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Exploring Pyroelectricity, Thermal and Photochemical Switching in a Hybrid Organic-Inorganic Crystal by In-situ X-ray Diffraction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Joshua J. Morris, Chris R. Bowen, Ben A. Coulson, Mark Eaton, Paul R. Raithby, Lucy K. Saunders, Jonathan M. Skelton, Qingping Wang, Mark R. Warren, Yan Zhang, Lauren Hatcher
The switching behavior of the novel hybrid material (FA)Na[Fe(CN)5(NO)].H2O (1) in response to temperature (T), light irradiation and electric field (E) is studied using in-situ X-ray diffraction (XRD). Crystals of 1 display piezoelectricity, pyroelectricity, second and third harmonic generation. XRD shows that the FA+ are disordered at room-temperature, but stepwise cooling from 273-100K induces gradual
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Stabilizing Lattice Oxygen through Mn Doping in NiCo2O4−d Spinel Electrocatalysts for Efficient and Durable Acid Oxygen Evolution Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Hongyu Zhao, Liu Zhu, Jie Yin, Jing Jin, Xin Du, Lei Tan, Yong Peng, Pinxian Xi, Chun-Hua Yan
Design the electrocatalysts without noble metal is still a challenge for oxygen evolution reaction (OER) in acid media. Herein, we reported the manganese doping method to decrease the concentration of oxygen vacancy (Vo) and form the Mn−O structure adjacent octahedral sites in spinel NiCo2O4−δ (NiMn1.5Co3O4−δ), which highly enhanced the activity and stability of spinel NiCo2O4−δ with a low overpotential
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Dimethyl Carbonate Synthesis from CO2 over CeO2 with Electron-enriched Lattice Oxygen Specises Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Guoqiang Hou, Qi Wang, Di Xu, Haifeng Fan, Kaidi Liu, Yangyang Li, Xiang-Kui Gu, Mingyue Ding
The direct synthesis of dimethyl carbonate (DMC) from CO2 has both theoretical and practical value in carbon neutrality, but its efficiency is far from the application requirements due to the lacks of understanding of reaction mechanism and rational design of catalyst. Herein, abundant electron-enriched lattice oxygen species were introduced into CeO2 catalyst by constructing a large number of point
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Self-Assembly Morphology Manipulation by Side-chain Engineering of Quinoxaline-Substituted Organic Photothermal Molecules for Efficient Solar-Thermal Conversion and Application Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Jing Li, Luoqing Wang, Yuyu Pan, Han Wang, Chenyang Zhang, Shizhang Li, Xian-Kai Chen, Tao Jia, Kai Wang
Organic photothermal materials have attracted more and more attention due to the structural diversity, flexibility, and compatibility. However, the energy conversion efficiency is limited due to the narrow absorption spectrum, strong reflection/transmittance and insufficient non-radiative decay. Herein, we synthesized two quinoxaline-based D-A-D-A-D type molecules with ethyl (BQE) or carboxylate (BQC)
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Near-Infrared Light Activated Formulation for the Spatially Controlled Release of CRISPR-Cas9 Ribonucleoprotein for Brain Gene Editing Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Susana Simões, Miguel Lino, Angela Barrera, Catarina Rebelo, Francesca Tomatis, Andreia Vilaça, Christopher Breunig, Andrea Neuner, João Peça, Ricardo González, Alexandra Carvalho, Stefan Stricker, Lino Ferreira
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Classifieds: Jobs and Awards, Products and Services Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18
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The Stability of Hydrogen-Bonded Ion-Pair Complex Unexpectedly Increases with Increasing Solvent Polarity Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Debashree Manna, Rabindranath Lo, Jaroslav Vacek, Vijay Madhav Miriyala, Petr Bouř, Tao Wu, Zuzana Osifova, Dana Nachtigallová, Martin Dračinský, Pavel Hobza
The generally observed decrease of the electrostatic energy in the complex with increasing solvent polarity has led to the assumption that the stability of the complexes with ion-pair hydrogen bonds decreases with increasing solvent polarity. Besides, the smaller solvent-accessible surface area (SASA) of the complex in comparison with the isolated subsystems results in a smaller solvation energy of
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The Celiac-Disease Superantigen Oligomerizes and Increases Permeability in an Enterocyte Cell Model Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Maria Georgina Herrera, Maria Julia Amundarain, Philipp W Dörfler, Veronica I Dodero
Celiac disease (CeD) is an autoimmune disorder triggered by gluten proteins, affecting approximately 1% of the global population. The 33-mer deamidated gliadin peptide (DGP) is a metabolically modified wheat-gluten superantigen for CeD. Here, we demonstrate that the 33-mer DGP spontaneously assembles into oligomers with a diameter of approximately 24 nm. The 33-mer DGP oligomers present two main secondary
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Radicalizing CO by Mononuclear Palladium(I) Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Tim Bruckhoff, Joachim Ballmann, Lutz H. Gade
