![](https://scdn.x-mol.com/css/images/icon-new-link.png)
样式: 排序: IF: - GO 导出 标记为已读
-
Non‐alternant Nanographenes Bearing N‐Doped Non‐hexagonal Pairs: Synthesis, Structural Analysis and Photophysical Properties Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-20 Huan Luo, Junzhi Liu
Introduction of nonhexagons and/or heteroatoms allows for finely tuning the physicochemical properties of nanographenes. Heteroatoms doping have dominated the modulation of nanographenes with tunable bandgap, rich electrochemical activities and so on. The pair of nonhexagons, for instance, pentagon‐heptagon pairs, have furnished nanographenes with aromatic and/or antiaromatic characteristics, open‐shell
-
Rigid‐Flexible Coupled Dendritic Molecule Doping: General Approach to Activate Commercial Polymers into Harsh Condition‐ Tolerant Multi‐Reusable Strong Supramolecular Adhesives Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-20 Jie Feng, Ziwei Lin, Yang Zhang, Long Fang, Qikai Zhu, Dingshan Yu
Developing functional adhesives combining strong adhesion, good recyclability and diverse harsh‐condition adaptability is a grand challenge. Here, we introduce a general dendritic molecule doping strategy to activate commercial polymers into a new family of supramolecular adhesives integrating high adhesion strength, ultralow temperature, water resistant and multi‐reusable properties. Our method involves
-
A Microscopically Heterogeneous Colloid Electrolyte for Extremely Fast‐Charging and Long‐Calendar‐Life Silicon‐Based Lithium‐Ion Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-20 Weifeng Zhang, Wenwu Zou, Guoxing Jiang, Shengguang Qi, Siyuan Peng, Huiyu Song, Zhiming Cui, Zhenxing Liang, Li Du
Fast‐charging capability and calendar life are critical metrics in rechargeable batteries, especially in silicon‐based batteries that are susceptible to sluggish Li+ desolvation kinetics and HF‐induced corrosion. No existing electrolyte simultaneously tackles both these pivotal challenges. Here we report a microscopically heterogeneous covalent organic nanosheet (CON) colloid electrolyte for extremely
-
A Multielectron and High‐Potential Spirobifluorene‐based Posolyte for Aqueous Redox Flow Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-20 Pan Wang, Shuai Pang, Lu Li, Yunlong Ji
The rising energy demand driven by human activity has posed pressing challenges in embracing renewable energy, necessitating advances in energy storage technologies to maximize their utilization efficiency. Recent studies in aqueous organic redox flow batteries focused primarily on the development of organic negative electrolytes, while the progress in organic positive electrolytes remains constrained
-
Dynamic Covalent Bonds Enabled Carbon Fiber Reinforced Polymers Recyclability and Material Circularity Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-20 Xiaotong Fan, Jie Zheng, Jayven Chee Chuan Yeo, Sheng Wang, Ke Li, Joseph Kinyanjui Muiruri, Nikos Hadjichristidis, Zibiao Li
Due to their remarkable features of lightweight, high strength, stiffness, high‐temperature resistance, and corrosion resistance, carbon fiber reinforced polymers (CFRPs) are extensively used in sports equipment, vehicles, aircraft, windmill blades, and other sectors. The urging need to develop a resource‐saving and environmentally responsible society requires the recycling of CFRPs. Traditional CFRPs
-
Leveraging Ion Pairing and Transport in Localized High‐Concentration Electrolytes for Reversible Lithium Metal Anodes at Low Temperatures Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-20 Zhengfei Zhao, Aoxuan Wang, Aosai Chen, Yumeng Zhao, Zhenglin Hu, Kai Wu, Jiayan Luo
Coulombic efficiency of over 99% is rarely achieved for Li metal anode below ‐40°C, hindering the practical application of high‐energy‐density Li metal batteries under extreme conditions. Herein, limiting factors for Li metal reversibility are investigated utilizing ether‐based localized high‐concentration electrolytes of different solvent‐diluent combinations. We find that along with the desolvation
-
Rationalizing Acidic Oxygen Evolution Reaction over IrO2: Essential Role of Hydronium Cation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-20 Tianyou Mou, Daniela A. Bushiri, Daniel V. Esposito, Ping Liu, Jingguang G. Chen
