样式: 排序: IF: - GO 导出 标记为已读
-
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
-
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
-
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
-
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
-
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
-
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
-
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
-
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 : 2024-04-18 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
-
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,
-
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
-
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
-
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
-
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
-
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
-
Graphical Abstract: Angew. Chem. Int. Ed. 18/2024 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-18
-
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
-
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
-
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
-
-
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
-
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
-
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)
-
-
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
-
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
-
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
-
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
-
-
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
-
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
-
-
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
-
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
-
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
-
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
-
Ternary Complex‐Templated Dynamic Combinatorial Chemistry for the Selection and Identification of Homo‐PROTACs Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Claudia J. Diehl, Alessandra Salerno, Alessio Ciulli
Dynamic combinatorial chemistry (DCC) leverages a reversible reaction to generate compound libraries from constituting building blocks under thermodynamic control. The position of this equilibrium can be biased by addition of a target macromolecule towards enrichment of bound ligands. While DCC has been applied to select ligands for a single target protein, its application to identifying chimeric molecules
-
Ethylenedioxythiophene‐based Small Molecular Donor with Multiple Conformation Locks for Organic Solar Cells with Efficiency of 19.3% Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Qian Xie, Xiangmeng Deng, Chaowei Zhao, Jie Fang, Dongdong Xia, Yuefeng Zhang, Feng Ding, Jiali Wang, Mengdi Li, Zhou Zhang, Chengyi Xiao, Xunfan Liao, Lang Jiang, Bin Huang, Runying Dai, Weiwei Li
Ternary organic solar cells (T‐OSCs) represent an efficient strategy for enhancing the performance of OSCs. Presently, the majority of high‐performance T‐OSCs incorporates well‐established Y‐acceptors or donor polymers as the third component. In this study, a novel class of conjugated small molecules has been introduced as the third component, demonstrating exceptional photovoltaic performance in T‐OSCs
-
Small Ionic Liquid‐based Molecule Drives Strong Adhesives Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Kai Liu, peiyi Wu
Nature has inspired scientists to fabricate adhesive materials for applications in many burgeoning areas. However, it is still a significant challenge to develop small‐molecule adhesives with high‐strength, low‐temperature and recyclable properties, although these merits are of great interest in various aspects. Herein, we report a series of strong adhesives based on low‐molecular‐weight molecular
-
Breaking Highly Ordered PtPbBi Intermetallic with Disordered Amorphous Phase for Boosting Electrocatalytic Hydrogen Evolution and Alcohol Oxidation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Fukai Feng, Chaoqun Ma, Sumei Han, Xiao Ma, Caihong He, Huaifang Zhang, Wenbin Cao, Xiangmin Meng, Jing Xia, Lijie Zhu, Yahui Tian, Qi Wang, Qinbai Yun, Qipeng Lu
Constructing amorphous/intermetallic (A/IMC) heterophase structures by breaking the highly ordered IMC phase with disordered amorphous phase is an effective way to improve the electrocatalytic performance of noble metal‐based IMC electrocatalysts because of the optimized electronic structure and abundant heterophase boundaries as active sites. In this study, we report the synthesis of ultrathin A/IMC