A mononuclear, T-shaped palladium(I) d9 metalloradical (3), stabilized by a bulky carbazole-based PNP-ligand, was obtained by reduction of palladium chloride or thermal Pd-C bond homolysis of the corresponding neopentyl complex. Pressurizing with CO gave the Pd(I) carbonyl complex, which was structurally characterized by X-ray diffraction. Delocalization of the unpaired electron to the carbonyl carbon
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Dual Enhancement of Phosphorescence and Circularly Polarized Luminescence through Entropically Driven Self-Assembly of a Platinum(II) Complex Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Yanqing Wang, Na Li, Liangwen Chu, Zelin Hao, Junyu Chen, Jiang Huang, Junlin Yan, Hongtao Bian, Pengfei Duan, Jing Liu, Yu Fang
Addressing the dual enhancement of circular polarization (glum) and luminescence quantum yield (QY) in circularly polarized luminescence (CPL) systems poses a significant challenge. In this study, we present an innovative strategy utilizing the entropically driven self-assembly of amphiphilic phosphorescent platinum(II) complexes (L-Pt) with tetraethylene glycol chains, resulting in unique temperature
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Light-Regulated Nucleation for Growing Highly Uniform Single-Crystalline Microrods Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Lishan Sun, Yanjun Gong, Yanxue Che, Hongwei Ji, Bing Liu, Yanke Che, Jincai Zhao
We report a light-irradiation method to control the synchronous nucleation of a donor-acceptor (D-A) fluorophore for growing highly uniform single-crystalline microrods, which is in sharp contrast to the prevailing methods of inhibiting spontaneous nucleation and additionally adding seeds. The D-A fluorophore was observed to undergo photoinduced electron transfer to CrCl3, leading to the generation
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Experimental Evidence for Non-Fermi-Contact J Coupling Across Chalcogen Bonds in Ionic Salt Cocrystal Polymorphs Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Tamali Nag, Victor V. Terskikh, David L. Bryce
A pair of novel polymorphic ionic cocrystals of 3,4-dicyanotelluradiazole and tetraphenylphosphonium bromide are synthesized and are characterized by single-crystal XRD. Strong and directional non-covalent chalcogen bonds (ChB) between Te and Br are analyzed via solid-state NMR to reveal large and anisotropic J(125Te,79/81Br) coupling tensors, providing unequivocal evidence for non-Fermi contact contributions
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Stereodivergent, Kinetically Controlled Isomerization of Terminal Alkenes via Nickel Catalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Camille Z. Rubel, Anne K. Ravn, Hang Chi Ho, Shenghua Yang, Zi-Qi Li, Keary Mark Engle, Julien C. Vantourout
Because internal alkenes are more challenging synthetic targets than terminal alkenes, metal-catalyzed olefin mono-transposition (i.e., positional isomerization) approaches have emerged to afford valuable E- or Z- internal alkenes from their complementary terminal alkene feedstocks. However, the applicability of these methods has been hampered by lack of generality, commercial availability of precatalysts
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Introducing Carborane Clusters into Crystalline Frameworks via Thiol-yne Click Chemistry for Energetic Materials Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Tian-Li Pu, Xu-Yang Wang, Zhi-Bing Sun, Xi-Yan Dong, Qian-You Wang, Shuang-Quan Zang
Crystalline frameworks represent a cutting-edge frontier in material science, and recently, there has been a surge of interest in energetic crystalline frameworks. However, the well-established porosity often leads to diminished output energy, necessitating a novel approach for performance enhancement. Thiol-yne coupling, a versatile metal-free click reaction, has been underutilized in crystalline
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Metabolic Glycoengineering-Enabled Molecularly Specific Acoustic Tweezing Cytometry for Targeted Mechanical Stimulation of Cell Surface Sialoglycans Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Weiping Li, Jiatong Guo, Eric C. Hobson, Xufeng Xue, Qingjiang Li, Jianping Fu, Cheri X. Deng, Zhongwu Guo
This study developed a new type of dibenzocyclooctyne (DBCO)-functionalized microbubbles (MBs) and validated their attachment to azide-labelled sialoglycans on human pluripotent stem cells (hPSCs) generated via metabolic glycoengineering (MGE). This enabled application of mechanical forces to sialoglycans on hPSCs via molecularly specific acoustic tweezing cytometry (mATC), i.e., displacing sialoglycan-anchored
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Reduction-Tolerance Electrolyte Design for High-Energy Lithium Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Chuangchao Sun, Ruhong Li, Suting Weng, Chunnan Zhu, Long Chen, Sen Jiang, Long Li, Xuezhang Xiao, Chengwu Liu, Lixin Chen, Tao Deng, Xuefeng Wang, Xiulin Fan
Lithium batteries employing Li or silicon (Si) anodes hold promise for the next-generation energy storage systems. However, their cycling behavior encounters rapid capacity degradation due to the vulnerability of solid electrolyte interphases (SEIs). Though anion-derived SEIs mitigate this degradation, the unavoidable reduction of solvents introduces heterogeneity to SEIs, leading to fractures during
