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Engineering a Proximity Biosensor via Constitutional Dynamic Chemistry Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Lu Gao, Ruiqi Zhang, Yanan Tang, Feng Li
Affinity binding-induced DNA assembly is a fundamental principle for designing proximity biosensors for sensitive and wash-free protein detection and imaging. However, current design strategies for these biosensors face an intrinsic trade-off between binding affinity and background signal. Here, we demonstrate that this intrinsic issue can be addressed by using constitutional dynamic chemistry as a
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Intrinsically Disordered Peptide Nanofibers from A Structured Motif within Proteins Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Yuchen Qiao, Ayisha Zia, Adrianna Shy, Grace Wu, Matthew Chu, Zhiyu Liu, Fengbin Wang, Bing Xu
Intrinsically disordered regions (IDRs) are ubiquitous in pro-teins, orchestrating complex cellular signaling through high-er-order protein assemblies. However, the properties and functions of intrinsically disordered peptide (IDP) assemblies are largely underexplored. This work unveiled a facile strategy for engineering IDP assemblies. We demonstrate that conjugating a structured motif derived from
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Organic Cage Encapsulated within Metal Cluster-Based Open Frameworks: A Single-Crystal Host-in-Host Material with Inter-Host Charge Cooperation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Zhao-Feng Wu, Jing-Wang Cui, Ke Zhao, Bin Tan, Si-Hua Liu, Xiao-Ying Huang, Jian-Ke Sun, Guo-Yu Yang
Integrating dissimilar building units of discrete organic cages and inorganic clusters into single-crystal supramolecular frameworks with tailored architectures and synergistic functions presents a significant challenge. Here, we presented our discovery of achieving such hybrids through electrostatically driven self-assembly of cationic ammonium organic cages with anionic lead iodide clusters. Notably
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Modular access to aliphatic polycarbonates with tunable properties and dual closed-loop recyclability by polycondensation−depolymerization−repolymerization strategy Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Bin Wang, Wei-Ning Liu, Mingqian Wang, Zhiqiang Ding, Yuesheng Li
Great achievements have been made in CO2/epoxide copolymerization and dialkyl carbonate/diol polycondensation, however, efficient preparation of high-molecular-weight (> 100 kDa) aliphatic polycarbonates with tunable properties and recyclability under mild conditions still remain as a great challenge. Herein, we presented a “polycondensation−depolymerization−repolymerization” strategy for structurally
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Triple Synergy Engineering via Metal-free Dual-Atom Incorporation for Self-sustaining Acidic Ammonia Electrosynthesis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Chuanzhen Feng, Kaiwen Bo, Jin Wan, Huijuan Zhang, Yu Wang
Electrochemical nitrate reduction reaction (NO3RR) for ammonia synthesis under acidic conditions offers significant advantages, like direct fertilizer production and prevention of ammonia volatilization. However, three critical challenges persist: instability of metal-based catalysts, competition from the hydrogen evolution reaction (HER), and proton depletion leading to species imbalance. Here, we
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Synergistic Effect of Boron and Oxygen Coordination on Ruthenium Clusters for Industrial Water Splitting in Alkaline Medium Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Huxu Lei, Weiwei Yang, Shengnan Hu, Luocai Yi, Chuanming Ma, Chengsi Hu, Fangren Qian, Ming Zhao, Lei Liu, Guangzhi Yang, Qingjun Chen
The alteration in the coordination environment of metal atoms can manipulate their electronic structure and regulate the electrocatalytic hydrogen evolution activity. In this work, the coordination environment of ruthenium clusters was successfully modulated by introducing the appropriate boron (B) and oxygen (O) elements into the reduced graphene oxide host. The electrochemical tests demonstrate that
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Anchoring Highly Unsaturated Nickel(II) Sites into a Metal–Organic Framework for Simultaneous High C2H2 Adsorption and Separation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Yi-Zhan Hao, Hui-Min Wen, Yi-Hong Yu, Xu Zhang, Yuanjing Cui, Banglin Chen, Bin Li, Guodong Qian
Separation of acetylene (C2H2) from carbon dioxide (CO2) remains a challenge to achieve both high C2H2 uptake and selectivity for a single material. Porous materials with routine OMSs often show the limitation in C2H2/CO2 separation due to the comparable binding affinity with the two gases. Herein, we report a new strategy of anchoring highly unsaturated nickel(II) sites into a large-pore MOF (Ni
