Large Libraries of Structurally Diverse Macrocycles Suitable for Membrane Permeation
Angew Chem Int Ed Engl. 2024 Apr 11:e202400350. doi: 10.1002/anie.202400350. Online ahead of print.ABSTRACTMacrocycles offer an attractive format for drug development due to their good binding properties and potential to cross cell membranes. To efficiently identify macrocyclic ligands for new targets, methods for the synthesis and screening of large combinatorial libraries of small cyclic peptides were developed, many of them using thiol groups for efficient peptide macrocyclization. However, a weakness of these libraries is that invariant thiol-containing building blocks such as cysteine are used, resulting in a region t...
Source: Angewandte Chemie - April 11, 2024 Category: Chemistry Authors: Alexander L Nielsen Zsolt Bognar Ganesh K Mothukuri Anne Zarda Mischa Schuttel Manuel L Merz Xinjian Ji Edward Will Monica Chinellato Christian R O Bartling Kristian Stromgaard Laura Cendron Alessandro Angelini Christian Heinis Source Type: research

Yang Wang
Angew Chem Int Ed Engl. 2024 Apr 11:e202405558. doi: 10.1002/anie.202405558. Online ahead of print.ABSTRACT"My biggest motivation is the excitement of obtaining new compounds and materials… My favorite piece of music is Beethoven's Moonlight Sonata." Find out more about Yang Wang in his Introducing… Profile.PMID:38602195 | DOI:10.1002/anie.202405558 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 11, 2024 Category: Chemistry Source Type: research

Water-Ice Microstructures and Hydration States of Acridinium Iodide Studied by Phosphorescence Spectroscopy
Angew Chem Int Ed Engl. 2024 Apr 11:e202405314. doi: 10.1002/anie.202405314. Online ahead of print.ABSTRACTIce has been suggested to have played a significant role in the origin of life partly owing to its ability to concentrate organic molecules and promote reaction efficiency. However, the techniques for studying organic molecules in ice are absorption-based, which limits the sensitivity of measurements. Here we introduce an emission-based method to study organic molecules in water ice: the phosphorescence displays high sensitivity depending on the hydration state of an organic salt probe, acridinium iodide (ADI). The de...
Source: Angewandte Chemie - April 11, 2024 Category: Chemistry Authors: Hongping Liu Hao Su Ning Chen Jie Cen Jiajia Tan Baicheng Zhang Xiaoyu Chen Aoyuan Cheng Shengquan Fu Xiaoguo Zhou Shilin Liu Xuepeng Zhang Shiyong Liu Yi Luo Guoqing Zhang Source Type: research

Ni-Catalyzed Linearizable Cyclization/Coupling with Detachable Silicon-Oxygen Linker: Access to 1,2-Oxasilolanes, 3-Hydroxysilanes and 4-Arylalkanols
Angew Chem Int Ed Engl. 2024 Apr 11:e202404679. doi: 10.1002/anie.202404679. Online ahead of print.ABSTRACTWe disclose a Ni-catalyzed cyclization/alkylmetal interception reaction in which products are readily linearized to permit regiodefined alkene dicarbofunctionalization. This method offers a convenient route to access 1,2-oxasilolane heterocycles, 3-hydroxysilanes and 4-arylalkanols with the formation of C(sp3)-C(sp3) bonds at primary and secondary alkyl carbon centers. In this reaction, a silicon-oxygen (Si-O) bond functions as a detachable linker that can be delinked with several hydride, alkyl, aryl and vinyl nucleo...
Source: Angewandte Chemie - April 11, 2024 Category: Chemistry Authors: Margaret G Lakomy Majji Shankar Ava C Del Rio Ramesh Giri Source Type: research

PolyBorylated Alkenes as Energy-Transfer Reactive Groups: Access to Multi-Borylated Cyclobutanes Combined with Hydrogen Atom Transfer Event
Angew Chem Int Ed Engl. 2024 Apr 11:e202405898. doi: 10.1002/anie.202405898. Online ahead of print.ABSTRACTWhile polyborylated alkenes are being recognized for their elevated status as highly valuable reagents in modern organic synthesis, allowing efficient access to a diverse array of transformations, including the formation of C-C and C-heteroatom bonds, their potential as energy-transfer reactive groups has remained unexplored. Yet, this potential holds the key to generating elusive polyborylated biradical species, which can be captured by olefins, thereby leading to the construction of new highly-borylated scaffolds. H...
Source: Angewandte Chemie - April 11, 2024 Category: Chemistry Authors: Nicole Hanania Nadim Eghbarieh Ahmad Masarwa Source Type: research

