Angewandte Chemie最新文献_第10页

Carlos M. Cruz

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-08-12 DOI: 10.1002/ange.6852524

Carlos M. Cruz

引用次数: 0

Sterically Engineered Mo─V Cluster Catalyst for Switchable Z/E-Selective Alkyne Hydrophosphorylation 空间工程Mo─V簇催化剂可切换Z/ e选择性炔烃加氢磷酸化

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-07-30 DOI: 10.1002/ange.8728083

Yu-Feng Liu, Bao-Kuan Chen, Guo-Ping Yang, Zhi-Ming Zhang

{"title":"Sterically Engineered Mo─V Cluster Catalyst for Switchable Z/E-Selective Alkyne Hydrophosphorylation","authors":"Yu-Feng Liu, Bao-Kuan Chen, Guo-Ping Yang, Zhi-Ming Zhang","doi":"10.1002/ange.8728083","DOIUrl":"https://doi.org/10.1002/ange.8728083","url":null,"abstract":"<div>\u0000 \u0000 Stereodivergent alkyne hydrophosphorylation represents a formidable challenge in synthetic chemistry, particularly for selective and tunable synthesis of (Z)- and (E)-alkenylphosphine oxides. Herein, we report a steric hindrance–mediated strategy that achieves switchable Z/E selectivity via rational design of a metal–organic-functionalized phosphovanadomolybdate [PMo8V4O40(VO)2][(VO)(IM)4]3·5.5H2O (IM = 1-methylimidazole), which features a highly congested steric environment. Steric repulsion between the cluster framework and substrate enables highly Z-selective hydrophosphorylation, affording β-(Z)-alkenylphosphine oxides in up to 81% yield with Z/E ratio of 21:1. Incorporation of AgOAc as a stereochemical modulator switches the pathway to afford β-(E)-products in up to 80% yield with E/Z ratios up to 15:1. This heterogeneous catalytic system exhibits broad substrate tolerance, accommodating a diverse range of terminal alkynes with excellent chemo- and regioselectivity, including in the functionalization of complex pharmaceuticals, agrochemicals, and natural products, and gram-scale reactions with pharmaceutical substrates were achieved in this catalytic system. These findings not only provide practical solutions for stereodivergent hydrophosphorylation but also offer fundamental insights into steric control in transition metal–catalyzed transformations.\u0000 </div>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ionic Liquid Electrolytes for Extreme Temperature Conditions: Challenges and Perspective 极端温度条件下的离子液体电解质：挑战和前景

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-08-10 DOI: 10.1002/ange.7793957

En Xie, Chengdong Liu, Xinghao Wang, Jian Wang, Zhen Chen, Huihua Li, Wenlong Cai, Hao Li, Yang Peng, Fanglin Wu, Stefano Passerini, Haolin Tang

{"title":"Ionic Liquid Electrolytes for Extreme Temperature Conditions: Challenges and Perspective","authors":"En Xie, Chengdong Liu, Xinghao Wang, Jian Wang, Zhen Chen, Huihua Li, Wenlong Cai, Hao Li, Yang Peng, Fanglin Wu, Stefano Passerini, Haolin Tang","doi":"10.1002/ange.7793957","DOIUrl":"https://doi.org/10.1002/ange.7793957","url":null,"abstract":"The increasing applications of electrochemical energy-storage systems in transportation, aerospace, and grid applications impose stringent requirements on electrolytes capable of operating safely and efficiently across extreme temperatures. Conventional carbonate- or ether- based electrolytes suffer from performance degradation and severe safety hazards in extreme thermal environments. Ionic liquid electrolytes (ILEs), distinguished by their intrinsic nonflammability and remarkable resistance to temperature-induced property fluctuations, are recognized as promising alternatives. Nonetheless, the development of wide-temperature ILEs is constrained by their complex temperature-dependent physicochemical behaviors and interfacial instabilities. In this review, the effects of temperature on the molecular configurations, physicochemical properties, and interfacial chemistry of ILEs are systematically elucidated. The challenges associated with ILEs operation under low- and high-temperature conditions are subsequently delineated, with particular emphasis on recent advances in molecular design and co-solvent strategies aimed at improving the wide-temperature performance of ILEs. Furthermore, the interfacial chemistry and electrode compatibility of ILE-based systems are examined to demonstrate their roles in dictating interphase stability and electrochemical durability. Integrating molecular-level insights with macroscopic performance characteristics, this review presents a unified framework correlating the structure of ILEs with temperature-dependent performance, providing valuable guidance for the rational design of next-generation wide-temperature ILEs toward high-safety and high-energy-density rechargeable batteries.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.7793957","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068349","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Acetylene Semi-Hydrogenation by Photocatalysis 光催化乙炔半加氢

