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
C(sp3)-H (N-Phenyltetrazole)thiolation as an Enabling Tool for Molecular Diversification
Angew Chem Int Ed Engl. 2024 Apr 24:e202404879. doi: 10.1002/anie.202404879. Online ahead of print.ABSTRACTMethods enabling the broad diversification of C(sp3)-H bonds from a common intermediate are especially valuable in chemical synthesis. Herein, we report a site-selective (N-phenyltetrazole)thiolation of aliphatic and (hetero)benzylic C(sp3)-H bonds using a commercially available disulfide to access N-phenyltetrazole thioethers. The thioether products are readily elaborated in diverse fragment couplings for C-C, C-O, or C-N construction. The C-H functionalization proceeds via a radical-chain pathway involving hydrogen ...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Ashley Zachmann Justine Drappeau Shubin Liu Erik John Alexanian Source Type: research
Discovery of a Plant 14-3-3 Inhibitor Possessing Isoform Selectivity and In Planta Activity
Angew Chem Int Ed Engl. 2024 Apr 24:e202400218. doi: 10.1002/anie.202400218. Online ahead of print.ABSTRACTSynthetic modulators for plant 14-3-3s are promising chemical tools both for understanding the 14-3-3-related signaling pathways and controlling plant physiology. Here, we describe a novel small-molecule inhibitor for 14-3-3 proteins ofArabidopsis thaliana. The inhibitor was identified from unexpected products in DMSO stock solution of an in-house chemical library. Mass spectroscopy, mutant-based analyses, fluorescence polarization assays, and thermal shift assaysrevealed that the inhibitor covalently binds to an allo...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Kotaro Nishiyama Yusuke Aihara Takehiro Suzuki Koji Takahashi Toshinori Kinoshita Naoshi Dohmae Ayato Sato Shinya Hagihara Source Type: research
A Thermosalient and Mechanically Compliant Organic Crystalline Optical Waveguide Switcher
Angew Chem Int Ed Engl. 2024 Apr 24:e202403914. doi: 10.1002/anie.202403914. Online ahead of print.ABSTRACTThe dense and ordered molecular arrangements endow dynamic molecular crystals with fast response, rapid energy conversion, low energy dissipation, and strong coupling between heat/light and mechanical energy. Most of the known dynamic crystals can only respond to a single stimulus, and materials that can respond to multiple stimuli are rare. Here, we report an organic crystalline material that can be bent plastically and is also thermosalient, as its crystals can move when they undergo a reversible phase transition. T...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Qi Di Marieh B Al-Handawi Liang Li Pan če Naumov Hongyu Zhang Source Type: research
Macrocycle-Based Charge Transfer Cocrystals with Dynamically Reversible Chiral Self-Sorting Display Chain Length-Selective Vapochromism to Alkyl Ketones
Angew Chem Int Ed Engl. 2024 Apr 24:e202407095. doi: 10.1002/anie.202407095. Online ahead of print.ABSTRACTChirality-driven self-sorting plays an essential role in controlling the biofunction of biosystems, such as the chiral double-helix structure of DNA from self-recognition by hydrogen bonding. However, achieving precise control over the chiral self-sorted structures and their functional properties for the bioinspired supramolecular systems still remains a challenge, not to mention realizing dynamically reversible regulation. Herein, we report an unprecedented saucer[4]arene-based charge transfer (CT) cocrystal system w...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Meng-Jie Gu Wei-Chen Guo Xiao-Ni Han Ying Han Chuan-Feng Chen Source Type: research
In-Situ Cyclized Polyacrylonitrile as an Electron Selective Layer for n-i-p Perovskite Solar Cell with Enhanced Efficiency and Stability
Angew Chem Int Ed Engl. 2024 Apr 24:e202403264. doi: 10.1002/anie.202403264. Online ahead of print.ABSTRACTIn-situ cyclized polyacrylonitrile (CPAN) is developed to replace n-type metal oxide semiconductors (TiO2 or SnO2) as an electron selective layer (ESL) for highly efficient and stable n-i-p perovskite solar cells (PSCs). The CPAN layer is fabricated via facile in-situ cyclization reaction of polyacrylonitrile (PAN) coated on a conducting glass substrate. The CPAN layer is robust and insoluble in common solvents, and possesses n-type semiconductor properties with a high electron mobility of 4.13 x 10-3 cm2 V-1 s-1. Wit...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Wei-Min Gu Ke-Jian Jiang Xinning Jiao Cai-Yan Gao Xin-Heng Fan Yanlin Song Lian-Ming Yang Source Type: research
Bioorthogonal Cu Single-atom Nanozyme for Synergistic Nanocatalytic Therapy, Photothermal Therapy, Cuproptosis, and Immunotherapy
