Angewandte Chemie International Edition最新文献_第8页

High-Entropy Engineering to Stabilize Single-Atom Ru Catalysts for Efficient and Durable Water Splitting 稳定单原子Ru催化剂的高熵工程用于高效和持久的水裂解

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.2676498

Peng-Fei Xie,Yun-Fan Yang,Ju-Zhen Zhang,Binbin He,Feng Zhang,Wenbo Zhao,Peng-Xiang Hou,Yan Sun,Wang Du,Yun Zu,Chang Liu,Yian Wang,Minhua Shao,Jin-Cheng Li

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Substrate Promiscuity of CHST1 Enables Efficient Synthesis of Galactose-6-O-Sulfated Glycans for Siglec Recognition Profiling CHST1的底物乱交性使半乳糖-6- o -硫酸甘聚糖的有效合成用于Siglec识别谱分析

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.4139901

Shumin Bao,Tangliang Shen,MohammadHossein Shabahang,Shuquan Fan,Hongshuai Lv,Guitao Bai,Jun Pan,Lei Li

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Synergistic Supramolecular Bonding Enables Self‐Reinforcing and Chemically Recyclable Sustainable Materials 协同超分子键使自我增强和化学可回收的可持续材料成为可能

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.4709247

Zhen Zhou, Xing‐Liang Li, Yao Li, Zheng‐Ming Li, Xiao‐Yang Xu, Ning Zhao, Xiu‐Li Wang, Teng Fu, Yu‐Zhong Wang

{"title":"Synergistic Supramolecular Bonding Enables Self‐Reinforcing and Chemically Recyclable Sustainable Materials","authors":"Zhen Zhou, Xing‐Liang Li, Yao Li, Zheng‐Ming Li, Xiao‐Yang Xu, Ning Zhao, Xiu‐Li Wang, Teng Fu, Yu‐Zhong Wang","doi":"10.1002/anie.4709247","DOIUrl":"https://doi.org/10.1002/anie.4709247","url":null,"abstract":"Developing polymer materials that break the long‐standing trade‐off between long‐term durability and efficient chemical recyclability remains a fundamental challenge. We report an environmentally self‐reinforcing and easily recyclable unprecedented biomass‐derived supramolecular polyester that circumvents this limitation through the synergistic integration of dynamic hydrogen bonds and halogen‐bond‐assisted depolymerization. Amide‐mediated hydrogen‐bond networks undergo environment‐activated supramolecular rearrangement under hygrothermal, ultraviolet, and electrical aging conditions, promoting chain realignment, recrystallization, and network densification. As a result, the material exhibits self‐reinforcing behavior, achieving an ultrahigh tensile strength of 138.4 MPa (61% increase) and a UV‐shielding efficiency of 98% (36% increase) while maintaining excellent electrical insulation. Simultaneously, halogen‐bond interactions enhance solvent penetration and facilitate ester activation, enabling rapid depolymerization in dichloromethane at ambient temperature. Monomers are recovered with >99% purity and >90% yield for closed‐loop repolymerization, while also enabling molecular upcycling into supramolecular adhesives exhibiting exceptional chemical resistance and an ultrahigh cryogenic bonding strength of 11.0 MPa at −196°C. This work establishes a supramolecular design principle that decouples service‐life reinforcement from end‐of‐life chemical deconstruction, providing a general strategy for reconciling durability and recyclability in polymeric materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"13 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

The Manifestation of the Electrochemical Potential Gradient in the Kinetic Landscapes of Interfacial Electrochemistry 电化学电位梯度在界面电化学动力学景观中的表现

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.6521153

Sebastian Z. Oener, Caroline J. Aschendorf, Jody Druce, Francisco Sarabia, Carlos Gomez Rodellar, Mathieu Lizée, Alex Ricardo Silva Olaya, Soumyadip Mondal, Raquel Anastacio Amaral, Hađer Sinanović, Beatriz Roldan Cuenya