Commercializable Naphthalene Diimide Anolytes for Neutral Aqueous Organic Redox Flow Batteries
Angew Chem Int Ed Engl. 2024 Apr 11:e202405427. doi: 10.1002/anie.202405427. Online ahead of print.ABSTRACTNeutral aqueous organic redox flow batteries (AORFBs) hold the potential to facilitate the transition of renewable energy sources from auxiliary to primary energy, the commercial production of anolyte materials still suffers from insufficient performance of high-concentration and the high cost of the preparation problem. To overcome these challenges, this study provides a hydrothermal synthesis methodology and introduces the charged functional groups into hydrophobic naphthalene diimide cores, and prepares a series of...
Source: Angewandte Chemie - April 11, 2024 Category: Chemistry Authors: Xu Liu Heng Zhang Chenjing Liu Zengrong Wang Xuri Zhang Haiyan Yu Yujie Zhao Ming-Jia Li Yinshi Li Ya-Ling He Gang He Source Type: research

In situ Formation of Platinum-Carbon Catalysts in Propane Dehydrogenation
Angew Chem Int Ed Engl. 2024 Apr 11:e202319887. doi: 10.1002/anie.202319887. Online ahead of print.ABSTRACTThe catalytic production of propylene via propane dehydrogenation (PDH) is a key reaction in the chemical industry. By combining operando transmission electron microscopy with density functional theory analysis, we show that the intercalation and ordering of carbon on Pt interstitials to form Pt-C solid solutions is relevant for increasing propylene production. More specifically, we found that at the point of enhanced propylene formation, the structure of platinum nanoparticles is transformed into a transient caesium ...
Source: Angewandte Chemie - April 11, 2024 Category: Chemistry Authors: Hannah C Nerl Milivoj Plodinec Thomas G ötsch Katarzyna Skorupska Robert Schl ögl Travis E Jones Thomas Lunkenbein Source Type: research

Strategies for Achieving Ultra-long ORR Durability - Rh Activates Interatomic Interactions in Alloys
Angew Chem Int Ed Engl. 2024 Apr 9:e202400549. doi: 10.1002/anie.202400549. Online ahead of print.ABSTRACTThe stability of platinum-based alloy catalysts is crucial for the future development of proton exchange membrane fuel cells, considering the potential dissolution of transition metals under complex operating conditions. Here, we report on a Rh-doped Pt3Co alloy that exhibits strong interatomic interactions, thereby enhancing the durability of fuel cells. The Rh-Pt3Co/C catalyst demonstrates exceptional catalytic activity for oxygen reduction reactions (ORR) (1.31 A mgPt-1 at 0.9 V vs. the reversible hydrogen electrode...
Source: Angewandte Chemie - April 10, 2024 Category: Chemistry Authors: Xiaoke Li Xiao Duan Siao Zhang Chuanjie Wang Kang Hua Zejin Wang Yongkang Wu Jia Li Jianguo Liu Source Type: research

Nonlinear Photochromic Reaction Based on Sensitizer-Free Triplet-Triplet Annihilation in a Perylene-Substituted Rhodamine Spirolactam
Angew Chem Int Ed Engl. 2024 Apr 10:e202404140. doi: 10.1002/anie.202404140. Online ahead of print.ABSTRACTNonlinear photochromic reactions that work with weak incoherent light are important for molecular operation with high spatial resolution, and multiple photofunctions based on single molecules. However, nonlinear photochromic compounds generally require complex molecular design, restricting accessibility in various fields. Herein, we report nonlinear photochromic properties in a perylene-substituted rhodamine spirolactam derivative (Rh-Pe), which is synthesized from rhodamine B in facile procedures. Direct excitation o...
Source: Angewandte Chemie - April 10, 2024 Category: Chemistry Authors: Genki Kawai Yuki Nagai Kanna Tsuji Yoshinori Okayasu Jiro Abe Yoichi Kobayashi Source Type: research

Assembly-Induced Dynamic Structural Color in a Host-Guest System for Time-Dependent Anticounterfeiting and Double-Lock Encryption
Angew Chem Int Ed Engl. 2024 Apr 10:e202401208. doi: 10.1002/anie.202401208. Online ahead of print.ABSTRACTManipulation of periodic micro/nanostructures in polymer film is of great importance for academics and industrial applications in anticounterfeiting. However, with the increasing demand on information security, materials with time-dependent features are urgently required, especially the material where the same information can appear more than once on the time scale. Here, one concise strategy to realize time-dependent anticounterfeiting and "double-lock" information encryption based on a host-guest system is proposed,...
Source: Angewandte Chemie - April 10, 2024 Category: Chemistry Authors: Yufan Ji Tianfu Song Haifeng Yu Source Type: research