The development of active, stable, and more affordable electrocatalysts for acidic oxygen evolution reaction (OER) is of great importance for the practical application of electrolyzers and the advancement of renewable energy conversion technologies. Currently, IrO2 is the only catalyst with high stability and activity, but a high cost. Further optimization of the catalyst is limited by the lack of
-
Plasmon‐Driven Highly Selective CO2 Photoreduction to C2H4 on Ionic Liquid‐Mediated Copper Nanowires Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-20 Hongli Liu, Bin Sun, Zaiqi Li, Difei Xiao, Zeyan Wang, Yuanyuan Liu, Zhaoke Zheng, Peng Wang, Ying Dai, Hefeng Cheng, Baibiao Huang
Selective CO2 photoreduction to value‐added multi‐carbon (C2+) feedstocks, such as C2H4, holds great promise in direct solar‐to‐chemical conversion for a carbon‐neutral future. Nevertheless, the performance is largely inhibited by the high energy barrier of C–C coupling process, thereby leading to C2+ products with low selectivity. Here we report that through facile surface immobilization of a 1‐e
-
The Effects of Pore Defects in π‐Extended Pentadecabenzo[9]helicene Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Ke-Lin Zhu, Zhi-Ao Li, Jiaqi Liang, Kang-Li Zou, Yun-Jia Shen, Han-Yuan Gong
The introduction of precise pore defects into nanocarbon structures results in the emergence of distinct physicochemical characteristics. However, there is a lack of research on non‐planar chiral nanographene involving precise pore defects. Herein, we have developed two analogues to the π‐extended pentadecabenzo[9]helicene (EP9H) containing embedded pore defects. Each molecule, namely extended dodecabenzo[7]helicene
-
Chelator‐Assisted Precipitation‐Based Separation of the Rare Earth Elements Neodymium and Dysprosium from Aqueous Solutions Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Yangyang Gao, Gerra L. Licup, Nicholas P. Bigham, David C. Cantu, Justin J. Wilson
The rare earth elements (REEs) are critical resources for many clean energy technologies, but are difficult to obtain in their elementally pure forms because of their nearly identical chemical properties. Here, an analogue of macropa, G‐macropa, was synthesized and employed for an aqueous precipitation‐based separation of Nd3+ and Dy3+. G‐macropa maintains the same thermodynamic preference for the
-
Optimizing Upconversion Quantum Yield via Structural Tuning of Dipyrrolonaphthyridinedione Annihilators Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Alexandra J. Lyons, Lukas Naimovičius, Simon K. Zhang, Andrew B. Pun
Triplet‐triplet annihilation upconversion (TTA‐UC) is a photophysical process in which two low‐energy photons are converted into one higher‐energy photon. This type of upconversion requires two species: a sensitizer that absorbs low‐energy light and transfers its energy to an annihilator, which emits higher‐energy light after TTA. In spite of the multitude of applications of TTA‐UC, few families of
-
Versatile Dehydration‐Assisted Functionalization of Quantum Dots and Rods Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Chi Chen, Xin Luo, Mark Bathe
Functionalization of quantum dots (QDs) and quantum rods (QRs) with ligands is essential for their further practical application across various domains. Dehydration‐assisted functionalization (DAF) is a versatile method applicable to a wide range of hydrophilic ligands with an affinity to the surface of QDs and QRs. This approach facilitates rapid one‐pot ligand exchange and dense modification by efficiently
-
Leap‐Type Response of Redox/Photo‐Active Lanthanide‐Based Metal‐Organic Frameworks for Early and Accurate Screening of Prostate Cancer Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Kaiming Ge, Guoli Chen, Dapeng Zhang, Ji-Na Hao, Yongsheng Li
The development of high‐accuracy technologies to distinguish the quite tiny concentration change of tumor markers between negative and positive is of vital significance for early screening and diagnosis of cancers, but is still a great challenge for the conventional biosensors because of their “gradual” detection mode. Herein, a unique “leap‐type” responsive lanthanide MOF‐based biosensor (designated
