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Switching CO2 Electroreduction Pathways between Ethylene and Ethanol via Tuning Microenvironment of the Coating on Copper Nanofibers Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Buxing Han, Xing Tong, Pei Zhang, Peng Chen, Zhuosen He, Xinchen Kang, Yaoyu Yin, Yingying Cheng, Meng Zhou, Lihong Jing, Ce Wang, Baocai Xu, Lirong Zheng, Xueqing Xing, Zhonghua Wu
Engineering the microenvironment of electrode surface is one of the effective means to tune the reaction pathways in CO2RR. In this work, we prepared copper nanofibers with conductive polypyrrole coating by polymerization of pyrrole using polyvinyl pyrrolidone (PVP) as template. As a result, the obtained copper nanofibers Cu/Cu2+1O/SHNC, exhibited a superhydrophobic surface, which demonstrated very
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How Can Materials Chemists Contribute to Food Supply Security in the Age of AI and Robotics? Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Ludovico Cademartiri
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Rational Design of Crystalline and Enantiomerically Pure Helicenes with Open-Shell Singlet Ground States Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Xinping Wang, Tao Wang, Shuxuan Tang, Xue Dong, Yu Zhao, Quanchun Sun, Shanshan Kong, Yue Zhao
Helicene diradical derivatives have attracted widespread attentions because of their unique magnetic and chiroptoelectronic properties, however, crystalline and enantiomerically pure forms of helicene diradicals are extremely rare. Herein, we describe the rational design and synthesis of o-quinone functionalized helicene diradicals with crystalline enantiomerical purity. Diradical dianion salt Rac-3K
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Honeycomb-Structured IrOx Foam Platelets as the Building Block of Anode Catalyst Layer in PEM Water Electrolyzer Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Zhoubing Xie, Hui Chen, Xiyang Wang, Yimin A. Wu, Zizhun Wang, Subhajit Jana, Yongcun Zou, Xiao Liang, Xiao Zhao, Xiaoxin Zou
Achieving robust long-term durability with high catalytic activity at low iridium loading remains one of great challenges for proton exchange membrane water electrolyzer (PEMWE). Herein, we report the low-temperature synthesis of iridium oxide foam platelets comprising edge-sharing IrO6 octahedral honeycomb framework, and demonstrate the structural advantages of this material for multilevel tuning
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A CaI2-Based Electrolyte Enabled by Borate Ester Anion Receptors for Reversible Ca-Organic and Ca-Se Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Zhen Hou, Rui Zhou, Kai Liu, Junwu Zhu, Biao Zhang
Passivating solid electrolyte interphases (SEIs) in Ca metal anodes constitute a long-standing challenge, as they block Ca2+ transport and inhibit reversible Ca deposition/stripping. Current solutions focus primarily on boron/aluminum-based electrolytes to mitigate such interfacial issues by producing Ca2+-conductive species, yet the complex synthetic procedure of these salts restricts the widespread
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Directional Ring Translocation in a pH- and Redox-Driven Tristable [2]Rotaxane Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Leonardo Andreoni, Jessica Groppi, Özlem Seven, Massimo Baroncini, Alberto Credi, Serena Silvi
We describe the synthesis and characterization of a [2]rotaxane comprising a dibenzo-24-crown-8 (DB24C8) macrocyclic component and a thread containing three recognition sites: ammonium (AmH+), bipyridinium (Bpy2+) and triazolium (Trz+). AmH+ and Bpy2+ are responsive to fully orthogonal stimuli, pH and electrochemical, which allows to precisely control the directional translation of the macrocycle along
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Dynamic Organic Phosphorescence Glass by Rigid-Soft Coupling Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Meng Zhang, Xiaohui Lan, Meijuan Ding, Chaoyi Han, Xing Wang Liu, Zhengong Meng, Zhen-Qiang Yu, Zhongfu An
Organic phosphorescence glass has garnered considerable attention owing to the excellent shaping ability and photophysical behavior, but facile construction from single-component phosphors is still challenging. Herein, a rigid-soft coupling design is adopted in organic phosphors of ICO, CCO and PCO, thus preparing phosphorescence glasses through melting-quenching method to give excellent shaping ability
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Partitioning / self-assembly of artificial water channels - toward controlled permselectivity through bilayer membrane Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Dan-Dan Su, Arie van der Lee, Mihail Barboiu
Artificial water channels (AWCs) have been extensively explored to mimic natural proteins, which enables to effectively transport water while blocking ions. As one of the first AWCs, self-assembled I-quartets (HCx) have showcased high water-permselectivity that can be enhanced by improving their distribution and stability within membrane. The use of long alkyl chains (n>8) is constrained by their low
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A Low-Acidity Chloride Electrolyte Enables Exceptional Reversibility and Stability in Aqueous Tin Metal Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Songyang Chang, Wentao Hou, Angelica Del Valle-Perez, Irfan Ullah, Shen Qiu, Jeileen Luciano Rodriguez, Liz M. Díaz-Vázquez, Lisandro Cunci, Gerardo Morell, Xianyong Wu