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Photocatalytic Functionalization of Dehydroalanine-Derived Peptides in Batch and Flow Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Nikolaos Kaplaneris, Merve Akdeniz, Méritxell Fillols, Francesca Arrighi, Fabian Raymenants, Gana Sanil, Daniel T. Gryko, Timothy Noel
Unnatural amino acids, and their synthesis via the late-stage functionalization (LSF) of peptides, play a crucial role in areas such as drug design and discovery. Historically, the LSF of biomolecules has predominantly utilized traditional synthetic methodologies that exploit nucleophilic residues, such as cysteine, lysine or tyrosine. In this study, we present a photocatalytic hydroarylation process
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Iso-E-Codelock: A Rebuilding-free Electrochemical Chip with a Customizable Decoding Probe for Real-Time and Portable Pathogen Diagnostics Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-18 Yichen Liu, Yidan Tang, Yin Bao, Kaiwei Cai, Baiyang Lu, Rujian Zhao, Chunxu Yu, Yan Du, Bingling Li
In order to realize portable pathogen diagnostics with easier quantitation, digitization and integration, we develop a ready-to-use electrochemical sensing strategy (Iso-E-Codelock) for real-time detection of isothermal nucleic acid amplification. Bridged by a branch DNA as codelock, the isothermal amplicon is transduced into increased current of an electrochemical probe, holding multiple advantages
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Robust Covalent Organic Framework Photocatalysts for H2O2 Production: Linkage Position Matters Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Tao Yang, De Zhang, Aiguo Kong, Yingying Zou, Ling Yuan, Chao Liu, Sijia Luo, Guangfeng Wei, Chengzhong Yu
Covalent organic frameworks (COFs) are promising photocatalysts for hydrogen peroxide (H2O2) synthesis. However, the nature of organic polymers makes the balance between high activity and stability challenging. We demonstrate that the linkage position matters in the design of robust COF photocatalysts with durable high activity without sacrificial reagents. COFs with ortho- and para-linkages (o-COFs
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Enhanced Detection of Novel Low-Frequency Gene Fusions via High-Yield Ligation and Multiplexed Enrichment Sequencing Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Yi Wu, Jinxiao Guo, Wenjun Li, Xuehao Xiu, Deepak Thirunavukarasu, Yudong Wang, Kai Wang, Weiyu Chen, David yu Zhang, Xiurong Yang, Chunhai Fan, Ping Song
Panel-based methods are commonly employed for the analysis of novel gene fusions in precision diagnostics and new drug development in cancer. However, these methods are constrained by limitations in ligation yield and the enrichment of novel gene fusions with low variant allele frequencies. In this study, we conducted a pioneering investigation into the stability of double-stranded adapter DNA, resulting
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The Influence of Ions on the Electrochemical Stability of Aqueous Electrolytes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Yiming Sui, Alexis Scida, Bo Li, Cheng Chen, Yanke Fu, Yanzhao Fang, Peter Alex Greaney, Tomas Osborn Popp, De-en Jiang, Chong Fang, Xiulei Ji
The electrochemical stability window of water is known to vary with the type and concentration of dissolved salts. However, the underlying influence of ions on the thermodynamic stability of aqueous solutions has not been fully understood. Here, we investigated the electrolytic behaviors of aqueous electrolytes as a function of different ions. Our findings indicate that ions with high ionic potential
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Entropy-Driven Direct Air Electrofixation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Yuntong Sun, Ming Li, Jingjing Duan, Markus Antonietti, Sheng Chen
According to the rule of chemical thermodynamics, the catalytic activation of small molecules (like N2 in air and CO2 in flue gas) generally exhibits a negative activity dependence on O2 owning to the competitive oxygen reduction reaction (ORR). Nevertheless, some catalysts can show positive activity dependence for N2 electrofixation, an important route to produce ammonia under ambient condition. Here
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The Impact of Metagenomics on Biocatalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Bethany N Hogg, Christian Schnepel, James D Finnigan, Simon J Charnock, Martin A Hayes, Nicholas John Turner
In the ever-growing demand for sustainable ways to produce high-value small molecules, biocatalysis has come to the forefront of greener routes to these chemicals. As such, the need to constantly find and optimise suitable biocatalysts for specific transformations has never been greater. Metagenome mining has been shown to rapidly expand the toolkit of promiscuous enzymes needed for new transformations
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Highly selective acetylene-to-ethylene electroreduction over Cd-decorated Cu catalyst with efficiently inhibited carbon-carbon coupling Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Zeping Wang, Chengyu Li, Gongao Peng, Run Shi, Lu Shang, Tierui Zhang