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-08-17 DOI: 10.1002/ange.5613575

Anna Fortunato, Brando Adranno, Sharon Silloni, Marianna Barbieri, Claudia Masia, Francesca Arcudi, Luka Đorđević

{"title":"Acetylene Semi-Hydrogenation by Photocatalysis","authors":"Anna Fortunato, Brando Adranno, Sharon Silloni, Marianna Barbieri, Claudia Masia, Francesca Arcudi, Luka Đorđević","doi":"10.1002/ange.5613575","DOIUrl":"https://doi.org/10.1002/ange.5613575","url":null,"abstract":"Acetylene to ethylene semi-hydrogenation is a cornerstone process in the production of polymer-grade feedstocks, yet it remains dominated by energy-intensive noble metal-based thermocatalysis. Photocatalysis is now emerging as a compelling alternative, using light to generate reactive intermediates under mild conditions and replacing hydrogen gas with safer proton sources such as water or alcohols. Although still in its infancy, this field is rapidly evolving, with a growing number of studies already achieving remarkable performances in both selectivity and efficiency. This Minireview provides an overview of photocatalytic acetylene semi-hydrogenation, framing recent advances within a broader industrial context. Emphasis is placed on mechanistic understanding, comparing π-complex, hydrogen atom transfer (HAT), and concerted proton-coupled electron transfer (CPET) pathways alongside the experimental tools used to distinguish them. Recent developments in both homogeneous and heterogeneous catalytic systems are discussed and key challenges related to efficiency, scalability, and techno-economic viability are presented, outlining design principles for next-generation, earth-abundant photocatalysts, and identifying opportunities for the transition from impurity removal to direct acetylene valorization.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.5613575","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068125","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Zähmung eines blauen Gases—Struktur und Chemie von Hexafluorthioaceton 蓝色气体结构的驯服与六氟硫丙酮的化学

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-07-16 DOI: 10.1002/ange.1044664

Hennes Günther, Antti J. Karttunen, Xiulan Xie, Frank Tambornino

引用次数: 0

Modulating Local Coordination in Single-Atom Catalysts: From Fundamental Concepts to Emerging Breakthroughs in Electrocatalysis 调节单原子催化剂的局部配位：从基本概念到电催化的新突破

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-08-05 DOI: 10.1002/ange.3059499

Ashwani Kumar, Harun Tüysüz

{"title":"Modulating Local Coordination in Single-Atom Catalysts: From Fundamental Concepts to Emerging Breakthroughs in Electrocatalysis","authors":"Ashwani Kumar, Harun Tüysüz","doi":"10.1002/ange.3059499","DOIUrl":"https://doi.org/10.1002/ange.3059499","url":null,"abstract":"Single-atom catalysts (SACs) have attracted significant interest due to their maximized atom efficiency, structural precision, and unique catalytic properties. While the central metal atom in SACs serves as the primary active site, its catalytic behavior is strongly influenced by the surrounding environment. The local coordination sphere plays a critical role in modulating the electronic structure and reaction pathway, thereby governing the overall activity, selectivity, and stability of SACs. Consequently, precise regulation of this coordination environment through rational engineering strategies is essential for optimizing the performance of SACs. Despite growing interest, comprehensive reviews systematically analyzing local coordination environments and metal-support interactions via electronic descriptors remain scarce, unlike synthesis/application-focused ones. In this review article, we provide an atomic-level, descriptor-driven analysis of coordination effects on the electrocatalytic performance of SACs, emphasizing the synergistic interplay between central metal atoms and their coordination spheres in activating key intermediates in reactions such as water splitting and oxygen/carbon dioxide reduction. We also highlight the unique features of advanced synthetic strategies for SACs, alongside the critical role of spectroscopic and microscopic techniques in elucidating structure–activity relationships, with particular focus on integrating operando investigations and theoretical calculations. Finally, recent advances, remaining challenges, and future opportunities in coordination-regulated SAC electrocatalysis are discussed.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.3059499","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068087","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electrochemical–Chemical Cascade Catalysis for Green Synthesis of Phenols Over a Three-Dimensional Hexaazatrinaphthalene-Based Covalent Organic Framework 三维六氮杂萘共价有机骨架上的电化学-化学级联催化绿色合成酚