-
Simultaneous Defect Passivation and Co‐catalyst Engineering Leads to Superior Photocatalytic Hydrogen Evolution on Metal Halide Perovskites Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Ting Xu, Yuxin Xie, Shengliang Qi, Hefeng Zhang, Weiguang Ma, Junhui Wang, Yuying Gao, Lianzhou Wang, Xu Zong
Metal halide perovskites (MHPs) have emerged as attractive candidates for producing green hydrogen via photocatalytic pathway. However, the presence of abundant defects and absence of efficient hydrogen evolution reaction (HER) active sites on MHPs seriously limit the solar‐to‐chemical (STC) conversion efficiency. Herein, to address this issue, we present a bi‐functionalization strategy through decorating
-
Radical 6‐Endo Addition Enables Pyridine Synthesis under Metal‐Free Conditions Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Xiaojuan Dong, Yingbo Shao, Zhengyi Liu, Xia Huang, Xiaosong Xue, Yiyun Chen
Metal‐free synthesis of heterocycles is highly sought after in the pharmaceutical industry and has garnered widespread attention due to its environmental sustainability and cost‐effectiveness. We report a radical 6‐endo addition method for pyridine synthesis from cyclopropylamides and alkynes under metal‐free conditions. Various terminal and substituted alkynes are inserted as C2 units into cyclopropylamides
-
Spatial Engineering of Heterotypic Antigens on a DNA Framework for the Preparation of Mosaic Nanoparticle Vaccines with Enhanced Immune Activation against SARS‐CoV‐2 Variants Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Yang Yang, Jialu Zhang, Yunyun Xu, Mingying Chen, Shengwen Wang, Guihong Lin, Yihao Huang, Chaoyong Yang, Yanling Song
Mosaic nanoparticle vaccines with heterotypic antigens exhibit broad‐spectrum antiviral capabilities, but the impact of antigen proportions and distribution patterns on vaccine‐induced immunity remains largely unexplored. Here, we present a DNA nanotechnology‐based strategy for spatially assembling heterotypic antigens to guide the rational design of mosaic nanoparticle vaccines. By utilizing two aptamers
-
Modulating Charge‐Transfer Excited States of Multiple Resonance Emitters via Intramolecular Covalent Bond Locking Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Tingting Huang, Yincai Xu, Xueying Lu, Yupei Qu, Jinbei Wei, Yue Wang
Advanced multiple resonance thermally activated delayed fluorescence (MR‐TADF) emitters with high efficiency and color purity have emerged as a research focus in developing ultra‐high‐definition displays. Herein, we disclose an approach to modulate charge‐transfer excited states of MR emitters via intramolecular covalent bond locking. This strategy can promote the evolution of strong intramolecular
-
Vaporchromic Domino Transformation and Polarized Photonic Heterojunctions of Organoplatinum Microrods Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Jian-Cheng Chen, Zhong-Liang Gong, Zhong-Qiu Li, Yuan-Yuan Zhao, Kun Tang, Dian-Xue Ma, Fa-Feng Xu, Yu-Wu Zhong
Photonic heterostructures with codable properties have shown great values as versatile information carriers at the micro and nanoscale. These heterostructures are typically prepared by a step‐by‐step growth or post‐functionalization method to achieve varied emission colors among different building blocks. In order to realize high‐throughput and multivariate information loading, we report here a strategy
-
Dynamically Cross‐linked Oligo[2]rotaxane Networks Mediated by Metal‐Coordination Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Ruixue Bai, Wenbin Wang, Wenzhe Gao, Mengling Yang, Xinhai Zhang, Chunyu Wang, Zhiwei Fan, Li Yang, Zhaoming Zhang, Xuzhou Yan
Polyrotaxanes (PRs) have attracted significant research attention due to their unique topological structures and high degrees of conformational freedom. Herein, we take advantage of an oligo[2]rotaxane to construct a novel class of dynamically cross‐linked rotaxane network (DCRN) mediated by metal‐coordination. The oligo[2]rotaxane skeleton offers several distinct advantages: In addition to retaining
-