{"title":"The Manifestation of the Electrochemical Potential Gradient in the Kinetic Landscapes of Interfacial Electrochemistry","authors":"Sebastian Z. Oener, Caroline J. Aschendorf, Jody Druce, Francisco Sarabia, Carlos Gomez Rodellar, Mathieu Lizée, Alex Ricardo Silva Olaya, Soumyadip Mondal, Raquel Anastacio Amaral, Hađer Sinanović, Beatriz Roldan Cuenya","doi":"10.1002/anie.6521153","DOIUrl":"https://doi.org/10.1002/anie.6521153","url":null,"abstract":"The electrochemical potential gradient constitutes a free energy driving force. Understanding how this gradient manifests itself and drives electronic and ionic charges through the bulk and across interfaces is important across the natural sciences, including in solar cells, batteries, heterogeneous and biocatalysis, and proton pumps and motors. Despite this, literature often misrepresents the electrochemical potential gradient. In the extreme, it is simply replaced by an electric field as an apparent driving force. Here, we use energy band diagrams to review the basics of electrochemical charge separation and to inform on the nonequilibrium boundary conditions in interfacial electrochemistry. We explain that the thermodynamic driving force along the reaction coordinate needs to be distinguished from chemical potential changes in the extended environment that can modulate activation barriers, without necessarily being a driving force themselves. To this end, we focus on the role of overpotential‐dependent excess charge and electric fields, before discussing overpotential‐dependent coverages and multistep reactions. We close by explaining how these local chemical potential changes give rise to a multidimensional kinetic landscape that cannot be compressed into single‐descriptor kinetics.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"53 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Mechanophotochemistry : Lighting up EDA Complexes in the Solid State 机械光化学：点燃固态的EDA配合物

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.9162701

Aniket Kumar Srivastawa, Eli Zysman‐Colman

{"title":"Mechanophotochemistry : Lighting up EDA Complexes in the Solid State","authors":"Aniket Kumar Srivastawa, Eli Zysman‐Colman","doi":"10.1002/anie.9162701","DOIUrl":"https://doi.org/10.1002/anie.9162701","url":null,"abstract":"Solvent arguably constitutes the single largest waste stream in synthesis. Mechanophotocatalysis , a synergistic union of mechanochemistry and photocatalysis, offers a solution to significantly reduce solvent use in photochemistry. Here, we show how photochemical reactions in the solid state can be driven by visible light using in situ formed electron donor–acceptor (EDA) complexes in air, obviating the need for an external photocatalyst. Under the optimized conditions, only 2–4 equiv. of solvent is used as a liquid‐assisted grinding (LAG) agent, thus significantly reducing solvent use. We demonstrate EDA mechanophotochemistry across five reactions: a Giese reaction; a C─S cross‐coupling reaction; a phosphorylation reaction; a sulfonylation reaction; and a Povarov reaction. While the first four proceeded readily and competitively with the solution‐state EDA photochemical reaction, the latter one, requiring O 2 as a terminal oxidant, does not. In investigating the sulfonylation reaction we further identify the first example of a photomechanoredox reaction in which the stainless‐steel milling ball directly participates in the reaction, revealing the milling medium as a previously unrecognized reactivity parameter. Together, these results establish visible light‐promoted mechanophotochemistry as a solvent‐minimized and viable alternative to solution‐state photochemical reactions.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173017","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Metal‐Center‐Controlled Fenton‐Like Reactivity of Biomimetic First‐Row Transition Metal Complexes in Aqueous Anticancer Catalysis 金属中心控制的仿生第一排过渡金属配合物在水抗癌催化中的类芬顿反应性

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.3481625

Hyungbin Park, Sungju Jung, Junho Lee, Myong‐Suk Park, Jiseon Ha, Hyeri Jeon, Chaeun Oh, Woo Kyun Bae, Kyung Hyun Yoo, Seungwoo Hong

