Assembly of Glycopeptides in Living Cells Resembling Viral Infection for Cargo Delivery
Angew Chem Int Ed Engl. 2024 Apr 24:e202404703. doi: 10.1002/anie.202404703. Online ahead of print.ABSTRACTSelf-assembly in living cells represents one versatile strategy for drug delivery; however, it suffers from the limited precision and efficiency. Inspired by viral traits, we here report a cascade targeting-hydrolysis-transformation (THT) assembly of glycosylated peptides in living cells holistically resembling viral infection for efficient cargo delivery and combined tumor therapy. We design a glycosylated peptide via incorporating a β-galactose-serine residue into bola-amphiphilic sequences. Co-assembling of the gl...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Feng Tian Ruo-Chen Guo Chunxia Wu Xin Liu Zeyu Zhang Yamei Wang Hao Wang Gongyu Li Zhilin Yu Source Type: research
Enantiopure [6]-Azairidahelicene by Dynamic Kinetic Resolution of a Configurationally Labile [4]-Helicene
Angew Chem Int Ed Engl. 2024 Apr 24:e202406663. doi: 10.1002/anie.202406663. Online ahead of print.ABSTRACTA pair of enantiopure [6]-azairidahelicenes incorporating chirality at the metal center and on the helicenic ligand were synthesized by dynamic kinetic resolution (dkr) of a configurationally labile [4]-helicenic ligand (4-(2-pyridyl)-benzo[g]phenanthrene, L1H) using bis-cyclometalated chiral-at-metal only iridium(III) precursors as chiral inductors. The origin of the observed dkr is attributed to the different conformation and stability of diastereomeric reaction intermediates formed during the cyclometalation proces...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Ariadna Pazos Carlos M Cruz Juan M Cuerva Ivan Rivilla Fernando P Coss ío Zoraida Freixa Source Type: research
Crystalline Porous Organic Frameworks Based on Multiple Dynamic Linkages
Angew Chem Int Ed Engl. 2024 Apr 24:e202405027. doi: 10.1002/anie.202405027. Online ahead of print.ABSTRACTA novel class of crystalline porous materials has been developed utilizing multilevel dynamic linkages, including covalent B-O, dative B←N and hydrogen bonds. Typically, boronic acids undergo in situ condensation to afford B3O3-based units, which further extend to molecular complexes or chains via B←N bonds. The obtained superstructures are subsequently interconnected via hydrogen bonds and π-π interactions, producing crystalline porous organic frameworks (CPOFs). The CPOFs display excellent solution processabil...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Bo Liu Panyue Guo Xinyu Guan Xuexue Tian Fei Du Weiqing Xie Hai-Long Jiang Source Type: research
Repurposing Visible-Light-Excited Ene-Reductases for Diastereo- and Enantioselective Lactones Synthesis
Angew Chem Int Ed Engl. 2024 Apr 24:e202402673. doi: 10.1002/anie.202402673. Online ahead of print.ABSTRACTRepurposing enzymes to catalyze non-natural asymmetric transformations that are difficult to achieve using traditional chemical methods is of significant importance. Although radical C-O bond formation has emerged as a powerful approach for constructing oxygen-containing compounds, controlling the stereochemistry poses a great challenge. Here we present the development of a dual bio-/photo-catalytic system comprising an ene-reductase and an organic dye for achieving stereoselective lactonizations. By integrating direc...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Jinhai Yu Qiaoyu Zhang Beibei Zhao Tianhang Wang Yu Zheng Binju Wang Yan Zhang Xiaoqiang Huang Source Type: research
Silylenes with a small chalcogenide substituent: Tuning frontier orbital energies from O to Te
Angew Chem Int Ed Engl. 2024 Apr 24:e202405319. doi: 10.1002/anie.202405319. Online ahead of print.ABSTRACTThe general synthesis of heteroleptic acyclic silylenes with a bulky carbazolyl substituent (dtbpCbz) is detailed and a series of compounds with a chalcogenide substituent of the type [(dtbpCbz)SiE16R] (E16R = OtBu, SEt, SePh, TePh) is reported. With the bulky carbazolyl substituent present, the chalcogenide moiety can be very small, as is shown by incorporating groups as small as ethyl, phenyl or tert-butyl. For the first time, the electronic properties of the silylene can be tuned along a complete series of chalcoge...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Maximilian P M üller Alexander Hinz Source Type: research
On the Dendrite-Suppressing Effect of Laser-Processed Polylactic Acid-Derived Carbon Coated Zinc Anode in Aqueous Zinc Ion Batteries