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Harnessing Lithium-Mediated Green Ammonia Synthesis with Water Electrolysis Boosted by Membrane Electrolyzer with Polyoxometalate Proton Shuttles Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Jun Miao, Cailing Chen, Li Cao, Reham Al Nuaimi, Zhen Li, Kuo-Wei Huang, Zhiping Lai
Integrating water electrolysis (WE) with lithium-mediated nitrogen reduction (Li-NRR) offers a sustainable route for green ammonia production by directly utilizing protons from water oxidation, eliminating reliance on grey or blue hydrogen. Here, polyoxometalates (POMs) function as electron-coupled proton buffers (ECPBs) to seamlessly link WE with Li-NRR in a three-compartment flow reactor comprising
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Enhancing the Built-in Electric Field of Thickness-Insensitive Small Molecule Cathode Interlayers for High-Efficiency and Stable Organic Solar Cells Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Yuxing Wang, Junjie Wen, Zhe Shang, Yanyi Zhong, Huixiang Zhang, Wenxu Liu, Wentian Han, Huanhuan Yang, Jiming Liu, Jiangbin Zhang, Hui Li, Yao Liu
The built-in electric field (BEF) is proposed as a critical design parameter for optimizing small-molecule cathode interlayer materials (SM-CIMs) in organic solar cells (OSCs). By strategically transforming imidazole-functionalized triads from a D-A-D to an A-D-A configuration and replacing the A unit with a more electron-deficient moiety, we developed three triads: (TBT)2NDI, (NDI)2TBT, and (PDI)2TBT
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Atomic Heterointerface Engineering and Non-Equilibrium Carrier Dynamics for Enhanced Photocatalysis in Halide Perovskite/MoS2 Systems Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Shaomin Peng, Changhai Guo, Jia Guo, Wei Song, Ming Sun, Guichuan Xing, Lin Yu
Solar-driven photocatalysis holds promise for fuel production, with halide perovskites leading owing to superior light absorption and carrier diffusion. However, precise control and understanding of interfacial charge separation dynamics in their heterostructures remain challenging. Using formamidinium lead bromide/molybdenum disulfide (FAPbBr3/MoS2) as a model, we engineered Pb-rich, Pb-neutral, and
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Cost-Effective and Low-Carbon Scalable Recycling of Waste Polyethylene Terephthalate Through Bio-Based Guaiacol-Enhanced Methanolysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Yunkai Yu, Yufei Zhang, Siming Zhu, Qingqing Mei
The global plastic waste crisis, particularly from polyethylene terephthalate (PET), demands sustainable recycling solutions. PET methanolysis offers a promising route to recover high-purity dimethyl terephthalate (DMT), but achieving scalable, cost-effective, and environmentally friendly processes under mild conditions remains challenging. This study introduces a bio-based catalytic system using guaiacol
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Oscillatory Strong Metal-Support Interaction in Pd/TiO2 under Redox Conditions Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Yuhui Chen, Jinting Hao, Kai Zhang, Songda Li, Zhongkang Han, Wentao Yuan, Ying Jiang, Ze Zhang, Yong Wang
Strong metal-support interaction (SMSI) plays a crucial role in catalysis, with its encapsulation configuration being highly dependent on the chemical environments. However, the dynamic behavior of SMSI under redox conditions remains insufficiently understood. Here, environmental transmission electron microscopy (ETEM) revealed that SMSI overlayers form stably on the surface of Pd/TiO2 nanocatalysts
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Bimetallic Designing Based on the Nucleation Rate of Prussian Blue Analogues for Enhanced Aqueous Zinc Ions Batteries with Glycerol-Water Hybrid Electrolytes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Biao Yang, Yuxin Shi, Gongjing Song, Chengang Pei, Yan Yan, Zhidong Chen, Huan Pang
A magical heterostructures of M-PBAs (M= Co, Cu, and Zn) encapsulated by V-PBA have been successfully obtained by a facile one-pot coprecipitation method based on the difference in the binding energies of between these metal ions and ligands, and the nucleation rates of different M-PBAs. Hence, due to the multiple redox pairs, open frameworks, ordered channels, and synergistic effect of two components
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Inverted Chiroptical Properties of Hybrid Metal Halides through Reversible Chiral Induction Driven by External and Internal Chirality Transfer Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Junjie Guan, Wenqing Han, Youpei Zhang, Jiuzhou Zhao, Shanshan Han, Yue Wang, Bona Fu, Hanwen Kang, Peihan Wang, Puxin Cheng, Yongshen Zheng, Jialiang Xu, Xian-He Bu
Chiral organic-inorganic hybrid metal halides (OIHMHs) are commonly constructed by introducing pairs of enantiomorphic chiral precursors through a single chirality transfer pathway, which may limit the regulation of chiral structrual diversity and chiroptoelectronic properties. Herein, we propose a new strategy for achieving reversible chiral induction of OIHMHs with inverted chiroptical properties