{"title":"Metal‐Center‐Controlled Fenton‐Like Reactivity of Biomimetic First‐Row Transition Metal Complexes in Aqueous Anticancer Catalysis","authors":"Hyungbin Park, Sungju Jung, Junho Lee, Myong‐Suk Park, Jiseon Ha, Hyeri Jeon, Chaeun Oh, Woo Kyun Bae, Kyung Hyun Yoo, Seungwoo Hong","doi":"10.1002/anie.3481625","DOIUrl":"https://doi.org/10.1002/anie.3481625","url":null,"abstract":"Catalytic oxidative cancer therapy exploits elevated hydrogen peroxide levels within tumor microenvironments to induce selective oxidative damage in malignant cells. However, many ROS‐generating therapeutic systems rely on heavy metals or structurally complex inorganic architectures, limiting their biological compatibility and catalytic selectivity. Inspired by nonheme iron‐mediated redox catalysis, we report a series of water‐soluble biomimetic first‐row transition metal complexes supported by a picolylamine‐derived nonheme ligand scaffold bearing a pendant hydroxyl group. Systematic variation of the metal center (Mn, Fe, Co, Ni, Cu, and Zn) generated divergent electrochemical behavior and distinct peroxide‐activation reactivity, yet only the iron complex, [Fe(N 2 Py 3 OH)] 2+ ( 1‐Fe ), promoted hydroxyl radical formation via Fenton‐like hydrogen peroxide activation in water. Spectroscopic, electrochemical, and crystallographic analyses revealed a biomimetic coordination environment that stabilizes a quasi‐reversible Fe(II)/Fe(III) redox couple suited to catalytic peroxide activation. In gastric cancer cells, 1‐Fe induced intracellular oxidative stress, mitochondrial depolarization, lipid peroxidation, and concomitant apoptosis and ferroptosis, while exhibiting negligible toxicity toward normal fibroblasts. In combination with paclitaxel, 1‐Fe produced synergistic antiproliferative activity in vitro and suppressed peritoneal tumor dissemination in vivo without overt systemic toxicity. Collectively, these results establish biomimetic iron complexes as molecular platforms for Fenton‐like oxidative catalysis in redox‐based cancer therapy.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"33 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173019","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Bridge‐Length‐Dependent Diradical and Mixed‐Valence Radical in Benzene Triimide Cages 三酰苯笼中桥长依赖的双自由基和混合价自由基

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.2242440

De‐Hui Tuo, Teng‐Yu Huang, Xu‐Dong Wang, Yu‐Fei Ao, Qi‐Qiang Wang, De‐Xian Wang

{"title":"Bridge‐Length‐Dependent Diradical and Mixed‐Valence Radical in Benzene Triimide Cages","authors":"De‐Hui Tuo, Teng‐Yu Huang, Xu‐Dong Wang, Yu‐Fei Ao, Qi‐Qiang Wang, De‐Xian Wang","doi":"10.1002/anie.2242440","DOIUrl":"https://doi.org/10.1002/anie.2242440","url":null,"abstract":"Supramolecular radical cages are captivating architectures in supramolecular chemistry and materials science; however, their construction and precise regulation of electronic states and magnetic properties remain substantially challenging. Herein, we report the synthesis, structures, and magnetic properties of a series of covalent organic radical cages, generated by reducing the benzene triimide (BTI) radical precursors within the corresponding neutral cages. The m ‐xylene‐bridged cage with two parallel BTI units separated by 5.4 Å undergoes stepwise reduction to afford both mixed‐valence monoradical and diradical cages. In contrast, the cavity‐expanded cage with naphthalene bridges (7.6 Å) preferentially gives a mixed‐valence monoradical even under excess reductant. This discrepancy originates from cavity‐mediated host–guest interactions of the radical cages, which selectively stabilize the mixed‐valence monoradical of the naphthalene‐bridged cage. All the radical cages exhibit good stability and are characterized by single‐crystal x‐ray diffraction, EPR, and UV–vis–NIR spectroscopy. For the m ‐xylene‐bridged diradical cage, the two BTI radical units are weakly coupled, exhibiting a singlet ground state with a narrow singlet–triplet energy gap (Δ E ST = –1.63 kcal/mol). The naphthalene‐bridged mixed‐valence monoradical cage features an unpaired electron delocalized over the two BTI units and exhibits antiferromagnetic interactions arising from its one‐dimensional linear assembly in the solid state.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"31 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172893","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Radical‐Mediated Surface Reconstruction of SnO 2 Nanocrystals Enables Efficient and Durable Perovskite Solar Cells and Modules 自由基介导的二氧化钛纳米晶体表面重建使高效耐用的钙钛矿太阳能电池和组件成为可能

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.4404754

Shiheng Wang, Jian Cheng, Xianglong Sun, Xiao Jiang, Qiqi Wang, Xiaolan Lu, Junru Chen, Yanlin Song, Yiqiang Zhang