Angew Chem Int Ed Engl. 2024 Apr 24:e202405048. doi: 10.1002/anie.202405048. Online ahead of print.ABSTRACTA major bottleneck limiting the commercialization of aqueous zinc ion batteries (AZIBs) is dendrite formation on the zinc anode during the plating/stripping process, which leads to rapid performance and device failure. In this regard, researchers are trying to design more stable anodes toward suppressing dendrite formation. One possible solution to tackle this problem and to extend the cycling life of AZIBs is to modify the zinc anode surface by coating carbonaceous materials, enabling controlled charge flux and unifo...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Maryam Abouali Sadaf Adhami Somayeh Asadi Haris Recep Yuksel Source Type: research
Bithiophene-Functionalized Infrared Two-Photon Absorption Metal Complexes as Single-Molecule Platforms for Synergistic Photodynamic, Photothermal, and Chemotherapy
Angew Chem Int Ed Engl. 2024 Apr 24:e202402028. doi: 10.1002/anie.202402028. Online ahead of print.ABSTRACTA planar conjugated ligand functionalized with bithiophene and its Ru(II), Os(II), and Ir(III) complexes have been constructed as single-molecule platform for synergistic photodynamic, photothermal, and chemotherapy. The complexes have significant two-photon absorption at 808 nm and remarkable singlet oxygen and superoxide anion production in aqueous solution and cells when exposed to 808 nm infrared irradiation. The most potent Ru(II) complex Ru7 enters tumor cells via the rare macropinocytosis, locates in both nucle...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Xue-Lian Li Meng-Fan Wang Li-Zhen Zeng Guo-Kui Li Run-Yu Zhao Fu-Dan Liu Yun Li Yu-Fei Yan Qishuai Liu Zhao Li Hongbin Zhang Xiaoxia Ren Feng Gao Source Type: research
Hyperbranched Vitrimer for Ultrahigh Energy Dissipation
Angew Chem Int Ed Engl. 2024 Apr 24:e202406937. doi: 10.1002/anie.202406937. Online ahead of print.ABSTRACTPolymers are ideally utilized as damping materials due to the high internal friction of molecular chains, enabling effective suppression of vibrations and noises in various fields. Current strategies rely on broadening the glass transition region or introducing additional relaxation components to enhance the energy dissipation capacity of polymeric damping materials. However, it remains a significant challenge to achieve high damping efficiency through structural control while maintaining dynamic characteristics. In t...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Lin Cheng Jun Zhao Zhongqiang Xiong Sijun Liu Xuzhou Yan Wei Yu Source Type: research
Synthesis of 18F-labeled Aryl Trifluoromethyl Sulfones, -Sulfoxides, and -Sulfides for Positron Emission Tomography
Angew Chem Int Ed Engl. 2024 Apr 24:e202404278. doi: 10.1002/anie.202404278. Online ahead of print.ABSTRACTPositron emission tomography (PET) is becoming increasingly important in nuclear medicine and drug discovery. To date, the development of many potential PET tracers is hampered by the lack of suitable synthetic pathways for their preparation. This is particularly true for the highly desired radiolabeling of compounds bearing [18F]CF3-groups. For instance, S(O)nCF3-groups (n = 0, 1, 2) serve as structural motif in a range of biologically active compounds, but their radiosynthesis remains largely unprecedented (for n = ...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Lukas Veth Albert D Windhorst Danielle J Vugts Source Type: research
Crystalline Olefin-Linked Chiral Covalent Organic Frameworks as a Platform for Asymmetric Catalysis
Angew Chem Int Ed Engl. 2024 Apr 24:e202405769. doi: 10.1002/anie.202405769. Online ahead of print.ABSTRACTThe construction of olefin-linked chiral covalent organic frameworks (COFs) with high crystallinity is highly desirable while remains great challenge due to the poor reversibility of the formation reaction for the olefin linkages during the in situ structural self-healing process. Herein, we successfully synthesized two sets of enantiomeric olefin-linked COFs. The chiral catalytic groups are uniformly distributed on the pore walls of COFs, resulting in the full exposure of catalytic sites to the reactants in asymmetri...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Ting He Ivan Keng Wee On Shuai Bi Ziyue Huang Jingjing Guo Zhifang Wang Yanli Zhao Source Type: research
A Photodynamic and Photochemotherapeutic Platinum-Iridium Charge-Transfer Conjugate for Anticancer Therapy
