Angewandte Chemie (International ed. in English)最新文献_第4页

Covalent Organic Frameworks Anchoring Single-Atom Pt for Three-Phase Interface-Assisted Photocatalytic Overall Water Splitting. 共价有机框架锚定单原子Pt用于三相界面辅助光催化全面水分解。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-18 DOI: 10.1002/anie.202515397

Ting-Ting Sun, Hao Zhang, Ya Wang, Nan-Nan Zhang, Lu-Hua Shao, Hong Dong, Feng-Ming Zhang

{"title":"Covalent Organic Frameworks Anchoring Single-Atom Pt for Three-Phase Interface-Assisted Photocatalytic Overall Water Splitting.","authors":"Ting-Ting Sun, Hao Zhang, Ya Wang, Nan-Nan Zhang, Lu-Hua Shao, Hong Dong, Feng-Ming Zhang","doi":"10.1002/anie.202515397","DOIUrl":"https://doi.org/10.1002/anie.202515397","url":null,"abstract":"Covalent organic frameworks (COFs) are promising photocatalysts for overall water splitting (OWS) due to their high crystallinity, porosity and tunable structures. However, current COF-based systems rely on cocatalysts, which suffer from low atomic utilization and poor distribution due to aggregation. In addition, the oxygen reduction reaction (ORR) backward reaction severely undermines catalytic efficiency and stability in long time reaction. Herein, we present a strategy that combines atomically dispersed Pt sites anchored via N/O coordination within triazine-based COFs and a gas-liquid-solid three-phase interface-assisted photocatalytic system to enhance both performance and durability. As a result, the Pt-TBPyT-COF achieves superior OWS performance with H2 and O2 evolution rates of 469.8 and 234.9 µmol·g-1·h-1, respectively, and an apparent quantum yield of 8.91% at 450 nm. Notably, the OWS via gas-liquid-solid three-phase interface-assisted method effectively suppresses ORR backward reaction and reaches average rates as high as 568.7 and 284.3 µmol·g-1·h-1 for H2 and O2 in 5 h, respectively, and maintained stable photocatalytic activity over a 30 h continuous reaction. Further, density functional theory calculations and in situ experiments reveal that the single-atoms Pt coordination accelerates *H desorption, while the triazine units in COFs benefits charge separation and reduced energy barriers of OER rate-determining step.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202515397"},"PeriodicalIF":16.9,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145083062","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

Difluoro Carbenes: From Genuine Gold Complexes to Unprecedented Metallacyclic Reactivity. 二氟碳烯：从真金配合物到空前的金属环反应性。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-18 DOI: 10.1002/anie.202515429

David Vesseur, Shuo Li, Nina Albouy, Pierre Lavedan, Sonia Mallet-Ladeira, Karinne Miqueu, Didier Bourissou

引用次数: 0

The First Ferrocene-Based Molecular Ferroelectric Accompanied by Spatial Symmetry Operation Breaking. 第一个伴有空间对称操作破缺的二茂铁基铁电分子。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-18 DOI: 10.1002/anie.202517414

