controllable production and practical application of 1O2 remain challenging. Herein, guided by theoretical simulations, a series of boron nitride‐based single‐atom
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A MOF@Metal Oxide Heterostructure Induced by Post‐Synthetic Gamma‐Ray Irradiation for Catalytic Reduction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Mingxing Zhang, Junchang Chen, Xiaofang Zhao, Xuanzhi Mao, Chunyang Li, Juan Diwu, Guozhong Wu, Zhifang Chai, Shuao Wang
Metal‐organic framework (MOF) based heterostructures, which exhibit enhanced or unexpected functionality and properties due to synergistic effects, are typically synthesized using post‐synthetic strategies. However, several reported post‐synthetic strategies remain unsatisfactory, considering issues such as damage to the crystallinity of MOFs, presence of impure phases, and high time and energy consumption
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Machine Learning Molecular Dynamics Shows Anomalous Entropic Effect on Catalysis via Surface Pre‐melting of Nanoclusters Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Fu-Qiang Gong, Yun-Pei Liu, Ye Wang, Weinan E, Zhong-Qun Tian, Jun Cheng
Due to the superior catalytic activity and efficient utilization of noble metals, nanocatalysts are extensively used in the modern industrial production of chemicals. The surface structures of these materials are significantly influenced by reactive adsorbates, leading to dynamic behavior under experimental conditions. The dynamic nature poses significant challenges in studying the structure‐activity
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The 18F‐Difluoromethyl Group: Challenges, Impact and Outlook Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Joseph Ford, Sebastiano Ortalli, Veronique Gouverneur
The difluoromethyl functionality has proven useful in drug discovery, as it can modulate the properties of bioactive molecules. For PET imaging, this structural motif has been largely underexploited in (pre)clinical radiotracers due to a lack of user‐friendly radiosynthetic routes. This Minireview provides an overview of the challenges facing radiochemists and summarises the efforts made to date to
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An All‐rounder for NIR‐II Phototheranostics: Well‐Tailored 1064 nm Excitable Molecule for Photothermal Combating Orthotopic Breast Cancer Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Dingyuan Yan, Zhijun Zhang, Jianyu Zhang, Xue Li, Qian Wu, Yixiong Gui, Jun Zhu, Miaomiao Kang, Xiaohui Chen, Ben Zhong Tang, Dong Wang
The second near‐infrared (NIR‐II, 1000–1700 nm) light‐activated organic photothermal agent that synchronously enables satisfying NIR‐II fluorescence imaging is highly warranted yet rather challenging on the basis of the overwhelming nonradiative decay. Herein, such an agent, namely TPABT‐TD, was tactfully designed and constructed via employing benzo[c]thiophene moiety as bulky electron donor/π‐bridge
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Hydrogen‐Bond‐Mediated Formation of C‐N or C=N Bond during Photocatalytic Reductive Coupling Reaction over CdS Nanosheets Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Jie He, Bo Han, Chensheng Xian, Zhao Hu, Tingfeng Fang, Zehui Zhang
Reductive amination of carbonyl compounds and nitro compounds represents a straightforward way to attain imines or secondary amines, but it is difficult to control the product selectivity. Herein, we report the selective formation of C−N or C=N bond readily manipulated through a solvent‐induced hydrogen bond bridge, facilitating the swift photocatalytic reductive coupling process. The reductive‐coupling
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Ratiometric Afterglow Luminescent Imaging of Matrix Metalloproteinase‐2 Activity via an Energy Diversion Process Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Weijing Huang, Wenhui Zeng, Zheng Huang, Daqing Fang, Hong Liu, Min Feng, Liang Mao, Deju Ye
Ratiometric afterglow luminescent (AGL) probes are attractive for in vivo imaging due to their high sensitivity and signal self‐calibration function. However, there are currently few ratiometric AGL probes available for imaging enzymatic activity in living organisms. Here, we present an energy diversion (ED) strategy that enables the design of an enzyme‐activated ratiometric AGL probe (RAG‐RGD) for