Angew Chem Int Ed Engl. 2024 Apr 24:e202400476. doi: 10.1002/anie.202400476. Online ahead of print.ABSTRACTThe novel hetero-dinuclear complex trans,trans,trans-[PtIV(py)2(N3)2(OH)(μ-OOCCH2CH2CONHCH2-bpyMe)IrIII(ppy)2]Cl (Pt-Ir), exhibits charge transfer between the acceptor photochemotherapeutic Pt(IV) (Pt-OH) and donor photodynamic Ir(III) (Ir-NH2) fragments. It is stable in the dark, but undergoes photodecomposition more rapidly than the Pt(IV) parent complex (Pt-OH) to generate Pt(II) species, an azidyl radical and 1O2. The Ir(III)* excited state, formed after irradiation, can oxidise NADH to NAD⋅ radicals and NAD+. ...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Huayun Shi Oliver W L Carter Fortuna Ponte Cinzia Imberti Miguel A Gomez-Gonzalez Fernando Cacho-Nerin Paul D Quinn Julia E Parker Emilia Sicilia Huaiyi Huang Peter J Sadler Source Type: research
Including the Ensemble of Unstructured Conformations in the Analysis of Protein's Native State by High-Pressure NMR Spectroscopy
Angew Chem Int Ed Engl. 2024 Apr 24:e202401343. doi: 10.1002/anie.202401343. Online ahead of print.ABSTRACTThe analysis of pressure induced changes in the chemical shift of proteins allows statements on structural fluctuations proteins exhibit at ambient pressure. The inherent issue of separating general pressure effects from structural related effects on the pressure dependence of chemical shifts has so far been addressed by considering the characteristics of random coil peptides on increasing pressure. In this work, chemically and pressure denatured states of the cold shock protein B from Bacillus subtilis (BsCspB) have ...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Frederic Berner Michael Kovermann Source Type: research
Record High Iodate Anion Capture by a Redox-Active Cationic Polymer Network
Angew Chem Int Ed Engl. 2024 Apr 24:e202400849. doi: 10.1002/anie.202400849. Online ahead of print.ABSTRACTAs a critical radioactive anionic contaminant, traditional adsorbents primarily remove iodate (IO3-) through ion exchange or hard acid-hard base interactions, but suffer from limited affinity and capacity. Herein, employing the synergistic effect of ion exchange and redox, we successfully synthesized a redox-active cationic polymer network (SCU-CPN-6, [C9H10O2N5•Cl]n) by merging guanidino groups with ion-exchange capability and phenolic groups with redox ability via a Schiff base reaction. SCU-CPN-6 exhibits a groun...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Qi Guo Jie Li Yuting Zhao Lingyi Li Linwei He Fuqiang Zhao Fuwan Zhai Mingxing Zhang Long Chen Zhifang Chai Shuao Wang Source Type: research
Hierarchical Self-assembly of Multidimensional Functional Materials from Sequence-defined Peptoids
In this study, we present a molecular-level understanding of the hierarchical assembly of sequence-defined peptoids into multidimensional functional materials, including twisted nanotube bundles serving as a highly efficient artificial light harvesting system. By employing synchrotron-based powder X-ray diffraction and analyzing single crystal structures of model compounds, we elucidated the molecular packing and mechanisms underlying the assembly of peptoids into multidimensional nanostructures. Our findings demonstrate that incorporating aromatic functional groups, such as tetraphenyl ethylene (TPE), at the termini of as...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Li Shao Dehong Hu Shao-Liang Zheng Thi Kim Hoang Trinh Wenhao Zhou Haoyu Wang Yanxu Zong Changning Li Chun-Long Chen Source Type: research
Paper Spray Mass Spectrometry with On-Paper Electrokinetic Manipulations: Part- Per-Trillion Detection of Per/Polyfluoroalkyl Substances in Water and Opioids in Urine
Angew Chem Int Ed Engl. 2024 Apr 24:e202401729. doi: 10.1002/anie.202401729. Online ahead of print.ABSTRACTWe developed a simple, paper-based device that enables sensitive detection by mass spectrometry (MS) without solid phase extraction or other sample preparation. Using glass fiber filter papers within a 3D printed holder, the device employs electrokinetic manipulations to stack, separate, and desalt charged molecules on paper prior to spray into the MS. Due to counter-balanced electroosmotic flow and electrophoresis, charged analytes stack on the paper and desalting occurs in minutes. One end of the paper strip was cut...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Magnus Rydberg Merlin Bruening Nicholas Manicke Source Type: research