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A Biodegradable Radical Polymer Enables High-Performance, Physically Transient Organic Memory Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-28 Jaehyoung Ko, Soeun Kim, Daeun Kim, Taeho Lim, Soyeong Jin, Youngdo Jeong, Yongho Joo, Sangho Cho
Electronic devices often demand high reliability and longevity, but they also contribute significantly to electronic waste. Physically transient electronics have thus emerged as a promising alternative in future electronics, particularly in wearable and implantable bioelectronics. In these applications, memristive materials have gained significant attention for their potential to realize neuromorphic
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Promoting Alkane Binding: Crystallization of a Cationic Manganese(I)-Pentane σ-Complex from Solution Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-27 Malte Sellin, James Duncan Watson, Julia Fischer, Graham Edwin Ball, Leslie David Field, Ingo Krossing
Transition metal–alkane σ-complexes are key intermediates in C-H activation and, until now, analysis of these species has been restricted to either the solution OR the solid state. Here we present a synthetic methodology that converts Mn2(CO)10 in a non-coordinating solvent environment to [Mn(CO)5]+ at room temperature, and this species binds n-pentane as the strongest interacting ligand available
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Enhancing Waste Plastic Hydrogenolysis on Ru/CeO2 through Concurrent Incorporation of Fe Single Atoms and FeOx Nanoclusters Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-27 Xiaomei Wang, Rui Zhang, Xueting Wu, Yuou Li, Zijian Wang, Meng Zhao, Shuyan Song, Hongjie Zhang, Xiao Wang
Ru-based catalysts have exhibited significant promise in converting waste plastics into valuable long-carbon chain products. However, their efficiency is hindered by the uncontrollable cascade hydrogenation, which stems from their exceptional reactivity for C-C cleavage. Herein, we reported a multi-scale regulation strategy by selectively anchoring Fe single atoms (SAs) and FeOx nanoclusters (NCs)
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p-p Orbital Hybridization Stabilizing Lattice Oxygen in Two-dimensional Amorphous RuOx for Efficient Acidic Oxygen Evolution Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-27 Yajing Mu, Dantong Zhang, Tianyi Gao, Lina Wang, Lei Zhang, Xiaoxin Zou, Weitao Zheng, Jinchang Fan, Xiaoqiang Cui
Developing efficient Ru-based catalysts is crucial in reducing reliance on costly Ir for the acidic oxygen evolution reaction (OER). However, these Ru-based catalysts face a fundamental stability challenge due to the highly reactive nature of lattice oxygen. In this work, we propose an effective strategy to stabilize lattice oxygen in two-dimensional amorphous RuOx through p-p orbital hybridization
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Integrative Lattice and Surface Engineering of Nanoscale Fe0 for Superior Dechlorination of Trichloroethene in Groundwater: Coordination in Reactivity, Selectivity and Stability Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-27 Feilong Gao, Guofang Xu, Mingyi Zhang, Honghong Lyu, Han Wu, Jingchun Tang, Xinhua Xu, Jianzhong He
Nanoscale zero-valent iron (nFe0) materials hold great promise in environmental remediation, yet achieving high reactivity, selectivity, and stability in reduction remains a long-standing challenge. Here, we address this challenge by innovatively employing Ni lattice and FeS surface engineering to fabricate novel nFe0-based nanomaterials (dubbed as FeNix@FeSy), featuring FeNi as the core and FeS as
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Iron-Doped Cobalt Molybdate Enhanced Electrochemiluminescence Imaging for Dynamic Multilevel Information Encryption System Construction and Biomarker Sensing Analysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-27 Jingui Chen, Tingting Wu, Yu Du, Huaiqing Zhao, Dan Wu, Hongmin Ma, Zhong Feng Gao, Xiang Ren, Qin Wei
Integrating electrochemiluminescence (ECL) imaging with a multilevel information encryption strategy overcomes the limitations of conventional encryption methods, which rely solely on abstract electrical signals, by providing intuitive visual outputs. Herein, a dynamic multilevel information encryption system based on ECL imaging was successfully constructed, which realizes robust protection and precisely
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Catalytic Enantioselective Reductive Arylation and Alkenylation of Sulfinylamines to Access Sulfinamides Enabled by Cobalt Catalysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-27 Junfeng Yang, Yin Yuan, Xinyu Tian, Hongxia Zheng, Yuze Li, Junliang Zhang
This study reports a cobalt-catalyzed enantioselective reductive arylation and alkenylation of sulfinylamines, facilitating the efficient synthesis of enantiopure sulfinamides. By employing a cobalt/chiral diphosphine and tridentate ligand system, a range of diverse aryl and alkenyl iodides were successfully transformed into sulfinamides, achieving high yields and excellent enantioselectivity. This
