Angewandte Chemie International Edition最新文献_第2页

Reductive Nitrogen Species Activation via Pulsed Electrolysis: Recent Advances and Future Prospects. 脉冲电解法活化还原性氮：最新进展及未来展望。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202516909

Kiarash Torabi,Rongji Liu,David Leander Troglauer,Christean Nickel,Guillermo Corea,Tiansheng Bai,Deping Li,Lijie Ci,Bahareh Feizi Mohazzab,Dandan Gao

{"title":"Reductive Nitrogen Species Activation via Pulsed Electrolysis: Recent Advances and Future Prospects.","authors":"Kiarash Torabi,Rongji Liu,David Leander Troglauer,Christean Nickel,Guillermo Corea,Tiansheng Bai,Deping Li,Lijie Ci,Bahareh Feizi Mohazzab,Dandan Gao","doi":"10.1002/anie.202516909","DOIUrl":"https://doi.org/10.1002/anie.202516909","url":null,"abstract":"The electrochemical reduction of nitrogen species offers a sustainable route to mitigate environmental nitrogen pollution while enabling the production of value-added chemicals such as ammonia, hydroxylamine, and C─N coupled organonitrogen compounds. However, the practical implementation of conventional potentiostatic methods is hindered by poor product selectivity and competing hydrogen evolution. Pulsed electrolysis has emerged as a transformative strategy to address these challenges by synchronizing catalyst surface dynamics with local microenvironmental changes and reaction kinetics. This mini-review highlights recent advances in pulsed electrolysis for nitrogen species reduction, with a particular focus on how dynamic potentials influence electrocatalyst behavior and the surrounding reaction environment. Key mechanistic insights and cutting-edge research findings are discussed, followed by an outlook on established systems and future directions toward scalable and energy-efficient nitrogen activation.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"11 1","pages":"e202516909"},"PeriodicalIF":16.6,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145357940","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

A Theory-Driven Moderation Strategy for Electrolyte Design Unlocks Stable Aqueous Zinc Deposition. 理论驱动的电解液设计缓和策略解锁稳定的水锌沉积。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202518262

Jingyi Wang,Hang Yang,Yunpeng Zhong,Jianrui Feng,Zhe Cui,Ruwei Chen,Jie Chen,Fangjia Zhao,Jiajia Huang,Guanjie He

{"title":"A Theory-Driven Moderation Strategy for Electrolyte Design Unlocks Stable Aqueous Zinc Deposition.","authors":"Jingyi Wang,Hang Yang,Yunpeng Zhong,Jianrui Feng,Zhe Cui,Ruwei Chen,Jie Chen,Fangjia Zhao,Jiajia Huang,Guanjie He","doi":"10.1002/anie.202518262","DOIUrl":"https://doi.org/10.1002/anie.202518262","url":null,"abstract":"How theoretically screened solvation characteristics of additives affect zinc deposition behavior has emerged as a critical question of both scientific and practical relevance. Here, using a series of structurally analogous alcohol-based molecules as a model system and guided by theoretical calculations, we establish a non-extremum empirical model for additive screening to balance the relationship between additive theoretically properties and the solvation/interface stability in aqueous Zn-ion battery electrolytes. Solvation capability, adsorption strength, and interfacial electrostatic properties were calculated to directly probe the critical role of a balanced set of molecular parameters in modulating Zn2+ coordination structure and interface stability. As a result, 1,6-hexanediol, exhibited a set of balanced and non-extremum molecular parameters, significantly enhanced the reversibility of zinc deposition/stripping, delivered the best electrochemical performance that extending the cycling lifespan to 2 600 h, which is consistent with the Sabatier principle. This study provides a new theoretical perspective for the rational screen of electrolyte additives and highlights the importance of expanding the selection criteria for optimizing interfacial stability.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"150 1","pages":"e202518262"},"PeriodicalIF":16.6,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145357832","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

Directing the Electrochemical C─N Coupling Toward Efficient Amide Synthesis via Ammonia Activation-Mediated Pathway. 通过氨活化介导途径引导电化学C─N偶联高效合成酰胺。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202518108

Zhenzhong Liu,Guangtao Ma,Jiawei Li,Junchi Xu,Li Xiong,Yuan Zhong,Hengjie Liu,Lejuan Cai,Ning Zhang,Yujie Xiong