Tin (Sn) metal has emerged as a promising anode for aqueous batteries, due to its high capacity, non-toxicity, and cost-effectiveness. However, Sn metal has often been coupled with strong and corrosive sulfuric acids (2-3 M), leading to severe electrode corrosion and hydrogen evolution issues. Although high efficiency and long cycling were reported, the results were achieved using high currents to
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Coupling Photocatalytic Hydrogen Production with Key Oxidation Reactions Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Jiayan Teng, Wenlu Li, Zhen Wei, Derek Hao, Lin Jing, Yuxi Liu, Hongxing Dai, Yongfa Zhu, Tianyi Ma, Jiguang Deng
Hydrogen represents a clean and sustainable energy source with wide applications in fuel cells and hydrogen energy storage systems. Photocatalytic strategies emerge as a green and promising solution for hydrogen production, which still reveals several critical challenges in enhancing the efficiency and stability and improving the whole value. This review systematically elaborates on various coupling
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Boron Ylide Enables Stereoselective Construction of gem-Diborylcyclopropanes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Tongchang Fang, Peng Zhang, Chao Liu
The stereoselective cyclopropanation of olefins with boron ylide is disclosed for the first time, providing a modular strategy for the synthesis of stereospecific diboryl-functionalized cyclopropanes. The chiral gem-diborylcyclopropanes are synthesized with excellent enantioselectivity with the aid of a chiral auxiliary. Based on the powerful transformable ability of boryl group, those challenging
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Ternary Eutectic Electrolyte for Flexible Wide-Temperature Zinc-Ion Batteries from -20 °C to 70 °C Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Qinbo Liu, Junfu Li, Doudou Xing, Yingjie Zhou, Feng Yan
Aqueous Zn-ion batteries (ZIBs) have attracted attention for grid applications due to their cost-effectiveness and high security. However, their lifespan decreases at high temperatures due to declining interfacial stability and increased side reactions. To address these challenges, a ternary deep eutectic solvent-based flexible electrolyte, comprised of ZnClO4·6H2O, butanedinitrile (BD), and LiCl in
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Ultrabroad Near Infrared Emitting Perovskites Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Sajid Saikia, Animesh Gopal, Radha Rathod, Aprajita Joshi, K. R. Priolkar, Surajit Saha, Pralay K. Santra, Kadhiravan Shanmuganathan, Angshuman Nag
Phosphor converted light emitting diodes (pc-LEDs) have revolutionized solid-state white lighting by replacing energy-inefficient filament-based incandescent lamps. However, such a pc-LED emitting ultrabroad near-infrared (NIR) radiations still remains a challenge, primarily because of the lack of ultrabroad NIR emitting phosphors. To address this issue, we have prepared 2.5% W4+-doped and 2.8% Mo4+-doped
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Exploiting Deep-Ultraviolet Nonlinear Optical Material Rb2ScB3O6F2 Originated from Congruously Oriented [B3O6] Groups Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Qianzhen Zhang, Ran An, Xifa Long, Zhihua Yang, Shilie Pan, Yun Yang
The exploration and research for deep-ultraviolet (UV) nonlinear optical (NLO) crystals are of great significance for all-solid-state lasers. This work is based on the excellent structural [B3O6] units which manipulate the excellent performances of famous commercial NLO crystal β-BaB2O4 (β-BBO) to explore new alternatives of deep-UV NLO materials. A deep-UV rare-earth metal borate fluoride Rb2ScB3O6F2
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Rare Earth Er-Nd Dual Single-Atomic Catalysts for Efficient Visible-light Induced CO2 Reduction to CnH2n+1OH (n=1, 2) Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-20 Pengyan Li, Zhenhong Qi, Dongpeng Yan
Efficient synthesis of CnH2n+1OH (n=1, 2) via photochemical CO2 reduction holds promise for achieving carbon neutrality but remains challenging. Here, we present rare-earth dual single atoms (SAs) catalysts containing ErN6 and NdN6 moieties, fabricated via an atom-confinement and coordination method. The dual Er-Nd SAs catalysts exhibit unprecedented generation rates of 1761.4 μmol g–1 h–1 and 987
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Ultra-Wide Modulation and Reversible Reconfiguration of a Flexible Organic Crystalline Optical Waveguide Between 645 and 731 nm Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Quanliang Chen, Baolei Tang, Kaiqi Ye, Hanlin Hu, Hongyu Zhang
Flexible organic crystalline optical waveguides, i.e., delivering input or self-emit lights through various dynamic organic crystals, have attracted increasing attentions in the past decade. However, the modulation of waveguide outputs relies on chemical design and substituent modification, being time-consuming and laborious. Here we report an elastic organic crystal that displays long-distance light
