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Emulating “Curvature-Enhanced Adsorbate Coverage” for Superconformal and Orientated Zn Electrodeposition in Zinc-ion-Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Yuxin Tang, Huibo Wang, Yi Liu, Mengyu Zhu, Yuejin Chen, Danling Chen, Zhimin Lin, Kexuan Wang, Zhu Xu, Shi Chen, Guichuan Xing, Oleksandr I. Malyi, YanYan Zhang
Uneven Zn deposition and unfavorable side reactions have prevented the reversibility of the Zn anode. Herein, we design a rearranged (002) textured Zn anode inspired by a traditional curvature-enhanced adsorbate coverage (CEAC) process to realize the highly reversible Zn anode. The rearranged (002) textured structure orientates the superconformal Zn deposition owing to the spatial deposition rate of
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Self-organized Patterns in Non-reciprocal Active Droplet Systems Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Yutong Liu, R. Kailasham, Pepijn G. Moerman, Aditya S. Khair, Lauren Zarzar
Non-equilibrium patterns are widespread in nature and often arise from the self-organization of constituents through nonreciprocal chemotactic interactions. In this study, we demonstrate how active oil-in-water droplet mixtures with predator-prey interactions can result in a variety of self-organized patterns. By manipulating physical parameters, the droplet diameter ratio and number ratio, we identify
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Multivalent Weak Protections Ultimately Enable Customizable DNA Grafting on Pristine Ag Colloids for Nanoplasmonics Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Lei Song, Xiaojun Song, Yanjuan Li, Yan Hao, Song Wang, Zhaoxiang Deng
Silver nanoparticles (AgNPs) have superior plasmonic properties surpassing other metals. However, a long-standing difficulty in valence/density-tunable DNA grafting of AgNPs disfavors their use in DNA-directed nanoplasmonics. Herein a close-to-ideal surface protection of pristine AgNPs against various notorious stability issues of Ag is achieved based on multidentate weak nucleobase bindings of non-programming
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γ-Ray Driven Aqueous-Phase Methane Conversions into Complex Molecules up to Glycine Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Fei Fang, Xiao Sun, Yuanxu Liu, Zhiwen Jiang, Mozhen Wang, Xuewu Ge, Weixin Huang
Fundamental understanding of initial evolutions of molecules in the universe is of great interest and importance. CH4 is one of the abundant simple molecules in the universe. Herein we report γ-ray, high-energy photons commonly existing in cosmic rays and unstable isotope decay, as an external energy to efficiently drives aqueous-phase CH4 conversions to various products with the presence of oxygen
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Inner Side Chain Modification of Small Molecule Acceptors Enables Lower Energy Loss and High Efficiency of Organic Solar Cells Processed with Non-halogenated Solvents Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 xiaojun li, Xiangxi Wu, Yufei Gong, Shucheng Qin, Haozhe He, Zekun Chen, Tongling Liang, Caixuan Wang, Dan Deng, Zhaozhao Bi, Wei Ma, Lei Meng, Yongfang Li
Organic solar cells (OSCs) processed with non-halogenated solvents usually suffer from excessive self-aggregation of small molecule acceptors (SMAs), severe phase separation and higher energy loss (Eloss), leading to reduced open-circuit voltage (Voc) and power conversion efficiency (PCE). Here, we designed and synthesized two SMAs L8-PhF and L8-PhMe by introducing different substituents (fluorine
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Stabilizing Hydrogen Radicals in Two-Dimensional Cobalt-Copper Mesoporous Nanoplates for Complete Nitrate Reduction Electrocatalysis to Ammonia Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Chenyu Han, Lizhi Sun, Shu Han, Ben Liu
Ambient electrochemical reduction of waste nitrate (NO3−) represents an alternative green route for sustainable ammonia (NH3) electrosynthesis in water. Despites some encouraged achievements, sluggish eight electron and nine proton reduction routes that involve multi-step hydrogenation pathways have severely hindered their NH3 Faradaic efficiency (FENH3) and yield rate. Herein, we develop a robust
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The Azide-Wittig Reaction Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Kushik Kushik, Andrey Petrov, Davide Ranieri, Luisa Edelmann, Torsten Beweries, Christian Hering-Junghans
The introduction of heteroatoms into conjugated organic molecules is an important strategy to tune their reactivity and physical properties. In this realm triazabutadienes (TBDs) of the general from R2C=N−N=NR’ are an interesting class of compounds, however, general synthetic protocols for their generation are limited. Based on the serendipitous finding that the sterically encumbered azide Mes*N3 (Mes*