-
Anion‐Coordination Foldamer‐Based Polymer Network: from Molecular Spring to Elastomer Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Jiangping Qin, Yongming Wang, Tian Wang, Na Wang, Wenhua Xu, Lin Cheng, Wei Yu, Xuzhou Yan, Lingyan Gao, Bo Zheng, Biao Wu
Foldamer is a scaled‐down version of coil spring, which can absorb and release energy by conformational change. Here, polymer networks with high‐density of molecular springs were developed by employing anion‐coordination‐based foldamers as the monomer. The coiling of the foldamer is controlled by oligourea ligands coordinating to chloride ions; subsequently, the folding and unfolding of foldamer conformations
-
Ternary Rotational Polyanion Coupling Enables Fast Li Ion Dynamics in Tetrafluoroborate Ion Doped Antiperovskite Li2OHCl Solid Electrolyte Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Juncao Bian, Sifan Ling, Bei Deng, Haibin Lin, Ruo Zhao, Long Kong, Huimin Yuan, Jinlong Zhu, Songbai Han, Liping Wang, Ruiqin Zhang, Yusheng Zhao, Zhouguang Lu
Li‐rich antiperovskite (LiRAP) hydroxyhalides are emerging as attractive solid electrolyte (SEs) for all‐solid‐state Li metal batteries (ASSLMBs) due to their low melting point, low cost, and ease of scaling‐up. The incorporation of rotational polyanions can reduce the activation energy and thus improve the Li ion conductivity of SEs. Herein, we propose a ternary rotational polyanion coupling strategy
-
Non‐Fluorinated Ethers to Mitigate Electrode Surface Reactivity in High‐Voltage NCM811‐Li Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Zhijie Wang, Xiangli Che, Danni Wang, Yanyan Wang, Xiaomei He, Ye Zhu, Biao Zhang
Lithium (Li) metal batteries (LMBs) with nickel (Ni)‐rich layered oxide cathodes exhibit twice the energy density of conventional Li‐ion batteries. However, their lifespan is limited by severe side reactions caused by high electrode reactivity. Fluorinated solvent‐based electrolytes can address this challenge, but they pose environmental and biological hazards. This work reports on the molecular engineering
-
Unveiling Crucial Chemical Processing Parameters Influencing the Performance of Solution‐processed Inorganic Thermoelectric Materials Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Christine Fiedler, Mariano Calcabrini, Yu Liu, Maria Ibáñez
Production of thermoelectric materials from solution‐processed particles involves the synthesis of particles, their purification and densification into pelletized material. Chemical changes that occur during each one of these steps render them performance determining. Particularly the purification steps, bypassed in conventional solid‐state synthesis, are the cause for large discrepancies among similar
-
Two‐Dimensional Conjugated Metal–Organic Frameworks with a Ring‐in‐Ring Topology and High Electrical Conductance Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Mingyu Yang, Yi Zhang, Renlong Zhu, Junjun Tan, Jinxin Liu, Wei Zhang, Meng Zhou, Zheng Meng
Electrically conducting two‐dimensional (2D) metal‐organic frameworks (MOFs) have garnered significant interest due to their remarkable structural tunability and outstanding electrical properties. However, the design and synthesis of high‐performance materials face challenges due to the limited availability of specific ligands and pore structures. In this study, we have employed a novel highly branched
-
Engineering of Halide Methyltransferase BxHMT through Dynamic Cross‐correlation Network Analysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Chun-Yu Gao, Gui-Ying Yang, Xu-Wei Ding, Jian-He Xu, Xiaolin Cheng, Gao-Wei Zheng, QI CHEN
Halide methyltransferases (HMTs) provide an effective way to regenerate S‐adenosyl methionine (SAM) from S‐adenosyl homocysteine and reactive electrophiles such as methyl iodide (MeI) or methyl toluene sulfonate (MeOTs). Compared with MeI, the cost‐effective unnatural substrate MeOTs can be accessible directly from cheap and abundant alcohols, but shows only limited reactivity in SAM production. Herein
-
Mitigating Sodium Ordering for Enhanced Solid Solution Behavior in Layered NaNiO2 Cathodes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Krishnakanth Sada, Steven Kmiec, Arumugam Manthiram