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-07-30 DOI: 10.1002/ange.8627939

Tao Yang, Fantao Kong, Aiguo Kong, Xiangzhi Cui, Jianlin Shi

{"title":"Electrochemical–Chemical Cascade Catalysis for Green Synthesis of Phenols Over a Three-Dimensional Hexaazatrinaphthalene-Based Covalent Organic Framework","authors":"Tao Yang, Fantao Kong, Aiguo Kong, Xiangzhi Cui, Jianlin Shi","doi":"10.1002/ange.8627939","DOIUrl":"https://doi.org/10.1002/ange.8627939","url":null,"abstract":"<div>\u0000 \u0000 Phenols are essential intermediates widely used in chemical and pharmaceutical industries, yet conventional synthetic routes typically demand energy-intensive conditions and multi-step procedures. Herein, we report a green and efficient cascade strategy for phenol synthesis that integrates in situ electrochemical hydrogen peroxide (H2O2) generation with chemical oxidation of arylboronic acids using molecular oxygen under mild conditions. This approach demonstrates excellent functional-group tolerance and broad substrate scope (20 examples), achieving high conversion and selectivity without employing toxic solvents. A three-dimensional covalent organic framework (3D COF) with hexaazatrinaphthalene (HATN) building units and htp topology is designed as a robust electrocatalyst, delivering a remarkable H2O2 production rate of ∼7.0 mol gcat−1 h−1. Mechanistic studies reveal that the abundant nitrogen sites in the COF backbone act as hydrogen-bond acceptors, which facilitate proton transfer, promote a well-matched proton-coupled electron transfer (PCET) process, and stabilize the key *OOH intermediate, thereby collectively enhancing the selectivity and activity of the 2e− oxygen reduction reaction. Techno-economic (TEA) analysis further validates the potential economic feasibility of this integrated route based on laboratory scale. This work highlights the potential of rationally engineered 3D COFs to bridge electrosynthesis and synthetic chemistry, offering a mild and sustainable alternative to conventional energy-intensive phenols production.\u0000 </div>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068424","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Quantifying Microenvironment Effect on Metal Electronic Structure With Experimentally Accessible Descriptor: Examples of MOF-Incorporated Pt Catalysts 用实验可及描述子量化微环境对金属电子结构的影响：以mof掺杂Pt催化剂为例

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-07-30 DOI: 10.1002/ange.6798793

Weidong Zhang, Jiajia Huang, Ruichao Xu, Wentao Han, Mingyang Shen, Zhongyuan Lin, Jing-Yao Liu, Zhihu Sun, Hai-Long Jiang

{"title":"Quantifying Microenvironment Effect on Metal Electronic Structure With Experimentally Accessible Descriptor: Examples of MOF-Incorporated Pt Catalysts","authors":"Weidong Zhang, Jiajia Huang, Ruichao Xu, Wentao Han, Mingyang Shen, Zhongyuan Lin, Jing-Yao Liu, Zhihu Sun, Hai-Long Jiang","doi":"10.1002/ange.6798793","DOIUrl":"https://doi.org/10.1002/ange.6798793","url":null,"abstract":"<div>\u0000 \u0000 The chemical microenvironment surrounding metal nanoparticles (NPs) plays crucial roles in regulating their electronic structures. However, due to the lack of quantitative descriptor, such effect has been understood largely in a qualitative manner. To address this issue, a series of reticular metal-organic frameworks (MOFs) with diverse functional groups (MIP-206-X, X = OH, OCH3, H, Cl, and F) were synthesized, and Pt NPs with similar sizes and loadings were incorporated to afford Pt@MIP-206-X for ammonia borane methanolysis. X-ray absorption near edge structure (XANES) was adopted to determine the d-orbital occupancy of Pt, and the electronic contribution from MOFs was quantified as the descriptor Δe, which was demonstrated to accurately describe the Pt-methanol adsorption strength (quantified by activation entropy and methanol desorption temperature) and exhibit an excellent linear correlation with catalytic activity. Isotopic analyses and DFT calculations revealed that a larger Δe strengthens methanol adsorption on Pt, promotes O─H bond cleavage as the rate-determining step (RDS), and leads to enhanced activity.\u0000 </div>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pairing a Zn1O1 Monomer With Oxide Supports via Dual Interfacial Metal–Oxygen Bonding for Stable Conversion of Syngas to Light Olefins 通过双界面金属-氧键将zn101单体与氧化物载体配对以稳定合成气转化为轻烯烃