Synergistic Active Heterostructure Design for Enhanced Two Electron Oxygen Reduction via Chemical and Electrochemical Reconstruction of Heterosulfides Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Kai Yu, Hongyuan Yang, Jie Xu, Weijie Yuan, Ruotao Yang, Meiling Hou, Zhenhui Kang, Yang Liu, Prashanth W. Menezes, Ziliang Chen
Transition metal sulfides, particularly heterostructures, represent a promising class of electrocatalysts for two electron oxygen reduction (2e− ORR), however, understanding the dynamic structural evolution of these catalysts during alkaline ORR remains relatively unexplored. Herein, NiS2/In2.77S4 heterostructure was synthesized as a precatalyst and through a series of comprehensive ex‐situ and in‐situ
-
Photo‐assisted chemical self‐rechargeable zinc ion batteries with high charging and discharging efficiency Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Xing-Yuan Du, Li-Na Song, Shuang Liang, Yi-Feng Wang, Yue Wang, Huan-Feng Wang, Ji-Jing Xu
Chemically self‐recharging zinc ion batteries (ZIBs), which are capable of auto‐recharging in ambient air, are promising in self‐powered battery systems. Nevertheless, the exclusive reliance on chemical energy from oxygen for ZIBs charging often would bring some obstacles in charging efficiency. Herein, we develop photo‐assisted chemically self‐recharging aqueous ZIBs with a heterojunction of MoS2/SnO2
-
Nonalternant B,N‐Embedded Helical Nanographenes Containing Azepines: Programmable Synthesis, Responsive Chiroptical Properties and Spontaneous Resolution into a Single‐Handed Helix Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-19 Weiwen Zhuang, Faan-Fung Hung, Chi-Ming Che, Junzhi Liu
Heteroatom‐embedded helical nanographenes (NGs) constitute an important and appealing class of intrinsically chiral materials. In this work, a series of B,N‐embedded helical NGs bearing azepines was synthesized via stepwise regioselective cyclodehydrogenation. First, the phenyl‐ or nitrogen‐bridged dimers were efficiently clipped into highly congested model compounds 1 and 2. Later, the controllable
-
Helicene Covalent Organic Frameworks for Robust Light Harvesting and Efficient Energy Transfers Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Cong Yin, Xingyao Ye, Shanshan Tao, Dan Zhao, Yongfeng Zhi, Donglin Jiang
Helicenes represent a class of fascinating π compounds with fused yet folded backbones. Despite their broad structural diversity, harnessing helicenes to develop well‐defined materials is still a formidable challenge. Here we report the synthesis of crystalline porous helicene materials by exploring helicenes to synthesize covalent 2D lattices and layered π frameworks. Topology‐directed polymerization
-
Stable Lithium Oxygen Batteries Enabled by Solvent‐diluent Interaction in N,N‐dimethylacetamide‐based Electrolytes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Dong-Yue Yang, Jia-Yi Du, Yue Yu, Ying-Qi Fan, Gang Huang, Xin-bo Zhang, Hongjie Zhang
In the pursuit of next‐generation ultrahigh‐energy‐density Li–O2 batteries, it is imperative to develop an electrolyte with stability against the strong oxidation environments. N,N‐dimethylacetamide (DMA) is a recognized solvent known for its robust resistance to the highly reactive reduced oxygen species, yet its application in Li–O2 batteries has been constrained due to its poor compatibility with
-
Challenges and Applications of Supramolecular Metalate Chemistry Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Joseph G. O’Connell-Danes, Bryne T. Ngwenya, Carole A. Morrison, Jason Love
While the supramolecular chemistry of simple anions is ubiquitous, the targeting and exploitation of their metal‐containing relatives, the metalates, is less well understood. This mini review highlights the latest advances in this emergent area by discussing the supramolecular chemistry of metalates thematically, with a focus on the exploitation of metalates in a diversity of applications, including
-
“Anions‐in‐Colloid” Hydrated Deep Eutectic Electrolyte for High Reversible Zinc Metal Anodes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Min Cheng, Diantao Li, Junlun Cao, Tianjiang Sun, Qiong Sun, Weijia Zhang, Zhengtai Zha, Mengyao Shi, Kai Zhang, Zhanliang Tao