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NIR-Activable Charge Transfer Agents for Synergistic Photoimmunotherapy Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Chu Wang, Wenbin Zhong, Xiaohuan Sun, Jingjing Guo, Yun Chen, Yue Zhao, Jie Han, Yanli Zhao
The combination of photothermal therapy (PTT) and photodynamic therapy (PDT) has become an attractive tumor treatment modality, yet the facile design of photoimmunotheranostic agents with efficient near infrared (NIR) light-absorbing and immune- activating capabilities remains a tremendous challenge. Herein, we developed a NIR-activable organic charge transfer complex (CTC), with perylene (PER) as
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Dipole Moment Dictates the Preferential Immobilization in Gel Electrolytes for Ah-level Aqueous Zinc-Metal Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Shaojie Zhang, Huaisheng Ao, Jingjing Dong, Dongdong Wang, Chenggang Wang, Xijin Xu, Zhiguo Hou, Jian Yang
Aqueous Zn-metal batteries are of great interest due to their high material abundance, low production cost, and excellent safety. However, they suffer from severe side reactions and notorious dendrite growth closely related to electrolytes. Here, in-situ generated zwitterionic polymers are used as gel electrolytes to overcome these problems. It is shown that anions and H2O, but not anions and cations
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Chiral Au@CeO2 Helical Nanorods with Spatially Separated Structures for Polarization-dependent N2 Photofixation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Fang Wang, Weimin Yang, Qi Ding, Xinhe Xing, liguang xu, Hengwei Lin, Chuanlai Xu, Si Li
Chiral photocatalytic nanomaterials possess numerous unique properties and hold promise for various applications in chemical synthesis, environmental protection, energy conversion, and photoelectric devices. Nevertheless, it is uncommon to develop effective means to enhance the asymmetric catalytic performances of chiral plasmonic nanomaterials. In this study, a type of L/D-Au@CeO2 helical nanorods
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Dinuclear Cyclometalated Pincer Nickel(II) Complexes with Metal-Metal-to-Ligand Charge Transfer Excited States and Near-Infrared Emission Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Mengyue Gao, Wai-Pong To, Glenna So Ming Tong, Lili Du, Kam-Hung Low, Zhou Tang, Wei Lu, Chi-Ming Che
Facile non-radiative decay of low-lying metal-centered (MC) d-d excited states has been well documented to pose a significant obstacle to the development of phosphorescent NiII complexes due to substantial structural distortions between the d-d excited state and the ground state. Herein, we prepared a series of dinuclear Ni2II,II complexes by using strong σ-donors, carbene-phenyl-carbene (CNHC^Cphenyl^CNHC)
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Inverse Design of Singlet Fission Materials with Uncertainty-Controlled Genetic Optimization Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Luca Schaufelberger, Jacob Terence Blaskovits, Ruben Laplaza, Kjell Jorner, Clemence Corminboeuf
Singlet fission has shown potential for boosting the power conversion efficiency of solar cells, but the scarcity of suitable molecular materials hinders its implementation. We introduce an uncertainty-controlled genetic algorithm (ucGA) based on ensemble machine learning predictions from different molecular representations that concurrently optimizes excited state energies, synthesizability, and singlet
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The Key Descriptors for Predicting the Exciton Binding Energy of Organic Photovoltaic Materials Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Lingyun Zhu, Miaofei Huang, Guangchao Han, Yuanping Yi, Zhixiang Wei
Exciton binding energy (Eb) is a key parameter to determine the mechanism and performance of organic optoelectronic devices. Small Eb benefits to reduce the interfacial energy offset and the energy loss of organic solar cells. However, quantum-chemical calculations of the Eb in solid state with considering electronic polarization effects are extremely time-consuming. Furthermore, current studies lack
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Rectifying Heterointerface Facilitated C-N Coupling Dynamics Enables Efficient Urea Electrosynthesis Under Ultralow Potentials Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Mingyu Cheng, Shao Wang, Zechuan Dai, Jing Xia, Bocheng Zhang, Pingyi Feng, Yin Zhu, Yangyang Zhang, Genqiang Zhang