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Desulfurdioxidative N‐N Coupling of N‐Arylhydroxylamines and N‐Sulfinylanilines: Reaction Development and Mechanism Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-19 Linwei Li, Yi Zhou, Zhenguo Xi, Zhaoquan Guo, Ji-Cheng Duan, Zhi-Xiang Yu, Hongyin Gao
A highly efficient and chemoselective approach for the divergent assembling of unsymmetrical hydrazines through an unprecedented intermolecular desulfurdioxidative N‐N coupling is developed. This metal free protocol employs readily accessible N‐arylhydroxylamines and N‐sulfinylanilines to provide highly valuable hydrazine products with good yields and excellent functional group tolerance under simple
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Discovery of (±)‐Penindolenes Reveals an Unusual Indole Ring Cleavage Pathway Catalyzed by P450 Monooxygenase Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Ling-Hong Meng, Takayoshi Awakawa, Xiao-Ming Li, Zhiyang Quan, Sui-Qun Yang, Bin-Gui Wang, Ikuro Abe
(±)‐Penindolenes A–D (1–4), the first representatives of indole terpenoids featuring a γ‐lactam skeleton, were isolated from the mangrove‐derived endophytic fungus Penicillium brocae MA‐231. Our bioactivity tests revealed their potent antimicrobial and acetylcholinesterase inhibitory activities. The biosynthetic reactions by the five enzymes PbaABCDE leading to γ‐lactam ring formation were identified
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Tailoring Zirconia Supported Intermetallic Platinum Alloy via Reactive Metal‐Support Interactions for High‐Performing Fuel Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Zijie Lin, Nadaraj Sathishkumar, Yu Xia, Shenzhou Li, Xuan Liu, Jialun Mao, Hao Shi, Gang Lu, Tanyuan Wang, Hsing-Lin Wang, Yunhui Huang, Lior Elbaz, Qing Li
Developing efficient and anti‐corrosive oxygen reduction reaction (ORR) catalysts is of great importance for the applications of proton exchange membrane fuel cells (PEMFCs). Herein, we report a novel approach to prepare metal oxides‐supported intermetallic Pt alloy nanoparticles (NPs) via the reactive metal‐support interaction (RMSI) as ORR catalysts, using Ni‐doped cubic ZrO2 (Ni/ZrO2) supported
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Genuine Carbene Versus Carbene‐Like Reactivity Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Jan Lorkowski, Patrick Yorkgitis, Melinda R Serrato, Milan Gembicky, Cezary Pietraszuk, Guy Bertrand, Rodolphe Jazzar
Singlet carbenes are not always isolable and often even elude direct detection. When they escape observation, their formation can sometimes be evidenced by in‐situ trapping experiments. However, is carbene‐like reactivity genuine evidence of carbene formation? Herein, using the first example of a spectroscopically characterized cyclic (amino)(aryl)carbene (CAArC), we cast doubt on the most common carbene
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Efficient Ultraviolet Circularly Polarized Luminescence in Zero‐Dimensional Hybrid Cerium Bromides Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Chen Li, Yi Wei, Yan Zhang, Zhishan Luo, Yulian Liu, Meiying He, Zewei Quan
Ultraviolet circularly polarized luminescence (UV‐CPL) with high photon energy shows great potential in polarized light sources and stereoselective photopolymerization. However, developing luminescent materials with high UV‐CPL performance remains challenging. Here, we report a pair of rare earth Ce3+‐based zero‐dimensional (0D) chiral hybrid metal halides (HMHs), R/S‐(C14H24N2)2CeBr7, which exhibits
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Isothermal Phase Transitions in Liquid Crystals Driven by Dynamic Covalent Chemistry Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Daniel Martínez, Tim Schlossarek, Frank Würthner, Bartolome Soberats
The dynamic nature of calamitic liquid crystals is exploited to perform isothermal phase transitions driven by dynamic covalent chemistry. For this purpose, nematic (N) arrays based on aldehyde 1 were treated with different amines (A‐E) in an on‐surface process, which resulted in different isothermal phase transitions. These phase transformations were caused by in‐situ imination reactions and are dependent
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Linkage Engineering in Covalent Organic Frameworks for Metal‐Free Electrocatalytic C2H4 Production from CO2 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Yang Xiao, Jie Lu, Kean Chen, Yuliang Cao, Chengtao Gong, Fu-Sheng Ke