Electrochemical acetylene reduction (EAR) employing Cu catalysts represents an environmentally friendly and cost-effective method for ethylene production and purification. However, Cu-based catalysts encounter product selectivity issues stemming from carbon-carbon coupling and other side reactions. We explored the use of secondary metals to modify Cu-based catalysts and identified Cd decoration as
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Reticular Modulation of Piezofluorochromic Behaviors in Organic Molecular Cages by Replacing Non-Luminous Components Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Yang Li, Kai Wang, Rui Feng, Jingtian Wang, Xiao-Juan Xi, Feifan Lang, Quanwen Li, Wei Li, Bo Zou, Jiandong Pang, Xian-He Bu
Organic piezochromic materials that manifest pressure-stimuli-responses are important in various fields such as data storage and anticounterfeiting. The manipulation of piezofluorochromic behaviors for these materials is promising but remains a great challenge. Herein, a non-luminous components regulated strategy is developed and organic molecular cages (OMCs), a burgeoning class of crystalline organic
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Enantioselective Hydrofunctionalization of Cyclobutenones: Total Synthesis of gem-Dimethylcyclobutane Natural Products Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-17 Shaowei Wang, Changxu Zhong, Yingchao Huang, Ping Lu
Cyclobutanes with a gem-dimethyl group are common motifs in natural products. However, strategies for constructing enantioenriched gem-dimethyl cyclobutanes are still underdeveloped. Herein, we report an enantioselective approach to synthesize a broad group of chiral 2,3-disubstituted cyclobutanones through sequential 1,4-conjugate addition/trapping/cross-coupling of readily available cyclobutenones
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Weakly Coordinating Diluent Modulated Solvation Chemistry for High‐Performance Sodium Metal Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Jiaxin Li, Simi Sui, Xunzhu Zhou, Kaixiang Lei, Qian Yang, Shenxu Chu, Lin Li, Yuqing Zhao, Mengjia Gu, Shulei Chou, Shijian Zheng
Diluents have been extensively employed to overcome the disadvantages of high viscosity and sluggish kinetics of high‐concentration electrolytes, but generally do not change the pristine solvation structure. Herein, a weakly coordinating diluent, hexafluoroisopropyl methyl ether (HFME), is applied to regulate the coordination of Na+ with diglyme and anion and form a diluent‐participated solvate. This
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Molecule and Microstructure Modulations of Cyano‐Containing Electrodes for High‐Performance Fully Organic Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Yongling Wang, Yunhai Zhu, Zixuan Chen, Xu Yang, Rongyu Zhang, Hengguo Wang, Yingkui Yang
Cyano‐containing electrodes usually promise high theoretical potentials while suffering from uncontrollable self‐dissolution and sluggish reaction kinetics. Herein, to remedy their limitations, an unprecedented core‐shell heterostructured electrode of carbon nanotubes encapsulated in poly(1,4‐dicyanoperfluorobenzene sulfide) (CNT@PFDCB) is rationally crafted via molecule and microstructure modulations
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Upcycling of Carbon Fiber/Thermoset Composites into High‐Performance Elastomers and Repurposed Carbon Fibers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Tiantian Yang, Xingyuan Lu, Xiaohan Wang, Xiang Wei, Ni An, Yixuan Li, Wenjie Wang, Xiang Li, Xu Fang, Junqi Sun
Recycling of carbon fiber‐reinforced polymer composites (CFRCs) based on thermosetting plastics is difficult. In the present study, high‐performance CFRCs are fabricated through complexation of aromatic pinacol‐cross‐linked polyurethane (PU‐AP) thermosets with carbon fiber (CF) cloths. PU‐AP thermosets exhibit a breaking strength of 95.5 MPa and toughness of 473.6 MJ m‐3 and contain abundant hydrogen‐bonding
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Manganese(I)‐Catalyzed Enantioselective C(sp2)‐C(sp3) Bond‐Forming for the Synthesis of Skipped Dienes with Synergistic Aminocatalysis Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Chuan-Gang Zhao, Junzhe Cai, Chaoyu Du, Qi Gao, Jie Han, Jin Xie
Mn(I)‐catalyzed enantioselective C‐C bond‐forming reactions represent a great challenge in homogeneous catalysis primarily due to a limited understanding of its mechanistic principles. Herein, we have developed an interesting catalytic strategy that leverages a synergistic combination of a dimeric manganese(I) catalyst and a chiral aminocatalyst to address this issue. A range of conjugated dienals
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Selective Peptide Cysteine Manipulation on Demand and Difficult Protein Chemical Synthesis Enabled by Controllable Acidolysis of N,S‐Benzylidene Thioacetals Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Hongxiang Wu, Zhenquan Sun, Xuechen Li
Although solid‐phase peptide synthesis combining with chemical ligation provides a way to build up customized polypeptides in general, many targets are still presenting challenges for the conventional synthetic process, such as hydrophobic proteins. New methods and strategies are still required to overcome these obstacles. In this study, kinetic studies of Cys/Pen ligation and its acidolysis were performed