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Molecular Design of Mono-Fluorinated Ether-Based Electrolyte for All-Climate Lithium-ion Batteries and Lithium-Metal Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Yejuan Xue, Yueda Wang, Heng Zhang, Weilong Kong, Yuxin Zhou, Bo Kang, Zhimei Huang, Hongfa Xiang
Fluorinated-ethers are promising electrolyte solvents in lithium metal batteries, for their high antioxidant and excellent reductive stability on Li anode. However, fluorinated-ethers with high fluorination degree suffer from low ionic conductivity and narrow temperature adaptibility. Herein, we synthesize a mono-fluorinated linear ether of bis(2-fluoroethoxy) methane (BFME) with enhanced solvated
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Constructing Donor-Acceptor Covalent Organic Frameworks for Highly Efficient H2O2 Photosynthesis Coupled with Oxidative Organic Transformations Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Jian-Chuan Liu, Chao Tuo, Wei-Yun Xiao, Ming-Yu Qi, Yusran Yusran, Zi-Tao Wang, Hui Li, Chun-Sheng Guo, Jia-Long Song, Shi-Lun Qiu, Yi-Jun Xu, Qianrong Fang
The development of photocatalytic systems that enable the simultaneous production of H2O2 and value-added organic chemicals presents a dual advantage: generating valuable products while maximizing the utilization of solar energy. Despite the potential, there are relatively few reports on photocatalysts capable of such dual functions. In this study, we synthesized a series of donor-acceptor covalent
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Indole-N-Linked Hydroperoxyl Adduct of Protein-Derived Cofactor Modulating Catalase-Peroxidase Functions Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Jiasong Li, Ran Duan, Ephrahime S. Traore, Romie C. Nguyen, Ian Davis, Wendell P. Griffth, Douglas C. Goodwin, Andrzej A. Jarzecki, Aimin Liu
Bifunctional catalase-peroxidase (KatG) features a posttranslational methionine-tyrosine-tryptophan (MYW) crosslinked cofactor crucial for its catalase function, enabling pathogens to neutralize hydrogen peroxide during infection. We discovered the presence of indole nitrogen-linked hydroperoxyl adduct (MYW-OOH) in Mycobacterium tuberculosis KatG in the solution state under ambient conditions, suggesting
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Disorder Over Pore Size: Boosting Supercapacitor Efficiency Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Hao Zhang, Yu Zhang, Zhenhai Wen
The urgent need for efficient energy storage systems has spotlighted supercapacitors and nanostructured porous carbon materials, which require structural optimization to enhance their performance and lifespan, necessitating advanced design and synthesis techniques. Recent research by Forse et al. published in Science reveals that structural disorder in nanoporous carbon materials significantly enhances
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A Customized Strategy Realizes Stable Cycle of Large-Capacity and High-Voltage Layered Cathode for Sodium-Ion Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Bo Peng, Zihao Zhou, Ji Shi, Sheng Xu, Jie Yang, Chengrong Xu, Daxian Zuo, Jie Xu, Lianbo Ma, Shaohua Guo, Haoshen Zhou
High-voltage P2-Na0.67Ni0.33Mn0.67O2 layered oxide cathode exhibits significant potential for sodium-ion batteries, owing to the elevated operating voltage and theoretical energy density beyond lithium iron phosphate, but the large-volume phase transition is the devil. Currently, this type cathode still suffers from stability–capacity trade-off dilemma. Herein, a concept of customized strategy via
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Polyoxometalate-Based Single-Atom Catalyst with Precise Structure and Extremely Exposed Active Site for Efficient H2 Evolution Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Zhuo-Ran Zhang, He-Yu Sui, Wen-Xiong Shi, Jing Ren, Shuang Yao, Tong-Bu Lu, Zhi-Ming Zhang
Single-atom catalysts with precise structure and extremely high catalytic efficiency remain a fervent focus in the fields of materials chemistry and catalytic science. Herein, a nickel-substituted polyoxometalate (POM) {NiSb6O4(H2O)3[β-Ni(hmta)SbW8O31]3}15- (NiPOM) with one extremely exposed nickel site [NiO3(H2O)3] was synthesized using the conventional aqueous method. The uniform dispersion of single
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Platinum-Group Metal High-Entropy Selenides for the Hydrogen Evolution Reaction Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Xiaohui Deng, Kohei Kusada, Tomokazu Yamamoto, Takaaki Toriyama, Yasukazu Murakami, Jo-Chi Tseng, Hiroki Yamada, Osami Sakata, Hirotaka Ashitani, Shogo Kawaguchi, Yoshiki Kubota, Hiroshi Kitagawa
The selenides of platinum-group metals (PGMs) are emerging as promising catalysts for diverse electrochemical reactions. To date, most studies have focused on single metal or bimetallic systems, whereas the preparation of a high-entropy (HE) selenide consisting of five or more PGM elements holds the promise to further enhance catalytic performance by introducing abundant active sites with various local
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Single Exposed Zn (0002) Plane and Sustainable Zn-Oriented Growth Achieving Highly Reversible Zinc Metal Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Da Zhang, Ziyang Song, Ling Miao, Yaokang Lv, Hui Duan, Mingfang Li, Lihua Gan, Mingxian Liu