Zn metal suffers from severe zinc dendrites, anion‐related side reactions, hydrogen evolution reaction (HER) and narrow electrochemical stable window (ESW). Herein, an“anions‐in‐colloid” hydrated deep eutectic electrolyte (ACDE‐3) is designed to improve the stability of zinc anode. The ACDE‐3 reconfigures the hydrogen‐bond (HB) network and regulates the solvation shell. More importantly, the hydroxyl‐rich
-
Controlled Protein‐Membrane Interactions Modulate Self‐Organization of Min Protein Patterns Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Mergime Hasani, Katharina Esch, Katja Zieske
Self‐organizing protein patterns are crucial for living systems, governing important cellular processes such as polarization and division. While the field of protein self‐organization has reached a point where basic pattern‐forming mechanisms can be reconstituted in vitro using purified proteins, understanding how cells can dynamically switch and modulate these patterns, especially when transiently
-
Conformational Locking Induced Enantioselective Diarylcarbene Insertion into B‐H and O‐H Bonds Using a Cationic Rh(I)/Diene Catalyst Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Weici Xu, Takeshi Yamakawa, Meiling Huang, Peilin Tian, Zhigen Jiang, Ming-Hua Xu
Transition‐metal‐catalyzed enantioselective transformations of aryl/aryl carbene are inherently challenging due to the difficulty in distinguishing between two arene rings in the reaction process thus remain largely less explored. The few successful examples reported so far, without exception, have all been catalyzed by Rh(II)‐complexes. Herein, we describe our successful development of a novel cationic
-
Dual Channel Emissions of Kasha and Anti‐Kasha from a Single Radical Molecule Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Zihao Zhu, Zhiyuan Kuang, Li Shen, Shengjie Wang, Xin Ai, Alim Abdurahman, Qiming Peng
Stable open‐shell luminescent radicals have recently attracted much attention due to their unique luminescence properties. However, a radical molecule with both Kasha and anti‐Kasha doublet emission properties has not been reported. Herein, we have successfully synthesized a stable chlorine‐substituted Chichibabin's hydrocarbon, TTM‐TTM, along with its mono‐radical counterpart, TTM‐HTTM. The emission
-
Constrained Catalytic Itinerary of a Retaining 3,6‐Anhydro‐D‐Galactosidase, a Key Enzyme in Red Algal Cell Wall Degradation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Michael D. Wallace, Irene Cuxart, Thomas Roret, Laura Guée, Aleksandra W. Debowski, Mirjam Czjzek, Carme Rovira, Keith A. Stubbs, Elizabeth Ficko-Blean
The marine Bacteroidota Zobellia galactanivorans has a polysaccharide utilization locus dedicated to the catabolism of the red algal cell wall galactan carrageenan and its unique and industrially important α‐3,6‐anhydro‐D‐galactose (ADG) monosaccharide. Here we present the first analysis of the specific molecular interactions the exo‐(α‐1,3)‐3,6‐anhydro‐D‐galactosidase ZgGH129 uses to cope with the
-
Regulating Anode‐electrolyte Interphasial Reactions by Zwitterionic Binder Chemistry in Lithium‐ion Batteries with High‐nickel Layered Oxide Cathodes and Silicon‐Graphite Anodes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Biyu Jin, Andrei Dolocan, Chen Liu, Zehao Cui, Arumugam Manthiram
The practical application of silicon (Si)‐based anodes faces challenges due to severe structural and interphasial degradations. These challenges are exacerbated in lithium‐ion batteries (LIBs) employing Si‐based anodes with high‐nickel layered oxide cathodes, as significant transition‐metal crossover catalyzes serious parasitic side reactions, leading to faster cell failure. While enhancing the mechanical
-
Coumarin‐Based Photodegradable Hydrogels Enable Two‐Photon Subtractive Biofabrication at 300 mm s−1 Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Wanwan Qiu, Christian Gehre, Jaime Pietrantuono Nepomuceno, Yinyin Bao, Zhiquan Li, Ralph Müller, Xiao‐Hua Qin
-
Reducing Dielectric Confinement Effect Enhances Carrier Separation in Two‐dimensional Hybrid Perovskite Photocatalysts Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Zhaohui Fang, Guohong Wang, Chen Guan, Jianjun Zhang, Quanjun Xiang