Chloro-Functionalized Ether-based Electrolyte for High-Voltage and Stable Potassium-Ion Batteries
Angew Chem Int Ed Engl. 2024 Apr 10:e202403269. doi: 10.1002/anie.202403269. Online ahead of print.ABSTRACTEther-based electrolyte is beneficial to obtaining good low-temperature performance and high ionic conductivity in potassium ion batteries. However, the dilute ether-based electrolytes usually result in ion-solvent co-intercalation of graphite, poor cycling stability, and hard to withstand high voltage cathodes above 4.0 V. To address the aforementioned issues, an electron-withdrawing group (chloro-substitution) was introduced to regulate the solid-electrolyte interphase (SEI) and enhance the oxidative stability of et...
Source: Angewandte Chemie - April 10, 2024 Category: Chemistry Authors: Yanyao Hu Hongwei Fu Yuanhui Geng Xiaoteng Yang Ling Fan Jiang Zhou Bingan Lu Source Type: research

Overcoming Electrostatic Interaction via Pulsed Electroreduction for Boosting the Electrocatalytic Urea Synthesis
Angew Chem Int Ed Engl. 2024 Apr 10:e202402684. doi: 10.1002/anie.202402684. Online ahead of print.ABSTRACTElectrocatalytic urea synthesis under ambient conditions offers a promising alternative strategy to the traditional energy-intensive urea industry protocol. Limited by the electrostatic interaction, the reduction reaction of anions at the cathode in the electrocatalytic system is not easily achievable. Here, we propose a novel strategy to overcome electrostatic interaction via pulsed electroreduction. We found that the reconstruction-resistant CuSiOx nanotube, with abundant atomic Cu-O-Si interfacial sites, exhibits u...
Source: Angewandte Chemie - April 10, 2024 Category: Chemistry Authors: Weibin Qiu Shimei Qin Yibao Li Ning Cao Weirong Cui Zedong Zhang Zechao Zhuang Dingsheng Wang Yong Zhang Source Type: research

An Artificial Enzyme for Asymmetric Nitrocyclopropanation of α,β-Unsaturated Aldehydes - Design and Evolution
Angew Chem Int Ed Engl. 2024 Apr 10:e202401635. doi: 10.1002/anie.202401635. Online ahead of print.ABSTRACTThe introduction of an abiological catalytic group into the binding pocket of a protein host allows for the expansion of enzyme chemistries. Here, we report the generation of an artificial enzyme by genetic encoding of a non-canonical amino acid that contains a secondary amine side chain. The non-canonical amino acid and the binding pocket function synergistically to catalyze the asymmetric nitrocyclopropanation of α,β-unsaturated aldehydes by the iminium activation mechanism. The designer enzyme was evolved to an o...
Source: Angewandte Chemie - April 10, 2024 Category: Chemistry Authors: Ming-Zhu Yu Ye Yuan Zhen-Jie Li Thittaya Kunthic He-Xiang Wang Chen Xu Zheng Xiang Source Type: research

Controllable Skeletal and Peripheral Editing of Pyrroles with Vinylcarbenes
Angew Chem Int Ed Engl. 2024 Apr 10:e202401359. doi: 10.1002/anie.202401359. Online ahead of print.ABSTRACTThe skeletal editing of azaarenes through insertion, deletion, or swapping of single atoms has recently gained considerable momentum in chemical synthesis. Here, we describe a practical skeletal editing strategy using vinylcarbenes in-situ generated from trifluoromethyl vinyl N-triftosylhydrazones, leading to the first dearomative skeletal editing of pyrroles through carbon-atom insertion. Furthermore, depending on the used catalyst and substrate, three types of peripheral editing reactions of pyrroles are also disclo...
Source: Angewandte Chemie - April 10, 2024 Category: Chemistry Authors: Yong Yang Qingmin Song Paramasivam Sivaguru Zhaohong Liu Dan Shi Tian Tian Graham de Ruiter Xihe Bi Source Type: research

Photoinduced C(sp3)-H Bicyclopentylation Enabled by an Electron Donor-Acceptor Complex-Mediated Chemoselective Three-Component Radical Relay
Angew Chem Int Ed Engl. 2024 Apr 10:e202400494. doi: 10.1002/anie.202400494. Online ahead of print.ABSTRACTThe photoredox electron donor-acceptor (EDA) complex-mediated radical coupling reaction has gained prominence in the field of organic synthesis, finding widespread application in two-component coupling reactions. However, EDA complex-promoted multi-component reactions are not well developed with only a limited number of examples have been reported. Herein, we report a photoinduced and EDA complex-promoted highly chemoselective three-component radical arylalkylation of [1.1.1]propellane, which allows the direct functio...
Source: Angewandte Chemie - April 10, 2024 Category: Chemistry Authors: Xiaobo Dang Zhixuan Li Jinlong Shang Chenyang Zhang Chao Wang Zhaoqing Xu Source Type: research