Electrocatalytic C-N coupling for urea synthesis from carbon dioxide (CO2) and nitrate (NO3-) offers a sustainable alternative to the traditional Bosch-Meiser method. However, the complexity of intermediates in co-reduction hampers simultaneous improvement in urea yield and Faradaic efficiency (FE). Herein, we developed a Cu/Cu2O Mott-Schottky catalyst with nanoscale rectifying heterointerfaces through
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Modulating the Inner Helmholtz Plane towards Stable Solid Electrolyte Interphase by Anion-π Interactions for High-Performance Anode-Free Lithium Metal Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Shaobo Ma, Jingteng Zhao, Huang Xiao, Qixin Gao, Fang Li, Congying Song, Guoxing Li
Anode-free lithium (Li) metal batteries (AFLBs) featured high energy density are viewed as the viable future energy storage technology. However, the irregular Li deposition and unstable solid electrolyte interphase (SEI) on anode current collectors reduce their cycling performance. Here, we propose a concept of anion-recognition electrodes enabled by anion-π interactions to regulate the inner Helmholtz
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Stapled Peptides as Inhibitors of mRNA Deadenylation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Sunit Pal, Ilja Gordijenko, Stefan Schmeing, Somarghya Biswas, Yasemin Akbulut, Raphael Gasper, Peter 't Hart
Therapeutic intervention targeting mRNA typically aims at reducing the levels of disease-causing sequences. Achieving the opposite effect of blocking the destruction of beneficial mRNA remains underexplored. The degradation of mRNA starts with the removal of poly(A) tails reducing their stability and translational activity which is mainly regulated by the CCR4-NOT complex. The subunit NOT9 binds various
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Allylic Epoxides Increase the Strain Energy of Cyclic Olefin Monomers for Ring-Opening Metathesis Polymerization Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Kyle R. Sylvester, Jessa R. Zovinka, Maya L. Milrod, Alexandra K. Stubin, Angela Rojas-Merchan, Kayla Alexander, Benjamin Ross Elling
Ring-opening metathesis polymerization (ROMP) is an effective method for synthesizing functional polymers, but since the technique typically relies on high ring strain cyclic olefins, the most common monomers are norbornene derivatives. The reliance on one class of monomer limits the obtainable properties of ROMP polymers. In this work, we investigate new bicyclic monomers synthesized via epoxidation
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Stereocontrolled Hydrogenation of Conjugated Enones to Alcohols via Dual Iridium-Catalysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Jia Zheng, Bram B. C. Peters, Rajendra K. Mallick, Pher G. Andersson
The concept of dual catalysis is an emerging area holding high potential in terms of preparative efficiency, yet faces severe challenges in compatibility of reaction conditions and interference of catalysts. The transition-metal catalyzed stereoselective hydrogenation of olefins and ketones typically proceeds under different reaction conditions and/or uses a different reductant. As a result, these
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Ligand-Insertion Strategy for Constructing 2D Conjugated Metal-Organic Framework with Large Pore Size for Electrochemical Analytics Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Xiu-Zhen Wang, Yue Chen, Xiao-Min Cao, Ru-Yi Li, Wei-Yan Chen, Yue Li, Dong-Sheng Guo
Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have shown great promise in various electrochemical applications due to their intrinsic electrical conductivity. A large pore aperture is a favorable feature of this type of material because it facilitates the mass transport of chemical species and electrolytes. In this work, we propose a ligand insertion strategy in which a linear ligand
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Visible-Light-Driven Solid-State Fluorescent Photoswitches for High-Level Information Encryption Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Zhiyuan Han, Meixia He, Gang Wang, Jean-Marie Lehn, Quan Li
Developing visible-light-driven fluorescent photoswitches in solid state remains an enormous challenge in smart materials. Such photoswitches are obtained from salicylaldimines through excited-state intramolecular proton transfer (ESIPT) and subsequent cis-trans isomerization strategies. By incorporating a bulky naphthalimide fluorophore into Schiff base, three photoswitches achieve dual-mode changes
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f-π* Back Bonding Orbital Induced by Lutetium-Based Conducting MOF Promotes Highly Selective CO 2 to CH 4 at Low Potential Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Fuqing Yu, Guangyao Zhang, Minxing Shu, Hongming Wang