To prevent dendrite growth and hydrogen evolution reaction, directional epitaxial growth of Zn2+ ions on Zn anode, especially along the lowest-surface-energy Zn (0002) plane, is pursued for highly reversible zinc metal batteries (ZMBs). However, designing single Zn (0002) exposed anodes for sustained uniaxial crystalline orientation of Zn electroplating faces challenges. Herein, we propose an anode
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Structure-Agnostic Bioactivity-Driven Combinatorial Biosynthesis Reveals New Antidiabetic and Anticancer Triterpenoids Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Yong Zhao, Yao-Tao Duan, Jie Zang, Morten H. Raadam, Irini Pateraki, Karel Miettinen, Dan Staerk, Sotirios C. Kampranis
Although combinatorial biosynthesis can dramatically expand the chemical structures of bioactive natural products to identify molecules with improved characteristics, progress in this direction has been hampered by the difficulty in isolating and characterizing the numerous produced compounds. This challenge could be overcome with improved designs that enable the analysis of the bioactivity of the
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Achieving Sub-ppm Sensitivity in SO2 Detection with a Chemically Stable Covalent Organic Framework Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Wei Zhao, Juan L. Obeso, Valeria B. López-Cervantes, Mounib Bahri, Elí Sánchez-González, Yoarhy A. Amador-Sánchez, Junyu Ren, Nigel D. Browning, Ricardo A. Peralta, Giovanni Barcaro, Susanna Monti, Diego Solis-Ibarra, Ilich A. Ibarra, Dan Zhao
We report the inaugural experimental investigation of covalent organic frameworks (COFs) to address the formidable challenge of SO2 detection. Specifically, an imine-functionalized COF (SonoCOF-9) demonstrated a modest and reversible SO2 sorption of 3.5 mmol g-1 at 1 bar and 298 K. At 0.1 bar (and 298 K), the total SO2 uptake reached 0.91 mmol g-1 with excellent reversibility for at least 50 adsorption-desorption
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Nonconventional Fluorescent Non-Isocyanate Polyurethane Foams for Multipurpose Sensing Applications Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Manas Mahapatra, Maxime Bourguignon, Bruno Grignard, Marylène Vandevenne, Moreno Galleni, Christophe Detrembleur
Fluorescent foams with interconnected pores are attractive for the detection and quantification of various products. However, many fluorescent probes are suffering from aggregation-caused fluorescence quenching in their solid/aggregated state, are costly, and/or not straightforward to incorporate in foams, limiting their utility for this application. Herein, non-isocyanate polyurethane foams, prepared
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Reactivity Inside Molecular Flasks: Acceleration Modes and Types of Selectivity Obtainable Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Leonidas-Dimitrios Syntrivanis, Konrad Tiefenbacher
There is increasing interest in the discovery and application of molecular flasks - supramolecular host structures capable of catalyzing organic reactions. Reminiscent of enzymes due to possessing a host cavity akin to an active site, molecular flasks can exhibit complex catalytic mechanisms and in many cases provide selectivity not achievable in bulk solvent. In this Review, we aim to organize the
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Magnetic Excitations in Ferromagnetically Coupled Spin-1 Nanographenes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Elia Turco, Fupeng Wu, Gonçalo Catarina, Nils Krane, Ji Ma, Roman Fasel, Xinliang Feng, Pascal Ruffieux
In the pursuit of high-spin building blocks for the formation of covalently bonded 1D or 2D materials with controlled magnetic interactions, $\pi$-electron magnetism offers an ideal framework to engineer ferromagnetic interactions between nanographenes. As a first step in this direction, we explore the spin properties of ferromagnetically coupled triangulenes -- triangular nanographenes with spin $S
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Multi-Stage Optimization of Pore Size and Shape in Pore-Space-Partitioned Metal-Organic Frameworks for Highly Selective and Sensitive Benzene Capture Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Yichong Chen, Wei Wang, Samuel Alston, Yuchen Xiao, Pooja Ajayan, Xianhui Bu, Pingyun Feng
Compared to exploratory development of new structure types, pushing the limits of isoreticular synthesis on a high-performance MOF platform may have higher probability of achieving targeted properties. Multi-modular MOF platforms could offer even more opportunities by expanding the scope of isoreticular chemistry. However, navigating isoreticular chemistry towards best properties on a multi-modular
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Multiple Resonance Quasi-fluorescence from BN-Doped Aromatic Compounds Modified with "Naphthalene" Units Approaches the BT.2020 Green Light Standard Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Tingting Feng, Xuewei Nie, Denghui Liu, Lin Wu, Xilin Mu, ziru xin, Bohong Liu, Hengxuan Qi, Jiasen Zhang, Wei Li, Shi-Jian Su, Ziyi Ge