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Boosting Current Density of Electrocatalytic CO2 Reduction using Metal-Enzyme Hybrid Cathodes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-27 Yeomin Kang, Yunjae Kim, Youngjin Doh, Jinwoo Lee, Jungbae Kim, Ki Tae Park
As one of promising solutions to global warming, electrocatalytic reduction of carbon dioxide (CO2RR) to liquid fuel has attracted great attention. A primary challenges in industrializing CO2RR technologies for producing liquid fuel is the mass transfer limitation of CO2, which significantly reduces the current density of CO2RR. This study proposes a new enzyme-enhanced electrocatalysis platform for
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Synergistic Regulation of Multi-Interface Chemistry by Functional Carbon Dots for High-Performance Composite Solid Electrolytes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-21 Huaxin Liu, Fangjun Zhu, Yinghao Zhang, Yuming Liu, Yi Zhang, Wentao Deng, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji
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Restricting Two‐Electron Oxygen Reduction via Secondary Coordinated Sulfur Enabling Ultralong‐Lifespan Zn‐Air Batteries Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 Xiehong Cao, Wenxian Liu, Jinxiu Feng, Henan Wang, Pu Wang, Dong Zheng, Wenhui Shi, Fangfang Wu, Tianqi Deng
The direct four‐electron oxygen reduction reaction (4e− ORR) critically governs efficiency and lifespan in metal‐air batteries and fuel cells, yet selectively suppressing competitive 2e− and stepwise 2e− pathways that generate corrosive hydrogen peroxide remains a major challenge. Herein, we demonstrate the strategic incorporation of secondary coordinated sulfur atoms into transition metal‐N‐C electrocatalysts
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Natural Sunlight‐Driven Activation of Inert Aryl Halides Using Plasmonic Cu@CdS with Polysulfide Active Sites Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 Yuemei Li, Shi-Yu Guo, Hongfei Gu, BingYu Wang, Peiwu Su, Xiuming Zhang, Haoqing Zhang, Shuping Zhang, Fanzhi Yang, Jia Liu, Qing-An Chen, Jiatao Zhang
Visible light photoredox catalysis has become a rapidly emerging area owing to its potential of using sunlight to tame previously hard‐to‐harness radicals for organic synthesis. At present, such blueprint faces a significant challenge, namely how to accomplish thermodynamically demanding reactions with sunlight encompassing a wide range of low energy photons. Here, we report a new reaction framework
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Metal‐Controlled Enantiodivergent Tandem Rearrangement to Synthesize 2H‐Azirines Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 Zhendong Yang, Maoping Pu, Liangkun Yang, Yuqiao Zhou, Hongda Wu, Bosheng Wang, Xiaoming Feng, Xiaohua Liu
A metal‐controlled enantiodivergent rearrangement of α‐diazo‐β‐keto oxime ethers has been developed. Switching the metal catalyst from Co(II) to Fe(II) with an identical ligand completely reverses the asymmetric induction. Both enantiomers of chiral 2H‐azirines and its derivatives are accessible under thermal or photolytic conditions. The cobalt‐based reaction is highly efficient even at 0.05 mol%
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De‐novo Design of Structure‐tunable Multivalent Chimeras for Tumor‐Targeted PD‐L1 Degradation and Potentiated Cancer Immunotherapy Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 Huiling Zhou, Bo Hou, Yiming Shan, Lujia Huang, Fangmin Chen, Siyuan Ren, Shunan Zhang, Jiaxing Pan, Yijing Dang, Haijun Yu, Zhiai Xu
Targeted protein degradation (TPD) technology holds significant potential for modulating protein homeostasis and treating diseases. However, current methods for degrading membrane protein highly depend on the lysosome‐targeting ligands or membrane receptors. In this study, we present a set of multivalent targeting chimeras (multi‐TACs) for tumor‐specific degradation of programmed death ligand 1 (PD‐L1)
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Inside Back Cover: Readily Visualized Perfluorooctanoic Acid Detection Using a Small Molecule Chemosensor Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 Yu‐Dong Yang, Qian Zhang, Xingchen Jin, Calvin V. Chau, Jian Yang, Graeme Henkelman, Xiaodong Chi, Han‐Yuan Gong, Richard J. Hooley, Jonathan L. Sessler
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Halogen Bonding Enable Improved Performance and Stability of Dion‐Jacobson Perovskite Solar Cells Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 jifei wang, Nanliu Liu, Qingqing Zou, Ying Li, Guoting Li, Yan Chen, Rongzhou Liang, Sijin Liu, Shiwei Lu, WeiKe Wang, Bing Ji, Lili Ke, Guozheng Nie, Hongpeng Zhou, Biao Liu, Yaxin Zhai, Yuanyuan Guo
The undesired phase distribution and intrinsic residual lattice strain remain the bottleneck for high‐performance and stable two‐dimensional (2D) or Q‐2D perovskite solar cells (PSCs), especially for the Dion‐Jacobson (DJ) type Q‐2D PSCs. Here, we showcase employing halogen bonds to stabilize the halide anions and fine‐tuning the residual lattice strain by introducing perfluorodecyl iodide (PFI). It