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The Transfer Dehydrogenation Method Enables a Family of High Crystalline Benzimidazole‐linked Cu (II)‐phthalocyanine‐based Covalent Organic Frameworks Films Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Qingsong Zhang, Zhiheng Zhu, Liping Liu, Haojie Huang, Xianjie Chen, Yangshuang Bian, Mingchao Shao, Xiaofang Wei, Chengyu Wang, Dong Wang, Jichen Dong, Yunlong Guo, Yongfa Zhu, Yunqi Liu
Heterocycle‐linked phthalocyanine‐based COFs with close‐packed π‒π conjugated structures are a kind of material with intrinsic electrical conductivity, and they are considered to be candidates for photoelectrical devices. Previous studies have revealed their applications for energy storage, gas sensors, and field effect transistors. However, their potential application in photodetector is still not
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Collective Synthesis of Highly Oxygenated (Furano)germacranolides Derived from Elephantopus mollis and Elephantopus tomentosus Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Rémi Patouret, Ning Cham, Shunsuke Chiba
Germacranolides, secondary metabolites produced by plants, have garnered academic and industrial interest due to their diverse and complex topology as well as a wide array of pharmacological activities. Molephantin, a highly oxygenated germacranolide isolated from medicinal plants, Elephantopus mollis and Elephantopus tomentosus, has exhibited anti‐tumor, inflammatory, and leishmanicidal activities
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Interfacial Engineering for Oriented Crystal Growth toward Dendrite‐Free Zn Anode for Aqueous Zinc Metal Battery Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Xunzhu Zhou, Bo Wen, Yichao Cai, Xiaomin Chen, Lin Li, Qing Zhao, Shulei Chou, Fujun Li
Zn deposition with a surface‐preferred (002) crystal plane has attracted extensive attention due to its inhibited dendrite growth and side reactions. However, the nucleation and growth of the Zn(002) crystal plane are closely related to the interfacial properties. Herein, oriented growth of Zn(002) crystal plane is realized on Ag‐modified surface that is directly visualized by in situ atomic force
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Vinyl‐Groups‐Anchored Covalent Organic Framework for Promoted Photocatalytic Hydrogen Peroxide Generation Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Hong Yu, Fengtao Zhang, Qian Chen, Pan-Ke Zhou, Wandong Xing, Sibo Wang, Guigang Zhang, Yi Jiang, Xiong Chen
Artificial photosynthesis of H2O2 from water and oxygen using semiconductor photocatalysts has attracted growing attention because of its green, environmentally friendly, and energy‐saving characteristics. Although covalent organic frameworks (COFs) are promising materials for photocatalytic H2O2 production by virtue of their structural and functional diversities, they typically suffer from low charge
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Simultaneous Inside and Outside Functionalization of Single‐Walled Carbon Nanotubes Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Jan Kraus, Laura Meingast, Janina Hald, Sebastian B. Beil, Johannes Biskupek, Christian L. Ritterhoff, Sebastian Gsänger, Jasmin Eisenkolb, Bernd Meyer, Ute Kaiser, Janina Maultzsch, Max von Delius
Functionalizing single‐walled carbon nanotubes (SWCNTs) in a robust way that does not affect the sp2 carbon framework is a considerable research challenge. Here we describe how triiodide salts of positively charged macrocycles can be used not only to functionalize SWCNTs from the outside, but simultaneously from the inside. We employed disulfide exchange in aqueous solvent to maximize the solvophobic
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Water‐Soluble Fluorescent Polymer Dyes with Tunable Emission Spectra for Flow Cytometry Applications Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Daniel Berndt, Dorina Glaap, Travis Jennings, Christian Dose, Daniel B. Werz, Dirk Norbert Hendrik Reckert
The application of spectrally unique, bright, and water‐soluble fluorescent dyes is indispensable for the analysis of biological systems. Multiparameter flow cytometry is a powerful tool for characterization of mixed cell populations. To discriminate the different cell populations, they are typically stained by a set of fluorescent reagents, e.g., antibody‐fluorophore conjugates. The number of parameters
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Elastic relaxor ferroelectric by thiol‐ene click reaction Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Bowen Li, Linping Wang, Liang Gao, Tianhua Xu, Dongyang Zhang, Fangzhou Li, Jike Lyu, Ren Zhu, Xin Gao, Heng Zhang, Ben-Lin Hu, Run-Wei Li
As ferroelectrics hold significance and application prospects in wearable devices, the elastification of ferroelectrics becomes more and more important. Nevertheless, achieving elastic ferroelectrics requires stringent synthesis conditions, while the elastification of relaxor ferroelectric materials remains unexplored, presenting an untapped potential for utilization in energy storage and actuation