Zunqi Liu, Jun-Chao Liu, Shu-Wen Xiong, Ren-Gen Xiong, Huan-Huan Chen

{"title":"The First Ferrocene-Based Molecular Ferroelectric Accompanied by Spatial Symmetry Operation Breaking.","authors":"Zunqi Liu, Jun-Chao Liu, Shu-Wen Xiong, Ren-Gen Xiong, Huan-Huan Chen","doi":"10.1002/anie.202517414","DOIUrl":"https://doi.org/10.1002/anie.202517414","url":null,"abstract":"Ferroelectric materials with switchable spontaneous polarization have attracted significant interest over the past decades. Molecular ferroelectrics particularly offer unique advantages such as structural tunability, inducible intrinsic homochirality, and ease of processing, features often unattainable in inorganic ceramics. Ferrocene derivatives have been widely used in pharmaceuticals, sensing, and solar energy conversion. However, developing a single-component ferrocene-based ferroelectric remains a major challenge. In this work, we report, for the first time, a chiral, single-component ferrocene-based ferroelectric, Fe(C5H5)(C5H4COO-CHOL), via the homochirality strategy. Notably, this compound undergoes a reversible structural phase transition at 193 K, switching from the polar space group C2 to another polar space group, P21, while maintaining the same point group. This transition only involves a symmetry operation change from a 2-fold rotation and screw rotation (C2) to a single 2-fold screw axis (P21). The ferroelectric nature was confirmed through piezoresponse force microscopy and polarization-electric field hysteresis loop measurements. Its non-centrosymmetric structure was validated by a polarized second-harmonic generation measurement. To our knowledge, this is the first report of a homochiral, single-component ferrocene-based ferroelectric undergoing phase transitions involving only spatial symmetry operation breaking. This work broadens the collection of chiral and ferrocene-based ferroelectrics and offers valuable insights for designing new ferroelectric materials.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202517414"},"PeriodicalIF":16.9,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145083154","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

Sustainable Fluorinated Silicon Dielectric Design for Enhanced Contact-Electro-Chemistry. 增强接触电化学的可持续氟化硅介电设计。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-18 DOI: 10.1002/anie.202517059

Ting Gan, Zhijian Li, Shaoxin Li, Hanbin Liu, Gehan Amaratunga, Zhonglin Wang, Di Wei

{"title":"Sustainable Fluorinated Silicon Dielectric Design for Enhanced Contact-Electro-Chemistry.","authors":"Ting Gan, Zhijian Li, Shaoxin Li, Hanbin Liu, Gehan Amaratunga, Zhonglin Wang, Di Wei","doi":"10.1002/anie.202517059","DOIUrl":"https://doi.org/10.1002/anie.202517059","url":null,"abstract":"Solid-liquid contact electrification (CE) has recently emerged as a powerful means of initiating interfacial chemical reactions via charge transfer. Fluorinated ethylene propylene (FEP) and polytetrafluoroethylene (PTFE) are frequently employed as solid dielectrics owing to their fluorine-rich surfaces, which exhibit strong electron-withdrawing characteristics. However, their high environmental cost and poor surface modifiability hinder the broader adoption of contact-electro-chemistry (CE-Chemistry). Here, we report a low-cost and tunable dielectric alternative based on silicon powder, surface-functionalized with fluorinated alkyl chains to mimic the interfacial properties of conventional fluoropolymers. Fluorinated silicon powders (F-Si) were synthesized via a mild self-assembly approach using 1H,1H,2H,2H-perfluorodecyltriethoxysilane. The resulting F-Si powders exhibited a 30-fold enhancement in methyl orange degradation efficiency compared to unmodified silicon, and a 4-fold improvement in phenol degradation relative to size-matched FEP powder. In contrast, aggressive fluorination via piranha-assisted pretreatment (P-F-Si) induced particle aggregation and loss of CE reactivity, highlighting the importance of controlled surface engineering. Furthermore, CE-Chemistry enabled the first noble-metal-free oxidation of I- to I3 -, establishing a low-energy, cost-effective paradigm for catalytic iodine conversion. Together, these advances provide a sustainable materials design framework for CE-Chemistry, with broad implications for scalable, green chemical transformation technologies.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202517059"},"PeriodicalIF":16.9,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145083190","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

Synthesis of Hydroxy-Functionalized Polyethylene via Radical Copolymerization of Ethylene with Alkenyl Boronate and Post-Polymerization Oxidation. 乙烯与硼酸烯基自由基共聚及聚合后氧化合成羟基功能化聚乙烯。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-18 DOI: 10.1002/anie.202518871

Tomoaki Kanazawa, Tommaso Posenato, Sébastien Norsic, Tsuyoshi Nishikawa, Makoto Ouchi, Jean Raynaud, Franck D'Agosto