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Day‐Long Organic Persistent Luminescence in Flexible Polymeric Materials Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 Longming Jin, Wanqi Mo, Ziyi Wang, Wei Hong
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Back Cover: Quantum Mechanical Tunnelling Probes With Redox Cycling for Ultra‐Sensitive Detection of Biomolecules Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 Long Yi, Tao Jiang, Ren Ren, Ji Cao, Joshua B. Edel, Aleksandar P. Ivanov, Longhua Tang
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Direct Synthesis of Poly(adipate)Esters via Catalytic Isomerizing Dual Hydroesterificative Polymerization of 1,3‐Butadiene Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-26 Jiawang Liu, Shen Gao, Lei Su, Xuehe Lu, Huiwen Yang, Jiaming Zou, Xi Yang, Shan Tang
Aliphatic polyesters, such as poly(adipate)esters, are attracting substantial attention as sustainable materials due to their degradability, recyclability, and versatility in various applications. However, the conventional production of poly(adipate)esters relies on energy‐intensive processes and petroleum‐derived adipic acid (AA), whose synthesis poses environmental concerns, including nitrous oxide
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Pyrazine‐Embedded Two‐Dimensional Conjugated Metal‐Organic Framework with Quasi‐Honeycomb Lattice for High‐Capacitance Lithium‐Ion Storage Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Xiangyu Li, Yangyang Feng, Shuai Fu, Tianrui Wu, Peng Liang, Xicheng Ma, Rashid Iqbal, Yuzhen Qian, Yandong Ma, Mischa Bonn, Hua Wang, Hongjie Dai, Jingcheng Hao, Renhao Dong
As a unique class of framework electronic materials, two‐dimensional conjugated metal‐organic frameworks (2D c‐MOFs) exhibit intrinsic porosity, superior electrical conductivity, and abundant active sites. These properties endow them with great potential in electrochemical lithium‐ion storage. However, the development of 2D c‐MOF‐based capacitors has encountered a bottleneck in enhancing Li‐ion storage
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Structures of Polyhydroxyalkanoate Synthase PhaC from Aeromonas caviae, Producing Biodegradable Plastics Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Min Fey Chek, Sun-Yong Kim, Tomoyuki Mori, Keiji Matsumoto, Shunsuke Sato, Toshio Hakoshima
Polyhydroxyalkanoate (PHA) is a biodegradable polyester that can serve as a promising alternative to petrochemical plastics which present a serious source of pollution. PHA synthase (PhaC) is a key enzyme responsible for producing a wide variety of PHAs in microorganisms. Here we present crystal structures of full‐length PhaC from Aeromonas caviae, a high‐performance PhaC employed for industrial use
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Control Over S(VI)‐Stereogenic Center: NHC‐Catalyzed Enantioselective Synthesis of N‐Acyl Cyclic Sulfonimidamides Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Soumen Barik, Fathima Dinsha Paravakkal, Priyanshu Gupta, Palash Roy, Akkattu T. Biju
The catalytic enantioselective synthesis of aza‐sulfur(VI) compounds holds significant potential in pharmaceuticals owing to their broad spectrum of biological properties. Herein, we report the first N‐heterocyclic carbene (NHC)‐organocatalyzed enantioselective synthesis of cyclic sulfonimidamides (SIAs). The free N‐H containing SIAs often exhibit configurational lability through tautomerization. We
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Cooperativity of Electron Transfer Coupled Spin Transitions in a Tetranuclear Fe/Co Prussian Blue Analogue Revealed by Ultrafast Spectroscopy Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Jan-Hendrik Borter, Simindokht Gol Kar, Sayan Kangsa Banik, Serhiy Demeshko, Rainer Oswald, Martí Gimferrer, Ricardo Mata, Dirk Schwarzer, Franc Meyer
Cooperative intermolecular interactions, usually observed in solid state, can confer useful properties to stimuli‐responsive spin transition materials. Here we evidence for the first time intramolecular cooperativity between the two Fe‐Co subunits of a molecular cyanido‐bridged square Fe2Co2 Prussian blue analog (PBA) in solution, which upon single photon excitation sequentially undergo electron transfer
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Generation, Capture, Storage and Release of Singlet Oxygen from A Perylene Diimide‐Based Metallacage for Oxygen Sensing Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Yali Hou, Yingjie Li, Dengke Han, Zeyuan Zhang, Jinping Zhang, Shijin Jian, Zixuan Li, Xianglong Duan, Haonan Peng, Yu Fang, Mingming Zhang
The controlled generation and utilization of singlet oxygen (1O2) are crucial for its diverse applications but remain challenging due to its high reactivity and short‐lived nature. Here, we report a box‐shaped metallacage prepared via multicomponent coordination‐driven self‐assembly using tetrapyridyl perylene diimide (PDI) and tetracarboxylate anthracene as building blocks. Upon photo‐irradiation