Electrocatalytic carbon dioxide reduction reaction (CO2RR) to produce ethylene (C2H4) is conducive to sustainable development of energy and environment. At present, most electrocatalysts for C2H4 production are limited to the heavy metal copper, meanwhile, achieving metal‐free catalysis remains a challenge. Noted piperazine with sp3 N hybridization is beneficial to CO2 capture, but CO2RR performance
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Probing Energy‐Funneling Kinetics in Nanocrystal Sublattices for Superior X‐ray Imaging Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Qinxia Wu, Xinqi Xu, Xiaokun Li, Hao Jiang, Xian Qin, Zhongzhu Hong, Xiaofeng Chen, Zhijian Yang, Xiangyu Ou, Lili Xie, Yu He, Sanyang Han, Qiushui Chen, Huanghao Yang
Long‐lasting radioluminescence scintillators have recently attracted substantial attention from both research and industrial communities, primarily due to their distinctive capabilities of converting and storing X‐ray energy. However, determination of energy‐conversion kinetics in these nanocrystals remaines unexplored. Here we investigate energy funneling kinetics in NaLuF4:Mn2+/Gd3+ nanocrystal sublattices
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An MBene Modulating the Buried SnO2/Perovskite Interface in Perovskite Solar Cells Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Yuning Zhang, Bo Yu, Yapeng Sun, Jiankai Zhang, Zhan Su, Huangzhong Yu
The interface of perovskite solar cells (PSCs) plays an important role in transferring and collecting charges. Interface defects are important factors affecting the efficiency and stability of PSCs. Here, the buried interface between SnO2 and the perovskite layer is bridged by two‐dimensional (2D) MBene, which improves charge transfer. MBene can deposit additional electrons on the surface of SnO2,
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Organometallic Chirality Sensing via “Click”‐like η6‐Arene Coordination with an Achiral Cp*Ru(II) Piano Stool Complex Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Eryn Nelson, Jeffery A. Bertke, F. Yushra Thanzeel, Christian Wolf
Piano stool complexes have been studied over many years and found widespread applications in organic synthesis, catalysis, materials and drug development. We now report the first examples of quantitative chiroptical molecular recognition of chiral compounds through click‐like η6‐arene coordination with readily available half sandwich complexes. This conceptually new approach to chirality sensing is
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Photogeneration of Chlorine Radical from a Self‐Assembled Fluorous 4CzIPN•Chloride Complex: Application in C–H bond Functionalization Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Victor Carré, Pascale Godard, Raphaël Méreau, Henri-Pierre Jacquot de Rouville, Gediminas Jonusauskas, Nathan McClenaghan, Thierry Tassaing, Jean-Marc Vincent
The chlorine radical is a strong HAT (Hydrogen Atom Transfer) agent that is very useful for the functionalization of C(sp3)–H bonds. Albeit highly attractive, its generation from the poorly oxidizable chloride ion mediated by an excited photoredox catalyst is a difficult task. We now report that 8Rf8‐4CzIPN, an electron‐deficient fluorous derivative of the benchmark 4CzIPN photoredox catalyst belonging
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Supramolecular Entanglement in a Hydrogen‐Bonded Organic Framework Enables Flexible‐Robust Porosity for Highly Efficient Purification of Natural Gas Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Chenghao Jiang, Jia-Xin Wang, Di Liu, Enyu Wu, Xiao-Wen Gu, Xu Zhang, Bin Li, Banglin Chen, Guodong Qian
The development of porous materials with flexible‐robust characteristics shows some unique advantages to target high performance for gas separation, but remains a daunting challenge to achieve so far. Herein, we report a carboxyl‐based hydrogen‐bonded organic framework (ZJU‐HOF‐8a) with flexible‐robust porosity for efficient purification of natural gas. ZJU‐HOF‐8a features a four‐fold interpenetrated
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Graphical Abstract: Angew. Chem. Int. Ed. 18/2024 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18
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Chemical Synthesis of Secretoglobin 3A2 Covalent Homodimer and Photocaged Monomeric Variants Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Thais Gazzi, Maria Heinke, Fabienne Landolt, Jeffrey W. Bode