Creating fluorophores that meet the Broadcast Service Television 2020 (BT.2020) standard is a significant achievement. In this paper, we present an innovative strategy that could revolutionize the development of high-performance narrowband fluorophores for ultra-high-definition displays. Our approach combines classic multi-resonance BN-doped fragments with naphthalene, creating two novel narrowband
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High-Temperature Solid-State Post-synthetic Modification of Highly Luminescent Cu(I) Metallacycles toward New Luminescent Thermic Tracers Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Christophe Lescop, Adrien Schlachter, Chendong Xu, Jana Schiller, Raquel Utrera Molero, Sébastien Kerneis, Guillaume Calvez, Karine Costuas, Manfred Scheer
A new luminescent Cu(I) tetrametallic metallacycle B is reported, featuring very rare semi-bridging aqua ligands. As heated markedly above room temperature, this compound undergoes in the solid-state a post-synthetic transformation, affording the new luminescent metallacycle C. Thermogravimetric analysis, IR spectroscopy and single crystals X-ray diffraction reveal that this alteration preserves the
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Anticancer Tetranuclear Cu(I) Complex Catalyzes a Click Reaction to Synthesize a Chemotherapeutic Agent in situ to Achieve Targeted Dual-Agent Combination Therapy for Cancer Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Xueyu Man, Wenjuan Li, Minghui Zhu, Shanhe Li, Gang Xu, Zhenlei Zhang, Feng Yang, Hong Liang
To develop next-generation metal-based drugs and dual-drug combination therapy for cancer, we proposed to develop a copper (Cu) complex that exerts anticancer function by integrating chemotherapy, immunotherapy and catalyzes a click reaction for the in situ synthesis of a chemotherapeutic agent, thereby achieving targeted dual-agent combination therapy. We designed and synthesized a tetranuclear Cu(I)
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Direct C3-H Alkylation and Alkenylation of Quinolines with Enones Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Liqing Xu, Xu Wang, Dezhi Yang, Xiaolong Yang, Dong Wang
Conversion of quinoline C-H bonds to C-C bonds is essential for obtaining the enormous array of derivatives required for pharmaceutical and agrochemical development. Despite over a century of synthetic efforts, the direct alkylation and alkenylation at C3-H positions in a wide array of quinoline precursors remain predominantly challenging and elusive. This report outlines the first successful quinoline
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Directly Regenerating of Spent LiCoO2 with Gradient F-doped Subsurface towards Ultra-stable Storage Properties Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Hai Lei, Xinwei Cui, Zihao Zeng, Chao Zhu, Wei Sun, Yue Yang, Peng Ge
As great potential recycling strategy, the direct regeneration of spent LiCoO2 (LCO) is beneficial for lowering environmental pollutions and promoting global sustainability. However, owing to the using of binder and electrolyte, some fluorine impurities would be remained into spent materials. Considering the doping behaviors of F-elements, their suitable content introducing would facilitate the energy-storage
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All-Atom Protein Sequence Design Based on Geometric Deep Learning Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Jiale Liu, Zheng Guo, Hantian You, Changsheng Zhang, Luhua Lai
Designing sequences for specific protein backbones is a key step in creating new functional proteins. Here, we introduce GeoSeqBuilder, a deep learning framework that integrates protein sequence generation with side chain conformation prediction to produce the complete all-atom structures for designed sequences. GeoSeqBuilder uses spatial geometric features from protein backbones and explicitly includes three-body
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Sulfonated Hydroxyaryl-Tetrazines with Increased pKa for Accelerated Bioorthogonal Click-to-Release Reactions in Cells Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-19 Michal Rahm, Patrick Keppel, Rastislav Dzijak, Martin Dračínský, Veronika Šlachtová, Simona Bellová, Paul E. Reyes-Gutiérrez, Sille Štěpánová, Jakob E. Raffler, Eva Tloušťová, Helena Mertlíková-Kaiserová, Hannes Mikula, Milan Vrabel
Bioorthogonal reactions that enable switching molecular functions by breaking chemical bonds have gained prominence, with the tetrazine-mediated cleavage of trans-cyclooctene caged compounds (click-to-release) being particularly noteworthy for its high versatility, biocompatibility, and fast reaction rates. Despite several recent advances, the development of highly reactive tetrazines enabling quantitative
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Stereoregular Poly(Phenyl Glycidyl Ethers): In Situ Formation of a Polyether Stereocomplex from a Racemic Monomer Mixture Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Geoffrey William Coates, Sandra Schüttner, Yiye Lu, Holger Frey
Polymer stereocomplex formation represents a promising research area as it can improve thermal and mechanical properties of co-crystallized polymer strands of opposite chirality. Polymers that form stereocomplexes commonly feature high stereoregularity and usually require sourcing from enantiopure monomer building blocks. Herein, we report the in situ polyether stereocomplex formation from racemic