The O‐type layered nickel oxides suffer from undesired co‐operative Jahn‐Teller distortion stemming from Ni3+ ions and undergo multiple biphasic structural transformations during the insertion/extraction of large Na+ ions, posing a significant challenge to stabilize the structural integrity. We present here a systematic investigation of the impact of substituting 5% divalent (Mg2+) or trivalent (Al3+
-
Electrochemical Asymmetric Radical Functionalization of Aldehydes Enabled by a Redox Shuttle Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Daniele Mazzarella, Chun Qi, Michael Vanzella, Andrea Sartorel, Giorgio Pelosi, Luca Dell'Amico
Aminocatalysis is a well‐established tool that enables the production of enantioenriched compounds under mild conditions. Its versatility is underscored by its seamless integration with various synthetic approaches. While the combination of aminocatalysis with metal catalysis, photochemistry, and stoichiometric oxidants has been extensively explored, its synergy with electrochemical activation remains
-
Fabrication of Large‐area Multi‐stimulus Responsive Thin Films via Interfacially Confined Irreversible Katritzky Reaction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Yuanhong Shu, Yan Luo, Hexi Wei, Lingya Peng, Jingjing Liang, Binbin zhai, Liping Ding, Yu Fang
Fabrication of large‐area thin films through irreversible reactions remains a formidable task. This study reports a breakthrough strategy for in situ synthesis of large‐area, free‐standing, robust and multi‐stimulus responsive thin films through a catalyst‐free and irreversible Katritzky reaction at a liquid–liquid interface. The as resulted films are featured with adjustable thickness of 1–3 μm and
-
Alveoli‐Inspired Carbon Cathodes with Interconnected Porous Structure and Asymmetric Coordinated Vanadium Sites for Superior Li‐S Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Rui Yan, Zhenyang Zhao, Ran Zhu, Min Wu, Xu Liu, Mohsen Adeli, Bo Yin, Chong Cheng, Shuang Li
Accelerating sulfur conversion catalysis to alleviate the shuttle effect has become a novel paradigm for effective Li‐S batteries. Although nitrogen‐coordinated metal single‐atom (M‐N4) catalysts have been investigated, further optimizing its utilization rate and catalytic activities is urgently needed for practical applications. Inspired by the natural alveoli tissue with interconnected structure
-
Development of an FeII Complex Exhibiting Intermolecular Proton Shifting Coupled Spin Transition Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Tianchi Ji, Shengqun Su, Shuqi Wu, Yuta Hori, Yasuteru Shigeta, Yubo Huang, Wenwei Zheng, Wenhuang Xu, Xiaopeng Zhang, Ryoji Kiyanagi, Koji Munakata, Takashi Ohhara, Takumi Nakanishi, Osamu Sato
In this study, we investigated reversible intermolecular proton shifting (IPS) coupled with spin transition (ST) in a novel FeII complex. The host FeII complex and the guest carboxylic acid anion were connected by intermolecular hydrogen bonds (IHBs). We extended the intramolecular proton transfer coupled ST phenomenon to the intermolecular system. The dynamic phenomenon was confirmed by variable‐temperature
-
Regulating Sulfur Redox Kinetics by Coupling Photocatalysis for High‐Performance Photo‐Assisted Lithium‐Sulfur Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Yuhao Liu, Feng Wu, Zhengqiang Hu, Fengling Zhang, Ke Wang, Li Li, Renjie Chen
Challenges such as shuttle effect have hindered the commercialization of lithium‐sulfur batteries (LSBs), despite their potential as high‐energy‐density storage devices. To address these issues, we explore the integration of solar energy into LSBs, creating a photo‐assisted lithium‐sulfur battery (PA‐LSB). The PA‐LSB provides a novel and sustainable solution by coupling the photocatalytic effect to
-
Molecular Engineering for Modulating Photocatalytic Hydrogen Evolution of Fully Conjugated 3D Covalent Organic Frameworks Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Yaqin Wang, Zelong Qiao, Han Li, Rui Zhang, Zhonghua Xiang, Dapeng Cao, Shitao Wang
Covalent organic frameworks (COFs) have recently shown great potential for photocatalytic hydrogen production. Currently almost all reports are focused on two‐dimensional (2D) COFs, while the 3D counterparts are rarely explored due to their non‐conjugated frameworks derived from the sp3 carbon based tetrahedral building blocks. Here, we rationally designed and synthesized a series of fully conjugated
-