The research on electrocatalytic carbon dioxide reduction (ECR) catalysts using renewable energy is particularly crucial in energy conversion studies, especially for viable hydrocarbon production. This study employs density functional theory calculations to screen a series of non-radioactive lanthanide two-dimensional metal-organic frameworks (MOFs) for product selectivity in ECR. Based on theoretical
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An Automated Electrochemical Flow Platform to Accelerate Library Synthesis and Reaction Optimization Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Eduardo Rial-Rodríguez, Jason D. Williams, David Cantillo, Thomas Fuchß, Alena Sommer, Hans-Michael Eggenweiler, C. Oliver Kappe, Gabriele Laudadio
Automated batch and flow reactors are well-established for high throughput experimentation in both thermal chemistry and photochemistry. However, the development of automated electrochemical platforms is hindered by cell miniaturization challenges in batch and difficulties in designing effective single-pass flow systems. In order to address these issues, we have designed and implemented a new, slug-based
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Chemo-Enzymatic Depolymerization of Functionalized Low-Molecular-Weight Polyethylene Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Uwe Bornscheuer, Thomas Oiffer, Friedemann Leipold, Philipp Süss, Daniel Breite, Jan Griebel, Muhammad Khurram, Yannick Branson, Erik de Vries, Agnes Schulze, Christiane A. Helm, Ren Wei
Polyethylene (PE) is the most commonly used plastic type in the world, contributing significantly to the plastic waste crisis. Microbial degradation of PE in natural environments is unlikely due to its inert saturated carbon-carbon backbones, which are difficult to break down by enzymes, challenging the development of a biocatalytic recycling method for PE waste. Here, we demonstrated the depolymerization
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Investigating Competing Inner- and Outer-Sphere Electron-Transfer Pathways in Copper Photoredox-Catalyzed Atom-Transfer Radical Additions: Closing the Cycle Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Le Nhan Pham, Angus Olding, Curtis C. Ho, Alex C. Bissember, Michelle L. Coote
This integrated computational and experimental study comprehensively examines the viability of competing inner-sphere electron transfer (ISET) and outer-sphere electron transfer (OSET) processes in [Cu(dap)2]+-mediated atom-transfer radical additions (ATRA) of olefins and CF3SO2Cl that can deliver both R–SO2Cl and R–Cl products. Five sterically- and electronically-varied representative alkenes were
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Oriented Titanium-MOF Membrane for Hydrogen Purification Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Sujing WANG, Sixing Chen, Mohammad Wahiduzzaman, Taotao Ji, Yi Liu, Yang Li, Chen Wang, Yanwei Sun, Gaohong He, Guillaume Maurin, Yi Liu
Precise hydrogen sorting from purge gas (H2/N2) and coke gas (H2/CH4), commonly carried out by cryogenic distillation, still suffers from low separation efficiency, high energy consumption, and considerable capital cost. Though still in its infancy, membrane technology offers a potential to achieve more efficient hydrogen purification. In this study, an optimum separation of hydrogen towards both methane
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Rational Construction of Cyanide-Functionalized D-A-π-D Covalent Organic Framework for Highly Efficient Overall H2O2 Photosynthesis from Air and Water Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Liecheng Guo, Lele Gong, Yuting Yang, Zhecheng Huang, Xing Liu, Feng Luo
Sacrificial-agent-free overall photosynthesis of H2O2 from water and air represents currently a promising route to reform the industrial anthraquinone production manner, but, still blocks by the requirement of pure O2 feedstock, due to the insufficient oxygen supply from water under air. Herein, we report a rational molecule design on COFs (covalent organic frameworks) equiped with cyanide-functionalized
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Front Cover: Transforming Red Phosphorus Photocatalysis: Dual Roles of Pre-Anchored Ru Single Atoms in Defect and Interface Engineering Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Junwei Bian, Wei Zhang, Yun Hau Ng, Zhuofeng Hu, Zhen Wei, Yuxi Liu, Jiguang Deng, Hongxing Dai, Lin Jing
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Inside Front Cover: Mitigating Intraphase Catalytic-Domain Transfer via CO2 Laser for Enhanced Nitrate-to-Ammonia Electroconversion and Zn-Nitrate Battery Behavior Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Yeryeong Lee, Jayaraman Theerthagiri, Nuttapon Yodsin, Ahreum Min, Cheol Joo Moon, Siriporn Jungsuttiwong, Myong Yong Choi