{"title":"Directing the Electrochemical C─N Coupling Toward Efficient Amide Synthesis via Ammonia Activation-Mediated Pathway.","authors":"Zhenzhong Liu,Guangtao Ma,Jiawei Li,Junchi Xu,Li Xiong,Yuan Zhong,Hengjie Liu,Lejuan Cai,Ning Zhang,Yujie Xiong","doi":"10.1002/anie.202518108","DOIUrl":"https://doi.org/10.1002/anie.202518108","url":null,"abstract":"Electrochemically oxidative C─N coupling using alcohol and ammonia as feedstocks offers a sustainable alternative for the chemosynthesis of amide organonitrogens. The achievements of high activity and selectivity yet remains challenging via the conventional alcohol oxidation pathway. Here, we present an alternative ammonia-activation mediated pathway to favor the electrochemical C─N coupling necessary. Spectroscopic and theoretical investigations untangle that this manipulated process begins with the oxidation of ammonia to endow active *NH2 species, which then efficiently couple with alcohol species to form C─N bonds. This alternative C─N coupling pathway exhibits accelerated kinetics and, more importantly, bypasses the formation of aldehyde intermediate, thereby preventing unfavorable overoxidation. As a result, this pathway achieves a high Faradaic efficiency of 50.1% and a carbon selectivity of 87.6% for efficient formamide electrosynthesis over a NiCuRu-based (oxy)hydroxide catalyst, with a productivity of 557.2 µmol cm-2 h-1. Such electrosynthetic approach further exhibit the universality of waste biomass/plastics-driven carbon feedstocks, achieving considerable Faradaic efficiencies of 32%-60%. Techno-economic analysis confirms the potential profitability of using renewable electricity input, highlighting the significant advantages of green chemical manufacturing for sustainable development.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"150 1","pages":"e202518108"},"PeriodicalIF":16.6,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145357655","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

Ni-Bridged Biphasic Molybdenum Carbide Interfaces: A Synergistic Catalyst for High-Performance Lithium-Selenium Batteries. 镍桥双相碳化钼界面：高性能锂硒电池的协同催化剂。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202519816

Jiayi Li,Hong Gao,Dingyi Zhang,Li Gao,Shijian Wang,Congcong Li,Xinyao Yuan,Chao Yuan,Xinming Nie,Jinqiang Zhang,Yufei Zhao,Guoxiu Wang,Hao Liu

{"title":"Ni-Bridged Biphasic Molybdenum Carbide Interfaces: A Synergistic Catalyst for High-Performance Lithium-Selenium Batteries.","authors":"Jiayi Li,Hong Gao,Dingyi Zhang,Li Gao,Shijian Wang,Congcong Li,Xinyao Yuan,Chao Yuan,Xinming Nie,Jinqiang Zhang,Yufei Zhao,Guoxiu Wang,Hao Liu","doi":"10.1002/anie.202519816","DOIUrl":"https://doi.org/10.1002/anie.202519816","url":null,"abstract":"Transition metal catalysts are key to developing high-performance lithium-selenium (Li-Se) batteries. Herein, we report a rationally designed Ni-bridged biphasic molybdenum carbide (Mo2C) with a multi-interface structure that exposes abundant active sites and significantly enhances the electrochemically reversibility of Li-Se batteries under high current operation. The synergistic integration of catalytic and conductive functions facilitates the rapid deposition and conversion of Se/Li2Sex, effectively preventing electrode passivation caused by inactive accumulation during high-rate and long-term cycling. Furthermore, Ni serves dual roles as a structural bridge to link Mo2C lattice and an electronic modulator to optimize the d-orbital configuration of Mo, thereby maximizing the catalytic efficiency of functionalized Mo2C. The synergistic effects of adsorption, desorption, and catalysis enable the rationally designed metal carbide/Se electrode to promote not only the rapid conversion of long-chain Li2Sen species but also the solid-solid transformation of Li2Se2 into Li2Se. As a result, the electrode achieves full-process catalytic conversion in Li-Se batteries, delivering excellent cycling stability and high-rate performance. Even under high Se loading (5.6 mg cm-2), the electrode delivers an initial capacity of 400 mAh g-1 at 0.1 C. These results highlight the effectiveness of the synergistic adsorption/desorption/catalysis mechanism in enabling a fast solid-solid conversion pathway for Li-Se batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"19 1","pages":"e202519816"},"PeriodicalIF":16.6,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145357652","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

Discovery of a Heme-Dependent Enzyme Catalyzing Nitrogen-Nitrogen Bond Formation in Kinamycin Biosynthesis. 在Kinamycin生物合成中催化氮-氮键形成的血红素依赖酶的发现。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202513778

Yuchun Zhao,Zhihong Xiao,Xiangyang Liu,Chenxi Zhu,Xingcan Liang,Xinyi He,Shuangjun Lin,Zixin Deng,Ming Jiang