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Static Organic p-n Junctions in Photoelectrodes for Solar Ammonia Production with 86% Internal Quantum Efficiency Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Yanjie Fang, Mengjie Li, Yifan Gao, Yingke Wen, Bing Shan
For photoelectrocatalytic cells, a limitation exists in finding appropriate photoelectrode configurations that couple efficient extraction of high-energy electrons from absorbed photons and selective catalysis. Here we report an organic p-n junction approach to fabricate molecular photoelectrodes for conversion of solar energy and nitrate into valuable ammonia product. Solar irradiation of the photoelectrode
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Highly Active Photoreduction of Atmospheric-Concentration CO2 into CH3COOH over Palladium Particles on Nb2O5 Nanosheets Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Jinyu Ding, Peijin Du, Peipei Li, Wenxiu Liu, Jiaqi Xu, Wensheng Yan, Yang Pan, Jun Hu, Junfa Zhu, Qingxia Chen, Xingchen Jiao, Yie Xie
The endeavor to drive CO2 photoreduction towards the synthesis of C2 products is largely thwarted by the colossal energy hurdle inherent in C−C coupling. Herein, we load active metal particles on metal oxide nanosheets to build the dual metal pair sites for steering C−C coupling to form C2 products. Taking Pd particles anchored on the Nb2O5 nanosheets as an example, the high-angle annular dark-field
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Anchoring Catalytic Metal Nodes within a Single-Crystalline Pyrazolate Metal-Organic Framework for Efficient Heterogeneous Catalysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Rong-Ran Liang, Zhaoyi Liu, Zongsu Han, Yihao Yang, Joshua Rushlow, Hong-Cai Zhou
The synthesis of single-crystalline and robust pyrazolate metal-organic frameworks (Pz-MOFs) capable of facilitating challenging organic transformations is fundamentally significant in catalysis. Here we demonstrate a metal-node-based catalytic site anchoring strategy by synthesizing a single-crystalline and robust Pz-MOF (PCN-1004). PCN-1004 features one-dimensional (1D) copper-Pz chains interconnected
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Entropy-Modulated Short-Chain Cathode for Low-Temperature All-Solid-State Li-S Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Wei Zhao, Yan Zhang, Qingsong Liu, Yajie Song, Xu Li, Liping Ren, Geping Yin, Shuaifeng Lou, Jiajun Wang
All-solid-state Li-S batteries (ASSLSBs) due to high theoretical energy density and exceptional safety are highly desirable for electric aircraft. However, as the flight altitude rises, the low-temperature performance is hampered by inadequate practical capacity. Here, we discover that low-temperature sulfur utilization is constrained by the multi-step endothermic conversion reaction. By introducing
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Interface Energy-Level Reorganization for Efficient Perovskite γ-Ray Detectors Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Mingjian Yuan, Yanxing Feng, Quanlin Chen, Xinlong Yan, Xinliang Fu, Di Wang, Zijin Ding, Saisai Li, Cong Geng, Linyue Gao, Jia Zhang, Fan Yang, Saif M. H. Qaid, Shuyan Gao, Yuanzhi Jiang
Metal halide perovskites are promising candidates for γ-ray spectrum detectors. However, achieving high-resolution energy spectra in single-photon pulse-height analysis mode remains challenging, due to the inevitable leakage currents degrade the recognizable fingerprint energies which is critical for resolving γ-ray spectroscopy. We demonstrate under high bias voltage, a deficient contact barrier can
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Selectivity Modulation of Multistep Reduction Reactions by Gold Nanoclusters Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Jing-Zheng Zhang, Yi-Bao Zhang, Hui-Li Chai, Hui-Ling Luo, Chen-Xia Du, Ren-Wu Huang, Shuang-Quan Zang
The selective synthesis of valuable azo- and azoxyaromatic chemicals via transfer coupling of nitroaromatic compounds has been achieved by fine-tuning the catalyst structure. Here, a direct method to modulate nitrobenzene reduction and selectively alter the product from azobenzene to azoxybenzene by employing the size effect of Au is reported. Au nanoclusters (NCs) with smaller sizes embedded in ZIF-8
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Stepwise One-Shot Borylation Reactions for Intersecting DABNA Substructures Exhibiting Bright Yellow‒Green Electroluminescence with EQE Beyond 40% and Mild Roll-Off Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Xin Xiong, Ting-Feng Chen, Rajat Walia, Xiao-Chun Fan, Ying-Chun Cheng, Hui Wang, Hao Wu, Xian-Kai Chen, Jia Yu, Kai Wang, Xiao-Hong Zhang
Boron/nitrogen (B/N)-doped polycyclic aromatic hydrocarbons (PAHs) with the multiple resonance (MR) effect are promising for organic light-emitting diodes (OLEDs) because of their narrowband emission and thermally activated delayed fluorescence (TADF) characteristics. Nevertheless, exploring the variety of such emitters is challenging because of the tricky and limited synthetic protocols. Herein, we
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Low‐Temperature Flexibility of Chiral Organic Crystals with Highly Efficient Second‐Harmonic Generation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Jiawei Lin, Jianmin Zhou, Zhihua Wang, Liang Li, Maolin Li, Jialiang Xu, Songgu Wu, Pance Naumov, Junbo Gong