Secretoglobin (SCGB) 3A2 belongs to an intriguing family of small, secreted proteins present only in mammals. Although members of the SCGB protein family have distinct amino‐acid sequences, they share structural similarities. Of particularly interest is the not yet fully understood self‐assembly ability of SCGBs, which arise from covalent disulfide dimerization and non‐covalent oligomerization. Recently
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Photo‐Induced Ruthenium‐Catalyzed C–H Arylation Polymerization at Ambient Temperature Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Takuya Michiyuki, Isaac Maksso, Lutz Ackermann
Transition metal‐catalyzed C–H arylation polymerization (CHAP) is an attractive tool for constructing π‐conjugated polymers in a sustainable manner. However, the existing methods primarily rely on palladium catalysis, which usually entails harsh reaction conditions and branching/cross‐linking. Here we report the first example of an ambient‐temperature ruthenium‐catalyzed C–H arylation polymerization
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Radical Homopolymerization of Linear α‐Olefins Enabled by 1,4‐Cyano Group Migration Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Bang An, Litao Zhou, Shuai Liu, Yaxin Zheng, Changhu Li, Feichen Cui, Chaowei Yue, Hua Liu, Yang Sui, Chonglei Ji, Jiajun Yan, yifan li
α‐Olefins are valued and abundant building blocks from fossil resources. They are widely used to provide small‐molecule or polymeric products. Despite numerous advantages of radical polymerization, it has been well‐documented as textbook knowledge that α‐olefins and their functionalized derivatives cannot be radically homopolymerized because of the degradative chain transfer side reactions. Herein
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Ideal Cage‐like Pores for Molecular Sieving of Butane Isomers with High Purity and Record Productivity Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Mingyan Wu, Zhenyu Ji, Yunzhe Zhou, Cheng Chen, Daqiang Yuan, Maochun Hong
n‐C4H10 and iso‐C4H10 are both important petrochemical raw materials. Considering the coexistence of the isomers in the production process, it is necessary to achieve their efficient separation through an economical way. However, to obtain high‐purity n‐C4H10 and iso‐C4H10 in one‐step separation process, developing iso‐C4H10‐exclusion adsorbents with high n‐C4H10 adsorption capacity is crucial. Herein
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Considerable Piezochromism in All‐Inorganic Zero‐Dimensional Perovskite Nanocrystals via Pressure‐Modulated Self‐Trapped Exciton Emission Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Zhiwei Ma, Songrui Yang, Yue Shi, Yuan Fu, Kai Wang, Guanjun Xiao, Bo Zou
Piezochromic materials refer to a class of matters that alter their photoluminescence (PL) colors in response to the external stimuli, which exhibit promising smart applications in anti‐counterfeiting, optoelectronic memory and pressure‐sensing. However, so far, most reported piezochromic materials have been confined to organic materials or hybrid materials containing organic moieties with limited
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Electrophilic Hydrosilylation of Electron‐Rich Alkenes Derived from Enamines Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18 Carlos Laglera-Gándara, Julián Jiménez-Pérez, Francisco José Fernández-de-Córdova, Pablo Ríos, Salvador Conejero
The low‐electron count, air‐stable, platinum complexes [Pt(ItBu’)(ItBu)][BArF] (C1) (ItBu=1,3‐di‐tert‐butylimidazol‐2‐ylidene), [Pt(SiPh)3(ItBuiPr)2][BArF] (C2) (ItBuiPr = 1‐tert‐butyl‐3‐iso‐propylimidazol‐2‐ylidene), [Pt(SiPh)3(ItBuMe)2][BArF] (C3), [Pt(GePh3)(ItBuiPr)2][BArF] (C4), [Pt(GePh)3(ItBuMe)2][BArF] (C5) and [Pt(GeEt)3(ItBuMe)2][BArF] (C6) (ItBuMe = 1‐tert‐butyl‐3‐methylimidazol‐2‐ylidene)
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Site‐Selective Radical Aromatic C–H Functionalization of Alloxazine and Flavin through Ground‐State Single Electron Transfer Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Agnideep Das, Oscar Charpentier, Cheriehan Hessin, Jules Schleinitz, David Pianca, Nolwenn Le Breton, Sylvie Choua, Laurence Grimaud, Christophe Gourlaouen, Marine Desage-El Murr
Flavins and their alloxazine isomers are key chemical scaffolds for bioinspired electron transfer strategies. Their properties can be fine‐tuned by functional groups, which must be introduced at an early stage of the synthesis as their aromatic ring is inert towards post‐functionalization. We show that the introduction of a remote metal‐binding redox site on alloxazine and flavin activates their aromatic