{"title":"Discovery of a Heme-Dependent Enzyme Catalyzing Nitrogen-Nitrogen Bond Formation in Kinamycin Biosynthesis.","authors":"Yuchun Zhao,Zhihong Xiao,Xiangyang Liu,Chenxi Zhu,Xingcan Liang,Xinyi He,Shuangjun Lin,Zixin Deng,Ming Jiang","doi":"10.1002/anie.202513778","DOIUrl":"https://doi.org/10.1002/anie.202513778","url":null,"abstract":"A nitrogen-nitrogen (N─N) bond is a core feature of diverse natural products with interesting structural and biological properties. Kinamycin and lomaiviticin, featuring a diazobenzo[b]fluorene core, exhibit exceptional potency as chemotherapeutic agents. However, the N─N bond forming step in their biosynthesis has remained elusive. Through extensive mutagenesis and biochemical studies, we herein report that Alp1J, belonging to a new family of heme-dependent enzymes, catalyzes the N─N bond formation in kinamycin biosynthesis. Interestingly, Alp1J forms a stable complex with its partner ferredoxin Alp1I, which can protect the cofactors and is critical for the N─N bond formation activity. With its partner ferredoxin, Alp1J catalyzes formation of the hydrazine intermediate directly from l-aspartate and nitrite by a pathway involving four-electron reduction. Our findings expand the knowledge of enzymatic N─N bond formation and show the potential for the discovery and development of novel N─N bond containing natural products through genome mining and synthetic biology.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"101 1","pages":"e202513778"},"PeriodicalIF":16.6,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145357656","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

Covalent Organic Framework Membranes with Asymmetric Wettability for Efficient Photocatalytic H2O2 Synthesis. 具有不对称润湿性的共价有机框架膜用于光催化合成H2O2。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202519513

Chi Qiao,Weipeng Xian,Zhuozhi Lai,Zhirou Huang,Qing Guo,Sai Wang,Zhifeng Dai,Yubing Xiong,Xiangju Meng,Shengqian Ma,Qi Sun

引用次数: 0

Flipping of a Non-productive Substrate Binding Conformation Facilitates Hydroxynitrile Lyase Catalyzed Hydrocyanation. 非生产性底物结合构象的翻转促进了羟基腈裂解酶催化的氢氰化。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202515778

Yu-Cong Zheng,Yong Mao,Qiang Geng,Fu-Long Li,Xu-Dong Kong,Yi-Ke Qi,Lin Zhang,Qi Chen,Zhi-Jun Zhang,Ran Hong,Yi-Lei Zhao,Hui-Lei Yu,Jian-He Xu

{"title":"Flipping of a Non-productive Substrate Binding Conformation Facilitates Hydroxynitrile Lyase Catalyzed Hydrocyanation.","authors":"Yu-Cong Zheng,Yong Mao,Qiang Geng,Fu-Long Li,Xu-Dong Kong,Yi-Ke Qi,Lin Zhang,Qi Chen,Zhi-Jun Zhang,Ran Hong,Yi-Lei Zhao,Hui-Lei Yu,Jian-He Xu","doi":"10.1002/anie.202515778","DOIUrl":"https://doi.org/10.1002/anie.202515778","url":null,"abstract":"Understanding enzyme-substrate conformational transformations is crucial to the design and engineering of biocatalysts. However, the mechanisms by which substrates undergo dynamic transformations that regulate the function of an enzyme remain poorly understood. Hydroxynitrile lyase from Prunus communis (PcHNL5) catalyzes the cleavage of cyanohydrins. Its reverse reaction holds significant synthetic potential for the preparation of pharmaceutical precursors. Using a combination of crystallography and computational experiments, a novel flipped substrate binding state is identified within the substrate tunnel of the PcHNL5L331A mutant. This binding state is non-productive and undergoes a conformational change before the catalytic cycle can proceed. Site-saturation mutagenesis led to the discovery of a triple mutant, PcHNL5L331A/S333V/P340L, that destabilizes the non-productive substrate binding state thereby facilitating its transition to the catalytically productive conformation and significantly enhancing catalytic efficiency. Crystallographic studies provide a structural description of the factors that stabilize versus destabilize the different binding conformers in the different enzyme variants and thus the differing catalytic efficiencies. These findings demonstrate that destabilizing unfavorable substrate binding conformations within an enzyme active site can improve functionality and provide a promising strategy for designing efficient biocatalysts.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"106 1","pages":"e202515778"},"PeriodicalIF":16.6,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145357790","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

Reliable Determination of Photoreaction Kinetics and Cyclization/Cycloreversion Quantum Yields for Dithienylethene Switches. 二乙烯开关光反应动力学和环化/环还原量子产率的可靠测定。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202514591

