Organo-Photocatalytic Anti-Markovnikov Hydroamidation of Alkenes with Sulfonyl Azides: A Combined Experimental and Computational Study
Angew Chem Int Ed Engl. 2024 Apr 17:e202406069. doi: 10.1002/anie.202406069. Online ahead of print.ABSTRACTThe 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 and unactivated alkenes, are suitable for this protocol, providing a convenient and practical method to construct ...
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Authors: Rui Fu Mengyu Xu Yujing Wang Xinxin Wu Xiaoguang Bao Source Type: research
Perfluorooxosulfate Salts as SOF4-Gas-Free Precursors to Multidimensional SuFEx Electrophiles
Angew Chem Int Ed Engl. 2024 Apr 17:e202403797. doi: 10.1002/anie.202403797. Online ahead of print.ABSTRACTSulfur(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 prime example of this, however their preparation from the scarcely available thionyl tetrafluoride (SOF4) limits this ch...
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Authors: Armir Zogu Karim Ullah Stefanos Spanopoulos Ermal Ismalaj Wim M De Borggraeve Joachim Demaerel Source Type: research
Quantitative Factors Introduced in the Feasibility Analysis of Reactive Oxygen Species (ROS)-Sensitive Triggers
Angew Chem Int Ed Engl. 2024 Apr 17:e202403880. doi: 10.1002/anie.202403880. Online ahead of print.ABSTRACTReactive 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 and intended sites and (2) appropriate reaction kinetics to ensure a sufficient level of selectivity for payload releas...
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Authors: Shameer M Kondengadan Binghe Wang Source Type: research
​Genuine Carbene Versus Carbene-Like Reactivity
Angew Chem Int Ed Engl. 2024 Apr 17:e202401020. doi: 10.1002/anie.202401020. Online ahead of print.ABSTRACTSinglet 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 trapping reactions as sufficient proof of carbene formation.PMID:38632078 | DOI:10.1002/anie.202401020 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Authors: Jan Lorkowski Patrick Yorkgitis Melinda R Serrato Milan Gembicky Cezary Pietraszuk Guy Bertrand Rodolphe Jazzar Source Type: research
Efficient Ultraviolet Circularly Polarized Luminescence in Zero-Dimensional Hybrid Cerium Bromides
Angew Chem Int Ed Engl. 2024 Apr 17:e202403727. doi: 10.1002/anie.202403727. Online ahead of print.ABSTRACTUltraviolet 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 characteristic UV emissions derived from the Ce 5d-4f transition. The compounds show simultaneously high photoluminesce...
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Authors: Chen Li Yi Wei Yan Zhang Zhishan Luo Yulian Liu Meiying He Zewei Quan Source Type: research
Blue Long Afterglow and Ultra Broadband Vis-NIR Emission from All-Inorganic Copper-Doped Silver Halide Single Crystals
Angew Chem Int Ed Engl. 2024 Apr 17:e202403927. doi: 10.1002/anie.202403927. Online ahead of print.ABSTRACTAll-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 s) by modulating defect states through doping engineering. The introduction of copper(I) ions into Rb2AgBr3 facilitate...