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Front Cover: Programmable Chemical Evolution with Natural/non-natural Building Blocks Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Ping Liu, Refeya Jannatul, Juan Chen, Lihua Hou, Mingjuan Gao, Pengjie Wang, Lulu Wang, Dekui Jin, Hao Chen, Rong Liu, Ran Wang, Yinhua Zhu, Bing Fang, Lirong Jia, Yanan Sun, Yixin Zhang, Fazheng Ren, Weilin Lin
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Front Cover: Allostery at a Protein-Protein Interface Harboring an Intermolecular Motional Network Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Sara Medina Gomez, Tye I. Gonzalez, Suresh K. Vasa, Rasmus Linser
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Inside Front Cover: Dissecting Exciton Dynamics in pH-Activatable Long-Wavelength Photosensitizers for Traceable Photodynamic Therapy Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Yurong Liu, Jing Zhang, Xuan Zhou, Yaru Wang, Shan Lei, Guangle Feng, Dong Wang, Peng Huang, Jing Lin
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Correspondence on “Visible-Light-Switchable Chalcone-Flavylium Photochromic Systems in Aqueous Media” Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-23 Nuno Basílio, A. Jorge Parola, Fernando Pina
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Inside Back Cover: Dissolution‐Recrystallization: A Novel Mechanism for Fluorochromic Detection of Th4+ Using Color‐Tunable Luminescent Metal‐Organic Frameworks Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Yunyi Cui, Huangjie Lu, Huiliang Hou, Yaoyao Bai, Junpu Yang, Yarui Li, Jie Qiu, Shuao Wang, Jian Lin
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Inside Back Cover: Coumarin‐Based Photodegradable Hydrogels Enable Two‐Photon Subtractive Biofabrication at 300 mm s‐1 Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-25 Wanwan Qiu, Christian Gehre, Jaime Pietrantuono Nepomuceno, Yinyin Bao, Zhiquan Li, Ralph Müller, Xiao‐Hua Qin
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Classifieds: Jobs and Awards, Products and Services Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24
Are you looking for a (new) job? Do you know someone who deserves an award? Are you trying to find a product or service to make your work more efficient? Our partners can help.
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Achieving Controllable Thermochromic Fluorescence via Synergistic Intramolecular Charge Transfer and Molecular Packing Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Weixu Feng, Sumin Lu, Yanhui Wu, Xiaotian Li, Dong Han, Yan Zhao, Wei Tian, Hongxia Yan
Thermochromic fluorescent materials (TFMs) have attracted significant attention due to their unique fluorescent colorimetric response to temperature. However, existing TFMs still suffer from weak stimulus responsiveness, broad temperature response ranges, uncontrollable emission color changes, and low quantum yields. In this study, we address these issues by designing and synthesizing three diketone-boron
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Boron-Doped Single-Molecule van der Waals Diode Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Yu-Ling Zou, Wenting Sun, Jiao Xun, Qing-Man Liang, Lichuan Chen, Tong-Ruo Diao, Jia Shi, De-Yin Wu, Chuandong Dou, Wenjing Hong, Zhong-Qun Tian, Yang Yang
Single-molecule diode was the first proposed device in molecular electronics. Despite the great efforts and advances over 50 years, the reported rectification ratios, the most critical parameter of a diode, remain moderate for the single-molecule diode. Herein, we report an approach to achieve a larger rectification ratio by adopting the combined strategies of p-type boron doping, the single-layer
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Drug Discovery and Screening Tool Development for Tauopathies by Focusing on Pathogenic Tau Repeat 3 Oligomers Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Soljee Yoon, Hye Yun Kim, Sohui Park, Minhae Cha, Kyeonghwan Kim, Songmin Lee, JiMin Kim, Saeyun Bhang, YoungSoo Kim
Comprehending early amyloidogenesis is essential for the development of effective therapeutic strategies. In tauopathies like Alzheimer’s disease (AD), the abnormal accumulation of tau protein is initiated by pathological tau seeds. Mounting evidence implies that the microtubule binding domain, consisting of three to four repeats, plays a pivotal role in this process, yet the exact region driving the
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Pairing Oxygen Reduction and Water Oxidation for Dual−pathway H2O2 Production Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-23 Xin Sun, Jindi Yang, Xiangkang Zeng, Lijun Guo, Chuanbiao Bie, Zhuyuan Wang, Kaige Sun, Aloka Kumar Sahu, Mike Tebyetekerwa, Thomas E. Rufford, Xiwang Zhang