Flexible crystals with unique mechanical properties have presented enormous applications in optoelectronics, soft robotics and sensors. However, there have been no reports of low‐temperature‐resistant flexible crystals with second‐order nonlinear optical properties (NLO). Here, we report the flexible chiral Schiff‐base crystals capable of efficient second harmonic generation (SHG). Both enantiomers
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Full‐Color Emissive Zirconium‐Organic Frameworks Constructed via in situ “One‐Pot” Single‐Site Modification for Tryptophan Detection and Energy Transfer Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Pu-Hao Fang, Lu-Lu Qu, Zhen-Sha Ma, Chao-Qin Han, Zhendong Li, Lei Wang, Kang Zhou, Jingbai Li, Xiao-Yuan Liu
Organic linker‐based luminescent metal‐organic frameworks (LMOFs) have received extensive studies due to the unlimited species of emissive organic linkers and tunable structure of MOFs. However, the multiple‐step organic synthesis is always a great challenge for the development of LMOFs. As an alternative strategy, in situ “one‐pot” strategy, in which the generation of emissive organic linkers and
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Circularly Polarized Lasing from Helical Superstructures of Chiral Organic Molecules Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Shizhe Ren, Zheng-Fei Liu, Penghao Li, Haidi Liu, Miaosen Lu, Kang Wang, Jiannian Yao, Haiyun Dong, Qingzheng Yang, Yong Sheng Zhao
Chiral supramolecular aggregates have the potential to explore circularly polarized lasing with large dissymmetry factors. However, the controllable assembly of chiral superstructures towards deterministic circularly polarized laser emission remains elusive. Here, we design a pair of chiral organic molecules capable of stacking into a pair of definite helical superstructures in microcrystals, which
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Meeting the UN Sustainable Development Goals with Mechanochemistry Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Jasna Alić, Moritz-Caspar Schlegel, Franziska Emmerling, Tomislav Stolar
Chemistry traditionally relies on reactions in solution, but this method is increasingly problematic due to the scale of chemical processes and their economic and environmental impact. Handling residual chemical waste, including solvents, incurs significant costs and environmental pressure. Conversely, novel chemical approaches are needed to address pressing societal issues such as climate change,
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Tuning Co‐operative Energy Transfer in Copper(I) Complexes Using Two‐Photon Absorbing Diimine‐Based Ligand Sensitizers Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Shawn Collins, Noémie Beaucage, Zujhar Singh, Jérémie Bourdon
Photocatalysis mediated by low energy light wavelengths has potential to enable safer, sustainable synthetic methods. A phenanthroline‐derived ligand bathocupSani, with a large two‐photon absorption (TPA) cross section was used to construct a heteroleptic complex [Cu(bathocupSani)(DPEPhos)]BF4 and a homoleptic complex [Cu(bathocupSani)2]BF4. The ligand and the respective homoleptic complex with copper
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An Ultrasound‐Activated Supramolecular Modulator Enhancing Autophagy to Prevent Ventricular Arrythmias Post‐Myocardial Infarction Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Yida Pang, Qian Li, Jiale Wang, Songyun Wang, Amit Sharma, Yuling Xu, Haoyuan Hu, Junrong Li, Shuang Liu, Yao Sun
Ventricular arrhythmias (VAs) triggered by myocardial infarction (MI) are the leading cause of sudden cardiac mortality worldwide. Current therapeutic strategies for managing MI‐induced VAs, such as left stellate ganglion resection and ablation, are suboptimal, highlighting the need to explore safer and more effective intervention strategies. Herein, we rationally designed two supramolecular sonosensitizers
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Atom Efficient Synthesis of Trimethine Cyanines Using Formaldehyde as a Single Carbon Source Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Sun Hyeok Lee, Taek-Jun Lee, Sourav Sarkar, Heewon Cho, Quynh Nguyen Nhu Pham, Young-Tae Chang
In this work, we present an innovative and atom‐efficient synthesis of trimethine cyanines (Cy3) using formaldehyde (FA) as a single‐carbon reagent. The widespread application of Cy3 dyes in bioimaging and genomics/proteomics is often limited by synthetic routes plagued with low atom economy and substantial side‐product formation. Through systematic investigation, we have developed a practical and
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Multi‐scale Hierarchical Organic Photocatalytic Platform for Self‐Suspending Sacrificial Hydrogen Production from Seawater Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Jingshuai Zhu, Jie Dang, Haoyuan Xiao, Yuqi Wang, Lei Ding, Jiaxin Zheng, Jianming Chen, Jianxiang Zhang, Xungai Wang, John H. Xin, Shiguo Chen, Yuanfeng Wang
The widespread application of photocatalysis for converting solar energy and seawater into hydrogen is generally hindered by limited catalyst activity and the lack of sustainable large‐scale platforms. Here, a multi‐scale hierarchical organic photocatalytic platform was developed, combining a photosensitive molecular heterojunction with a molecular‐scale gradient energy level alignment and micro‐nanoscale