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Synergistic Ru Species on Poly(heptazine imide) Enabling Efficient Photocatalytic CO2 reduction with H2O Beyond 800 nm Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Bo Su, Sibo Wang, Wandong Xing, Kunlong Liu, Sung-Fu Hung, Xiong Chen, Yuanxing Fang, Guigang Zhang, Huabin Zhang, Xinchen Wang
Photocatalytic CO2 conversion with H2O to carbonaceous fuels is a desirable strategy for CO2 management and solar utilization, yet its efficiency remains suboptimal. Herein, efficient and durable CO2 photoreduction is realized over a RuNPs/Ru‐PHI catalyst assembled by anchoring Ru single atoms (SAs) and nanoparticles (NPs) onto poly(heptazine imide) (PHI) via the in‐plane Ru‐N4 coordination and interfacial
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Unprecedented Tetravalent Uranium Photocatalysts for Efficient C(sp3)–C(sp3) Bond Cleavage and Formation Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Xingxing Gong, Lian-Wei Ye, Zong-Chang Han, Yue Zhao, Jin Xie, Han-Shi Hu, Jun Li, Congqing Zhu
Photocatalysis is a pivotal area in synthetic chemistry. Despite extensive application potential in nuclear industry, uranium‐based photocatalysts are historically limited to uranyl(VI/V) redox cycle. Here, we report the discovery of the first tetravalent uranium [U(IV)] photocatalyst that enables efficient C(sp3)–C(sp3) bond cleavage and formation under ideal visible light. The U(IV) alkoxy species
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Structural Basis for the Catalytic Mechanism of ATP‐Dependent Diazotase CmaA6 Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Seiji Kawai, Masayuki Karasawa, Yoshitaka Moriwaki, Tohru Terada, Yohei Katsuyama, Yasuo Ohnishi
Although several diazotases have been recently reported, the details of the reaction mechanism are not yet understood. In this study, we investigated the mechanism of CmaA6, an ATP‐dependent diazotase that catalyzes the diazotization of 3‐aminocoumaric acid using nitrous acid. X‐ray crystallography and cryogenic electron microscopy‐single particle analysis revealed CmaA6 structures in the substrate‐free
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Surface Transformation in Lanthanum Nickelate for Enhanced Oxygen Evolution Catalysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Jia-Wei Zhao, Kaihang Yue, Lili Wu, Jiarui Yang, Deyan Luan, Xitian Zhang, Xiong-Wen (David) Lou
Nickel‐based perovskite oxides are identified as promising candidates for oxygen evolution reaction (OER) catalysts in view of their low cost, highly tunable structure, and potential high activity. However, the performance and catalyst design are hindered by their sluggish surface reconstruction kinetics. We introduce a ferric ion pre‐etching strategy to enhance the surface reconstruction of typical
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Hyperpolarization Modulation of the T‐type hCav3.2 Channel by Human Synenkephalin [1–53], a Shrew Neurotoxin Analogue without Paralytic Effects Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Ryo Fukuoka, Yusuke Yano, Nozomi Hara, Chihiro Sadamoto, Andres D. Maturana, Masaki Kita
Mammalian secreted venoms mainly consist of peptides and proteases used for defense or predation. Blarina paralytic peptides (BPPs), mealworm‐targeting neurotoxins from shrew, are very similar to human synenkephalin. This peptide is released from proenkephalin in the brain along with opioid peptides that mediate analgesic and antidepressant effects, though its physiological function is unclear. Here
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Enhancing C–C Bond Cleavage of Glycerol Electrooxidation through Spin‐selective Electron Donation in Pd–PdS2–Cox Heterostructural Nanosheets Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Pei Liu, Hao Ma, Yuchen Qin, Junjun Li, Fengwang Li, Jinyu Ye, Qiudi Guo, Ning Su, Chao Gao, Lixia Xie, Xia Sheng, Shiju Zhao, Guangce Jiang, Yunlai Ren, Yuanmiao Sun, Zhicheng Zhang
As a 4d–transition metal, the spin state of Pd is extremely difficult to directly regulate for the optimized d orbital states owing to the strong spin–orbit coupling effect and further extended d orbital. Herein, we devise "spin–selective electron donation" strategy to tune specific d orbital electrons of Pd inspired by Dewar−Chatt−Duncanson model theory. Co−S−Pd bridges with different spin–states
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Bridging the Interlayer Binding to Ordered π‐Conjugated Units for Constructing High‐Performing Light Polarization Crystals Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Haotian Qiu, Ran An, Chen Cui, Zhi Li, Jinfeng Yang, Xiaochuang Wang, Xueling Hou, Junjie Li, Juanjuan Lu, Jun Sun, Zhihua Yang, Shilie Pan, Miriding Mutailipu
The light polarization modulation involves the capacity to respond selectively to light‐mater interaction and is dependent on the optical anisotropy of crystalline materials. The π‐conjugated component is almost typically utilized to produce such materials in the short‐wave ultraviolet region, however, the conflicting link between high optical anisotropy and strong layered habit is difficult to reconcile