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Authors: Sijia Wang Runze Liu Juntao Li Caixia Meng Jianyong Liu Junsheng Chen Pengfei Cheng Kaifeng Wu Source Type: research
Corrigendum: Effects of Deuterium Isotopes on Pt(II) Complexes and Their Impact on Organic NIR Emitters
Angew Chem Int Ed Engl. 2024 Apr 16:e202406057. doi: 10.1002/anie.202406057. Online ahead of print.NO ABSTRACTPMID:38627971 | DOI:10.1002/anie.202406057 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Source Type: research
Jiaoyi Ning
Angew Chem Int Ed Engl. 2024 Apr 16:e202406154. doi: 10.1002/anie.202406154. Online ahead of print.ABSTRACT"The most important future applications of my research are flexible/wearable electronic devices… The biggest challenge facing my generation of scientists is the intense pressure to secure tenure and research funding within limited timelines, while most groundbreaking discoveries requires long-term experience and knowledge accumulation…" Find out more about Jiaoyi Ning in her Introducing… Profile.PMID:38627973 | DOI:10.1002/anie.202406154 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Source Type: research
Alex J. Plajer
Angew Chem Int Ed Engl. 2024 Apr 16:e202406012. doi: 10.1002/anie.202406012. Online ahead of print.ABSTRACT"A key experience in my education/career was receiving a lot of scientific freedom during my PhD which gave me the confidence to go independent comparatively early… My favorite saying is: 'Failure is success in progress.' " Find out more about Alex J. Plajer in his Introducing… Profile.PMID:38627976 | DOI:10.1002/anie.202406012 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Source Type: research
Vakayil K. Praveen
Angew Chem Int Ed Engl. 2024 Apr 16:e202406217. doi: 10.1002/anie.202406217. Online ahead of print.ABSTRACT"I am waiting for the day when someone will invent a 'truly living artificial cell'… My favorite saying is: 'Live as if you were to die tomorrow. Learn as if you were to live forever.' " Find out more about Vakayil K. Praveen in his Introducing… Profile.PMID:38627983 | DOI:10.1002/anie.202406217 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Source Type: research
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 Engl. 2024 Apr 17:e202401989. doi: 10.1002/anie.202401989. Online ahead of print.ABSTRACTWhile 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 work, we demonstrate that extreme "antipodes" of the "worlds of catalysis" such as syngas-based high-pressure hydroformy...
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Authors: Hannah Bork Kim E Na ße Andreas J Vorholt Harald Gr öger Source Type: research
A Dicopper(II)-Based Carbonic Anhydrase Model - Quantum-Chemical Evaluation of the Mechanistic Pathway
Angew Chem Int Ed Engl. 2024 Apr 17:e202319530. doi: 10.1002/anie.202319530. Online ahead of print.ABSTRACTThe 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 that copper(II) is coordinated to patellamide derivatives in Prochloron cells. An interesting question therefore is, ...
Source: Angewandte Chemie - April 17, 2024 Category: Chemistry Authors: Peter Comba Gunasekaran Velmurugan Philipp Baur Source Type: research
Breaking Highly Ordered PtPbBi Intermetallic with Disordered Amorphous Phase for Boosting Electrocatalytic Hydrogen Evolution and Alcohol Oxidation
In this study, we report the synthesis of ultrathin A/IMC PtPbBi nanosheets (NSs) for boosting hydrogen evolution reaction (HER) and alcohol oxidation reactions. The resulting A/IMC PtPbBi NSs exhibit a remarkably low overpotential of only 25 mV at 10 mA cm-2 for the HER in an acidic electrolyte, together with outstanding stability for 100 h. In addition, the PtPbBi NSs show high mass activities for methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR), which are 13.2 and 14.5 times higher than those of commercial Pt/C, respectively. Density functional theory calculations demonstrate that the synergistic e...
Source: Angewandte Chemie - April 16, 2024 Category: Chemistry Authors: 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 Source Type: research
Fabrication of Large-area Multi-stimulus Responsive Thin Films via Interfacially Confined Irreversible Katritzky Reaction
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 an area up to 50 cm². The thin films exhibit fast photo-mechanical motions (a response time of ca 0.1 s), vapor-mechanical motions, as well as photo-chromic and solvato-chromic behaviors. It was revealed that the reason behind the observable motions is proton transfer from the imine groups to the carbonyl structures wi...
Source: Angewandte Chemie - April 16, 2024 Category: Chemistry Authors: Yuanhong Shu Yan Luo Hexi Wei Lingya Peng Jingjing Liang Binbin Zhai Liping Ding Yu Fang Source Type: research
Umbrella-Shaped Amphiphiles: Internal Alkylation of an Aromatic Micelle and Its Impact on Cavity Features
Angew Chem Int Ed Engl. 2024 Apr 15:e202404088. doi: 10.1002/anie.202404088. Online ahead of print.ABSTRACTTo 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 significantly enhances the stability of the micellar structures against dilution (up to 9 μM) and heat (up to >120 Â...
Source: Angewandte Chemie - April 16, 2024 Category: Chemistry Authors: Masaya Endo Shinji Aoyama Yoshitaka Tsuchido Lorenzo Catti Michito Yoshizawa Source Type: research
