Meta-Selective Copper-Catalyzed C-H Arylation of Pyridines and Isoquinolines through Dearomatized Intermediates
Angew Chem Int Ed Engl. 2024 Apr 18:e202405385. doi: 10.1002/anie.202405385. Online ahead of print.ABSTRACTC(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, a copper-catalyzed meta-selective C-H arylation of pyridines and isoquinolines through bench-stable dearomatized interme...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Shu-Min Guo Pengwei Xu Armido Studer Source Type: research
Conjugation and Topology Engineering of 2D π-d Conjugated Metal-Organic Frameworks for Robust Potassium Organic Batteries
Angew Chem Int Ed Engl. 2024 Apr 18:e202405239. doi: 10.1002/anie.202405239. Online ahead of print.ABSTRACTThe 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 engineering to demonstrate the application of 2D c-MOFs in robust potassium-ion batteries (PIBs) for the first time...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Linqi Cheng Meiling Qi Jie Yu Xupeng Zhang Heng-Guo Wang Fengchao Cui Yinghui Wang Source Type: research
Radical Homopolymerization of Linear α-Olefins Enabled by 1,4-Cyano Group Migration
Angew Chem Int Ed Engl. 2024 Apr 18:e202402511. doi: 10.1002/anie.202402511. Online ahead of print.ABSTRACTα-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, we report our studies on the homopolymerization of thiocyanate functionalized α-olefins enabled by 1,4-cyano group mig...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Bang An Litao Zhou Shuai Liu Yaxin Zheng Changhu Li Feichen Cui Chaowei Yue Hua Liu Yang Sui Chonglei Ji Jiajun Yan Yifan Li Source Type: research
Ideal Cage-like Pores for Molecular Sieving of Butane Isomers with High Purity and Record Productivity
Angew Chem Int Ed Engl. 2024 Apr 18:e202319674. doi: 10.1002/anie.202319674. Online ahead of print.ABSTRACTn-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, we report a cage-like MOF (SIFSIX-Cu-TPA) with small windows and large cavities which can selectively allow smaller n...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Mingyan Wu Zhenyu Ji Yunzhe Zhou Cheng Chen Daqiang Yuan Maochun Hong Source Type: research
Tailoring Zirconia Supported Intermetallic Platinum Alloy via Reactive Metal-Support Interactions for High-Performing Fuel Cells
Angew Chem Int Ed Engl. 2024 Apr 18:e202400751. doi: 10.1002/anie.202400751. Online ahead of print.ABSTRACTDeveloping 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 L10-PtNi NPs as a proof of concept. Benefiting from the Ni migration during RMSI, the oxygen vacancy concentration in the ...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: 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 Source Type: research
Photogeneration of Chlorine Radical from a Self-Assembled Fluorous 4CzIPN •Chloride Complex: Application in C-H bond Functionalization
Angew Chem Int Ed Engl. 2024 Apr 18:e202402964. doi: 10.1002/anie.202402964. Online ahead of print.ABSTRACTThe 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 to the donor-acceptor carbazole-cyanoarene family, is not only a better photooxidant than 4CzIPN, but also becomes an...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Victor Carr é Pascale Godard Rapha ël Méreau Henri-Pierre Jacquot de Rouville Gediminas Jonusauskas Nathan McClenaghan Thierry Tassaing Jean-Marc Vincent Source Type: research
An MBene Modulating the Buried SnO2/Perovskite Interface in Perovskite Solar Cells
Angew Chem Int Ed Engl. 2024 Apr 18:e202404385. doi: 10.1002/anie.202404385. Online ahead of print.ABSTRACTThe 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, passivate its surface defects and facilitate the charge collection. Moreover, the dipole moment formed at the interface in...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Yuning Zhang Bo Yu Yapeng Sun Jiankai Zhang Zhan Su Huangzhong Yu Source Type: research
Corrigendum: Fast Reaction Kinetics and Commendable Low-Temperature Adaptability of Zinc Batteries Enabled by Aprotic Water-Acetamide Symbiotic Solvation Sheath