Angew Chem Int Ed Engl. 2024 Apr 23:e202405937. doi: 10.1002/anie.202405937. Online ahead of print.ABSTRACTSingle-atom nanozymes (SAzymes) with atomically dispersed active sites are potential substitutes for natural enzymes. A systematic study of its multiple functions can in-depth understand SAzymes's nature, which remains elusive. Here, we develop a novel ultrafast synthesis of sputtered SAzymes by in situ bombarding-embedding technique. Using this method, sputtered copper (Cu) SAzymes (CuSA) is developed with unreported unique planar Cu-C3 coordinated configuration. To enhance the tumor-specific targeting, we employ a b...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Luyan Wu Huihui Lin Xiang Cao Qiang Tong Fangqi Yang Yinxing Miao Deju Ye Quli Fan Source Type: research
Living Self-Assembly of Monodisperse Micron-Sized Polymer Vesicles
Angew Chem Int Ed Engl. 2024 Apr 23:e202404589. doi: 10.1002/anie.202404589. Online ahead of print.ABSTRACTArtificial vesicles are recognized as powerful platforms for a large body of research across the disciplines of chemistry, physics and biology. Despite the great progress, control of the size distribution to make uniform vesicles remains fundamentally difficult due to the highly uncontrollable growth kinetics, especially for micron-sized vesicles. Here we report a template-free living self-assembly method to prepare monodisperse vesicles around 1 μm from an alternating copolymer. The polymer forms nanodisks (ca. 9 nm...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Hui Pan Changxu Zhang Wenfeng Jiang Yongfeng Zhou Source Type: research
The Role of Hydrogen Bonds in Thermally Responsive Crystallization-Driven Template Autocatalysis
Angew Chem Int Ed Engl. 2024 Apr 23:e202404838. doi: 10.1002/anie.202404838. Online ahead of print.ABSTRACTAutocatalysis has been well recognized to implicate in the emergence of life and is intrinsic to the biomolecular replication. Recently, an efficient template autocatalysis driven by solvent-free crystallization has been reported. Herein, we unveil the role of intermolecular hydrogen (H) bonds formed by amides in crystallization-driven template autocatalysis (CDTA), which involves the autocatalytic activity, template selectivity, and thermal responsiveness. We found that the thermal-induced cis-trans isomerization of ...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Huimin Wu Qing-Xuan Chen Yang Su Zhen Chen Source Type: research
Crown Ether Electrolyte Induced Li2O2 Amorphization for Low Polarization and Long Lifespan Li-O2 batteries
Angew Chem Int Ed Engl. 2024 Apr 24:e202403521. doi: 10.1002/anie.202403521. Online ahead of print.ABSTRACTLithium-oxygen batteries possess an extremely high theoretical energy density, rendering them a prime candidate for next-generation secondary batteries. However, they still face multiple problems such as huge charge polarization and poor cycle life, which lay a significant gap between laboratory research and commercial applications. In this work, we adapt 15-crown-5 ether (C15) as solvent to regulate the generation of discharge products in lithium-oxygen batteries. The coronal structure endows C15 with strong affinity...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Meng Li Jiaxin Wu Zichang You Zhongqin Dai Yuanfan Gu Lei Shi Meifen Wu Zhaoyin Wen Source Type: research
Building Co16-N3-based UiO-MOF to Expand Design Parameters for MOF Photosensitization
Angew Chem Int Ed Engl. 2024 Apr 24:e202402374. doi: 10.1002/anie.202402374. Online ahead of print.ABSTRACTThe construction of secondary building units (SBUs) in versatile metal-organic frameworks (MOFs) represents a promising method for developing multi-functional materials, especially for improving their sensitizing ability. Herein, we developed a dual small molecules auxiliary strategy to construct a high-nuclear transition-metal-based UiO-architecture Co16-MOF-BDC with visible-light-absorbing capacity. Remarkably, the N3- molecule in hexadecameric cobalt azide SBU offers novel modification sites to precise bonding of s...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Guang-Chen Guo Jiong-Peng Zhao Song Guo Wen-Xiong Shi Fu-Chen Liu Tong-Bu Lu Zhi-Ming Zhang Source Type: research
An Integrative Chemical Recycling Approach for Catalytic Oxidation of Epoxy Resin and in-situ Separation of Degraded Products
Angew Chem Int Ed Engl. 2024 Apr 24:e202405912. doi: 10.1002/anie.202405912. Online ahead of print.ABSTRACTAlthough many approaches have been proposed to recycling waste epoxy resin (EP), the separation of mixed degraded products remains a challenge due to their similar structures. To address this, we present a catalytic oxidation strategy that enables mild degradation of EP and in-situ separation of degraded products through supramolecular interactions. The oxidative degradation relies on FeIV=O radicals with strong oxidizing properties, which are generated from the electron transfer of FeCl2 with reaction reagents. As th...
Source: Angewandte Chemie - April 24, 2024 Category: Chemistry Authors: Lulu Liu Xuehui Liu Xiaohui Li Shimei Xu Yu-Zhong Wang Source Type: research
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