{"title":"Radical‐Mediated Surface Reconstruction of SnO 2 Nanocrystals Enables Efficient and Durable Perovskite Solar Cells and Modules","authors":"Shiheng Wang, Jian Cheng, Xianglong Sun, Xiao Jiang, Qiqi Wang, Xiaolan Lu, Junru Chen, Yanlin Song, Yiqiang Zhang","doi":"10.1002/anie.4404754","DOIUrl":"https://doi.org/10.1002/anie.4404754","url":null,"abstract":"Charge‐transport layers fundamentally dictate interfacial recombination, carrier extraction, and operational stability in perovskite solar cells (PSCs), yet scalable routes to simultaneously regulate their colloidal stability and defect chemistry remain elusive. Here, we report a radical‐mediated surface reconstruction strategy for ligand‐free SnO 2 nanocrystals that enables concurrent gains in device efficiency, scalability, and durability. Sonochemical activation generates hydroxyl radicals that selectively passivate oxygen‐deficient Sn sites while inducing electrostatically stabilized dispersions with exceptional shelf stability, allowing the SnO 2 colloids to be stored for over 2 years without aggregation or performance degradation. This stabilization enables the formation of uniform electron transport layers with reduced trap density and enhanced electron mobility. These improvements promote buried‐interface perovskite crystallization and accelerate charge extraction, yielding PSCs with an efficiency of 26.47% (certified 26.12%). Importantly, the strategy is inherently scalable, enabling a perovskite module (∼110 cm 2 ) with an efficiency of 21.45%. Devices exhibit enhanced operational stability, retaining 92% efficiency after 1000 h thermal aging (ISOS‐D‐2), maintaining 88% efficiency under maximum power point tracking (ISOS‐L‐1), and showing negligible degradation over 500 thermal cycles (ISOS‐T‐3). These results establish radical‐mediated engineering of SnO 2 nanocrystals as a general pathway in perovskite photovoltaics, bridging high efficiency, large‐area manufacturability, and long‐term operational stability.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"7 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172944","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Circularly Polarized Light Amplifies Spin Polarization for Efficient Photoredox Chemistry in a Chiral Magnetic Catalyst 圆偏振光放大自旋极化用于手性磁性催化剂的高效光氧化还原化学

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.8457661

Shuaikun Ji, Jiahong Liu, Hui Ai, Qingli Wang, Caiwei Zhang, Junting Wang, Xianghong Niu, Jiatao Zhang, Yiou Wang

{"title":"Circularly Polarized Light Amplifies Spin Polarization for Efficient Photoredox Chemistry in a Chiral Magnetic Catalyst","authors":"Shuaikun Ji, Jiahong Liu, Hui Ai, Qingli Wang, Caiwei Zhang, Junting Wang, Xianghong Niu, Jiatao Zhang, Yiou Wang","doi":"10.1002/anie.8457661","DOIUrl":"https://doi.org/10.1002/anie.8457661","url":null,"abstract":"Photocatalysis offers a promising route to sustainable energy, yet the role of carrier spin in charge transport and interfacial redox chemistry remains poorly understood. Chiral and magnetic catalysts selectively transmit spin‐compatible carriers, whereas non‐polarized light generates mixed‐spin populations, limiting carrier utilization. Herein, we demonstrate that circularly polarized light (CPL) reversibly modulates spin‐dependent carrier transport in Ni‐cocatalyst‐decorated, cysteine‐modified CdS nanorods, thereby promoting spin‐sensitive carrier utilization during aqueous methanol reforming. Optimized D(−)‐CdS/Ni exhibits a 71.1% higher hydrogen evolution rate under left‐handed CPL (LCP) than under right‐handed CPL (RCP) at identical light intensity and spectrum, achieving an apparent quantum efficiency of 74.4% at 420 nm while promoting methanol oxidation toward formic acid. CPL‐coupled magnetic conductive atomic force microscopy reveals that LCP increases the apparent spin polarization from 70.9% in the dark to 89.1%, whereas RCP suppresses it to 12.8%. Spin‐polarized calculations identify nonequivalent electronic channels, while spectroscopic and kinetic measurements support enhanced carrier extraction and reduced recombination under LCP. Together, these findings establish photon handedness as a reversible optical variable for modulating spin‐selective transport and photoredox chemistry, offering a strategy to complement material‐encoded spin filtering with dynamic optical control of carrier utilization.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"11 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173014","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chalcogen-Bond-Driven Electrochemical Bromide Sequestration in Benzothiazole-Functionalized Covalent Organic Frameworks 苯并噻唑功能化共价有机骨架中硫键驱动的电化学溴化物封存

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-15 DOI: 10.1002/anie.9495644

Najat Maher Aldaqqa,Rajesh Dhanushkotti,Sara Vaca-Chacon,Sushil Kumar,Thibault Terencio,Kyriaki Polychronopoulou,Gisha Elizabeth Luckachan,Dinesh Shetty

引用次数: 0