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Rocking‐Chair Aqueous Fluoride‐ion Batteries Enabled by Hydrogen Bonding Competition Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Huijian Wang, Chengjun Lei, Tingting Liu, Chen Xu, Xin He, Xiao Liang
Aqueous fluoride ion batteries (FIBs) have garnered attention for their high theoretical energy density, yet they are challenged by sluggish fluorination kinetics, active material dissolution, and electrolyte instability. Here, we present a room temperature rocking‐chair aqueous FIBs featuring KOAc‐KF binary salt electrolytes, enabling concurrent fluorination and defluorination reactions at both cathode
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Catalyst‐Free α‐Acetyl Cinnamate/Acetoacetate Exchange to Enable High Creep‐Resistant Vitrimers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Hongzhi Feng, Sheng Wang, Jason Y.C. Lim, Bofan Li, Wendy Rusli, Feng Liu, Nikos Hadjichristidis, Zibiao Li, Jin Zhu
Vitrimers represent an emerging class of polymeric materials that combine the desirable characteristics of both thermoplastics and thermosets achieved through the design of dynamic covalent bonds within the polymer networks. However, these materials are prone to creep due to the inherent instability of dynamic covalent bonds. Consequently, there are pressing demands for the development of robust and
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Co Single‐atom Reverse Hydrogen Spillover for Efficient Electrochemical Water Dissociation and Dechlorination Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Qian Zheng, Hengyue Xu, Yancai Yao, Jie Dai, Jiaxian Wang, Wei Hou, Long Zhao, Xingyue Zou, Guangming Zhan, Ruizhao Wang, Kaiyuan Wang, Lizhi Zhang
Efficient water dissociation to atomic hydrogen (H*) with restrained recombination of H* is crucial for improving the H* utilization for electrochemical dechlorination, but is currently limited by the lack of feasible electrodes. Here, we developed a monolithic single‐atom electrode with Co single atoms anchored on the inherent oxide layer of titanium foam (Co1‐TiOx/Ti), which can efficiently dissociate
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Enabling Closed‐Loop Circularity of “Non‐Polymerizable” α, β‐Conjugated Lactone towards High‐performance Polyester with the Assistance of Cyclopentadiene Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Xiao-Tong Wu, Chun Yang, Jian-Shu Xi, Changxia Shi, Fu-Sheng Du, Zi-Chen Li
Chemical recycling of polymers to monomers presents a promising solution to the escalating crisis associated with plastic waste. Despite considerable progress made in this field, the primary efforts have been focused on redesigning new monomers to produce readily recyclable polymers. In contrast, limited research into the potential of seemingly "non‐polymerizable" monomers has been conducted. Herein
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N‐Heteroaromatic Fluoroalkylation through Ligand Coupling Reaction of Sulfones Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Huamin Liang, Qian Wang, Xin Zhou, Rongyi Zhang, Min Zhou, Jun Wei, Chuanfa Ni, Jinbo Hu
Ligand coupling on hypervalent main group elements has emerged as a pivotal methodology for the synthesis of functionalized N‐heteroaromatic compounds in recent years due to the avoidance of transition metals and the mildness of the reaction conditions. In this direction, the reaction of N‐heteroaryl sulfur(IV) and N‐heteroaryl phosphorus(V) compounds has been well studied. However, the ligand coupling
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Contact‐Electro‐Catalysis for Direct Oxidation of Methane under Ambient Conditions Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Weixin Li, Jikai Sun, Mingda Wang, Jiajia Xu, Yanjie Wang, Li Yang, Ran Yan, Haoxian He, Shuai Wang, Wei-Qiao Deng, Zhong-Qun Tian, Feng Ru Fan
The conversion of methane under ambient conditions has attracted significant attention. Although advancements have been made using active oxygen species from photo‐ and electro‐ chemical processes, challenges such as complex catalyst design, costly oxidants, and unwanted byproducts remain. This study exploits the concept of contact‐electro‐catalysis, initiating chemical reactions through charge exchange
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Porous Ceramic Metal‐Based Flow Battery Composite Membrane Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Kang Huang, Feiyan Mu, Xiaoxuan Hou, Hongyan Cao, Xin Liu, Ting Chen, Yu Xia, Zhi Xu
In metal‐based flow battery, membranes significantly impact energy conversion efficiency and security. Unfortunately, damages to the membrane occur due to gradual accumulation of metal dendrites, causing short circuits and shortening cycle life. Herein, we developed a rigid hierarchical porous ceramic flow battery composite membrane with a sub‐10‐nm‐thick polyelectrolyte coating to achieve high ion
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Control of the Hydroquinone/Benzoquinone Redox State in High‐Mobility Semiconducting Conjugated Coordination Polymers Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Xing Huang, Yang Li, Shuai Fu, Chao Ma, Yang Lu, Mingchao Wang, Peng Zhang, Ze Li, Feng He, Chuanhui Huang, Zhongquan Liao, Ye Zou, Shengqiang Zhou, Manfred Helm, Petko St. Petkov, Hai I. Wang, Mischa Bonn, Jian Li, Wei Xu, Renhao Dong, Xinliang Feng