Hydrogen peroxide (H2O2) is a crucial chemical applied in various industry sectors. However, the current industrial anthraquinone process for H2O2 synthesis is carbon-intensive. With sunlight and renewable electricity as energy inputs, photocatalysis and electrocatalysis have great potential for green H2O2 production from oxygen (O2) and water (H2O). Herein, we review the advances in pairing two-electron
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Bidentate Coordination Enables Anions‐Regulated Solvation Structure for Advanced Aqueous Zinc Metal Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Dongdong Wang, Rui Li, Jingjing Dong, Zhongchao Bai, Nana Wang, Shi Xue Dou, Jian Yang
Rechargeable aqueous Zn metal batteries (AZMBs) are attractive for stationary energy storage due to their low cost and high safety. However, their practical application is hindered by the excessive use of zinc anodes and poor high‐temperature performance, caused by severe side reactions and dendritic growth issues. Here, an electrolyte design strategy is reported based on bidentate coordination of
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Cross‐Coupling of Gaseous Alkanes with (Hetero)Aryl Bromides via Dual Nickel/Photoredox Catalysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Akshay M. Nair, Pol Martínez-Balart, Sergio Barbeira-Arán, Martín Fañanás-Mastral
Gaseous alkanes represent the most abundant carbon‐based chemical feedstocks in our planet. However, the intrinsic inertness of their C‐H bonds has rendered the use of these alkanes very difficult for purposes beyond aerobic combustion and energy intensive processes. Thus, clean and energy‐efficient transformations for their use in synthetic organic chemistry are still rare. Here we report a catalytic
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Visualizing Active Sites in Electrospun Photoactive Membranes via Fluorescence Lifetime Imaging Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Anzhela Galstyan, Fabian Terlau, Hanna M. Martin
Interest in antibacterial nanomaterials has surged in recent years, driven by the rise in antibiotic resistance among microbes. However, their practical application remains limited because many crucial properties have yet to be thoroughly investigated. In this study, we have developed novel nanofibrous membranes based on hydrophilic polyacrylonitrile (PAN) or hydrophobic polycaprolactone (PCL) with
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Harnessing 4f Electron Itinerancy for Integrated Dual‐Band Redox Systems Boosts Lithium‐Oxygen Batteries Electrocatalysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Mengyao Huang, Lina Song, Nan Wang, Yaning Fu, Rongchang Ren, Zhongjun Li, Youcai Lu, Jijing Xu, Qing-chao Liu
In‐depth comprehension and manipulation of band occupation at metal centers are crucial for facilitating effective adsorption and electron transfer in lithium‐oxygen battery (LOB) reactions. Rare earth elements play a unique role in band hybridization due to their deep orbitals and strong localization of 4f electrons. Herein, we anchor single Ce atoms onto CoO, constructing a highly active and stable
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Development of DuoMYC: a synthetic cell penetrant miniprotein that efficiently inhibits the oncogenic transcription factor MYC Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Brecht D. Ellenbroek, Jan Pascal Kahler, Damiano Arella, Cherina Lin, Willem Jespers, Eliane Ann-Katrin Züger, Micha Drukker, Sebastian J. Pomplun
The master regulator transcription factor MYC is implicated in numerous human cancers, and its targeting is a long‐standing challenge in drug development. MYC is a typical ‘undruggable’ target, with no binding pockets on its DNA binding domain and extensive intrinsically disordered regions. Rather than trying to target MYC directly with classical modalities, here we engineer synthetic miniproteins
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An Expedient Route to Bio‐based Polyacrylate Alternatives with Inherent Degradation Capabilities by Organic Catalysis for Polymerization of Muconate Esters Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Daniel Taton, Thomas Dardé, Emilie Diomar, Schultze Xavier
The quest for polymers that would be at the same time bio‐based and degradable after usage, in addition to offering chemical post‐modification options, remains a daunting challenge in contemporary polymer science. Despite advances in polymer chemistry, attempts at controlling the chain‐growth polymerization of muconate esters remain unexplored. Here we show that dialkyl muconates can be rapidly polymerized