引用次数: 0

Jess M. Clough. 杰西·m·克拉夫。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-18 DOI: 10.1002/anie.202519808

Jess M Clough

引用次数: 0

Bifunctional Silylene-Aminoborane Enables Cooperative Activation of Unsaturated Bonds and Access to Heteroatom-Enriched Polycycle. 双功能硅烯-氨基硼烷使不饱和键协同活化和获得富集杂原子的多环。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-17 DOI: 10.1002/anie.202515808

Zheng Su, Mingdong Zhong, Xixi Meng, Ren Gao, Jiancheng Li, Minyi Yuan, Herbert W Roesky, Shaoguang Zhang

引用次数: 0

Circularly Polarized Luminescence Optical Waveguides Based on One-Dimensional Hybrid Copper-Silver Bromide Crystal. 基于一维杂化铜-溴化银晶体的圆偏振发光光波导。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-17 DOI: 10.1002/anie.202515434

Yuxuan Wang, Yi Wei, Xiaofan Xu, Huimin Kang, Shizhe Ren, Hilary Zhang, Yong Sheng Zhao, Zewei Quan

{"title":"Circularly Polarized Luminescence Optical Waveguides Based on One-Dimensional Hybrid Copper-Silver Bromide Crystal.","authors":"Yuxuan Wang, Yi Wei, Xiaofan Xu, Huimin Kang, Shizhe Ren, Hilary Zhang, Yong Sheng Zhao, Zewei Quan","doi":"10.1002/anie.202515434","DOIUrl":"https://doi.org/10.1002/anie.202515434","url":null,"abstract":"Chiroptical waveguides, capable of generating and propagating circularly polarized light (CPL), hold significant promise for next-generation optoelectronic devices. However, developing novel, efficient chiroptical waveguides remains challenging, due to the difficulty of integrating strong intrinsic chiroptical activity with efficient directional light transport within a single crystalline material. Here, we report a new enantiomeric pair of chiral hybrid metal halides, (S/R-C5H14N2)CuAgBr4 (S/R-CuAg), featuring a one-dimensional inorganic structure. Ag incorporation enhances photoluminescence quantum yield from 0.6% to 18.6%, while enabling bright CPL emissions with dissymmetry factors (glum) of ± 7 × 10-3. The tightly packed inorganic lattice and highly anisotropic microstructure of S/R-CuAg exhibit a low optical loss coefficient of 9.6 × 10-3 dB µm-1. Crucially, microrod crystals of S/R-CuAg function as efficient chiroptical waveguides, simultaneously emitting and propagating CPL under unpolarized light excitation. This work establishes chiral hybrid metal halides as a viable platform for circularly polarized waveguide applications.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202515434"},"PeriodicalIF":16.9,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145083050","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

Modulating Adsorption Intermediate Metastability for Tip-Directed Zinc Stripping and Suppressed Vanadium Dissolution Toward Long-Cycling Zinc-Vanadium Batteries. 对长循环锌-钒电池的定向锌剥离和抑制钒溶解的调节吸附中间亚稳态。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202515085

Zixin Han, Zuyang Hu, Xiaolong Jiang, Haoxin Liu, Kai Bai, Jianlong Cong, Yufei Zhang, Wencheng Du, Minghui Ye, Yongchao Tang, Xiaoqing Liu, Zhipeng Wen, Cheng Chao Li