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closo‐Carboranyl Analogs of β‐Arylethylamines: Direct Synthesis from Alkenes via EnT‐Catalysis Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Fritz Paulus, Corinna Heusel, Marc Jaspers, Lilli M. Amrehn, Florian Schreiner, Debanjan Rana, Constantin G. Daniliuc, Michael Ryan Hansen, Frank Glorius
closo‐Carboranes are icosahedral carbon‐boron clusters with unique properties and broad applicability. They particularly stand out in the context of drug development as privileged structural motifs for boron neutron capture therapy (BNCT) and as highly hydrophobic bioisosteres for the rotational volume of phenyl rings. Herein, we unveil the synthesis of N‐protected carboranyl analogs of β‐arylethylamines
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Coordinative Ring‐Opening Polymerization of Limonene Carbamate towards Phosgene‐ and Isocyanate‐Free Polyurethane Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Jonas Futter, Leon Ferdinand Richter, Stefanie Hörl, Bernhard Rieger, Moritz Kränzlein
This study presents a phosgene‐ and isocyanate‐free route for the synthesis of polyurethanes using (R)‐limonene as a bio‐based starting material. The synthesis of the cyclic limonene‐based carbamate monomer LU is achieved in high yields using dimethyl carbonate as a sustainable, less hazardous phosgene surrogate and is verified by NMR, SC‐XRD, ESI‐MS, GC‐MS, and elemental analysis. Polymerizations
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Aqueous Self‐Assembly of Cylindrical and Tapered Bottlebrush Block Copolymers Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Clark Vu, Narjess Abu Amara, Mohammed Alaboalirat, Einat Nativ‐Roth, Ran Zalk, Wellington Leite, Jan‐Michael Carrillo, Ronit Bitton, John B. Matson
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Reduction of the Thermal Conductivity of Polyurethanes by Fluorination: Impact of Crystallinity, Atomic Density, and Sound Velocity Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25 Jingyi Zhou, Chen Chen, Jinchi Sun, Thomas R. Fielitz, Weijun Zhou, David G. Cahill, Paul V. Braun
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Correction to “High‐Connectivity 3D Covalent Organic Frameworks with pdp Net for Efficient C2H2/CO2 Separation” Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-25
J. Zhang, H. Zheng, F. Chen, Z. Wang, H. Li, F. Sun, D. Zhao, V. Valtchev, S. Qiu, Q. Fang, Angew. Chem. Int. Ed. 2025, 64, e202500161. https://doi.org/10.1002/anie.202500161 In the original publication, the description of [8+6]-c connectivity in the pdp network did not fully align with established topological nomenclature standards (Accounts of Chemical Research 2008, 41, 1782; Crystal Growth & Design
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In Quest of Chemical Probes for DNA Methylation Reader Proteins: Nucleoside and Dimer Analogues of 5‐Methylcytosine Interact with MBD2 Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Jean Contreras, Sophie Vichier-Guerre, Laurence Dugué, Frédéric Bonhomme, Corinne Jallet, Minh-Ha Nguyen, Bruno Vitorge, Alessandra Feoli, Gianluca Sbardella, J. Iñaki Guijarro, Paola Arimondo
DNA methylation modulates gene expression without altering the DNA sequence. Aberrant DNA methylation patterns characterise a wide range of diseases, from cancer to neurological disorders, and serve as validated therapeutic targets and diagnostic tools. Among the proteins involved in DNA methylation regulation, the human reader Methyl‐CpG Binding Domain 2 protein (MBD2) exhibits a strong preference
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Donor‐π‐Acceptor Photoinitiators for High‐Efficiency Visible LED and Sunlight Polymerization and High‐Precision 3D Printing Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Jacques Lalevee, Ji Feng, Tong Gao, Fabrice Morlet-Savary, Michael Schmitt, Celine Dietlin, Jing Zhang, Pu Xiao, Frédéric Dumur, Xiaotong Peng
This study presents the development and evaluation of five dyes with varying conjugated energy levels and donor‐π‐acceptor (D‐π‐A) structures as photoinitiators for free radical polymerization. Their photoinitiation efficiencies are systematically assessed under both visible‐light LED and sunlight. Notably, the conversions reach up to 81% within just 30 s under sunlight, demonstrating the ultra‐fast
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Macrocyclic Peptide Probes for Immunomodulatory Protein CD59: Potent Modulators of Bacterial Toxin Activity and Antibody‐Dependent Cytotoxicity Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Edward William Tate, Jasmine K. Bickel, Ammar. I. S. Ahmed, Aidan B. Pidd, Rhodri M. Morgan, Tom E. McAllister, Sam M. Horrell, Emma C. Couves, Hemavathi Nagaraj, Edward J. Bartlett, Kamel El Omari, Akane Kawamura, Doryen Bubeck
CD59 is an immunomodulatory cell surface receptor associated with human disease. Despite its importance in complement regulation and bacterial pathogenesis, CD59 remains a challenging therapeutic target. Research to date has focused on antibody or protein‐based strategies. Here we present a new approach to target CD59 using macrocyclic peptides with low nanomolar affinity for CD59. Through X‐ray crystallographic