Angew Chem Int Ed Engl. 2024 Apr 18:e202406762. doi: 10.1002/anie.202406762. Online ahead of print.NO ABSTRACTPMID:38634524 | DOI:10.1002/anie.202406762 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Source Type: research
Organometallic Chirality Sensing via "Click"-like η6-Arene Coordination with an Achiral Cp*Ru(II) Piano Stool Complex
Angew Chem Int Ed Engl. 2024 Apr 18:e202404594. doi: 10.1002/anie.202404594. Online ahead of print.ABSTRACTPiano 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 based on irreversible acetonitrile displacement of [Cp*Ru(CH3CN)3]PF6 by an aromatic target molecule, a process that is ...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Eryn Nelson Jeffery A Bertke F Yushra Thanzeel Christian Wolf Source Type: research
Linkage Engineering in Covalent Organic Frameworks for Metal-Free Electrocatalytic C2H4 Production from CO2
Angew Chem Int Ed Engl. 2024 Apr 18:e202404738. doi: 10.1002/anie.202404738. Online ahead of print.ABSTRACTElectrocatalytic 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 and mechanism have been lacking. Herein, based on linkage engineering, we construct a novel high-density sp3 N catalytic...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Yang Xiao Jie Lu Kean Chen Yuliang Cao Chengtao Gong Fu-Sheng Ke Source Type: research
Electrophilic Hydrosilylation of Electron-Rich Alkenes Derived from Enamines
Angew Chem Int Ed Engl. 2024 Apr 18:e202404859. doi: 10.1002/anie.202404859. Online ahead of print.ABSTRACTThe 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) are efficient catalysts (particularly the germyl derivatives) in both the silylative dehydrocoupling and hydrosilylatio...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Carlos Laglera-G ándara Juli án Jiménez-Pérez Francisco Jos é Fernández-de-Córdova Pablo R íos Salvador Conejero Source Type: research
Probing Energy-Funneling Kinetics in Nanocrystal Sublattices for Superior X-ray Imaging
Angew Chem Int Ed Engl. 2024 Apr 18:e202404177. doi: 10.1002/anie.202404177. Online ahead of print.ABSTRACTLong-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 via Gd3+-driven microenvironment engineering and Mn2+-mediated radioluminescence profiling. Our photophysical s...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: 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 Source Type: research
Photo-Induced Ruthenium-Catalyzed C-H Arylation Polymerization at Ambient Temperature
Angew Chem Int Ed Engl. 2024 Apr 18:e202400845. doi: 10.1002/anie.202400845. Online ahead of print.ABSTRACTTransition 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 induced by visible light irradiation. The present polymerization can produce various meta- and para-linked polymers in ...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Takuya Michiyuki Isaac Maksso Lutz Ackermann Source Type: research
Chemical Synthesis of Secretoglobin 3A2 Covalent Homodimer and Photocaged Monomeric Variants
In this report, we document the chemical synthesis of SCGB3A2 in multi-milligram quantities. Key to access both monomeric and homo-dimeric SCGB3A2 analogues was the use of KAHA ligation and enabled masking of the cysteine residue. The synthetic proteins were used to investigate SCGB3A2 self-assembly profile, confirming their high propensity to dimerization even in the absence of the key Cys residue.PMID:38635000 | DOI:10.1002/anie.202404992 (Source: Angewandte Chemie)
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Thais Gazzi Maria Heinke Fabienne Landolt Jeffrey W Bode Source Type: research
Considerable Piezochromism in All-Inorganic Zero-Dimensional Perovskite Nanocrystals via Pressure-Modulated Self-Trapped Exciton Emission
Angew Chem Int Ed Engl. 2024 Apr 18:e202406015. doi: 10.1002/anie.202406015. Online ahead of print.ABSTRACTPiezochromic 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 piezochromic range of less than 100 nm in visible region. Here, we achieved an intriguing piezochromism in all-inorganic z...
Source: Angewandte Chemie - April 18, 2024 Category: Chemistry Authors: Zhiwei Ma Songrui Yang Yue Shi Yuan Fu Kai Wang Guanjun Xiao Bo Zou Source Type: research