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Thermally‐stable single‐site Pd on CeO2 catalyst for selective amination of phenols to aromatic amines without external hydrogen Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Yaqin Wang, Bingfeng Chen, Lina Li, Xuelei Mei, Yucheng Gu, Haihong Wu, Mingyuan He, Buxing Han
Developing a new route to produce aromatic amines as key chemicals from renewable phenols is a benign alternative to current fossil‐based routes like nitroaromatic hydrogenation, but is challenging because of the high dissociation energy of the Ar‐OH bond and difficulty in controlling side reactions. Herein, an aerosolizing‐pyrolysis strategy was developed to prepare high‐density single‐site cationic
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Orderly Coating of Bilayer Polymer to Tailor Microenvironment for Efficient C‐N Coupling Toward Highly Selective Urea Electrosynthesis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Zhichao Wang, Mengfan Wang, Qiyang Cheng, Yanzheng He, Sisi Liu, Jie Liu, Xiaolei Yuan, Yunfei Huan, Tao Qian, Chenglin Yan
Electrosynthesis of urea from co‐reduction of carbon dioxide and nitrate is a promising alternative to the industrial process. However, the overwhelming existence of proton and nitrate as well as the insufficient supply of CO2 at the reaction interface usually result in complex product distributions from individual nitrate reduction or hydrogen evolution, instead of C‐N coupling. In this work, we systematically
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p‐Block Metal Based Single‐Atom Catalysts Surpass Transition‐Metal Counterparts in Photocatalytic H2O2 Production Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Haijiao Lu, Hanqing Yin, Jeffrey Harmer, Mu Xiao, Jiakang You, Peng Chen, Tongen Lin, Aijun Du, Zhiliang Wang, Lianzhou Wang
Growing interest in p‐block metal single‐atom catalysts (PM‐SACs) is driven by their low toxicity, economic viability, and transition metal‐like catalytic properties. However, selection criteria for p‐block single‐atom species and catalytic mechanisms of PM‐SACs remain unclear. This study explores the catalytic abilities of PM‐SACs and their transition metal counterparts (TM‐SACs) based on polymetric
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Synergize Strong and Reactive Metal‐Support Interactions to Construct Sub‐2 nm Metal Phosphide Cluster for Enhanced Selective Hydrogenation Activities Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Zemin Chen, Xinyu Li, Guangyue Xu, Tianci Xiao, Dechen Wang, Chufei Wang, Kaihang Zhang, Jiong Li, Yang Pan, Yan Qiao, Ying Zhang
Strong metal‐support interactions (SMSI) are crucial for stabilizing sub‐2 nm metal sites, e.g. single atom (M1) or cluster (Mn). However, further optimizing sub‐2 nm sites to break the activity–stability trade‐off due to excessive interactions remains significant challenges. Accordingly, for the first time, we propose synergizing SMSI with reactive metal‐support interactions (RMSI). Comprehensive
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A Green and Efficient Electrocatalytic Route for the Highly‐Selective Oxidation of C–H Bonds in Aromatics over 1D Co3O4‐Based Nanoarrays Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Zhaohui Yin, Zirui Gao, Lan Luo, Xiaohui Zhang, Wenxiang Hou, Wenjing Dai, Shuheng Tian, Xuetao Qin, Maolin Wang, Mi Peng, Kaihua Li, Songbo Wang, Lei Zhang, Hong Wang, Jianxin Li, Qingjun Zhu, Bowen Cheng, Zhen Yin, Ding Ma
Electrocatalytic oxidation of C‐H bonds in hydrocarbons represents an efficient and sustainable strategy for the synthesis of value‐added chemicals. Herein, a highly selective and continuous‐flow electrochemical oxidation process of toluene to various oxygenated products (benzyl alcohol, benzaldehyde, and benzyl acetate) is developed with the electrocatalytic membrane electrodes (ECMEs). The selectivity
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Catalytic Edges in One‐Dimensional Covalent Organic Frameworks for the Oxygen Reduction Reaction Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Yumeng Chang, Chao Lin, Haifeng Wang, Xiaotong Wu, Luyao Zou, Jixin Shi, Qi Xiao, Qing Xu, Xiaopeng Li, Wei Luo
Metal‐free covalent organic frameworks (COFs) are employed in oxygen reduction reactions (ORR) because of their diverse structural units and controllable catalytic sites, and the edge sites have high catalytic activity than the basal sites. However, it is still challenge to modulate the edge sites in COFs, because the extended frameworks in two‐ or three‐dimensional topologies resulted in limited edge
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Nanohoops Favour Light‐Induced Energy Transfer over Charge Separation in Porphyrin/[10]CPP/Fullerene Rotaxanes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Fabian Schwer, Simon Zank, Markus Freiberger, Fabian M. Steudel, Niklas Geue, Lei Ye, Perdita E. Barran, Thomas Drewello, Dirk Guldi, Max von Delius