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The nature of structural defects in ZIF‐8 revealed with 1H and 31P MAS NMR and X‐ray absorption spectroscopy Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Anton A. Gabrienko, Somboon Chaemchuen, Zongkui Kou, Naoki Ogiwara, Hiroshi Kitagawa, Alexander E. Khudozhitkov, Alexander G. Stepanov, Daniil I. Kolokolov, Francis Verpoort
The metal‐organic frameworks (MOFs) attract interest as potential catalysts whose catalytic properties are driven by defects. Several methods have been proposed for the defects‐inducing synthesis of MOFs. However, the active species formed on the defective sites remain elusive and uncharacterized, as the spectroscopic fingerprints of these species are hidden by the regular structure signals. In this
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Interfacially Fabricated Covalent Organic Framework Membranes for Film‐based Fluorescence Humidity Sensors and Moisture Driven Actuators Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Xiangquan Liu, Rongrong Huang, Lingya Peng, Jinglun Yang, Junbao Yan, Binbin Zhai, Yan Luo, Chi Zhang, Shuwen Tan, Xiaoyan Liu, Liping Ding, Yu Fang
Rapid, on‐site measurement of ppm‐level humidity in real time remains a challenge. In this work, we fabricated a few micrometer thick, β‐ketoenamine‐linked covalent organic framework (COF) membrane via interfacially confined condensation of 1,3,5‐tris‐(4‐aminophenyl)triazine (TTA) with 1,3,5‐tri‐formylphloroglucinol (TP). Based on the super‐sensitive and reversible response of the COF membrane to water
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Chemical Synergic Stabilization of High Br‐Content Mixed‐Halide Wide‐Bandgap Perovskites for Durable Multi‐Terminal Tandem Solar Cells with Minimized Pb Leakage Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Meifang Yang, Ying Tan, Guo Yang, Xueqing Chang, Tian Tian, Wenguang Li, Yuxuan Fang, Jinliang Shen, Shaopeng Yang, Wu-Qiang Wu
High Br‐content mixed‐halide perovskites with wide‐bandgap (WBG) of 1.6‐2.0 eV have showcased vast potential to be used in tandem solar cells. However, they often suffer from severe halide segregation, phase separation and ion migration issues, which would accelerate the decomposition of perovskites films, deteriorate the photovoltaic performance and even aggravate the lead leakage from damaged devices
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Photocatalytic PPh3‐Mediated Synthesis of C3‐Functionalized Indoles via Radical Annulation of Nitroarenes and Alkenes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Jingjing Zhang, Christian Mück-Lichtenfeld, Maxim Aleksa Wiethoff, Armido Studer
Oxidatively generated phosphine radical cations are reactive intermediates that can be used for the generation of carbon and heteroatom centered radicals via deoxygenation processes. Such P‐radical cations can readily be generated via single electron transfer oxidation using a redox catalyst. Cheap and commercially available nitroarenes are ideal nitrogen sources for the construction of organic amines
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Opening the Hysteresis Loop in Ferromagnetic Fe3GeTe2 Nanosheets Through Functionalization with TCNQ Molecules Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Govind Sasi Kumar, Alberto M. Ruiz, Jaime Garcia-Oliver, Yan Xin, José J. Baldoví, Michael Shatruk
Ferromagnetic metal Fe3GeTe2 (FGT), whose structure exhibits weak van‐der‐Waals interactions between 5‐atom thick layers, was subjected to liquid‐phase exfoliation (LPE) in N‐methyl pyrrolidone (NMP) to yield a suspension of nanosheets that were separated into several fractions by successive centrifugation at different speeds. Electron microscopy confirmed successful exfoliation of bulk FGT to nanosheets
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Boron Cluster Anions Dissolve en masse in Lipids Causing Membrane Expansion and Thinning Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Andrea Barba-Bon, Alae El Haitami, Coralie Pasquier, Ivana Nikšić-Franjić, Olivier Diat, Pierre Bauduin, Sophie Cantin, Werner M. Nau
Boron clusters are applied in medicinal chemistry because of their high stability in biological environments and intrinsic ability to capture neutrons. However, their intermolecular interactions with lipid membranes, which is critical for their cellular delivery and biocompatibility, have not been comprehensively investigated. In this study, we combine different experimental methods – Langmuir monolayer
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Metal‐Free Wet Chemistry for the Fast Gram‐Scale Synthesis of γ‐Graphyne and its Derivatives Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-18 Tao Song, Hong Liu, Haiyuan Zou, Cheng Wang, Siyan Shu, Hao Dai, Lele Duan
γ‐Graphyne (GY), an emerging carbon allotrope, is envisioned to offer various alluring properties and broad applicability. While significant progress has been made in the synthesis of GY over recent decades, its widespread application hinges on developing efficient, scalable, and accessible synthetic methods for the production of GY and its derivatives. Here we report a facile metal‐free nucleophilic