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Corrigendum: Effects of Deuterium Isotopes on Pt(II) Complexes and Their Impact on Organic NIR Emitters Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17
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Merging High‐Pressure Syngas Metal Catalysis and Biocatalysis in Tandem One‐Pot Processes for the Synthesis of Non‐chiral and Chiral Alcohols from Alkenes in Water Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Hannah Bork, Kim E. Naße, Andreas J. Vorholt, Harald Gröger
While simultaneously proceeding reactions are among the most fascinating features of biosynthesis, this concept of tandem processes also offers high potential in the chemical industry in terms of less waste production and improved process efficiency and sustainability. Although examples of one‐pot chemoenzymatic syntheses exist, the combination of completely different reaction types is rare. In this
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Organo‐Photocatalytic Anti‐Markovnikov Hydroamidation of Alkenes with Sulfonyl Azides: A Combined Experimental and Computational Study Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Rui Fu, Mengyu Xu, Yujing Wang, Xinxin Wu, Xiaoguang Bao
The construction of C(sp3)−N bonds via direct N‐centered radical addition with olefins under benign conditions is a desirable but challenging strategy. Herein, we describe an organo‐photocatalytic approach to achieve anti‐Markovnikov alkene hydroamidation with sulfonyl azides in a highly efficient manner under transition‐metal‐free and mild conditions. A broad range of substrates, including both activated
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SilE‐R and SilE‐S ‐ DABB Proteins Catalyzing Enantiospecific Hydrolysis of Organosilyl Ethers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Lisa M. Pick, Viviane Oehme, Julia Hartmann, Jessica Wenzlaff, Qingyun Tang, Gideon Grogan, Marion B. Ansorge-Schumacher
Silyl ethers fulfil a fundamental role in synthetic organic chemistry as protecting groups and their selective cleavage is an important factor in their application. We present here for the first time two enzymes, SilE‐R and SilE‐S, which are able to hydrolyze silyl ethers. They belong to the stress‐response A/B barrel domain (DABB) family and are able to cleave the Si‐O bond with opposite enantiopreference
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Quantitative Factors Introduced in the Feasibility Analysis of Reactive Oxygen Species (ROS)‐Sensitive Triggers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Shameer M. Kondengadan, Binghe Wang
Reactive oxygen species (ROS) are critical for cellular signaling. Various pathophysiological conditions are also associated with elevated levels of ROS. Hence, ROS‐sensitive triggers have been extensively used for selective payload delivery. Such applications are predicated on two key functions: (1) a sufficient magnitude of concentration difference for the interested ROS between normal tissue/cells
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A Zeolitic Octahedral Metal Oxide with Ultrahigh Porosity for High‐temperature and High‐humidity Alkyne/Alkene Separation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-17 Baokai Ma, Panpan Hu, Liangcheng Zou, Qianqian Zhu, Lifeng Zhang, Satoshi Ishikawa, Wataru Ueda, Yanshuo Li, Zhenxin Zhang
Zeolitic octahedral metal oxide is a newly synthesized all‐inorganic zeolitic material and has been used for adsorption, separation, and catalysis. Herein, a new zeolitic octahedral metal oxide was synthesized and characterized. The porous framework was established through the assembly of [P2Mo13O50] clusters with PO4 linkers. Guest molecules occupied the framework, which could be removed through heat
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Selective Arylation of RNA 2′‐OH Groups via SNAr Reaction with Trialkylammonium Heterocycles Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Sayantan Chatterjee, Lu Xiao, Wenrui Zhong, Sheng Feng, Eric T. Kool
Small‐molecule reactions at the 2′‐OH groups of RNA enable useful applications for transcriptome technology and biology. To date, all reactions have involved carbonyl acylation and mechanistically related sulfonylation, limiting the types of modifications and properties that can be achieved. Here we report that electron‐deficient heteroaryl species selectively react with 2′‐OH groups of RNA in water