Jakub Drapała,Krzysztof Durka,Katarzyna N Jarzembska,Radosław Kamiński

引用次数: 0

Ionic Covalent Organic Framework Membranes for Rapid Moisture-Driven Actuation and Sensing. 用于快速水分驱动驱动和传感的离子共价有机框架膜。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-24 DOI: 10.1002/anie.202521896

Xin Liu,Weibin Lin,Jinrong Wang,Fang Fang,Pei Yu,Niveen M Khashab

{"title":"Ionic Covalent Organic Framework Membranes for Rapid Moisture-Driven Actuation and Sensing.","authors":"Xin Liu,Weibin Lin,Jinrong Wang,Fang Fang,Pei Yu,Niveen M Khashab","doi":"10.1002/anie.202521896","DOIUrl":"https://doi.org/10.1002/anie.202521896","url":null,"abstract":"The development of smart materials capable of rapid and reversible responses to ambient humidity is essential for next-generation sensors, monitoring systems, and adaptive devices. Covalent organic frameworks (COFs), with their tunable porosity and designable architectures, represent a promising class of materials for such stimuli-responsive systems, yet practical implementation remains limited. In this study, we report a self-standing ionic COF membrane, synthesized by integrating hydrogen-bonding ionic functionalities into the framework backbone. This rational design endows the membrane with exceptional moisture-driven actuation and sensing behavior. The unique hydrogen bonding interactions within the framework facilitate rapid water uptake and release, enabling a rapid response time of 1 s. The membrane demonstrates excellent mechanical flexibility, high water sorption capacity, and robust cycling durability. Results from DFT calculations and MD simulations revealed that water molecules could strongly adsorb onto the membrane via hydrogen bonding to modulate its micropore structure and facilitate its responsive behavior. Furthermore, its responsive behavior to subtle humidity changes makes it suitable for applications such as human-interfacing soft actuators, smart switches, and soil moisture sensors. This study highlights the utility of ionic COF membranes as a versatile platform for creating next-generation intelligent materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"1 1","pages":"e202521896"},"PeriodicalIF":16.6,"publicationDate":"2025-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145357700","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

Ultrawideband Emission of Bi3+ Ions Spanning Visible to Near-Infrared Spectral Regions (400 nm-1700 nm). 跨越可见光至近红外光谱区（400 nm-1700 nm）的Bi3+离子的超宽带发射。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-23 DOI: 10.1002/anie.202520587

Huimin Li,Xiaoman Shi,Ran Pang,Ruiping Deng,Mekhrdod S Kurboniyon,Lihong Jiang,Da Li,Su Zhang,Hongjie Zhang

{"title":"Ultrawideband Emission of Bi3+ Ions Spanning Visible to Near-Infrared Spectral Regions (400 nm-1700 nm).","authors":"Huimin Li,Xiaoman Shi,Ran Pang,Ruiping Deng,Mekhrdod S Kurboniyon,Lihong Jiang,Da Li,Su Zhang,Hongjie Zhang","doi":"10.1002/anie.202520587","DOIUrl":"https://doi.org/10.1002/anie.202520587","url":null,"abstract":"Although Bi3+ ions exhibit exceptional luminescent properties and spectral tunability, their potential as activators for near-infrared (NIR) ultrawideband emission remains underexplored, while transition metal ions such as Ni2+, Fe3+, and Cr3+/4+ have long been the predominant candidates in this demanding research area. Herein, we demonstrate ultrawideband emission from 400 to 1700 nm in K2MgGeO4:Bi3+ (KMGO:Bi3+), achieving an internal quantum efficiency (IQE) of 88.02% and external quantum efficiency (EQE) of 66.41%. The emission spectrum features interconnected visible and NIR bands, peaking at 614 and 1125 nm, respectively. Notably, the full width at half-maximum (FWHM) of the NIR band exceeds 340 nm, significantly broader than most of the conventional phosphors doped with transition metal ions. Through a comprehensive combination of experimental investigations and crystal structure analysis, we elucidate the underlying mechanism of this ultra-broadband emission, attributing it to Bi3+ centers formed by the substitution of K+ and Mg2+ sites. This work expands the role of Bi3+ ions as activators in the second NIR (NIR-II) region, offering new insights into the design of ultra-broadband-emitting materials and introducing the only known phosphor capable of spanning the full 400 nm to 1700 nm spectrum, thereby filling a longstanding gap in this field.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"52 1","pages":"e202520587"},"PeriodicalIF":16.6,"publicationDate":"2025-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145339314","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