[2]Rotaxanes offer unique opportunities for studying and modulating charge separation and energy transfer, because the mechanical bond allows the robust, yet spatially dynamic tethering of photoactive groups. In this work, we synthesized [2]rotaxane triads comprising a central (aza)[10]CPP⊃C60 bis‐adduct complex and two zinc porphyrin stoppers to address how the movable nanohoop affects light‐induced
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Ion‐Pairing Chromonic Liquid Crystals via Alternately Stacked Assembly of Amphiphilic Charged π‐Electronic Systems Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Yuto Maruyama, Koji Harano, Hayato Kanai, Yasuhiro Ishida, Hiroki Tanaka, Shinya Sugiura, Hiromitsu Maeda
In this study, a new assembly strategy for lyotropic chromonic liquid crystals (LCLCs) is proposed using iπ–iπ interactions, mainly comprising electrostatic and dispersion forces, between charged π‐electronic systems to form stacking structures supported by the hydration of triethylene glycol (TEG) units. Meso‐TEG‐aryl‐substituted porphyrin AuIII complex, an amphiphilic π‐electronic cation, showed
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Electronic Response and Charge Inversion at Polarized Gold Electrode Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Linnéa Andersson, Michiel Sprik, Juerg Hutter, Chao Zhang
We have studied polarized Au(100) and Au(111) electrodes immersed in electrolyte solution by implementing finite‐field methods in density functional theory‐based molecular dynamics simulations. This allows us to directly compute the Helmholtz capacitance of electric double layer by including both electronic and ionic degrees of freedom, and the results turn out to be in excellent agreement with experiments
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Solid‐Liquid‐Gas Three‐Phase Indirect Electrolysis Enabled by Affinity Auxiliary Imparted Covalent Organic Frameworks Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Yi-Rong Wang, Ming Yue, Gang Liu, Jia-Li Zhang, Qi Li, Jing-Wen Shi, Jia-Yong Weng, Run-Han Li, Yifa Chen, Shun-Li Li, Ya-Qian Lan
The design of efficient heterogenous redox mediators with favorable affinity to substrate and electrolyte are much desired yet still challenging for the development of indirect electrolysis system. Herein, for the first time, we have developed a solid‐liquid‐gas three‐phase indirect electrolysis system based on a covalent organic framework (Dha‐COF‐Cu) as heterogenous redox mediator for S‐S coupling
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Hollow Hydrogels for Excellent Aerial Water Collection and Autonomous Release Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-24 Lidong Zhang, Shumin Liang, Marieh Al Handawi, Tao Chen, Panče Naumov
Air moisture is a valuable and omnipresent resource of fresh water. However, traditional water collectors come with an enduring problem of the water‐release step, which requires special devices and additional energy to remove the water from the adsorbent, such as heat, sunlight, or both. Herein, we report the first composite conical hollow hydrogel to harvest water from aerial humidity. This hollow
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Molecular Photoswitching Unlocks Glucose Oxidase for Synergistically Reinforcing Fenton Reactions for Antitumor Chemodynamic Therapy Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-23 Zhiyuan Tian, Zicheng Wang, Weier Bao, Baerlike Wujieti, Ming Liu, Xiaojuan Li, Zhecheng Ma, Wei Cui
We have developed a new type of nanoparticles with potent antitumor activity photoactivatable via the combination of molecular photoswitching of spiropyran (SP) and enzymatic reaction of glucose oxidase (GOx). As two key processes involved therein, Fe(III)‐to‐Fe(II) photoreduction in Fe(III) metal‐organic frameworks (MOFs) brings about the release of free Fe2+/Fe3+ while the photoswitching of SP to
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Atmosphere Induces Tunable Oxygen Vacancies to Stabilize Single‐Atom Copper in Ceria for Robust Electrocatalytic CO2 Reduction to CH4 Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2024-09-23 Fang Huang, Xiangyu Chen, Huanhuan Sun, Qingduo Zeng, Junjie Ma, Dong Wei, Jinliang Zhu, Zhengjun Chen, Taoyuan Liang, Xucai Yin, Xijun Liu, Jing Xu, Huibing He
Electrochemical carbon dioxide reduction (ECO2RR) shows great potential to create high‐value carbon‐based chemicals, while designing advanced catalysts at the atomic level remains challenging. The ECO2RR performance is largely dependent on the catalyst microelectronic structure that can be effectively modulated through surface defect engineering. Here, we provide an atmosphere‐assisted low‐temperature