Umbrella‐Shaped Amphiphiles: Internal Alkylation of an Aromatic Micelle and Its Impact on Cavity Features Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Masaya Endo, Shinji Aoyama, Yoshitaka Tsuchido, Lorenzo Catti, Michito Yoshizawa
To develop new hybrid micelles with alkyl/polyaromatic core‐shell structures, we synthesized umbrella‐shaped amphiphiles bearing a bent anthracene dimer with a linear alkyl chain (i.e., octyl and hexadecyl groups). The amphiphiles quantitatively assemble into spherical micelles (~2‐3 nm in core diameter), possessing an alkylated cavity surrounded by a polyaromatic framework, in water. The alkylation
-
Photoswitching Reagent for Super‐resolution Fluorescence Microscopy Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Ga-eun Go, Uidon Jeong, Hyunbum Park, Seokran Go, Doory Kim
Single‐molecule localization microscopy (SMLM) has revolutionized optical microscopy by exceeding the diffraction limit and revealing previously unattainable nanoscale details of cellular structures and molecular dynamics. This super‐resolution imaging capability relies on fluorophore photoswitching, which is crucial for optimizing the imaging conditions and accurately determining the fluorophore positions
-
Expedient Access to 18F‐Fluoroheteroarenes via Deaminative Radiofluorination of Aniline‐Derived Pyridinium Salts Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Joseph Ford, Sebastiano Ortalli, Zijun Chen, Jeroen Sap, Matthew Tredwell, Veronique Gouverneur
Herein, we disclose that pyridinium salts derived from abundant (hetero)anilines represent a novel precursor class for nucleophilic aromatic substitution reactions with [18F]fluoride. The value of this new 18F‐fluorodeamination is demonstrated with the synthesis of over 30 structurally diverse and complex heteroaryl 18F‐fluorides, several derived from scaffolds that were yet to be labelled with fluorine‐18
-
N‐(sulfonio)sulfilimine reagents: Non‐oxidizing Sources of Electrophilic Nitrogen Atom for Skeletal Editing Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Tobias Heilmann, Juan M Lopez-Soria, Johannes Ulbrich, Johannes Kircher, Zhen Li, Brigitte Worbs, Christopher Golz, Ricardo A Mata, Manuel Alcarazo
The one‐pot synthesis of λ4‐dibenzothiophen‐5‐imino‐N‐dibenzothiophenium triflate (1) in multigram scale is reported. This compound reacts with Rh2(esp)2 (esp = α,α,α′,α′‐tetramethyl‐1,3‐benzenedipropionic acid) generating a Rh‐coordinated sulfonitrene species, which is able to transfer the electrophilic nitrene moiety to olefins. When indenes are used as substrates, isoquinolines are obtained in good
-
Indocyanine Green‐based Nanoprobe for In Vivo Detection of Cellular Senescence Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-16 Andrew G Baker, Muhamad Hartono, Hui-Ling Ou, Andrea Bistrović Popov, Emma L Brown, James Joseph, Monika Golinska, Estela González-Gualda, David Marcias, Jianfeng Ge, Mary Denholm, Samir Morsli, Chandan Sanghera, Thomas R Else, Heather F Greer, Aude Vernet, Sarah E Bohndiek, Ljiljana Fruk, Daniel Muñoz-Espín
There is an urgent need to improve conventional cancer‐treatments by preventing detrimental side effects, cancer recurrence and metastases. Recent studies have shown that presence of senescent cells in tissues treated with chemo‐ or radiotherapy can be used to predict the effectiveness of cancer treatment. However, although the accumulation of senescent cells is one of the hallmarks of cancer, surprisingly
-
Back Cover: PAM‐Engineered Toehold Switches as Input‐Responsive Activators of CRISPR‐Cas12a for Sensing Applications (Angew. Chem. Int. Ed. 17/2024) Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-15 Neda Bagheri, Alejandro Chamorro, Andrea Idili, Alessandro Porchetta
-
Graphical Abstract: Angew. Chem. Int. Ed. 17/2024 Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-15
-
Tuning Electron Delocalization of Redox‐Active Porous Aromatic Framework for Low‐Temperature Aqueous Zn–K Hybrid Batteries with Air Self‐Chargeability Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-04-15 Junhao Wang, Xupeng Zhang, Zhaoli Liu, Jie Yu, Heng-Guo Wang, Xing-Long Wu, Fengchao Cui, Guangshan Zhu
Air self‐charging aqueous batteries promise to integrate energy harvesting technology and battery systems, potentially overcoming a heavy reliance on energy and the spatiotemporal environment. However, the exploitation of multifunctional air self‐charging battery systems using promising cathode materials and suitable charge carriers remains challenging. Herein, for the first time, we developed low‐temperature