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Metal‐Organic Cages Assembled from {Ni6} Nodes for Selective CO2 Reduction Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Man-Ting Lv, Meng-Di Cui, Kai-Peng Bai, Yu Jiang, Wei-Peng Chen, Na-Na Sun, Xiang-Quan Hu, Chang Huang, Qing-Yuan Yang, Yan-Zhen Zheng
Constructing cluster‐based nodes and using them as catalytic sites can bring new structure and function for metal‐organic cages (MOCs). However, successful examples are very limited. Herein, we found that a 2‐mercapto‐5‐methyl‐1,3,4‐thiadiazole (Hmmt) based {Ni6} subunit is robust in building such MOCs. The {Ni6} node is based on the central Ni4 cubane and two wing Ni(II) ions with virtually three
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A Carboxylate‐based Hydrophilic Organic Photovoltaic Catalyst with a Large Molecular Dipole Moment for High‐Performance Photocatalytic Hydrogen Evolution Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Hua Sun, Jianan Fan, Rong Fan, Po Sun, Shifan Wang, Danfeng Wang, Peiyang Gu, Wenyi Tan, Yongfa Zhu
Achieving ultrafast dissociation of photogenerated excitons and efficient charge transport within the photocatalyst is a fundamental issue. Additionally, enhancing the interaction between semiconductors and water is crucial for efficient photocatalytic water splitting. Herein, we synthesized a carboxylate‐based hydrophilic polymer, hPTB7‐Th. Exposed carboxylates enhance semiconductor‐water interfacial
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Enhancing Cold Adaptation of Bidomain Amylases by High‐Throughput Computational Engineering Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Zhongyue J. Yang, Ning Ding, Yaoyukun Jiang, Robbie Ge, Qianzhen Shao, Wook Shin, Xinchun Ran
Cold‐adapted bidomain enzymes have the potential to foster industrial sustainability by reducing energy consumption and greenhouse gas emissions. Despite their allure, these benefits are unattainable as the molecular basis of cold adaptation remains elusive and there are no strategies to guide the acquisition of this behavior. To uncover principles of cold adaptation, we selected the cold‐adapted Saccharophagus
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Single‐Atom Fe Catalysts with Improved Metal Loading for Efficient Ammonia Synthesis under Mild Conditions Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Yuting Jiang, Ziquan Chen, Tao Peng, Long Jiao, Xiulian Pan, Xinhe Bao, Hai-Long Jiang
Ammonia synthesis is a cornerstone in the chemical industry. Given the traditional Haber‐Bosch (H‐B) process requires very high temperature and pressure, it is imperative to develop catalysts capable of facilitating ammonia synthesis under mild conditions. In this work, a post‐metal replacement strategy is developed to improve the Fe loading in single‐atom Fe‐implanted N‐doped carbon catalysts. Starting
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Metathetical Exchange, Synthesis and Carbon Dioxide Addition of Higher Homologues of Group 9 Metal Carbynes Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Lennart Gerhard Holzapfel, Johanna Manegold, Stefan Florian Clewing, Hartmut Schubert, Klaus Eichele, Lars Wesemann
A one‐pot synthesis for previously unknown heavy homologues of group 9 metal carbynes [(Me3P)3CoºGeAr*] (1), [(Me3P)3RhºGeAr*] (2), [(Me3P)3IrºGeAr*] (3), [(Me3P)3IrºSnAr*] (5), and [(Et3P)3IrºPbAr*] (7) is presented [Ar* = C6H3‐2,6‐(Trip)2, Trip = 2,4,6‐C6H2iPr3]. During these preparations the tetrylidynes [(Me3P)3RhºSnAr*] (4), and [(Me3P)3RhºPbAr*] (6), were also prepared in a one‐pot procedure
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Development of an Organoautocatalyzed Double σ‐Bond C(sp2)‐N Transamination Metathesis Reaction Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Volker Klein, Florian Schuster, Jonas Amthor, Harald Maid, Prabhakar Bijalwan, Fahmi Himo, Stefano Santoro, Svetlana B. Tsogoeva
The transamination reaction, which involves the conversion of one amine to another, traditionally relies on biological enzyme catalysts. Although chemists have recently developed a few transition metal‐catalyzed methods, mimicking these enzymes to interconvert amine groups in acyclic substrates via transamination metathesis of a single C(sp2)–N bond, transamination of cyclic tertiary amines has remained
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On‐Membrane Supramolecular Assemblies Serving as Bioorthogonal Gating for Melphalan Angew. Chem. Int. Ed. (IF 16.1) Pub Date : 2025-04-24 Hanlin Xu, Qingxin Yao, Xiaoqian Hu, Debin Zheng, Chao Ren, Zhibin Ren, Yuan Gao
Covalent drugs have experienced a revival in recent decades due to their advantageous pharmacodynamic profiles and targeting of “undruggable” proteins. However, balancing selectivity, reactivity, and potency is essential for the safe and effective drugs. Here we employ a cell‐selective bioorthogonal prodrug design to enhance the selectivity for covalent inhibitors without compromising the reactivity