Conjugated coordination polymers (c‐CPs) are unique organic‐inorganic hybrid semiconductors with intrinsically high electrical conductivity and excellent charge carrier mobility. However, it remains a challenge in tailoring electronic structures, due to the lack of clear guidelines. Here, we develop a strategy wherein controlling the redox state of hydroquinone/benzoquinone (HQ/BQ) ligands allows for
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Carrier Protein Interaction with Competing Adenylation and Epimerization Domains in a Nonribosomal Peptide Synthetase Analyzed by FRET Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Anna-Lena Feldberg, Florian Mayerthaler, Jennifer Rüschenbaum, Jonas Kröger, Henning D. Mootz
In multi‐domain nonribosomal peptide synthetases (NRPSs) the order of domains and their catalytic specificities dictate the structure of the peptide product. Peptidyl‐carrier proteins (PCPs) bind activated amino acids and channel elongating peptidyl intermediates along the protein template. To this end, fine‐tuned interactions with the catalytic domains and large‐scale PCP translocations are necessary
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Abiotic Methane Production Driven by Ubiquitous Non‐Fenton‐Type Reactive Oxygen Species Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Jie Ye, Andong Hu, Chao Gao, Fengqi Li, Lei Li, Yulin Guo, Guoping Ren, Bing Li, Christopher Rensing, Kenneth H. Nealson, Shungui Zhou, Yujie Xiong
Abiotic CH4 production driven by Fenton‐type reactive oxygen species (ROS) has been confirmed to be an indispensable component of the atmospheric CH4 budget. While the chemical reactions independent of Fenton chemistry to ROS are ubiquitous in nature, it remains unknown whether the produced ROS can drive abiotic CH4 production. Here, we first demonstrated the abiotic CH4 production at the soil‒water
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Copper Nanodrugs by Atom Transfer Radical Polymerization Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Peng Chen, Ziyan Song, Xuxia Yao, Weibin Wang, Lisong Teng, Krzysztof Matyjaszewski, Weipu Zhu
In this study, some copper catalysts used for atom transfer radical polymerization (ATRP) were explored as efficient anti‐tumor agents. The aqueous solution of copper‐containing nanoparticles with uniform spheric morphology was in situ prepared through a copper‐catalyzed activator generated by electron transfer (AGET) ATRP in water. Nanoparticles were then directly injected into tumor‐bearing mice
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Cyanide‐based Covalent Organic Frameworks for Enhanced Overall Photocatalytic Hydrogen Peroxide Production Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-16 Enbo Zhou, Futong Wang, Yangdan Hui, Yaobing Wang
Photocatalytic oxygen reduction to produce hydrogen peroxide (H2O2) is a promising route to providing oxidants for various industrial applications. However, the lack of well‐designed photocatalysts for efficient overall H2O2 production in pure water has impeded ongoing research and practical thrusts. Here we present a cyanide‐based covalent organic framework (TBTN‐COFs) combining 2,4,6‐trimethylbenzene‐1
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Complementary Weaknesses: A Win‐Win Approach for rGO/CdS to Improve the Energy Conversion Performance of Integrated Photorechargeable Li‐S Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-15 Tianzhen Yang, Haoning Mao, Qianqian Zhang, Chao Xu, Qiongzhi Gao, Xin Cai, Shengsen Zhang, Yueping Fang, Xiaosong Zhou, Feng Peng, Siyuan Yang
Integrating solar energy into rechargeable battery systems represents a significant advancement towards sustainable energy storage solutions. Herein, we propose a win‐win solution to reduce the shuttle effect of polysulfide and improve the photocorrosion stability of CdS, thereby enhancing the energy conversion efficiency of rGO/CdS‐based photorechargeable integrated lithium‐sulfur batteries (PRLSBs)
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Selective Stereoretention of Carbohydrates upon C‐C Cleavage Enabling D‐Glyceric Acid Production with High Optical Purity over Ag/γ‐Al2O3 catalyst Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-15 Ruofeng Yang, Shuguang Xu, Xiaoyan Wang, Yuan Xiao, Jianmei Li, Changwei Hu
Chiral carboxylic acid production from renewable biomass by chemocatalysis is vitally important for reducing our carbon footprint, but remains underdeveloped. We herein establish a strategy that make use of a stereogenic center of biomass to achieve a rare example of D‐glyceric acid production with the highest yield (86.8%) reported to date as well as an excellent ee value (>99%). Unlike traditional
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Synthesis and Reactivity of the [NCCCO]– Cyanoketenate Anion Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-14 Tongtong Wang, Zhuangzhuang Guo, Laura E English, Douglas W Stephan, Andrew R. Jupp, Maotong Xu
Cyanoketene is a fundamental molecule that is actively being searched for in the interstellar medium. Its deprotonated form (cyanoketenate) is a heterocumulene that is isoelectronic to carbon suboxide whose structure has been the subject of debate. However, the investigation of cyanoketene and its derivatives is hampered by the lack of practical synthetic routes to these compounds. We report the first