Two‐dimensional organic‐inorganic hybrid perovskites ( OIHPs) with alternating structure of the organic and inorganic layers have a natural quantum well structure. The difference of dielectric constants between organic and inorganic layers in this structure results in the enhancement of dielectric confinement effect, which exhibits a large exciton binding energy and hinders the separation of electron‐hole
-
Photocatalytic Multisite Functionalization of Unactivated Terminal Alkenes by Merging Polar Cycloaddition and Radical Ring‐Opening Process Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Haidong Liu, Yi-Peng Wang, Hui Wang, Kewei Ren, Longfei Liu, Luzhen Dang, Cheng-Qiang Wang, Chao Feng
Although highly appealing for rapid access of molecular complexity, multi‐functionalization of alkenes that allows incorporation of more than two functional groups remains a prominent challenge. Herein, we report a novel strategy that merges dipolar cycloaddition with photoredox promoted radical ring‐opening remote C(sp3)–H functionalization, thus enabling a smooth 1,2,5‐trifunctionalization of unactivated
-
Regulating Spin Polarization via Axial Nitrogen Traction at Fe‐N5 Sites Enhanced Electrocatalytic CO2 Reduction for Zn‐CO2 Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Yanran Bao, Jiayong Xiao, Yongkang Huang, Youzhi Li, Siyu Yao, Ming Qiu, Xiaoxuan Yang, Lecheng Lei, Zhongjian Li, Yang Hou, Gang Wu, Bin Yang
Single Fe sites have been explored as promising catalysts for the CO2 reduction reaction to value‐added CO. Herein, we introduce a novel molten salt synthesis strategy for developing axial nitrogen‐coordinated Fe‐N5 sites on ultrathin defect‐rich carbon nanosheets, aiming to modulate the reaction pathway precisely. This distinctive architecture weakens the spin polarization at the Fe sites, promoting
-
Green Solvent γ‐Valerolactone (GVL) Facilitates Photocatalytic C−H Bond Activation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Xuejiao Wu, Shunji Xie, Dario Vangestel, He Zhao, Bert F. Sels
Solvents can significantly influence chemical reactions in condensed phases. Their critical properties are increasingly recognized in various research domains such as organic synthesis and biomass valorization. However, in semiconductor photocatalysis, solvents are primarily viewed as mediums for dissolving and diffusing substances, with their potential beneficial effects on photocatalytic conversions
-
Toggling the Oxygen Affinity between Anthracenes and Naphthalenes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Torsten Linker, Werner Fudickar
We present the design of an anthracenyl⎯naphthyl (ANT⎯NAPH) dyad and its application as a luminescent 4‐stage photo switch. Both segments can individually react with singlet oxygen to switch off an optical response. In their initial form the larger ANT component reacts significantly faster and thus an ANTO2⎯NAPH stage is turned on, observed by optical response of the remaining NAPH. To reduce its reactivity
-
Interception and Synthetic Application of Diradical and Diene Forms of Dual‐Nature Azabicyclic o‐Quinodimethanes Generated by 6p‐Azaelectrocyclization Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Shankar Majji, Daniel J. Lee, Supuni I. N. Hewa Inaththappulige, Ayush Acharya, Hemant P. Yennawar, Ramesh Giri
We demonstrate that 2‐alkenylarylaldimines and ketimines undergo thermal 6p‐azaelectrocyclization to generate a wide range of azabicyclic o‐quinodimethanes (o‐QDMs). These o‐QDMs exist as a hybrid of a diene and a benzylic diradical. The diradical nature was confirmed by their ability to undergo dimerization and react with H‐atom donor, 2,2,6,6‐Tetramethylpiperidin‐1‐yl)oxyl (TEMPO) and O2. In addition
-
Enantioselective Copper‐Catalyzed Sequential Hydrosilylation of Arylmethylenecyclopropanes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Bin Fu, Lianghua Wang, Kexin Chen, Xiuping Yuan, Jianjun Yin, Simin Wang, Dazhen Shi, Bo Zhu, Wei Guan, Qian Zhang, Tao Xiong