{"title":"Modulating Adsorption Intermediate Metastability for Tip-Directed Zinc Stripping and Suppressed Vanadium Dissolution Toward Long-Cycling Zinc-Vanadium Batteries.","authors":"Zixin Han, Zuyang Hu, Xiaolong Jiang, Haoxin Liu, Kai Bai, Jianlong Cong, Yufei Zhang, Wencheng Du, Minghui Ye, Yongchao Tang, Xiaoqing Liu, Zhipeng Wen, Cheng Chao Li","doi":"10.1002/anie.202515085","DOIUrl":"https://doi.org/10.1002/anie.202515085","url":null,"abstract":"The metastable adsorbed intermediates formed during the lattice detachment of Zn atoms and Vn + ions govern the reaction kinetics and interfacial morphology evolution during dissolution. Resultant inhomogeneous Zn stripping and progressive V dissolution synergistically promote dead Zn formation and cathode material degradation, substantially impeding the commercialization of Zn-V batteries. Here, to facilitate Zn tip-stripping electrochemistry and suppressed vanadium dissolution, a robust adhesion ionic liquid ([BVIM]Br) modified PAM gel electrolyte (PAM-IL) was strategically designed. Leveraging steric hindrance of polymer segments and the directional coordination of anions and cations, the PAM-IL electrolyte delocalizes charge accumulation and suppresses overstabilization of tip-localized complexes, thereby reversing the adsorption asymmetry behavior (ΔGads-tip > ΔGads-root) to achieve tip-targeted zinc stripping. Concurrently, strong ion-dipole interactions within PAM-IL elevate the activation barrier for V dissolution and combine with its butyl-functionalized hydrophobic moieties to impede water molecule penetration and suppress vanadium dissolution. Therefore, the as-prepared Zn||PAM-IL||NH4V4O10 batteries deliver a reversible capacity of 266.4 mAh g-1 at 1 A g-1 after 2000 cycles and retained a higher capacity retention (82.3%) after 250 cycles than aqueous electrolyte (28.1%) with extreme-low current density of 0.2 A g-1. Furthermore, the PAM-IL exhibits exceptional cycling stability over a wide temperature range, from 0 °C to 60 °C.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202515085"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145077156","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

High-Entropy Metallene Aerogels: A New Balancer for *H Production and Consumption in Nitrate Reduction Reaction. 高熵金属烯气凝胶：硝酸还原反应中*H生成和消耗的新型平衡剂。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2025-09-16 DOI: 10.1002/anie.202505156

Hanjun Li, Zhen Huang, Yimin Wang, Guangtong Hai, Wei-Hsiang Huang, Chun-Chi Chang, Min-Hsin Yeh, Feili Lai, Nan Zhang, Tianxi Liu

{"title":"High-Entropy Metallene Aerogels: A New Balancer for *H Production and Consumption in Nitrate Reduction Reaction.","authors":"Hanjun Li, Zhen Huang, Yimin Wang, Guangtong Hai, Wei-Hsiang Huang, Chun-Chi Chang, Min-Hsin Yeh, Feili Lai, Nan Zhang, Tianxi Liu","doi":"10.1002/anie.202505156","DOIUrl":"https://doi.org/10.1002/anie.202505156","url":null,"abstract":"High-entropy metallene aerogels (HEMAs), synergizing high-entropy metallenes and metallic aerogels, face challenges in achieving single-phase structures due to multi-metallic nucleation/growth disparities, hindering two-dimensional anisotropic growth and three-dimensional assembly of multi-component nanocrystals. Herein, the universal preparation of HEMAs was achieved by a seed-mediated synthetic route for electrochemical nitrate reduction reaction (NO3RR). PdCuSnCoNi HEMAs exhibit maximum Faradaic efficiency and yield rate of NH3 up to 99.5% and 4117.8 µg h-1 mgcat. -1, surpassing those of Pd metallene aerogels (MAs). In situ attenuated total reflection infrared absorption spectroscopy, online differential electrochemical mass spectrometry and density functional theory calculations reveal kinetic match for *NO3 to *NO2 and *NO2 to *NH3, with the energy barrier for *NO2 formation (potential-determining step) being lower than that for *H to H2, balancing production and consumption of *H and facilitating NH3 generation on PdCuSnCoNi HEMAs. This study paves the way for efficient NO3RR catalysts and guides rational design for diverse electrocatalytic systems.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e202505156"},"PeriodicalIF":16.9,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145077147","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