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-07-31 DOI: 10.1002/ange.3069256

Hengwei Wang, Jie Luo, Shang Li, Lulu Xu, Yuxing Xu, Huiting Wang, Xinyu Liu, Zhihu Sun, Shiqiang Wei, Wei-Xue Li, Junling Lu

{"title":"Pairing a Zn1O1 Monomer With Oxide Supports via Dual Interfacial Metal–Oxygen Bonding for Stable Conversion of Syngas to Light Olefins","authors":"Hengwei Wang, Jie Luo, Shang Li, Lulu Xu, Yuxing Xu, Huiting Wang, Xinyu Liu, Zhihu Sun, Shiqiang Wei, Wei-Xue Li, Junling Lu","doi":"10.1002/ange.3069256","DOIUrl":"https://doi.org/10.1002/ange.3069256","url":null,"abstract":"<div>\u0000 \u0000 Atomically dispersed metal oxides on oxide supports have garnered significant attention for their exceptional catalytic activity and selectivity, yet their practical application is often limited by poor stability. Here, we demonstrate that unlike isolated metal atoms on oxide supports, the stability of oxide monomers (e.g., Zn1O1, a prototype motif for a variety of (de)hydrogenation reactions) on oxide supports (M'O'x) tightly relies on delicate pairing of two interfacial bonds: Zn–O' and O–M'. Supports with too low oxygen vacancy formation energy (Ev) fail to firmly anchor the O anion in Zn1O1, whereas those with excessively high Ev bind weakly to the cationic Zn. Tetragonal ZrO2(100), possessing a moderate Ev, was theoretically screened to enable simultaneous optimization of the dual interfacial bonding and was experimentally verified through the anchoring of high-density Zn1 oxo monomers (1.5 Zn·nm−2) with exceptional resistance to aggregation and volatilization under harsh reductive conditions. When integrated with SAPO-34 zeolite for syngas conversion, this bifunctional catalyst achieves an unprecedented light olefins production rate (25.6 mmol·gcat−1·h−1) and sustains remarkable stability for over 200 h at 400 °C, outperforming all previously reported catalysts. The interfacial pairing principle provides a foundational guideline for designing highly stable and active atomically dispersed metal oxo catalysts.\u0000 </div>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068608","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tailoring Photonic Transport in Cluster-Assembled Crystals via Atomic-Level Coordination Engineering 利用原子级配位工程剪裁团簇组装晶体中的光子输运

Angewandte Chemie Pub Date : 2026-09-28 Epub Date: 2026-07-31 DOI: 10.1002/ange.8418370

Xiao Wei, Tinghui Zhang, Haoqi Li, Chen Zhu, Yan kuai, Xi Kang, Manzhou Zhu

{"title":"Tailoring Photonic Transport in Cluster-Assembled Crystals via Atomic-Level Coordination Engineering","authors":"Xiao Wei, Tinghui Zhang, Haoqi Li, Chen Zhu, Yan kuai, Xi Kang, Manzhou Zhu","doi":"10.1002/ange.8418370","DOIUrl":"https://doi.org/10.1002/ange.8418370","url":null,"abstract":"<div>\u0000 \u0000 The development of efficient optical waveguides requires precise control over photonic transport properties, yet linking atomic-level structure to device performance remains challenging. This study demonstrates that atomic-level coordination engineering of metal nanoclusters enables tailored photonic transport in cluster-assembled crystals. Using bidentate phosphine ligands as molecular scalpels, we constructed a series of Pt1Agx (x = 18–37) nanoclusters with identical icosahedral kernels but systematically varied peripheral structures. The resulting crystals exhibit exceptionally low optical loss coefficient, with the Pt1Ag18SR8Cl2(DPPP)4 (SR = 1-adamantanethiol, DPPP = 1,3-bis(diphenylphosphino)propane. Pt1Ag18-I for short.) crystal achieving a record-low among cluster-based active optical waveguides value of 6.4 × 10−4 dB µm−1. We establish quantitative positive correlations between waveguide performance and four key photophysical parameters: photoluminescence quantum yield, lifetime, refractive index, and polarization degree. This work provides a quantitative empirical structure–activity relationship (SAR) model for designing advanced photonic materials, bridging atomic-scale precision with macroscopic optical device functionality for next-generation integrated photonics.\u0000 </div>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 40","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149068550","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0