Despite impressive advances in the construction of enantioenriched silacarbocycles featuring silicon‐stereogenic centers via a selection of well‐defined sila‐synthons, the development of a more convenient and economic method with readily available starting materials is significantly less explored and remains a considerable challenge. Herein, we report the first example of copper‐catalyzed sequential
-
Biosynthesis of the Non‐canonical C17 Sesquiterpenoids Chlororaphen A and B from Pseudomonas chlororaphis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Houchao Xu, Heng Li, Bernd Goldfuss, Gregor Schnakenburg, Jeroen S. Dickschat
Chlororaphens A and B are structurally unique non‐canonical C17 sesquiterpenoids from Pseudomonas chlororaphis that are made by two SAM‐dependent methyltransferases and a type I terpene synthase. This study addresses the mechanism of their formation in isotopic labelling experiments and DFT calculations. The results demonstrate an astonishing complexity with distribution of labellings within a cyclopentane
-
Bis‐Silylene‐Supported Aluminium Atoms with Aluminylene and Alane Character Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-18 Matthias Driess, Artemis Saddington, Shicheng Dong, Shenglai Yao, Jun Zhu
The suitability of electron‐rich bis‐silylenes, specifically the neutral chelating [SiII(Xant)SiII] ligand (SiII = PhC(NtBu)2Si, Xant = 9,9dimethylxanthene) and the anionic [SiII(NAcrid)SiII)]‒ pincer ligand (NAcrid = 2,7,9,9‐tetramethylacridane), has been successfully probed to stabilize monovalent bis‐silylene‐supported aluminium complexes (aluminylenes). At first, the unprecedented aluminium(III)
-
-
-
Corrigendum: Sequence‐Tunable Phase Behavior and Intrinsic Fluorescence in Dynamically Interacting Peptides Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17
-
Sulfurized Two‐Dimensional Conductive Metal‐Organic Framework as a High‐Performance Cathode Material for Rechargeable Mg Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Yu Mu, James Nyakuchena, Yang Wang, James R. Wilkes, Tongtong Luo, Michael Goldstein, Brooke Elander, Udayan Mohanty, Junwei Lucas Bao, Jier Huang, Dunwei Wang
Rechargeable Mg batteries are a promising energy storage technology to overcome the limitations inherent to Li ion batteries. A critical challenge in advancing Mg batteries is the lack of suitable cathode materials. In this work, we report a cathode design that incorporates S functionality into two‐dimensional metal‐organic‐frameworks (2D‐MOFs). This new cathode material enables good Mg2+ storage capacity
-
Covalent Triazine Based Frameworks with Donor‐Donor‐π‐Acceptor Structures for Dendrite‐Free Lithium Metal Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Xiao-Meng Lu, Haichao Wang, Yiwen Sun, Yi Xu, Weiwei Sun, Yang Wu, Yifan Zhang, Chao Yang, Yong Wang
The appearance of disordered lithium dendrites and fragile solid electrolyte interfaces (SEI) significantly hinder the serviceability of lithium metal batteries. Herein, guided by theoretical predictions, a multi‐component covalent triazine framework with partially electronegative channels (4C‐TA0.5TF0.5‐CTF) is incorporated as a protective layer to modulate the interface stability of the lithium metal
-
Multiplexed Shortwave Infrared Imaging Highlights Anatomical Structures in Mice Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Xingjian Zhong, Amish Patel, Yidan Sun, Alexander M. Saeboe, Allison Dennis
Multiplexed fluorescence in vivo imaging remains challenging due to the attenuation and scattering of visible and traditional near infrared (NIR‐I, 650 – 950 nm) wavelengths. Fluorescence imaging using short‐wave infrared (SWIR, 1000 – 1700 nm, a.k.a. NIR‐II) light enables deeper tissue penetration due to reduced tissue scattering as well as minimal background autofluorescence. SWIR‐emitting semiconductor
-
-
-
-
-
Progressive endergonic synthesis of Diels‐Alder adducts driven by chemical energy Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Shaymaa Al Shehimy, Hai-Dang Le, Shuntaro Amano, Simone Di Noja, Luca Monari, Giulio Ragazzon
The overwhelming majority of artificial chemical reaction networks respond to stimuli by relaxing towards an equilibrium state. The opposite response – moving away from equilibrium – can afford the endergonic synthesis of molecules, of which only rare examples have been reported. Here, we report six examples of Diels‐Alder adducts accumulated in an endergonic process and use this strategy to realize