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An Ultralow‐concentration and Moisture‐resistant Electrolyte of Lithium Difluoro(oxalato)borate in Carbonate Solvents for Stable Cycling in Practical Lithium‐ion Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-14 Zhishan Liu, Wentao Hou, Haoran Tian, Qian Qiu, Irfan Ullah, Shen Qiu, Wei Sun, Qian Yu, Jinliang Yuan, Lan Xia, Xianyong Wu
The electrolyte concentration not only impacts the battery performance but also affects the battery cost and manufacturing. Currently, most studies focus on high‐concentration (>3 M) or localized high‐concentration electrolytes (~1 M); however, the expensive lithium salt imposes a major concern. Most recently, ultralow concentration electrolytes (<0.3 M) have emerged as intriguing alternatives for
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A 3D Hierarchical Host with Gradient‐Distributed Dielectric Properties toward Dendrite‐free Lithium Metal Anode Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-14 Yueying Zhang, Meng Yao, Tuan Wang, Hao Wu, Yun Zhang
The conventional conductive three‐dimensional (3D) host fails to effectively stabilize lithium metal anodes (LMAs) due to the internal incongruity arising from nonuniform lithium‐ion gradient and uniform electric fields. This results in undesirable Li "top‐growth" behavior and dendritic Li growth, significantly impeding the practical application of LMAs. Herein, we construct a 3D hierarchical host
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Discovery of Terminal Oxazole‐Bearing Natural Products by a Targeted Metabologenomic Approach Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-14 Jiyoon Park, Yern-Hyerk Shin, Sunghoon Hwang, Jungwoo Kim, Dong Hyun Moon, Ilnam Kang, Yoon-Joo Ko, Beomkoo Chung, Hyungsung Nam, Seokhee Kim, Kyuho Moon, Ki-Bong Oh, Jang-Cheon Cho, Sang Kook Lee, Dong-Chan Oh
A targeted metabologenomic method was developed to selectively discover terminal oxazole‐bearing natural products from bacteria. For this, genes encoding oxazole cyclase, a key enzyme in terminal oxazole biosynthesis, were chosen as the genomic signature to screen bacterial strains that may produce oxazole‐bearing compounds. Sixteen strains were identified from the screening of a bacterial DNA library
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Catalytic Ring Expanding Difluorination: An Enantioselective Platform to Access β,β‐Difluorinated Carbocycles Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-14 Louise Ruyet, Christoph Roblick, Joel Häfliger, Zi-Xuan Wang, Tobias Jürgen Stoffels, Constantin Daniliuc, Ryan Gilmour
Cyclic β,β‐difluoro‐carbonyl compounds have a venerable history as drug discovery leads, but limitations in the synthesis arsenal continue to impede chemical space exploration. This challenge is particularly acute in the arena of fluorinated medium rings where installing the difluoromethylene unit subtly alters the ring conformation by expanding the internal angle (∠C‐CF2‐C > ∠C‐CH2‐C): this provides
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6‐Strand to Stable 10/12 Helix Conformational Switch by Incorporating Flexible β‐hGly in the Homooligomers of Camphor Derived β‐Amino Acid: NMR and X‐ray Crystallographic Evidence Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-14 Genji Sukumar, Rahul Suryavanshi, Kiranmai Nayani, Prathama S. Mainkar, Jupally Prashanth, Balasubramanian Sridhar, Akella V. S. Sarma, Jagadeesh Bharatam, Srivari Chandrasekhar
Rational design of unnatural amino acid building blocks capable of stabilizing predictable secondary structures similar to protein fragments is pivotal for foldamer chemistry/catalysis. Here, we introduce novel β‐amino acid building blocks: [1S,2R,4R]exoCDA and [1S,2S,4R]endoCDA, derived from the abundantly available R(+)‐camphor, which is traditionally known for its medicinal value. Further, we demonstrate
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Li3PO4‐Enriched SEI on Graphite Anode Boosts Li+ De‐Solvation Enabling Fast‐Charging and Low‐Temperature Lithium‐Ion Batteries Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-14 Chaonan Wang, Yuansen Xie, Yingshan Huang, Shaoyun Zhou, Huanyu Xie, Hongchang Jin, Hengxing Ji
Li+ de‐solvation at solid‐electrolyte interphase (SEI)‐electrolyte interface stands as a pivotal step that imposes limitations on the fast‐charging capability and low‐temperature performance of lithium‐ion batteries (LIBs). Unraveling the contributions of key constituents in the SEI that facilitate Li+ de‐solvation and deciphering their mechanisms, as a design principle for the interphasial structure
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Programming of Supercrystals Using Replicable DNA‐Functionalized Colloids Angew. Chem. Int. Ed. (IF 16.6) Pub Date : 2024-03-14 Xiaoyun Sun, Wenqiang Hua, Xiaoyu Liu, Jing Jin, Jianing Zhang, Jie Tian, Bin Zheng, Wei Jiang, Dongbao Yao, Haojun Liang
The development of self‐replicating systems is of great importance in research on the origin of life. As the most iconic molecules, nucleic acids have provided prominent examples of the fabrication of self‐replicating artificial nanostructures. However, it is still challenging to construct sophisticated synthetic systems that can create large‐scale or three‐dimensionally ordered nanomaterials using