-
Intense Circularly Polarized Luminescence Induced by Chiral Supramolecular Assembly: The Importance of Intermolecular Electronic Coupling Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Zheng-Fei Liu, Xin-Xin Liu, Han Zhang, Lan Zeng, Li-Ya Niu, Peng-Zhong Chen, Wei-Hai Fang, Xiaojun Peng, Ganglong Cui, Qing-Zheng Yang
Herein we report on circularly polarized luminescence (CPL) emission originating from supramolecular chirality of organic microcrystals with a |glum| value up to 0.11. The microcrystals were prepared from highly emissive difluoroboron β‐diketonate (BF2dbk) dyes R‐1 or S‐1 with chiral binaphthol (BINOL) skeletons. R‐1 and S‐1 exhibit undetectable CPL signals in solution but manifest intense CPL emission
-
Customized Photoelectrochemical C–N and C–P Formation Enabled by Tailored Deposition on Photoanodes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 jinghao wang, Caoyu Yang, Huiwen Gao, Lulu Zuo, Zhiyu Guo, Pengqi Yang, Siyang Li, Zhiyong Tang
Photoelectrochemistry (PEC) is burgeoning as an innovative solution to organic synthesis. However, the current PEC system suffers limited reaction types and unsatisfactory performances. Herein, we employ efficient BiVO4 photoanode with tailored deposition layers for customizing two PEC approaches toward C–N and C–P formation. Notably, our process proceeds under mild reaction conditions, easily available
-
Atroposelective Synthesis of Axial Biaryls by Dynamic Kinetic Resolution Using Engineered Imine Reductases Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Xinyue Hao, Zhuangfei Tian, Zhouchang Yao, Tienan Zang, Shucheng Song, Liang Lin, Tianzhang Qiao, Ling Huang, Haigen Fu
Axially chiral biaryls are ubiquitous scaffolds in natural products, bioactive molecules, chiral ligands and catalysts, but biocatalytic methods for their asymmetric synthesis are limited. Here, we report a highly efficient biocatalytic route for the atroposelective synthesis of biaryls via dynamic kinetic resolution (DKR). This DKR approach features a transient six‐membered aza‐acetal bridge‐promoted
-
Highly tough slide‐crosslinked gel polymer electrolyte for stable lithium metal batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Xuetian Deng, Jing Chen, Xin Jia, Xinyu Da, Yuanjun Zhao, Yiyang Gao, Yang Gao, Xiangpeng Kong, Shujiang Ding, Guoxin Gao
Gel polymer electrolytes (GPEs) hold great promise for the practical application of lithium metal batteries. However, conventional GPEs hardly resists lithium dendrites growth and maintains long‐term cycling stability of the battery due to its poor mechanical performance. Inspired by the slide‐ring structure of polyrotaxanes (PRs), herein we developed a dynamic slide‐crosslinked gel polymer electrolyte
-
Iron(II)‐Catalyzed 1,2‐Diamination of Styrenes Installing a Terminal NH2 Group Alongside Unprotected Amines Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Valentyn Pozhydaiev, Antonio Paparesta, Joseph Moran, David Leboeuf
1,2‐Diamination of alkenes represents an attractive way to generate differentiated vicinal diamines, which are prevalent motifs in biologically active compounds and catalysts. However, existing methods are usually limited in scope and produce diamines where one or both nitrogens are protected, adding synthetic steps for deprotection and further N‐functionalization to reach a desired target. Furthermore
-
Delocalized Orbitals Over Metal Clusters and Organic Linkers Enable Boosted Charge Transfer in Metal‐Organic Framework for Overall CO2 Photoreduction Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-07-17 Hai-Xiong Liu, Zi-Jian Zhou, Lei Xie, Chen Liu, Lei Cai, Xin-Ping Wu, Tian-Fu Liu
The conversion of CO2 to C2 through photocatalysis poses significant challenges, and one of the biggest hurdles stems from the sluggishness of the multi‐electron transfer process. Herein, taking metal‐organic framework (PFC‐98) as a model photocatalyst, we report a new strategy to facilitate charge separation. This strategy involves matching the energy levels of the lowest unoccupied node and linker
-
-